UC- 41, Health and Safety

N U C L E A R S A F E T Y Q U A R T E R L Y R E P O R T

F E B R U A R Y , MARCH, A P R I L , 1 9 7 0

FOR

U S A E C D I V I S I O N O F R E A C T O R D E V E L O P M E N T A N D TECHNOLOGY

T h e S t a f f o f B a t t e l l e - N o r t h w e s t

May 1 9 7 0

BATTELLE MEMORIAL INSTITUTE PACIFIC NORTHWEST LABORATORIES RI CHLAND, WASHINGTON 99352

I P r i n t e d i n t h e Uni ted S t a t e s o f America I Ava i l ab l e from I C lear inghouse f o r Fede ra l S c i e n t i f i c and Techn ica l In fo rmat ion I Na t i ona l Bureau o f S t anda rds , U.S. Department o f Commerce I S p r i n g f i e l d , V i r g i n i a 22151 I I P r i c e : P r i n t e d Copy $ 3 . 0 0 ; Microf iche $ 0 . 6 5

N U C L E A R S A F E T Y Q U A R T E R L Y R E P O R T

F E B R U A R Y , MARCH, A P R I L , 1 9 7 0

FOR

U S A E C D I V I S I O N O F R E A C T O R D E V E L O P M E N T A N D T E C H N O L O G Y

BY T h e S t a f f o f B a t t e l l e - N o r t h w e s t

FOREWORD

T h i s r e p o r t i s t h e t h i r t e e n t h o f a s e r i e s i n which P a c i f i c

Nor thwest L a b o r a t o r i e s r e p o r t s i t s n u c l e a r s a f e t y - r e l a t e d

s t u d i e s b e i n g pe r fo rmed f o r t h e USAEC D i v i s i o n o f R e a c t o r

Development and Technology.

P R E V I O U S R E P O R T S I N T H I S S E R I E S

BNWL-433

BNWL- 537

BNWL- 7 5 4

BNWL- 816

BNWL- 885

BNWL- 894

BNWL-926

BNWL-1009

BNWL-1084

BNWL-1187

BNWL-1266

BNWL-1315

J a n u a r y , F e b r u a r y , March

A p r i l , May, June

J u l y , Augus t , September , Oc tobe r

November, December, 1967, J a n u a r y

F e b r u a r y , March, A p r i l

May, J u n e , J u l y

Augus t , September , Oc tobe r

November, December, 1968 , J a n u a r y

F e b r u a r y , March, A p r i l

May, J u n e , J u l y

Augus t , September , Oc tobe r

1 November, Qecember, 1969, J a n u a r y

TABLE OF CONTENTS

1. SUMMARY. . 1.1

2 . E N G I N E E R E D SAFETY SYSTEMS STUDIES . . 2 . 1

Conta inment Systems Exper iment - G . J. Rogers . . 2 . 1

F i s s i o n P r o d u c t T r a n s p o r t S t u d i e s - R. K . H i l l i a r d , J . D. McCormack, and L . F . C o l e m a n . . 2 . 1

Coo lan t Blowdown S t u d i e s - R. T. Allemann, W . C . Townsend, A . S . N e u l s , M . E . Wi therspoon and A. J . McElf resh . . 2.19

3 . PRESSURE BEARING COMPONENT EVALUATION AND MONITORING STUDIES . . 3 . 1

Crack D e t e c t i o n i n P r e s s u r e P i p i n g by A c o u s t i c Emiss ion - P. H . Hu t ton and J . B . Ve t r ano . . 3 . 1

Work P l a n n e d f o r Next Q u a r t e r . . 3.9

4 . ENVIRONMENTAL STUDIES . . 4 . 1

C a l c u l a t i o n o f t h e P o t e n t i a l Env i ronmen ta l R a d i o l o g i c a l Consequences o f R e a c t o r A c c i d e n t s - M. M . Hendr i ckson . . 4 . 1

Reg iona l Model ing o f S u r f a c e Water Tempera ture f rom P r o j e c t e d Power Growth - R. T. J a s k e and D. E . P e t e r s o n . . 4 . 1 3

5 . FIXATION OF RADIOACTIVE RESIDUES . . 5 . 1

O v e r a l l S t a t u s o f WSEP R a d i o a c t i v e Demons t r a t ions . 5 . 1

Spray S o l i d i f i c a t i o n . . 5.2

L a b o r a t o r y S t u d i e s . . 5 . 2

I n - P o t M e l t i n g Development . . 5.2

C o r r o s i o n S t u d i e s . 5 . 7

A n a l y s i s of Rad io ru then ium i n WSEP S o l i d i f i e d Waste P r o d u c t s . . . . 5.9

E n g i n e e r i n g S t u d i e s . . 5.10

I n - P o t M e l t i n g Development . . 5.10

R a d i o a c t i v e Demons t r a t ions . . 5.15

Spray S o l i d i f i c a t i o n Run SS-11 . 5 .15

A u x i l i a r y P r o c e s s Equipment Per formance Dur ing Run SS-11 . . 5.20

Spray S o l i d i f i c a t i o n Run SS-12 (IPM) . . 5.29

High-Level Wastes f rom Advanced R e p r o c e s s i n g Techniques . . 5.33

E v a l u a t i o n o f S o l i d i f i e d Waste P r o d u c t s . 5.37

N o n r a d i o a c t i v e L a b o r a t o r y S t u d i e s . . 5.37

Mel t S e g r e g a t i o n S t u d i e s o f S i m u l a t e d S o l i d i f i e d Wastes S t o r e d a t High Tempera tures f o r Extended P e r i o d s 5.37

P r o d u c t Measurement, T e s t i n g and S t o r a g e 5 . 4 2

S o l i d s S t o r a g e E n g i n e e r i n g T e s t F a c i l i t y (SSETF) . 5 . 4 2

6 . HEAVY SECTION STEEL TECHNOLOGY PROGRAM . . 6 . 1

I r r a d i a t i o n E f f e c t on t h e F r a c t u r e o f Heavy S e c t i o n P r e s s u r e V e s s e l S t e e l s - C . W . H u n t e r , J . A . W i l l i a m s , and C . L . H e l l e r i c h . 6 . 1

N U C L E A R S A F E T Y Q U A R T E R L Y R E P O R T

F E B R U A R Y , MARCH, A P R I L , 1 9 7 0

FOR

U S A E C D I V I S I O N O F R E A C T O R D E V E L O P M E N T A N D T E C H N O L O G Y

BY

T h e S t a f f o f B a t t e l l e - N o r t h w e s t

1 . SUMMARY

E N G I N E E R E D S A F E T Y S Y S T E M S S T U D I E S

Containment Svs tems E x ~ e r i m e n t (CSEI

The s e r i e s o f f i v e l a r g e s c a l e d e m o n s t r a t i o n r u n s t o

e v a l u a t e t h e per formance o f a i r c l e a n i n g sys t ems i n removing

a i r b o r n e f i s s i o n p r o d u c t s i n a con ta inmen t v e s s e l was comple ted

w i t h two runs d u r i n g t h e q u a r t e r . Run A-16 e v a l u a t e d s y s t e m

per formance d u r i n g an e x t e n d e d d u r a t i o n r e l e a s e o f f i s s i o n

p r o d u c t a e r o s o l m a t e r i a l . Run A-17 e v a l u a t e d sys t em p e r f o r -

mance a t a h i g h e r f low r a t e t h a n i n p r e c e d i n g r u n s .

R e s u l t s from t h e s e runs were c o n s i s t e n t w i t h p r e d i c t i o n s

o f s i m p l e m a t h e m a t i c a l models b a s e d on a w e l l mixed gas volume

f o r a b o u t 2 h r a f t e r t h e s t a r t o f a i r c l e a n i n g sys t em o p e r a t i o n .

A f t e r 2 h r , t h e removal r a t e o f f i s s i o n p r o d u c t s was s l o w e r .

The e a r l y removal r a t e was s l i g h t l y s l o w e r t h a n p r e d i c t e d f o r

most f i s s i o n p r o d u c t s ; however , t h e e l e m e n t a l i o d i n e was

removed more r a p i d l y t h a n p r e d i c t e d . The more r a p i d removal

o f e l e m e n t a l i o d i n e i s b e l i e v e d t o r e s u l t from t h e e f f e c t o f

h i g h e r gas p h a s e v e l o c i t y induced by t h e a i r c l e a n i n g l o o p

o p e r a t i o n . The h i g h e r gas v e l o c i t y r e s u l t e d i n a more r a p i d

d e p o s i t i o n o f e l e m e n t a l i o d i n e by n a t u r a l p r o c e s s e s .

A s e r i e s o f s m a l l s c a l e e x p e r i m e n t s was pe r fo rmed i n a

9 0 5 - l i t e r s t a i n l e s s s t e e l t a n k t o e v a l u a t e t h e g a s - l i q u i d

d i s t r i b u t i o n o f i o d i n e i n b a s e - b o r a t e con ta inmen t s p r a y

s o l u t i o n s . Such d a t a a r e needed f o r p r e d i c t i o n s o f s p r a y s y s -

tem e f f e c t i v e n e s s i n removing a i r b o r n e e l e m e n t a l i o d i n e i n con-

t a i n m e n t . C o n t r a r y t o t h e o r e t i c a l p r e d i c t i o n s , t h e d i s t r i b u t i o n

c o e f f i c i e n t a t t h e i n s t a n t o f i o d i n e r e l e a s e was found t o

i n c r e a s e w i t h i n c r e a s i n g l i q u i d p h a s e i o d i n e c o n c e n t r a t i o n . I n

a l l c a s e s , v a l u e s were s u f f i c i e n t l y h i g h ( ~ 5 0 0 0 ) t o c a u s e

n e g l i g i b l e l i q u i d p h a s e t r a n s f e r r e s i s t a n c e .

A d d i t i o n a l blowdown e x p e r i m e n t s were comple ted i n which

v o i d f r a c t i o n d a t a i n t h e o u t l e t p i p e were o b t a i n e d f o r com-

p a r i s o n w i t h h i g h s p e e d p h o t o g r a p h i c r e c o r d s o f b u b b l e forma-

t i o n i n t h e o u t l e t .

P R E S S U R E B E A R I N G COMPONENT E V A L U A T I O N A N D M O N I T O R I N G S T U D I E S

Crack D e t e c t i o n i n P r e s s u r e P i p i n g by A c o u s t i c Emiss ion

S tudy o f a c o u s t i c e m i s s i o n p roduced by t h e f a t i g u e f a i l u r e

p r o c e s s i n m e t a l h a s r e s u l t e d i n t a n g i b l e e v i d e n c e t h a t t h e

n u c l e a t i o n o f a macrocrack i s i d e n t i f i a b l e by i t s a c o u s t i c

e m i s s i o n , The same work a l s o p roduced e v i d e n c e o f t h e f l a w

s i z e r e s o l u t i o n a t t a i n a b l e i n ca rbon s t e e l by a c o u s t i c e m i s s i o n -

i . e . , m i c r o c r a c k i n g produced r e a d i l y d e t e c t a b l e e m i s s i o n .

P a p e r s on a c o u s t i c e m i s s i o n were p r e s e n t e d a t t h r e e t e c h -

n i c a l group mee t ings d u r i n g t h i s r e p o r t p e r i o d .

F I X A T I O N O F R A D I O A C T I V E R E S I D U E S

To d a t e , 29 r a d i o a c t i v e d e m o n s t r a t i o n s i n WSEP have been

comple ted w i t h s i m u l a t e d w a s t e s which c o n t a i n e d a p p r o x i m a t e l y

45 M C i o f mixed r a d i o n u c l i d e s b e i n g c o n v e r t e d t o s o l i d s .

Dur ing t h e r e p o r t p e r i o d , a p p r o x i m a t e l y 4 . 5 M C i o f r a d i o -

a c t i v i t y were p r o c e s s e d d u r i n g t h e 1 1 t h and 1 2 t h s p r a y s o l i d i -

f i c a t i o n r u n s . Spray s o l i d i f i c a t i o n Run SS-11 p r o c e s s e d a

s i m u l a t e d Purex Waste t y p i c a l o f t h a t which would r e s u l t from

t h e r e p r o c e s s i n g o f a LMFBR c o r e f u e l (100,000 MWd/tonne a t

200 MW/tonne) and marked t h e comple t ion o f WSEP s p r a y s o l i d i -

f i e r runs u s i n g a h i g h - t e m p e r a t u r e p l a t i n u m m e l t e r . Sp ray

S o l i d i f i c a t i o n Run SS-12 (IPM) was s u c c e s s f u l l y comple ted

u s i n g t h e B a t t e l l e - N o r t h w e s t deve loped i n - p o t m e l t i n g t e c h -

n i q u e . During t h i s r u n , s p r a y c a l c i n e d PW-4m w a s t e was m e l t e d

w i t h a b o r o s i l i c a t e g l a s s f r i t d i r e c t l y i n t h e f i n a l s t o r a g e

c o n t a i n e r w i t h o u t t h e need f o r a p l a t i n u m m e l t e r . Only 1 . 9 %

o f t h e ru thenium i n t h e p r o c e s s e d f e e d was v o l a t i l i z e d from

t h e s p r a y s o l i d i f i e r d u r i n g Run SS-12 (IPM) which v e r i f i e s t h e

r e s u l t s o f deve lopmenta l r u n s which i n d i c a t e d t h a t t h e

ru then ium v o l a t i l i z a t i o n from t h e s p r a y s o l i d i f i e r was r educed

s i g n i f i c a n t l y when p h o s p h o r i c a c i d was n o t added t o t h e f e e d .

A new method f o r a n a l y z i n g l o 6 ~ u i n t h e s p r a y s o l i d i f i e r

and i n t h e phospha te g l a s s s o l i d i f i e d w a s t e p r o d u c t s was

developed s u c c e s s f u l l y . The t e c h n i q u e i n v o l v e s t h e d i r e c t

gamma s c a n o f t h e s o l i d samples and ( u n l i k e p r e v i o u s d i s s o l u -

t i o n t e c h n i q u e s ) r o u t i n e l y g i v e s h i g h ru thenium r e c o v e r i e s .

H E A V Y S E C T I O N S T E E L T E C H N O L O G Y P R O G R A M

I r r a d i a t i o n E f f e c t s on t h e F r a c t u r e o f Heavy S e c t i o n

P r e s s u r e V e s s e l S t e e l s

I r r a d i a t i o n o f 1- i n . - t h i c k t r a n s v e r s e o r i e n t a t i o n b a s e

m a t e r i a l and submerged a r c weldment specimens have been

s c h e d u l e d f o r t h e E T R- M 3 l o o p d u r i n g Cycles 108 , 1 0 9 A , 111,

and 1 1 2 . S p e c i f i c gamma h e a t e x p e r i m e n t s i n t h e ATR have

been comple ted , which w i l l e n a b l e t h e f i n a l d e s i g n and con-

s t r u c t i o n o f t h e 4 - i n . - t h i c k specimen f a c i l i t y . The f a t i g u e

c r a c k p r o p a g a t i o n r a t e i n i r r a d i a t e d spec imens may be d o u b l e

t h a t o f u n i r r a d i a t e d m a t e r i a l .

2 . E N G I N E E R E D S A F E T Y S Y S T E M S S T U D I E S

C O N T A I N M E N T S Y S T E M S E X P E R I M E N T - G. J . R o g e r s

F i s s i o n P r o d u c t T r a n s p o r t S t u d i e s - R. K . H i l l i a r d ,

J . D. McCormack, and L . F. Coleman

Large A i r C lean ing System Exper iments - J . D. McCormack

T e s t s were c o n t i n u e d o f a i r c l e a n i n g s y s tems o p e r a t i n g

w i t h i n a con ta inmen t v e s s e l under l o s s - o f - c o o l a n t a c c i d e n t

c o n d i t i o n s . Two r u n s a r e r e p o r t e d . Run A-16 i n v o l v e d a 2 - h r

l i n e a r f i s s i o n p r o d u c t s i m u l a n t r e l e a s e . For Run A - 1 7 , t h e 3 a i r f low was i n c r e a s e d from a nominal 1000 t o 1850 f t / m i n e

The e x p e r i m e n t a l c o n d i t i o n s a r e summarized i n T a b l e 2 . 1 . T h i s

comple te s t h e p l a n n e d s e r i e s o f f i v e a i r c l e a n i n g t e s t s .

TABLE 2.1. Summary of Run Conditions

Date

Containment Atmosphere S a t u r a t e d Steam-Air S a t u r a t e d Steam-Air

Tempera tu re , OF 245 246

P r e s s u r e , p s i a 48 48

Loop f low, a c t u a l f t 3 / m i n 1000

T e s t D u r a t i o n , h r 45

Loop Components Condenser , AT - 2 OF ( i n o r d e r of f low) Demis te r 1 8 - i n .

d i a m e t e r P r e f i l t e r A b s o l u t e P a r t i c u -

l a t e F i l t e r 3 Charcoa l Beds i n

S e r i e s , 1 - i n . - t h i c k each

Condenser , AT %1 OF Demis ter 2 x 2 f t ,

s q u a r e - Abso lu te P a r t i c u -

l a t e F i l t e r 3 Charcoa l Beds i n

S e r i e s , 1 - i n . - t h i c k e a c h

A e r o s o l R e l e a s e I 2 60 min, 104 g 10 min, 100 g

d u r a t i o n and C s 120 min, 215 g 10 min, 2 g

amount d e l i v e r e d U02 120 min, $1 g 20 min, %1 g

t o v e s s e l

a tmosphere CH31 10 min, 5 g 10 min, 5 g

Run A-16 t e s t e d t h e e f f e c t i v e n e s s o f t h e a i r c l e a n i n g l o o p

f o r f i s s i o n p r o d u c t s i m u l a n t removal d u r i n g c o n d i t i o n s o f an

ex tended FP r e l e a s e . The f low was e s t a b l i s h e d th rough t h e

t e s t loop j u s t b e f o r e commencement o f a e r o s o l r e l e a s e . The

i o d i n e was r e l e a s e d a t a un i fo rm r a t e f o r 50 min and a l l i o d i n e

r e l e a s e was s t o p p e d a t 60 min. The cesium was r e l e a s e d a t a

l i n e a r r a t e f o r 120 min. The c o n c e n t r a t i o n s i n t h e main gas

s p a c e were p l o t t e d a s a f u n c t i o n o f t ime i n F i g u r e 2 . 1 and 2 . 2 .

I t a p p e a r s t h a t n o t a l l o f t h e r e l e a s e d a e r o s o l was u n i f o r m l y

d i s t r i b u t e d th roughou t t h e gas s p a c e and t h a t some i o d i n e and

cesium were d e p o s i t e d r a p i d l y n e a r t h e p o i n t o f r e l e a s e i n t h e

d r y w e l l .

I f t h e r e l e a s e r a t e i s c o n s t a n t and t h e r e l e a s e d mass i s

u n i f o r m l y d i s p e r s e d th roughou t t h e gas s p a c e , E q u a t i o n (1) can

be used t o s o l v e f o r t h e t o t a l mass r e l e a s e d . (1)

where Wo = t o t a l mass r e l e a s e d i n t ime tR, g

A = o v e r a l l removal r a t e c o n s t a n t , rnin - 1

V = gas volume, m 3

tR = t ime d u r a t i o n o f r e l e a s e , min

t = t ime a f t e r s t a r t of r e l e a s e , rnin

= c o n c e n t r a t i o n i n gas s p a c e a t t ime t , g/m 3

By u s i n g E q u a t i o n (1) i t i s c a l c u l a t e d t h a t 4 8 g o f cesium

and 2 2 g o f i o d i n e were r e l e a s e d t o t h e main room gas s p a c e .

The uranium r e l e a s e was n o t un i fo rm a s ev idenced by t h e d e c r e a s -

i n g c o n c e n t r a t i o n d u r i n g t h e r e l e a s e p e r i o d . The removal o f

m a t e r i a l from t h e gas s p a c e by t h e l o o p can be found from t h e

o b s e r v e d c o n c e n t r a t i o n h a l f - t i m e s and by a l lowance f o r t h e

n a t u r a l removal r a t e s , a s de te rmined from o t h e r exper imen t s

d u r i n g t imes where t h e a i r loop was n o t o p e r a t i n g . T h i s p e r -

formance i s i n d i c a t e d i n Tab le 2 . 2 .

TABLE 2 . 2 . Aeroso l Behav io r i n CSE Run A-16 (a)

Concen t ra t ion H a l f ~ T i m e , min

Measured, N a t u r a l Only C'Cmax N a t u r a l , . (Average o f s C a l c u l a t e d , a t

Form and Loop 8 CSE Runs) Loop Only t = 1000 min

Elementa l I o d i n e 7 . 3 15 1 4 . 3 1 . 8 x

Methyl I o d i d e 16 - 16 1 . 7 x

Cesium 9 . 3 4 7 11 .5 8 x 1 0 - '

P a r t i c u l a t e Iod ine 15 3 6 25 .7 3

Uranium ~ 1 6 3 1 3 3

Average 2 0 . 1

a. E x p e c t e d t = 0 . 6 9 3 V - ( 0 . 6 9 3 ) ( 2 1 , 0 0 0 ) = 1 4 . min

1 / 2 F 1 0 2 0

The obse rved removal r a t e s a r e i n r e a s o n a b l e agreement

w i t h t h e c a l c u l a t e d removal w i t h t h e e x c e p t i o n o f p a r t i c l e

a s s o c i a t e d i o d i n e fo rms , f o r which t h e n e t removal was s l o w e r

t h a n e x p e c t e d . T h i s may i n p a r t be induced by a s low con-

t i n u e d r e l e a s e from t h e d e l i v e r y l i n e d u r i n g t h e b a l a n c e o f

t h e cesium r e l e a s e . The uranium h a l f - t i m e i s u n c e r t a i n

because o f t h e low c o u n t i n g r a t e s . The 16-min h a l f - t i m e f o r

methyl i o d i d e i s c o n s i s t e n t w i t h a bed e f f i c i e n c y o f 8 8 % . The

c h a r c o a l beds were m o i s t u r e e q u i l i b r a t e d b e f o r e u s e , and t h i s

i s known t o r educe t h e bed e f f i c i e n c y .

A f t e r t h e t e s t , t h e l o o p i n v e n t o r y was de te rmined and

t h e amount o f i o d i n e and cesium on t h e v a r i o u s components i s

g i v e n i n T a b l e 2 . 3 f o r Runs A-16 and A-17. I t i s obvious

t h a t much o f t h e i o d i n e i n Run A-16 was p a r t i c u l a t e (p robab ly

Cs I ) , a s can be s e e n from t h e a i r b o r n e forms i n F i g u r e 2 . 1

and from t h e l a r g e amount on t h e d e m i s t e r and f i l t e r components.

T h i s i s t h o u g h t t o have been induced by t h e l a r g e amount o f

cesium r e l e a s e d s i m u l t a n e o u s l y w i t h t h e i o d i n e . The amount o f

i o d i n e r e c o v e r e d from t h e loop a f t e r Run A-16 was h i g h e r t h a n

TABLE 2 . 3 .

HEX Condensa te

Demis t e r

P r e f i l t e r

HEPA

F i r s t Charcoa l Bed

1 s t h a l f

2nd h a l f

Second Charcoa l Bed

1 s t h a l f

2nd h a l f

T h i r d Charcoa l Bed

1st h a l f

2nd h a l f

T o t a l , g

C a l c u l a t e d , g

P o s t Run Loop Inventory , ( p e r c e n t of t o t a l m a t e r i a l ecovered on LOOP Components) ( a f

Run A-16 Run A-17 C s I C s I

11 9 . 2 4 . 8 4 . 0

a . Based o n t h e t o t a l m a t e r i a l r e c o v e r e d from t h e l o o p .

b . Based on Cmaz and 1 2 0 min u n i f o r m r e l e a s e .

c . Based on Cmar and 6 0 min u n i f o r m r e l e a s e .

d . Based o n c o n c e n t r a t i o n a t 30 min and r emova l r a t e a t 30 t o 6 0 m in .

e x p e c t e d from t h e c a l c u l a t e d r e l e a s e . T h i s may have been

caused by t h e d e s o r p t i o n o f i o d i n e from t h e s u r f a c e s o f t h e

con ta inmen t v e s s e l w i t h s u b s e q u e n t r e c o v e r y by t h e l o o p . Desorp-

t i o n c o u l d be e x p e c t e d a s a r e s u l t o f t h e d e c r e a s i n g i o d i n e

c o n c e n t r a t i o n and p o s s i b l y a s a r e s u l t o f d e c r e a s i n g h u m i d i t y . (2)

A l t e r n a t i v e l y , t h e r e l e a s e t o t h e con ta inmen t v e s s e l may n o t

have been l i n e a r , and t h e e s t i m a t i o n o f t h e t o t a l q u a n t i t y

r e l e a s e d t o t h e main room may be low.

The e f f i c i e n c y o f t h e v a r i o u s loop components was measured

s e v e r a l t imes d u r i n g t h e run by sampl ing from t h e l o o p w i t h

Maypacks. Tab le 2 .4 summarizes t h e d e c o n t a m i n a t i o n f a c t o r s

o b t a i n e d by t h e s e v e r a l measurements . The t a b l e shows t h a t

t h e l o o p per formance remained e s s e n t i a l l y c o n s t a n t d u r i n g t h e

f i r s t two h r .

Run A-17 was s i m i l a r t o A-15, r e p o r t e d p r e v i o u s l y , ( 3 ) 3 e x c e p t t h a t t h e loop f low was m a i n t a i n e d a t 1820 f t /min

3 r a t h e r t h a n 1000 f t /min. Allowing f o r s t eam condensed by

t h e H E X , t h e f low was 5 . 3 main room volumes p e r h r . The

s i m u l a n t s were r e l e a s e d i n t o t h e s t e a m - a i r a tmosphere . Sam-

p l e s were t a k e n t o e s t a b l i s h t h e removal r e s u l t i n g from

n a t u r a l p r o c e s s e s , and t h e n t h e loop f low was s t a r t e d . The

c h a r c o a l beds had been s a t u r a t e d w i t h m o i s t u r e p r i o r t o t h e

a e r o s o l r e l e a s e . F i g u r e s 2 . 3 and 2 .4 g i v e t h e main room con-

c e n t r a t i o n s . Tab le 2 .5 p r e s e n t s t h e obse rved h a l f - t i m e s .

Reasonable agreement w i t h t h e loop removal and t h a t c a l -

c u l a t e d on t h e b a s i s o f a w e l l mixed main room volume was

o b t a i n e d , w i t h t h e obse rved removal b e i n g s l i g h t l y s l o w e r

than p r e d i c t e d , e x c e p t f o r e l e m e n t a l i o d i n e , which was

removed more r a p i d l y from t h e gas s p a c e . The methyl i o d i d e

removal r a t e i n d i c a t e d a c h a r c o a l bed e f f i c i e n c y o f 7 2 % . P r e - 3 v i o u s CSE t e s t s a t 1000 f t /min w i t h m o i s t u r e s a t u r a t e d c h a r -

c o a l beds have g i v e n 7 7 t o 88% e f f i c i e n c i e s . The i n c r e a s e d

f low th rough t h e bed d i d n o t reduce t h e e f f i c i e n c y q u i t e a s

much as a n t i c i p a t e d from t h e commonly a c c e p t a b l e e x p r e s s i o n .

f = exp ( -kd /v ) (2)

which r e l a t e s t h e f r a c t i o n n o t removed, f , bed d e p t h , d , and

gas v e l o c i t y , v . E s t i m a t e s o f t h e decon tamina t ion f a c t o r s

f o r t h e f i l t e r l o o p components a r e g i v e n i n Table 2.6 a t

s e v e r a l run t i m e s .

M A I N R O O M ( A V E R A G E O F 8 L O C A T I O N )

O T O T A L

o F I L T E R ( P A R T I C L E S )

O S C R E E N S ( E L E M E N T A L )

A A C P A P E R

v C H A R C O A L B E D I C H 3 1 )

4 8 p s i a . 2 4 7 ' ~ L O O P F L O W 1850 C F M

- \

K- - \---

- --- \ \ --- -*

- R E L E A S E O V E R

- N O T E C H A N G E I N

F A N O N T I M E S C A L E

v I I !,/ I I I PV

S T E A M O F F

0 100 200 300 9 0 0 1 5 0 0 2 1 0 0 2 7 0 0

R U N T I M E , M I N U T E S

FIGURE 2 . 3 . Iod ine Concentra t ion i n The Main Gas Space - CSE Run A 1 7

FIGURE 2 . 4 . Cesium and Uranium C o n c e n t r a t i o n i n The Main Gas Space - CSE Run A 1 7

AVERAGE OF 8 * 10

0 C E S I U M

U R A N I U M

C E S I U M t1,2:7.7 M I N

0

-

- n

[I v -

- -

1 0 - 1

-

-RELEASE OVER

FAN ON

-

I I .:,/IME sCA:E

STEAM OFF

10 -2 . I I Y 0 100 200 300 900 1500 2100 2700

RUN T IME, M INUTES

TABLE 2 .5 . Aerosol Behavior i n CSE Run A-17 (a)

Concent ra t ion Half Time, min Na tu ra l Natura l Loop Only,

Form Only P lus Loop Ca lcu l a t ed

Elemental I 2 1 3 3 . 8 5 . 4

Methyl Iod ide - 11 11

Cesium 33 7 . 7 10

P a r t i c u l a t e Iod ine 25

Uranium

Average

a . E x p e c t e d t f o r l o o p = ' a ' g 3 = 7 . 9 1 / 2 v

To summarize, t h e a e r o s o l behav ior du r ing both Runs A-16

and A-17 was c o n s i s t e n t wi th a c o n s t a n t f r a c t i o n removed from a

well-mixed volume f o r about 2 h r a f t e r r e l e a s e , a t which time

the removal r a t e s slowed. The i n i t i a l removal was s l i g h t l y

s lower than would be p r e d i c t e d by X = loop flow/main room

volume, excep t f o r e lementa l i od ine which was removed more

r a p i d l y than expected i n Run A - 1 7 . This may be exp la ined by

inc rea sed n a t u r a l removal r a t e s caused by the loop flow

a s s i s t i n g t he n a t u r a l convect ion v e l o c i t i e s w i t h i n t he con-

ta inment v e s s e l .

TABLE 2.6 . Loop Decontamination Factors , CSE Run A-17

D e c o n t a m i n a t i o n actor'^) t = 35 min t = 60 min t = 80 min

Cs I E L a - CH I C s -- I -3- ---- --- 1 CH,L HEX 1 . 2 1 . 3 - 1 . 2 1 . 6 - 1 . 2 1 . 4 -

Demis t e r 6 . 2 1 . 3 - 3 . 7 1.1 - 2 . 4 2 . 5 -

HEPA 4 4 1 . 6 - 40 8 5 > 1 3

F i r s t C h a r c o a l Bed 470 1 . 7 1 . 7 - 1 . 7

Second C h a r c o a l Bed > 7

T h i r d C h a r c o a l Bed

o v e r a l l 27 ,000 > a 0 0 0 12 1900 > I 2 0 10 520 > I 8 0 7 . 5

1 D F , DF = c o n c e n t r a t i o n i n / c o n c e n t r a t i o n o u t . a. E f f i c i e n c y = 1 - -. b . Loop f low s t a r t e d a t 30 min .

c . B e s t e s t i m a t e o f t o t a l D F

I o d i n e Gas- L iau id P a r t i t i o n - L . F . Coleman

Gas -aqueous d i s t r i b u t i o n d a t a f o r i o d i n e a r e n e c e s s a r y t o

m a t h e m a t i c a l l y model t h e n e t b e n e f i t o f e n g i n e e r e d s a f e g u a r d s

sys t ems such a s aqueous s p r a y s . The d i s t r i b u t i o n v a l u e i s r e l e -

v a n t i n two ways, (1) t h e magni tude o f t h e d i s t r i b u t i o n v a l u e

w i l l l i m i t t h e r a t e o f removal o f i o d i n e from t h e gas p h a s e

when drop s a t u r a t i o n can e x i s t , i . e .

where Cg

= gas p h a s e c o n c e n t r a t i o n

F = s p r a y f low r a t e

V = gas volume

t = t ime

H e f f = i n s t a n t a n e o u s d i s t r i b u t i o n c o e f f i c i e n t ( n e g l e c t i n g s low chemica l r e a c t i o n s )

and (2) t h e f i n a l d i s t r i b u t i o n a t l o n g e r t imes ( h o u r s , d a y s ,

weeks) where chemica l r e a c t i o n s have t ended toward e q u i l i b r i u m :

where = c o n c e n t r a t i o n i n l i q u i d phase

H = d i s t r i b u t i o n c o e f f i c i e n t a t e q u i l i b r i u m e q

E q u a t i o n s (3) and (4) r e p r e s e n t s i m p l i f i e d t ime- bound ing con-

d i t i o n s ; more p r e c i s e d e s c r i p t i o n s f o r o v e r a l l i o d i n e removal

would i n c l u d e g a s , s u r f a c e and s o l u t i o n p h a s e r a t e and e q u i l i b -

r ium d a t a f o r a l l i o d i n e forms p r e s e n t i n t h e c o n t a i n m e n t

env i ronment . Nine e x p e r i m e n t s were conduc ted t o e v a l u a t e t h e g a s - l i q u i d

d i s t r i b u t i o n o f i o d i n e i n aqueous -base b o r a t e s y s tems. The

e x p e r i m e n t s were per formed i n a 3 - f t - d i a m e t e r , 9 0 5 - l i t e r - v o l u m e

s t a i n l e s s s t e e l v e s s e l w i t h t h e aqueous phase d i s t r i b u t e d on

t h e v e s s e l w a l l t o m a i n t a i n i s o t h e r m a l c o n d i t i o n s and a w e t t e d

v e s s e l w a l l . A more d e t a i l e d d i s c u s s i o n o f a p p a r a t u s and p r o -

cedures was p r e s e n t e d i n a p r e v i o u s r e p o r t . (3)

Tab le 2 . 7 l i s t s t h e e x p e r i m e n t a l c o n d i t i o n s f o r t h e t e s t .

program. R e s u l t s from two t e s t s , E-1 and E - 2 , were p r e v i o u s l y

r e p o r t e d (3) b u t a r e i n c l u d e d h e r e t o g i v e a comple te s e t o f

r e s u l t s .

Exper imen ta l P rocedure

The 9 0 5 - l i t e r v e s s e l was b r o u g h t t o i s o t h e r m a l , i s o b a r i c

c o n d i t i o n s w i t h t h e c o n t a i n e d 100 l i t e r , pH 9 . 5 , 3000-ppm

boron , b a s e - b o r a t e aqueous phase . Thermal ly r e g u l a t e d s t eam

a d d i t i o n t o i n t e r n a l h e a t t r a n s f e r c o i l s r e p l e n i s h e d h e a t

l o s s e s .

The aqueous p h a s e was pumped from t h e bot tom o f t h e aque-

ous p o o l t o t h e t o p p o r t i o n o f t h e c y l i n . d r i c a 1 v e s s e l w a l l s

and d i s t r i b u t e d by a c i r c u m f e r e n t i a l , p e r f o r a t e d r i n g .

S t a b l e e l e m e n t a l i o d i n e t r a c e d w i t h 13'1 was i n t r o d u c e d

i n t o t h e sys tem by e i t h e r of t h r e e methods: (1) aqueous phase

i o d i n e a d d i t i o n t o t h e l i q u i d p o o l , ( 2 ) s o l i d i o d i n e v o l a t i l i z e d

t o t h e gas p h a s e , o r (3 ) s o l i d i o d i n e i n ampoules c r u s h e d w i t h i n

t h e l i q u i d r e c i r c u l a t i n g l o o p .

Gas phase samples were c o l l e c t e d d i r e c t l y from c o n t a i n -

ment by i n s e r t i o n and wi thdrawal o f Maypack s a m p l e r s . ( 4 ) The

volume o f gas sampled was 10 l i t e r s (STP). These volumes were

c o r r e c t e d t o y i e l d t h e a c t u a l volumes f o r t h e p a r t i c u l a r con-

t a i n m e n t c o n d i t i o n s . F i l t e r e d a i r was added t o t h e sys tem t o r e p l e n i s h l o s s e s

i n c u r r e d by sampl ing .

F i f t y m l volume l i q u i d samples were removed from t h e

l i q u i d r e c i r c u l a t i o n l o o p a t t ime i n t e r v a l s e q u i v a l e n t t o gas

sampl ing t i m e s . T h i s volume was s m a l l r e l a t i v e t o t h e 100 l i t e r

p o o l volume and d i d n o t d i s r u p t t h e g a s - l i q u i d volume r a t i o .

TABLE 2.7. Iodine Partition Experimental Conditions (a)

Average Iodine

Concentration Pressure In Aqueous

Expriment Temp, O C psia Phase, mg/R Release Yethod

E 1 8 0 24 0.011 gas phase, vaporized elemental iodine

E 2 8 0 2 4 0.0097 liquid phase, aqueous solution of iodine added

E 3 120 4 9 0.010 liquid phase, aqueous solution of iodine added

N E 4 120 4 9 0.52 liquid phase, aqueous solution of iodine added I-' P E 5 120 4 9 3.55 liquid phase, aqueous solution of iodine added

E 6 12 0 4 9 0.28 gas phase, vaporized elemental iodine

E 7 120 4 9 0.66 gas phase, vaporized elemental iodine

E 8 120 4 9 28 liquid phase, crystalline iodine added to

aqueous system

E 11 120 4 9 25 liquid phase, crystalline iodine added to

aqueous system

a . A l l e x p e r i m e n t s u s e d pH 9 . 4 t o pH 9 . 5 b a s e b o r a t e ; 3000 ppm b o r o n a s b o r i c a c i d p l u s flaOH. Gas and l i q u i d vo lumes were 8 0 6 and 200 4 P e s p e c t i v e l y . W a l l f i l m l i q u i d f l ow r a t e 1 5 k / m i n .

I o d i n e c o n c e n t r a t i o n s i n gas and l i q u i d samples were

o b t a i n e d by gamma energy a n a l y t i c a l t e c h n i q u e s .

R e s u l t s and D i s c u s s i o n

F i g u r e 2 . 5 i l l u s t r a t e s how t h e b a s i c a n a l y t i c a l d a t a were

h a n d l e d . Gas phase c o n c e n t r a t i o n v e r s u s t ime c u r v e s were

o b t a i n e d f o r t h e i n d i v i d u a l components o f t h e gas sample r

a p p a r a t u s r a t h e r t h a n t o t a l i o d i n e t o d e t e c t any v a r i a n c e i n

i o d i n e b e h a v i o r . I n o r g a n i c i o d i n e t o t a l s exc luded t h e g ranu-

l a r c h a r c o a l bed component o f t h e Maypack which i s i n d i c a t i v e

o f methyl i o d i n e c o n c e n t r a t i o n . Methyl i o d i d e c o n c e n t r a t i o n

was i n c i d e n t a l t o t o t a l gas phase i o d i n e a t e a r l y t imes e x c e p t

i n Exper iment E - 1 where d i f f i c u l t i e s were e n c o u n t e r e d d u r i n g

t h e i o d i n e r e l e a s e t o con ta inment . T o t a l i n o r g a n i c i o d i n e

v a l u e s were e x t r a p o l a t e d t o t ime ze ro i n t e r c e p t t o o b t a i n

i n i t i a l d i s t r i b u t i o n v a l u e s .

The i n i t i a l d i s t r i b u t i o n v a l u e o b t a i n e d by t h i s t e c h n i q u e

would r e l a t e t o t h e p r e d i c t i v e c a s e f o r i n i t i a l s p r a y washout

r a t e s where drop f a l l r e s i d e n c e t imes a r e on t h e o r d e r o f

seconds . I f H e f f were i n f i n i t e , t h e maximum removal r a t e would

be gas phase mass t r a n s f e r l i m i t e d . For s m a l l v a l u e s o f W e f f ,

where drop s a t u r a t i o n i s p o s s i b l e , t h e r a t e o f removal from

t h e gas phase i s l i m i t e d by t h e v a l u e of H e f f .

An a p p a r e n t f i r s t - o r d e r s o l u t i o n phase r e a c t i o n w i t h a

30 t o 40 min h a l f l i f e was obse rved i n a l l t h e 120 " C e x p e r i -

ments . Th i s i s i l l u s t r a t e d i n F i g u r e 2 . 5 , where e l e m e n t a l

i o d i n e was i n j e c t e d d i r e c t l y i n t o t h e aqueous phase . For a

gas phase r e l e a s e , an a d d i t i o n a l g a s phase mass t r a n s f e r

l i m i t e d r a t e w i t h a much s h o r t e r h a l f l i f e ( 5 t o 8 ) minutes

would a l s o have been obse rved . A f i r s t - o r d e r s o l u t i o n phase

r e a c t i o n h a v i n g an approximate r a t e c o n s t a n t o f 3 x s e c - 1

such as t h e e a r l y removal cu rve o f F i g u r e 2 .5 would n o t con-

t r i b u t e markedly t o t h e t o t a l i n i t i a l removal o f i o d i n e by

- - - - q GLASS FILTERS

- - - - - 0 S l LVER SCREENS -

\ I N

V A CHARCOAL CHARCOAL PAPER BED - -

- 0 TOTAL INORGAN IC, Z O + O + A -

---llH +- +---- +----- +- - - - - - - - - - - - \\ + - - -

t1,2'500 M l N AVG. LIQUID CONC. 1 . 0 ~ 1 0 - ~ m g / ~ 1 - - - - -

- A oP A A & 0 0 - - - A 1 2 0 ~ ~ -

A 0 0

0 0 B

118 '~

8 - - - - A A

soOc A - - O 0 -

A - - %

v

El 30°c 0

- v n V 0 2 3 ' ~

El AA - - - El - - V v8

q ca v - - q

-

1-

TIME, MINUTES

FIGURE 2.5 . Iod ine Behavior Versus T i m e - Experiment E 3

s p r a y s s i n c e s p r a y d rop r e s i d e n c e t i m e s would be on t h e o r d e r

o f s e c o n d s . However, r e a c t i o n r a t e s o f t h i s magnitude would

c o n t r i b u t e t o t h e d e c o n t a m i n a t i o n which c o u l d b e e f f e c t e d by

s p r a y s o v e r an e x t e n d e d p e r i o d o f t i m e . I n t h e o b s e r v e d

c a s e s , t h i s i n t e r m e d i a t e removal r a t e p r o c e s s l a s t e d f o r a b o u t

150 min, a f t e r which a much s l o w e r removal r a t e p r o c e s s was

i n v o l v e d , w i t h a removal r a t e c o n s t a n t on t h e o r d e r o f - 1 s e c .

A t t h e l o n g e r t i m e p e r i o d s i n F i g u r e 2 . 5 , i o d i n e d i s -

t r i b u t i o n on t h e Maypack s a m p l e r components changed t o t h e

p o i n t where an a p p r e c i a b l e f r a c t i o n o f t h e gasborne i o d i n e

mass appea red on t h e c h a r c o a l p a p e r component. A t e a r l y t i m e s ,

t h e b u l k of t h e i o d i n e was p r e s e n t on t h e s i l v e r components .

S i n c e t h i s b e h a v i o r i s o b s e r v e d f o r e x p e r i m e n t s a t d i f f e r e n t

i o d i n e mass l e v e l s , i t does n o t a p p e a r t o b e a sampl ing problem

(changes i n i o d i n e d i s t r i b u t i o n caused by mass l o a d i n g o f t h e

Maypack components) b u t r a t h e r a s s o c i a t e d w i t h d i f f e r e n t chemi-

c a l forms o f i o d i n e . For th.e c o n d i t i o n s i n v e s t i g a t e d , t h e

c o n c e n t r a t i o n o f t h e s e s e c o n d a r y i o d i n e s p e c i e s would n o t b e

i n f l u e n t i a l i n t h e o v e r a l l n u c l e a r s a f e t y problem.

Ano the r e f f e c t which i s shown i n F i g u r e 2 .5 i s t h e

i n c r e a s e i n t h e p a r t i t i o n c o e f f i c i e n t a t l o n g e r t i m e s w i t h a

d e c r e a s e i n t e m p e r a t u r s . I n a d d i t i o n , t h e p a r t i t i o n v a l u e

n e a r l y r e t u r n e d t o i t s p r e v i o u s v a l u e when t h e t e m p e r a t u r e was

a g a i n r a i s e d .

T a b l e 2 .8 l i s t s some o f t h e d a t a p e r t i n e n t t o t h e n i n e

e x p e r i m e n t s pe r fo rmed . E x a c t d u p l i c a t i o n o f r e s u l t s was n o t

p o s s i b l e , and t h e v a r i a t i o n i n t h e i n i t i a l p a r t i t i o n v a l u e was

a s g r e a t between d u p l i c a t e e x p e r i m e n t s a s i t was between

r e l e a s e t e c h n i q u e s (gas o r l i q u i d p h a s e i n j e c t i o n o f i o d i n e ) .

T h e o r e t i c a l v a l u e s f o r t h e e q u i l i b r i u m p a r t i t i o n v a l u e s ( 5 )

Ln I 0 rl

v

TI' I 0 d X TI'

0 0 0 . 0 CV Ln

0 0 0 . 0 0 TJ'

0 0 0

4

d N

d I 0 rl X N

Ln

I I

TI' I 0 r i X m

I I

0 0 0 . M 03

0 0 Ln . Ln

d I 0 d X In

Ln

6 5 would be abou t 3 x l o 9 , 6 x 10 and 1 x 10 a t t h e t h r e e i o d i n e

c o n c e n t r a t i o n ranges i n v e s t i g a t e d .

The v a l u e o f t h e z e r o - t i m e p a r t i t i o n c o e f f i c i e n t , H e f f ,

i s p l o t t e d a s a f u n c t i o n o f i o d i n e c o n c e n t r a t i o n i n t h e

l i q u i d phase i n F i g u r e 2 .6 . C o n t r a r y t o t h e o r y , t h e c o e f -

f i c i e n t i n c r e a s e d w i t h i n c r e a s i n g l i q u i d c o n c e n t r a t i o n . I n

a l l c a s e s , however, t h e v a l u e s were s u f f i c i e n t l y h i g h (>5000)

t o c a u s e l i q u i d phase t r a n s f e r r e s i s t a n c e i n f a l l i n g d rops t o

be n e g l i b l e and t o a l l o w r a p i d removal o f i n o r g a n i c i o d i n e

from con ta inment gas s p a c e s by b a s e - b o r a t e s p r a y s . Cont inued

removal , though a t a s l o w e r r a t e , would o c c u r because o f t h e

chemical r e a c t i o n s w i t h i n t h e l i q u i d . A f t e r s e v e r a l hours o f

r e c i r c u l a t i o n , t h e c o n c e n t r a t i o n o f i n o r g a n i c i o d i n e i n t h e

gas s p a c e would be reduced by a b o u t a f a c t o r o f 10 from t h e

v a l u e o b t a i n e d b y t h e i n i t i a l f r e s h s p r a y p e r i o d .

Coo lan t Blowdown S t u d i e s - A 1 1 emann , Townsend,

A. S . Neu l s , M. E . Witherspoon and A . J . McElf resh

3 A r e a c t o r s i m u l a t o r v e s s e l w i t h a volumeof 150 f t . d e s i g n e d f o r o p e r a t i o n a t 600 O F and 2750 p s i g i s b e i n g used

i n exper imen t s t o s t u d y l o s s - o f - c o o l a n t a c c i d e n t s . The ob j e c -

t i v e s of t h e exper imen t s i n c l u d e t e s t i n g t h e v a l i d i t y o f

ma themat ica l models used f o r p r e d i c t i n g t h e consequences of a

l o s s - o f - c o o l a n t r e a c t o r a c c i d e n t . The v e s s e l i s mounted i n a

s t e e 1 framework w i t h t h e d i s c h a r g e n o z z l e d i r e c t e d h o r i z o n t a l l y .

The blowdown a p p a r a t u s i s i n s t r u m e n t e d t o measure i n t e r n a l p r e s -

s u r e s , t e m p e r a t u r e s , l i q u i d l e v e l , v o i d f r a c t i o n o f t h e f l u i d

i n t h e e x i t d u c t , mass o f f l u i d r emain ing i n t h e v e s s e l ,

t h r u s t r e a c t i o n f o r c e s , s h e l l s t r e s s e s , and f o r c e s on r e a c t o r

dummy c o r e s t r u c t u r e s ( F i g u r e 2.7) . During t h i s r e p o r t i n g p e r i o d t h e mid-nozz le (Nozzle B )

s e r i e s o f blowdowns was comple ted and i n s t a l l a t i o n was begun

A E l l

A E8

TOTAL IODINE CONCENTRATION I N L IQUID, mglL

FIGURE 2 . 6 . I od ine P a r t i t i o n Value V e r s u s Concent ra t ion

T I M E D O M A I N R E F L E C T O M E T E R

- 6

E

D E N S I T O M E T E R

P R E S S U R E GAGE I E W PORT WINDOW

T H E R M O C O U P L E

BLOWDOWN NO

N O T E : L E T T E R S A T H R O U G H Z I N D I C A T E V E S S E L

a N

N O Z Z L E S -

FIGURE 2.7. CSE Blowdown T e s t Vessel

o f a dummy c o r e which i s d e s i g n e d t o model t h e i n t e r n a l geome-

t r y o f a p r e s s u r i z e d w a t e r r e a c t o r .

Void F r a c t i o n - Q u a l i t y Measurements

The v o i d f r a c t i o n i n t h e o u t l e t p i p e h a s been o b s e r v e d t o

i n c r e a s e w i t h n o z z l e s i z e and t h e a s s o c i a t e d i n c r e a s e i n q u a l i t y

i s t h e p r o b a b l e c a u s e o f t h e d e c r e a s e i n mass v e l c i t y w i t h

o r i f i c e s i z e . T h i s d e c r e a s e i n mass v e l o c i t y a p p e a r s t o c o r -

r e l a t e w i t h t h e c a v i t a t i o n number.

The r e d u c t i o n i n t h e mass v e l o c i t y w i t h n o z z l e s i z e ( 6 ) h a s

r e q u i r e d a c ~ e f f i c i e n t ( ~ ) t o c o r r e c t t h e o r e t i c a l f lows t o a c t u a l

f l o w s . The i n c r e a s e i n q u a l i t y i s n o t s u f f i c i e n t l y e x p l a i n e d

by c o n s i d e r a t i o n s o f bubb le r i s e and s e p a r a t i o n w i t h i n t h e

v e s s e l . T y p i c a l codes which c o n s i d e r bubb le r i s e phenomena

[FLASH, ( 8 ) BURP, RELAPSE ( l o ) ] s t i l l r e q u i r e a c o e f f i c i e n t t o

g i v e a r e a s o n a b l e p r e d i c t i o n f o r t h i s s p e c i a l c a s e .

The t e s t s e r i e s j u s t comple ted i n c l u d e d two r u n s i n which

t h e v o i d f r a c t i o n i n t h e t e s t s e c t i o n ( F i g u r e s 2.7 and 2 . 8 ) was

measured w i t h a n e u t r o n d e n s i t o m e t e r . I n t h i s d e v i c e , n e u t r o n

modera t ion i s u s e d a s a measure o f t h e amount o f l i q u i d i n t h e

p i p e . The n e u t r o n d e t e c t o r d a t a were c o n v e r t e d t o q u a l i t y

v a l u e s by t h e code DENPRfl deve loped f o r t h e p u r p o s e . Example

o f t h e s e q u a l i t y d a t a a r e shown i n ( F i g u r e s 2 . 9 and 2 . 1 0 ) . The

d a t a a r e s c a t t e r e d b e c a u s e t h e d i g i t i z e d r e c o r d i n g t e c h n i q u e

t r a n s m i t s o c c a s i o n a l v a l u e s t h a t r e p r e s e n t p h y s i c a l l y u n r e a l i s -

t i c s i t u a t i o n s which i n t r o d u c e i n s t a b i l i t y i n t o t h e d e t e c t o r

o u t p u t - t o - q u a l i t y c o n v e r s i o n e q u a t i o n s . However, t h e o v e r a l l

v a l u e s and t r e n d s a r e c b v i c u s . The low q u a l i t y p o r t i o n of t h e

r u n e a r l y i n t h e blowdown i s f o l l o w e d by a r a p i d t r a n s i t i o n t o

h i g h q u a l i t y f l o w . The low q u a l i t y r e g i o n i s c h a r a c t e r i s t i c of

t h e s a t u r a t e d f low regime of blowdown. The v a l u e of t h e q u a l i t y

d u r i n g t h e s a t u r a t e d f l o w regime i s a b o u t 1 . 5 x l o - ' f o r a

T I M E , SECONDS

r

-

I

I

-

-

FIGURE 2.9. Q u a l i t y i n Test Sec t ion

-

BLOWDOWN 8 - 8 2 S T A R T CONDI TI ONS 1100 p s i a - 5 3 0 ; ~

6 " ( N O M ) O R I F I C E , A R E A - 0 . 1 4 6 7 F T

I

BLOWDOWN B-85 START CONDITIONS 998 p s i a - 487'~ 2"(NOM) ORIFICE, AREA-0.0155 F T ~

TIME - SECONDS

FIGURE 2.10. Quality in Test Section

6 i n . (nominal ) b r e a k and 2 x 1 0 - Q f o a 2 - i n . (nominal )

d i a m e t e r b r e a k . Al though t h e blowdowns were s t a r t e d a t 530

and 487 OF r e s p e c t i v e l y , t h e p r e d i c t e d (on t h e b a s i s o f i s e n -

t r o p i c expans ion) v a l u e s o f q u a l i t y i n t h e p i p e c o n t e n t s a r e

1 . 7 x 1 0 ' ~ and 1 . 4 x l o - ' r e s p e c t i v e l y . Hence, t h e s m a l l b r e a k

had a much lower q u a l i t y f l o w t h a n e x p e c t e d , and i t was much l o w e r

t h a n f o r t h e l a r g e r o r i f i c e blowdown t e s t . E a r l i e r d a t a t a k e n w i t h

t h e n e u t r o n d e n s i t o m e t e r had a l s o shown t h a t t h e mass v e l o c i t y

d e c r e a s e was a s s o c i a t e d w i t h o r i f i c e s i z e d e c r e a s e . ( 6 ) These

d a t a a l s o showed a mass v e l o c i t y d e c r e a s e w i t h q u a l i t y , (11) a s

p r e d i c t e d by most two-phase c r i t i c a l f low t h e o r i e s .

The e x p e r i m e n t s o f L i e n h a r d and S tephenson ( I 2 ) show t h e

same e f f e c t o f s i z e a s do t h e s e e x p e r i m e n t s ; t h a t i s , t h e c a v i -

t a t i o n number i s p r o p o r t i o n a l t o a r e a t o t h e - 0 . 3 3 power. And

s i n c e t h e c a v i t a t i o n number i s

i t can b e conc luded t h a t G c r i t s h o u l d be p r o p o r t i o n a l t o ( a r e a

o f o r i f i c e ) - 0.166

T h i s r e s u l t i s c l o s e t o what has been found by d i r e c t

e x p e r i m e n t i n p r e v i o u s work a t CSE and o t h e r s i t e s . (6 )

The i m p l i c a t i o n i s t h a t t h e l a r g e r b r e a k a l l o w s h i g h e r

f low r a t e s which g i v e s more t u r b u l e n c e and a lower c a v i t a t i o n

number; hence more b u b b l e n u c l e i i a r e t r i g g e r e d t o form b u b b l e s .

The l a r g e r number o f b u b b l e s g i v e s a h i g h e r q u a l i t y which

l i m i t s t h e mass v e l o c i t y t o a lower v a l u e t h a n w i t h s m a l l e r

b r e a k s .

Pho tographs t a k e n o f t h e f l u i d i n t h e t e s t s e c t i o n do n o t

c o n t r a d i c t t h i s t h e o r y . High s p e e d motion p i c t u r e s t a k e n

th rough t h e window o f t h e t e s t s e c t i o n ( F i g u r e 2 .8) u s i n g c r o s s

i l l u m i n a t i o n showed i n d i v i d u a l b u b b l e s moving a t m e a s u r a b l e 2 r a t e s ( F i g u r e 2.11) f o r s m a l l (0 .0155 f t ) b r e a k s .

MOI

I N D I V I

FIGURE 2.11. High Speed Film Strips

I n l a r g e r b r e a k s no i n d i v i d u a l b u b b l e s were s e e n i n s p i t e

o f a h i g h e r q u a l i t y r e g i s t e r e d by t h e n e u t r o n d e n s i t o m e t e r . 2 However, e a r l y i n t h e blowdown f o r a l a r g e o r i f i c e (0 .253 f t ) ,

a mi lky c l o u d was s e e n moving r a p i d l y w i t h t h e f l u i d . Hence,

i t a p p e a r s t h a t much s m a l l e r b u t more numerous b u b b l e s a r e

formed a s t h e b r e a k s i z e i s i n c r e a s e d . For s m a l l b r e a k s

f ewer b u b b l e s a r e formed which a r e a b l e t o grow t o v i s i b l e

s i z e i n t h e t ime a v a i l a b l e .

To a p p l y t h i s c o n c l u s i o n t o r e a c t o r p i p e f a i l u r e s would

assume t h a t f o r t h e l a r g e b r e a k s s u f f i c i e n t t u r b u l e n c e and

n u c l e a t i o n s i t e s e x i s t f o r t h e f low r a t e t o be l i m i t e d by

s t eam q u a l i t y . Smal l b r e a k s t o o , may a c t a s even s m a l l e r

e x i t s , g i v i n g lower mass l o s s r a t e s t h a n s t a t i c t e s t s ,

because i n i t i a l t u r b u l e n c e and n u c l e a t i o n s i t e s p r e s e n t i n

a f l o w i n g l o o p g i v e a h i g h e r q u a l i t y a t t h e b r e a k t h a n i n

t h e s t a g n a n t CSE t e s t s . However, s i n c e t h e q u a l i t y o f t h e

f low i s h i g h l y dependen t upon t h e t e m p e r a t u r e - p r e s s u r e a t

t h e o u t l e t r e l a t i v e t o t h a t i n o t h e r p a r t s o f t h e s y s t e m , t h e

d e t e r m i n a t i o n o f t h e f l u i d c o n d i t i o n s h o u l d b e pe r fo rmed

c a r e f u l l y . For example, emergency c o r e c o o l i n g w a t e r , i f

mixed w i t h a blowdown f l o w , c o u l d i n c r e a s e t h e f l o w r a t e

th rough the b r e a k by an amount g r e a t e r t h a n t h e c o o l a n t a d d i -

t i o n r a t e . Hence, t h e f l u i d l o s s would b e f a s t e r t h a n w i t h o u t

t h e emergency c o o l a n t a d d i t i o n .

References

I . J . G . Knudsen and R. K . H i l l i a r d . F i s s i o n P r o d u c t T r a n s - o r t by N a t u r a l P r o c e s s e s i n C o n t a i n m e n t V e s s e l s ,

!NWL-943, p . 35 . B a t t e Z l e - N o r t h w e s t , R i c h l a n d , W a s h i n g t o n , January 1969 .

2. R. E . Adams e t a l . " B e h a v i o r o f R a d i o a c t i v e A e r o s o l s , I f

N u c l e a r S a f e t y Program Annual P r o g r e s s R e p o r t f o r P e r i o d Ending December 31, 1969, ORNL 4511, p p . 45- 46 . Oak R idge N a t i o n a l L a b o r a t o r y , Oak R i d g e , T e n n e s s e e , March 1970 .

3 . N u c l e a r S a f e t y Q u a r t e r l y R e p o r t , November, December 1969, January 1970 , BNWL-2315-1, p p . 2 . 1 -2 .12 . B a t t e Z Z e - N o r t h w e s t , R i c h l a n d , W a s h i n g t o n , March 19 70 .

4 . J . D . McCormack. Maypack B e h a v i o r i n t h e C o n t a i n m e n t S y s t e m s Exper imen t- A . P e n e t r a t i n g A n a l y s i s , BNWL-1145. B a t t e Z l e - N o r t h w e s t , ~ i c h l a n d , W a s h i n g t o n , A u g u s t 1969 .

5 . A . E . J . E g g l e t o n . A T h e o r e t i c a l E x a m i n a t i o n o f I o d i n e - Wa te r P a r t i t i o n C o e f f i c i e n t s - , AERE-R-4889. A t o m i c Znergy R e s e a r c h E s t a b l i s h m e n t , H a r w e l l , Eng land , February 1967 .

6 . N u c l e a r S a f e t y Q u a r t e r l y R e p o r t , November, December 196 7 , January 1968, BNWL- 816. B a t t e Z Z e - N o r t h w e s t , ~ i c h l a n d , W a s h i n g t o n , S e p t e m b e r 1968 .

7 . N u c l e a r S a f e t y Q u a r t e r l y R e p o r t , A u g u s t t h r o u g h O c t o b e r 1968, BNWL-926. B a t t e Z l e - N o r t h w e s t , R i c h l a n d , W a s h i n g t o n , December 1968 .

H . Murvhu. and V . 0 . D a v i s . FLASH2:

M u l t i n o d e R e a c t o r P l a n t Dur ing Los s- o f- Coo Zan t , WAPD-TM-666. B e t t i s A t o m i c Power L a b o r a t o r u , P i t t s b u r q h , P e n n s v Z v a n i a , - - " - - A p r i l 1967 .

9 . N . P . W i l b u r n . v o i d F r a c t i o n P r o f i l e i n a N u c l e a r R e a c t o r V e s s e l Dur ing C o o l a n t Blowdown, BNWL-1295. B a t t e Z Z e - N o r t h w e s t , R i c h l a n d , W a s h i n g t o n , A p r i l 1970.

10 . K . V . Moore and W . H . R e t t i g . RELAP2: A D i g i t a l Program f o r R e a c t o r Blowdown and Power E x c u r s i o n A n a l y s i s , 100 -1 7263 . P h i l l i p s P e t r o l e u m Company, I d a h o F a l l s , I d a h o , March 1968 .

11 . N u c l e a r S a f e t y Q u a r t e r l y R e p o r t , May t h r o u g h June 1968 , BNWL-894. B a t t e Z l e - N o r t h w e s t , R i c h l a n d , W a s h i n g t o n , O c t o b e r 1968 .

12. J . H. Lienhard and J . M . S t ephenson . "Temperature and S c a l e E f f e c t s upon C a v i t a t i o n and F lash ing i n Free and Submerged Je ts ," J . B a s i c Eng., v o l . 8 8 , p p . 525-532, June 1966,

3 . PRESSURE B E A R I N G COMPONENT E V A L U A T I O N

AND M O N I T O R I N G S T U D I E S

CRACK D E T E C T I O N I N PRESSURE P I P I N G B Y A C O U S T I C E M I S S I O N - P . H . H u t t o n a n d J. B . V e t r a n o

I n t r o d u c t i o n

The term " a c o u s t i c emission" d e s c r i b e s a p h y s i c a l phenome-

non which can be u t i l i z e d t o d e t e c t f l aw format ion and growth

i n s o l i d m a t e r i a l s on a r e a l time b a s i s . Acous t ic emiss ion

c o n s i s t s o f e l a s t i c waves produced i n a s o l i d by energy

r e l e a s e d dur ing deformat ion and f r a c t u r e . These waves a r e

d e t e c t a b l e a t t he m a t e r i a l s u r f a c e some d i s t a n c e from t h e

s o u r c e , the reby p rov id ing the means t o d e t e c t t h e p resence of

f l aws remotely a t t he time they a r e formed o r grow.

The USAEC1s Div i s ion of Reactor Development and Tech-

nology has sponsored work a t Ba t t e l l e - Nor thwes t f a c i l i t i e s

s i n c e February, 1966 d i r e c t e d toward a p p l i c a t i o n of a c o u s t i c

emiss ion t o d e t e c t crack format ion and growth i n n u c l e a r

r e a c t o r p r e s s u r e boundar ies . A proven system t o perform t h i s

func t ion would be a s i g n i f i c a n t a d j u n c t t o n u c l e a r s a f e t y .

Rela ted work on t h e i n - p l a n t a p p l i c a t i o n phase has a l s o

been done a t t h e Idaho T e s t S i t e , Idaho F a l l s under DRDT

sponsorsh ip .

There i s a d i s t i n c t p o t e n t i a l f o r a p p l i c a t i o n of a c o u s t i c

emiss ion t o t h e i n t e g r i t y s u r v e i l l a n c e p o r t i o n of t h e LMFBR

program.

Reduction i n program scope and l i m i t e d funding has c u r -

t a i l e d program a c t i v i t y du r ing t h e p a s t q u a r t e r .

Discuss ion

Task 1 - Signa l Ana lys i s and C h a r a c t e r i z a t i o n

One of t he major needs i n a c o u s t i c emiss ion technology a t

t h i s time i s s u b s t a n t i a t e d c r i t e r i a f o r i n t e r p r e t a t i o n of

a c o u s t i c e m i s s i o n i n f o r m a t i o n . I n v e s t i g a t i o n o f a c o u s t i c emis-

s i o n from m e t a l f a t i g u e h a s c o n t r i b u t e d a c r i t e r i o n p o i n t and

h a s a l s o p r o v i d e d e v i d e n c e toward d e f i n i n g minimum d e t e c t a b l e

f l a w s i z e .

F a t i g u e t e s t s o f a v a r i e t y o f m e t a l s (2024-T3 aluminum,

Type 304 SS, h i g h - n i c k e l s t e e l , and m i l d c a r b o n s t e e l ) i n b o t h

h i g h and low c y c l e f a t i g u e h a s shown a c o n s i s t e n t a c o u s t i c

e m i s s i o n p r e c u r s o r t o t h e appea rance o f a v i s i b l e macroc rack .

Al though i t was s u s p e c t e d t h a t t h i s i n d i c a t i o n was g e n e r a t e d

by t h e i n i t i a l n u c l e a t i o n o f a macroc rack , c o n f i r m i n g i n f o r m a-

t i o n was needed. A s i m p l e n o t c h e d , c a n t i l e v e r beam f a t i g u e

specimen o f Type A-212-B ca rbon s t e e l was chosen f o r i n v e s t i -

g a t i o n o f t h e mechanism p r o d u c i n g t h e a c o u s t i c e m i s s i o n bench-

mark. T h i s was t e s t e d under h i g h c y c l e , t e n s i o n - t e n s i o n

f a t i g u e . F i g u r e 3 . 1 shows t h e specimen shape and l o a d c y c l e .

Also shown i n F i g u r e 3 . 1 i s t h e a c o u s t i c e m i s s i o n r e s p o n s e

c u r v e . The i n c r e a s i n g e m i s s i o n r e s p o n s e from 390,000 t o

630,000 c y c l e s i s a t t r i b u t e d t o m i c r o c r a c k i n g . The t e s t was

s h u t down o v e r n i g h t a t 570,000 c y c l e s and when t h e t e s t was

resumed, t h e e m i s s i o n s t a r t e d a t e s s e n t i a l l y t h e same l e v e l i t

had a t t a i n e d when t h e t e s t was s t o p p e d . A t 630,000 c y c l e s t h e

t e s t was a g a i n s t o p p e d and t h e spec imen was removed f o r examina-

t i o n . The s u r f a c e was p o l i s h e d and l i g h t l y e t c h e d t o i n s p e c t

m i c r o s c o p i c a l l y f o r any e v i d e n c e o f a macrocrack . S i n c e none

was f o u n d , i t was a g a i n i n s t a l l e d i n t h e t e s t f i x t u r e and

c y c l i n g resumed. The e m i s s i o n l e v e l , however, s t a r t e d much

lower t h a n t h e p r e v i o u s p o i n t . T h i s i s a t t r i b u t e d t o t h e

p o l i s h i n g which removed many m i c r o c r a c k s i t e s f rom t h e h i g h

s t r e s s a r e a . The a b r u p t i n c r e a s e i n a c o u s t i c e m i s s i o n which

p r e c e d e d t h e a p p e a r a n c e o f a v i s i b l e c r a c k o c c u r r e d a t

705,000 c y c l e s . The specimen was c y c l e d an a d d i t i o n a l

11 ,000 c y c l e s and t h e n removed f o r m e t a l l o g r a p h i c e x a m i n a t i o n .

M e t a l l o g r a p h i c i n s p e c t i o n r e v e a l e d an abundance o f mic ro -

c r a c k s on b o t h s i d e s o f t h e specimen n e a r t h e r o o t o f t h e n o t c h .

F i g u r e 3 . 2 a shows an example o f t h e s e a t a d e p t h o f %0.010 i n .

f rom t h e s u r f a c e . F u r t h e r i n v e s t i g a t i o n r e v e a l e d one macro-

c r a c k a t a d e p t h o f $0.125 i n . i n t o t h e spec imen. T h i s i s shown

i n F i g u r e s 3 . 2 b , 3 . 2 c , and 3 .2d . I t was % 0 . 0 0 2 - i n . deep and

e s t i m a t e d t o b e $0.030 i n . l o n g . No o t h e r macrocracks were

d i s c o v e r e d . These d a t a p r o v i d e s u b s t a n t i a t i o n f o r t h e c o n c l u -

s i o n t h a t t h e a b r u p t i n c r e a s e i n a c o u s t i c e m i s s i o n o b s e r v e d i n

f a t i g u e t e s t i n g i s a r e s u l t o f macrocrack n u c l e a t i o n . The d a t a

a l s o i n d i c a t e t h a t m i c r o c r a c k i n g , a t l e a s t i n c a r b o n s t e e l , i s

r e a d i l y d e t e c t a b l e by a c o u s t i c e m i s s i o n . T h i s c o n t r i b u t e s t o

d e f i n i t i o n o f minimum d e t e c t a b l e f l a w s i z e .

Task 2 - Sensor D e v e l o ~ m e n t

Task 3 - S i g n a l C o n d i t i o n i n g System

Task 4 - Data Ana lyze r and Readout System

Task 5 - A p p l i c a t i o n E n g i n e e r i n g

No s i g n i f i c a n t developments have been made on any o f t h e s e

t a s k s .

Task 6 - C o o p e r a t i v e Work w i t h Idaho N u c l e a r

L i a i s o n h a s been c o n t i n u e d w i t h Idaho Nuc lea r I n c . by

t e l e p h o n e and by a mee t ing a t R i c h l a n d on A p r i l 27 , w h e r e i n

program s t a t u s was r ev iewed .

G e n e r a l . P a p e r s on t h e s u b j e c t o f a c o u s t i c e m i s s i o n work

pe r fo rmed u n d e r t h i s program were p r e s e n t e d t o t h r e e t e c h n i c a l

group mee t ings t h i s p a s t q u a r t e r . These were :

A c o u s t i c Emiss ion - What I t I s and I t s A m l i c a t i o n t o

E v a l u a t e S t r u c t u r a l Soundness o f S o l i d s , BNWL-SA-2983,

P. H . H u t t o n , F e b r u a r y , 1970 p r e s e n t e d a t t h e C e n t r a l Ohio

S e c t i o n , ASNT, Februa ry 1 7 , 1970 a t Columbus, Oh io , and

t h e Chicago S e c t i o n , ASNT, February 1 9 , 1970 a t Ch icago ,

I l l i n o i s .

A c o u s t i c Emiss ion A p p l i e d t o D e t e r m i n a t i o n o f S t r u c t u r a l

I n t e g r i t y , BNWL-SA-3147, P. H . H u t t o n , March, 1970

p r e s e n t e d a t t h e 1 1 t h Open Meet ing o f t h e Mechanica l

F a i l u r e s P r e v e n t i o n Group, A p r i l 8 , 1970 a t W i l l i a m s b u r g ,

V i r g i n i a .

WORK P L A N N E D F O R N E X T Q U A R T E R

E f f o r t i n t e n d e d f o r t h e n e x t q u a r t e r i n c l u d e s :

S tudy o f wave p r o p a g a t i o n i n p i p e s .

* Complete s t u d y o f s i g n a l a t t e n u a t i o n v e r s u s f r e q u e n c y

i n r a n g e o f s i g n i f i c a n c e t o a c o u s t i c e m i s s i o n d e t e c t i o n .

Document f e a s i b i l i t y a s s e s s m e n t o f u s i n g wedge-mounted

l i t h i u m n i o b a t e s h e a r s e n s o r s f o r h i g h - t e m p e r a t u r e

a c o u s t i c e m i s s i o n d e t e c t i o n .

Apply a c o u s t i c e m i s s i o n m o n i t o r i n g t o f a t i g u e t e s t o f

2 4 i n . d i a m e t e r p i p e t e e a t f a c i l i t i e s o f Combustion

E n g i n e e r i n g , C h a t t a n o o g a , Tenn. t o c o n f i r m t h a t macrocrack

n u c l e a t i o n can be d e t e c t e d i n a l a r g e spec imen a s w e l l

a s i n l a b o r a t o r y spec imens .

E N V I R O N M E N T A L S T U D I E S

C A L C U L A T I O N O F T H E P O T E N T I A L E N V I R O N M E N T A L R A D I O L O G I C A L

C O N S E Q U E N C E S O F R E A C T O R A C C I D E N T S - M . M . Hendrickson

Early in 1967 the USAEC Division of Reactor Development

and Technology (DRDT) asked several companies and laboratories

to participate in a survey to compare methods of calculating

potential environmental radiological consequences of reactor

accidents. The survey consisted of a test problem for which

the participants were asked to submit calculations of thyroid

doses and whole body gamma doses from an airborne plume at

specified distances from a hypothetical reactor accident.

Large differences were observed among the answers for the

whole body gamma dose. As a result RDT authorized Battelle-

Northwest to undertake a program to develop improved methods

for estimating reactor accident consequences with the imme-

diate objective of developing an improved method for the whole

body gamma dose calculation.

Several of the participants used sophisticated computer

codes to perform the gamma dose calculation. Some of the codes

perform integrations over the dimensions of the plume and

others assume the cloud to be semi-infinite in size and of

uniform concentration. A detailed study of the methods used has revealed significant differences in all of the calcula-

tions. As a consequence of this study a general computer code

has been developed based on insight gained from the work of

the participants.

Although the main purpose of the code is the calculation

of the whole body gamma dose, calculations are also included

which permit accountability for the effects on the source term

of the events of a hypothetical reactor accident.

Hence the computer program is divided into three main subroutines:

Subroutine SOURCE - 1, determination of the important nuclides available for release

Subroutine BAFFLE - 2, calculation of the nuclide release rate to the atmosphere

Subroutine EXDOSE - 3, calculation of the external whole body gamma dose.

A description of each main portion of the code is given

below. A fourth subroutine to calculate the internal dose will

be added in the future.

The code is applicable to BWR's, PWR's, LMFBR's, experimen-

tal reactors, production reactors and some other nuclear

facilities.

SOURCE - Initial Nuclide Inventorv

The accurate calculation of radionuclide inventories is

complex and depends upon many variables. A very sophisticated

calculation would use a multigroup cross section model and

detailed description of core components, fuel and geometry.

Although such a calculation is not included in the present code,

a provision is available whereby inventories obtained from such

calculations may be specified (in curies) for specific isotopes.

With this provision the results of any type of inventory calcu-

lation may be used with the code. Radionuclides not produced

through normal fission and decay reactions (i.e. activation

products) may also be supplied as input.

The inventory of radiologically significant radionuclides

of most reactors can be described adequately by a simple one-

group cross section calculation. An adaptation of such a com-

puter code (RIBD - Radio Isotope Buildup and Decay) has been included in SOURCE. A multiple chain grid processor is used

which calculates nuclide concentrations resulting from two

fission sources (for example, 2 3 5 ~ and 239~u) with normal

down-chain decay by b e t a emiss ion and i somer ic t r a n s f e r s and

i n t e r c h a i n coupl ing r e s u l t i n g from n-gamma r e a c t i o n s .

The maximum number of members al lowed i n a c h a i n i s n i n e ,

and t h e maximum number of cha ins i s 96. The program c o n t a i n s

on t a p e two l i b r a r i e s of d a t a f o r 450 n u c l i d e s each ; one

l i b r a r y i s f o r f a s t r e a c t o r c a l c u l a t i o n s and t h e o t h e r i s f o r

thermal r e a c t o r c a l c u l a t i o n s . Data con ta ined i n t h e l i b r a r i e s

i nc lude p h y s i c a l h a l f - l i v e s , d i r e c t y i e l d s from 2 3 5 ~ f i s s i o n ,

d i r e c t y i e l d s from 2 3 9 ~ ~ f i s s i o n , neu t ron c a p t u r e c r o s s s e c -

t i o n s , average y decay e n e r g i e s pe r d i s i n t e g r a t i o n , average

B decay e n e r g i e s pe r d i s i n t e g r a t i o n , and branching r a t i o s t o

account f o r v a r i o u s modes of t r a n s i t i o n t o and from i somer ic

s t a t e s .

When t h e inven tory c a l c u l a t i o n i s u sed , t h e code s u p p l i e s

t h e f i s s i o n produc t inven tory a t t h e t ime of r e a c t o r shutdown

and a l s o f o r n ine decay t imes a f t e r shutdown ( s p e c i f i e d a s

i n p u t ) . The i nven to ry f o r shutdown o r any one of t h e n ine

decay t imes may be taken a s t h e i n i t i a l inven tory f o r t h e

c a l c u l a t i o n s t o fo l l ow . The d e s i r e d i n i t i a l inven tory

( s p e c i f i e d o r c a l c u l a t e d ) i s s t o r e d f o r use i n t h e containment

model c a l c u l a t i o n ( sub rou t ine BAFFLE).

The inpu t parameters f o r t h e i nven to ry c a l c u l a t i o n i nc lude

power l e v e l , o p e r a t i n g t ime, f l u x paramete r , 2 3 5 ~ c a p t u r e c r o s s

s e c t i o n , t h e i n i t i a l r a t i o of second t o f i r s t s p e c i e s f i s s i o n s ,

and n ine decay t imes .

BAFFLE - Containment Release C a l c u l a t i o n

The r a t e a t which n u c l i d e s a r e r e l e a s e d t o t h e atmosphere

i s c a l c u l a t e d by a g e n e r a l i z e d model f o r d e s c r i b i n g a e r o s o l

behavior and subsequent r e l e a s e u s ing f r a c t i o n a l s e t t l i n g

r a t e s and f r a c t i o n a l l e a k r a t e s . The model may be used t o

d e s c r i b e r e l e a s e from f u e l through a t h r e e - b a r r i e r (o r fewer)

system wi th f i l t r a t i o n and s e t t l i n g accounted f o r i n each

barrier. A diagram of the containment model is given in b

Figure 4.1. To reduce computing time the following simplifying

assumptions were made:

Instantaneous mixing in each vessel

Fallout and leak rates may be considered constant for a

short time interval

Isotopes becoming airborne from settled material come only

from the mass present at the beginning of the interval

Material released from the filters comes only from material

present on the filters at the beginning of the interval.

These assumptions make the system of differential equations

for nuclide concentrations in each compartment analytically

solvable and of the form Mass (t) = 2 ~ ~ e - ~ i ~ where the summation i

is over all previous nuclides in the mass chain and all previous

compartments. The Ai and Bi are functions of fractional leak

rates, removal rates, filter efficiencies, nuclide half-lives

and fractional decay yields. This portion of the code then

produces a series of nuclide release rates and time points to be

used in the subroutine EXDOSE.

The generalized model allows use of theoretical or experi-

mental data for fractional leakage and settling rates by simply

picking time-rate points from a graph. Thus as progress is made

in the field of aerosol behavior it will be convenient to use

the newly acquired data without code modification. As an example

Figures 4.2 and 4.3 show how data might look that would be used

as input to the code for a hypothetical accident. Data points

which might be selected for use as input are marked with circles.

Note that the points are not uniformly spaced but are bunched

in regions of maximum change. The time rate points calculated

internally by linear interpolation are printed out so they can

be checked against the original data.

L~ = L E A K R A T E F R O M C O M P A R T P I E N T @ T O C O M P A R T M E N T @ , s e c - 1

si = S E T T LI N G A N D P L A T E O U T R A T E F O R B A R RI E R a , s e c - 1

F = F I L T E R F A C T O R

L 1 6 I

-

L 1 8

L 1 4 0 F U E L

L 1 2 L 2 8

t V

FIGURE 4.1. Multiple Containment Model

4 . 5

@

A T M O S P H E R E

0 L 2 3 - + F -- 3 8

4 - B A R R I E R 1 I 8 I

F I L T E R E I T H E R 0 R

S E T T L I N G A N D P L A T E O U T 1 /

/ 34 -4 '

L 2 4 4 8

I L 7

S E T T L I N G A N D

L . II

8 4 5 - + F

B A R R I E R 2

L 5 6 b--' 4 6

0

L 6 8

5 8

4 ).

I I

'2 F I L T E R

S E T T L I N G A N D P L A T E O U T 2

E I T H E R O R

I /

/

7 I *

7 8 t

i - -

F I L T E R

r

-0 L 6 7 - B A R R I E R 3 , s 3

t F

0

F U E L T O B A R R I E R 1

B A R R I E R 1 T O B A R R I E R 2

1 0 - ~ ' 0 1 0 0 0 2 0 0 0 3 0 0 0 4 0 0 0 5 0 0 0

T I M E A F T E R A C C I D E N T C O M M E N C E S , s e c

FIGURE 4.2. Typical Leak Rate Data

1 0 0 0 2 0 0 0 3 0 0 0 4 0 0 0

T I M E A F T E R A C C I D E N T C 0 ; - I M E N C E S , s e c

-

S, , F O R B A R R I E R 1

- - - - 4

S 2 , F O R B A R R I E R 2

w - w 1 4

I I

FIGURE 4 .3 . T y p i c a l S e t t l i n g R a t e D a t a

-

If this proposed method of describing containment system

action becomes generally used it will be desirable for those

conducting tests to report their data in terms usable in this

system, i.e. make available the results of aerosol behavior

tests in terms of settling rate as a function of time for vari-

ous nuclides.

The input parameters for the containment calculation include

the time interval for which nuclide release rates are to be cal-

culated, the number of time intervals to be considered, the num-

ber of time-rate points to be entered, the times for the time-

rate data, the rates for the time-rate data, and filter factors.

Filter factors may be specified for individual isotopes or for

groups of isotopes, i.e. noble gases, halogens, volatile solids,

and all remaining fission products. Fractional leak rates and

removal rates describe the containment system being modeled.

Unspecified rates are set to zero.

EXDOSE - Whole Body Gamma Dose Calculation

The subroutine EXDOSE calculates the external whole body

gamma dose based on the release rate data generated in the

subroutine BAFFLE. Dose rates may be calculated with the semi-

infinite cloud assumption or for a finite cloud. The semi-

infinite cloud calculation is well documented and will not be

discussed here. An exact solution to the finite cloud problem

has not been found. A precise and generalized numerical solu-

tion of the finite cloud dose problem is possible but is imprac-

tical because it would take unreasonably long running time on

the computer and because all of the necessary data are not now

available to describe exactly all of the phenomena involved.

A truly precise solution would for example require the descrip-

tion of the activity throughout the space domain as a function

of time. Neither usable models nor tests have been devised

(much less conducted) which provide such detailed information.

To o b t a i n a p r a c t i c a l s o l u t i o n t o t h e problem, t h e

fo l lowing assumptions were made:

The r e c e p t o r i s on o r beneath t h e c loud c e n t e r l i n e a t

ground l e v e l downwind of t h e r e l e a s e p o i n t .

D i f fu s ion a long t h e d i r e c t i o n of t r a v e l can be ignored.

L a t e r a l and v e r t i c a l crosswind d i f f u s i o n s a r e desc r ibed

by normal d i s t r i b u t i o n f u n c t i o n s .

Cloud d e p l e t i o n by f a l l o u t , washout, and r a i n o u t i s no t

inc luded .

The c o n t r i b u t i o n t o t h e dose r a t e from a i r b o r n e n u c l i d e s

a t d i s t a n c e s beyond t h r e e s t anda rd d e v i a t i o n s i n t h e v e r -

t i c a l and l a t e r a l d i r e c t i o n s i s i n s i g n i f i c a n t . (For

e l e v a t e d r e l e a s e , v e r t i c a l l i m i t s a r e - 3 a z t o H + 30,

where H i s h e i g h t of r e l e a s e . )

The c o n t r i b u t i o n i s i n s i g n i f i c a n t beyond 2 4 2 0 meters

away from t h e r e c e p t o r i n t h e d i r e c t i o n of t r a v e l .

(The i n t e g r a t i o n l i m i t s ( 5 ) and ( 6 ) a r e s u b j e c t t o

change. )

For each dose c a l c u l a t i o n t h e fo l lowing parameters a r e

s p e c i f i e d : d i s t a n c e from r e l e a s e p o i n t t o r e c e p t o r , l e n g t h

of r e l e a s e p e r i o d , l e n g t h of exposure p e r i o d , h e i g h t of

r e l e a s e , average wind speed i n d i r e c t i o n of t r a v e l , and t h e

d i s p e r s i o n parameters a and a,. Three methods a r e a v a i l a b l e Y t o account f o r a tmospher ic d i s p e r s i o n of t h e plume.

Hanford model ( b i v a r i a t e normal mode d i s p e r s i o n equa t ion

w i th o be ing time dependent and o Z a f u n c t i o n of time Y

and a tmospher ic s t a b i l i t y ) . Su t ton model.

D i r e c t i npu t of oy and o Z f o r each p o i n t on t h e i n t e g r a -

t i o n g r i d i n t h e d i r e c t i o n of t r a v e l . ( B i v a r i a t e normal

mode d i s p e r s i o n equa t ion i s used - w i t h oy and o ~ i npu t

from P a s q u i l l o r o t h e r s o u r c e ) .

The direct input of dispersion parameters oy and o,

allows an unlimited variety of atmospheric conditions to be

studied.

In Models 1 and 3 the dispersion (time integral of air

concentration) is accounted for by the commonly used equation

x = Q' 2 - exp [ - Y + 2 1

lToyoz u 2oy2 20, 2

(continuous point source, receptor at ground level)

The Hanford model for long-period releases is described in

the 1968 edition of Meteorology and Atomic Energy pp. 380-392.

The dose integration kernel is

B(E,R)e -a (E) R Dk(X,Y,Z,t,E) = K(E)

where

Dk = dose kernel as a function of position, time and

nuclide y-energy,

rad 3 cm sec

= instantaneous cloud concentration as a function of (6) position

curie / curie released ( cm3 ) R = distance from exposure point to kernel in cloud, (cm).

B = Taylor buildup factor, a function of nuclide y-energy

(dimensionless)

a = attenuation coefficient, a function of y-energy,

(cm-l)

K = dose rate conversion factor, a function of y-energy

rads ( C set) (photon/sec) - radsocm 2 sec photon curie curie-sec

The dose kernel is integrated over time and space to

obtain the dose in rads.

For each set of data the code first calculates the dose

rate per curie per cm of cloud (in direction of travel) for

each of 16 energy groups. These dose rate factors involve

integration over the y-z plane at each of the points on the

integration grid in the direction of cloud travel. The points

in the direction of travel are chosen around the exposure

point to ensure accuracy in the numerical integration. The

dose per cm at each point is calculated as

Dose per cm = C Dose Rate (Curies) ceidt /oT i:otopes energies ( r e cm ) where Fei is the fraction of gamma energy from nuclide i in

energy level e.

The dose is given by

Dose fX2 (dose per cm) dx

X1

The amount of each nuclide ("curies" in above equations)

at each integration point is calculated as a function of time.

. The calculation accounts for chain decay with branching in a

similar fashion to the initial inventory calculation of

subroutine SOURCE.

The gamma energy spectrum has been divided into 16 energy

groups as listed in Table 4.1. The main reason for considering

16 energy groups is that a 16 group data library is available.

TABLE 4.1. Energy Groups

Upper L i m i t Average Energy, Group No. Energy, MeV MeV

Much t ime and money has been i n v e s t e d i n t h e development of

t h i s l i b r a r y . A s i n g l e group c a l c u l a t i o n was n o t used s i n c e

such a c a l c u l a t i o n c o u l d i n t r o d u c e s i g n i f i c a n t e r r o r f o r i n d i -

v i d u a l n u c l i d e s .

Computer Requirements

The code h a s been programmed i n FORTRAN V f o r t h e

Univac 1108 computer o p e r a t e d by Computer Sc ience C o r p o r a t i o n

a t R i c h l a n d , Washington. The Univac 1108 h a s a v a i l a b l e a mag-

n e t i c c o r e memory of 36 b i t words t h a t t o t a l s 131,072, 4 5 m i l -

l i o n words of magne t i c drum memory, and 8 compat ib le UNISERVO

V I I I C t a p e d r i v e s . The code p r e s e n t l y u s e s o n l y two t a p e d r i v e s

( f o r d a t a s t o r a g e ) . The s i z e o f t h e main s u b r o u t i n e s (SOURCE,

BAFFLE and EXDOSE) d i c t a t e s t h a t o n l y one be i n t h e c o r e a t a

t i m e . T h e r e f o r e , t h e t a p e d r i v e s a r e n e c e s s a r y t o s t o r e d a t a

from one s u b r o u t i n e w h i l e t h e n e x t s u b r o u t i n e i s b e i n g loaded

(drum memory may a l s o be used i n s t e a d o f t a p e s ) . F i g u r e 4 . 4

i l l u s t r a t e s t h e r e l a t i o n o f t a p e d r i v e s and drums f o r t h e f o u r

main s u b r o u t i n e s . T h i s r e l a t i o n a l l o w s t h e s u b r o u t i n e t o be

e n t e r e d i n any o r d e r . For example a t y p i c a l r u n may have t h e

f o l l o w i n g c a l l i n g sequence :

SOURCE ( f o r i n v e n t o r y ) - 5 t o 30 s e c computer t ime

BAFFLE ( f o r r e l e a s e ) - 5 t o 60 s e c

EXDOSE (y - d o s e f o r 1 s t m e t e o r o l o g i c a l c o n d i t i o n ) - 10 t o 30

EXDOSE (y - dose f o r 2nd m e t e o r o l o g i c a l c o n d i t i o n ) - 10 t o 30

BAFFLE ( d i f f e r e n t r e l e a s e o f same i n v e n t o r y )

EXDOSE (y - d o s e f o r 1st m e t e o r o l o g i c a l c o n d i t i o n )

EXDOSE (y - d o s e f o r 2nd m e t e o r o l o g i c a l c o n d i t i o n )

SOURCE (new i n v e n t o r y ) 2 e t c . R E G I O N A L M O D E L I N G O F S U R F A C E WATER T E M P E R A T U R E FROM P R O J E C T E D

POWER GROWTH - R. T . J a s k e a n d D . E . P e t e r s o n

A r e p o r t , P o t e n t i a l Thermal E f f e c t s o f An Expanding Power

I n d u s t r y : Upper M i s s i s s i p p i R ive r B a s i n , was comple ted i n

d r a f t form d u r i n g t h e r e p o r t p e r i o d . The r e s u l t s a r e summarized

i n F i g u r e s 4 . 5 , 4 . 6 , and 4 . 7 , a v e r a g e and low f l o w c o o l i n g c a p a c -

i t i e s o f t h e Upper M i s s i s s i p p i R ive r from Roya l ton , Minnesota

t o A l t o n , I l l i n o i s . D i r e c t c o o l i n g c a p a c i t i e s were s i m u l a t e d

by means o f t h e MAXPWR computer code . C o n s t r a i n t s were a tem-

p e r a t u r e enve lope o f 5 O F above n a t u r a l background and i n c r e -

m e n t a l a d v e c t e d h e a t i n c r e a s e s o f 800 t h e r m a l megawatts (MWt).

Because o f a combina t ion o f r e l a t i v e l y low s t r e a m f l o w and low

energy exchange w i t h t h e a tmosphere , November was found t o be

t h e c r i t i c a l month f o r b o t h a v e r a g e and low-f low c o n d i t i o n s ,

w i t h t o t a l UMRB c a p a c i t i e s o f 61,000 MWt and 46,000 MWt

r e s p e c t i v e l y .

f C A R D R E A D E R 1

S O U R C E

I P R I N T E R I C A R D R E A D E R

B A F F L E

I C A R D R E A D E R 1

7 E X D O S E I- 1

I P R I N T E R 1

FIGURE 4 . 4 . C o d e F l o w Diagram

FIGURF: 4.5. Average Direc.t Cooling Capacity of Upper Mississippi River

.-

- T O T A L - U P P E R M I S S I S S I P P I R I V E R B A S I N

-

-

-

-

-

- T O T A L - M A I N S T E M A T A L T O N

-

-

S U B T O T A L - M A I N - R O C K R I V E R (R14 4 7 8 )

- S U B T O T A L - M A I N S T E M B E L O W C H I P P E W A R I V E R ( R M 7 6 2 )

FIGURE 4.6. Low Flow Direct Cooling Capacity of Mississippi River

P R O B A B I L I T Y , %

FIGURE 4.7. Upper Mississippi River Basin Local Direct Cooling Capacities

I n g e n e r a l , coo l ing c a p a c i t i e s were adequate a long t h e

main stem M i s s i s s i p p i t o a s s i m i l a t e and d i s s i p a t e p r o j e c t e d

1980 thermal l oads . Upstream of t h e conf luence of t h e Missis-

s i p p i and Chippewa R ive r s , i n t h e S t . Paul-Minneapol is a r e a ,

low flow h e a t s i n k c a p a c i t i e s were found t o be marg ina l wi th

r e s p e c t t o p r e s e n t loads i n t h e downtown a r e a and w i t h r e s p e c t

t o 1980 loads i n a d j a c e n t reaches of t h e M i s s i s s i p p i , Minnesota

and S t . Croix Rivers . T r i b u t a r y s t r eams , i nc lud ing t h e

Minnesota, S t . Cro ix , Chippewa, Cedar-Iowa, Des Moines and

I l l i n o i s Rivers have i n s u f f i c i e n t coo l ing c a p a c i t i e s wi thout

a n c i l l a r y coo l ing f a c i l i t i e s under low flow c o n d i t i o n s f o r p ro -

j e c t e d 1980 and/or 1990 l o a d s . C a p a c i t i e s of t h e Wisconsin an.d

Rock Rivers a r e adequate f o r 1980 c o n d i t i o n s p r i m a r i l y because

of an expected low l e v e l i n c r e a s e i n l o c a l gene ra t i ng c a p a c i t y .

Rock River thermal c a p a c i t i e s a r e inadequa te f o r p r o j e c t e d

1990 l o a d s . The lower Wisconsin R ive r , which has a l o c a l h e a t

s i n k c a p a c i t y of 900 MWt o r g r e a t e r 99% of t h e t ime , may remain

wi thout s i g n i f i c a n t sources of thermal e f f l u e n t s through 1990

because t h e nearby c e n t r a l s e c t i o n of t h e Upper M i s s i s s i p p i

cou ld accommodate p r o j e c t e d loads wi thout a u x i l i a r y coo l ing

f a c i l i t i e s . By 1990 p r o j e c t e d gene ra t i ng c a p a c i t y i n t h e

Rock I s land-Mol ine-Eas t Moline-Davenport (Quad C i t i e s ) a r e a

would be marginal wi th r e s p e c t t o c a l c u l a t e d low-flow coo l ing

c a p a c i t i e s . A s i m i l a r c o n d i t i o n ho lds i n t h e A l ton- S t . Louis

a r e a . A t t h e 99% p r o b a b i l i t y l e v e l l o c a l c a p a c i t i e s a r e

4600 MWt i n t h e Quad C i t i e s , 6000 MWt a t Al ton and 8100 MWt

a t S t . Louis . If sou rces of thermal e f f l u e n t s a r e no t con-

c e n t r a t e d i n s h o r t r eaches , a tmospher ic d i s s i p a t i o n would

i n c r e a s e a r e a c a p a c i t y s i g n i f i c a n t l y .

S imula t ions of 1964 tempera tures of t h e Missour i River

from Sioux C i t y , Iowa t o S t . Louis and of t h e Upper M i s s i s s i p p i

River from Al ton t o Ca i ro , I l l i n o i s were completed s a t i s f a c t o r i l y

dur ing t h e r e p o r t p e r i o d . Determinat ions of t h e 5 O F h e a t s i n k

capacities of the Missouri River and the lowermost 200 miles

of the Upper Mississippi River are scheduled for May and June.

MAXPWR simulations of thermal capacities of the Columbia-Snake

River system within a temperature envelope of 2 O F are also

scheduled for May and June.

Reference

1 . NucZear S a f e t y Q u a r t e r l y R e p o r t , November, December , l969 , J a n u a r y , 1970 , BNWL-1315-1. B a t t e Z Z e - N o r t h w e s t , R i c h l a n d , W a s h i n g t o n , March 1970 .

5. F I X A T I O N O F R A D I O A C T I V E R E S I D U E S

O V E R A L L S T A T U S O F W S E P R A D I O A C T I V E D E M O N S T R A T I O N S

K . J . S c h n e i d e r

Table 5.1 shows the overall status of the radioactive demon-

strations in WSEP as of April 30, 1970. A total of 29 demon-

strations have been completed: 6 in the pot calcination pro-

cess, 11 in the phosphate glass solidification process, and 12

with the spray solidification process. Approximately 45 MCi

of mixed radionuclides representing waste from about 263,000

MWd of electrical power have been converted to solids. This

amount of waste represents 65 days of all the nuclear power

capacity in the United States as of February 1, 1970. The total

on-line processing time for solidification of these wastes was

also 65 days.

TABLE 5.1. Overall Status of WSEP Radioactive Demonstrations

Runs Completed

Megacuries Solidified

Equivalent Tonnes (a) Processed

MWde Represented by Waste (b )

Tonne/Day Rate (a)

Maximum kW in One Pot

Maximum W/L in Pot

Maximum Centerline Temperature in Pot, OC

Liters Solid/Tonne (a)

Solidification Methods Phosphate

Pot Spray Glass Total

6 12 11 2 9

4.0 21.5 19 4 5

a. Tonne i s a m e t r i c tonne (1000 k g , o r 2205 l b l o f o r i g i n a l f u e l . b . Assuming 33% t h e r m a l e f f i c i e n c y and 20,000 MWd/tonne. c . T h i s v a l u e i s f o r 6 - i n . d i a m e t e r p o t s , whereas t h e comparabZe vaZues f o r

t h e po t and s p r a y s o l i d i f i e r s a r e f o r 8 - i n . d i a m e t e r p o t s . d . For 8 - i n . d i a m e t e r p o t s , t h e maximum i s 1 9 5 K/L. e . T o t a l s t o d a t e from a Z t p r o c e s s e s .

S P R A Y S O L I D I F I C A T I O N

L A B O R A T O R Y S T U D I E S

I n - P o t M e l t i n g Development - J . E . Mendel and J . N . S t r o d e

The l a b o r a t o r y program t o deve lop chemica l f l o w s h e e t s f o r

t h e f i n a l two WSEP s p r a y s o l i d i f i e r runs where in t h e s p r a y c a l -

c i n e d w a s t e w i l l be me l t ed d i r e c t l y i n t h e f i n a l s t o r a g e con-

t a i n e r ( i n - p o t m e l t i n g ) i s n e a r l y comple te . The e f f e c t s o f

such p a r a m e t e r s a s f l u x c o m p o s i t i o n , r a t i o o f f l u x t o w a s t e c a l -

c i n e , chemica l a d d i t i o n s t o t h e was te b e f o r e c a l c i n a t i o n , and

p r o c e s s i n g t e m p e r a t u r e have been examined.

For t h e i n - p o t m e l t i n g r u n s t h e c o n t i n u o u s p l a t i n u m m e l t e r

of t h e WSEP s p r a y s o l i d i f i e r h a s been r e p l a c e d w i t h a s p e c i a l

s p o o l - p i e c e c o n t a i n i n g a p o r t f o r t h e a d d i t i o n of a s o l i d f l u x -

i n g a g e n t . The s o l i d f l u x i n g a g e n t i s added t o combine w i t h

t h e c a l c i n e i n t h e c o r r e c t r a t i o t o form a m o n o l i t h i c p r o d u c t

upon f u s i o n i n t h e s t a i n l e s s s t e e l r e c e i v e r , which is a l s o t h e

f i n a l s t o r a g e v e s s e l . The f l u x i n g a g e n t must have c e r t a i n

p r o p e r t i e s : . a R e l a t i v e l y low m e l t i n g p o i n t s o t h a t f u s i o n c a n be

c a r r i e d o u t i n s t a i n l e s s s t e e l c o n t a i n e r s .

Low c o r r o s i v i t y t o s t a i n l e s s s t e e l .

A b i l i t y t o combine w i t h c a l c i n e t o form a r e l a t i v e l y

homogeneous s o l i d f r e e o f v o i d s p a c e s .

a Low l e a c h a b i l i t y .

Composi t ions o f t h e s o l i d f l u x i n g a g e n t s which were c o n s i d e r e d

i n t h e l a b o r a t o r y t e s t program a r e g i v e n i n Tab le 5 . 2 . These were . a l l g l a s s f r i t s which were o b t a i n e d commercia l ly o r , i n t h e c a s e

t h e p h o s p h a t e - c o n t a i n i n g f r i t s , p r e p a r e d i n t h e l a b o r a t o r y .

L imi ted t e s t s were a l s o made u s i n g t h e compounds B203 and NaP03

f o r f l u x i n g .

TABLE 5.2. Flux Compositions Used for In-Pot Mel t ing T e s t s

B o r o s i l i c o P h o s p h a t e P h o s p h a t e Approx imate F r i t F r i t F r i t F r i t F r i t Coke Glass F r i t ' lass F r i t

C o m p o s i t i o n , w t % 1 1 1 ' ~ ) 1 1 1 - 1 ~ ' ~ ) 1 8 0 6 ( ~ ) 7 8 - l ( a ) 1 4 1 ~ ' ~ ) - - - - - B o t t l e I I1 111 IV - v B2°3 2 6 3 6 30 2 3 1 8 2 8 30 24 26

SiO, 3 7 3 2 3 6 2 0 5 5 7 3 3 2 34 2 8 30 4.

Na20-K20 11 10 16 1 19 16 1 4 . 5 1 6 26 2 7 8 4

ZnO 1 8 15 9 9

B a O

F

PbO

A c c e l e r a t e d Leach R a t e , %

Weight Loss

F i r s t 24 h r 0 . 0 9

Second 24 h r 0 . 0 5

T h i r d 24 h r 0 . 0 2

O v e r a l l , 72 h r 0 . 1 6

a . Manufac tured by American P o r c e l a i n Enamel Company, Muskegon, Mich igan .

The l a b o r a t o r y t e s t s made were of two types : b a t c h me l t s

of 20 t o 50 g and cont inuous runs i n 2 - i n . d iamete r p o t s t o

make about 1500 g of me l t . For t h e ba t ch m e l t s , s o l i d f l u x

and c a l c i n e were premixed; f o r t h e cont inuous runs f l u x and

c a l c i n e were added semicont inuously i n two s t reams a t t h e

d e s i r e d r a t i o . The c a l c i n e powder which was used was prepared

from t h e PW-4m waste composit ion and was e i t h e r ba t ch c a l c i n e d

and ground i n t h e l a b o r a t o r y o r p repared i n t he c o l d develop-

mental sp ray c a l c i n e r . I n e i t h e r ca se t h e c a l c i n e p a r t i c l e s

were q u i t e f i n e w i th more than 95% pass ing a 200 mesh s c r e e n .

Various s i z e s of f r i t p a r t i c l e s have been used , b u t i n most

ca se s t h e f r i t p a r t i c l e s have been cons ide rab ly l a r g e r than

t h e c a l c i n e p a r t i c l e s .

The f l u x chosen f o r i n - p o t mel t ing Runs SS-12 and 1 3 was

f r i t 111-15 (composit ion g iven i n Table 5 . 2 ) , a low-mel t ing

b o r o s i l i c a t e g l a s s . The d e c i s i o n was based p r i n c i p a l l y upon

c o n s i d e r a t i o n s of p o t e n t i a l p o t c o r r o s i o n and mel t q u a l i t y ,

i . e . , l e a c h a b i l i t y and homogeneity.

Vo id - f r ee me l t s were ob t a ined wi th B203 and NaP03 f l u x i n g ,

b u t t h e p roduc ts were undes i r ab ly l eachab le and, i n t h e c a s e of

NaP03, t h e mel t was unacceptably c o r r o s i v e t o s t a i n l e s s s t e e l .

Phosphate g l a s s f r i t s I and I 1 y i e l d e d homogeneous me l t s a t

950 O C con ta in ing 30 w t % PW-4m i n l a b o r a t o r y ba t ch t e s t s . The

mel t proved too c o r r o s i v e f o r f u r t h e r c o n s i d e r a t i o n however.

I n a cont inuous run i n a 2 - i n . p o t made of 304L s t a i n l e s s s t e e l

t h e p o t w a l l corroded through a f t e r 2 4 h r a t 950 O C . Of t h e

fou r b o r o s i l i c - p h o s p h a t e g l a s s f r i t s which were examined

b r i e f l y , composit ion I y i e l d e d the most homogeneous m e l t s , b u t

temperatures above 950 "C were r e q u i r e d ( t h e a r b i t r a r y upper

o p e r a t i n g temperature f o r i n - p o t mel t ing i n 304L s t a i n l e s s

s t e e l p o t s ) . Coke b o t t l e g l a s s , a soda l ime s i l i c a t e formula-

t i o n , a l s o r e q u i r e d temperatures above 950 O C t o o b t a i n void

free melts. Melts with coke bottle glass also had 2 to 3 vol%

of a second phase which floated on the glass melt and solidified

to a soluble yellow microcrystalline phase.

The borosilicate frits were studied in most detail. Melts

of calcine plus the lead-containing frit (frit 78-1) were about

an order of magnitude more corrosive to stainless steel than

melts made with borosilicate frits not containing lead. Since

frit 78-1 was also relatively leachable, it was rejected from

further consideration. The remaining three borosilicate frits

(frits 111, 1806, and 1415) all yielded void-free melts at

950 O C , but shared a common characteristic: a second phase

was formed similar to that observed with coke bottle glass.

The most yellow phase was found in melts prepared with frit

1415. Frits 111 and 1506 were about equal in their tendency

to form the yellow phase. Since frit 111 was much less leach-

able it was chosen for development studies.

Because the yellow phase has several undesirable features,

discussed in more detail later, considerable effort was expended

in determining methods of minimizing the amount of yellow phase

present. The composition of the yellow phase is quite complex,

but its presence in borosilicate-waste melts has been traced to

one element, molybdenum, a high yield fission product. The

yellow phase is not observed in either borate or phosphate-waste

melts. Thus it can be concluded that silicate concentration

in the melt is an important factor. Additions of phosphate to

frit 111 prevented yellow phase formation but the melts were

somewhat porous and the corrosion problem was increased. Addi-

tions of borate to frit 111 also decreased yellow phase forma-

tion although somewhat less effectively, and this was the solu-

tion finally adopted. Frit 111-15 represents a compromise between

higher leach rates resulting from more borate and less yellow

phase resulting from reduced silicate.

The a l lowable r a t i o of waste c a l c i n e t o g l a s s f r i t i s very

dependent upon p roces s ing temperature and f r i t p a r t i c l e s i z e .

The r a t i o can be i nc rea sed a t h ighe r temperatures and w i t h s m a l l e r

f r i t s i z e . For t h e WSEP runs t h e upper t empera ture l i m i t i s

950 O C and t h e f r i t s i z e i s -6+10 mesh. The need f o r t h e r e l -

a t i v e l y l a r g e f r i t p a r t i c l e s i s imposed by t h e c o n f i g u r a t i o n

of t h e WSEP s o l i d f l u x a d d i t i o n system. The maximum a l lowab le

r a t i o of c a l c i n e t o f r i t i n t h e WSEP runs appears t o be about

30:70 by weigh t . Laboratory t e s t s i n d i c a t e t h a t t h i s r a t i o

could be 50:50 i f -100 mesh f r i t were used. I n l a b o r a t o r y

s t u d i e s of combining waste c a l c i n e and g l a s s f r i t conducted

a t o t h e r s i t e s -100 mesh f r i t was used.*

Various c a t i o n s were added t o t h e waste p r i o r t o c a l c i n -

a t i o n and t h e i r e f f e c t i v e n e s s i n p reven t ing fo rmat ion of t h e

molybdenum second phase was eva lua t ed . A t t h e sugges t i on of

D r . W . Guber of t h e Kar lsruhe Research Cente r , t i t a n i u m was

inc luded i n t h e t e s t s . Although l a r g e amounts were r e q u i r e d

(over one mole pe r l i t e r i n waste a t 378 l i t e r s pe r tonne)

t i t a n i u m d i d i n h i b i t s e p a r a t i o n of t he yellow phase b u t

m , ine ra l i za t i on i n t h e product was i nc rea sed . Seve ra l d i v a l e n t

c a t i o n s a l s o proved somewhat e f f e c t i v e , and calc ium and z i n c

a t 0 . 6 5 and 0.50 moles per l i t e r , r e s p e c t i v e l y , were s e l e c t e d

f o r use i n Run SS-12. However, t h e optimum chemical t echn ique

f o r p r even t ing fo rmat ion of t h e molybdenum second phase i n t h e

i n - p o t mel t ing f lowshee t has no t y e t been found.

Resu l t s of l a b o r a t o r y t e s t s have i n d i c a t e d t h a t r a i s i n g

t h e o p e r a t i n g temperature 1 0 0 O C , t o 1050 O C , e l i m i n a t e s t h e

* Bimonthly r e p o r t s , Chemica 2 Techno logy Group, Chemis t ry and Chemical Eng ineer ing D i v i s i o n , Nuclear Eng ineer ing Depart- ment , Brookhaven NationaZ Labora tory . J u l y , 1965 through Augus t , 1967.

H . W . Godbee, N . M . Davis , D i s p e r s i o n o f S imula ted High- Leve l R a d i o a c t i v e Waste Powders i n a Glass M a t r i x , ORNL-TM-1897. August 4 , 1967.

yellow phase completely. Gravimetric experiments show that

since less than 5% of the yellow phase is volatilized in 24 hr

at 1050 OC, dissolution in the borosilicate melt must occur

at the higher temperatures. When the processing temperature is

950 OC there is also some suspension of calcine particles within

the glassy matrix. These dissolve rapidly at 1050 OC.

The yellow phase from developmental spray calciner Run DSC-41

product was collected and analyzed. Globules of yellow phase

were found at the top and the bottom of the filled pot in the

following amounts:

Top yellow phase Approximately 50 g.

Bottom yellow phase Approximately 100 g.

Total weight of melt Approximately 89.1 kg.

Some of the properties of the yellow phase are compared with

the bulk phase in Table 5.3. Molybdenum is concentrated almost

exclusively in the second phase. Of the long-lived fission

products, strontium is not concentrated strongly in the yellow

phase but cesium is. This was demonstrated in a special labor-

atory preparation (DSC-41 used potassium as a stand-in for cesium).

The yellow phase contained 12.3 wt% cesium versus 2.5 wt% in

the bulk glass.

Corrosion Studies - R. F. I\,Ianess

Corrosion of 304L and of 310 stainless steel was evaluated

in a melt composed of 30 wt% PW-4m waste calcine from Run

DSC-32* and 70 wt% of borosilicate glass frit 111-15 (see

Table 5.2). Specimens of 304L exposed to the melt phase at

950, 1000 and 1050 "C corroded at rates of 0.02, 1.5, and 8.1

in./yr, respectively. Corrosion rates of specimens exposed to

the melt-vapor interface were about 50% higher than those of

TABLE 5.3. Characteristics of Second Phase in DSC-41 Product

TOP Bottom Yellow Bulk Yellow Phase Mel t Phase

304L SS C o r r o s i o n 0 .44 0.02 0 .44 r a t e a t 950 O C , i n . / y r

M e l t i n g p o i n t s , " C 700 950 9 75 - D e n s i t y , g/cm3 3.116 3.102 3.731

A c c e l e r a t e d Leach T e s t a t 950 O C

% Weight Loss

F i r s t 24 h r 7 8 .-2 1 . 4 22.8

Second 2 4 h r 4 .4 1.1 1.1

T h i r d 24 h r 3.8 1.1 0.68

O v e r a l l % w t l o s s 79 .8 3.6 24.2

Compos i t i on , w t % ( a >

Nd <1 0 . 8 1

C e cO.1 3 0 .5

a . T h e a n a l y s e s w e r e made b y s p a r k s o u r c e mass s p e c t r o g r a p h y and a r e e s t i m a t e d t o b e a c c u r a t e t o a f a c t o r o f t h r e e .

specimens exposed to the melt phase only. Specimens of 310

exposed to the melt phase at 1000, 1050, and 1100 O C corroded

at rates of 0.025, 6 . 2 9 , and 2.1 in./yr, respectively. Ccrro-

sion rates of spscir,lens expose:! t~ the ktcrface were

about 508 higher, largely dge to preferential attack at the

interface rbthe.r th2n heavy vapcr phase c'3rrosi.cn.

Analysis of Radioruthenium in WSEP Solidified Waste Products -

M. R. Schwab and F. E. Holt

A nondestructive direct count method was developed for the

analysis of Ruthenium-106 in melt samples from the spray solidi-

fication and phosphate glass radioactive demonstration runs in

WSEP. With the Direct Count method, the melt samples are weighed,

then gamma scanned directly instead of dissolving the sample and

gamma counting a small aqueous alignot of the product sample.

The gamma counting results for the dissolved product solutions

have routinely given low ruthenium recoveries because of an

incomplete dissolution of solid samples. Prior to Run PG-11,

the total radioruthenium reported for each filled receiver pot

was determined indirectly from the total Ruthenium-106 in the

feed to the solidifier less the total Ruthenium-106 found in

the condensates downstream from the solidifier. This indirect

analysis indicated that from 80 to 95% of the input ruthen-

ium should be contained in the phosphate glass solidified waste

and from 25 to 50% should be contained in the spray solidified

waste product. The results from the ruthenium balances for

Runs PG-11, SS-11, and SS-12 are given in Table 5.4 with the

Direct Count method used for the solid waste analyses. Good

ruthenium recoveries are indicated. The Direct Count method

for the first time actually verifies with a relatively high

degree of confidence that the majority of the ruthenium not

found downstream of the solidifier is indeed contained in

the solidified waste.

TABLE 5.4. Material Balances for Ruthenium-106 in WSEP Radioactive Demonstrations (a)

Run Run Run PG-11 SS-11 SS-12

( b -

Product 0.833 0.182 1.030

Evaporator (TK-113)

Melter Condensate 0.074 - - - - (TK- 117)

Total Recovery 0.91 0.91 1.05

a . The d a t a a r e r e p ~ r t e d a s t h e f r a c t i o n o f Ru then ium- 106 f ed t o t h e s o z i d i f i e r and t h e a c c u r a c y o f d a t a i s w i t h i n 5 t o 1 0 % .

b . P r o d u c t a n a l y s i s v i a t h e d i r e c t c o u n t m e t h o d .

E N G I N E E R I N G S T U D I E S

In-Pot Meltine Develo~ment - J. D. Moore

Developmental spray solidifier Runs DSC-40 and 41 were made

using the in-pot melting technique. During the runs simulated

PW-4m waste with added calcium and zinc (see Table 5.5 for detailed

feed compositions) was dried to a calcine in the spray calciner

and the calcine was melted in the storage pot at 950 O C with a

solid borosilicate glass frit. The zinc and calcium salts were

added to improve melt product homogeneity. In DSC-41, zinc

nitrate additive was used instead of zinc oxide (which was used

in DSC-40) to reduce feed solids content to improve feed flow

stability. With zinc nitrate, the feed solids content was only

10 vol% as compared to 40 vol% with zinc oxide. More stable

feed flow was achieved with the lower solids-containing feed.

TABLE 5.5. PW-4m Feed Composition for Developmental Spray Solidifier Runs

Basis: 378 liters/tonne Concentration Run Number Chemicals

~ e + ~

Fission Products

MOO;'

sr+'

~a+'

Rb + Cs (used K + )

(Y + RE)+^ z~o+' RU+

Rh (used CO+')

~ g +

cd+'

Te (used s0i2)

Pd (used ~ i + ~ , included above)

Tc (used MOO;', included above)

Additives

ZnO

Zn (NO3) 2

Glass frit(d) (added as solid to melt pot) 406 g/L 406 g/L (70% by weight of final product)

a . Nominal Fe c o n c e n t r a t i o n i s 0 .05g. Exces s i s Ru s u b s t i t u t e . b . Nominal Na c o n c e n t r a t i o n i s O . I M _ . Exces s Na i s from u s i n g Ua2Mo04'2H20

f o r Mo a d d i t i o n . c . Nominal Ru c o n c e n t r a t i o n i s 0.082M_. d. 1 1 1 - 1 5 , American P o r c e l a i n Enamel Co.

I n DSC-40, b o r o s i l i c a t e g l a s s f r i t 111-15 ( -6 mesh) was added

t o t h e p o t a t 5 min i n t e r v a l s . DSC-41 was run t o determine

if me l t homogeneity would be a f f e c t e d i f t h e f r i t a d d i t i o n f r e -

quency was decreased t o once every 30 min. The once every

30 min a d d i t i o n was thought t o be a p r a c t i c a l f requency a t

which t o add s o l i d s t o t h e p o t i n t h e WSEP spray s o l i d i f i c a t i o n

p r o c e s s . I n both r u n s , t h e average s o l i d s me l t i ng r a t e was

9.4 kg/hr i n c l u d i n g 6.6 kg/hr of g l a s s f r i t . The l a r g e r f r i t

ba tches used i n DSC-41 taxed t h e p o t me l t i ng c a p a c i t y more t han

t h e s m a l l e r , more f r e q u e n t l y added ba tches of DSC-40. I n t h e

l a t t e r r un , t h e average tempera ture of t h e mel t s u r f a c e was

h ighe r (determined by b r i g h t n e s s of c o l o r ) t han i n DSC-41.

Both 304L s t a i n l e s s s t e e l p roduc t po t s were f i l l e d t o a

l e v e l of 30 t o 33 i n . wi th mel t and mainta ined a t a fu rnace

tempera ture of 950 "C f o r 1 2 h r a f t e r t he runs were s h u t

down. A f t e r c o o l i n g , t h e po t s were s e c t i o n e d l o n g i t u d i n a l l y

f o r v i s u a l i n s p e c t i o n . No evidence of po t w a l l o r thermowell

c o r r o s i o n was found. The g l a s s p roduc t of DSC-41 was n o t a s

homogeneous a s t h e p roduc t from DSC-40. The produc t con ta ined

s e v e r a l vo ids up t o 1 i n . i n d iamete r and t h e c a l c i n e d i d n o t

appear t o be a s complete ly d i s s o l v e d i n t h e g l a s s a s i t was i n

DSC-40. I n t h e WSEP, however, t h e me l t would be h o t t e r i n t h e

c e n t e r because of i n t e r n a l r a d i o a c t i v e h e a t g e n e r a t i o n , and

produc t homogeneity should be b e t t e r than t h a t observed i n DSC-41.

Also , i n c r e a s i n g t h e s o l i d s a d d i t i o n f requency t o a t l e a s t once

every 15 min should probably improve t h e p roduc t homo-

g e n e i t y .

Traces of a yellow c r y s t a l l i n e m a t e r i a l was i n t e r s p e r s e d

throughout t he p roduc t i n both p o t s , b u t the m a t e r i a l was much

more abundant (about 1% of t o t a l mel t volume) i n t h e mel t from

DSC-41 a s d i s cus sed i n a p rev ious s e c t i o n . The g l a s s y mel t i n

t h e bottom 4 i n . of both po t s had a mot t l ed gray c o l o r , whi le

t h e r e s t of t h e g l a s s was dark brown. Although chemical

ana lyses of p roduc t samples showed t h a t ruthenium was 4 t o 9

t imes more concen t r a t ed i n t h e bottom than i n t h e t op of t h e

p o t , t h e gray c o l o r could n o t be a t t r i b u t e d t o ruthenium s i n c e

dark brown g l a s s samples nea r t he bottom of t he p o t con ta ined

about t h e same amount of ruthenium as t h e g ray- co lo red samples.

Leach t e s t s on g l a s s y me l t samples from both p o t s were

conducted t o determine i f p roduc t s o l u b i l i t y was a f f e c t e d by

t h e f l u x a d d i t i o n f requency. Samples were leached f o r t h r e e days

i n d i s t i l l e d wate r hea t ed t o 95 O C . Water was changed every

2 4 h r , and t h e samples were weighed t o determine weight l o s s

from l each ing . I t was found t h a t t h e p roduc t s o l u b i l i t i e s were

n o t s i g n i f i c a n t l y d i f f e r e n t (3% s o l u b l e f o r DSC-40 and 3.9%

s o l u b l e f o r DSC-41).

Spray c a l c i n e r o p e r a t i o n was r e l a t i v e l y smooth i n both runs .

Operat ing cond i t i ons and r e s u l t s of both runs a r e summarized i n

Table 5 .6 . I n DSC-40, f eed f low was no t a s s t a b l e a s i n DSC-41

f o r reasons mentioned p r e v i o u s l y , and t h e sp ray nozz le plugged

fou r t imes e a r l y i n t h e run . The f low was main ta ined , however,

when t h e atomizing a i r f low was reduced from 6.3 t o 5.5 scfm.

Ca lc ine d e p o s i t s on t h e i n n e r w a l l s of t h e c a l c i n e r were l e s s

than 1 / 8 - i n . t h i c k fo l lowing both runs . V i sua l acces s through

t h e g l a s s window i n t o t h e po t was adequate s i n c e it was nec-

e s s a r y t o s e e only t h e r ed glow from i n s i d e t h e p o t . The i nne r

s i d e of t h e window was coa ted wi th a t h i n l a y e r of powder, b u t

v i s i o n was n o t f u l l y b locked.

Less t han 1% of t h e f eed ruthenium was v o l a t i l i z e d i n

DSC-40 and only 6% v o l a t i l i z e d dur ing DSC-41.

I t was concluded from t h e s e runs t h a t an adequate s o l i d

p roduc t could be a t t a i n e d by f u s i n g PW-4m waste c a l c i n e wi th

b o r o s i l i c a t e f r i t 111-15 us ing t h e i n - p o t me l t i ng t echn ique ;

t h i s f lowshee t was chosen f o r demons t ra t ion i n WSEP.

TABLE 5.6. Summary of Developmental Spray Solidifier Runs

Run Number

Feed type Feed concentration, liters/tonne

Additives

Feed total acidity, M - H+ at 378 liters/tonne

Feed consumed, liters

Average feed rate, liters/hr

Calciner furnace temperature, OC

Calciner vacuum, inches of water

Atomizing air

Atomizing glass flow, scfm

Filter blowback pressure, psig

Filter pressure drop, end of run, inches of water

Melt storage pot temperature, "C

Solid glass frit added to melt pot, kg

Frit addition frequency, min

Glass frit (solid add to pot) , Ca(NO3I2 ZnO

0.53

205

20.5

700

8

air

5.5 to 6.3

30 (steam)

7

950

55.4 5

Product collected, kg 7 9

Product density, g/cm 3 3.1

Product solubility, wt% (a) 3.0

Product concentration, liters/tonne 59

Particulate DF, feed to condensate 770

Ruthenium volatilized, % of total feed ruthenium <1

Glass frit (solid add to pot) , Ca(NO3I2 Zn (NO3) 2 2.57

150

air

5.7

42 (air)

a . Produc t Leached f o r 3-day per iod i n 9 5 O C d i s t i l l e d w a t e r . Water changed e v e r y 2 4 h r .

R A D I O A C T I V E D E M O N S T R A T I O N S

Spray Solidification Run SS-11 - W. R. Bond

The twenty-eighth pilot plant demonstration of solidifica-

tion of high level radioactive waste was successfully completed

with the eleventh spray solidification Run SS-11. Run SS-11

was the first spray solidifier run with LMFBR waste; however,

the waste as processed was not too different from the PW-4m waste

that was demonstrated in Runs SS-9 and SS-10." Differences were

a slightly changed fission product spectrum and the addition

of selenium, tellurium, antimony, and tin since these elements

become more significant in the higher burnup fast reactor fuels.

The completion of Run SS-11 marks the completion of the radio-

active spray solidifier runs using a high temperature platinum

melter . During Run SS-11, a simulated waste equivalent to that

resulting from the reprocessing of 0.54 tonne of LMFBR core fuel

(100,000 MWd/tonne at 200 MW/tonne) with an equivalent aging

time of 2.2 years was processed to produce 186 kg of ceramic

product. The 60 liters of radioactive ceramic produced a heat

rate density of 170 W/liter (10,900 W total based on analytical

data and 10,200 W total based on pot calorimetry) in an 8-in.

diameter 304L stainless steel melt receiver. The steady-state

pot centerline temperature in the air-cooled furnace was 759 OC,

and the centerline-to-wall temperature difference was 353 OC.

These values indicate an effective thermal conductivity of 1.24 2

W/ (m2) (OC/m) [O. 72 Btuj (hr) (ft ) (OF/ft)] for the ceramic product.

The solidifier was fed 669 liters of adjusted LMFBR feed

(additives of 3.4M - NaOH, 2.17M - Fe(N03)3, and 5.6M - H3P04 based

on 378 litersltonne) at 1230 liters/tonne in 45 hr. The

feed containing 3,110,000 Ci of radioactivity including 14,400

* BNWL-1074, 69-1 and BNWL-1186, 69-2.

Ci of radioactive ruthenium was reduced in volume by a factor

of 11.2, or 3.4 on a 378 liters/tonne basis. A summary of run data for Run SS-11 is presented in Table 5.7, and the feed compo-

sition for the run is given in Table 5.8.

TABLE 5.7. Summary Data for WSEP Spray Solidification Run SS-11

Operational Data

Date

Operating Mode Feed Type

Feed, liters/tonne

Total Feed to Solidifier, liters

Total Feed Time, hr

Average Feed Rate, liters/hr

Equivalent Waste to Solidifier, tonne

Volume Reduction, Feed Volume/Product Volume

Volume Reduction if Feed Were at 378 liters/tonne

Filled Pot Data

Total Curies in Feed to Pot

Total Curies of Ru in Feed to Solidifier

Product in Pot, liters

Product in Pot, liters/tonne Heat Generation Rate in Pot, W

Equivalent Aging Time, years g Temperature in "Air-Cooled" Furnace, "C E to Wall Temperature Difference, "C Effective Thermal Conductivit of Product in 1 an Air-Cooled Furnace, W/ (m ) ("C/m)

3/2/70-3/4/70

A

LMFBR

12 30

669

4 5

14.9

0.54

11.2

3.4

a . Based on c o r e f u e l o n l y a t 1 0 0 , 0 0 0 MWd/tonne and 2 0 0 MW/tonne.

TABLE 5.8. LMFBR Feed Composition for Spray ~ol'idif ication Run SS-11

Component

H+

~ e + ~

~ r + ~

Concentration, M_(a) . --

~ b + + CS+ (added K + ) 0 . 2 2 9

z~o+' + ~b as Z ~ O "

R U + ~

R U + ~ (added ~ e + ~ )

Rh+' (added CO+')

~d+' (added Ni'')

Ag+' (added CU")

~d+' (added CU+')

Additive to Feed

Na+

Fe+3(b)

A1+3(b)

PO;

a . M o l a r i t i e s a r e a t 3 7 8 l i t e r s / t o n n e .

b . Nominal Fe a d d i t i v e i s 2 . 1 7 ! , h o w e v e r e x c e s s A 2 i n t h e w a s t e from t h e p r o c e s s i n g p l a n t was u s e d a s a s u b s t i t u t e f o r F e .

The operation of the spray solidification systems was very

smooth. The principal process factors (atomization, filter oper-

ations, atomizing air and feed flow control) performed very . satisfactorily. A newly installed atomizing nozzle with improved

atomizing air pressure control produced the steadiest internal

calciner temperatures and calcine fall to the melter that has

been observed during the radioactive spray runs. An inspection

of the inside of the solidifier after the run revealed that

essentially no deposition of calcine occurred during the run.

During the run 73% of the ruthenium in the feed processed

was volatilized from the solidifier. Although the ruthenium

volatility was higher than in some previous runs, it was in

general expected for the phosphoric-acid-containing feed. Only

0.013% of the nonvolatiles in the feed processed during the run

were entrained from the solidifier. This represents a cumulative

decontamination factor (DF) for - nonvolatiles across the solidifier

off-gas filters of 7.7 x lo5 which is in agreement with instan- 3 4 taneous DF1s which ranged from 2.9 x 10 to 6.0 x 10 .

The LMFBR melt was batch discharged from the nelter via the

drain freeze-valve into the unheated stainless steel receiver

pot. The melter drain rate during discharge averaged approxi-

mately 34 liters/hr which is about a 40% faster drain rate than

that attained with PW-4m melt during Run SS-lo.* Although it

was necessary to reduce the melter temperature approximately

50 to 100 O C after each dump to seal the freeze valve and stop

the melter from dripping, an even fill of the receiver pot was

achieved.

Following the run the platinum melter was removed from the

melter furnace and it was found that the melter had four large

indentations in the side of it as shown in Figure 5.1. The melter

at the time of removal had experienced approximately 650 hr

of intermittent service with temperatures ranging from 900 to

1200 O C and a vacuum of 0 to 20 in, of water, The melter had

been visually examined prior to Run SS-5 after approximately

220 hr of service, and it had one slight indentation located

in the same area as the indentation labeled number 2 in

Figure 5.1, but it was considerably less pronounced. The exact

cause of the distortion of the platinum melter is not known at

this time, but is to be investigated further, A similar distor-

tion of a platinum melter occurred at Brookhaven National

Laboratory* and was attributed to the negative melter operating

pressure and the reduced creep resistance of the platinum

caused by the long process exposures, A subsequent Brookhaven melter was fabricated with increased wall thickness and

stiffener rings welded to the outside melter wall to increase

strength.

Auxiliarv Process Eaui~ment Performance Durine Run SS-11 - J. N. Hartley

During Run SS-11 the WSEP auxiliaries were operated in

a Mode A arrangement as illustrated in Figure 5.2. The radio-

nuclide distribution for Run SS-11 is summarized in Table 5.9.

A modified solidifier condenser and condenser off-gas

filtering system was installed prior to Run SS-11 to improve

decontamination of the solidifier off-gas. The modified

s-olidifier condenser and off-gas filtering system is shown in

Figure 5.3. The bottom half of the condenser tubes were filled

with pall rings (reduced from 5/8-in, to 1/2-in. diameter by

mechanical press) to improve the condenser performance, Filling

the tubes completely would have substantially increased the

* R. F. Drager, L. C, Emma, J, J. Fedelem, L. P. Hatch, Gerald Strickland, E. J . TuthiZZ, and G, G. Weth. ~evelopment of the Phosphate Glass Process for Ultimate Disposal of High- Level Radioactive Wastes, BBL-50130 (T-505). rook haven Bational Laboratory, Upton, New York, January 1968.

FIGURE 5.2, WSEP Auxiliary Process Equipment (Mod A Arrangement for Run SS-11)

I P W t-' wl

I f3

Neg 700405-2 Neg 700405-5

FIGURE 5.3. New Solidifier Condenser and Offgas Filtering System

TABLE 5.9. Radionuclide Distribution in WSEP ~uxiliaries for Run SS-11

Evapora tor (TK- 113)

F r a c t i o n of E a u i v a l e n t Feed R a d i o a c t i v i t y - - - - - - . - -

For T o t a l ~ u n i n E f f l u e n t Streams Ru-106 CePr - 144

F r a c t i o n a t o r (TK-115) 2 . 1 x l o - 6 < 4

F r a c t i o n a t o r f is till ate 5 .3 x l o - 6 8 x 1 0 - l o Rece iver (TK-116)

Scrubber (TK- 118) 1 .9 x l o - ' 7.7

Offgas from Scrubber 1 .8 x 1 . 4 x 10-'I

Offgas t o S t ack < 2 x l o - 1 o 3 x 1 0 - l ~

R a t i o ( F r a c t i o n a t o r D i s t i l l a t e 1 .6 x 10 4 2 . 2 x 10 2

R a d i o a c t i v i t y t o 10CFR20)

R a t i o (Scrubber Offgas Radio- 4.9 x 1 0 2 3.8 x 10 1

a c t i v i t y t o 10CFR20)

R a t i o (Stack Offgas Radio- < 4 7.8 a c t i v i t y t o 10CFR20)

pressure drop across the condenser to a point that vacuum

requirements for the spray solidifier could not be met.

Radionuclides in the process off-gas are shown in Table 5.10.

The solidifier condenser off-gas contained an average of

5.7 x pci/cm3 of Ru-106 and 4.3 x lom5 pci/cm3 of CePr-144.

The cumulative decontamination factors (DF1s) across the solidi-

fier condenser were 1400 for Ru-106 and 6500 for CePr-144. This

was an improvement over previous results by factors of 10 to 100.

The off-gas leaving the solidifier condenser off-gas filter con-

tained an average of 2.8 x loe6 p ~ i / c m ~ of Ru-106 and 2.6 x

pci/cm3 of CePr- 144. These values indicated average instantaneous 3 DF's across the filter of 2.0 x 10 for Ru-106 and 16 for CePr-144.

The accumulation of radioruthenium in the auxiliaries as

seen in Figure 5.4 was generally typical of previous runs. However,

the radioruthenium accumulation in the fractionator was not

linear as was the case in previous runs, The ruthenium

TABLE 5.10.

Sample P e r i o d S o l i d i f i e r Condense r Sample Kun Time, h r O f f g a s , uCi /cm3 sumher Start Ru-106 CePr -144

N Sample P e r i o d F r a c t i o n a t o r Condense r P Samplc Kun Time, h r O f f g a s , uCi/cm3

Nunher S t a r t End Ru-106 CePr - 144

8 45 .5 54 .5 2 . 2 a lo .6 4 . 3 x l o - s Average 5 .0 x 3 . 3

Radionuclides in Process Offgas

O f f g a s Crom S o l i d i f i e r Condense r F i l t e r , vCi /cm3

R I I - 1 nh C e P r - 1 4 4

O f f g a s f rom F-112 A h s o l u t e F i l t e r , pCi /cm3

Ru-106 C e P r - 1 4 4

5 . 8 ." 10.' 1 .4 x 10.'

8 . 4 x -.-

I . ~ x 1 0 - 7 ( a ) . - .

4 . 9 x 1 0 - 9 1 . 2 x 1 0 - ~

4.6 x . . -

9 . 8 x l o - ' - - -

4 . 4 x l o - 8 1 . 3 x l o - '

E v a p o r a t o r C o n d e n s e r Of f g a s , uCi /cm3

Ku-106 - CePr -144

, F i n a l O f f g a s f rom S c r u b b e r uCl / cm> - R a t i o t o 10CFR2O--

Ru-106 CePr -144 R u - i U 6 r - 1 6 4

1 . 0 x loe1' 4 . 1 x l o - ' 5 x 1 0 - I 1 . 0 x l o 1

6 . 1 ~ 1 0 - @ 2 . 5 ~ 1 0 - ~ 3 . 1 ~ 1 0 ~ 6 . 3 x l o 1

a . Fzcluded from a u t r a g e e

I t-' W P m

I P3

FIGURE 5.4. Radiorutheniun Accumulation in WSEP Auxiliaries --

During Run SS-11

1 0 - I

1 o - ~

- - - -

T K - 1 1 3 ; - - /-- - - S E E F I G U R E 2 FOR - T A N K L O C A T I O N S

- - - - - - -

- - - - - - -

- - - - - - -

I I I I I I 0 1 5 3 0 4 5 6 0 7 5 9 0 1 0 5

% F E E D F E D TO S O L I D I F I E R

accumulation seemed t o l e v e l o u t a f t e r an i n i t i a l jump e a r l y

i n t h e run . Basing t h e accumulation i n t h e f r a c t i c n a t o r on

t h e evapora to r condensate s t ream samples, t h e t o t a l accumulat ion

should have been a f a c t o r of about 20 l e s s . This f a c t i n d i c a t s s

t h a t t h e ruthenium accumulation may have been caused p r i m a r i l y

by i n t e r n a l contaminat ion e a r l y i n t h e run.

The a ~ i x i l i a r y evapora tor ope ra t ed on about 5.7M - HNO w i th 3 an overhead a c i d i t y ranging from 0.1 t o 0.8Y - FINO3. I n s t a n t a -

neous ruthenium D F ' s a c r o s s t h e evapora tor ranged f r ~ m

4.4 x l o 3 t o 1 .3 x l o 5 . These va lues were g e n e r a l l y a f a c t o r

of 13 t o 100 g r e a t e r t han i n p rev ious runs wi th f eed on t o t h e

s o l i d i f i e r , i n d i c a t i n g (a long wi th gas sample r e s u l t s ) t h a t

t h e new modif ied condenser and o f f - g a s f i l t e r were s topp ing

t h e ca r ryove r of ruthenium i n t h e noncondensible gas s t ream

from t h e s o l i d i f i e r condenser. However, t h e r e was a g a i n no

r e a l appa ren t c o r r e l a t i o n between evapora tor overhead a c i d i t y

and ruthenium in s t an t aneous D F ' s . This was a t t r i b u t e d t o

ox ides of n i t r o g e n n o t being scrubbed o u t complete ly by t h e

s o l i d i f i e r condenser. The s o l i d i f i e r condenser only s topped

4 1 % of t h e t o t a l n i t r o g e n i n t h e s o l i d i f i e r o f f - gas . P a r t of

t h e remaining 59% was scrubbed o u t by t h e evapora tor condenser

i n c r e a s i n g t h e evapora tor overhead a c i d i t y , and r e s u l t i n g i n

no c o r r e l a t i o n between ruthenium in s t an t aneous D F ' s and over-

hsad a c i d i t y . That ruthenium e q u i v a l e n t t o 2 . 1 x l o - ' % of

t h a t f e d t o t h e s o l i d i f i e r accumulated i n t h e f r a c t i o n a t o r

i n d i c a t e d a cumulat ive ruthenium DF of 350 ac ros s t h e - evapora to r , and t h a t l e s s than 4 x l o - ' % of t h e CePr-144

r e p r e s e n t i n g n o n v o l a t i l e s accumulated i n t h e f r a c t i o n a t o r

i n d i c a t e d a cumxlat ive DF f o r n o n v o l a t i l e s of g r e a t e r t han 2 4 x 1 0 .

The cumulat ive DF a c r o s s t h e f r a c t i o n a t o r was 6.3 x 1 0 2

3 f o r Ru-106 and 1.3 x 10 f o r CePr-144 r e p r e s e n t i n g n o n v o l a t i l e s .

During Run SS-11, 80% of t h e f r a c t i o n a t o r d i s t i l l a t e was

r ecyc l ed t o t h e evapora tor a s s t r i p wate r whi le t h e remaining

2 0 % was accumulated i n t h e d i s t i l l a t e r e c e i v e r . The f r a c t i o n

of e q u i v a l e n t f eed r a d i o a c t i v i t y t h a t accumulated i n t h e f r a c -

t i o n a t o r d i s t i l l a t e r e c e i v e r was 5.3 x l o m 6 f o r Ru-106 and

8 x f o r CePr-144. The c o n c e n t r a t i o n of r a d i o n u c l i d e i n

t h e accumulated f r a c t i o n a t o r d i s t i l l a t e (fina.1 aqueous e f f l u e n t )

was above lOCFR2O r e l e a s e l i m i t s by 1.6 x l o 4 f o r Ru-106 and 2 2 .2 x 10 f o r CePr-144.

The o f f - gas l eav ing t h e f r a c t i o n a t o r condenser con ta ined

an average of 5 x pci/cm3 of Ru-106 and 3.3 x pCi/cm 3

CePr-144. The o f f - g a s i s f i l t e r e d through a high e f f i c i e n c y

f i l t e r be fo re e n t e r i n g t h e sc rubber . The o f f - gas l eav ing t h e - -

f i l t e r con ta ined 4.4 x l o m 8 uci/cm3 of Ru-106 and 1.3 x

pci/cm3 CePr-144 which i n d i c a t e d D F 1 s a c r o s s t h e f i l t e r of

1.1 x 1 0 ' f o r Ru-106 and 2 5 f o r CePr-144 ( r e p r e s e n t i n g par-

t i c u l a t e DF). The DF f o r p a r t i c u l a t e s was lower by a f a c t o r of

about 100 than i n p rev ious runs .

The f r a c t i o n of e q u i v a l e n t f eed r a d i o a c t i v i t y t h a t accumu-

l a t e d i n t h e o f f - g a s sc rubber was 1.8 x 1 0 ' ~ f o r Ru-106 and

1 . 4 x 1 0 -I1 f o r CePr-144. However, u s ing t h e r e s u l t s from gas

samples t aken p r i o r t o t h e s c rubbe r , t h e f r a c t i o n of f eed r ad io-

a c t i v i t y was 3.8 x l o m 9 f o r Ru-106 and 5.8 x 1 0 - I ' f o r CePr-144.

This d i sc repancy could have been caused by i n t e r n a l contaminat ion

i n t h e scrubber and p ip ing l ead ing t o t h e sc rubber .

The o f f - g a s sc rubber was i n a d v e r t e n t l y s t a r t e d wi th 0.44M - NaOH i n s t e a d of t he u s u a l 2M - NaOH. The sc rubber became neu-

t r a l i z e d a f t e r 30% of t h e f eed had been f e d t o t h e s o l i d i f i e r

a t which time t h e accumulation r a t e of n i t r o g e n dropped o f f

r a p i d l y u n t i l a t about 60% feed f e d no more n i t r o g e n accumulated.

F igure 5.5 shows d a t a from t h e a u x i l i a r y sc rubber ope ra t i on . A

t o t a l of 15% of t h e n i t r o g e n f e d t o t h e s o l i d i f i e r accumulated

i n t h e scrubber . Using t h e i n i t i a l n i t r o g e n accumulation r a t e

0 1 0 3 0 5 0 7 0 9 0

% FEED FED TO S O L I D I F I E R

FIGURE 5.5. Auxiliary Scrubber Operation

b e f o r e t h e s c rubbe r became n e u t r a l i z e d and e x t r a p o l a t i n g f o r

t h e e n t i r e run i n d i c a t e s t h a t about 30% of t he f eed n i t r o g e n

should have accumulated i n t h e s c rubbe r , There fore , about 15%

escaped wi th t h e sc rubber o f f - gas .

The f i n a l p rocess o f f - g a s l eav ing t h e sc rubber con ta ined - 8 3 a n average of 9.8 x 10 p ~ i / c r n ~ of Ru-106 and 1.5 x pCi/cm

of CePr-144. These va lues were above 10CFR20 r e l e a s e l i m i t s

by f a c t o r s of 4.9 x 1 0 ' f o r Ru-106 and 3.8 x 1 0 ' f o r CePr-144.

However, a f t e r t h e sc rubber o f f - g a s was f i l t e r e d twice more and

combined w i t h b u i l d i n g v e n t i l a t i o n a i r , t h e r a d i o a c t i v i t y

r e l e a s e d w i th t h e o f f - g a s t o t h e s t a c k was w e l l below 1 0 C F R 2 0

r e l e a s e l i m i t s .

Spray Solidification Run SS-12(IPM) - W, R. Bond

Run SS-12(IPM) was successfully completed using the in-pot

melting technique wherein spray calcined PW-4m waste was

melted with a borosilicate glass frit directly in the final

storage container. The WSEP spray calciner had been coupled

directly to the receiver pot for this run via a special spool-

piece, and the solid frit was added directly to the pot via a

solids feeder attached to the spool piece.

During Run SS-12(IPM), a simulated waste equivalent to that

resulting from the reprocessing of 0.54 tonne of power reactor

fuel (45,000 MWd/tonne at 30 MW/tonne) with an equivalent aging

time of 1.3 years was processed to produce 162 kg of product.

The 54 liters of radioactive solid produced a heat rate density

of 89 W/liter (4900 W total based on analytical data and 4800 W total based on pot calorimetry) in an 8-in. diameter 304L

stainless steel melt receiver. The steady-state pot centerline

temperature in the air-cooled furnace was 474 "C, and the

centerline-to-wall temperature difference was 197 OC. These

values indicate an effective thermal conductivity of

1.12 ~/(rn~)(OC/m) [0.65 Btu/(hr)(ft2)(OF/ft)] for the product.

The effective thermal conductivity of the product while molten

during processing was approximately 3 to 4 times higher than

this and consequently pot centerline temperatures did not

exceed 980 OC despite pot wall temperatures of 900 to 950 OC,

The calciner was fed 301 liters of adjusted PW-4m feed

(additives of 0.65M - Ca(N03)2 and 0.5M - Zn(NOj)2 based on 378

liters/tonne) at 556 liters/tonne in 28 hr. The resulting

calcine was combined with 109 kg of borosilicate glass frit in

the receiver pot, The feed containing 1,380,000 Ci of

radioactivity including 6800 Ci of radioactive ruthenium was

reduced in volume by a factor of 5.6, or 3 . 8 on a 378

liters/tonne basis, A summary of run data for SS-12 is pre- sented in Table 5.11 and the feed composition for the run is

given in Table 5.12.

TABLE 5.11. Summary Data for WSEP Spray Solidification Run SS-12 (IPM)

Operational - Data

Date

Operating Mode

Feed Type

Feed, liters/tonne

Total Feed to Solidifier, liters

Total Feed Time, hr

Average Feed Rate, liters/hr 10.8

Equivalent Waste To Solidifier, tonne 0 . 5 4

Volume' Reduction, Feed Volume/Product Volume 5.6

Volume Reduction if Feed were at 378 liters/tonne 3 .8

Filled Pot Data

Total Curies in Feed to Pct

Total Curies of Ru in Feed to Solidifier

Froduct in Pot, liters

Product in Pot, liters/tonne

Heat Generation Rate in Pot, I$

Equivalent Aging Time, years

Temperature in "Air-Cooled" Furnace, OC

5 to Wall Temperature Difference, "C Effective Thermal Conductivity of Product in

an Air-Cool.ed Furnace, W / (rr.2) (OC/n!)

a . T h i s i s 1 5 % h i g h e r t h a n d e s i r e d , due t o t h e a d d i t i o n o f e x t r a b o r o s i l i c a t e f l u x t o compensa t e f o r e x c e s s s o d i u m and a luminum i n t h e f e e d .

TABLE 5.12. PW-4m Feed Composition for Spray Solidification Run SS-12 (IPM)

Component

H+

~ e *

cr+

~ i * ~

A I + ~

Na+

Concentration, M ~ ~ ) - - -

so;' - - - - 2

MOO;' + TC as MOO^ 0.161

~ r + ~ 0.036

~a+' 0.041

~ b + + CS+ (added K + ) 0.092

(Y + RE)+^ 0.325(~)

R U + ~

R U + ~ (added ~1'~)

~ h " (added CO+') 0.013

~ d + ~ (added ~ i + ~ ) 0.043

Ag+' (added CU+') 0.0016

cd" (added CU+') 0.0025

Additive to Feed

ca+'

Additive to Pot

Borosilicate glass frit

a . M o l a r i t i e s a re a t 378 l i t e r s / t o n n e . b . The nomirral k l c o n c e n t r a t i o n i s 0.001g, however e x c e s s A Z

was p r e s e z t i n t h e was t e f r o v t h e p ~ c c e s s i n g p l a n t used t o s i m u l a t e t h e PW-4m f e e d .

c. The nominal Na c o n c e n t r a t i o n i s 0 . I b l , however 0.322M Na was added a s Na2MoO4 and t h e remain ing e x c e s s r e s u l t e d from t h e p roces s ing p l a n t w a s t e .

d . Does n o t i n c l u d e t h e 2.3M N O ; added w i t h t h e = d d i t i v e s . e . The nominal RE c o n c e n t r a t i o n i s 0.274M_, however e x c e s s

RE was p r e s e n t i n t h e p r o c e s s i n g p l a n t w a s t e . f. For t h e nominal PW-4g feed t h e b o r o s i l i c a t e f r i t r e q u i r e -

ment i s 478 g / l i t e r , however e x t r a f r i t was added t o compensate f o r e x c e s s Na and A1 i n t h e f e ed .

During t h e f i r s t 4 h r of Run SS-12(IPM) t h e sp ray c a l c i n e r

average feed r a t e was approximately 15 l i t e r s / h r , and t h e i n- po t

mel t ing process e a s i l y kep t up wi th t h e c a l c i n e r a t a me l t

forming r a t e of approximately 2 .7 l i t e r s / h r . The normal mel t

forming c a p a c i t y f o r an 8- in . d iameter po t i s expected t o

exceed 3 l i t e r s l h r based on co ld development runs o r more t han

double t h e mel t forming c a p a c i t y of t h e 10- in . d iameter sp ray

and phosphate g l a s s m e l t e r s . During t h i s run however, t h e

sp ray c a l c i n e r c a p a c i t y was l i m i t e d f o r some unknown reason and

except f o r t h e f i r s t few hours of t h e run i t was n o t p o s s i b l e

t o exceed a f eed r a t e of 11 l i t e r s / h r (a mel t forming r a t e of

2.0 l i t e r s / h r ) wi thout producing a s i g n i f i c a n t drop i n t h e

c a l c i n e r i n t e r n a l t empera tures . Although poor f eed a tomiza t ion

would be suspec ted a s a cause f o r t h e reduced c a p a c i t y , t h e

atomizing a i r and f eed f low c o n t r o l were very s a t i s f a c t o r y

dur ing t he run. An i n s p e c t i o n of t h e f eed nozz le and t h e

i n t e r n a l s of t h e c a l c i n e r i s planned t o determine t h e cause of

t h e problem. A dec rease i n c a l c i n e r c a p a c i t y d i d n o t occur

w i th t h e same type f eed dur ing co ld development sp ray c a l c i n e

runs .

The sp ray c a l c i n e r f eed was i n t e r r u p t e d twice du r ing Run

SS-12(IPM) f o r a t o t a l of 4.4 h r . The f i r s t shutdown was

made t o enab le an e v a l u a t i o n of why t h e c a l c i n e r c a p a c i t y was

l i m i t e d , and t h e second was made whi le a f a i l e d c a l c i n e r v i b r a t o r

was r ep l aced . The performance of t h e spray c a l c i n e r o f f - g a s

f i l t e r s was very s a t i s f a c t o r y dur ing t h e run a s t h e f i l t e r p r e s -

s u r e drop was main ta ined a t 3.3 i n , of water and only 0 . 0 1 4 %

of t h e p a r t i c u l a t e s were e n t r a i n e d from t h e c a l c i n e r .

Ruthenium v o l a t i l i z a t i o n from t h e s o l i d i f i e r dur ing

SS-12(IPM) was only 1 .9% of t h e ruthenium i n t h e f e e d t o t h e

s o l i d i f i e r . This compares wi th p rev ious spray runs where

40 t o 7 5 % of t h e ruthenium was v o l a t i l i z e d , The dec rease dur ing

t h i s run was a n t i c i p a t e d from t h e r e s u l t s of co ld development 1 runs and is exp la ined by t h e absence of phosphor ic a c i d i n t h e

f eed t o t h e sp ray c a l c i n e r ,

H I G H - L E V E L WASTES F R O M A D V A N C E D R E P R O C E S S I N G T E C H N I Q U E S

K. J. S c h n e i d e r

A review of advancements i n f u e l r ep roces s ing technology

was made t o determine t h e e f f e c t s of l i k e l y changes on t h e com-

p o s i t i o n s of h i g h - l e v e l wastes i n t h e Waste S o l i d i f i c a t i o n

Demonstrat ion Program. I t was concluded t h a t a l l known near -

f u t u r e changes i n waste composit ions have been inc luded i n t h e

e x i s t i n g waste program, Wastes from aqueous r ep roces s ing of

LWR f u e l s a r e b racke ted by t h e r e f e r e n c e WSEP composit ions PW-1,

PW-2, and PW-4m. Wastes from aqueous r ep roces s ing of LMFBR f u e l s

a r e b racke ted by t h e above r e f e r e n c e composit ion p l u s t h e

r e f e r e n c e LMFBR composit ion, For e i t h e r LWR o r LMFBR f u e l s non-

aqueous r ep roces s ing techniques which s i g n i f i c a n t l y change t h e

waste composit ion a r e no t y e t w e l l enough de f ined t o do major

s t u d i e s on t he h i g h - l e v e l waste. A d i s c u s s i o n of t h e a n t i c i p a t e d

changes i n h i g h- l e v e l wastes from rep roces s ing of LMFBR f u e l s

i s p re sen t ed below,

The h ighe r f u e l exposure and s p e c i f i c power and t h e use of

plutonium enrichment r a t h e r t han Uranium-235 i n t h e c o r e f u e l

of LMFBR1s w i l l r e s u l t i n h ighe r f i s s i o n product c o n t e n t s and

h e a t gene ra t i on r a t e s , and i n a d i f f e r e n t d i s t r i b u t i o n of

f i s s i o n produc ts i n t h e waste , These d i f f e r e n c e s w i l l be h i g h l y

dependent upon t h e r e a c t o r de s ign , and u l t i m a t e l y upon f u t u r e

d e c i s i o n s r e l a t i n g t o t h e p roces s ing of b l a n k e t f u e l wi th o r

wi thout c o r e f u e l , The importance of t h e s e i tems can be b e s t

i l l u s t r a t e d by Table 5-13 which p r e s e n t s concep tua l f a s t r e a c t o r

c h a r a c t e r i s t i c s ,

TABLE 5.13. Summary of Conceptual LMFBR Characteristics (a)

E q u i l i b r i u m R e f u e l i n g R a t e , E q u i l i b r i u m Burnup , MT/yr f o r e a c h 1000 MWe R e a c t o r

MWd/MT P r o d u c i n g 310,000 MWde/yr A x i a l R a d i a l A x i a l R a d i a l

LMFBR Type Core B l a n k e t B l a n k e t ~ v e r a ~ e ( b ) C o r e B l a n k e t B l a n k e t

R e f e r e n c e Oxide 80 ,000 2 ,500 8 , 1 0 0 33 ,000 8 .497 4 .952 1 C . 04

Advanced o x i d e ( c ) 96 ,500 2 ,500 6 , 0 0 0 35,600 6 .764 5 . 5 35 7 .845

Advanced Oxide 97 ,500 2 ,800 5 ,700 26 ,600 6 .289 5 . 8 9 3 14 .659

Advanced 104 ,500 8 ,700 9 , 0 0 0 4 1 , 7 0 0 6 . 1 3 1 6 . 8 8 4 4 . 7 9 8

C a r b i d e 79,500 3 ,000 3 ,800 1 9 , 6 0 0 8 . 9 7 3 5 . 6 1 1 3 .169

Advanced C a r b i d e 110 ,300 5 , 9 0 0 8 , 3 0 0 47 ,300 6 .455 2 .670 7 .591

a . Data from WASH- 1 0 9 9 , " R e a c t o r Fue Z C y c l e C o s t s f o r N u c l e a r Power E v a l u a t i o n " , ( R e p o r t o f t h e Fue l R e c y c l e Task F o r c e ) , D r a f t I I .

b . W e i g h t e d a v e r a g e o f c o r e , a x i a l b l a n k e t and r a d i a l b l a n k e t . c . P o s i t i v e s o d i u m c o e f f i c i e n t . d . N e g a t i v e sod ium c o e f f i c i e n t . e . Data from G e n e r a l E l e c t r i c Company, " F a s t B r e e d e r R e a c t o r Fo l low- on S t u d y " , 1 9 6 9 .

The equ i l i b r ium burnup ( i n terms of t h e weighted average

of t h e c o r e f u e l , a x i a l b l a n k e t s , and r a d i a l b l a n k e t ) i s i n t h e

I range of p r o j e c t e d thermal r e a c t o r f u e l i n most ca se s , However,

t h i s equ i l i b r ium burnup is based upon the assumption t h a t t h e

r a d i a l b l a n k e t w i l l be mixed wi th t h e co re and a x i a l b l a n k e t

dur ing f u e l p rocess ing , This mode of o p e r a t i o n has n o t y e t

been demonstrated t o be t h e most economical, I t may be more

economical t o p rocess t h e r a d i a l b l anke t s e p a r a t e l y i n some

o t h e r manner, I n most c a s e s , t h e c o r e and a x i a l b l a n k e t s w i l l

be con ta ined i n t h e same f u e l p i n and w i l l be blended dur ing

process ing . I f t h e r a d i a l b l anke t i s p rocessed s e p a r a t e l y , t h e

equ i l i b r ium burnup w i l l be much h ighe r f o r t h e mixture of c o r e

f u e l and a x i a l b l anke t ,

I t must a l s o be s t r e s s e d t h a t t h e h e a t gene ra t i on r a t e w i l l

be h ighe r ( e s p e c i a l l y a t s h o r t coo l ing t imes) i n a mix ture of

f a s t r e a c t o r f u e l wi th a g iven equ i l i b r ium o r average burnup

than i n a thermal r e a c t o r f u e l wi th t h e same burnup. This d i f -

f e r ence occurs because, i n t he case of t h e mixed f a s t r e a c t o r

f u e l , most of t h e f i s s i o n produc t r a d i o a c t i v i t y is c o n t r i b u t e d

by t h e c o r e f u e l , The co re f u e l o p e r a t e s a t a much h ighe r

s p e c i f i c power t han thermal r e a c t o r f u e l and t h e p roduc t ion r a t e

and c o n c e n t r a t i o n of s h o r t - l i v e d f i s s i o n produc ts i n c r e a s e s a s

t h e s p e c i f i c power i n c r e a s e s .

The f i s s i o n product spectrum w i l l a l s o be d i f f e r e n t i n waste

from f a s t r e a c t o r f u e l p rocess ing . This d i f f e r e n c e i s due t o t h e

d i f f e r e n t i r r a d i a t i o n c o n d i t i o n s , t h e plutonium enrichment i n

t h e f u e l , and h ighe r neu t ron energy i n a f a s t r e a c t o r , For

example, t h e r e l a t i v e amounts of Ruthenium-106 w i l l be i nc rea sed

s e v e r a l - f o l d i n wastes from p roces s ing of f a s t r e a c t o r f u e l ,

The r e l a t i v e amounts of cadmium, t i n , antimony, se lenium, and

t e l l u r i u m i n t h e co re f u e l w i l l a l s o be i nc rea sed by f a c t o r s

up t o 3, Some of t h e s e l a t t e r f i s s i o n p roduc t s , no t ab ly

selenium, t e l l u r i u m , and antimony, t end t o be v o l a t i l e l i k e

ruthenium a t h igh tempera tures and could complicate was te

s o l i d i f i c a t i o n processes .

Table 5,13 shows t h a t t h e burnup of t h e c o r e f u e l i n t h e

concep tua l "advanced" r e a c t o r s i s h ighe r than i n t he r e f e r e n c e

r e a c t o r s , Thus, t h e h ighe r burnups, t h e h ighe r s p e c i f i c power

i n f a s t r e a c t o r c o r e f u e l , t h e d i f f e r e n t spectrum of f i s s i o n

produc ts i n t h e f u e l , and t h e p o s s i b i l i t y t h a t t h e r a d i a l

b l a n k e t w i l l be p rocessed s e p a r a t e l y r e q u i r e e v a l u a t i o n i n

s o l i d i f i c a t i o n s t u d i e s w i th f a s t r e a c t o r wastes .

The f u t u r e p o t e n t i a l of c a r b i d e- f u e l e d LMFBRs i s n o t

c l e a r a t t h i s t ime, Follow-on s t u d i e s of LMFBR concep tua l

de s igns have i n d i c a t e d a n t i c i p a t e d improved performance of

ox ide- fue l ed r e a c t o r s compared t o c a r b i d e - f u e l e d r e a c t o r s ,

Consequently, s t u d i e s wi th h i g h- l e v e l wastes from c a r b i d e -

f u e l e d r e a c t o r s a r e b e l i e v e d t o be unnecessary u n t i l t h e

c a r b i d e - f u e l e d r e a c t o r s appear more promising.

I n t h e Waste S o l i d i f i c a t i o n Demonstrat ion Program, t h e

t o t a l f i s s i o n produc t c o n t e n t of wastes from LMFBRs, r a d i o-

a c t i v e p l u s non rad ioac t ive , was s e l e c t e d t o be r e p r e s e n t a t i v e

of a c o r e f u e l i r r a d i a t e d t o 100,000 MWd/tonne a t 200

MW/tonne. A chemica l ly c l e a n waste composit ion was s e l e c t e d

because such a composi t ion r e p r e s e n t s t h e "worst" case i n

terms of s t o r a g e tempera tures , f i s s i o n produc t c o n c e n t r a t i o n ,

and t h e amount of p o t e n t i a l l y v o l a t i l e f i s s i o n produc ts p e r

con ta ine r . The o t h e r r e f e r e n c e waste composit ions i n t h e

Waste S o l i d i f i c a t i o n Demonstrat ion Program a r e b e l i e v e d t o

b r a c k e t t he o t h e r c h a r a c t e r i s t i c s o f most c u r r e n t l y a n t i c i -

pa t ed h i g h- l e v e l waste composit ions from LMFBR1s .

P o t e n t i a l key non rad ioac t ive c o n s t i t u e n t s i n h i g h- l e v e l

wastes from rep roces s ing of LMFBR f u e l s t h a t may be p r e s e n t i n

l a r g e q u a n t i t i e s a r e i r o n , ( p r i m a r i l y from p a r t i a l d i s s o l u t i o n

of t h e s t a i n l e s s s t e e l c l add ing o r from t h e use of f e r r o u s i o n

a s a chemical reducing agen t ) and sodium (p r imar i l y from t r e a t -

ment of t h e o rgan ic s o l v e n t ) , The probable maximum amounts of

t h e s e c o n s t i t u e n t s i n combined wastes a r e shown i n Table 5-14

and a r e compared wi th a d j u s t e d LMFBR waste composit ions i n

WSEP demons t ra t ions ,

A s shown, t h e c o n c e n t r a t i o n of t h e key c o n s t i t u e n t s i n t h e

WSEP demonstra t ions w i t h LMFBR was tes , i n combination wi th t h e

t h r e e r e f e r e n c e LWR waste composit ions used i n t h e WSEP program,

b r a c k e t t h e a n t i c i p a t e d range of h i g h - l e v e l waste composi t ions ,

even when combined wi th o t h e r f u e l r ep roces s ing was tes , I n v e s t i -

g a t i o n of t h e o t h e r primary d i f f e r e n c e s i n wastes from LMFBR

f u e l r ep roces s ing (namely t h e h ighe r c o n t e n t of f i s s i o n pro-

d u c t s , t h e l a r g e r amounts of p o t e n t i a l l y v o l a t i l e f i s s i o n pro-

d u c t s , and t h e h ighe r l e v e l s of h e a t from f i s s i o n produc t ) have

been included i n t h e program s t u d i e s .

E V A L U A T I O N O F S O L I D I F I E D W A S T E P R O D U C T S

N O N R A D I O A C T I V E L A B O R A T O R Y S T U D I E S

Melt See reea t ion S tud i e s of Simulated S o l i d i f i e d Wastes S tored

a t High Temperatures f o r Extended Per iods - C . Hampton

A s tudy of t h e behavior of s imula ted WSEP mel t s when s t o r e d

a t t empera tures up t o 950 O C was conducted. Simulated phosphate

g l a s s and spray s o l i d i f i e r PW-1, PW-2, PW-4m, and LMFBR mel t s

were used i n t h e s tudy.

The s o l i d i f i e d wastes were a l l mel ted a t 950 O C t o f a c i l i -

t a t e ea se i n handl ing. The r e s u l t i n g me l t s were then broken

i n t o p i e c e s . A weighed amount of mel t was p laced i n an alumina

c r u c i b l e and t h e weight of t h e e n t i r e assembly recorded. The

c r u c i b l e and sample were then p laced i n t h e s t o r a g e fu rnace and

TABLE 5.14. Key Constituents in High-Level Wastes from Reprocessing of LMFBR Fuels

l l y p o t h e t i c a l C o n c e n t r a t i o n a t 100 g a l W a s t e / t o n n e , M

U i s s o l u t i o n ~ l ~ h a ' ~ ) c o u n t e r ( a ) Probable" ) Maximum T o t a l i n WSEP of 10% Waste C leanup S c r u b b e r ~ a x i r n u m ' ~ ) Minimum T o t a l i n WSEP P h o s p h a t e

C o n s t i t u e n t C l a d d i n g blaximum Waste , Maximum Waste , Maximum T o t a l T o t a l Spray Kuns G l a s s Runs L : ~ + 3 1 .22 0 . 2 8 .--- - - - - 1 .50 0 . 1 2 . 2 6 0 . 9 3

F i s s i o n P r o d u c t s

a . The a m o u n t s s h o l ~ n o b t a i n e d from K. E . ULanco, Oak R i d g e N a t i o n a l L a b o r a t o r y , J a n u a r y , 1 9 7 0 .

b . A s s u m e s o n e c y c l e u s i n g amine s o l v e n t .

c . The a m o u n t s shown o b t a i n e d from G . L. R i c h a r d s o n , B a t t e l l e - N o r t h w e s t , November , 1 9 6 9 .

hea ted t o 950 O C and processed f o r approximately 1 h r . The

f i n a l temperature was t hen a d j u s t e d t o t h e s t o r a g e tempera ture

i n d i c a t e d i n Table 5.15. When s t o r a g e temperature was reached

(wi th in one day) t h e me l t s were mainta ined a t t h i s tempera-

t u r e f o r 8 weeks. A t t h e end of 8 weeks t h e samples were

cooled s lowly over a 2 t o 3 day p e r i o d by s lowly dec reas ing

t h e fu rnace temperature . A f t e r coo l ing , t h e c r u c i b l e s were

sawed i n h a l f and t h e mel t s i n spec t ed v i s u a l l y f o r phase

s e g r e g a t i o n and o t h e r p h y s i c a l changes. La t e r t h e samples

were analyzed f o r e lementa l s e g r e g a t i o n by comparing com-

p o s i t i o n of top and bottom phases . The s o l u b i l i t y of top

and bottom phases were a l s o checked,

The thermal s t a b i l i t y of phosphate g l a s s e s , wi th r e l a t i o n -

s h i p t o phase s e p a r a t i o n , i s s u p e r i o r t o t h a t of sp ray mel t s .

However, i n d i c a t i o n s a r e t h a t f o r long- term s t o r a g e t h e end

r e s u l t i s t h e same. The me l t s a l l showed phase s e p a r a t i o n o r

s e g r e g a t i o n a t 950 O C a f t e r 8 weeks s t o r a g e , comparable t o

t h a t shown i n F igure 5.6.

Spray s o l i d i f i e r me l t s a t t h e lower temperatures c f

750 "C and 850 " C appeared to b t unifcrm o r hoincgenz~us.

However, t h e 2hospliate g l a s s melt; sllowed phasc s e p a r a t i ~ n

a t 850 O C , No chemical a n a l y s i s a s y e t has been made on t h e

me l t s s t o r e d a t t h e s e lower t empera tures ,

The phosphate g l a s s PW-4m and sp ray s o l i d i f i e r PW-4m me l t s

s t o r e d a t 950 O C were chosen t o r e p r e s e n t phosphate g l a s s and

spray produc ts t h a t had been processed a t 950 O C f o r 8 weeks,

These samples were analyzed f o r cesium, ruthenium, s t ron t ium,

and r a r e e a r t h s . Samples were t aken from t h e top and bottom

l a y e r of each me l t t o compare e lementa l composit ion, The

fo l lowing r e s u l t s were ob t a ined and a r e compared wi th t h e

c a l c u l a t e d r e s u l t s from t h e o r i g i n a l e lementa l i n p u t a s

shown i n Table 5-16.

TABLE 5.15. Melt Storage Temperature and Melt Condition After 8 Weeks

Phosphate Glass Melts

PW- 1 PW-2 PW-4m LMFBR

Spray Solidifier Melts 750°C 850°C 950°C ---

PW-1 H H P S PW-2 H H P S PW-4m H H P S LMFBR ki H PS

H - Homogeneous.

FS - F a i n t phase s e p a r a t i o n .

PS - Phase s e p a r a t i o n v e r y d i s t i n c t .

TABLE 5-16. Chemical Analysis of Phosphate Glass and Spray Solidifier Melts Stored at 950 OC for 8 Weeks

Theoretical wt% of Melt

Phosphate Glass Spray Solidifier Element PW-4m Melt PW-4m Melt

C s 2.06 2.65

Ru 0.63 0.81

4 87.2 62 .O

Sr 0.62 0.79

Results of Analysis as ~ t % ( ~ )

Phosphate Glass PW-4m Melt Spray Solidifier PW-4m Melt Element Top Phase Bottom Phase Top Phase Bottom Phase

RE 7.0 as oxide

a . I t s h o u l d be n o t e d t h a t d i s s o l v i n g t h e p r o d u c t s f o r a n a l y s i s was a v e r y d i f f i c u l t p r o c e s s and i n c o m p l e t e s o l u t i o n may a c c o u n t f o r some o f t h e d e c r e p a n c i e s b e t w e e n t h e o r e t i c a l and a c t u a l w e i g h t p e r c e n t s .

I 1 /SMOOTH G L A S S

C R Y S T A L L I N E P H A S E W I T H T H E O F P A C K E D S A N D .

T H I S P H A S E C R U M B L E S E A S I L Y .

Phosphate Glass Melt Stored a t 950 O C

N E E D L E S OR F I B E R S

P A L E T O P P H A S E O F L I G H T COLOR N I T H F I B E R OR N E E D L E NETWORK

SMOOTt i C E R A M I C

Spray S o l i d i f i e r Melt Stored a t 9 5 0 OC

FIGURE 5.6, Typical Phase Separat ion of Phosphate G l a s s and Spray S o l i d i f i e r Melts Stored a t 950 OC

L e a c h a b i l i t y t e s t s were a l s o run on the phases and a r e

r epo r t ed i n Table 5,17,

TABLE 5.17. Leachability of Phosphate Glass and Spray Solidifier PW-Pm Melts Stored at 950 O C

for 8 Weeks

F i r s t Second Thi rd Spray S o l i d i f i e r Melt 2 4 h r 2 4 h r 2 4 h r To ta l

Top Phase 10.29% 0.59% 0.19% 11.07%

Bottom Phase 8 .22% 0.37% 0.10% 8.69%

Phosphate Glass Melt

Top Phase 0.35% 0.59% 0.93% 1.87%

Bottom Phase 0.62% 1 . 4 1 % 1 .61% 3.64%

PRODUCT MEASUREMENT, T E S T I N G AND STORAGE

S o l i d s S torage Engineer ing Tes t F a c i l i t y (SSETF)

R. J , Thompson

Table 5,18 shows t h e s o l i d i f i e d waste c c n t a i n e r s t h a t have

been t r a n s f e r r e d t o SSETF f o r environmental t e s t i n g . The waste

c o n t a i n e r from WSEP Run SS-10 was added t o t h e environmental

t e s t program du r ing t h i s r e p o r t pe r iod . The maximum c o n t a i n e r

t empera tures r e p o r t e d i n Table 5 - 1 8 a r e somewhat lower t han p r e -

v i o u s l y r e p o r t e d due t o a minor i n t e r r u p t i o n i n e l e c t r i c a l power

t o e x t e r n a l l y hea t ed po t s . The reduced temperatures a r e a s h o r t -

t ime even t and temperatures w i l l be r e s t o r e d t o t h e h ighe r l e v e l s .

The i r r e g u l a r temperature p r o f i l e s r e p o r t e d p r e v i o u s l y f o r

WSEP Run SS-8 waste c o n t a i n e r has been r e so lved . The p o t

thermocouples were r ep l aced and t h e i r r e g u l a r t empera ture

r ead ings e l imina t ed . While t h e waste c o n t a i n e r was o u t of t h e

environmental t e s t pod, c a r e f u l s i n g l e thermocouple t empera ture

scans were made of t h e i n t e rmed ia t e and c e n t e r l i n e thermowells ,

These scans s u b s t a n t i a t e d t h e f a c t t h a t temperature p r o f i l e

i r r e g u l a r i t i e s were due t o f a u l t y thermocouples.

TABLE 5-18, SSETF Environmental Test Summary (a)

Max imum Run Number D a t e ' I 'emperature " (1 P o t Number T e s t i n g Pod P o t

C u b i c l e Number S t a r t e d Envi ronment -- Pod Wall (i SS-4 9 / 1 1 / 6 9 Water 74 76 1 3 8 40 A - 2 1 - 3

1 0 / 1 / 6 9 Water 79 1 0 0 1 5 7

1 1 / 1 7 / 6 9 A i r 1 0 0 - - - 2 5 3

1 / 5 / 7 0 A i r 2 2 1 - - - 3 5 7

2 / 9 / 7 0 Water 2 4 29 1 7 6

a . T e m p e r a t u r e d a t a r e c o r d e d 4 - 1 4 - 7 0 .

6. H E A V Y S E C T I O N S T E E L T E C H N O L O G Y PROGRAM

I R R A D I A T I O N E F F E C T ON T H E F R A C T U R E O F H E A V Y S E C T I O N P R E S S U R E

V E S S E L S T E E L S - C . W . Hunter, J . A . Williams, a n d C. L . He l l e r i ch

Specimen I r r a d i a t i o n s

The i r r a d i a t i o n f a c i l i t i e s i n use o r under development

a r e t h e ETR M-3 h o t wate r loop f o r i r r a d i a t i o n of 1 - i n . - t h i c k

f r a c t u r e mechanics specimens (IT CT) and t h e ATR capsu le f o r

4T CT specimens. The i r r a d i a t i o n of specimens i n t h e ETR M-3

loop du r ing Cycles 1 0 1 through 104B have been p rev ious ly

d e s c r i b e d . The t e s t i n g of specimens from Cycle 101 i s

complete, a s i s t h e t e s t i n g of t e n s i l e specimens from

Cycle 102. Fa t igue p re - c racks a r e be ing prepared i n t he

1 T CT specimens from Cycles 1 0 2 and 103. The t e n s i l e and

f r a c t u r e specimens from 1 0 4 B a r e being r ead i ed f o r t e s t i n g .

I r r a d i a t i o n s i n t h e M-3 loop w i l l be commenced aga in w i t h

Cycle 108 i n June; t h e a n t i c i p a t e d c y c l e s through February 1971

a r e 108, 109A, 111, and 1 1 2 . Both t r a n s v e r s e (WR) o r i e n t a t i o n

base p l a t e and weldment w i l l be i r r a d i a t e d . Seve ra l of t h e

s i x t ubes con ta in ing t e n s i l e specimens w i l l be modified t o

accep t Charpy specimens.

The ATR - 4 T i r r a d i a t i o n f a c i l i t y w i l l occupy 1 0 r e f l e c t o r

p o s i t i o n s ON-3 through ON-12. S p e c i f i c s t u d i e s of t h e f a s t

neu t ron f l u x and gamma h e a t i n g i n t he se p o s i t i o n s have been

conducted r e c e n t l y . The gamma h e a t i n g va lues a r e l i s t e d i n

Table 6 .1 . P o s i t i o n s ON-3, O N - 4 , and ON-5 a r e a t t h e f r o n t

f a c e and h o t t e s t s i d e of t he specimen, whi le ON-9 i s a t t he

back f a c e . These va lues were measured w i t h g r a p h i t e a t a

r e a c t o r power of 1.65 MW and e x t r a p o l a t e d t o 250 MW. These

p r e s e n t va lues a r e deemed more accu ra t e t han t h e va lues p r e -

v i o u s l y r e p o r t e d . (3 ) These p rev ious va lues were from sup-

posedly s i m i l a r , b u t appa ren t ly no t i d e n t i c a l sou th r e f l e c t o r

p o s i t i o n s numbered 0 s - 3 through 0s -12 . These l a t e s t va lues

i n d i c a t e t h a t t he average gamma h e a t i n g w i l l be 0.30 W/g a t t he

f r o n t f a c e of t h e specimens and 0 . 1 5 a t t h e back f a c e . The

ana lyse s of t h e f a s t neu t ron f l u x i n P o s i t i o n ON-3 through

ON-12 have n o t y e t been completed.

TABLE 6 . 1 . Gamma Heat Genera t ion ( a ) i n S e l e c t Ref l e c t o r P o s i t i o n s t o be Occupied by t h e 4T Capsule i n t h e ATR

P o s i t i o n Above Core Bottom, i n .

9 1 5 2 1 2 7 33 3 9 45 51

O N- 3 w / g 0 . 2 1 0.26 0.26 0.26 0 . 2 4 0.19 0 . 1 2 0.07

a . De t e rmined w i t h g r a p h i t e a t 1 . 6 5 M W , ~ x t r a p o l a t e d t o 2 5 0 M W .

The gene ra l f e a t u r e s of t h e ATR - 4T capsu l e have been

p r e v i o u s l y d e s c r i b e d . (3) Two independent subcapsu les w i th two

specimens each w i l l be employed. The fou r specimens w i l l con-

s i s t of two t r a n s v e r s e (WR) o r i e n t a t i o n and one l o n g i t u d i n a l

( W ) o r i e n t a t i o n specimens of base m a t e r i a l and one weld-metal

specimen. The most c r i t i c a l f e a t u r e of t h e des ign w i l l be t o

main ta in t h e neces sa ry gas gap of approximately 0 .012- in .

between the specimens and the w a l l s of t he capsu l e , whi le

main ta in ing t h e c a p a b i l i t y t o w i th s t and a h y d r o s t a t i c f o r c e of

70,000 l b on t h e l a r g e r f a c e s of t h e capsu l e . To meet t h i s

requ i rement , t h e i n s i d e w a l l s of t he capsu le w i l l be r e l i e f

machined l eav ing smal l bea r ing pads d i s t r i b u t e d un i formly .

In a d d i t i o n t o main ta in ing t h e d e s i r e d ga.p spac ing , t he bea r ing

pads w i l l remove about t w o - t h i r d s o f t he h e a t gene ra t ed .

I r r a d i a t i o n i s scheduled t o commence ATR Cycle 5.

Base M a t e r i a l S t u d i e s of ASTM A533-B

The m a t e r i a l b e i n g s t u d i e d i s q u a r t e r t h rough c e n t e r

t h i c k n e s s l o c a t i o n s from t h e 1 2 - i n . ASTM A533 Grade B C l a s s

I HSST Program P l a t e 02 . P a s t and c u r r e n t e f f o r t s a r e c e n t e r e d

w i t h t h e f r a c t u r e o f RW o r i e n t a t i o n 1 T CT and t e n s i l e specimens 19 2

i r r a d i a t e d from 1 t o 8 x 10 n/cm (E > 1 MeV) a t 540 O F .

F u t u r e e f f o r t s w i l l be a t t h e same i r r a d i a t i o n c o n d i t i o n s b u t

w i l l a l s o i n c l u d e Charpy impact f r a c t u r e and 4T CT spec imens ,

and w i l l emphasize t h e WR o r i e n t a t i o n b e h a v i o r . The l o n g i -

t u d i n a l t e n s i l e spec imens i r r a d i a t e d a t 2 x 1019 and " 2 4 .4 x 10'' n/cm (E > 1 MeV) have been t e s t e d , a s have some of

t h e RW o r i e n t a t i o n 1 T CT spec imens a t 2 x 10'' n/cm2. E i g h t

s i m i l a r l y i r r a d i a t e d 1 T CT specimens a r e b e i n g f a t i g u e p r e -

c r a c k e d . T e s t i n g emphas is w i t h t h e s e w i l l be t o d e f i n e more

c l e a r l y b o t h t h e low- and h i g h - t e m p e r a t u r e p o r t i o n s o f t h e

KI , c u r v e .

The p r e v i o u s l y r e p o r t e d (3) f l u e n c e e f f e c t t e n s i l e r e s u l t s

h a s been r e p l o t t e d i n F i g u r e 6 . 1 t o i n d i c a t e t h e p e r c e n t a g e

i n c r e a s e i n p r o p e r t i e s a s a f u n c t i o n o f f l u e n c e . The room

t e m p e r a t u r e p r o p e r t i e s a r e more r e s p o n s i v e t o i n c r e a s e d f l u e n c e .

A l so t h e r e l a t i v e i n c r e a s e i n y i e l d s t r e n g t h i s g r e a t e r t h a n

t h a t o f u l t i m a t e s t r e n g t h and i t i s a l s o more r e s p o n s i v e t o

i n c r e a s e d f l u e n c e . T h i s b e h a v i o r r e d u c e s t h e margin between

y i e l d and r u p t u r e .

The c e n t e r p l a n e o f t h e 4T CT spec imens w i l l be 3.5 i n .

from t h e p l a t e s u r f a c e , which i s s l i g h t l y d e e p e r t h a n a 1 / 4 t

p o s i t i o n . N e v e r t h e l e s s , t h e r e w i l l s t i l l be abou t 0 . 5 - i n . of

h i g h e r s t r e n g t h and toughness m a t e r i a l on one s i d e o f t h e

spec imen.

Weldment S tudy of ASTM A533-B

The m a t e r i a l s b e i n g e v a l u a t e d a r e t h e 1 2 - i n . - t h i c k

A533 Grade B C l a s s I submerged a r c HSST weldment s e c t i o n s

FLUENCE, n / c m 2 ( E >1 MeV)

R ; Q U A R T E R T H I C K N E S S I R R A D I A T E D A T 510oF

- ,500'~

Y I E L D - STRENGTH

-

STRENGTH ' -

-

N e g 7 0 1 7 9 1 3 - 1

FIGURE 6 . 1 . HSST P l a t e 0 2 A 5 3 3 - B , C l a s s I

I I I l l I I I I I I l l

des igna t ed 51A and 54. The u t i l i z a t i o n of 1 T CT and double

c a n t i l e v e r beam (DCB) specimens t o determine t h e toughness -

p r o f i l e through Sec t ion 5 1 A has been p rev ious ly desc r ibed . (1,2)

The no tches of t h e CT specimens a r e p a r a l l e l t o t he weldment

l o c a t e d i n t h e f i v e fo l lowing a r e a s :

a t h e weld metal c e n t e r ,

t he w e l d - d i l u t i o n r eg ion on the we ld - s ide of t h e f u s i o n l i n e ,

a t h e r eg ion of a u s t e n i t i c g r a i n growth on the HAZ-side of

t he f u s i o n l i n e ,

a t h e c e n t e r of t h e HAZ, and

a t h e o u t e r boundary of t h e HAZ.

Nine specimens have been machined from each of t h e s e a r e a s and

f o u r specimens from each of t h e A , B , and C a r e a s have been 2 i r r a d i a t e d a t 540 O F t o 1 .5 t o 2.5 x 1 0 1 9 n/cm . Some p r c -

i r r a d i a t i o n f r a c t u r e thoughness p r o p e r t i e s i n a r e a s A , B , and

C a r e l i s t e d i n Table 6 .2 and compared wi th HSST base p l a t e

0 2 i n F igure 6 . 2 . The DCB toughness va lues f o r f r a c t u r e

pe rpend icu l a r through t h e weld metal compare f a v o r a b l y wi th

t h e 1 T CT r e s u l t s i n a r e a A . I t i s a l s o r e a d i l y apparen t t h a t

t h e t r a n s i t i o n temperature of t h e weldment i s lower than t h a t

of base p l a t e 0 2 .

Commencing wi th ETR Cycle 108, 4 a d d i t i o n a l 1 T CT s p e c i -

mens from a r e a A of weldment 5 1 A w i l l begin i r r a d i a t i o n a t 2 540 O F toward a f l uence of 8 x 1 0 1 9 n/cm . Beginning Cycle 111,

4 specimens from a r e a D of weldment 5 1 A w i l l be i r r a d i a t e d f o r 2 a f l uence of 1 .5 t o 2.5 x lo1' n/cm . One 4 T CT specimen from

a r e a A of weldment 54 w i l l be i r r a d i a t e d w i th t h e t h r e e base

p l a t e specimens i n t h e ATR-4T c a p s u l e .

S t r a i n Aging Embri t t lement

The i n t e n t of t h i s s tudy i s t o determine t h e d e l e t e r i o u s

e f f e c t s of i r r a d i a t i o n and thermal aging upon a v e s s e l which

has been s u b j e c t e d t o a p l a s t i c s t r a i n a t t h e r o o t s of c r a c k s ,

TABLE 6.2. Fracture Toughness of A533-B Submerged Arc HSST Weldment Section 51A, Determined with 1T CT Specimens Parallel to the Weldment

Crack Distance (a> Test Crack K K ~ c ( b l

Specimen From Fusion Temperature Length Load OF C a, in. l b

Q Identification Line, Mils ksidin. k s i K

Weld Metal Center, A

51A 5031 51A 5032 51A 5033 51A 5034

a 51A 5035

cn Weld Dilution Area, B

Area of y Grain Growth, C

a. The d i s t a n c e i n m i l s from t h e f u s i o n l i n e t o t h e c r a c k t i p i n a r e a s B and C . 2

b. V a l i d K l c v a l u e s per t h e c r i t e r i a : a , B 2 . 5 (K / o y s ) . Q

*

, *

Z

*2

5

aT

a A

0

WE

-

\ *

-w

\

am

+

\

+s

z

I\/ *

\ m

a=

- \

= -

\ W

0

3

\ @

= 2051

\ - m

-I

\ \ *

\ -

z Z

\

0- 0

\ * C3

'\ 0

t

3 w

\

-

LL

@=

\ Y

\ \

a

\ -

\ J

1

a

\

\ >

\O

\ Z

-

\ -

W

m

@=

o

a

a

W-

+~

z

+

fx 0

5

; 5

N O

Z 0

t

z z 2~

a

O-

~Z

E

-

+

cn 2

ZN

rn

O

W,

a

3 A

B n

IL

L 0

oo

a

m

4

0 z

n -

f l a w s , o r no t ches . The d e t a i l s of t h e s tudy and i t s r e l a t i o n

t o warm p r e s t r e s s i n g have been p r e v i o u s l y desc r ibed . Five

1 T CT specimens have been s t r a i n e d f o r 1 h r and 550 OF w i t h

s t r e s s i n t e n s i t y l e v e l s of 35,000 and 60,000 p s i d i n . These,

a long w i t h a s e r i e s of t e n s i l e specimens s t r a i n e d 1% and 10%

a t 100 OF, have been the rma l ly aged f o r 1000 h r a t 540 O F .

S i m i l a r l y s t r a i n e d t e n s i l e specimens have been i r r a d i a t e d a t 2 510 O F t o f l u e n c e l e v e l s from 1 . 5 t o 4 . 4 x 1 0 1 9 n/cm .

Fa t igue Crack P r e p a r a t i o n i n CT Specimens

I n l i n e a r e l a s t i c f r a c t u r e toughness d e t e r m i n a t i o n , t he

c r i t i c a l s t r e s s i n t e n s i t y (XI,) i s t h a t f o r f r a c t u r e i n i t i a t i o n

from a s h a r p f a t i g u e c r ack . Hence, t h e p r e p a r a t i o n of a f a t i g u e

c rack i n t h e f r a c t u r e specimens i s a neces sa ry p r e l i m i n a r y t o

a c t u a l tou.ghness de t e rmina t ions . Cons idera t ion of t h e l oad ing

c o n d i t i o n s dur ing such f a t i g u e c rack p r e p a r a t i o n p rov ides an

oppor tun i ty t o e x t r a c t some in fo rma t ion on f a t i g u e c r ack

behav io r . To be s u r e , t h e s e load ing cond i t i ons were n o t

in tended t o p rov ide pure p ropaga t ion d a t a , such a s t h e c r ack

growth r a t e pe r c y c l e (da/dn) ve r sus c y c l i c s t r e s s i n t e n s i t y

(AK) r e l a t i o n s h i p developed by P a r i s . ( 4 ) Neve r the l e s s , t h i s

i n fo rma t ion does o f f e r some examples of and i n s i g h t i n t o t h e

p r a c t i c a l s i t u a t i o n of c rack i n i t i a t i o n , s t a l l i n g , and

r e - i n i t i a t i o n , ( i ncuba t ion ) a s w e l l a s p ropaga t ion .

The d e t a i l s of t h e f a t i g u e c rack ing have been p r e v i o u s l y

d e s c r i b e d . (3) The e f f e c t i v e c r ack growth f o r i n i t i a t i o n

and p ropaga t ion i n t h e base m a t e r i a l and weldment approached

pure c r ack propaga t ion r a t e s , w i t h a d i s t i n c t p r o p e n s i t y f o r

h ind rance . The f a t i g u e c rack propaga t ion i n i r r a d i a t e d base

m a t e r i a l specimens has provided an oppor tun i ty f o r a cu r so ry

assessment of t h e i r r a d i a t i o n e f f e c t on f a t i g u e . The comparison

i n Table 6 . 3 i s sugges t i ve of a doubl ing of t h e e f f e c t i v e p r o -

paga t ion r a t e induced by i r r a d i a t i o n .

TABLE 6 . 3 . I r r a d i a t i o n I n f l u e n c e on t h e E f f e c t i v e F a t i g u e Crack E x t e n s i o n Behavior i n 1T CT Specimens o f ASTM A533-B from HSST P l a t e 0 2

Irradiated Unirradiated 1.5 to 2.5 x 1019n/cm2

Fatigue AK Crack Rate AK Crack Rate Step p s i K p s i =

1 26,100 26,060 (from machined

notch)

R e f e r e n c e s

1 . N u c l e a r S a f e t y Q u a r t e r l y P r o g r e s s R e p o r t , M a y , J u n e , J u l y 1 9 6 9 , BNWL- 1187 , pp. 6 . 1 - 6 . 2 0 . ~ a t t e Z l e - N o r t h w e s t , R i c h Z a n d , W a s h i n g t o n , S e p t e m b e r 1 9 6 9 .

2 . N? S e p t e m b e r , O c t o b e r 1 9 6 9 , BNWL- 1266 , p ~ 6 . 1 - 6 . 1 6 . B a t t e l Z e - ~ o r t h w e s t , R i c h Z a n d , W a s h i n g t o n , D e c e m b e r 1 9 6 9 .

3 . f l u c l e a r S a f e t y Q u a r t e r Zy P r o g r e s s R e p o r t , N o u e m b e 3 D e c e m b e r 1 9 6 9 , J a n u a r y 1 9 7 0 , B N W L - 2 3 1 5 - 1 , p p . 6 . 2 - 6 . 1 9 . B a t t e Z l e - N o r t h w e s t , R i c h l a n d , W a s h i n g t o n , M a r c h 1 9 7 0 .

4 . H . H . J o h n s o n a n d P . C . P a r i s . " S u b c r i t i c a l F l a w G r o w t h " , E n g i n e e r i n g F r a c t u r e ~ e c h a n i c s , v o l . 1 , n o . 1 , pp. 3 - 4 5 . 1 9 6 8 .

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J. M. Nielson R. E. Nightingale D. P. OIKeefe H. M. Parker D. W. Pearce L. T. Pedersen H. N. Pederson A. M. Platt D. L. Reid R. L. Richardson 'd. D. Richmond G. J. Rogers (10) L. C. Schwendiman D. E. Simpson J. C. Spanner R. G. Wheeler J. A. WilLiams N. G. Wittenbrock D. C. Worlton Patent Section (2) Technical Information

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