1 serving the power industry problem solvedhps.ne.uiuc.edu/rets-remp/pastworkshops/2010/4 gel... ·...

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14C COMPOUNDS OF INTEREST

Organic Carbon Gases – primary form for PWRs14CH4 and other hydrocarbons

Inorganic Carbon Gases – primary form for BWRs14CO2, 14CO not formed in appreciable quantities

Particulate CarbonCarbonate, bicarbonate, incorporated in debris

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SAMPLE MATRICES

AirPotentially high moistureLimited oxygen at some locations% levels of hydrogen at some locations14C activities can vary by factor of 106 between locationsWide range of gas flow rates and pressure at sample locations

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ANALYTICAL PROTOCOL REQUIREMENTS

Differentiate between organic, inorganic, and particulate 14CAccommodate wide range of sample activitiesSeparate 14C from other interferencesHandle flammable, low oxygen atmospheresEmploy practical sample times and gas volumes

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ANALYTICAL PROTOCOL REQUIREMENTS

Accommodate differences in sample flow, sample pressureAdaptable to differences in process interface hardwareEmploy hardware that can be reliably and conveniently transported to and returned from facilities

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PRIOR STUDIES

Thompson – 1978Combustion/mol sieve/cryo-trap/LSC

Kunz – 1985Combustion/Ascarite/cryo-trap/gas proportional counter

IAEA – 2004Review including combustion/NaOH soln/LSC

Magnusson – 2008Combustion/NaOH soln/LSC

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SAMPLE COLLECTION SYSTEM

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CHEMICAL REACTIONS

CO2 AdsorptionCO2 + 2NaOH Na2CO3 + H2ONa2CO3 + CO2 + H2O 2NaHCO3

CO2 DesorptionNaHCO3 + HNO3 NaNO3 + H2CO3

H2CO3 H2O + CO2

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CHEMICAL REACTIONS

CombustionCH4 + 2O2 CO2 + 2H2O

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METHANE COMBUSTION EFFICIENCY 2 LPM

0

10

20

30

40

50

60

70

0 200 400 600 800 1000 1200

Temperature F

Met

hane

Con

cent

ratio

n pp

mv

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CO2 ADSORPTION EFFICIENCY 1LPM

0

50

100

150

200

250

300

350

400

450

0 50 100 150 200 250 300 350 400

Minutes

CO

2 C

once

ntra

tion

ppm

v

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14C LABORATORY DISTILLATION APPARATUS

Air Flow Inlet

To Vacuum

Condenser

Digestion Flask: Solid Sorbent

Tritium Trap (HCl)

CO2 trap

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VALIDATION OF SAMPLE ANALYSIS PROTOCOL

Method Blank0.042 pCi/L (4.2 x10-11 uCi/ml)Based on a 2 hour sample at 300 ml/min gas sample flow rate

LCS95.1 +/- 3% for spike equivalent to 2.0 pCi/L (2x10-9 uCi/ml) (total volume sampled=3.6 x104ml)

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VALIDATION OF SAMPLE COLLECTION AND ANALYSIS PROTOCOL

14C

14C

14C

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VALIDATION OF SAMPLE COLLECTION AND ANALYSIS PROTOCOL

71.71 99%71.71 97%71.71 92%71.71 94%71.71 95%71.71 91%71.71 96%71.71 96%71.71 98%71.71 91%

Average 95%

Nominal(pCi/sample)

LCS Recovery%

LCS(spiked into flask w/ascarite)

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VALIDATION OF SAMPLE COLLECTION AND ANALYSIS PROTOCOL

10486.49 83%10486.49 85%10486.49 82%

71.71 85%71.71 85%71.71 85%717.08 90%

Average 86%

Nominal(pCi/sample)

LCS Recovery%

Wet DigestionWet Digestion of standard to produce 14CO2

in sample gas stream

71.71 99%71.71 91%71.71 94%717.08 92%717.08 91%

Average 93%

Wet Digestion of standard followed by combustion to produce 14CO2 in sample gas

stream

Wet Digestion/Combustion

Nominal(pCi/sample)

LCS Recovery%

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SAMPLE COLLECTION HARDWARE

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SAMPLE COLLECTION HARDWARE

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EQUIPMENT AND SAMPLE SHIPPING

Sample box – limited quantity radioactive materialSample tubes – contain sodium hydroxide (a hazardous material), excepted quantity

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EQUIPMENT PERFORMANCE PARAMETERS

Carbon to CO2 Conversion Efficiency>95%CO2 Capture Efficiency>95%14C Measurement Range (to Date) <7x10-11 to 5x10-3 uCi/mlSample Rate (typical, other sample rates can be used) 0.1 - 3 liters per minutePower Requirements120V 20 ampSample Collection Interface uses an interface adaptor that can appropriately extract sample gas from plant systems under a wide range of plant gas flow and pressure conditions