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Original Article Inuence of hydrogen concentration on burst parameters of Zircaloy-4 cladding tube under simulated loss-of-coolant accident Siddharth Suman Department of Mechanical Engineering, Indian Institute of Technology Patna, Patna, 801 103, India article info Article history: Received 3 January 2020 Received in revised form 13 February 2020 Accepted 14 February 2020 Available online 15 February 2020 Keywords: Hydride Burst criterion LOCA Rupture Zircaloy-4 Cladding abstract Single-tube burst tests on hydrogenated Zircaloy-4 nuclear fuel cladding under simulated loss-of-coolant accident are conducted to evaluate the impact of hydrogen on burst parameters. The heating rate and initial pressure are varied from 5 K/s to 150 K/s and 5 bare80 bar, respectively. The hydrogen concen- tration in the cladding is in the range of 0e2000 wppm. Burst stress is lower for hydrogenated cladding in a-phase. A signicant loss of ductility is observed in a-phase and lower a þ b-phase for hydrogenated cladding. However, the burst strain is higher for hydrogenated cladding in b-phase. There is a sigmoidal dependency of rupture area with initial stress and rupture area is larger for hydrogenated cladding. A novel burst stress correlation for hydrogenated Zircaloy-4 cladding has been proposed. © 2020 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). 1. Introduction Zircaloy-4 is used as a nuclear fuel cladding in water reactors. Zirconium transforms from the hexagonal close-packed a-phase to the body centered cubic b-phase at 865 C and atmospheric pres- sure. However, the alloying elements that convert zirconium to Zircaloy-4 alters the transformation temperature as well as intro- duce a temperature region of about 150 C in which the a and b phases coexist [1]. Zircaloy-4 fuel cladding undergoes water-side corrosion during service and as a result hydrogen is produced [2,3]. Zr þ 2H 2 O / Zr O 2 þ 4H (1a) 4H þ 2Zr / 2Zr H 2 (1b) A fraction of hydrogen diffuses into Zircaloy-4 since hydrogen is more stable as solution in the a-phase of zirconium alloy matrix than in gaseous form. Hydrogen in solution in the a-zirconium lattice occupies the tetrahedral interstices in the hexagonal a-zir- conium unit cell. The hydrogen in solid solution form in the a-zir- conium matrix is highly mobile at nuclear reactor operating conditions, it migrates down both the concentration and the tem- perature gradients while migrates up a stress gradient [4e6]. The diffused hydrogen precipitates and forms brittle zirconium hydride phase after exceeding a limiting concentration for the given con- ditions of temperature and hydrogen pressure. It is well established that precipitation of hydride alters the critical properties of fuel cladding like dimensional stability, mechanical strength, corrosion, and creep behaviour of the cladding [7]. During normal operation of the reactor, cladding tube is sub- jected to temperatures in the range of 290e350 C and a compressive hoop stress of 40e80 MPa because of pressurised coolant overpressure. The cladding tube is also internally pressur- ised with helium of the order of 2 MPa to improve thermal con- ductivity at the fuel pellet-cladding interface, and to reduce the probability of mechanical interaction between pellet and cladding during service [8e10]. In a loss-of-coolant accident (LOCA), there is a decrease in the system pressure outside of the cladding and the heat transfer from the fuel. The decrease in the outside coolant pressure gives rise to hoop stress while decrease in the heat transfer rate causes a rapid increase in the temperature of the cladding. As a result, the creep deformation or ballooning of the fuel cladding occurs which may cause its bursting. Moreover, ballooning of the fuel cladding may result in a blockage of the coolant sub- channel that in turn may impair the fuel coolability [11]. The basic parameters controlling deformation of the cladding during the rst phase of loss-of-coolant accident (LOCA) are tensile hoop stress, temperature ramp, and creep strength. Single-tube E-mail address: [email protected]. Contents lists available at ScienceDirect Nuclear Engineering and Technology journal homepage: www.elsevier.com/locate/net https://doi.org/10.1016/j.net.2020.02.009 1738-5733/© 2020 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/ licenses/by-nc-nd/4.0/). Nuclear Engineering and Technology 52 (2020) 2047e2053

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Page 1: Influence of hydrogen concentration on burst parameters of … · phases coexist [1]. Zircaloy-4 fuel cladding undergoes water-side corrosion during service and as a result hydrogen

lable at ScienceDirect

Nuclear Engineering and Technology 52 (2020) 2047e2053

Contents lists avai

Nuclear Engineering and Technology

journal homepage: www.elsevier .com/locate/net

Original Article

Influence of hydrogen concentration on burst parameters of Zircaloy-4cladding tube under simulated loss-of-coolant accident

Siddharth SumanDepartment of Mechanical Engineering, Indian Institute of Technology Patna, Patna, 801 103, India

a r t i c l e i n f o

Article history:Received 3 January 2020Received in revised form13 February 2020Accepted 14 February 2020Available online 15 February 2020

Keywords:HydrideBurst criterionLOCARuptureZircaloy-4Cladding

E-mail address: [email protected].

https://doi.org/10.1016/j.net.2020.02.0091738-5733/© 2020 Korean Nuclear Society, Publishedlicenses/by-nc-nd/4.0/).

a b s t r a c t

Single-tube burst tests on hydrogenated Zircaloy-4 nuclear fuel cladding under simulated loss-of-coolantaccident are conducted to evaluate the impact of hydrogen on burst parameters. The heating rate andinitial pressure are varied from 5 K/s to 150 K/s and 5 bare80 bar, respectively. The hydrogen concen-tration in the cladding is in the range of 0e2000 wppm. Burst stress is lower for hydrogenated claddingin a-phase. A significant loss of ductility is observed in a-phase and lower a þ b-phase for hydrogenatedcladding. However, the burst strain is higher for hydrogenated cladding in b-phase. There is a sigmoidaldependency of rupture area with initial stress and rupture area is larger for hydrogenated cladding. Anovel burst stress correlation for hydrogenated Zircaloy-4 cladding has been proposed.© 2020 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the

CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction

Zircaloy-4 is used as a nuclear fuel cladding in water reactors.Zirconium transforms from the hexagonal close-packed a-phase tothe body centered cubic b-phase at 865 �C and atmospheric pres-sure. However, the alloying elements that convert zirconium toZircaloy-4 alters the transformation temperature as well as intro-duce a temperature region of about 150 �C in which the a and b

phases coexist [1]. Zircaloy-4 fuel cladding undergoes water-sidecorrosion during service and as a result hydrogen is produced [2,3].

Zr þ 2H2O/ Zr O2 þ 4H (1a)

4H þ 2Zr / 2Zr H2 (1b)

A fraction of hydrogen diffuses into Zircaloy-4 since hydrogen ismore stable as solution in the a-phase of zirconium alloy matrixthan in gaseous form. Hydrogen in solution in the a-zirconiumlattice occupies the tetrahedral interstices in the hexagonal a-zir-conium unit cell. The hydrogen in solid solution form in the a-zir-conium matrix is highly mobile at nuclear reactor operatingconditions, it migrates down both the concentration and the tem-perature gradients while migrates up a stress gradient [4e6]. The

by Elsevier Korea LLC. This is an

diffused hydrogen precipitates and forms brittle zirconium hydridephase after exceeding a limiting concentration for the given con-ditions of temperature and hydrogen pressure. It is well establishedthat precipitation of hydride alters the critical properties of fuelcladding like dimensional stability, mechanical strength, corrosion,and creep behaviour of the cladding [7].

During normal operation of the reactor, cladding tube is sub-jected to temperatures in the range of 290e350 �C and acompressive hoop stress of 40e80 MPa because of pressurisedcoolant overpressure. The cladding tube is also internally pressur-ised with helium of the order of 2 MPa to improve thermal con-ductivity at the fuel pellet-cladding interface, and to reduce theprobability of mechanical interaction between pellet and claddingduring service [8e10]. In a loss-of-coolant accident (LOCA), there isa decrease in the system pressure outside of the cladding and theheat transfer from the fuel. The decrease in the outside coolantpressure gives rise to hoop stress while decrease in the heattransfer rate causes a rapid increase in the temperature of thecladding. As a result, the creep deformation or ballooning of the fuelcladding occurs whichmay cause its bursting. Moreover, ballooningof the fuel cladding may result in a blockage of the coolant sub-channel that in turn may impair the fuel coolability [11].

The basic parameters controlling deformation of the claddingduring the first phase of loss-of-coolant accident (LOCA) are tensilehoop stress, temperature ramp, and creep strength. Single-tube

open access article under the CC BY-NC-ND license (http://creativecommons.org/

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S. Suman / Nuclear Engineering and Technology 52 (2020) 2047e20532048

burst test performed outside of reactor constitutes the bulk of theavailable open literature and it has largely served to elucidate theeffects of these basic parameters on the burst behaviour of thecladding during LOCA as well as in the development of the burstcriterion. Swelling or ballooning of the cladding which eventuallyleads to bursting during LOCA is primarily a function of creepstrength which is influenced by the hydride precipitation. Inaddition, the presence of hydrogenda b-phase stabiliserdalsoshifts the phase transformation temperature of the Zircaloy clad-ding. Brachet et al. [12] investigated the influence of hydrogencontent on the phase transformation temperature using calorim-eter and burst behaviour using single-tube burst test approach. Thetests were performed on pre-hydrided Zircaloy-4 claddingswherein hydrogen concentrations ranged from 100 ppm to1000 ppm. It was reported that a/b phase transformation temper-ature decreases with the increase in hydrogen content as well ashydrogen decreases both creep strength and ductility of the ma-terial, the effect being greater for higher hydrogen content. Theypropounded that these results are not only due to the effect ofhydrogen on the a/b phase transformation shift but also by anintrinsic effect of hydrogen on the creep behaviour, especially in thea-phase and lower a þ b-phase temperature ranges. Thus, theyemphasised the need of a burst criterion incorporating the role ofhydride during LOCA for Zircaloy-4. Another important finding oftheir study was that deformation behaviour is mainly linked to thehydrogen uptake associated with the cladding oxidation, and thatthe irradiation defects anneal out and play no significant roleduring the first phase of LOCA. Kim et al. [13] studied the individualeffects of the surface oxide (20 mm and 50 mm thick) and theabsorbed hydrogen (300 ppm and 1000 ppm) on the behaviour ofZircaloy-4 cladding during LOCA. Their findings about the effects ofhydrogenwere similar to the findings of the Brachet et al. [12]. Thisinvestigation added that oxide layer also affected the high tem-perature ballooning behaviour by arresting the intra-granulardeformation of the a-grain up to 700 �C. Uetsuka et al. [14] con-ducted integral tests of rod-burst, oxidation and thermal-shockwith the objective of understanding the failure behaviour ofZircaloy-4 cladding during LOCA, especially during quenchingstage. Even though the primary focus of their study was to evaluatethe failure boundary of oxidation condition of the cladding duringquenching stage of LOCA, it was established that hydrogen absor-bed by the Zircaloy-4 cladding played a dominant role in the frac-ture and majority of the cladding failed at the location of themaximumhydrogen concentration. In their investigation, hydrogenwas picked up by the cladding during the oxidation process and,thus role of hydrogen could not be identified with distinctiveness.Nagase and Fuketa [15,16] in their two investigations similar to thestudy of Uetsuka et al. [14] used pre-hydrided Zircaloy-4 claddingtube to understand the exclusive role of hydrogen on its failurebearing capacity during LOCA. It was concluded that both rupturetemperature and circumferential burst strain decreased with anincrease in the initial hydrogen concentration. Moreover, fracturethreshold for the amount of oxidation was also reduced by an in-crease in the initial hydrogen concentration.

It is evident from the succinct literature review that there is noclear understanding about the effects of hydrogen on the defor-mation behaviour of Zircaloy cladding during the first phase ofLOCA. There has been no investigation reported in the open liter-ature except that of Brachet et al. [12] which emphasised the needof a new burst criterion incorporating the effects of hydrogen. In thepresent research work, an extensive single-clad burst test on pre-hydrided Zircaloy-4 fuel cladding, whose as-received compositionis provided in Table 1, has been conducted to understand the role ofhydrogen concentration on the burst behaviour during the firstphase of LOCA. In addition, burst correlation for as-received

Zircaloy-4 is also developed for the reference and developingdistinctive understanding about the role of hydrogen on burstparameters.

2. Experimental setup and procedure

This section describes the indigenously designed and developedclad burst facility. It has the following main components as shownin Fig. 1: clad heating setup, pressurisation setup, arrangement formaintaining inert atmosphere inside the burst chamber, tempera-ture and pressure measuring instruments, and high-speed dataacquisition system.

The burst chamber (1), a cuboidal enclosure having dimensions1.0 m � 0.5 m � 1.0 m, is mounted on heavy mild steel frame. Itsrear, top, and bottom sides are made up of 5 mm thick mild steelplate while other three sides are made up of 10 mm thick trans-parent acrylic plates. The heating arrangement for the clad spec-imen (2) at a required rate consists of 64 kVA rectifier (3) with acontrol unit (4) and a display unit (5). In order to avoid the devel-opment of axial stresses in clad specimen, copper clamps of thespecimen are connected to copper bus bars (6) by means of flexibleelectric cables (7) having high current carrying capacity. An argongas cylinder (8) is connected to the cladding specimen through acontrol valve for internal pressurisation. Once the clad tube isinternally pressurised at the desired pressure, the valve is closed. Inorder to conduct burst experiment in inert atmosphere, an addi-tional argon gas cylinder (9) is used to purge argon inside the burstenclosure through a perforated copper tube right under the clad-ding specimen. This ensures the presence of an inert atmospherenear the clad specimen. A vent is provided at the top of theenclosure to evacuate the air and excess argon. The temperaturefield of clad specimen is captured by thermal imaging camera (10).The online temperature and pressure data have been acquired withhigh speed data acquisition system (11). The burst video is recordedusing high speed camera (12). The data is stored in the computerusing LabVIEW 2017 program.

The experimental procedure involves three major activities,namely, specimen preparation, leak testing and the burst test. Thesample preparation requires: (a) charging the as-received claddingspecimen with desired hydrogen concentration (b) spot welding oftwo thermocouples at its outer surface and (c) fixing ferrule jointbetween the open end of clad specimen and pressurised gas con-necting line. The cladding specimen is hydrogenated using thegaseous hydrogen charging facility. This gaseous charging facility,based on a modified Sievert's apparatus, consists of a cylindricalglass chamber placed inside the furnace. The clad specimen isweighed and then placed inside the chamber. The glass chamber isevacuated to create a vacuum of the order 10�5 Pa. Subsequently,the specimen chamber is heated to the temperature of 363 �C.Depending upon the weight of the sample and target hydrogenconcentration, hydrogen is released into the specimen chamber upto a pre-computed pressure. The amount of hydrogen picked up bythe sample is calculated from difference between the initial and thefinal pressure readings recorded at ambient temperature. Two K-type thermocouples are spot welded on the outer surface of spec-imen before being installed in the enclosure for internal pressur-isation and heating. The specimen is connected to pressurising lineusing brass ferrule and nut-connector assembly. Pressure inside thecladding specimen is set to a desired value by operating the regu-lator mounted on argon cylinder. Once the required internal pres-sure is achieved, the gate valve present just before the cladding-pressurising junction is shut-off which disconnects the specimenfrom pressurising gas line. It ensures that even a small variation inthe internal pressure during heating of the cladding is recorded.The pressure transducer reading is monitored for at least of 300 s to

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Table 1Composition of Zircaloy-4 fuel cladding.

Name of alloy Alloy composition

tin iron chromium carbon oxygen hydrogen

Zircaloy-4 1.25 wt% 0.24 wt% 0.09 wt% 225 ppm 1100 ppm 12 ppm

Fig. 1. Description of the experimental setup.

Table 2Range of input parameters for the burst tests on Zircaloy-4 cladding.

Parameter Value Unit

Clad tube outer diameter 13.08 mmClad tube wall thickness, S0 0.41 mmClad tube total length 150 mmClad tube effective heating length 100 mmInternal overpressure, p0 5, 20, 40, 80 barHeating rate, h 4e150 K/sHydrogen concentration, Hc 0e2000 wppm

S. Suman / Nuclear Engineering and Technology 52 (2020) 2047e2053 2049

identify any leakage in the test section. Another hole on the rearwall right below cladding specimen is provided for purging argoninside the chamber using another argon gas cylinder. The gas ispurged into the chamber through a perforated copper tube. Theperforated tube is placed at a distance below the clad specimen. Theidea is to create an argon rich (inert) atmosphere around the cladspecimen. Moreover, perforated tube is positioned and flow rate ofargon gas is adjusted in such away that convection near heated cladspecimen remains as small as possible. The argon purging is initi-ated a fewminutes before the test. A vent is provided on chamber'sroof to facilitate the escape of air and excess argon. Thermal im-aging camera and high-speed camera are started. Rectifier isswitched ON and the required magnitude of direct current isapplied (to achieve a particular heating rate) to the claddingspecimen by operating control unit's knob. The temperature startsrising at a particular rate corresponding to the set current value.Cladding specimen undergoes ballooning leading to its burst as theclad attains a certain temperature. The burst video is recorded us-ing high speed camera at 5000 frames per second. Time, pressure,and temperature at the instant of burst are termed as burst time,burst pressure and burst temperature, respectively. Burst data isacquired and stored in computer using high speed data acquisitionsystem. Burst specimen is disassembled and high resolution imageis captured, especially of the burst location for further image pro-cessing. Then after the post-burst measurements of thickness and

circumference at burst location are performed. Finally, a small pieceis cut from the burst site and the hydrogen concentration at theburst location is determined using the LECO RH IE inert gas fusionanalyser. This procedure is repeated for each burst test.

The range of operating parameters has been provided in Table 2.The heating rate, internal overpressure, and hydrogen concentra-tion in the Zircaloy-4 cladding specimen are varied. Two tests areconducted for the identical set of input parameters, in other words,repeatability is kept as 2.

3. Results and discussion

Each cladding specimen is subjected to a given heating rate andinternal pressure. Both temperature and pressure increase during

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S. Suman / Nuclear Engineering and Technology 52 (2020) 2047e20532050

heating of the cladding specimen. The internal pressure rises due toheating and then there is a slight decrease in it due to increase involume caused by the ballooning of the cladding. Eventually clad-ding bursts and it is characterised by the sudden drop of internalpressure to zero. The instant at which this sudden drop in pressureoccurs is taken as burst time. The temperature and the internalpressure corresponding to this time is called burst temperature (TB)and burst pressure (pB), respectively. The burst hoop stress, andburst hoop strain are evaluated as described in Ref. [17].

3.1. Effects of internal pressure (p0) and heating rate (h)

While heating as well as during ballooning, the internal pres-sure of the cladding does not remain constant. Variations in pres-sure are non-linear given the simultaneous increase in temperatureand non-symmetrical increase in volume due to ballooning. Fig. 2shows the effects of heating rate (h) and internal pressure (p0) onrate of pressure rise (g) for as-received cladding with assumptionthat variations was linear. It is seen that rate of pressure increase ishigher for high internal pressure and high heating rate.

For low internal pressure or hoop stress, the burst happens athigher temperature corresponding to b-phase. With increase ininternal pressure, the burst temperature shifts towards lowertemperatures corresponding to a-phase of the Zircaloy-4 claddingas evident from post-burst pictures A and C in Fig. 3. The bursttemperature decreased to 936 K from 1177 K on increasing theinitial internal pressure from 2 MPa to 8 MPa. Fig. 4 shows therelationship of burst stress with burst temperature for both as-received and hydrogenated claddings at a heating rate of 5e10 K/s. The bursts stress is significantly lower for cladding hydrogenatedwith 450e600 wppm compared to as-received cladding in a-phase.This reduction in failure bearing stress is exhibited because ofhydrogen in the cladding and this reduction in burst stress is largerfor higher hydrogen contents. However, as burst temperature shiftsto mixed aþ b-phase regime the effects of hydride reduce and in b-phase the burst stress is similar to as-received cladding or higherthan as-received cladding. Similar observation of higher burststrength for hydrogenated cladding at higher burst temperatureswas also reported earlier by Brachet et al. [8].

Burst strain for as-received cladding attains a maxima in a-phase and dip sharply in mixed aþ b-phase regime given change in

Fig. 2. Rate of pressure rise for as-received cladding at different heating rates andinternal pressures.

material property due to phase transformation. For low internalpressure when burst temperatures start shifting towards highertemperatures, another peak in burst strain is observed, as shown inFig. 5. The burst strain for Zircaloy-4 cladding hydrogenated up to600 wppm, there is remarkable decrease in burst strain. This loss inductility is observed in a-phase and lower a þ b-phase whicheliminated the first maxima peak observed for as-received clad-ding. This reduction in ductility is more pronounced for higherhydrogen content. The burst strain decreased by 27% for 600 wppmwhile it was decreased by 63% for 2000 wppm compared to as-received cladding. For 2000 wppm, even the second maximapeak is eliminated and loss of ductility is observed up to the end ofa-phase to b-phase transformation. In b-phase, the hydrogenatedcladding shows more ductility compared to as-received cladding.At higher temperatures corresponding to b-phase, the more con-centration of hydrogen is in solid solution form rather thanprecipitated hydride. This hydrogen enhanced ductility may beattributed to the effects of hydrogen atmospheres and not ofprecipitated hydride which reduces ductility like in a-phase.Hydrogen atmospheres reduces the elastic interactions betweendislocations and other internal stress fields by a mechanism knownas elastic shielding and soften the material [18].

3.2. Rupture area

The burst opening area is evaluated using a java based opensource image processing program named ImageJ. The high res-olution image of cladding post-burst is taken against a standardscale and processed in the ImageJ to determine the burst openingarea, as shown in Fig. 6. Rupture area is critical for calculation ofhydrogen generation due to double side corrosion of the claddingas well as to estimate the amount of radioactive elements leakageinto the core. It is found that burst opening area of cladding isstrongly dependent on the initial pressure or stress in the clad-ding as plotted in Fig. 7. The relationship between initial pressureand opening area is of sigmoidal nature, it increases very sharplywhen pressure is raised from 0.5 MPa to 2 MPa but it saturatestowards 8 MPa. For hydrogenated cladding tested at higherpressure when burst happens in a-phase, the burst area issignificantly higher. It implicates the brittle tearing as may beseen from post-burst images C and D in Fig. 3. For identicalconditions, cladding hydrogenated to 1500 wppm has six timeshigher burst opening even though the burst strain is just 3% less.Dependence of burst area on the heating rate is not observedeither for as-received or hydrogenated cladding.

3.3. Burst stress correlations

One of the main objectives of the present extensive single-cladburst tests is to develop a burst stress correlation for hydrogenat-ed Zircaloy-4 cladding tube. Need of a different burst criterion forhydrogenated claddingdof which burst correlation is an integralpartdwas already emphasised in the work of Brachet et al. [12]. Ithas been already established that the burst stress is only a functionof burst temperature for the clad tube bursting in an inert envi-ronment [10,17,19e21] and it is given as:

sB ¼ a exp ð�b TBÞ (2)

where a and b are the experimentally determined material-dependent parameters. sB and TB are burst stress and burst tem-perature respectively. Nevertheless, these experimentally deter-mined parameters may be influenced by other operating variablessuch as the heating rate or test atmosphere like inert, air or steam[21].

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Fig. 3. Visual examination of the Zircaloy-4 cladding tubes after burst test at different conditions.

Fig. 4. Effects of hydrogen on burst stress of Zircaloy-4 cladding. Fig. 5. Effects of hydrogen on burst strain of Zircaloy-4 cladding.

S. Suman / Nuclear Engineering and Technology 52 (2020) 2047e2053 2051

Dependence of burst stress on burst temperature for as-receivedcladding obtained during the present investigation as well as fromstudy conducted on Zircaloy-4 having similar chemical composi-tion [17,19] is shown in Fig. 8. The value of material dependentconstants ‘a’ and ‘b’ are evaluated using the regression analyses onthe burst data. The values of these constants are phase dependent

and thus have different values in a-phase, a þ b-phase, and b-phase. For hydrogenated cladding tubes, the burst stress is found tobe dependent not only on burst temperature but also hydrogenconcentration. Thus, a new correlation incorporating the effect ofhydrogen concentration, in accordance with correlation given byErbacher et al. [20] for oxidized Zircaloy-4 cladding, is proposed as:

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Fig. 6. Evaluation of rupture opening area.

Fig. 7. Influence of hydrogen on rupture opening area of Zircaloy-4 cladding.

Fig. 8. Burst stress correlation for as-received Zircaloy-4 cladding.

Fig. 9. Burst stress correlation for hydrogenated Zircaloy-4 cladding.

S. Suman / Nuclear Engineering and Technology 52 (2020) 2047e20532052

sB ¼ a $ expð�b TBÞ $expð�c HcÞ (3)

where c is hydrogen influenced material parameters and Hc ishydrogen concertation in the cladding. The burst stress obtainedduring this study is plotted against burst temperature in Fig. 9 and

the material dependent parameters is again evaluated usingregression analyses. The burst correlation curves corresponding tolimiting range of hydrogen concentration, that is 0 ppm and2000 ppm, are also drawn in Fig. 9. Majority of data lies withinthese curves attesting the accuracy of the proposed correlation.There is too less data in mixed aþb-phase for hydrogenated clad-ding to form any conclusive understanding. However, the burstcharacteristics in a-phase and b-phase may be interpolated to formsome understanding about rupture behaviour of hydrogenatedZircaloy-4 cladding in mixed aþb-phase. Another noteworthyremark regarding the developed burst correlation for hydrogenatedcladding is that phase transformation of cladding influenced byhydrogen concentration is not considered and this may also influ-ence the burst parameters to a certain extent.

The burst correlations obtained for Zircaloy-4 cladding in thepresent research is provided in Table 3. Burst correlation obtainedby Erbacher et al. [20] based on oxygen concentration in Zircaloy-4cladding has also been included in Table 3 for the sake of com-parison and completeness since correlation for hydrogenatedcladding was proposed in accordance with this.

4. Conclusions

Single-clad burst tests are performed on both as-received andhydrogenated Zircaloy-4 fuel cladding under postulated first phaseof loss-of-coolant accident conditions. The as-received cladding ishydrogenated using gaseous hydrogen charging method and theconcentration of hydrogen in the Zircaloy-4 cladding specimens isin the range of 10 wppm to 2000 wppm. The heating rate is variedfrom 4 K/s to 150 K/s while initial internal overpressure is in therange of 5 bare80 bar. Following conclusions are drawn from thepresent burst investigation on both as-received and pre-hydridedZircaloy-4 cladding specimens:

� For as-received cladding specimens, burst strain is higher for theburst temperature falling in a-phase region, attains minima ina þ b-phase, and again increases in b-phase. The phase trans-formation of Zircaloy-4, from an anisotropic hexagonal close-packed a-phase to an isotropic body centered cubic b-phase,may be attributed for this behaviour.

� Hydrogenated Zircaloy-4 cladding exhibits reduced ductility inthe a-phase region, the effect being greater for high hydrogenconcentration.

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Table 3Burst stress correlations for Zircaloy-4 cladding in different environments.

Range of Parameters Correlation Phase Material dependent parameters

a b c

MPa K�1 ppm�1

As-received cladding in inert environmentHeating rate ¼ 4e150 K/sInitial hoop stress ¼ 5e150 MPa [present, 17, 19]

as-received: sB ¼ a $expð� b TBÞ a 1458 0.00218 e

a þ b 4.002 � 108 0.01375 e

b 733 0.00284 e

As-received cladding in steam environmentHeating rate ¼ 1e30 K/sInitial pressure ¼ 1e14 MPa [20]

oxidation:sB ¼ a $expð� b TBÞ $exp"�

�Ox� Ox00:00095

�2#

a 830 0.001 e

a þ b 3000 0.003 e

b 2300 0.003 e

Hydrogenated cladding in inert environmentHeating rate ¼ 4e150 K/sInitial hoop stress ¼ 4e150 MPaHydrogen concentration ¼ 0e2000 wppm [present]

hydrogenated: sB ¼ a $expð� b TBÞ $expð� c HcÞ a 9023 0.004227 0.0003805a þ b 33890 0.005665 0.0006223b 67 0.000809 0.0000683

S. Suman / Nuclear Engineering and Technology 52 (2020) 2047e2053 2053

� The increase of hydrogen content eliminates the minima ofburst strain observed in the mixed a þ b-phase for as-receivedcladdings.

� Influence of hydrogen concentration is significantly reduced inb-phase, and the burst strain value is comparable to that of as-received claddings.

� Burst opening area is strongly dependent on the initial stressirrespective of the hydrogen concentration in the Zircaloy-4cladding. For higher internal pressure, the burst area is largerfor hydrogenated cladding.

� Burst stress is sensitive to hydrogen concentration and a newburst correlation incorporating hydrogen concentration isproposed.

Declaration of competing interest

The authors declare that they have no known competingfinancial interests or personal relationships that could haveappeared to influence the work reported in this paper.

Acknowledgment

I sincerely acknowledge the Board of Research in Nuclear Sci-ences (BRNS), Government of India No. 36(2)/14/30/2014-BRNS/1665 for providing the financial support needed to carry out thepresent work. This work is a part of author's doctoral thesisdefended at Indian Institute of Technology Patna, India and su-pervisions of Dr. Khan and Dr. Pathak are acknowledged.

Appendix A. Supplementary data

Supplementary data to this article can be found online athttps://doi.org/10.1016/j.net.2020.02.009.

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