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MINOR ACTINIDE TRANSMUTATION FUELCYCLEAND MANAGEMENT IN GFR600 KEYWORDS:transmutation,gas- cooled fast reactor, nonuniform ZOLTÁN PERKÓ,a* JAN LEEN KLOOSTERMAN,a and minoractinidecontent SÁNDOR FEHÉRb aDelftUniversityofTechnology,DepartmentofRadiation,RadionuclidesandReactors Mekelweg15,Delft,Netherlands bBudapestUniversityofTechnology,InstituteofNuclearTechniques Mu˝egyetemrakpart3,Budapest,Hungary ReceivedSeptember24,2010 AcceptedforPublicationMarch10,2011 Within the Generation IV initiative, the gas-cooled than 3%. By feeding MAs as well (constant MA content fast reactor (GFR) is one of the reactors dedicated to strategy),thereactivityhasasteadyincreasefromcycle minor actinide (MA) transmutation. This paper summa- tocycle,predominantlydueto238Pubreedingfrom237Np. rizestheresearchperformedwiththeGFR600reference The effects of the isotopic composition of the pluto- designinordertoassessitsMAburningcapabilities.For nium and MAs were also examined by performing cal- the study, modules of the SCALE program system were culationswithdataspecifictothespentfueloftraditional used. western pressure water reactors and Russian type Single-cycleparametricstudieswereperformedwith VVER440 reactors. Despite the considerably different cores having different MA content and spatial distribu- MA vectors, no significant deviation was found in their tion. It was shown that the addition of MAs to the fuel overalltransmutation.However,thePucompositionhad greatlyreducedthereactivitylossduringburnup.More- astrongeffectonthereactivityandthedelayedneutron over,thehighertheMAcontentofthecore,thehigherthe fraction in the first cycles. fraction of it that was fissioned; however, the more the Finally, cores having nonuniform MA content were delayed neutron fraction and the fuel temperature coef- investigated.ItwasfoundthatthoughtheMAdestruction ficient degraded. Significant reduction can be achieved efficiency was significantly higher in the middle of the in the amounts of neptunium and americium, while cu- corethanattheedge,movingsomeoftheMAsfromthe rium isotopes accumulate. outer regions to the center resulted in only minor im- Thestudyofmultipleconsecutivecyclesshowedthat provement in their destruction. However, the spectral by adding only depleted uranium (DU) to the repro- changes caused by the rearrangement increased the cessedactinidesinfuelfabrication(pureDUfeedstrat- k-effective,whichallowedhigherburnupsandincreased egy),upto70%oftheinitiallyloadedMAscanbefissioned MA destruction. Unfortunately, some of the safety pa- inthefirstfivecycles.Moreover,thereactorcanbemade rameters of the reactor degraded. criticalduringthattimeiftheinitialMAcontentishigher I. INTRODUCTION prominentinsustainabilitybyhavingaclosedfuelcycle and a self-breeder core.1 In such a system all actinides In2002theGenerationIVinitiativedraftedthemost would be recovered from the spent nuclear fuel of the importantrequirementsthatfuturenuclearreactorsshould reactor during reprocessing, and they would be used in meet and embraced six reactor concepts that have the fuel fabrication for the same reactor; thus, only fission highestpotentialtodoso.Oneofthedesignsisthegas- products ~FPs! and actinides due to reprocessing losses cooled fast reactor ~GFR!, which is anticipated to be wouldbesenttothegeologicalrepositories.Atthesame time,onlyfertileisotopeswouldhavetobeaddedtothe *E-mail:[email protected] recovered actinides during fuel manufacturing because NUCLEARTECHNOLOGY VOL.177 JAN.2012 83 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 oftheefficientbreeding.Thesewouldobviouslyresultin II. MODELING GFR600 a significantly reduced spent fuel output and in a better use of fissile materials compared to today’s reactors. As a reference GFR, the CEA-designed “effective” TheGFRisalsoenvisionedtoplayanimportantrole GFR600conceptwaschosen,featuring600-MW~thermal! innuclearwastemanagement.Presentreactorsaremostly power, plate-type fuel, and high-pressure helium cool- operatedinanopenfuelcycleinwhichthespentfuelis ant. The exact details of the reactor are easy to find in notreprocessedandallactinidesendupaswastetogether mostrelevantarticles~seeRefs.3,7,and8forexample!; with the fission products. This is not only disadvanta- here, only the most important parameters are repeated. geousfromthewastemanagementbutalsofromthefuel The core consists of 112 fuel assemblies ~FAs! ar- economicspointofview,sinceononehandtheactinides rangedinsixringsaroundacentralpiece;theseannular increase the volume, heat load, and radioactivity of the regions are referred to as the six regions of the core nuclearwasteandrepresentitslong-termdanger;onthe @region 1 being the outermost, region 6 the innermost other hand, many fissile isotopes are discharged instead ring,plusthecentralpiece~coloredlightgreenandred! ofbeingreusedinthermalreactors.Hence,itisdesirable inFig.1,respectively#.Eachassemblyishexagonal,has toshifttoanuclearsystemwherethespentfuelisalways a120-degrotationalsymmetry,andcontains21fuelplates reprocessed, all actinides are recycled, and only fission in3compartments,eachhaving7parallelplatesfixedby productsaredisposedof~togetherwiththereprocessing theassemblywrapperandtheY-shapedcentralmechan- losses!. The reuse of uranium and plutonium is already ical restraint ~see Fig. 2!. The fuel concept is based on possibleasmixed-oxide~MOX!fuelinappropriatether- dispersed fuel—the ceramic actinide compound ~acti- mal reactors, but minor actinides ~MAs! are not usable nidecarbide,70V0V%a!isembeddedinaninertceramic today since they are not fissile in present commercial matrix~SiC,30V0V%!formingtheCERCERfuel.The reactors ~nor is it daily practice to recover and reuse structuralmaterialisalsoSiC~cladding,assemblywrap- plutonium from spent MOX fuel!. The situation is dif- per, etc.!, while the reflector is Zr Si . In the reference 3 2 ferent in fast reactors, where because of the increased fuel,theactinidecompoundismadeupby84n0n%bUC energyofneutronsallactinidesaremorefissionableand ~natural uranium! and 16 n0n% PuC ~legacy plutonium the buildup of heavier isotopes via capture is less prob- fromspentfuel!.Thesemainparametersaresummarized able. This leads to the idea of using them as actinide inTable I. burners in order to effectively destroy actinides gained It was investigated how MAs can be destroyed by byreprocessingthespentfuelofotherreactors.Themain adding them to the fuel. In these burnup calculations it focus is on the elimination of MAs ~neptunium, ameri- wassupposedthattheysubstitutesomeoftheuraniumin cium,andcurium!astheyrepresentsignificantheatload thefuel;hence,theactinidecompoundwaschosentobe andneutronsourceinthespentfuelandarenotthermally made up by 16 n0n% PuC, X n0n% MA carbide, and fissile. ~84-X! n0n% UC ~the exact composition in the nonuni- In the European GCFR-Specific Targeted Research formcaseisdetailedinSec.IV.B!.Toexaminetheeffects Program ~STREP!, an extensive study was done on the of the isotopic composition of the recycled plutonium MA transmutational capabilities of GFRs. The calcula- andMAs,twosetsofdatawereusedinourstudycorre- tionswerebasedonaone-dimensionalmodeloftheCEA- sponding to the spent fuel of western pressurized water designed “effective” GFR600 reactor concept. Among reactors ~PWRs! and Russian VVER440 reactors, re- otherissuesanalyzedwasthepotentialofburningMAs— spectively. The former composition is based on the stemmingfromlegacyspentfuel—bymixingthemuni- “Pu-2016”scenariostudyofCEAandrepresentstwice- formlytothefuel~forashortreview,seeRefs.2and3; recycled MOX fuel expected to be accessible in 2016 fordetails,seeRefs.4and5!.Tofinalizethiswork,afull ~Ref. 2!, while the latter is characteristic of 45 GWd0 three-dimensional ~3-D! model of the reactor was built tonneUburnupand5yearsofcooling~Ref.9!~theexact usingtheSCALEprogramsystem,6andadditionalburnup isotopiccompositionscanbeseeninTableII!.Intherest calculationswereperformedtoconfirmearlierresults,to ofthispaper,thesetwocompositionswillbereferredto analyze the effects of the isotopic composition of MAs as the PWR and theVVER cases, respectively. and plutonium, and to study the performance of cores having spatially nonuniform MAcontent. II.A. The KENO-VI Model of Reactor Thestructureofthispaperisasfollows.InSec.IIa shortintroductionisgiventotheGFR600design,andthe To study the actinide transmutational capabilities, modelsusedinthecalculationsarepresented.SectionIII theTRITON6 module10 of the SCALE program system details the effects of adding MAs uniformly to the fuel. was used that couples traditional SCALE modules to Section IV describes the transmutational capabilities of performautomaticburnupcalculation.Ateverytimestep, GFR600—in Sec. IV.A the results of single and multi- first resonance self-shielding was performed with the cycle uniform are presented, while in Sec IV.B those of nonuniformMAburningareinterpreted.SectionVcon- aVolumepercentage. tains a short summary of the results. bMolpercentage. 84 NUCLEARTECHNOLOGY VOL.177 JAN.2012 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 Fig.1. TheKENO-VImodelofGFR600~thevisualizationwasdonewithKENO3D!. the fuel inside the plates. Next, a transport calculation wasdonebytheKENO-VIMonteCarlocriticalitymod- ule, after which the KMART6 module collapsed fluxes and cross sections to the three-group format that the ORIGEN-Sburnupmodulerequirestodeterminethenew compositionofthefuel,subsequentlyfinishingthetime step. The computations were based on the 238-group ENDF0B-Vcross-section data library. TheKENO-VImodelfollowstheexactgeometryof thereactor~seeFig.1!.However,asnodetailedreflector concept had been designed for GFR600, both the axial and the radial reflectors were modeled as homogeneous mixtures of reflector, coolant, and structural material in correspondencewithearlierstudies.5Thecompositionof the reflectors can be seen inTable III. The temperatures of the fuel, the cladding, and the reflector are 9908C, 6658C, and 5658C, respectively. Burnup periods of 1300 effective full-power days were chosen corresponding to the planned 5% FIMAburnup Fig.2. TheNEWTmodeloftheFAsofGFR600. of the fuel. When studying consecutive cycles, cooling periodsof5yearswereinsertedbetweenthecampaigns ~i.e., burnup periods!. BONAMIandNITAWLmodules~intheunresolvedand Based on the results of the transport calculations, the resolved resonance regions, respectively!, applying certainquantitiesweredeterminedononehandtobetter the SYMMSLABCELLoption ~corresponding to an in- understandthechangeofreactivityduringburnupandon finite array of parallel fuel, cladding, and coolant slabs! the other hand to study the safety of the reactor. For the withfuel0cladding0coolantratiosof35%010%055%~in formerpurpose,theworthoftheisotopeswasintroduced accordancewiththeiractualvolumefractionsintheFA! ~see Sec. II.C!; for the latter, the fundamental delayed andsettingthewidthofthefuelslabequaltothewidthof neutron fraction was determined ~see Sec. II.D!. As a NUCLEARTECHNOLOGY VOL.177 JAN.2012 85 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 TABLE I MainCharacteristicsofGFR600 CoreParameters AssemblyParameters Thermalpower 600MW NumberofFAsincore 112 Powerdensity 103MW0m3 NumberofplatesperFA 21 Coreheight0diameter 1.95m01.95m Fuelcomposition~UPuC0SiC! 70030V0V% Coolantinlet0outlettemperature 4908C08508C Fueltemperature 9908C Coolantmaterial Helium Claddingmaterial SiC FuelParameters NaturalUComposition SiCdensity 3.21g0cm3 235Ufraction 0.7n0n% UPuCdensity 13.62g0cm3 238Ufraction 99.3n0n% Porosity 15% TABLE II TABLE III IsotopicCompositionofPWRandVVERSpentFuel* CompositionoftheReflectors PlutoniumVector MAVector AxialTop AxialBottom0 Reflector RadialReflector Fraction~n0n%! Fraction~n0n%! Material ~%! ~%! Isotope PWR VVER Isotope PWR VVER Hecoolant 40 20 238Pu 2.7 2.71 237Np 16.86 48.89 SiCstructure 10 10 239Pu 56 54.86 241Am 60.64 31.56 Zr3Si2reflector 50 70 240Pu 25.9 23.38 242mAm 0.23 0.11 241Pu 7.4 12.27 243Am 15.69 14.65 *Involumefractions. 242Pu 7.3 6.78 242Cm 0.02 0.001 241Am 0.7 0 243Cm 0.07 0.049 244Cm 5.14 4.43 245Cm 1.25 0.26 Therefore,asecondmodelofthereactorwasassem- 246Cm 0.1 0.05 bled for the FTC calculation. While building this new *Notethatthemostsignificantdifferencesareduetothehighercool- model, it was sought to remain as close to the actual ingtimeofthePWRspentfuel. design as possible; that is why the NEWT module11 of SCALE was chosen. In this two-dimensional discrete ordinatesmethodcode,itwaspossibletoapplytheexact geometry of the FA~except for the third dimension, the safetyfeaturethefueltemperaturecoefficient~FTC!was axialleakagewasonlytakenintoaccountbyabuckling alsocalculatedasafunctionofburnupandMAcontent; factor, specifying the 195-cm height of the assemblies!. however, it required a new model of the reactor to be However, because of the unusual shape of the GFR600 built ~see Sec. II.B!. FA ~containing thin fuel plates aligned in three direc- tions!,averyfinegridstructurewasneededforNEWTto II.B. The NEWT Model of the Reactor work properly ~see Fig. 2!. One of the most important advantages of using the It was concluded that the calculations for the full KENO-VI module was that a precise description of the coreapplyingtheexactgeometryofeveryfuelassembly complicatedgeometryoftheGFR600wasfeasible.How- wouldhavetakentoomuchtime.Hence,firstaunit-cell ever,whendeterminingtheFTC,thedirectcalculations calculation was made for each region with the actual carriedoutwiththeMonteCarlotransportcodeapplying geometry and a white boundary condition ~NEWTdoes the 3-D model of the reactor proved to be inconclusive, not support periodic boundary condition on edges that asthedifferencebetweenthek-effectiveforthereference are not parallel with the x- or the y-axis!. Then, the ho- andanelevatedfueltemperaturewassmallandhadhigh mogenized macroscopic cross sections were filled into variance.Consequently,thecoefficientsobtainedthisway the full core NEWTmodel so that it could be used with didnotshowcleardependenceontheburnuportheminor amuchroughergrid~seeFig.3!.Foreverytimestep,two actinidecontent;thedeviationswereburiedinthevariance. criticality calculations were performed—one with the 86 NUCLEARTECHNOLOGY VOL.177 JAN.2012 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 ( ~s ! ~t!F ~t! a i,r,g r,g ~s ! ~t!(cid:2) g(cid:2)~t,r,f! ~2! a i,r ( F ~t! r,g g(cid:2)~t,r,f! and ( ~ns ! ~t!F ~t! f i,r,g r,g ~ns ! ~t!(cid:2) g(cid:2)~t,r,f! . ~3! f i,r ( F ~t! r,g g(cid:2)~t,r,f! InEqs.~2!and~3!thesummationsareoverthethree energygroups~thermal,resonance,andfast!requiredby ORIGEN-S. To take into account the quantity of the isotopes as well, their macroscopic worth can be defined as W ~t!(cid:2)N ~t!w ~t! , ~4! i,r i,r i,r Fig.3. TheNEWTmodelofthewholecoreofGFR600with homogenizedFAs. whereN ~t! isthenumberdensityofisotopeiinregion i,r ratthegiventime.Finally,thetotalworthoftheisotopes canbeintroducedastheiraveragemacroscopicworth~in nominalfueltemperatureandonewitha1008Cincreased the rest of this paper, worth will always refer to this temperature—then the k-effective values were used to value!: gaintheFTCvalues@seeEq.~8!later#.Withthismethod theFTCshowedanexplicitdependenceonboththeMA 6 V W~t!(cid:2) (W ~t! r , ~5! cfroonmtetnhteoMftohnetecoCraeralondcatlhceulbautironnusp,,wuhnilcikhewtheoresescdaetrtievreedd i r(cid:2)1 i,r Vcore aroundtheNEWTvalues.Cross-sectionprocessingwas where done the same way as in the KENO-VI model. V (cid:2)volume of the fuel in region r r II.C. Worth Calculations V (cid:2)volume of the core. core To measure the influence of the individual isotopes Addinguptheworthofallisotopesinthefuel,weobtain on the reactivity, traditionally the reactivity weights are thefissionabilityofthefuel~Fiss ~t!(cid:2)( W~t!!.By introduced as w (cid:2) ~ns ! (cid:3) ~s ! ~Refs. 12 and 13!, fuel i i i f i a i addingtheworthofcladdingandcoolantisotopestothis where the brackets indicate spectrum-averaged values. value, the fissionability of the core is determined: Using this definition, a space- and time-dependent mi- croscopicworthcanbeintroducedforeachisotope“i”in each region “r” of the reactor as Fiss~t!(cid:2) ( Fiss ~t! . ~6! l l(cid:2)~fuel,cladding,coolant! w ~t!(cid:2)~ns ! ~t!(cid:3)~s ! ~t! . ~1! i,r f i,r a i,r The changes of the fissionability—especially in the The meaning of Eq. ~1! is quite straightforward; it uniform cores—closely follow the changes of the reac- showswhetheranisotopeatthegivenregionofthecore tivity.4,14 This provides a powerful tool to examine the contributespositivelyornegativelytotheneutronecon- behavior of the reactor; by analyzing the worth of the omy at the given time. The nuclei with positive micro- individual isotopes, a good understanding of the basic scopic worth ~w ~t! (cid:4) 0! can be regarded more as processes taking place in the reactor can be gained. i,r fissionable,whilethosewithnegativemicroscopicworth Three types of isotopes can be distinguished in the ~w ~t!(cid:5)0!canberegardedmoreasabsorberisotopes, fuel as follows: i,r since the former produce more and the latter produce 1. Fissionable isotopes: heavy metal isotopes hav- fewer neutrons than they absorb. ingpositiveworth~theirtotalworthisreferredto The spectrum-averaged values necessary to deter- as HMp worth! mine the microscopic worths can easily be calculated usingthethreegroupfluxesandcrosssectionscomputed 2. Absorber isotopes: heavy metal isotopes having by the KMART6 module via collapsing the 238 group negativeworth~theirtotalworthisreferredtoas values estimated by KENO-VI: HMn worth! NUCLEARTECHNOLOGY VOL.177 JAN.2012 87 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 3. Fission products: isotopes produced by fission, Using the TSUNAMI-3D module15 of SCALE ~apply- plus the Si and C isotopes of the fuel ~their total ing the 3-D KENO-VI model of the reactor! k-effective worth is referred to as FPworth!. sensitivity coefficients @S ~t!# were obtained for all k,Sxi,,rg reactions~x! ofthefuelisotopes~i! inallenergygroups Naturally,thetotalfuelworthisgivenbythesumof ~g! and regions ~r! of the core, then self-shielding cal- the HMp, HMn, and FPworth at any time. culationswerecarriedoutforthereference~T (cid:2)9908C! ref andtheincreasedfueltemperature~T (cid:2)10908C!using II.D. Safety Assessment per the CSAS-MG sequence. The resulting cross sections of all relevant reactionsc of the fuel isotopes were read Two safety parameters of the reactor were calcu- from the AMPX working libraries @si,r,~990!~t! and lated, the fundamental delayed neutron fraction ~DNF! x,g si,r,~1090!~t! microscopic cross sections#, then the sen- and the FTC. The former substantially influences the x,g sitivitycoefficientswereusedtocalculatethek-effective dynamicsofthereactorandourabilitytooperateitwhile change due to isotope i ~Dk ~t!! and the isotopic contri- the latter is a measure of the most important prompt i butions to the FTC ~FTC ~t!!: feedback effect. i ThefundamentalDNFwasestimatedbysimplytak- ing the delayed to total neutron production ratio ~as no Dki~t!(cid:2)ke~9ff90!~t!(((Sk,Sxi,,rg~t! adjoint calculations were performed, the more usual ef- r x g fective DNF was not determined!: (cid:2)(cid:2) si,r,~1090!~t!(cid:3)si,r,~990!~t! (cid:6) x,g x,g ~9! nD~E!Sf~rs,E,t!F~rs,E,t!dr3dE sxi,,gr,~~990!!~t! b~t!(cid:2) (cid:2)(cid:2) and n~E!S ~r,E,t!F~r,E,t!dr3dE f s s (Dk ~t! 1 i ( (6 (~nD!i,gNi,r~t!~sf!i,r,g~t!Fr,g~t!Vr FTC~t!(cid:2) 100 ki~990!~t! (cid:2)(FTCi~t! . ~10! (cid:2) i r(cid:2)1 g eff i 6 Withthistechniquetheimportanceoftheindividual ( ( (~n! N ~t!~s ! ~t!F ~t!V i,g i,r f i,r,g r,g r isotopeswasrevealed,andthedependenceoftheFTCon i r(cid:2)1 g theburnupandtheMAcontentofthecorebecameclear. (cid:2)(b ~t! . ~7! i i III. THE EFFECTS OF ADDING MAs TO THE FUEL In Eq. ~7!, ~n ! is the average number of delayed, D i,g while~n! istheaveragetotalnumberofneutronspro- i,g duced by the fission of isotope i, induced by a neutron First,theeffectsofsubstitutingsomeoftheuranium withanenergyingroupg.Furthermoreb ~t! isthecon- in the fuel with MAs were investigated. Using the i tribution of isotope i to the delayed neutron fraction. KENO-VImodelofthereactorburnup,calculationswere TheFTCwasestimateddirectlybyusingk-effective performedwithcoreshavinguniforminitialMAcontent values from criticality calculations with the reference of different amount and origin. The results discussed in and a 1008C increased fuel temperature: this section correspond to the first cycle, and they show (cid:3) (cid:4) thattheMAshaveadecisiveinfluenceonthereactivity, 1 k~1090!~t!(cid:3)k~990!~t! 1 FTC~t!(cid:2) eff eff . ~8! as well as on the safety parameters and the MA trans- 100 k~990!~t! K mutational capabilities of the reactor. eff AsdiscussedinSec.II.B,whendeterminingtheFTC III.A. Effects on Reactivity thek-effectivevaluesfromtheNEWTmodelwereused in Eq. ~8! since the coefficients calculated with the Thechangeofreactivityduringburnupincoreshav- KENO-VI model were too scattered, showing no clear ing different initial VVER MA content can be seen in trends. Fig. 4. Two important effects should be observed: the At last, to better understand the dependence of the FTC on the burnup and the MA content of the core, cThereactionstakenintoaccountareelasticandinelasticscat- FTCvalueswerealsocalculatedwithperturbationtech- tering,fission,radiativecapture,andn,2n;moreover,varia- niquesforfourspecificcases@atthebeginningofburnup tionduetothechangeinnwasaccountedfor,asthesensitivities ~BOB! and at the end of burnup ~EOB! in the core to all these are automatically calculated by TSUNAMI-3D having 0% and 10% uniform initial PWR MAcontent#. ~Ref.15!. 88 NUCLEARTECHNOLOGY VOL.177 JAN.2012 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 higheramountof237Nppresent.Theincreaseintheworth ofthefissionableminoractinideisotopesduringthecam- paign also gets more significant with the MA content, mainlyduetotheincreasedproductionof 242mAmfrom 241Am. Obviously, both these effects decrease the reac- tivity loss. In Ref. 14 it is shown that two major differences arise between the PWR and the VVER cases: Both the initialreactivityandthereactivitylossduringburnupare higher in the VVER case. The former is caused by the higherinitial241PucontentoftheVVERplutonium,while the latter is explained by the more rapidly decreasing 241Pu and the slowly increasing 242mAm worth ~due to theloweramountof 241Ampresentintheshortercooled VVER spent fuel!. Fig.4. Thereactivityduringburnupincoreshavingdifferent III.B. Effects on Safety Parameters initialVVERMAcontent~X!.e In the previous section it was shown that the addi- tion of MAs to the fuel has beneficial effects on the reactivityandmakesitpossibletoreachhigherburnups additionofMAsdecreasestheinitialreactivityd andthe and consequently higher MA destruction. The safety reactivitylossalike.Thesearethesameeffectsthatwere of the reactor is, however, negatively affected by the shown with PWR MAs in earlier studies.2 Obviously, presence of MAs. As can be seen in Fig. 6, the DNF both are advantageous from the reactor operation point decreases with the increasing MA content, though its ofviewsinceasmallerreactivityhastobesuppressedin decline during burnup is almost entirely independent of thebeginningandintroducedduringburnup~athighini- that. For understanding, see Fig. 7, where the plotted tial PWR MA contents the reactivity swing even turns positive!. Moreover, the decreased reactivity loss en- values are 100{~biX%~0!0(ibi0%~0!!; i.e., the contribu- tionofisotopegroupitothedelayedneutronfractionat ables longer campaigns and higher burnup values, con- BOB is compared to the DNF at BOB in the core hav- sequently increasing the MA destruction ~seen later in ing 0% initial VVER MA content. The majority of de- Figs. 13 and 14!. layed neutrons is produced by plutonium ~239Pu and The decreased initial reactivity can be explained by 241Pu primarily! and uranium ~238U mainly!; moreover, theworthofabsorberisotopes.TheMAmixhasamore the decreased number of delayed neutrons produced by negative microscopic worth than the uranium it substi- the decreasing amount of uranium present in the fuel is tutes ~though this negative microscopic worth becomes basically compensated by the MA isotopes ~mostly by smaller as the MAcontent of the fuel increases!; hence, the reactivity decreases with its addition.14f 237Np!. The true cause of the decrease in the DNF is that the contribution of the unchanged amount of pluto- Thedecreasedreactivitylossduringburnup,aswell nium in the fuel decreases since the MAs make the asthedifferencesbetweenthePWRandtheVVERcase spectrum harder, increasing the prompt, but leaving the canbeexplainedbytheworthofthefissionableisotopes. delayed neutron yield unaffected. AscanbeseeninFig.5,theplutoniumworthdominates In Ref. 14 it is shown that the DNF is higher in the thetotalHMpworthineverycase,anditsdecreasedur- VVER case ~mainly due to the higher amount of 241Pu ingburnupgetssmallerwiththeincreasingMAcontent; and 237Np! but also has a more rapid decrease during in the PWR case it even stays constant. This is mostly burnup~as241Puisbeingconsumedmorerapidly!.gThis causedbythemorerobustproductionof 238Pufromthe difference, however, disappears in later cycles. The FTC during burnup calculated with the NEWT dThisistrueonlyforsmallMAcontents.Substitutingahigher model of the reactor can be seen in Fig. 8 for cores amountoftheuraniumwiththeMAmixstartstoincreasethe having different initial PWR MA content.h Note that initialreactivity. eThevaluesgiveninthelegendsaretheXvaluesinSec.II. justliketheDNF,theDopplercoefficientalsodecreases fTheturn-backoftheinitialreactivityathigherMAcontentsis causedbythefactthatthemicroscopicworthoftheMAmix gTheDNFatBOBis'0.360%and'0.325%incoreshaving and the uranium becomes less negative with the increasing 0%and10%uniforminitialPWRMAcontents,respectively, MAcontentduetothecausedspectralhardening;hence,after whilethedecreaseduringthefirstirradiationis0.015%with a point the substitution of some uranium with stronger ab- both cores compared to the more than 0.02% decrease ob- sorberMAsiscounterbalancedbytheincreaseintheworthof servedintheVVERcase. therestoftheabsorbersinthecore. hTheVVERcaseisbasicallyidenticaltothePWR. NUCLEARTECHNOLOGY VOL.177 JAN.2012 89 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 Fig.5. BreakdownofHMpworthincoreshavingdifferentuniforminitialPWRandVVERMAcontent.ThecomponentsofHMp worthareasfollows:total~blue(cid:2)!,Pu~blue(cid:3)!, 235U~red▫!,Cm~red(cid:7)!, 242mAm~red(cid:5)!.Axesontheleftbelongto thebluegraphs,axesontherighttotheredgraphs.AllworthiscomparedtothetotalHMpworthatBOBincoreshaving 3%uniforminitialMAcontent;i.e.,theplottedvaluesare100{WX%~t!0~( W3%~0!!. i i:Wi~0!(cid:4)0 i Fig.7. TheDNFatBOBcomparedtoreferencecaseincores Fig.6. TheDNFduringburnupincoreshavingdifferentini- havingdifferentinitialVVERMAcontent.Therepre- tialVVERMAcontent.NotethattheadditionofMAs sented DNF producing isotope groups are as follows: decreases the DNF, but the change during burnup is total~blueline!,Uisotopes~blue(cid:2)!,Puisotopes~blue unaffected. x!,andMAisotopes~red▫!. 90 NUCLEARTECHNOLOGY VOL.177 JAN.2012 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 238UdecreaseandthespectralhardeningduetotheMA accumulationbothdecreasetheFTC,whileathighMA contentsthespectralsofteningduetotheMAconsump- tion counterbalances the effect of the decreasing 238U. III.C. Effects on Spent Fuel Properties AstheGFRisplannedforoperationinaclosedfuel cycle, its spent fuel will have to be reprocessed after every irradiation, and the recovered actinides will have to be incorporated in the new fuel of the reactor. It is important to know what conditions are to be expected duringtheseprocedures;hence,theeffectsthattheaddi- tionofMAstothefuelwouldhaveontheoverallradio- activity, the thermal heat, and the neutron source of the spentfuelwereanalyzed.Thesequantitiescaneasilybe Fig.8. TheFTCduringburnupincoreshavingdifferentuni- computedwiththeORIGEN-SmoduleofSCALE,andin forminitialPWRMAcontent. SCALE 6 they are automatically included in the TRI- TON calculations.All results in this section correspond to the spent fuel from the whole core ~containing 14.8 in absolute value with the addition of MAs. However, tonnesofheavymetalsand800kgofFPs!afterthefirst unlike the DNF, the change of the FTC during burnup cycle ~i.e., time 0 is the discharge moment!. depends on the initial MA content of the core—at low The MAs have the most significant effect on the MAcontentstheFTCdecreasesinabsolutevalue,while neutron source of the spent fuel. Immediately after ir- at high contents it stays almost constant. As discussed radiation for 1300 days the total neutron source of the in Sec. II.D, the isotopic contributions to the FTC were spentfuelfromthefullcorehaving3%initialVVERMA calculatedforfourspecificcaseswithperturbationmeth- content is ;5(cid:6)1011 n0s, which is roughly 8 times the ods; the results are presented in Fig. 9. Uranium-238 is valuecalculatedfortheMAfreecore~6.5(cid:6)1010 n0s!i; clearlydominant,andspectrumeffectscanalsobeseen. moreover,thisdifferenceonlyincreasesduringthecool- In the MA free core the ;785-kg decrease in the 238U ing period to over a factor of 13 @neutrons from sponta- contenttogetherwitha70-kgincreaseintheMAamount neousfissionand~a,n! reactionsareaccountedfor,the correspond to a decrease of (cid:3)0.21 pcm0K in the FTC delayedneutronspresentinthefirstfewminutesafterthe during burnup, while in the core having 10% initial reactor is shut down are neglected#. With the further PWR MA content the 610-kg decrease of 238U along addition of MAs, the neutron source basically rises lin- with the 314-kg decrease of MAs basically leave the early to ;1.4 (cid:6) 1012 n0s at 10% initial VVER MA FTC unchanged. Consequently, at low MAcontents the content.j Thereasonforthisincreasecaneasilybeunderstood by taking a look at Fig. 10. Notice that the curium iso- topes clearly dominate the neutron source of the spent fuel during the whole cooling period.As is discussed in Sec. IV.A, the more curium that is present at the begin- ningofburnup,themoreisleftattheend,consequently resulting in stronger neutron emission. Anotherimportantaspectduringreprocessingisthe heat load of the spent fuel. Just like the neutron source, the thermal power also increases with the MA content of the fuel, however to a lesser extent. The heat pro- duced by the spent fuel from the full core having 10% and no initial VVER MA content at discharge ~i.e., immediately after the first irradiation! is 4.7 MW and 2.7 MW, respectively ~6 MW and 2.7 MW in the PWRcase!.Thismodestincreaseisbecauseasignificant iThesituationissimilarinthePWRcase,thevaluesareslightly higher~6.7(cid:6)1011n0sand7.1(cid:6)1010n0s,respectively!,just Fig.9. The isotopic contributions to the FTC coefficient in likethedifference~approximately9times!. coreshavingdifferentuniforminitialPWRMAcontent. j1.9(cid:6)1012 n0sinthePWRcase. NUCLEARTECHNOLOGY VOL.177 JAN.2012 91 Perkóetal. MINORACTINIDETRANSMUTATIONINTHEGFR600 Fig.10. Thetotalneutronsourceofnuclidesinthespentfuel Fig.12. Theactivityoftheheavymetalelementsinthespent ofthefullcorehaving5%initialVVERMAcontent fuel of the full core having 5% initial VVER MA during the cooling period following the first irradia- contentduringthecoolingperiodof5yearsfollowing tion.Delayedneutronsareneglected. thefirstirradiation. portion of the thermal power can be attributed to the ofneptunium,americium,andplutoniumisbasicallysin- FPs,whichbuildupverysimilarlyinthedifferentcores gularly due to 238Np, 242mAm, and 238Pu.The expected if the burnup is the same. heat load during fuel manufacturing from the actinide Actinides from the spent fuel will have to be incor- mix recovered from the spent fuel of cores having 10% poratedintothenewfuelofthereactor;hence,itisworth and0%initialVVERMAcontentafter5yearsofcooling takingalookattheirheatloadseparately.Duringmostof is27.9W0kgand3.3W0kg,respectively~31.6W0kgand the cooling period, curium isotopes are responsible for 3.3W0kg in the PWR case!. the bulk of the heat ~see Fig. 11!, while at the end plu- The addition of MAs also results in a more radio- tonium isotopes become increasingly dominant ~as cu- active spent fuel; however, this increase is very modest rium isotopes have shorter half-lives!. The curium heat as the short-term radioactivity is dominated by the FPs productionismainlydueto242Cmand244Cm,whilethat ~just like the thermal power!. The total radioactivity of the spent fuel immediately after irradiation from cores having 10% and no initial VVER MA content is 2.7(cid:6) 1019 Bqand2.6(cid:6)1019 Bq,respectively~2.8(cid:6)1019 Bq and2.6(cid:6)1019 BqinthePWRcase!,whiletheexpected valuesfromthereprocessedactinidesduringfuelmanu- facturingare72GBq0gand43GBq0g~64GBq0gand33 GBq0g in the PWR case!. As can be seen in Fig. 12, mostly plutonium is responsible for the activity. IV. TRANSMUTATIONAL CAPABILITIES Themaingoalofourinvestigationwastoassessthe MAtransmutational capabilities of the GFR.As the re- actor is planned for operation in a closed fuel cycle in which the spent fuel is always reprocessed and all the recovered actinides ~including the MAs! are incorpo- ratedintonewFAs,itwasenvisionedthattheextraMAs thataresoughttobedestroyedwouldsimplybeaddedto the recovered ~or the initial! actinides and no specific Fig.11. Thethermalpoweroftheheavymetalelementsinthe spent fuel of the full core having 5% initial VVER target assemblies would be embedded into the design. MAcontentduringthecoolingperiodof5yearsfol- First, spatially uniform transmutation was consid- lowingthefirstirradiation. ered where the MA content of the fuel had no spatial 92 NUCLEARTECHNOLOGY VOL.177 JAN.2012

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FUEL CYCLE AND MANAGEMENT KEYWORDS: transmutation,gas-cooled fast reactor, nonuniform minor actinide content MINOR ACTINIDE TRANSMUTATION IN GFR600
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