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Burnup Determinaton of Nuclear Fuel

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Burnup Determinaton of Nuclear Fuel MASS SPECTROSCOPY Original Papers Vol17.No4,December1969 Burnup Determinaton of Nuclear Fuel KIYOSHI I NOUE,*KAORU TANIGUCHI,*TOSHIFUMI MURATA,** HIDEHIKO MITSUI*AND AKIRA DOI* (Received August16,1969) A general description of burnup determining experiments is presented for making vivid a part of mass spectrometry,in comparison of results obtained from radiochemical and nondestructive analyses. Specimen of nuclear fuel was grains of uranium dioxide irradiated in a nuclear reactor for about200 days,and its burnup was found to be8,000MWD/T with sufficient consistency in the experimental results. 1.Introduction method is included in the first approach, Extensive studies on nuclear fuel and the second approach includes radio burnup analysis have been made in the chemical and nondestructive methods. past,since burnup is one of fundamental Both of the radiochemical and nondes quantities required in a fuel research structive methods essentially measure program.Burnup is also an important radioactivities of fission products formed quantity for design and operation of in a nuclear fuel.The former has an ac power reactors from a standpoint of ceptable precision with low cost and safety as well as operability. simple procedure,but the development A wide variety of methods have of a good method for the later remains been developed to determine burnup of an engineering target. irradiated fuel.Principal procedures This paper presents a general de used so far have been based on meas scription on the burnup determining ex ments of: periments for a uranium dioxide fuel (1)Changes in isotopic composition of specimen.Comparing the mass spectro fissioning elements in a nuclear metry method with the other methods, fuel brought about during irradia the contribution it can make to the tion. burnup determination of nuclear fuels (2)Amount of fission products form will be made clear. in a nuclear fuel during irradiation.ed It has been generally accepted that a 2.Specimen of Nuclear Fuel. mass spectrometric measurement is more Irradiated1) accurate than other methods in current Experiments were carried out for use,because it directly analyzes an iso burnup determination of a uranium di topic composition of uranium or plutoni oxide fuel.The isotopic composition of um in a nuclear fuel before and after uranium in the uranium dioxide was irradiation.The mass spectrometric natural before neutron irradiation.The *Nuclear Energy Div.,Cent.Research Lab.,Hitachi Ltd.(Ozenji,Kawasaki,Kanagawa,Japan) **Sixth Div.,Hitachi Research Lab.,Hitachi Ltd.(Saiwai-cho,Hitachi,Ibaraki,Japan) ―830― Burnup Determinaton of Nuclear Fuel specimen was grains from a uranium di fuel matrix.As the specimen was small oxide pellet irradiated in the nuclear re grains of uranium dioxide,zirconium and actor named HFR(the Netherlands)at a cerium are suitable rather than cesium heat generation of50watt per gram of for the burnup indicator,although137Cs uranium dioxide for an irradiation period has been recommended as the first choice of200days.This fuel,therefore,was for the burnup measurement. estimated roughly to be about10,000 3.2Chemical treatment for analysis MWD/T of burnup.The burnup unit of The specimen dissolved in nitric MWD/T is applicable when the fuel acid containing as carriers non-radio performance is emphasized from the view active zirconium,cesium,cerium and point of heat generation in nuclear power others,so that absorption losses of reactors. radioactive isotopes on the glassware wall were reduced.This sample solution 3.Radiochemical Determination of was stored for the experiments after Burnup2) diluting with water. 3.1Selection of burnup indicators The isotopes in the solution were The radioactive isotopes to serve separated following chemical procedures. as burnup indicators should be selected The95Zr sample was purified by to satisfy certain requirements for the coprecipitating with lanthanium fluoride radiochemical analysis.Some of these from others in the sample solution and requirements are summarized as3): was precipitated as barium fluozirconate. (1)Essentially no migration in irradi After dissolving the precipitate with ating fuel matrix. nitric acid,further purification was con (2)Low destruction cross-section and ducted repeatedly and the95Zr sample low formation cross-section from was mounted as mandalate.The chemical adjacent mass chains. preparation of the other samples of (3)Well established fission yield that 137Cs and144Ce were also made by prefererably is constant for al precipitation method,in the forms of fissioning species and is indepenl chloroplatinate for the137Cs sample and dent of neutron energy. of oxalate for the144Ce sample. (4)Good emission characteristics for Radioactive standards were pre radiation spectrometry or dosime pared as follows:The95Zr solution was try. standardized at the United Kingdom Isotopes selected here were95Zr, Atomic Energy Authority,where a spe 137Cs and144ce .These are suitable cific activity of95Zr was1.12•~10-14 considering the requirements,and more Ci per gram of0.1M formalin solution. over have simple chemistry,high fission The95Zr solution was diluted with water yield and long half life in known decay containing zirconium carrier,and the schemes.Cesium,however,shows a 95Zr standard was fixed on a glass great tendency to migrate in the fuel filter as precipitate of mandalate.The matrix during high-temperature irradia other standards of137Cs and144Ce were ation,whereas zirconium and cerium are also prepared as precipitate of their relatively non-volatile and then are apt chloroplatinate or oxalate in a similar to remain associated with uranium in the procedure as the samples to be compared. ―831― K.Inoue,K.Taniguchi,T.Murata,H.Mitsui and A.Doi 3.3Radioactivity measurement and its 144Ce1 .64•~10-1Ci/g(•}2%) analysis 3.4Burnup calculation Gamma activity of the137Cs sample Calculations to estimate the speci was measured by comparison of0.66 men burnup were made,using the number MeV photopeak with that of the137Cs of atoms obtained from the specific ac standard,using a multi-channel pulse tivity for each fission product .Here,it height analyzer with3•g•~3•hNaI scin was assumed that fission products were tillation crystal.Comparative determi formed only by thermal fission of235U nation of the95Zr or144Ce activity in and of239PU transmuted from238U . each sample was-made by gamma spec The results are summarized in Table1 , trometry and beta-ray counting through and the burnup values ranged from6,100 a certain thickness of shield.In later to9,400MWD/T of uranium.Assump measurements,a Geiger-Muller counter tion was made that the fission energy is was used with mica and aluminum shields. 205MeV per fission of235U or239PU, The analytical results of radioacti and so that the burnup unit in MWD/T vity measured for each burnup indicator is equivalent to2.63•~1015fissions per were the followings,in specific activity gram of fissioning element. per gram of uranium in the specimen. The accuracy of the analyses was esti 4.Mass Spectrometric Determination mated from errors involved in the pro of Burnup4,5) cesses of standard preparation,chemical 4.1Mass spectrometer separation and radioactivity measurement. A mass spectrometer used in the 95Zr8 .25•~10-3Ci/g(•}5%) burnup analysis of the specimen was of 137Cs2 .84•~10-2Ci/g(•}3%) 90•‹sector type with350mm radius of Table1.Summary of radiochemical burnup determination. Burnup indicator 95Zr 137CS 144Ce For 235U fission fission yield 6.2 x 10-2 6.15 x102 6 .0 x 10-2 number of fission 1.05x 1016 1.16 x 1016 942 x 1015 (fiss/mgof U) For 239Pu fission fission yield 5.9x 10-2 6 .63x 10-2 5.3 x 10 2 number of fission 8.85 x1015 1.28 x 1016 6.50 x1015 (fiss/ mg of U Total number of 1.94 x1016 2 .44 x1016 1.59 x 1016 fission (fiss /my of U Burnup value 7,500 9 ,400 6,100 MWD/Tof U ―832― Burnup Determinaton of Nuclear Fuel curvature.This spectrometer was equi from Fig.1. pped with a thermal-ionization ion source Figure2shows a typical spectrum in single-filament•@ arrangement for most of the specimen.It was found that63.0 of this experiment.6) %of235U had fissioned and that12.1% Typical adjustment for the present ex of235U had transmuted to236U,refer periment was: red to the estimated amount of235U in Ion accelerating voltage3,500V natural uranium dioxide before irradia Source slit0.1mm tion.Therefore the contribution to Detector slit0.6to0.8mm burnup of this specimen by the fissioning Voltage supply for10-stage electron of235U was determined to be4,370 multiplier1,800V MVVD/T of uranium. Output resistance of multiplier1011ƒ¶ 4.3Mass spectrometry of fission Minimum voltage range for250mm products 238U is transmuted into239PU by recording width1mV Highest operating pressure in neutron capture reaction and succeeding analyzer tube5•~10-7mmHg The ion accelerating voltage could be 12 raised to5,000V,and the ion current detection system had the capability of 11 detecting a current of 10-17A.As the available resolving power was about500, 10 it was enough to separate the heavy element isotopes. 9 The sample solution was used with 8 out any chemical separation prior to = commencing the mass spectrometry,be ⊃7 cause it is desirable to simplify the き analytical procedure.The solution was .ムと6 pipetted and evaporated to dryness on a filament,and then the ion source was ε5 assembled with this filament. 岳 4.2Mass spectrometry of uranium ヒ4 A typical spectrum such as shown 己 in Fig.1was obtained from a reference ⊂3 2 unirradiated natural uranium dioxide specimen.From this figure,the isotopic 2 ratio between235U and238U was de termined to be7.15•~10-3,which 1 agrees well with available data for 0 natural uranium.No preirradiation 270267 measurement was performed for the burnup specimen,but the isotopic com MGSs-to-charge rotio position of uranium before irradiation Fig.1.Mass spectrum of natural uranium for might be referred to the value obtained unirradiated uranium dioxide.
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