燃料元件破坏性燃耗测量过程的质量控制
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摘要
燃耗是核燃料元件最重要的性能指标之一,其准确测量对新型燃料元件研制和换料周期确定等具有重要意义。破坏性燃耗测量属于强放射性下的精细化学分析,需建立系统的方法对测量过程进行质量控制,确保测量数据准确可靠。本文从方法适用性分析、数据预估、质谱干扰分析、样品污染分析、多种方法验证等方面介绍了破坏性燃耗测量过程质量控制的方法。剖析了重同位素法、~(148)Nd监测体法、~(145)Nd+~(146)Nd监测体法、~(137)Cs监测体法等的优缺点和适用范围。介绍了由裂变产额比值预估钕同位素丰度比、由铀同位素丰度比预估燃耗值的方法。分析了质谱测量时由Ce和Sm同位素造成的同量异位素干扰及其检测、排除手段。针对天然本底污染和样品间的交叉污染,分别论述了两种污染源的判断和修正技巧。还探讨了对燃耗值、稀释剂浓度、同位素丰度比等关键数据进行对比验证的方法。
Burnup is an important index of nuclear fuel elements after irradiation. And the accurate measurement of burnup value is of great significance for the research of new kind of nuclear fuel element as well as for the optimization of the reload cycle. How-ever, the destructive fuel burnup measurement is a refined chemical analysis in the environment of strong radioactivity. In order to ensure the accuracy of the measured data, establishing a systematic method to control quality is very necessary. In the present paper, the process of quality control method for destructive fuel burnup measurement was introduced from different aspects, such as the suitability of the analytical method, data forecast, mass spectrum interference, sample contamination, multiple method validation and so on. The merits and demerits of the heavy isotope method, ~(148)Nd, ~(145)Nd+~(146)Nd and ~(137)Cs monitor methods were analyzed. In addition, the ratios of fission yield were used to estimate the isotopic abundance ratios of Nd and the isotopic abundance ratios of U to estimate the burnup values. Moreover, the detection and elimination means for the mass spectrum interferences caused by Ce and Sm were also analyzed. For the natural background pollution and cross-contamination between samples, the judgment skills and correction methods were studied respectively. Finally, the compare verification methods of burnup value, spike concentration and isotope abundance ratio were also discussed in detail.
Burnup is an important index of nuclear fuel elements after irradiation. And the accurate measurement of burnup value is of great significance for the research of new kind of nuclear fuel element as well as for the optimization of the reload cycle. How-ever, the destructive fuel burnup measurement is a refined chemical analysis in the environment of strong radioactivity. In order to ensure the accuracy of the measured data, establishing a systematic method to control quality is very necessary. In the present paper, the process of quality control method for destructive fuel burnup measurement was introduced from different aspects, such as the suitability of the analytical method, data forecast, mass spectrum interference, sample contamination, multiple method validation and so on. The merits and demerits of the heavy isotope method, ~(148)Nd, ~(145)Nd+~(146)Nd and ~(137)Cs monitor methods were analyzed. In addition, the ratios of fission yield were used to estimate the isotopic abundance ratios of Nd and the isotopic abundance ratios of U to estimate the burnup values. Moreover, the detection and elimination means for the mass spectrum interferences caused by Ce and Sm were also analyzed. For the natural background pollution and cross-contamination between samples, the judgment skills and correction methods were studied respectively. Finally, the compare verification methods of burnup value, spike concentration and isotope abundance ratio were also discussed in detail.
引文
[1] 李桃生,方栋. 核燃料的燃耗测量方法综述[J]. 核电子学与探测技术,2005,25(6):852-857. LI Taosheng, FANG Dong. Introduction to burn-up measurement method of nuclear fuel[J]. Nuclear Electronics & Detection Technology, 2005, 25(6): 852-857(in Chinese).
[2] KOLE?KA M, VIERERBL L, MAREK M, et al. Determination of IRT-2M fuel burnup by gamma spectrometry[J]. Appl Radiat Isot, 2016, 107: 92-97.
[3] KIM J S, JEON Y S, PARK S D, et al. Analysis of high burnup pressurized water reactor fuel using uranium, plutonium, neodymium, and cesium isotope correlations with burnup[J]. Nuclear Engineering & Technology, 2015, 47(7): 924-933.
[4] ASTM E321-96 (2012) Standard test method for atom percent fission in uranium and plutonium fuel (neodymium-148 method)[S]. West Conshohocken, PA: ASTM International, 2012.
[5] BERA S, BALASUBRAMANIAN R, DATTA A, et al. Burn-up measurements on dissolver solution of mixed oxide fuel using HPLC-mass spectrometric method[J]. International Journal of Analytical Mass Spectrometry and Chromatography, 2013, 1(1): 55-60.
[6] SMU?EK W, BORKOWSKI M. Separation of some burn-up monitors from the UO2-Al nuclear fuel[J]. Journal of Radioanalytical Chemistry, 1976, 31(1): 31-44.
[7] KIM J S, JEON Y S, PARK S D, et al. Burnup determination of high burnup and dry processed fuels based on isotope dilution mass spectrometric measurements[J]. Journal of Nuclear Science and Technology, 2007, 44(7): 1 015-1 023.
[8] 廖祖民. HFETR燃料元件燃耗测定的重同位素方法研究[J]. 核动力工程,1989,10(2):65-69. LIAO Zumin. Study of heavy isotope method for burnup determination of fuel element from HFETR[J]. Nuclear Power Engineering, 1989, 10(2): 65-69(in Chinese).
[9] 张春华,廖祖民,于生棣,等. 用148Nd法分析核燃料的燃耗[J]. 核动力工程,1983,4(3):7-12. ZHANG Chunhua, LIAO Zumin, YU Shengdi, et al. The burnup determination of nuclear fuels by the neodymium-148 method[J]. Nuclear Power Engineering, 1983, 4(3): 7-12 (in Chinese).
[10] KRTIL J, SUS F, BULOVI■, et al. Experience with the neodymium method for determination of nuclear fuel burn-up[J]. Journal of Radioanalytical and Nuclear Chemistry, 1984, 83(1): 61-66.
[11] HERMANN A, STEPHAN H, BELL G. On the use of neodymium isotopes in burnup analysis of spent nuclear fuel[J]. Isotopenpraxis, 1988, 24(2): 85-88.
[12] 陈云明,张劲松,梁帮宏,等. 同位素稀释质谱-γ能谱法测定天然铀燃料元件燃耗[J]. 四川大学学报:自然科学版,2016,53(5):1 076-1 080. CHEN Yunming, ZHANG Jingsong, LIANG Banghong, et al. Burnup determination of natural uranium fuel by isotope dilution mass spectrometry and gamma spectroscopy[J]. Journal of Sichuan University: Natural Science Edition, 2016, 53(5): 1 076-1 080(in Chinese).
[13] 杨留成,朱荣保,林灿生,等. 用γ能谱法破坏性测定秦山核电站考验元件燃耗[J]. 核化学与放射化学,1992,14(4):246-252. YANG Liucheng, ZHU Rongbao, LIN Can-sheng, et al. Destructive determination of burnup of tested fuel element of Qinshan Nuclear Power Plant by γ spectrometry[J]. Journal of Nuclear and Radiochemistry, 1992, 14(4): 246-252(in Chinese).
[14] CARUSO S, GüNTHER-LEOPOLD I, MURPHY M F, et al. Comparison of optimised germanium gamma spectrometry and multicollector inductively coupled plasma mass spectrometry for the determination of 134Cs, 137Cs and 154Eu single ratios in highly burnt UO2[J]. Nuclear Instruments and Methods in Physics Research A, 2008, 589(3): 425-435.
[15] 梁帮宏,张劲松,李兵,等. 负热电离质谱法测定核燃料裂变产物中钼同位素比值[J]. 质谱学报,2016,37(2):134-139. LIANG Banghong, ZHANG Jinsong, LI Bing, et al. Determination of molybdenum isotope ratios in fission products of nuclear fuel by negative thermal ionization mass spectrometry[J]. Journal of Chinese Mass Spectrometry Society, 2016, 37(2): 134-139(in Chinese).
[2] KOLE?KA M, VIERERBL L, MAREK M, et al. Determination of IRT-2M fuel burnup by gamma spectrometry[J]. Appl Radiat Isot, 2016, 107: 92-97.
[3] KIM J S, JEON Y S, PARK S D, et al. Analysis of high burnup pressurized water reactor fuel using uranium, plutonium, neodymium, and cesium isotope correlations with burnup[J]. Nuclear Engineering & Technology, 2015, 47(7): 924-933.
[4] ASTM E321-96 (2012) Standard test method for atom percent fission in uranium and plutonium fuel (neodymium-148 method)[S]. West Conshohocken, PA: ASTM International, 2012.
[5] BERA S, BALASUBRAMANIAN R, DATTA A, et al. Burn-up measurements on dissolver solution of mixed oxide fuel using HPLC-mass spectrometric method[J]. International Journal of Analytical Mass Spectrometry and Chromatography, 2013, 1(1): 55-60.
[6] SMU?EK W, BORKOWSKI M. Separation of some burn-up monitors from the UO2-Al nuclear fuel[J]. Journal of Radioanalytical Chemistry, 1976, 31(1): 31-44.
[7] KIM J S, JEON Y S, PARK S D, et al. Burnup determination of high burnup and dry processed fuels based on isotope dilution mass spectrometric measurements[J]. Journal of Nuclear Science and Technology, 2007, 44(7): 1 015-1 023.
[8] 廖祖民. HFETR燃料元件燃耗测定的重同位素方法研究[J]. 核动力工程,1989,10(2):65-69. LIAO Zumin. Study of heavy isotope method for burnup determination of fuel element from HFETR[J]. Nuclear Power Engineering, 1989, 10(2): 65-69(in Chinese).
[9] 张春华,廖祖民,于生棣,等. 用148Nd法分析核燃料的燃耗[J]. 核动力工程,1983,4(3):7-12. ZHANG Chunhua, LIAO Zumin, YU Shengdi, et al. The burnup determination of nuclear fuels by the neodymium-148 method[J]. Nuclear Power Engineering, 1983, 4(3): 7-12 (in Chinese).
[10] KRTIL J, SUS F, BULOVI■, et al. Experience with the neodymium method for determination of nuclear fuel burn-up[J]. Journal of Radioanalytical and Nuclear Chemistry, 1984, 83(1): 61-66.
[11] HERMANN A, STEPHAN H, BELL G. On the use of neodymium isotopes in burnup analysis of spent nuclear fuel[J]. Isotopenpraxis, 1988, 24(2): 85-88.
[12] 陈云明,张劲松,梁帮宏,等. 同位素稀释质谱-γ能谱法测定天然铀燃料元件燃耗[J]. 四川大学学报:自然科学版,2016,53(5):1 076-1 080. CHEN Yunming, ZHANG Jingsong, LIANG Banghong, et al. Burnup determination of natural uranium fuel by isotope dilution mass spectrometry and gamma spectroscopy[J]. Journal of Sichuan University: Natural Science Edition, 2016, 53(5): 1 076-1 080(in Chinese).
[13] 杨留成,朱荣保,林灿生,等. 用γ能谱法破坏性测定秦山核电站考验元件燃耗[J]. 核化学与放射化学,1992,14(4):246-252. YANG Liucheng, ZHU Rongbao, LIN Can-sheng, et al. Destructive determination of burnup of tested fuel element of Qinshan Nuclear Power Plant by γ spectrometry[J]. Journal of Nuclear and Radiochemistry, 1992, 14(4): 246-252(in Chinese).
[14] CARUSO S, GüNTHER-LEOPOLD I, MURPHY M F, et al. Comparison of optimised germanium gamma spectrometry and multicollector inductively coupled plasma mass spectrometry for the determination of 134Cs, 137Cs and 154Eu single ratios in highly burnt UO2[J]. Nuclear Instruments and Methods in Physics Research A, 2008, 589(3): 425-435.
[15] 梁帮宏,张劲松,李兵,等. 负热电离质谱法测定核燃料裂变产物中钼同位素比值[J]. 质谱学报,2016,37(2):134-139. LIANG Banghong, ZHANG Jinsong, LI Bing, et al. Determination of molybdenum isotope ratios in fission products of nuclear fuel by negative thermal ionization mass spectrometry[J]. Journal of Chinese Mass Spectrometry Society, 2016, 37(2): 134-139(in Chinese).
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