高温气冷堆及其乏燃料中核素的质谱分析技术

Research Progress of Inorganic Mass Spectrometry Applied to Analysis of Nuclear Elements from High-Temperature Gas-Cooled Reactor and Its Spent Fuel

  • 摘要: 质谱技术发展初期主要用于与核工业相关的无机同位素丰度的测定,随着核工业的兴起与发展,质谱技术被广泛应用于核燃料与核材料中杂质分析、核燃料燃耗测定以及核素分析等领域。本工作从质谱技术用于高温气冷堆运行中产生的氚检测、乏燃料中痕量钚(Pu)和镎(Np)测定以及乏燃料中14C测定的原理及应用、研究方法的优缺点三方面展开论述,阐述了用于高温气冷堆及其乏燃料中核素分析方面的气体同位素质谱仪(GIMS)、电感耦合等离子体质谱仪(ICP-MS)、激光共振电离质谱仪(LRIMS)以及加速器质谱仪(AMS)的研制及应用现状,分析了仪器本身及其应用方面存在的问题及发展趋势,讨论了未来相关质谱技术的发展方向,并提出可能的解决方案。为了使质谱技术能够更加有效地应用于高温气冷堆的研究,迫切需要发展体积小、结构简单、便于操作的智能化仪器。

     

    Abstract: At the preliminary stage of mass spectrometry (MS) technology development, it was mainly applied to determine the nuclear industry related inorganic isotope abundance. With the rapid development of nuclear industry, MS has been employed to analyze the impurities in nuclear fuel and nuclear materials, burnup of nuclear fuels, and nuclides from high-temperature gas-cooled reactor (HTGR). The study mainly discussed the basic principles, application, and the research method’s advantages and disadvantages of inorganic mass spectrometry applied to analysis of tritium from HTGR, trace amounts of plutonium and neptunium and 14C in its spent fuel. The application and R&D status of gas isotope mass spectrometer (GIMS), inductively coupled plasma mass spectrometer (ICP-MS), laser resonance ionization mass spectrometry (LRIMS), and accelerator mass spectrometer (AMS) at domestic and abroad were introduced, and problems of the instruments, application and development tendency were pointed out. The low resolution GIMS has the disadvantages of strict conditions, limited scope of application, and complex error during the analysis of hydrogen isotopes, while the high resolution GIMS is overcome the disadvantages of low resolution GIMS, and able to realize the rapid and accurate analysis with low determinative error. However, high resolution GIMS is embargoed due to the special military applications, and need to independently develop it by China. The disadvantages of ICP-MS such as poor anti-interference performance, low resolution, analyze by destroy the simple, and severe inhibition effects for space charge leads its low accuracy, which limit the application in nuclear field. Although there are prominent advantages for LRIMS, it still has poor reproducibility of laser source as one of laser MS, and need further research. China is developing rapidly in import and independent R&D of AMS, but there are many problems in the spent fuel and other nuclear industry related application and R&D field, such as low sensitivity and limited determination of special or several nuclides. The main application of AMS with gas ion source is determination of 14C, and the sensitivity reaches to 10-16. Until now, the R&D of gas ion source for AMS hasn’t be reported in China. This study discussed future developing direction of relevant mass spectrometry and outlined the potential solutions. In order to improve the efficiency of MS application on HTGR research, it is urgent to develop the easy operating intelligent instruments with small volume and simple structure.

     

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