辐照后HTR-10球形燃料元件电化学解体及裂变产物分布研究

Electrochemical Deconsolidation and Fission Product Distribution of Post-irradiated HTR-10 Spherical Fuel Element

  • 摘要: 辐照后检验是开展燃料性能评价的重要手段。在10 MW高温气冷堆(HTR-10)球形燃料元件的辐照后检验中,为研究元件中TRISO包覆燃料颗粒的破损机制,本文利用基于电化学氧化原理的两步解体法,对所选元件(燃耗约35 GW·d/tU)进行了包覆燃料颗粒与基体石墨的分离,获得了元件中不同位置区域的包覆燃料颗粒、解体石墨粉和电解液,通过γ能谱定量分析了解体石墨粉和电解液中的放射性核素成分及含量,并基于此明确了放射性核素在辐照后球形燃料元件基体石墨中的分布。结果表明:部分电解液中裂变产物137Cs与144Ce活度显著高于其他电解液样品,表明其对应区域中可能存在破损包覆燃料颗粒;元件表层位置对应的电解液中活化产物60Co高于内部区域,主要来源于HTR10一回路的放射性粉尘沾污。本工作初步建立了高温气冷堆辐照后球形燃料元件电化学解体和解体样品分析测试的平台及方法,为TRISO型包覆燃料颗粒破损机制分析及其堆内行为研究提供了重要基础。

     

    Abstract: Post-irradiation examination is an essential method for fuel performance evaluation. In order to study the distribution of radionuclides in fuel elements as well as the irradiation damage mechanism of TRISO coated fuel particles in spherical fuel element of 10 MW high temperature gascooled reactor (HTR10), a spherical element with moderate burnup of about 35 GW·d/tU was disassembled by twostep electrochemical deconsolidation method. The principle of this method is electrochemical oxidation of graphite. Coated fuel particles, deconsolidated graphite matrix powder and electrolytes from different regions of the element were obtained. The radionuclides in powder and electrolyte were quantitatively analyzed by the γ spectrum method. The efficiency of the γ spectrum measuring system was calibrated by a semiempirical method in order to withstand the interference by background contaminations. The results show that there are two types of radionuclides in the irradiated HTR10 spherical fuel element deconsolidated graphite matrix powder and electrolyte. Fission product nuclides such as 144Ce/144Pr, 137Cs/134Cs, 152Eu/154Eu/155Eu and 95Zr/95Nb, are generated by fission reaction of free uranium contamination in the graphite matrix. Activation product nuclides such as 75Se, 60Co, 54Mn and 46Sc, are directly generated by the activation of impurities in the graphite matrix, and also adsorbed or contaminated from the primary activation fragments by the graphite matrix. The distribution of radionuclides in the graphite matrix of the irradiated spherical fuel element was also determined. Electrolyte samples with higher reactivity of 137Cs and 144Ce are found, indicating that the coated fuel particles in the corresponding area may be damaged. The damage can cause the fuel kernel to contact the electrolyte during the electrochemical disintegration process, and part of the radionuclides is dissolved into the electrolyte. The consistency of volatile and nonvolatile fission products indicates that the damaged particle didn’t undergo long high temperature history. The results show that the content of various fission products in the graphite matrix of the irradiated HTR10 fuel element is negligible when the structure of the coated fuel particle is intact, which reflects the good inclusion of the TRISO coated fuel particles on the radioactive fission products. On the other hand, the activation products are uniformly distributed in the interior of the whole spherical fuel element, while the content of activation products increases significantly on the outer surface of the element and nonuniformly distribute. In this work, a platform and a method for electrochemical deconsolidation of spherical fuel elements were established, as well as an analysis and a test on deconsolidation samples. Results are important for research on damage mechanism analysis and radiation behavior of TRISO coated fuel particles.

     

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