辐照石墨球中氚扩散系数测量方法研究

Measurement Method of Diffusion Coefficient of Tritium-in Irradiated Graphite Spheres

  • 摘要: 研究氚在石墨中的扩散行为,对于理解和掌握核能系统中氚的输运过程有着重要意义。目前氚在石墨中扩散系数的测量实验较少,所得数据相差很大。本文利用10 MW高温气冷实验堆(HTR-10)辐照石墨球,提出两种测量一定温度范围内氚在石墨中扩散系数的方法:一种是基于氚从石墨中的累积释放份额,另一种是基于氚从石墨中的释放率。在此基础上,设计了相应的实验系统,比较了两种测量方法的特点,基于累积释放份额的实验方法,适合对含有多种易于释放核素的介质材料进行测量,其近似公式的绝对误差在4×10-4以内。此外,结合HTR-10上氚源项研究结果探讨了氚在辐照石墨球中扩散行为的影响因素,为未来HTR-10辐照石墨球中测定氚的扩散系数和掌握氚在石墨材料中的输运机制提供了重要研究基础。

     

    Abstract: Tritium is the most important fuel in fusion reactors and one of the important radionuclides in fission reactors. The study of the diffusion behavior of tritium in graphite is of great significance to understand and grasp the transport process of tritium in nuclear energy systems. Regarding the measurement methods of diffusion coefficients, they can be classified into three types: permeation method, profiling method and release method. There are few experiments to measure the diffusion coefficient of tritium in graphite, and the obtained data vary greatly. Using the irradiated graphite spheres in 10 MW High Temperature Gas-cooled Experimental Reactor (HTR-10), two methods were proposed to measure the diffusion coefficient of tritium in graphite within a certain range of temperature. One is based on the cumulative release fraction of tritium from graphite, and the other is based on the release rate of tritium from graphite. The quantitative relationships between the cumulative release fraction and diffusion coefficient, and between the release rate and diffusion coefficient in spherical materials were derived in detail, and the factors that may have an influence on the experimental measurement results were discussed. The corresponding experimental systems were designed and the characteristics of the two measurement methods were compared. The experimental method based on the cumulative release fraction is suitable for the measurement of materials containing a variety of easily released nuclides, such as noble gas nuclides or 14C. The cumulative release fraction of tritium can be measured, and the measurement results will be not affected by the presence of other radionuclides. The advantage of the experimental method based on the release rate is that it is a fast and real-time measurement method. However, if other radionuclides are present in the irradiated graphite spheres, they can interfere with the online measured values of tritium. The factors affecting the diffusion behavior of tritium in irradiated graphite spheres were discussed in conjunction with the results of the tritium source term study on HTR-10. The diffusion behavior of tritium in HTR-10 irradiated graphite spheres may be affected by the microstructure and composition of the material. Future studies based on the first-principle calculations should consider the impurities, defects, and grain boundaries of graphite materials to determine the theoretical diffusion coefficients, and compare them with experimental measurements to elucidate the diffusion mechanism of tritium in graphite materials. Current study can provide an important research basis for determining the diffusion coefficient of tritium in irradiated graphite spheres of HTR-10 and mastering the transport mechanism of tritium in graphite materials in the future.

     

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