氢同位素在锆合金中的扩散研究进展

    Diffusion of Hydrogen Isotopes in Zirconium Alloys

    • 摘要: 氚,是核电站常见的放射性产物,因原子半径小极易扩散渗透且易被生物体吸收,放射性危害大。压水堆中裂变产生的氚主要经由燃料包壳进入一回路,是氚重要的释放来源。2011年日本福岛事故发生后,氢同位素在锆合金包壳中的扩散研究引发极大关注。本文概述了近60年氢同位素在锆合金中扩散系数的测量方法,如质谱法、电化学法等,并介绍了主要测试方法的研究进展。研究结果表明,合金元素成分变化、表面氧化物、氢化物形成是影响氢同位素在锆合金中扩散的关键因素。分别探讨了在这些影响因素下氢同位素在锆合金中扩散系数的实验和计算方法。此外,还对未来氢同位素在锆合金中扩散研究的方向进行了讨论,可为先进燃料包壳、耐事故涂层的氚扩散系数测量以及氚渗透风险评价提供参考。

       

      Abstract: Tritium is a common radioactive product in nuclear power plants. It is easy to diffuse, penetrate and be easily absorbed by organisms due to its small atomic radius. The tritium produced by fission in pressurized water reactors(PWR) mainly enters the primary circuit through the fuel envelope and serves as an important source of tritium release. Following the Fukushima accident in Japan in 2011, the diffusion of hydrogen isotopes in zirconium alloy cladding has garnered significant attention. The diffusion coefficient, a key parameter for evaluating the risks associated with hydrogen isotope diffusion, is typically measured using gas-driven permeation and electrochemical hydrogen permeation testing methods, as introduced in this study. Moreover, the diffusion mechanism of hydrogen through zirconium alloys under different conditions is discussed in detail. Alloying elements and impurities in zirconium alloys have been reported to provide hydrogen trapping sites. When tin(Sn), iron(Fe), chromium(Cr) and nickel(Ni) coexist, the hydrogen diffusion coefficient decreases. The formation of zirconium hydride and oxides also affects the hydrogen isotope permeation rates differently. Due to lattice distortion and formation of microcracks in zirconium alloy, zirconium hydride results in an increased hydrogen isotope diffusion coefficient. Conversely, the formation of oxides, such as zirconia, on the surface of zirconium alloys can act as hydrogen permeation barriers, preventing further permeation or absorption of hydrogen isotope atoms. A more detailed discussion is presented in the paper. In light of these findings, further exploration of the behavior of hydrogen isotopes in zirconium alloy cladding is essential to enhance the safety of nuclear power plants. To this end, future research endeavors should focus on advanced hydrogen analytical techniques and multiscale modeling approaches. Innovative experimental methodologies could yield more precise data on hydrogen diffusion. Leveraging advanced analytical techniques such as neutron scattering and molecular dynamics simulations could provide deeper insights into the diffusion mechanisms. Integrating multiscale modeling approaches facilitates a comprehensive understanding of hydrogen diffusion in zirconium alloys. Combining atomistic simulations with continuum-scale models enables researchers to elucidate the complex interactions between hydrogen atoms, alloying elements, and microstructural features. Additional studies are necessary to investigate the diffusion of hydrogen isotopes in zirconium alloy in the near future.

       

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