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中国物理学会期刊

U3Si2中Xe的溶解扩散行为及Al原子掺杂的影响

Xenon Dissolution and Diffusion in U3Si2: The Influence of Aluminium Doping

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  • U3Si2作为一种极具潜力的耐事故燃料,其服役性能受到裂变气体积累及其诱导肿胀行为的显著影响。作为主要裂变气体产物,Xe占裂变气体总量的85%以上。本文采用第一性原理方法,系统研究了U3Si2中Xe的溶解、成团与扩散行为。由于Xe原子尺寸较大,其更易溶解于U3Si2中的空位缺陷,并且在间隙位点难以自发形成稳定的双原子团簇。扩散势垒计算结果表明,Xe在U3Si2中的扩散具有明显各向异性:间隙扩散能垒较高,而空位辅助扩散能垒显著较低,说明空位辅助机制主导Xe在U3Si2中的扩散过程。此外,Al掺杂可进一步降低局域环境中Xe的溶解能和扩散势垒,表明其有利于Xe的局域溶解、成团与扩散。上述结果从原子尺度阐明了Xe在U3Si2中的行为特征及Al掺杂的影响,并为理解裂变气体的早期演化行为及优化U3Si2燃料体系提供了理论依据。

     

    U3Si2 is regarded as a highly promising accident-tolerant fuel because of its high uranium density, high thermal conductivity, and favorable thermophysical properties. Under irradiation, however, the accumulation, migration, and aggregation of fission-gas atoms, particularly Xe, can induce bubble formation, fuel swelling, and performance degradation. In this work, first-principles calculations based on density functional theory with the Hubbard correction (DFT+U) were performed to systematically investigate the dissolution, cluster formation, and diffusion behaviors of Xe in U3Si2, as well as the effect of local Al doping on these processes. The results show that Xe has large positive dissolution energies at interstitial sites, indicating an extremely low interstitial solubility in U3Si2. Among the interstitial configurations considered, only the Int1 site can stably accommodate a Xe atom, whereas Xe atoms at the other interstitial sites are unstable after structural relaxation. In contrast, Xe is more favorably incorporated into vacancy defects because of the larger local free volume provided by vacancies. The calculated binding energies of Xe-Xe pairs at neighboring interstitial sites are negative, indicating that Xe does not spontaneously form stable diatomic clusters through an interstitial clustering mechanism in U3Si2. Migration-barrier calculations further reveal a clear mechanistic difference in Xe diffusion. Interstitial diffusion involves relatively high migration barriers and pronounced anisotropy, whereas vacancy-assisted diffusion exhibits much lower barriers, indicating that vacancy-assisted migration is the dominant diffusion mechanism for Xe in U3Si2. The introduction of Al further modifies the local behavior of Xe. Al doping lowers the dissolution energy of Xe at both interstitial and vacancy-related sites, reduces the local lattice distortion induced by Xe incorporation, and changes the Xe-Xe interaction at neighboring interstitial sites from repulsive to attractive. In addition, Al doping significantly decreases the migration barriers of representative interstitial and vacancy-assisted diffusion pathways, although it does not change the dominant role of the vacancy-assisted diffusion mechanism. These results indicate that local Al doping can promote the dissolution, cluster formation, and diffusion of Xe in U3Si2, and may therefore accelerate the subsequent evolution of fission-gas behavior. This work clarifies the atomic-scale evolution characteristics of Xe in U3Si2 and reveals the potentially unfavorable effect of Al doping on the resistance of U3Si2 to fission-gas-induced swelling. The present results provide a theoretical basis for understanding fission-gas behavior in U3Si2-based fuels and for optimizing their performance as accident-tolerant nuclear fuels.

     

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