Adsorption and separation effects of typical metal nuclides on the WS2 surface: a DFT study

IF 1.6 4区化学 Q4 CHEMISTRY, PHYSICAL

Theoretical Chemistry Accounts Pub Date : 2024-03-25 DOI:10.1007/s00214-024-03108-x

Haifei Chen, Yawei Chen, Yongsheng Cui, Shaoyang Ren, Xuan Chen

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Abstract

The fission products brought about by the growth of nuclear energy is increasing, and their radioactivity will seriously jeopardize human health and pollute the environment. The recycling of radioactive materials has become a problem that needs to be solved nowadays. In this paper, we simulate the adsorption behaviors of typical fission products Cs, Sr, and Co on the surface of WS₂ based on first-principle study. 3 × 3 supercell is selected by convergence test and calculate and compare the parameters of adsorption sites, adsorption energy, and charge transfer. At the microelectronic level, we analyze the interactions of WS₂ with the three nuclides in detail. In addition, the effect of temperature on the adsorption rate of each nuclide on the WS₂ surface is further evaluated by empirical equations. The results show that fissionable metal nuclides tend to be located at the top of the metal atoms of two-dimensional transition metal sulfides (top site of the W atom of WS₂), and Co, moreover, has a much larger adsorption energy than that of Cs and Sr due to its binding to W in a form similar to covalent bonds. Moreover, under high temperature conditions, WS₂ is more favorable for selecting Co and separating it from Cs and Sr. WS₂ is expected to be an excellent material for the separation and recovery of radionuclide Co.

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典型金属核素在 WS2 表面的吸附和分离效应：DFT 研究

核能发展带来的裂变产物越来越多，其放射性将严重危害人类健康和污染环境。放射性物质的回收利用已成为当前亟待解决的问题。本文基于第一性原理研究，模拟了典型裂变产物铯、锶和钴在 WS2 表面的吸附行为。通过收敛测试选择了 3 × 3 超级囚室，并计算和比较了吸附位点、吸附能和电荷转移等参数。在微电子层面，我们详细分析了 WS2 与三种核素的相互作用。此外，我们还通过经验方程进一步评估了温度对每种核素在 WS2 表面吸附率的影响。结果表明，裂变金属核素倾向于位于二维过渡金属硫化物的金属原子顶部（WS2 的 W 原子顶部位点），而 Co 由于以类似共价键的形式与 W 结合，其吸附能比 Cs 和 Sr 大得多。此外，在高温条件下，WS2 更有利于选择 Co 并将其从 Cs 和 Sr 中分离出来。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Theoretical Chemistry Accounts 化学-物理化学

CiteScore

3.40

自引率

0.00%

发文量

审稿时长

3.8 months

期刊介绍： TCA publishes papers in all fields of theoretical chemistry, computational chemistry, and modeling. Fundamental studies as well as applications are included in the scope. In many cases, theorists and computational chemists have special concerns which reach either across the vertical borders of the special disciplines in chemistry or else across the horizontal borders of structure, spectra, synthesis, and dynamics. TCA is especially interested in papers that impact upon multiple chemical disciplines.