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Density functional theory study of the adsorption of elemental mercury on a 1T-MoS2 monolayer

关于单层1T-MoS2 吸附元素汞的密度泛函理论研 究

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Abstract

Elemental mercury has become a global concern because of its significant impact on human health and the ecosystem. A lot of effort has been put towards the removal of elemental mercury from the 2H-MoS2 (prismatic structure of MoS2). However, the mechanism of 1T-MoS2 (polytype structure of MoS2) in Hg0 capture remains unexplored. In this study, density functional theory (DFT) was adopted to investigate the adsorption mechanism of Hg on a 1T-MoS2 monolayer. The different possible adsorption positions on the 1T-MoS2 were examined. For different adsorption configurations, the changes in electronic property were also studied to understand the adsorption process. The results elucidated that chemisorption dominates the adsorption between Hg0 atoms and the 1T-MoS2. It was found that the TMo (on top of the Mo atom) position is the strongest adsorption configuration among all the possible adsorption positions. The adsorption of Hg0 atoms on the 1T-MoS2 monolayer is influenced by adjacent S and Mo atoms. The adsorbate Hg0 atom is found being oxidized on the TMo position of the 1T-MoS2 with an adsorption energy of −1.091 eV. From the partial density of states (PDOS) analysis of the atoms, the strong interaction between Hg0 and the 1T-MoS2 surface is caused by the significant overlap among the d orbitals of the mercury atom and the s orbital of the S atom and p and d orbitals of the Mo atom.

摘要

目 的

探索1T-MoS2 (多型结构的二硫化钼) 的除汞机制。

方 法

1. 采用密度泛函理论 (DFT) 分析Hg0 在1T-MoS2单层上的吸附机理。2. 考察1T-MoS2的不同吸附位置。3. 对不同的吸附构型, 研究电子吸附前后的变化, 从而进一步了解吸附过程。

结 论

1. 化学吸附是Hg 原子与1T-MoS2单层吸附的主导因素。同时, 在所有可能的吸附位置中, TMo (在钼原子上方) 的位置是最强烈的吸附构型。 2. 汞 (Hg) 原子在1T-MoS2单层上的吸附受邻近 的硫 (S) 和钼 (Mo) 原子的影响。3. 吸附的汞 (Hg) 原子在1T-MoS2的TMo位置上会被氧化, 其吸附能为−1.091 eV。4. 从局部态密度 (PDOS) 分析来看, Hg 原子和1T-MoS2表面之间的相互作 用是由汞 (Hg) 原子的d 轨道与硫 (S) 原子的s 轨道及钼 (Mo)原子的p 轨道和d 轨道重叠所致。

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Acknowledgements

The University of Nottingham Ningbo China is acknowledged for the provision of a full scholarship to the first author.

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Authors and Affiliations

  1. Municipal Key Laboratory of Clean Energy Conversion Technologies, The University of Nottingham Ningbo China, Ningbo, 315100, China

    Xue-liang Mu, Hai-tao Zhao & Tao Wu

  2. College of Energy Engineering, Zhejiang University, Hangzhou, 310027, China

    Xiang Gao & Hai-tao Zhao

  3. School of Chemistry, The University of Nottingham, Nottingham, NG7 2RD, UK

    Michael George

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  1. Xue-liang Mu
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  2. Xiang Gao
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  3. Hai-tao Zhao
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  4. Michael George
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  5. Tao Wu
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Correspondence to Tao Wu.

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Project supported by the Ningbo Bureau of Science and Technology (No. 2012B82011), the Ningbo Natural Science Foundation (No. 2017A610060), the National Natural Science Foundation of China (No. 51706114), and the China Postdoctoral Science Foundation (No. 2016M601942)

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Mu, Xl., Gao, X., Zhao, Ht. et al. Density functional theory study of the adsorption of elemental mercury on a 1T-MoS2 monolayer. J. Zhejiang Univ. Sci. A 19, 60–67 (2018). https://doi.org/10.1631/jzus.A1700079

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