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CLC number: X511; TK09

On-line Access: 2018-01-12

Received: 2017-02-13

Revision Accepted: 2017-10-17

Crosschecked: 2017-12-15

Cited: 1

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Citations:  Bibtex RefMan EndNote GB/T7714

 ORCID:

Tao Wu

https://orcid.org/0000-0001-6469-9613

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Journal of Zhejiang University SCIENCE A 2018 Vol.19 No.1 P.60-67

http://doi.org/10.1631/jzus.A1700079


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


Author(s):  Xue-liang Mu, Xiang Gao, Hai-tao Zhao, Michael George, Tao Wu

Affiliation(s):  Municipal Key Laboratory of Clean Energy Conversion Technologies, The University of Nottingham Ningbo China, Ningbo 315100, China; more

Corresponding email(s):   tao.wu@nottingham.edu.cn

Key Words:  1T-MoS2 monolayer, Mercury capture, Adsorption mechanism, Density functional theory (DFT)


Xue-liang Mu, Xiang Gao, Hai-tao Zhao, Michael George, Tao Wu. Density functional theory study of the adsorption of elemental mercury on a 1T-MoS2 monolayer[J]. Journal of Zhejiang University Science A, 2018, 19(1): 60-67.

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author="Xue-liang Mu, Xiang Gao, Hai-tao Zhao, Michael George, Tao Wu",
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publisher="Zhejiang University Press & Springer",
doi="10.1631/jzus.A1700079"
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%T Density functional theory study of the adsorption of elemental mercury on a 1T-MoS2 monolayer
%A Xue-liang Mu
%A Xiang Gao
%A Hai-tao Zhao
%A Michael George
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%J Journal of Zhejiang University SCIENCE A
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%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A1700079

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T1 - Density functional theory study of the adsorption of elemental mercury on a 1T-MoS2 monolayer
A1 - Xue-liang Mu
A1 - Xiang Gao
A1 - Hai-tao Zhao
A1 - Michael George
A1 - Tao Wu
J0 - Journal of Zhejiang University Science A
VL - 19
IS - 1
SP - 60
EP - 67
%@ 1673-565X
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PB - Zhejiang University Press & Springer
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DOI - 10.1631/jzus.A1700079


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.

关于单层1T-MoS2吸附元素汞的密度泛函理论研究

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.

关键词:单层1T-MoS2;汞捕捉;吸附机制;密度泛函理论(DFT)

Darkslateblue:Affiliate; Royal Blue:Author; Turquoise:Article

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