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
Clicked: 4061
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.
@article{title="Density functional theory study of the adsorption of elemental mercury on a 1T-MoS2 monolayer",
author="Xue-liang Mu, Xiang Gao, Hai-tao Zhao, Michael George, Tao Wu",
journal="Journal of Zhejiang University Science A",
volume="19",
number="1",
pages="60-67",
year="2018",
publisher="Zhejiang University Press & Springer",
doi="10.1631/jzus.A1700079"
}
%0 Journal Article
%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
%A Tao Wu
%J Journal of Zhejiang University SCIENCE A
%V 19
%N 1
%P 60-67
%@ 1673-565X
%D 2018
%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A1700079
TY - JOUR
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
Y1 - 2018
PB - Zhejiang University Press & Springer
ER -
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.
[1]Aboud S, Sasmaz E, Wilcox J, 2008. Mercury adsorption on PdAu, PdAg and PdCu alloys. Main Group Chemistry, 7(3):205-215.
[2]Asasian N, Kaghazchi T, 2015. Sulfurized activated carbons and their mercury adsorption/desorption behavior in aqueous phase. International Journal of Environmental Science and Technology, 12(8):2511-2522.
[3]Atkins PW, 2001. Physical Chemistry. Oxford University Press, UK.
[4]Chadi DJ, 1977. Special points for Brillouin-zone integratuibs. Physical Review B, 13:5188-5192.
[5]Chhowalla M, Shin HS, Eda G, et al., 2013. The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets. Nature Chemistry, 5(4):263-275.
[6]Clark SJ, Segall MD, Pickard CJ, et al., 2005. First principles methods using CASTEP. Zeitschrift Fur Kristallographie, 220:567-570.
[7]Delley B, 1986. Calculated electron distribution for terafluoroterephthalonitrile (TFT). Chemical Physics, 110(2-3):329-338.
[8]EPA (Environmental Protection Agency), 2011. National Emission Standards for Hazardous Air Pollutants from Coil-and Oil-fired Electric Utility Steam Generating Units and Standards of Performance for Fossil-Fuel-Fired Electric Utility, Industrial-Commercial-Institutional, and Small Industrial-Commercial-Institutional Steam Generating Units. https://www.federalregister.gov/articles/2016/04/ 06/2016-06563/national-emission-standards-for-hazardous-air-pollutants-from-coal--and-oil-fired-electric-utility [Accessed on Feb. 15, 2016].
[9]Enyashin AN, Seifert G, 2012. Density-functional study of LixMoS2 intercalates (0≤x≤1). Computational and Theoretical Chemistry, 999:13-20.
[10]Galbreath KC, Zygarlicke CJ, 1996. Mercury speciation in coal combustion and gasification flue gases. Environmental Science & Technology, 30(8):2421-2426.
[11]Gao G, Jiao Y, Ma F, et al., 2015. Charge mediated semiconducting-to-metallic phase transition in molybdenum disulfide monolayer and hydrogen evolution reaction in new 1T’ phase. The Journal of Physical Chemistry C, 119(23):13124-13128.
[12]Gao Y, Zhang Z, Wu J, et al., 2013. A critical review on the heterogeneous catalytic oxidation of elemental mercury in flue gases. Environmental Science & Technology, 47(19):10813-10823.
[13]Eda G, Fujita T, Yamaguchi H, et al., 2012. Coherent atomic and electronic heterostructures of single-layer MoS2. ACS Nano, 6(8):7311-7317.
[14]Hasnip PJ, Refson K, Probert MI, et al., 2014. Density functional theory in the solid state. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, 372:20130270.
[15]Huang Z, Hao G, He C, et al., 2013. Density functional theory study of Fe adatoms adsorbed monolayer and bilayer MoS2 sheets. Journal of Applied Physics, 114:083706.
[16]Johansen VC, 2003. Mercury speciation in other combustion sources: a literature review. Portland Cement Association, 2578:20.
[17]Jones DW, 1999. Exposure or absorption and the crucial question of limits for mercury. Journal of the Canadian Dental Association, 65(1):42-46.
[18]Liang S, Wang Y, Cinnirella S, et al., 2015. Atmospheric mercury footprints of nations. Environmental Science & Technology, 49(6):3566-3574.
[19]Lim D, Wilcox J, 2013. Heterogeneous mercury oxidation on Au(111) from first principles. Environmental Science & Technology, 47(15):8515-8522.
[20]Liu D, Chen X, Li D, 2010. Simulation of MoS2 crystal structure and the experimental study of thermal decomposition. Journal of Molecular Structure, 980(1-3):66-71.
[21]Ortmann F, Bechstedt F, Schmidt WG, 2006. Semiempirical van der Waals correction to the density functional description of solids and molecular structures. Physical Review B, 73(20):205101.
[22]Pfrommer BG, Cote M, Louie SG, et al., 1997. Relaxation of crystals with the quasi-Newton method. Journal of Computational Physics, 131:233-240.
[23]Praveen A, 2003. Mercury Emissions from Coal Fired Power Plants. Northeast States for Coordinated Air Use Management.
[24]Presto AA, Granite EJ, 2006. Survey of Catalysts for Oxidation of Mercury in Flue Gas. Environmental Science & Technology, 40(18):5601-5609.
[25]Putungan DB, Kuo JL, 2014. Structural and electronic properties of monolayer 1T-MoS2 phase, and its interaction with water adsorbed on perfect, single S-vacated and MoS2-unit-vacated surface: density functional theory calculations. Integrated Ferroelectrics, 156(1):93-101.
[26]Sato T, Nakai H, 2009. Density functional method including weak interactions: dispersion coefficients based on the local response approximation. The Journal of Chemical Physics, 131(22):224104.
[27]UNEP (United Nations Environment Programme), 2002. Global Mercury Assessment. http://www.unep.org [Accessed on Jan. 15, 2016].
[28]UNEP (United Nations Environment Programme), 2013a. Final Act of the Conference of Plenipotentiaries on the Minamata Convention on Mercury. http://www.mercuryconvention.org [Accessed on Apr. 15, 2016].
[29]UNEP (United Nations Environment Programme), 2013b. Global Mercury Assessment 2013: Sources, Emissions, Releases, and Environmental Transport. https://www. unep.org [Accessed on Apr. 15, 2016].
[30]UNEP (United Nations Environment Programme), 2013c. The Minamata Convention on Mercury. https://www. mercuryconvention.org/Convention/tabid/3426/ [Accessed on Apr. 15, 2016].
[31]Vanderbilt D, 1990. Soft self-consistent pseudopotentials in a generalized eigenvalue formalism. Physical Review B, 41(11):7892-7895.
[32]Wypych F, Schollhorn R, 1992. 1T-MoS2, a new metallic modification of molybdenum disulfide. Journal of the Chemical Society, Chemical Communications, (19):1386-1388.
[33]Wypych F, Weber T, Prins R, 1998. Scanning tunneling microscopic investigation of 1T-MoS2. Chemistry of Materials, 10(3):723-727.
[34]Yin Z, Li H, Li H, et al., 2011. Single-layer MoS2 phototransistors. ACS Nano, 6(1):74-80.
[35]Zhao H, Yang G, Gao X, et al., 2016. Hg0 capture over CoMoS/γ-Al2O3 with MoS2 nanosheets at low temperatures. Environmental Science & Technology, 50(2):1056-1064.
Open peer comments: Debate/Discuss/Question/Opinion
<1>