MoS2-supported Au31 for CO hydrogenation: A first-principle study

Jiang, Tao; Le, Duy; Rahman, Talat S.

doi:10.1116/1.5142853

Title: MoS₂-supported Au₃₁ for CO hydrogenation: A first-principle study

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Abstract

While the basal plane of single-layer molybdenum disulphide (MoS₂) is inert, attempts have been made to functionalize it chemically through the creation of defects and/or addition of dopants. With nanoparticles as dopants, the authors present density functional theory-based calculations of the hydrogenation of CO on a 31-atom, bilayer Au cluster supported on single-layer MoS₂ (Au31/MoS₂). Not surprisingly, the adsorption and reaction of all species involved in the hydrogenation occur at the edges of the cluster—the regions at which the interaction between MoS₂ and the Au cluster is tracked to be the strongest. The authors find two possible mechanisms that lead to the formation of methanol: (1) CO* → CHO* → CH₂O* → CH₃O* → CH₃OH* and (2) CO* → CHO* → HCOH* → CH2OH* → CH3OH*, where * indicates the adsorbed species. Detailed analysis of the reaction pathways, however, does not result in favoring one mechanism over the other. Rather, both mechanisms are facile. In addition, the rate-limiting step in each mechanism is found to be the formation of the formyl radical group (CO* + H* → CHO*).

Authors:

^[1];

^[2];

^[2]

Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics
Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics; Univ. of Central Florida, Orlando, FL (United States). Renewable Energy and Chemical Transformations Cluster

Publication Date:: Fri May 01 00:00:00 EDT 2020

Research Org.:: Univ. of Central Florida, Orlando, FL (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1800399

Grant/Contract Number:: FG02-07ER15842

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Vacuum Science and Technology A

Additional Journal Information:: Journal Volume: 38; Journal Issue: 3; Journal ID: ISSN 0734-2101

Publisher:: American Vacuum Society / AIP

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Materials Science; Physics; First-principle calculations; Syngas; Hydrogenation process; Density functional theory; Adsorption; Reaction mechanisms; Crystal structure; 2D materials; Transition metal chalcogenides; Nanoparticles

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                    Jiang, Tao, Le, Duy, and Rahman, Talat S. MoS2-supported Au31 for CO hydrogenation: A first-principle study.  United States: N. p., 2020. 
Web.  doi:10.1116/1.5142853.

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                    Jiang, Tao, Le, Duy, & Rahman, Talat S. MoS2-supported Au31 for CO hydrogenation: A first-principle study.  United States.  https://doi.org/10.1116/1.5142853

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                    Jiang, Tao, Le, Duy, and Rahman, Talat S. Fri .  
"MoS2-supported Au31 for CO hydrogenation: A first-principle study".  United States.  https://doi.org/10.1116/1.5142853.  https://www.osti.gov/servlets/purl/1800399.

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@article{osti_1800399,

  title        = {MoS2-supported Au31 for CO hydrogenation: A first-principle study},

  author       = {Jiang, Tao and Le, Duy and Rahman, Talat S.},

  abstractNote = {While the basal plane of single-layer molybdenum disulphide (MoS2) is inert, attempts have been made to functionalize it chemically through the creation of defects and/or addition of dopants. With nanoparticles as dopants, the authors present density functional theory-based calculations of the hydrogenation of CO on a 31-atom, bilayer Au cluster supported on single-layer MoS2 (Au31/MoS2). Not surprisingly, the adsorption and reaction of all species involved in the hydrogenation occur at the edges of the cluster—the regions at which the interaction between MoS2 and the Au cluster is tracked to be the strongest. The authors find two possible mechanisms that lead to the formation of methanol: (1) CO* → CHO* → CH2O* → CH3O* → CH3OH* and (2) CO* → CHO* → HCOH* → CH2OH* → CH3OH*, where * indicates the adsorbed species. Detailed analysis of the reaction pathways, however, does not result in favoring one mechanism over the other. Rather, both mechanisms are facile. In addition, the rate-limiting step in each mechanism is found to be the formation of the formyl radical group (CO* + H* → CHO*).},

  doi          = {10.1116/1.5142853},

  journal      = {Journal of Vacuum Science and Technology A},

  number       = 3,

  volume       = 38,

  place        = {United States},

  year         = {Fri May 01 00:00:00 EDT 2020},

  month        = {Fri May 01 00:00:00 EDT 2020}

}

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Title: MoS2-supported Au31 for CO hydrogenation: A first-principle study

Abstract

Citation Formats

Title: MoS₂-supported Au₃₁ for CO hydrogenation: A first-principle study