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

Journal Article · Fri May 01 00:00:00 EDT 2020 · Journal of Vacuum Science and Technology A

DOI:https://doi.org/10.1116/1.5142853· OSTI ID:1800399

Jiang, Tao ^[1]; Le, Duy ^[2]; Rahman, Talat S. ^[2]

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1. Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics; University of Central Florida
2. 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

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*).

• Research Organization: Univ. of Central Florida, Orlando, FL (United States)
• Sponsoring Organization: USDOE Office of Science (SC)
• Grant/Contract Number: FG02-07ER15842
• OSTI ID: 1800399
• Journal Information: Journal of Vacuum Science and Technology A, Journal Name: Journal of Vacuum Science and Technology A Journal Issue: 3 Vol. 38; ISSN 0734-2101
• Publisher: American Vacuum Society / AIP
• Country of Publication: United States
• Language: English

Related Subjects

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