Owing to its low cost, abundancy, and potential catalytic applications, molybdenum disulfide (MoS2) attracts a great deal of attention for rational designing of cheap and efficient catalyst for alcohol synthesis from syngas. Because of the inertness of basal plane, it is necessary to find way to activate MoS2 for enhancing its reactivity. Herein, by means of density functional theory calculations of reaction pathways and activation energy barriers, we show that MoS2 with sulfur vacancy row supported by the Cu(111) surface is a promising catalyst for higher alcohol synthesis from syngas. Our calculations suggest that the potential products of the synthesis include methanol, ethanol, formaldehyde, methane, and water, among which ethanol, methane, and water are thermodynamically favorable. The reactivity of the catalyst is traced to the strong MoS2-Cu(111) interaction which leads to enlargement of vacancy row region, and to the charge transfer from Cu to MoS2 resulting in a shift of the frontier states (d orbitals of the exposed Mo atoms) making it closer to the Fermi level. Kinetic Monte Carlo (kMC) simulations show that about 80% selectivity towards ethanol can be achieved with H2/CO ratio of 0.5-1.5 and at a pressure of 1-2MPa, an ideal condition for industrial catalysts. Overall, our results from DFT+kMC simulations provide insights into the reaction mechanism behind the conversion of syngas into the higher alcohols, and thus help providing guidelines for rational design of MoS2/Cu-based catalyst for higher alcohol synthesis from syngas.

Copper-supported single layer MoS2 for higher alcohol synthesis from syngas: A DFT + kMC study

2019 Spring National Meeting

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