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Towards Higher Alcohol Formation using a single-layer MoS2 activated Au on Silica: Methanol Carbonylation to Acetaldehyde

preprint
submitted on 25.04.2019, 21:13 and posted on 29.04.2019, 18:21 by Kortney Almeida, Katerina L. Chagoya, Alan Felix, Tao Jiang, Duy Le, Takat B. Rawal, Prescott E. Evans, Michelle Wurch, 1 Koichi Yamaguchi, Peter A. Dowben, Ludwig Bartels, Talat S. Rahman, Richard G. Blair

We demonstrate that a fused silica substrate can be rendered active for acetaldehyde (CH3CHO) synthesis from a gas mixture of carbon monoxide (CO) and methanol (CH3OH) under mild process conditions (308 kPa and 393 K) by deposition first of a homogenous single-layer MoS2 film and subsequently of a sub-mnonolayer (1 Angstrom) loading of gold. In operando monitoring of the catalyst performance in a flow reactor reveals uncompromised activity even after 2 hours on stream. The carbonylation of methanol to a C2 species represents a crucial step toward the formation of higher alcohols from syngas derived from methane or biomass. Characterization of the film by imaging and spectroscopy reveals that the single-layer MoS2 film disperses the gold loading into nanoscale islands; density functional theory (DFT) calculations identify low-coordinated edge sites on these islands as active centers for the carbon-carbon coupling at barriers significantly below 1 eV.

Funding

US Department of Energy grant DE-FG02-07ER15842

History

Email Address of Submitting Author

bartels@ucr.edu

Institution

University of California at Riverside

Country

USA

ORCID For Submitting Author

0000-0002-3964-4538

Declaration of Conflict of Interest

None

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