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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 and posted on 29.04.2019 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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