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Methanol carbonylation to acetaldehyde on Au particles supported by single-layer MoS2 grown on silica

Journal Article · · Journal of Physics. Condensed Matter
 [1];  [2];  [2];  [2];  [2];  [3];  [4];  [1];  [1];  [4];  [1];  [2];  [2]
  1. Univ. of California, Riverside, CA (United States)
  2. Univ. of Central Florida, Orlando, FL (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. of Nebraska, Lincoln, NE (United States)
+ Show Author Affiliations
Homogenous single-layer MoS2 films coated with sub-single layer amounts of gold are found to isolate the reaction of methanol with carbon monoxide, the fundamental step toward higher alcohols, from an array of possible surface reactions. Active surfaces were prepared from homogenous single-layer MoS2 films coated with sub-single layer amounts of gold. These gold atoms formed clusters on the MoS2 surface. A gas mixture of carbon monoxide (CO) and methanol (CH3OH) was partially converted to acetaldehyde (CH3CHO) under mild process conditions (308 kPa and 393 K). This carbonylation of methanol to a C2 species is a critical step toward the formation of higher alcohols. Density functional theory modeling of critical steps of the catalytic process identify a viable reaction pathway. Imaging and spectroscopic methods revealed that the single layer of MoS2 facilitated formation of nanoscale gold islands, which appear to sinter through Ostwald ripening. Here, the formation of acetaldehyde by the catalytic carbonylation of methanol over supported gold clusters is an important step toward realizing controlled production of useful molecules from low carbon-count precursors.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; FG02-07ER15842
OSTI ID:
1855628
Journal Information:
Journal of Physics. Condensed Matter, Journal Name: Journal of Physics. Condensed Matter Journal Issue: 10 Vol. 34; ISSN 0953-8984
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

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Supplementary data for "Methanol carbonylation to acetaldehyde on Au particles supported by single-layer MoS2 grown on silica" journalarticle January 2021

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Related Subjects

2D catalyst
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
DFT
MoS 2
acetaldehyde
gold
methanol