Mechanism of Methanol Decomposition over Single-Site Pt1/CeO2 Catalyst: A DRIFTS Study

Qi, Zhiyuan; Chen, Luning; Zhang, Shuchen; Su, Ji; Somorjai, Gabor A.

doi:10.1021/jacs.0c10728

Title: Mechanism of Methanol Decomposition over Single-Site Pt₁/CeO₂ Catalyst: A DRIFTS Study

Journal Article · Thu Dec 24 00:00:00 UTC 2020 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.0c10728 · OSTI ID:1835089

^[1]; Chen, Luning ^[1]; Zhang, Shuchen ^[1]; Su, Ji ^[1];

^[2]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Single-site catalysts have drawn broad attention in catalysis because of their maximum atomic utilization and unique catalytic performance. Early work in our group has shown a 40-fold higher activity of methanol decomposition over single-site Pt₁/CeO₂ catalyst than CeO₂ supported 2.5 nm Pt nanoparticles, while a molecular-level understanding of such enhancement is lacking. Herein, the reaction mechanism of methanol decomposition over Pt₁/CeO₂ was carefully investigated using in situ DRIFTS, and a reaction pathway was proposed. Methanol molecules were dissociatively adsorbed on nanoceria support first, followed by the diffusion of as-formed methoxy species onto Pt single sites where the dehydrogenation occurs and results in the weakly bonded CO. The ease of methanol dissociative adsorption on nanoceria support and the tailored electronic property of Pt₁ via the metal-support interaction are believed to be strongly correlated with the high activity of Pt₁/CeO₂.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1835089

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 1 Vol. 143; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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