Insights into the effect of metal ratio on cooperative redox enhancement effects over au- and pd-mediated alcohol oxidation

Zhao, Liang, Akdim, Ouardia, Huang, Xiaoyang, Wang, Kai, Douthwaite, Mark, Pattisson, Samuel, Lewis, Richard J., Lin, Runjia, Yao, Bingqing, Morgan, David J. ORCID: https://orcid.org/0000-0002-6571-5731, Shaw, Greg, He, Qian ORCID: https://orcid.org/0000-0003-4891-3581, Bethell, Donald, McIntosh, Steven, Kiely, Christopher J. ORCID: https://orcid.org/0000-0001-5412-0970 and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2023. Insights into the effect of metal ratio on cooperative redox enhancement effects over au- and pd-mediated alcohol oxidation. ACS Catalysis 13 (5) , pp. 2892-2903. 10.1021/acscatal.2c06284

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Abstract

The aerobic oxidation of alcohols and aldehydes over supported heterogeneous catalysts can be considered as comprising two complementary and linked processes: dehydrogenation and oxygen reduction. Significant rate enhancements can be observed when these processes are catalyzed by independent active sites, coupled by electron transport between the two catalysts. This effect, termed cooperative redox enhancement (CORE), could significantly influence how researchers approach catalyst design, but a greater understanding of the factors which influence it is required. Herein, we demonstrate that the Au/Pd ratio used in physical mixtures of monometallic catalysts and phase-separated Au and Pd bimetallic catalysts dramatically influences the degree to which CORE effects can promote alcohol oxidation. Perhaps more interestingly, the roles of Au and Pd in this coupled system are determined to be interchangeable. Preliminarily, we hypothesize that this is attributed to the relative rates of the coupled reactions and demonstrate how physical properties can influence this. This deeper understanding of the factors which influence CORE is an important development in bimetallic catalysis.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	American Chemical Society
ISSN:	2155-5435
Funders:	Chinese Scholarship Council, EPSRC National Facility for XPS (�HarwellXPS�)
Date of First Compliant Deposit:	17 February 2023
Date of Acceptance:	30 January 2023
Last Modified:	05 Jan 2024 08:25
URI:	https://orca.cardiff.ac.uk/id/eprint/157112

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