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Electrochemical polarization of disparate catalytic sites drives thermochemical rate enhancement

Daniel, IsaacT., Kim, Bohyeon, Douthwaite, Mark, Pattisson, Samuel, Lewis, Richard J., Cline, Joseph, Morgan, David J. ORCID: https://orcid.org/0000-0002-6571-5731, Bethell, Donald, Kiely, Christopher J., McIntosh, Steven and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2023. Electrochemical polarization of disparate catalytic sites drives thermochemical rate enhancement. ACS Catalysis 13 (21) , pp. 14189-14198. 10.1021/acscatal.3c03364

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Abstract

Supported bimetallic catalysts commonly exhibit higher rates of reaction compared to their monometallic counterparts, but the origin of these enhancements is often poorly defined. The recent discovery that cooperative redox enhancement effects in Au–Pd systems promote bimetallic catalysis in thermochemical oxidation is an important development in this field. This effect aligns two important research fields, thermo- and electrocatalysis, but questions relating to the generality and origin of the effect remain. Here, we demonstrate that these effects can be observed in reactions over a range of bimetal combinations and reveal the origin using a combination of electrochemical and material characterization. We disclose that the observed activity enhancement in thermochemical systems is a result of the electrochemical polarization of two disparate catalytic sites. This forms an alternative operating potential for a given bimetallic system that increases the driving force of each of the composite half reactions in oxidative dehydrogenation. We therefore uncover the physicochemical descriptors that dictate whether these enhancement effects will be exhibited by a particular combination of supported metal catalysts and determine the magnitude of the effect.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Cardiff Catalysis Institute (CCI)
Chemistry
Additional Information: License information from Publisher: LICENSE 1: URL: https://creativecommons.org/licenses/by/4.0/, Start Date: 2023-10-20
Publisher: American Chemical Society
ISSN: 2155-5435
Date of First Compliant Deposit: 7 November 2023
Date of Acceptance: 28 September 2023
Last Modified: 05 Jan 2024 04:44
URI: https://orca.cardiff.ac.uk/id/eprint/163702

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