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Identification of active catalysts for the acceptorless dehydrogenation of alcohols to carbonyls

Wang, Tao, Sha, Jin, Sabbe, Maarten, Sautet, Philippe, Pera-Titus, Marc and Michel, Carine 2021. Identification of active catalysts for the acceptorless dehydrogenation of alcohols to carbonyls. Nature Communications 12 (1) , 5100. 10.1038/s41467-021-25214-1

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Abstract

Acceptorless dehydrogenation into carbonyls and molecular hydrogen is an attractive strategy to valorize (biobased) alcohols. Using 2-octanol dehydrogenation as benchmark reaction in a continuous reactor, a library of metal-supported catalysts is tested to validate the predictive level of catalytic activity for combined DFT and micro-kinetic modeling. Based on a series of transition metals, scaling relations are determined as a function of two descriptors, i.e. the surface binding energies of atomic carbon and oxygen. Then, a volcano-shape relation based on both descriptors is derived, paving the way to further optimization of active catalysts. Evaluation of 294 diluted alloys but also a series of carbides and nitrides with the volcano map identified 12 promising candidates with potentially improved activity for alcohol dehydrogenation, which provides useful guidance for experimental catalyst design. Further screening identifies β-Mo2N and γ-Mo2N exposing mostly (001) and (100) facets as potential candidates for alcohol dehydrogenation.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Additional Information: This article is licensed under a Creative Commons Attribution 4.0 International License
Publisher: Nature Research
ISSN: 2041-1723
Date of First Compliant Deposit: 10 March 2022
Date of Acceptance: 20 July 2021
Last Modified: 22 Mar 2022 10:15
URI: https://orca.cardiff.ac.uk/id/eprint/148282

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