Electrochemical carbonyl reduction on single-site M-N-C catalysts.

Autor: Ju W; Chemical Engineering Division, Department of Chemistry, Technical University Berlin, Berlin, Germany., Bagger A; Department of Physics, Technical University of Denmark, Lyngby, Denmark., Saharie NR; Institute Charles Gerhardt Montpellier, Univ. Montpellier, CNRS, ENSCM, Montpellier, France., Möhle S; Chemical Engineering Division, Department of Chemistry, Technical University Berlin, Berlin, Germany., Wang J; Chemical Engineering Division, Department of Chemistry, Technical University Berlin, Berlin, Germany., Jaouen F; Institute Charles Gerhardt Montpellier, Univ. Montpellier, CNRS, ENSCM, Montpellier, France., Rossmeisl J; Department of Chemistry, University Copenhagen, Universitetsparken 5, 2100, Copenhagen, Denmark., Strasser P; Chemical Engineering Division, Department of Chemistry, Technical University Berlin, Berlin, Germany. pstrasser@tu-berlin.de.
Jazyk: angličtina
Zdroj: Communications chemistry [Commun Chem] 2023 Sep 30; Vol. 6 (1), pp. 212. Date of Electronic Publication: 2023 Sep 30.
DOI: 10.1038/s42004-023-01008-y
Abstrakt: Electrochemical conversion of organic compounds holds promise for advancing sustainable synthesis and catalysis. This study explored electrochemical carbonyl hydrogenation on single-site M-N-C (Metal Nitrogen-doped Carbon) catalysts using formaldehyde, acetaldehyde, and acetone as model reactants. We strive to correlate and understand the selectivity dependence on the nature of the metal centers. Density Functional Theory calculations revealed similar binding energetics for carbonyl groups through oxygen-down or carbon-down adsorption due to oxygen and carbon scaling. Fe-N-C exhibited specific oxyphilicity and could selectively reduce aldehydes to hydrocarbons. By contrast, the carbophilic Co-N-C selectively converted acetaldehyde and acetone to ethanol and 2-propanol, respectively. We claim that the oxyphilicity of the active sites and consequent adsorption geometry (oxygen-down vs. carbon-down) are crucial in controlling product selectivity. These findings offer mechanistic insights into electrochemical carbonyl hydrogenation and can guide the development of efficient and sustainable electrocatalytic valorization of biomass-derived compounds.
(© 2023. Springer Nature Limited.)
Databáze: MEDLINE
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