High current density microkinetic and electronic structure analysis of CO2 reduction using Co and Fe complexes on gas diffusion electrode

Xiaofei Lu, Busra Dereli, Tatsuya Shinagawa, Mohamed Eddaoudi, Luigi Cavallo, Kazuhiro Takanabe

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10 Scopus citations

Abstract

Reaction mechanisms of electrocatalytic CO2 reduction into CO over Co or Fe complexes were examined using gas diffusion electrodes to meet the requirement of high current densities for industrial deployment. Our experimental and theoretical calculation results consistently revealed that the Fe-based molecular catalysts exhibited more positive redox potentials relevant to CO2 electrocatalysis but disfavored the desorption of generated CO, especially at high overpotentials, failing to achieve appreciable reaction rates. Distinctively, the heterogenized Co-based molecular complexes were found to be tolerant to the high coverage of CO at steady state on the active site and achieved rates exceeding 100 mA cm−2 toward exclusive CO evolution. Density-functional theory calculations not only disclosed the redox non-innocent tetraphenylporphyrins and phthalocyanines during electrocatalytic CO2 reduction but also corroborated the energetics, especially for CO2 and CO adsorption, accounting for distinctive reaction pathways between Co and Fe complexes.
Original languageEnglish (US)
JournalChem Catalysis
DOIs
StatePublished - Apr 12 2022

Bibliographical note

KAUST Repository Item: Exported on 2022-04-14
Acknowledgements: Part of this work was supported by JSPS KAKENHI grant 19KK0126 and King Abdullah University of Science and Technology AMPM research center collaborative funding

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