Correlations between experiments and simulations for formic acid oxidation
Bagger, Alexander (University of Copenhagen. Department of Chemistry)
Jensen, Kim D. (University of Copenhagen. Department of Chemistry)
Rashedi, Maryam (University of Tehran. College of Science)
Luo, Rui (Nanjing University of Science & Technology. School of Environmental and Biological Engineering)
Du, Jia (University of Bern. Department of Chemistry, Biochemistry and Pharmaceutical Sciences)
Zhang, Damin (University of Bern. Department of Chemistry, Biochemistry and Pharmaceutical Sciences)
Pereira, Inês J. (University of Copenhagen. Department of Chemistry)
Escudero-Escribano, María (Institut Català de Nanociència i Nanotecnologia)
Arenz, Matthias (University of Bern. Department of Chemistry, Biochemistry and Pharmaceutical Sciences)
Rossmeisl, Jan (University of Copenhagen. Department of Chemistry)

Data:	2022
Resum:	Electrocatalytic conversion of formic acid oxidation to CO2 and the related CO2 reduction to formic acid represent a potential closed carbon-loop based on renewable energy. However, formic acid fuel cells are inhibited by the formation of site-blocking species during the formic acid oxidation reaction. Recent studies have elucidated how the binding of carbon and hydrogen on catalyst surfaces promote CO2 reduction towards CO and formic acid. This has also given fundamental insights into the reverse reaction, i. e. the oxidation of formic acid. In this work, simulations on multiple materials have been combined with formic acid oxidation experiments on electrocatalysts to shed light on the reaction and the accompanying catalytic limitations. We correlate data on different catalysts to show that (i) formate, which is the proposed formic acid oxidation intermediate, has similar binding energetics on Pt, Pd and Ag, while Ag does not work as a catalyst, and (ii) *H adsorbed on the surface results in *CO formation and poisoning through a chemical disproportionation step. Using these results, the fundamental limitations can be revealed and progress our understanding of the mechanism of the formic acid oxidation reaction.
Drets:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.
Llengua:	Anglès
Document:	Article ; recerca ; Versió publicada
Publicat a:	Chemical science, Vol. 13, Issue 45 (December 2022) , p. 13409-13417, ISSN 2041-6539

DOI: 10.1039/d2sc05160e
PMID: 36507186

9 p, 1.5 MB

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