Correlations between experiments and simulations for formic acid oxidation

Alexander Bagger*, Kim D. Jensen, Maryam Rashedi, Jia Du, Rui Luo, Damin Zhang, Ines J. Pereira, Maria Escudero-Escribano, Matthias Arenz, Jan Rossmeisl

*Corresponding author af dette arbejde

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

2 Citationer (Scopus)
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Abstract

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.

OriginalsprogEngelsk
TidsskriftChemical Science
Vol/bind13
Udgave nummer45
Sider (fra-til)13409-13417
Antal sider9
ISSN2041-6520
DOI
StatusUdgivet - 2022

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