Correlations in Formic Acid Oxidation

15 September 2022, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

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 to 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 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 .

Supplementary materials

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Title
SI: Correlations in Formic Acid Oxidation
Description
SI contains: extensive literature study, formic acid oxidation reaction electrocatalytic performance scheme, Elements relevant for screening FAOR catalysts, formic acid oxidation reaction test on various catalysts
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