Correlations between experiments and simulations for formic acid oxidation
Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
Standard
Correlations between experiments and simulations for formic acid oxidation. / Bagger, Alexander; Jensen, Kim D.; Rashedi, Maryam; Du, Jia; Luo, Rui; Zhang, Damin; Pereira, Ines J.; Escudero-Escribano, Maria; Arenz, Matthias; Rossmeisl, Jan.
I: Chemical Science, Bind 13, Nr. 45, 2022, s. 13409-13417.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
Harvard
APA
Vancouver
Author
Bibtex
}
RIS
TY - JOUR
T1 - Correlations between experiments and simulations for formic acid oxidation
AU - Bagger, Alexander
AU - Jensen, Kim D.
AU - Rashedi, Maryam
AU - Du, Jia
AU - Luo, Rui
AU - Zhang, Damin
AU - Pereira, Ines J.
AU - Escudero-Escribano, Maria
AU - Arenz, Matthias
AU - Rossmeisl, Jan
PY - 2022
Y1 - 2022
N2 - 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.
AB - 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.
KW - NOBLE-METAL ELECTRODES
KW - ELECTROCATALYTIC OXIDATION
KW - ELECTROCHEMICAL REDUCTION
KW - PLATINUM-ELECTRODES
KW - CARBON-MONOXIDE
KW - MECHANISM
KW - ELECTROOXIDATION
KW - CO2
KW - METHANOL
KW - PD
U2 - 10.1039/d2sc05160e
DO - 10.1039/d2sc05160e
M3 - Journal article
C2 - 36507186
VL - 13
SP - 13409
EP - 13417
JO - Chemical Science
JF - Chemical Science
SN - 2041-6520
IS - 45
ER -
ID: 327055903