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Modeling the HCOOH/CO 2 Electrocatalytic Reaction: When Details Are Key
Author(s) -
Steinmann Stephan N.,
Michel Carine,
Schwiedernoch Renate,
Filhol JeanSebastien,
Sautet Philippe
Publication year - 2015
Publication title -
chemphyschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.016
H-Index - 140
eISSN - 1439-7641
pISSN - 1439-4235
DOI - 10.1002/cphc.201500187
Subject(s) - formic acid , formate , electron transfer , electrochemistry , chemistry , desorption , limiting , nickel , electrocatalyst , kinetic energy , inorganic chemistry , catalysis , photochemistry , electrode , organic chemistry , adsorption , physics , mechanical engineering , engineering , quantum mechanics
Our first principles simulations of the electrooxidation of formic acid over nickel identify the reorientation of the formate intermediate and the desorption of CO 2 as the rate‐limiting steps. Although they are not associated with an electron transfer, these barriers are strongly modified when the electrochemical potential is explicitly accounted for and when modeling the influence of the solvent. Hence, such a level of modeling is key to understand the kinetic limitations that penalize the reaction.