title: Modeling the HCOOH/CO2 Electrocatalytic Reaction: When Details Are Key.
abstract: Our first principles simulations of the electrooxidation of formic acid over nickel identify the reorientation of the formate intermediate and the desorption of CO2 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.
authors.affiliation: Université de Lyon, Ecole Normale Supérieure de Lyon, Laboratoire de Chimie, 46 allee d'Italie, Lyon (France).
authors.forename: Stephan N
authors.initials: SN
authors.lastname: Steinmann
authors.affiliation: Université de Lyon, Ecole Normale Supérieure de Lyon, Laboratoire de Chimie, 46 allee d'Italie, Lyon (France).|CNRS, Laboratoire de Chimie, UMR 5182, 46 allee d'Italie, Lyon (France).
authors.forename: Carine
authors.initials: C
authors.lastname: Michel
authors.affiliation: Eco-Efficient Products and Processes Laboratory (E2P2 L), UMI 3464 Solvay/CNRS, Shanghai (PR China).
authors.forename: Renate
authors.initials: R
authors.lastname: Schwiedernoch
authors.affiliation: CTMM, Institut Charles Gerhardt Montpellier UMR 5253, Universite Montpellier 2, Place E Bataillon, Montpellier (France).
authors.forename: Jean-Sebastien
authors.initials: JS
authors.lastname: Filhol
authors.affiliation: Université de Lyon, Ecole Normale Supérieure de Lyon, Laboratoire de Chimie, 46 allee d'Italie, Lyon (France). philippe.sautet@ens-lyon.fr.|CNRS, Laboratoire de Chimie, UMR 5182, 46 allee d'Italie, Lyon (France). philippe.sautet@ens-lyon.fr.
authors.forename: Philippe
authors.initials: P
authors.lastname: Sautet
keywords: density functional calculations; electrocatalysis; electrochemistry; formic acid; heterogeneous catalysis