Journal article

Publication year: 2015

Pages: 707-713

Journal: ChemElectroChem

Volume number: 2

Issue number: 5

DOI Link: https://doi.org/10.1002/celc.201402430

Publisher: Wiley

Abstract: 

By using the ab initio atomistic thermodynamics approach guided by a DFT‐derived volcano curve, we demonstrate that the thermodynamic part of the reaction barrier to the oxygen evolution reaction (OER) over RuO2(110) can be significantly reduced when moderately lowering the free adsorption energy of oxygen to the catalytically active Ru center (Rucus). With the selective replacement of metal sites in the second coordination shell of Rucus, the free oxygen adsorption energy is reduced by about 0.8 and 1.0 eV for Cr and Ir, respectively. The weakening of Rucus and oxygen‐on‐top (RucusOot) bonding results in a substantial decrease in the thermodynamic part of the reaction barrier (Gibbs free‐energy loss) by 180 meV for Cr and 150 meV for Ir. The presented strategy is motivated by homogeneous metal catalysis where dedicated modifications of the ligands are able to tune the catalytic performance of the active metal center.

Harvard Citation style: Exner, K., Anton, J., Jacob, T. and Over, H. (2015) Ligand Effects and Their Impact on Electrocatalytic Processes Exemplified with the Oxygen Evolution Reaction (OER) on RuO2(110), ChemElectroChem, 2(5), pp. 707-713. https://doi.org/10.1002/celc.201402430

APA Citation style: Exner, K., Anton, J., Jacob, T., & Over, H. (2015). Ligand Effects and Their Impact on Electrocatalytic Processes Exemplified with the Oxygen Evolution Reaction (OER) on RuO2(110). ChemElectroChem. 2(5), 707-713. https://doi.org/10.1002/celc.201402430