Journal article

Publication year: 2018

Pages: 1864-1879

Journal: ACS Catalysis

Volume number: 8

Issue number: 3

DOI Link: https://doi.org/10.1021/acscatal.7b03142

Publisher: American Chemical Society

Abstract: 

Extended Tafel plots at various temperatures for an electrocatalyzed reaction and (possibly) its reversed reaction on single-crystalline model electrodes allow for constructing the (essential part of the) free energy surface, in particular the free energies of the transition states (TS). Free energies of the reaction intermediates (RIs) including the chemical nature of active surface sites (S) are hardly accessible to experiment and need therefore to be taken from constrained ab initio thermodynamics calculations. The compact compilation of experimental kinetic data in the form of a free energy diagram enables a critical assessment and validation of theoretical free energy landscapes based on first-principles kinetics. For three prototypical electrocatalyzed reactions, namely the chlorine evolution reaction (CER) and oxygen evolution reaction (OER) over RuO2(110) as well as hydrogen evolution reaction (HER) on Pt(111), we exemplify this universal approach and discuss potential benefits for theoretical modeling of electrocatalyzed reaction.

Harvard Citation style: Exner, K., Sohrabnejad-Eskan, I. and Over, H. (2018) A Universal Approach To Determine the Free Energy Diagram of an Electrocatalytic Reaction, ACS Catalysis, 8(3), pp. 1864-1879. https://doi.org/10.1021/acscatal.7b03142

APA Citation style: Exner, K., Sohrabnejad-Eskan, I., & Over, H. (2018). A Universal Approach To Determine the Free Energy Diagram of an Electrocatalytic Reaction. ACS Catalysis. 8(3), 1864-1879. https://doi.org/10.1021/acscatal.7b03142