3 years ago

Full Free Energy Diagram of an Electrocatalytic Reaction over a Single-Crystalline Model Electrode

Full Free Energy Diagram of an Electrocatalytic Reaction over a Single-Crystalline Model Electrode
Josef Anton, Iman Sohrabnejad-Eskan, Herbert Over, Timo Jacob, Kai S. Exner
A long-term aim of chemical kinetics is to gain detailed information on the full free energy diagram along the reaction coordinate of electrocatalytic processes such as those encountered in fuel cells, batteries, and industrial electrolysis. We present here a universal approach to construct the free energy landscape of an electrocatalyzed reaction over a single-crystalline model electrode without relying on full kinetics from first principles, a highly computer-resource-demanding approach. The free energies of the transition states are determined by a dedicated evaluation scheme of experimental Tafel plots, whereas ab initio thermodynamics calculations provide the free energies of the reaction intermediates. We exemplified this approach with the chlorine and oxygen evolution reactions over a well-defined RuO2(110) model electrode, both reactions constitute large-scale industrial processes. Seeing is believing: An intimate interplay between ab initio thermodynamics DFT calculations in the form of surface Pourbaix diagrams and experimentally measured Tafel plots over single-crystalline model electrodes allows the construction of the free energy landscape along the reaction coordinate, which enables in-depth insight into the performance of an electrocatalyst.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/celc.201700687

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