期刊
ACS CATALYSIS
卷 8, 期 3, 页码 1864-1879出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b03142
关键词
Tafel slope; electrocatalysis; free energy diagram; ab initio thermodynamics; generalized Butler-Volmer equation; chlorine evolution reaction (CER); oxygen evolution reaction (OER); hydrogen evolution reaction (HER)
资金
- BMBF [05K2016-HEXCHEM]
- Alexander von Humboldt Foundation
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.
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