期刊
ACS CATALYSIS
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02411
关键词
electrocatalyst; water splitting; perovskite oxide; oxygen vacancies; ordering
资金
- National Science Foundation (NSF) [DMR-1943085]
The translated article discusses the enhanced electrocatalytic performance for water electrolysis, achieved through increased ordering of oxygen vacancies in the structural network of oxides. The change in the average ionic radius of the A-site metals leads to an increase in the concentration and ordering of oxygen vacancies, resulting in improved electrocatalytic activity for hydrogen-evolution and oxygen-evolution reactions. The proposed method has significant importance in the field.
Electrocatalytic splitting of water is a promising method of hydrogen generation. Here, we report an enhanced electrocatalytic performance for water electrolysis, achieved through a progressive increase in the ordering of oxygen vacancies in the structural network of oxides. In transition from Sr2FeCoO(6-delta) (disordered) to CaSrFeCoO6-delta (ordered) and Ca2FeCoO(6-delta) (highly ordered), the change in the average ionic radius of the A-site metals leads to an increase in the concentration and ordering of oxygen vacancies, resulting in a progressive enhancement of the electrocatalytic activity for both cathodic and anodic half-reactions of water splitting, i.e., hydrogen-evolution (HER) and oxygen-evolution (OER) reactions. The OER electrocatalysis is particularly important, as it is considered the bottleneck for water electrolysis. These electrocatalysts show better activity than the precious metal catalyst RuO2. In contrast to most bifunctional catalysts reported to date, these catalysts can be used in bulk form, without the need for nanofabrication, composite formation, or any additional processing. Density functional theory calculations indicate that the vacancy order leads to a shift of the electronic bands toward the Fermi level. We propose that the ordering of oxygen vacancies can be used as a handle for the design of highly active electrocatalysts.
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