期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202218738
关键词
Fe-VI Intermediate; NiFe Catalyst; Oxygen Evolution Reaction; Spectroelectrochemistry; Water Oxidation
In this study, the active center of NiFe-based catalysts for oxygen evolution reaction (OER) was identified as Fe through the detection of highly-oxidized Fe-VI intermediates leached into the electrolyte. Furthermore, the incorporation of Co into NiFe-based catalyst was found to enhance the formation of Fe-VI active species and improve the OER activity of the catalyst. These findings provide insights into the mechanisms for sustainable generation of Fe-VI active species in NiFe-based catalysts and lay the foundation for the design of more efficient and stable OER catalysts.
In situ detection of highly-oxidized metal intermediates is the key to identifying the active center of an oxygen evolution reaction (OER) catalyst, but it remains challenging for NiFe-based catalysts in an aqueous solution under working conditions. Here, by utilizing the dynamic stability of the (FeO42-)-O-VI intermediates in a self-healing water oxidation cycle of NiFe-based catalyst, the highly-oxidized Fe-VI intermediates leached into the electrolyte are directly detected by simple spectroelectrochemistry. Our results provide direct evidence that Fe is the active center in NiFe-based OER catalysts. Furthermore, it is revealed that the incorporation of Co into NiFe-based catalyst facilitates the formation of Fe-VI active species, thus enhancing the OER activity of NiCoFe-based catalyst. The insights into the mechanisms for the sustainable generation of Fe-VI active species in these NiFe-based catalysts lay the foundation for the design of more efficient and stable OER catalysts.
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