期刊
ADVANCED ENERGY MATERIALS
卷 11, 期 36, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202101737
关键词
catalyst activation; Co-based electrocatalysts; electrochemical reconstruction; electrolyte; oxygen evolution reaction
类别
资金
- Bundesministerium fur Bildung und Forschung (BMBF) [05K19KE1]
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [EXC 2008-390540038-UniSysCat]
- Posgrado en Quimica and Vicerrectoria de Investigacion (UCR)
- CONICIT-MICIT (Costa Rica)
- European Research Council (ERC) under the European Union [804092]
- Projekt DEAL
- European Research Council (ERC) [804092] Funding Source: European Research Council (ERC)
The study used erythrite as a Co-based OER electrocatalyst to evaluate its catalytic properties during in situ restructuring into an amorphous Co-based catalyst in four different electrolytes, noting that only the carbonate electrolyte can activate the catalyst material. Despite a decrease in TOF by a factor of 28, the number of redox active sites increased by a factor of 56, resulting in a twofold increase in current of the restructured catalyst.
The requirements for beneficial materials restructuring into a higher performance oxygen evolution reaction (OER) electrocatalyst are still a largely open question. Here erythrite (Co-3(AsO4)(2)center dot 8H(2)O) is used as a Co-based OER electrocatalyst to evaluate its catalytic properties during in situ restructuring into an amorphous Co-based catalyst in four different electrolytes at pH 7. Using diffraction, microscopy, and spectroscopy, a strong effect in the restructuring behavior is observed depending of the anions in the electrolyte. Only carbonate electrolyte can activate the catalyst material, which is related to its slow restructuring process. While the catalyst turnover frequency (TOF) undesirably reduces by a factor of 28, the number of redox active sites continuously increases to a factor of 56, which results in an overall twofold increase in current of the restructured catalyst after 800 cycles. The activation is attributed to an adequate local order, a high Co oxidation state close to 3+, and a high number of redox-active Co ions. These three requirements for beneficial restructuring provide new insights into the rational design of high-performance OER catalysts by electrochemical restructuring.
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