Operando formation of highly efficient electrocatalysts induced by heteroatom leaching

Cong Liu, Bingbao Mei, Zhaoping Shi, Zheng Jiang, Junjie Ge, Wei Xing, Ping Song () and Weilin Xu ()
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Cong Liu: Chinese Academy of Sciences
Bingbao Mei: Chinese Academy of Sciences
Zhaoping Shi: Chinese Academy of Sciences
Zheng Jiang: University of Science and Technology of China
Junjie Ge: Chinese Academy of Sciences
Wei Xing: Chinese Academy of Sciences
Ping Song: Chinese Academy of Sciences
Weilin Xu: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Heterogeneous nano-electrocatalysts doped with nonmetal atoms have been studied extensively based on the so-called dopant-based active sites, while little attention has been paid to the stability of these dopants under working conditions. In this work, we reveal significantly, when the redox working potential is too low negatively or too high positively, the active sites based on these dopants actually tend to collapse. It means that some previously observed “remarkable catalytic performance” actually originated from some unknown active sites formed in situ. Take the Bi-F for the CO2RR as an example, results show that the observed remarkable activity and stability were not directly from F-based active sites, but the defective Bi sites formed in situ after the dopant leaching. Such a fact is unveiled from several heteroatom-doped nanocatalysts for four typical reactions (CO2RR, HER, ORR, and OER). This work provides insight into the role of dopants in electrocatalysis.

Date: 2024
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DOI: 10.1038/s41467-023-44480-9

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