Structural transformation of highly active metal–organic framework electrocatalysts during the oxygen evolution reaction

Shenlong Zhao, Chunhui Tan, Chun-Ting He, Pengfei An, Feng Xie, Shuai Jiang, Yanfei Zhu, Kuang-Hsu Wu, Binwei Zhang, Haijing Li, Jing Zhang, Yuan Chen, Shaoqin Liu (), Juncai Dong () and Zhiyong Tang ()
Additional contact information
Shenlong Zhao: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology
Chunhui Tan: Institute of High Energy Physics, Chinese Academy of Sciences
Chun-Ting He: Jiangxi Normal University
Pengfei An: Institute of High Energy Physics, Chinese Academy of Sciences
Feng Xie: King Abdullah University of Science and Technology
Shuai Jiang: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology
Yanfei Zhu: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology
Kuang-Hsu Wu: The University of Sydney
Binwei Zhang: The University of Sydney
Haijing Li: Institute of High Energy Physics, Chinese Academy of Sciences
Jing Zhang: Institute of High Energy Physics, Chinese Academy of Sciences
Yuan Chen: The University of Sydney
Shaoqin Liu: Harbin Institute of Technology
Juncai Dong: Institute of High Energy Physics, Chinese Academy of Sciences
Zhiyong Tang: CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology

Nature Energy, 2020, vol. 5, issue 11, 881-890

Abstract: Abstract Metal–organic frameworks (MOFs) are increasingly being investigated as electrocatalysts for the oxygen evolution reaction (OER). Despite their promising catalytic activity, many fundamental questions concerning their structure−performance relationships—especially those regarding the roles of active species—remain to be answered. Here we show the structural transformation of a Ni0.5Co0.5-MOF-74 during the OER by operando X-ray absorption spectroscopy analysis and high-resolution transmission electron microscopy imaging. We suggest that Ni0.5Co0.5OOH0.75, with abundant oxygen vacancies and high oxidation states, forms in situ and is responsible for the high OER activity observed. The ratio of Ni to Co in the bimetallic centres alters the geometric and electronic structure of as-formed active species and in turn the catalytic activity. Based on our understanding of this system, we fabricate a Ni0.9Fe0.1-MOF that delivers low overpotentials of 198 mV and 231 mV at 10 mA cm−2 and 20 mA cm−2, respectively.

Date: 2020
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DOI: 10.1038/s41560-020-00709-1

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