Substrate strain tunes operando geometric distortion and oxygen reduction activity of CuN2C2 single-atom sites

Guokang Han, Xue Zhang, Wei Liu, Qinghua Zhang, Zhiqiang Wang, Jun Cheng, Tao Yao, Lin Gu, Chunyu Du (), Yunzhi Gao and Geping Yin
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Guokang Han: Harbin Institute of Technology
Xue Zhang: Xiamen University
Wei Liu: University of Science and Technology of China
Qinghua Zhang: Chinese Academy of Sciences
Zhiqiang Wang: University of Western Ontario
Jun Cheng: Xiamen University
Tao Yao: University of Science and Technology of China
Lin Gu: Chinese Academy of Sciences
Chunyu Du: Harbin Institute of Technology
Yunzhi Gao: Harbin Institute of Technology
Geping Yin: Harbin Institute of Technology

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Single-atom catalysts are becoming increasingly significant to numerous energy conversion reactions. However, their rational design and construction remain quite challenging due to the poorly understood structure–function relationship. Here we demonstrate the dynamic behavior of CuN2C2 site during operando oxygen reduction reaction, revealing a substrate-strain tuned geometry distortion of active sites and its correlation with the activity. Our best CuN2C2 site, on carbon nanotube with 8 nm diameter, delivers a sixfold activity promotion relative to graphene. Density functional theory and X-ray absorption spectroscopy reveal that reasonable substrate strain allows the optimized distortion, where Cu bonds strongly with the oxygen species while maintaining intimate coordination with C/N atoms. The optimized distortion facilitates the electron transfer from Cu to the adsorbed O, greatly boosting the oxygen reduction activity. This work uncovers the structure–function relationship of single-atom catalysts in terms of carbon substrate, and provides guidance to their future design and activity promotion.

Date: 2021
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DOI: 10.1038/s41467-021-26747-1

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