Self-healing Cu single-atom catalyst for high-performance electrocatalytic CO2 methanation

Wanyu Shen, Xiaoping Gao, Qichen Liu, Peng Li, Rui Huang, Yi Tan, Zihan Wang, Yilin Zhang, Fan Zhao, Xin Wang, Shiyu Ji (), Xusheng Zheng (), Yu Zhang () and Yuen Wu ()
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Wanyu Shen: University of Science and Technology of China
Xiaoping Gao: Ningbo University of Technology
Qichen Liu: University of Science and Technology of China
Peng Li: University of Science and Technology of China
Rui Huang: University of Science and Technology of China
Yi Tan: University of Science and Technology of China
Zihan Wang: University of Science and Technology of China
Yilin Zhang: University of Science and Technology of China
Fan Zhao: University of Science and Technology of China
Xin Wang: University of Science and Technology of China
Shiyu Ji: University of Science and Technology of China
Xusheng Zheng: University of Science and Technology of China
Yu Zhang: University of Science and Technology of China
Yuen Wu: University of Science and Technology of China

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract To address the escalating challenge of atmospheric CO2 emissions, this study proposes a self-healing Cu single atom (SA) catalyst design. By partially cleaving Cu-N bonds via hydrogen evolution reaction (HER), coordinatively unsaturated Cu sites form and spontaneously bond with adjacent ZrO2 clusters which are strategically positioned near the Cu SA, creating a hybrid Cu-N/O structure with enhanced performance. In situ Raman and X-ray absorption fine structure (XAFS) measurements confirm the dynamic reconstruction of coordination environment from CuN4 to CuN1O2 under electrochemical conditions. The reconstructed CuN1O2 achieve observed performance for CO2-to-CH4 conversion, reaching a Faradaic efficiency of 87.06 ± 3.22% at −500 mA cm−2 and 80.21 ± 1.01% at −1000 mA cm−2, which are threefold and tenfold higher than those of pristine CuN4. Furthermore, a 25-h stability test with 500 mA cm−2 current density in a membrane electrode assembly (MEA) electrolyzer demonstrates minimal activity decay (

Date: 2025
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DOI: 10.1038/s41467-025-63274-9

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