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<p>To address the escalating challenge of atmospheric CO<sub>2</sub> 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 ZrO<sub>2</sub> 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 CuN<sub>4</sub> to CuN<sub>1</sub>O<sub>2</sub> under electrochemical conditions. The reconstructed CuN<sub>1</sub>O<sub>2</sub> achieve observed performance for CO<sub>2</sub>-to-CH<sub>4</sub> conversion, reaching a Faradaic efficiency of 87.06 ± 3.22% at −500 mA cm<sup>−2</sup> and 80.21 ± 1.01% at −1000 mA cm<sup>−2</sup>, which are threefold and tenfold higher than those of pristine CuN<sub>4</sub>. Furthermore, a 25-h stability test with 500 mA cm<sup>−2</sup> current density in a membrane electrode assembly (MEA) electrolyzer demonstrates minimal activity decay (&lt; 3%). Density functional theory (DFT) calculations demonstrate that self-healing mechanisms optimize intermediate adsorption and electron distribution. This strategy enables efficient muti-electron transfer processes under industrial conditions, working to improve the stability of single-atom catalysts and develop scalable catalytic systems.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月26日

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  • 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,
  • Yuen Wu

摘要

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 (< 3%). Density functional theory (DFT) calculations demonstrate that self-healing mechanisms optimize intermediate adsorption and electron distribution. This strategy enables efficient muti-electron transfer processes under industrial conditions, working to improve the stability of single-atom catalysts and develop scalable catalytic systems.