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<p>Interphases are critical in electrochemical systems, influencing performance by controlling ion transport and stability. This study explores a metal-organic interphase in the electrocatalytic reduction of CO<sub>2</sub> (CO<sub>2</sub>RR) on Cu, extending the concept of interphases to CO<sub>2</sub> conversion. Investigating organic modifications on CuO<sub>x</sub>, we discover metal-organic interphases over 10 nm thick in highly ethanol-selective systems, contrary to the expected monolayer adsorption. Using an automated platform, 1080 CO<sub>2</sub>RR experiments with 180 molecular modifiers identify functional groups affecting selectivity for ethanol and multi-carbon (C<sub>2+</sub>) products. We find that these modifiers consistently produce metal-organic interphases on the Cu or CuO<sub>x</sub> surface. These interphases modulate Cu coordination, CO<sub>2</sub>RR intermediates, and interfacial water configuration, significantly improving electrocatalytic performance. Testing across 11 CuO<sub>x</sub>-based catalysts validates this approach, culminating in the development of two electrocatalysts that achieve ~80% faradaic efficiency for C<sub>2+</sub> products with ethanol partial current densities up to 328 and 507 mA cm<sup>−2</sup>. This study highlights the pivotal role of interphases in CO<sub>2</sub>RR, advancing CO<sub>2</sub> conversion technologies.</p>

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Observation of metal-organic interphase in Cu-based electrochemical CO2-to-ethanol conversion

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年2月28日

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  • Yan Shen,
  • Nan Fang,
  • Xinru Liu,
  • Yu Ling,
  • Yuming Su,
  • Tian Tan,
  • Feng Chen,
  • He Lin,
  • Boxuan Zhao,
  • Jin Wang,
  • Duanhui Si,
  • Shunji Xie,
  • Ye Wang,
  • Da Zhou,
  • Teng Zhang,
  • Rong Cao,
  • Cheng Wang

摘要

Interphases are critical in electrochemical systems, influencing performance by controlling ion transport and stability. This study explores a metal-organic interphase in the electrocatalytic reduction of CO2 (CO2RR) on Cu, extending the concept of interphases to CO2 conversion. Investigating organic modifications on CuOx, we discover metal-organic interphases over 10 nm thick in highly ethanol-selective systems, contrary to the expected monolayer adsorption. Using an automated platform, 1080 CO2RR experiments with 180 molecular modifiers identify functional groups affecting selectivity for ethanol and multi-carbon (C2+) products. We find that these modifiers consistently produce metal-organic interphases on the Cu or CuOx surface. These interphases modulate Cu coordination, CO2RR intermediates, and interfacial water configuration, significantly improving electrocatalytic performance. Testing across 11 CuOx-based catalysts validates this approach, culminating in the development of two electrocatalysts that achieve ~80% faradaic efficiency for C2+ products with ethanol partial current densities up to 328 and 507 mA cm−2. This study highlights the pivotal role of interphases in CO2RR, advancing CO2 conversion technologies.