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

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 () and Cheng Wang ()
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Yan Shen: Xiamen University
Nan Fang: Xiamen University
Xinru Liu: Xiamen University
Yu Ling: Xiamen University
Yuming Su: Xiamen University
Tian Tan: Xiamen University
Feng Chen: Chinese Academy of Sciences
He Lin: Xiamen University
Boxuan Zhao: Xiamen University
Jin Wang: Chinese Academy of Sciences
Duanhui Si: Chinese Academy of Sciences
Shunji Xie: Xiamen University
Ye Wang: Xiamen University
Da Zhou: Xiamen University
Teng Zhang: Chinese Academy of Sciences
Rong Cao: Chinese Academy of Sciences
Cheng Wang: Xiamen University

Nature Communications, 2025, vol. 16, issue 1, 1-18

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-57221-x

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