Local Coordination‐Dependent CO <sub>2</sub> Reduction Activity of Bimetallic Cu─Al Catalysts for Selective Ethylene/Ethanol Electrosynthesis

The formation of bimetallic catalysts has been widely adopted to improve CO<sub>2</sub> reduction selectivity. However, discrepancies in product distribution in the literature, even among catalysts with identical bimetal compositions, suggest the involvement of distinct reaction pathways. Here, we report that ethylene and ethanol selectivity are strongly influenced by the atomic coordination of metals. We prepared two model catalysts, namely interface-CuAl (dominated by Cu/CuAlO<sub>2</sub> interfaces) and doping-CuAl (with Al doped into the Cu lattice). Both catalysts demonstrate excellent C<sub>2+</sub> Faradaic efficiency (FE) of 65%-85%. However, interface-CuAl primarily produces ethylene with an FE of 67.6%, seven-fold higher than FE<sub>ethanol</sub>. Conversely, doping-CuAl favors ethanol production, reaching a maximum FE<sub>ethanol</sub> of 43.7%, four times higher than FE<sub>ethylene</sub>. Extended X-ray absorption fine structure and in situ Fourier transform infrared spectrometry reveal distinct adsorption abilities of Cu and different intermediate coverages. Complementary theoretical calculation further elucidates the critical role of *CHCOH bifurcation. Specifically, favorable C-O cleavage at interface-CuAl promotes ethylene production, whereas Cu-C scission at doping-CuAl favors ethanol production. Beyond CO<sub>2</sub> electroreduction, CuAl catalysts also demonstrate phase-dependent nitrate reduction activity, underscoring the importance of atomic coordination in catalysis. This study provides fundamental insights into the structure-selectivity relationship of bimetallic catalysts for selective chemical production.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-11-10
DOI
https://doi.org/10.1002/anie.202520291
Citations
2
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
Field-Weighted Citation Impact
0.78
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article

Local Coordination‐Dependent CO 2 Reduction Activity of Bimetallic Cu─Al Catalysts for Selective Ethylene/Ethanol Electrosynthesis

Ruquan Ye, Chenyang Xia, Yinger Xin, Hanchen Shen et al.
2 citations
Angewandte Chemie International Edition
Ammonia Synthesis and Nitrogen Reduction
0.78
article

Local Coordination‐Dependent CO 2 Reduction Activity of Bimetallic Cu─Al Catalysts for Selective Ethylene/Ethanol Electrosynthesis

Ruquan Ye, Chenyang Xia, Yinger Xin, Hanchen Shen, Shibo Xi, Zhihao Li, Liang Chang, Yun Mi Song, Lin Gan, Minghui Zhu, Jixun Zhang, Tao Yang, Qiu Jiang, Zhengxiao Guo, Shenlong Zhao, Yangbo Ma, Ben Zhong Tang, Xue Wang, Ziyun Wang, Haoran Wu, Mingming He, Weihua Guo, Xingyu Wang, Geng Li
article en
2 citations

Abstract

The formation of bimetallic catalysts has been widely adopted to improve CO<sub>2</sub> reduction selectivity. However, discrepancies in product distribution in the literature, even among catalysts with identical bimetal compositions, suggest the involvement of distinct reaction pathways. Here, we report that ethylene and ethanol selectivity are strongly influenced by the atomic coordination of metals. We prepared two model catalysts, namely interface-CuAl (dominated by Cu/CuAlO<sub>2</sub> interfaces) and doping-CuAl (with Al doped into the Cu lattice). Both catalysts demonstrate excellent C<sub>2+</sub> Faradaic efficiency (FE) of 65%-85%. However, interface-CuAl primarily produces ethylene with an FE of 67.6%, seven-fold higher than FE<sub>ethanol</sub>. Conversely, doping-CuAl favors ethanol production, reaching a maximum FE<sub>ethanol</sub> of 43.7%, four times higher than FE<sub>ethylene</sub>. Extended X-ray absorption fine structure and in situ Fourier transform infrared spectrometry reveal distinct adsorption abilities of Cu and different intermediate coverages. Complementary theoretical calculation further elucidates the critical role of *CHCOH bifurcation. Specifically, favorable C-O cleavage at interface-CuAl promotes ethylene production, whereas Cu-C scission at doping-CuAl favors ethanol production. Beyond CO<sub>2</sub> electroreduction, CuAl catalysts also demonstrate phase-dependent nitrate reduction activity, underscoring the importance of atomic coordination in catalysis. This study provides fundamental insights into the structure-selectivity relationship of bimetallic catalysts for selective chemical production.

Angewandte Chemie International EditionVol. 65(2)
Agency for Science, Technology and Research (SG), East China University of Science and Technology (CN), University of Electronic Science and Technology of China (CN), University of Auckland (NZ), City University of Hong Kong (HK), Chengdu University of Technology (CN), City University of Hong Kong, Shenzhen Research Institute (CN), Institute of Chemical and Engineering Sciences (SG), Tsinghua–Berkeley Shenzhen Institute (CN), Chinese University of Hong Kong, Shenzhen (CN), National Center for Nanoscience and Technology (CN), State Key Laboratory of Chemical Engineering (CN), University of Hong Kong (HK)
Openalex Percentile: Top 27%
Ammonia Synthesis and Nitrogen Reduction
0.78
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