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Local Coordination-Dependent CO2 Reduction Activity of Bimetallic Cu─Al Catalysts for Selective Ethylene/Ethanol Electrosynthesis
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DOI：10.1002/anie.202520291.png)
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Abstract
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The formation of bimetallic catalysts has been widely adopted to improve CO2 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/CuAlO2 interfaces) and doping-CuAl (with Al doped into the Cu lattice). Both catalysts demonstrate excellent C2+ Faradaic efficiency (FE) of 65%–85%. However, interface-CuAl primarily produces ethylene with an FE of 67.6%, seven-fold higher than FEethanol. Conversely, doping-CuAl favors ethanol production, reaching a maximum FEethanol of 43.7%, four times higher than FEethylene. 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 CO2 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.
Keywords:
Bimetallic catalysts
Carbon dioxide reduction reaction
Coordination-dependent
Ethylene/Ethanol selectivity
Laser synthesis
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