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Crystal Facet-Dependent Metal-Support Interaction for Stabilizing Cuδ+ Species Toward Efficient CO2 Electroreduction
Airong Xu1, Lanyue Zhang1, Yuanhua Sun1
1School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences At the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
None:
Cuδ+ species are recognized as optimal active sites for the electrocatalytic CO2 reduction reaction. While metal-support interactions (MSIs) modulate the local microenvironment of Cuδ+, the intrinsic contribution of support crystallographic facets to these interactions remains obscured by interfering oxygen vacancies. In this work, we present a definitive study decoupling the facet effect from vacancy-related variables by utilizing CeO2 supports with comparable oxygen vacancy concentrations. Our findings reveal that Cu single atoms supported on various CeO2 facets follow a pronounced facet-dependent stability order of Cu/CeO2-(110) > Cu/CeO2-(100) > Cu/CeO2-(111), yet exhibit facet-independent methane Faraday efficiency (∼80% at -200 mA/cm2). Mechanistic studies unravel this dichotomy, revealing that identical Cu coordination environments drive the uniform initial activity, whereas distinct surface electronic structures dictate long-term stability by modulating facet-dependent MSIs. Specifically, the (110) facet exhibits the strongest MSI, acting as a robust "electron buffer" that securely anchors high-valent Cuδ+ species and effectively retards their irreversible reductive agglomeration into clusters. By establishing an unambiguous structure-performance relationship under single-variable conditions, this study provides a rational geometric descriptor for designing long-lasting CO2 conversion catalysts.
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