Surface Facets Reconstruction in Copper‐Based Materials for Enhanced Electrochemical CO2 Reduction

The unavoidable and unpredictable surface reconstruction of metallic copper (Cu) during the electrocatalytic carbon dioxide (CO₂) reduction process is a double-edged sword affecting the production of high-value-added hydrocarbon products. It is crucial to control the surface facet reconstruction and regulate the targeted facets/facet interfaces, and further understand the mechanism between activity/selectivity and the reconstructed structure of Cu for CO₂ reduction. Based on the current catalyst design methods, a facile strategy combining chemical reduction and electro-reduction is proposed to achieve specified Cu(111) facets and the Cu(110)/(111) interfaces in reconstructed Cu derived from cuprous oxide (Cu₂O). The surface facet reconstruction significantly boosted the electrocatalytic conversion of CO₂ into multi-carbon (C₂₊) products comparing to the unmodified catalyst. Theoretical and experimental analyses show that the Cu(110)/(111)s interface between Cu(110) and a small amount of Cu(111) can tailor the reaction routes and lower the reaction energy barrier of C-C coupling to ethylene (C₂H₄). The work will guide the surface facets reconstruction strategy for Cu-based CO₂ electrocatalysts, providing a promising paradigm to understand the structural variation in catalysts.