Strain in Copper/Ceria Heterostructure Promotes Electrosynthesis of Multicarbon Products

Elastic strains in metallic catalysts induce enhanced selectivity for carbon dioxide reduction (CO₂R) toward valuable multicarbon (C₂₊) products. However, under working conditions, the structure of catalysts inevitably undergoes reconstruction, hardly retaining the initial strain. Herein, we present a metal/metal oxide synthetic strategy to introduce and maintain the tensile strain in a copper/ceria heterostructure, enabled by the presence of a thin interface layer of Cu₂O/CeO₂. The tensile strain in the copper domain and deficient electron environment around interfacial Cu sites resulted in strengthened adsorption of carbonaceous intermediates and promoted *CO dimerization. The strain effect in the copper/ceria heterostructure leads to an improved C₂₊ selectivity with a maximum Faradaic efficiency of 76.4% and a half-cell power conversion efficiency of 49.1%. The fundamental insights gained from this system can facilitate the rational design of heterostructure catalysts for CO₂R.