Synergistic interface engineering of Cu-O-Zr with dispersed Ag sites for selective CO2 electroreduction into C2 products

A heterostructured Ag/Cu 2 O-ZrO₂ catalyst was synthesized via an interface engineering strategy. • The Ag/Cu 2 O-ZrO₂ possesses a substantial number of Cu-O-Zr heterointerfaces with dispersed Ag sites • The optimized Ag/Cu 2 O-ZrO₂ catalyst demonstrates exceptional CO₂-to-C 2 fuels conversion performance. • Possible mechanism for boosting electroreduction of CO 2 reduction was proposed. • The present work sheds light on the customization of interfacial engineering with dispersed active sites. The efficient electrocatalytic reduction of carbon dioxide (CO 2 ) into multi‑carbon (C 2+ ) products is critical for sustainable carbon management, yet remains limited by poor selectivity and sluggish C C coupling kinetics. Herein, a heterostructured Ag/Cu 2 O-ZrO 2 catalyst was synthesized via an interface engineering strategy to promote C 2 production during CO 2 electroreduction. The incorporation of highly dispersed Ag nanoparticles and ZrO 2 domains onto Cu 2 O nanocrystals generates abundant Cu-O-Zr heterointerfaces, which synergistically regulate the local electronic environment and intermediate conversion behavior. In this catalytic system, the dispersed Ag sites act as efficient *CO-generating centers to enrich local CO coverage, while the Cu-O-Zr interfacial domains stabilize oxygen-containing C C coupling intermediates and facilitate their subsequent hydrogenation toward C 2 products. Benefiting from the tandem synergy between CO enrichment and interfacial intermediate stabilization, Ag/Cu 2 O-ZrO 2 catalyst achieves a high C 2 Faradaic efficiency of 78.2% and a C 2 partial current density of 17.1 mA·cm −2 at −1.3 V vs. RHE, outperforming Cu 2 O and Cu 2 O-ZrO 2 counterparts. In situ infrared spectroscopy reveals the efficient evolution of key intermediates from *COOH to *CO and subsequently to *OCCO during electrocatalysis. Meanwhile, DFT calculations demonstrate that Ag promotes *CO accumulation and suppresses its premature desorption, whereas the Cu-O-Zr interface stabilizes *OCCO and *CHCHO intermediates and lowers the corresponding energy barriers for C 2 formation. This work provides mechanistic insights into tandem interface engineering for selective CO 2 electroreduction toward multi‑carbon fuels through the spatially cooperative regulation of CO generation and C C coupling pathways. Download: Download high-res image (321KB) Download: Download full-size image