Hydroxyl-rich Zn/Co-based bimetallic layered catalyst for enhanced CO2 electrolysis to CO

Local CO2 concentration and efficient electron transfer are critical for facilitating CO2 activation. Herein, we developed a hydroxyl-rich Zn/Co layered double hydroxide (Zn2Co3(OH)10∙2 H2O) via a facile solvothermal method. The electronic interaction between Zn and Co not only induces the formation of abundant oxygen vacancies but also creates electron-enriched Co sites, collectively establishing a highly synergistic catalytic center. Simultaneously, the rich hydroxyl groups on the catalyst surface enhance the local CO2 concentration and serve as a proton reservoir. Owing to this unique configuration, the catalyst achieves a high Faradaic efficiency for CO (exceeding 88%) over a wide potential window (-1.13 V to −0.73 V vs. RHE) and a current density of 50 mA cm−2. Mechanistic studies reveal that the synergistic center promotes the formation and stabilization of the key *COOH intermediate, enabling efficient CO2-to-CO conversion at a reduced overpotential. This work highlights the importance of engineering bimetallic electronic synergy in designing high-performance CO2 reduction electrocatalysts.