“Two Ships in a Bottle” Design for Zn–Ag–O Catalyst Enabling Selective and Long-Lasting CO2 Electroreduction

• DOI: 10.1021/jacs.0c12418
• Publication Date: 2021-04-16T02:27:40Z
• Authors: Zhen Zhang; Guobin Wen; Dan Luo; Bohua Ren; Yanfei Zhu; Rui Gao; Haozhen Dou; Guiru Sun; Ming Feng; Zhengyu Bai; Aiping Yu; Zhongwei Chen
• Keywords: Bimetallic strip

Electrochemical CO2 reduction (CO2RR) using renewable energy sources represents a sustainable means of producing carbon-neutral fuels. Unfortunately, low efficiency, poor product selectivity, and rapid deactivation are among the most intractable challenges CO2RR electrocatalysts. Here, we strategically propose "two ships in bottle" design for ternary Zn–Ag–O catalysts, where ZnO Ag phases twinned to constitute an individual ultrafine nanoparticle impregnated inside nanopores ultrahigh-surface-area carbon matrix. Bimetallic electron configurations modulated by constructing interface, density reconfiguration arising from delocalization enhances stabilization *COOH intermediate favorable CO production, while promoting selectivity suppressing HCOOH generation altering rate-limiting step toward high thermodynamic barrier forming HCOO*. Moreover, pore-constriction mechanism restricts bimetallic particles nanosized dimensions with abundant heterointerfaces exposed active sites, meanwhile prohibiting detachment agglomeration nanoparticles during enhanced stability. The designed catalysts realize 60.9% efficiency 94.1 ± 4.0% Faradaic CO, together remarkable stability over 6 days. Beyond providing high-performance electrocatalyst, this work presents promising catalyst-design strategy efficient conversion.