Boron‐Doping Engineering in AgCd Bimetallic Catalyst Enabling Efficient CO2 Electroreduction to CO and Aqueous Zn‐CO2 Batteries

Abstract The limited adsorption and activation of CO 2 on catalyst and the high energy barrier for intermediate formation hinder the development of electrochemical CO 2 reduction reactions (CO 2 RR). Herein, this work reports a boron (B) doping engineering in AgCd bimetals to alleviate the above limitations for efficient CO 2 electroreduction to CO and aqueous Zn‐CO 2 batteries. Specifically, the B‐doped AgCd bimetallic catalyst (AgCd‐B) is prepared via a simple reduction reaction at room temperature. A combination of in situ experiments and density functional theory (DFT) calculations demonstrates that B‐doping simultaneously enhances the adsorption and activation of CO 2 and reduces the binding energy of the intermediates by moderating the electronic structure of bimetals. As a result, the AgCd‐B catalyst exhibits a high CO Faraday efficiency (FE CO ) of 99% at −0.8 V versus reversible hydrogen electrode (RHE). Additionally, it maintains a FE CO over 92% at a wide potential window of 600 mV (−0.6 to −1.1 V versus RHE). Furthermore, the AgCd‐B catalyst coupled with the Zn anode to assemble aqueous Zn‐CO 2 batteries shows a power density of 20.18 mW cm −2 and a recharge time of 33 h.