In-Situ Constructuring of Copper-Doped Bismuth Catalyst for Highly Efficient CO_2 Electrolysis to Formate in Ampere-Level

摘要

CO_2 electrochemical reduction (CO2RR) can mitigate environmental issueswhile providing valuable products, yet challenging in activity, selectivity, andstability. Here, a CuS-Bi_2S_3 heterojunction precursor is reported that can insitu reconstruct to Cu-doped Bismuth (CDB) electrocatalyst during CO_2RR.The CDB exhibits an industrial-compatible current density of ~(?1).1 A cm~(?2)and a record-high formate formation rate of 21.0 mmol h~(?1) cm~(?2) at ?0.86 Vversus the reversible hydrogen electrode toward CO_2RR to formate, dramaticallyoutperforming currently reported catalysts. Importantly, the ultrawidepotential region of 1050 mV with high formate Faradaic efficiency of over 90and superior long-term stability for more than 100 h at ?400 mA cm~(?2) can alsobe realized. Experimental and theoretical studies reveal that the remarkableCO_2RR performance of CDB results from the doping effect of Cu which optimizesadsorption of the *OCHO and boosts the structural stability of metallicbismuth catalyst. This study provides valuable inspiration for the design ofelement-doping electrocatalysts to enhance catalytic activity and durability.