Copper–Indium Binary Catalyst on a Gas Diffusion Electrode for High-Performance CO₂ Electrochemical Reduction with Record CO Production Efficiency

Abstract

Cu-In metallic hybrid is a promising non-noble catalyst for selective electrochemical CO₂ reduction (eCO₂R) to CO, but the lack of direct assembly with a gas diffusion electrode (GDE) limits the further development of eCO₂R to CO with both high Faradaic efficiency (FE) and high current density. In this study, an in situ electrochemical spontaneous precipitation (ESP) method was applied for the first time to prepare GDE-combined Cu-In electrocatalysts. The optimum Cu-In catalyst consists of a nanoscale "core-shell" structure of polycrystalline Cu_<i>x</i>O covered by the amorphous In(OH)₃ interface. Higher than 90% FE of CO production has been achieved. With the synergy of a GDE flow cell and 1 M KOH catholyte, a current density of ∼200 mA cm^-2 was reached at -1.17 V (reversible hydrogen electrode), which enabled a CO yield efficiency record of 3.05 mg min^-1(CO₂/15 mL min^-1 with a 2 cm² electrode). The ratios between CO and H₂ produced can be effectively modulated via fine-tuning ESP conditions demonstrating possibility of generating CO or syngas with tuneable ratios. The present study provides a simple approach for constructing novel catalytic interfaces with dual active centers for eCO₂R and other emerging electrochemical catalysis research.