Altering preferential product selectivity in electrocatalytic CO2 reduction over fluorine-modified CuIn bimetallic materials

Integrating carbon dioxide (CO₂)-derived renewable technologies into the petrochemical industry presents a promising avenue for carbon neutrality. The renewable-energy-powered electrochemical CO₂ reduction (eCO₂R) process, particularly over Cu-based electrocatalysts, is a valuable asset for our decarbonization efforts to avoid climate consequences. Intending to enhance process efficiency, this work is a distinctive case study emphasizing the need to develop electrocatalysts in conjunction with adjusting operating conditions. A representative case is presented using fluorine-modified CuIn bimetallic electrocatalysts with tunable In/Cu ratios, demonstrating how to alter selectivity preferences based on reactor configuration: Our optimized catalyst system led to the highest faradaic efficiency (FE) for C₂₊ products of 68 % and the highest C₁ FE of 80 % using gas diffusion electrodes (GDE)- and H-cell-type based electrolyzer, respectively. Moreover, the controllable In/Cu ratio and the degree of fluoride doping played a pivotal role in governing the physicochemical properties of the bimetallic electrocatalysts and their eCO₂R performance. Diverse characterization tools offered systematic insights into the relationships between catalyst structure and properties, reactor configuration, electrolyte, and performance, aiming to enhance the Technology Readiness Level of the eCO₂R process.