Lattice Charge Tuning-Driven Multi-Carbon Products from Carbon Dioxide

Mitigating global CO2 concentrations from anthropogenic sources through electrochemical conversion to value-added chemicals is the need of the hour. In this work, the fundamental concept of "Lattice Charge" has been strategically manipulated in materials to selectively produce multi-carbon products from greenhouse CO2 gas. To achieve this, a series of catalysts within a well-known ABX2 family (A = Ag, Cu; B = In, Ga, Fe; X = S, Se) have been explored, which exhibit significant activity toward the electrochemical CO2 reduction reaction (eCO2RR) and results in the formation of higher carbon chemicals including C3 products, acetone, and energy-dense isopropanol (FE = 24.5 ± 2.5%). The Hirshfeld charge analysis technique highlighted the structure–activity correlation and the importance of the optimized lattice charge distribution as a crucial tool to manipulate the eCO2RR product in electrocatalyst designs, and the real-time in situ ATR-FTIR technique probes the crucial intermediate species adsorbed during the CO2 reduction process.