CO2 electrolysis to multicarbon products in strong acid

Abstract

Carbon dioxide electroreduction (CO₂R) is being actively studied as a promising route to convert carbon emissions to valuable chemicals and fuels. However, the fraction of input CO₂ that is productively reduced has typically been very low, <2% for multicarbon products; the balance reacts with hydroxide to form carbonate in both alkaline and neutral reactors. Acidic electrolytes would overcome this limitation, but hydrogen evolution has hitherto dominated under those conditions. We report that concentrating potassium cations in the vicinity of electrochemically active sites accelerates CO₂ activation to enable efficient CO₂R in acid. We achieve CO₂R on copper at pH <1 with a single-pass CO₂ utilization of 77%, including a conversion efficiency of 50% toward multicarbon products (ethylene, ethanol, and 1-propanol) at a current density of 1.2 amperes per square centimeter and a full-cell voltage of 4.2 volts.