Enhanced kinetics of CO2 electro-reduction on a hollow gas bubbling electrode in molten ternary carbonates

Abstract

Electrochemical reduction of CO2 to value-added carbon and oxygen in lithium-containing molten carbonates at 723 K is a promising approach to the efficient utilization of CO2. It was recently reported that the cathodic process in this transformation is controlled by the sluggish diffusion of the generated O2− ions. The formation of Li2O on the cathode results in partial cathodic passivation of the cathode. To accelerate the reaction kinetics and also eliminate the concentration polarization of the resulting Li2O, the effect of bubbling CO2 through a hollow electrode was examined in this work using a home-made hollow gas bubbling (HGB) electrode. The localised CO2 bubbling not only accelerates the transport of O2− ions by agitating the electrolyte nearby, but the CO2 also reacts with Li2O to form the more soluble Li2CO3. Cyclic voltammetry (CV), linear sweep voltammetry (LSV) and constant current electrolysis were conducted in the melt at 723 K to study the depolarization mechanisms involved in the CO2 bubbling reaction. Using the HGB electrode, the steady-state current density increased from 15.3 mA/cm2 to ~200 mA/cm2 at a potential of −2.4 V (vs. Ag/Ag2SO4). The HGB electrode effectively improved the cathodic kinetics, which is beneficial for CO2 capture and electrochemical conversion. Keywords: CO2 conversion, Molten carbonates, Passivation, Electrode kinetics