MECHANISTIC INSIGHTS INTO THE ELECTROCHEMICAL REDUCTION OF CARBON DIOXIDE ON COPPER ELECTRODES

Abstract

The electrochemical reduction of carbon dioxide on Cu electrodes using renewable electricity is a highly promising approach to generate a sustainable supply of useful fuels and chemical feedstocks. In this thesis, we first examined the effects of *CO coverage and surface structure on the selective formation of ethylene, by performing electrochemical studies and theoretical calculations on Cu single-crystal surfaces. The electrolyte anion was also found to greatly enhance the formation of ethylene and ethanol, with their catalytic performance directly related to the anion’s adsorption strengths on the Cu surfaces. We further reported the unique dopant effect of sulfur on copper surface for selective formate production and demonstrated a clear positive correlation between the surface sulfur content and the production of formate. A good understanding of these factors will allow the efficient and selective conversion of carbon dioxide to high-value added molecules to be achieved.