Stabilization of Cu+ via Strong Electronic Interaction for Selective and Stable CO2 Electroreduction

Copper oxide-based materials effectively electrocatalyze carbon dioxide reduction (CO2RR). To comprehend their role and achieve high CO2RR activity, Cu+ in copper oxides must be stabilized. As an electrocatalyst, Cu2O nanoparticles were decorated with hexagonal boron nitride (h-BN) nanosheets to stabilize Cu+. The C2H4/CO ratio increased 1.62-fold in the CO2RR with Cu2O-BN compared to that with Cu2O. Experimental and theoretical studies confirmed strong electronic interactions between the two components in Cu2O-BN, which strengthens the Cu-O bonds. Electrophilic h-BN receives partial electron density from Cu2O, protecting the Cu-O bonds from electron attack during the CO2RR and stabilizing the Cu+ species during long-term electrolysis. The well-retained Cu+ species enhanced the C-2 product selectivity and improved the stability of Cu2O-BN. This work offers new insight into the metal-valence-state-dependent selectivity of catalysts, enabling the design of advanced catalysts.