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

ABSTRACT

Copper oxide-based materials effectively electrocatalyze carbon dioxide reduction (CO2 RR). To comprehend their role and achieve high CO2 RR activity, Cu+ in copper oxides must be stabilized. As an electrocatalyst, Cu2 O nanoparticles were decorated with hexagonal boron nitride (h-BN) nanosheets to stabilize Cu+ . The C2 H4 /CO ratio increased 1.62-fold in the CO2 RR with Cu2 O-BN compared to that with Cu2 O. Experimental and theoretical studies confirmed strong electronic interactions between the two components in Cu2 O-BN, which strengthens the Cu-O bonds. Electrophilic h-BN receives partial electron density from Cu2 O, protecting the Cu-O bonds from electron attack during the CO2 RR and stabilizing the Cu+ species during long-term electrolysis. The well-retained Cu+ species enhanced the C2 product selectivity and improved the stability of Cu2 O-BN. This work offers new insight into the metal-valence-state-dependent selectivity of catalysts, enabling the design of advanced catalysts.