Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 31, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202205832
Keywords
CO2 Electroreduction; Copper Valence State; Cu2O; Hexagonal Boron Nitride; Strong Electronic Interaction
Categories
Funding
- National Natural Science Foundation of China [21575016, U20A20154]
- National Program for Support of Top-notch Young Professionals
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This study successfully stabilized Cu+ in copper oxides by decorating Cu2O nanoparticles with hexagonal boron nitride (h-BN) nanosheets, leading to enhanced activity and selectivity for carbon dioxide reduction. The strong electronic interactions between the h-BN and Cu2O components in Cu2O-BN were confirmed by experimental and theoretical studies, strengthening the Cu-O bonds. By protecting the Cu-O bonds from electron attack, the electrophilic h-BN stabilized the Cu+ species during long-term electrolysis.
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.
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