Solar-driven CO_(2)conversion into value-added chemical provides an attractive strategy for sustainable development.However,the enhanced CO_(2)photoreduction performance with target product selectivity remains a major...Solar-driven CO_(2)conversion into value-added chemical provides an attractive strategy for sustainable development.However,the enhanced CO_(2)photoreduction performance with target product selectivity remains a major challenge.Here,we develop a novel strategy involving Cu_(2)O nanoparticles in situ grown on the surface of ZIF-67-derived Co@C-N nanocages(CC)to create abundant active sites and appropriate heterointerfaces.A remarkable CO selectivity of 95.7%with a yield of 117.39μmol g-1h-1and an apparent quantum efficiency as high as 1.88%at 420 nm was obtained over CC-60 catalyst in pure water,which was 87.6 times higher than that of pure Cu_(2)O.Theoretical calculations and experiments indicated that Co@C-N nanocages as charge mediator not only rapidly trap photogenerated electrons to promote charge separation efficiency,but also regulate the d-band center of Cu atoms to move to the Fermi energy level,thereby optimizing the reaction kinetics to facilitate the highly selective conversion of the key intermediate*CO desorption to CO.展开更多
基金supported by the National Natural Science Foundation of China(22372013 and 22278042)Changzhou Leading Innovative Talents Introduction and Cultivation(CQ20230108)。
文摘Solar-driven CO_(2)conversion into value-added chemical provides an attractive strategy for sustainable development.However,the enhanced CO_(2)photoreduction performance with target product selectivity remains a major challenge.Here,we develop a novel strategy involving Cu_(2)O nanoparticles in situ grown on the surface of ZIF-67-derived Co@C-N nanocages(CC)to create abundant active sites and appropriate heterointerfaces.A remarkable CO selectivity of 95.7%with a yield of 117.39μmol g-1h-1and an apparent quantum efficiency as high as 1.88%at 420 nm was obtained over CC-60 catalyst in pure water,which was 87.6 times higher than that of pure Cu_(2)O.Theoretical calculations and experiments indicated that Co@C-N nanocages as charge mediator not only rapidly trap photogenerated electrons to promote charge separation efficiency,but also regulate the d-band center of Cu atoms to move to the Fermi energy level,thereby optimizing the reaction kinetics to facilitate the highly selective conversion of the key intermediate*CO desorption to CO.
