Discovering highly selective catalysts is key to achieve effective CO_(2) photoreduction to hydrocarbon fuels.In this work,we construct an ultrathin dimension-matched S-scheme Bi_(3)NbO_(7)/g-C_(3)N_(4) heterostructur...Discovering highly selective catalysts is key to achieve effective CO_(2) photoreduction to hydrocarbon fuels.In this work,we construct an ultrathin dimension-matched S-scheme Bi_(3)NbO_(7)/g-C_(3)N_(4) heterostructure,which permits the highly selective photocatalytic reduction of CO_(2) to CH_(4),as shown by 13C isotopic measurements.Density functional theory calculations combined with solid-state characterization confirm the electron transfer from g-C_(3)N_(4) nanosheets to Bi_(3)NbO_(7),establishing an internal electric field.The internal electric field drives photogenerated electrons from Bi_(3)NbO_(7) to g-C_(3)N_(4),as revealed by in-situ X-ray photoelectron spectroscopy,demonstrating the presence of an S-scheme charge transfer path in Bi_(3)NbO_(7)/g-C_(3)N_(4) heterostructures allowing efficient and selective CO2 photoreduction.As a result,the optimized sample achieved a CH_(4) evolution rate of 37.59μmol·g^(-1)·h^(-1),a ca.15-fold enhancement compared to ultrathin g-C_(3)N_(4) nanosheets,and also retained stability after 10 reaction cycles and 40 h of simulated solar irradiation with no sacrificial reagents.The optimized Bi3 Nb O7/g-C_(3)N_(4) composites achieve almost 90%selectivity for CH_(4) production over CO.展开更多
文摘Discovering highly selective catalysts is key to achieve effective CO_(2) photoreduction to hydrocarbon fuels.In this work,we construct an ultrathin dimension-matched S-scheme Bi_(3)NbO_(7)/g-C_(3)N_(4) heterostructure,which permits the highly selective photocatalytic reduction of CO_(2) to CH_(4),as shown by 13C isotopic measurements.Density functional theory calculations combined with solid-state characterization confirm the electron transfer from g-C_(3)N_(4) nanosheets to Bi_(3)NbO_(7),establishing an internal electric field.The internal electric field drives photogenerated electrons from Bi_(3)NbO_(7) to g-C_(3)N_(4),as revealed by in-situ X-ray photoelectron spectroscopy,demonstrating the presence of an S-scheme charge transfer path in Bi_(3)NbO_(7)/g-C_(3)N_(4) heterostructures allowing efficient and selective CO2 photoreduction.As a result,the optimized sample achieved a CH_(4) evolution rate of 37.59μmol·g^(-1)·h^(-1),a ca.15-fold enhancement compared to ultrathin g-C_(3)N_(4) nanosheets,and also retained stability after 10 reaction cycles and 40 h of simulated solar irradiation with no sacrificial reagents.The optimized Bi3 Nb O7/g-C_(3)N_(4) composites achieve almost 90%selectivity for CH_(4) production over CO.
