Direct-Z-scheme g-C_(3)N_(4)/Ti_(3)C_(2)/TiO_(2)photocatalyst with giant internal electric field was prepared by onestep aqueous sonication self-assembly method using g-C_(3)N_(4)and MXene of Ti_(3)C_(2)as the source ...Direct-Z-scheme g-C_(3)N_(4)/Ti_(3)C_(2)/TiO_(2)photocatalyst with giant internal electric field was prepared by onestep aqueous sonication self-assembly method using g-C_(3)N_(4)and MXene of Ti_(3)C_(2)as the source materials.The chemical composition and structure of the catalysts was characterized by FT-IR,XRD,SEM,TEM,and XPS.The XPS characterization indicated that Ti_(3)C_(2)was partially oxidized to TiO_(2)during the composite process.As a result,an efficient direct-Z-scheme heterojunction structure consisting of the g-C_(3)N_(4)and TiO_(2)with Ti_(3)C_(2)as an electron bridge was constructed.The photocatalytic performance of the prepared catalysts was evaluated by degrading the Rhodamine B(RhB)wastewater.Compared with the single g-C_(3)N_(4),the g-C_(3)N_(4)/Ti_(3)C_(2)/TiO_(2)composite photocatalyst exhibited efficient and stable photocatalytic degradation ability,with a degradation efficiency as high as 99.2%for RhB under optimal conditions(2%Ti_(3)C_(2),pH=3).The high degradation performance of g-C_(3)N_(4)/Ti_(3)C_(2)/TiO_(2)for RhB was attributed to the combination of Ti_(3)C_(2),TiO_(2),and g-C_(3)N_(4)components,forming a direct-Z-scheme heterojunction with a high-speed electron transport channel structure.The role of Z-scheme heterojunctions in electron transport is verified by photoelectrochemical characterization,along with photoluminescence(PL).Our research provides a simple method to design photocatalysts by constructing direct-Z-scheme electron transport channels for highly efficient treatment of dye wastewater.展开更多
Over the past decade, graphitic carbon nitride(g-C_(3)N_(4)) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C_(3)N_(4) is stil...Over the past decade, graphitic carbon nitride(g-C_(3)N_(4)) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C_(3)N_(4) is still confronted with a general fatal issue of insufficient supply of thermodynamically active photocarriers due to its inferior solar harvesting ability and sluggish charge transfer dynamics. Fortunately, this could be significantly alleviated by the “all-in-one” defect engineering strategy, which enables a simultaneous amelioration of both textural uniqueness and intrinsic electronic band structures. To this end, we have summarized an unprecedently comprehensive discussion on defect controls including the vacancy/non-metallic dopant creation with optimized electronic band structure and electronic density, metallic doping with ultraactive coordinated environment(M–N_(x), M–C_(2)N_(2), M–O bonding), functional group grafting with optimized band structure, and promoted crystallinity with extended conjugation π system with weakened interlayered van der Waals interaction. Among them, the defect states induced by various defect types such as N vacancy, P/S/halogen dopants, and cyano group in boosting solar harvesting and accelerating photocarrier transfer have also been emphasized. More importantly, the shallow defect traps identified by femtosecond transient absorption spectra(fs-TAS) have also been highlighted. It is believed that this review would pave the way for future readers with a unique insight into a more precise defective g-C_(3)N_(4) “customization”, motivating more profound thinking and flourishing research outputs on g-C_(3)N_(4)-based photocatalysis.展开更多
基金supported by the National Natural Science Foundation of China(22078138)the Natural Science Foundation of Jiangxi Province(20202ACBL203009).
文摘Direct-Z-scheme g-C_(3)N_(4)/Ti_(3)C_(2)/TiO_(2)photocatalyst with giant internal electric field was prepared by onestep aqueous sonication self-assembly method using g-C_(3)N_(4)and MXene of Ti_(3)C_(2)as the source materials.The chemical composition and structure of the catalysts was characterized by FT-IR,XRD,SEM,TEM,and XPS.The XPS characterization indicated that Ti_(3)C_(2)was partially oxidized to TiO_(2)during the composite process.As a result,an efficient direct-Z-scheme heterojunction structure consisting of the g-C_(3)N_(4)and TiO_(2)with Ti_(3)C_(2)as an electron bridge was constructed.The photocatalytic performance of the prepared catalysts was evaluated by degrading the Rhodamine B(RhB)wastewater.Compared with the single g-C_(3)N_(4),the g-C_(3)N_(4)/Ti_(3)C_(2)/TiO_(2)composite photocatalyst exhibited efficient and stable photocatalytic degradation ability,with a degradation efficiency as high as 99.2%for RhB under optimal conditions(2%Ti_(3)C_(2),pH=3).The high degradation performance of g-C_(3)N_(4)/Ti_(3)C_(2)/TiO_(2)for RhB was attributed to the combination of Ti_(3)C_(2),TiO_(2),and g-C_(3)N_(4)components,forming a direct-Z-scheme heterojunction with a high-speed electron transport channel structure.The role of Z-scheme heterojunctions in electron transport is verified by photoelectrochemical characterization,along with photoluminescence(PL).Our research provides a simple method to design photocatalysts by constructing direct-Z-scheme electron transport channels for highly efficient treatment of dye wastewater.
基金the support of the Australia Research Council (ARC) through the Discovery Project (DP230101040)the Natural Science Foundation of Shandong Province (ZR2022QB139, No. ZR2020KF025)+3 种基金the Starting Research Fund (Grant No. 20210122) from the Ludong Universitythe Natural Science Foundation of China (12274190) from the Ludong Universitythe support of the Shandong Youth Innovation Team Introduction and Education Programthe Special Fund for Taishan Scholars Project (No. tsqn202211186) in Shandong Province。
文摘Over the past decade, graphitic carbon nitride(g-C_(3)N_(4)) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C_(3)N_(4) is still confronted with a general fatal issue of insufficient supply of thermodynamically active photocarriers due to its inferior solar harvesting ability and sluggish charge transfer dynamics. Fortunately, this could be significantly alleviated by the “all-in-one” defect engineering strategy, which enables a simultaneous amelioration of both textural uniqueness and intrinsic electronic band structures. To this end, we have summarized an unprecedently comprehensive discussion on defect controls including the vacancy/non-metallic dopant creation with optimized electronic band structure and electronic density, metallic doping with ultraactive coordinated environment(M–N_(x), M–C_(2)N_(2), M–O bonding), functional group grafting with optimized band structure, and promoted crystallinity with extended conjugation π system with weakened interlayered van der Waals interaction. Among them, the defect states induced by various defect types such as N vacancy, P/S/halogen dopants, and cyano group in boosting solar harvesting and accelerating photocarrier transfer have also been emphasized. More importantly, the shallow defect traps identified by femtosecond transient absorption spectra(fs-TAS) have also been highlighted. It is believed that this review would pave the way for future readers with a unique insight into a more precise defective g-C_(3)N_(4) “customization”, motivating more profound thinking and flourishing research outputs on g-C_(3)N_(4)-based photocatalysis.