The rational fabrication of an efficient heterojunction is critical to the enhancement of photocatalytic hydrogen(H_(2)) evolution performance.Herein,a new-fashioned graphitic-carbon nitride(g-C_(3) N_(4)) based isoty...The rational fabrication of an efficient heterojunction is critical to the enhancement of photocatalytic hydrogen(H_(2)) evolution performance.Herein,a new-fashioned graphitic-carbon nitride(g-C_(3) N_(4)) based isotype step-scheme(S-scheme) heterojunction composed of sulfur-doped and sulfur-free active sites is developed by liquid sulfur-mediation of exfoliated g-C_(3) N_(4).Particularly,the liquid sulfur not only contributes to the full contact between sulfur species and exfoliated g-C_(3) N_(4),but also creates sulfur-doping and abundant pores,since self-gas foaming effect of sulfur vapor.Moreover,the S-doped and S-free active sites located in the structural unit of C_(3) N_(4) jointly construct a typical sulfur-doped g-C_(3) N_(4)/g-C_(3) N_(4) isotype step-scheme heterojunction,which endows highly efficient photocatalytic reaction process.Therefore,the optimal sample possesses remarkable photocatalytic H_(2) evolution activity(5548.1 μmol g^(-1) h^(-1)) and robust durability.Most importantly,the investigation will open up a new path for the exploration of other carbon-based isotype S-scheme heterojunctions.展开更多
The rational construction of a high-efficiency stepscheme heterojunctions is an effective strategy to accelerate the photocatalytic H_(2).Unfortunately,the variant energy-level matching between two different semicondu...The rational construction of a high-efficiency stepscheme heterojunctions is an effective strategy to accelerate the photocatalytic H_(2).Unfortunately,the variant energy-level matching between two different semiconductor confers limited the photocatalytic performance.Herein,a newfangled graphitic-carbon nitride(g-C_(3)N_(4))based isotype step-scheme heterojunction,which consists of sulfur-doped and defective active sites in one microstructural unit,is successfully developed by in-situ polymerizing N,N-dimethylformamide(DMF)and urea,accompanied by sulfur(S)powder.Therein,the polymerization between the amino groups of DMF and the amide group of urea endows the formation of rich defects.The propulsive integration of S-dopants contributes to the excellent fluffiness and dispersibility of lamellar g-C_(3)N_(4).Moreover,the developed heterojunction exhibits a significantly enlarged surface area,thus leading to the more exposed catalytically active sites.Most importantly,the simultaneous introduction of S-doping and defects in the units of g-C_(3)N_(4) also results in a significant improvement in the separation,transfer and recombination efficiency of photo-excited electron-hole pairs.Therefore,the resulting isotype step-scheme heterojunction possesses a superior photocatalytic H_(2) evolution activity in comparison with pristine g-C_(3)N_(4).The newly afforded metal-free isotype step-scheme heterojunction in this work will supply a new insight into coupling strategies of heteroatoms doping and defect engineering for various photocatalytic systems.展开更多
基金supported by the National Natural Science Foundation of China (Nos.62004143 and 21975084)the Central Government Guided Local Science and Technology Development Special Fund Project (No.2020ZYYD033)+5 种基金the Natural Science Foundation of Hubei Province (No.2021CFB133)the Opening Fund of Key Laboratory of Rare Mineral,Ministry of Natural Resources(No.KLRM-KF 202005)the Opening Fund of Key Laboratory for Green Chemical Process of Ministry of Education of Wuhan Institute of Technology (No.GCP202101)the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage (HUST),Ministry of Education (No.2021JYBKF05)the Innovation Project of Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education (No.LCX2021003)the 12^(th) Graduate Education Innovation Fund of Wuhan Institute of Technology (No.CX2020341)。
文摘The rational fabrication of an efficient heterojunction is critical to the enhancement of photocatalytic hydrogen(H_(2)) evolution performance.Herein,a new-fashioned graphitic-carbon nitride(g-C_(3) N_(4)) based isotype step-scheme(S-scheme) heterojunction composed of sulfur-doped and sulfur-free active sites is developed by liquid sulfur-mediation of exfoliated g-C_(3) N_(4).Particularly,the liquid sulfur not only contributes to the full contact between sulfur species and exfoliated g-C_(3) N_(4),but also creates sulfur-doping and abundant pores,since self-gas foaming effect of sulfur vapor.Moreover,the S-doped and S-free active sites located in the structural unit of C_(3) N_(4) jointly construct a typical sulfur-doped g-C_(3) N_(4)/g-C_(3) N_(4) isotype step-scheme heterojunction,which endows highly efficient photocatalytic reaction process.Therefore,the optimal sample possesses remarkable photocatalytic H_(2) evolution activity(5548.1 μmol g^(-1) h^(-1)) and robust durability.Most importantly,the investigation will open up a new path for the exploration of other carbon-based isotype S-scheme heterojunctions.
基金This work was supported by the National Natural Science Foundation of China(No.62004143)the Central Government Guided Local Science and Technology Development Special Fund Project(No.2020ZYYD033)+4 种基金the Natural Science Foundation of Hubei Province(No.2021CFB133)the Opening Fund of Key Laboratory of Rare Mineral Ministry of Natural Resources(No.KLRM-KF 202005)the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage(HUST),Ministry of Education(No.2021JYBKF05)the Opening Fund of Key Laboratory for Green Chemical Process of Ministry of Education of Wuhan Institute of Technology(No.GCP202101)the Innovation Project of Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education(No.LCX2021003)。
文摘The rational construction of a high-efficiency stepscheme heterojunctions is an effective strategy to accelerate the photocatalytic H_(2).Unfortunately,the variant energy-level matching between two different semiconductor confers limited the photocatalytic performance.Herein,a newfangled graphitic-carbon nitride(g-C_(3)N_(4))based isotype step-scheme heterojunction,which consists of sulfur-doped and defective active sites in one microstructural unit,is successfully developed by in-situ polymerizing N,N-dimethylformamide(DMF)and urea,accompanied by sulfur(S)powder.Therein,the polymerization between the amino groups of DMF and the amide group of urea endows the formation of rich defects.The propulsive integration of S-dopants contributes to the excellent fluffiness and dispersibility of lamellar g-C_(3)N_(4).Moreover,the developed heterojunction exhibits a significantly enlarged surface area,thus leading to the more exposed catalytically active sites.Most importantly,the simultaneous introduction of S-doping and defects in the units of g-C_(3)N_(4) also results in a significant improvement in the separation,transfer and recombination efficiency of photo-excited electron-hole pairs.Therefore,the resulting isotype step-scheme heterojunction possesses a superior photocatalytic H_(2) evolution activity in comparison with pristine g-C_(3)N_(4).The newly afforded metal-free isotype step-scheme heterojunction in this work will supply a new insight into coupling strategies of heteroatoms doping and defect engineering for various photocatalytic systems.
