Using low-cost precipitated silica(SiO2) as the carrier,a ternary SiO2-TiO2/g-C3N4 composite photocatalyst was prepared via the sol-gel method associated with a wet-grinding process.The asprepared composite exhibits p...Using low-cost precipitated silica(SiO2) as the carrier,a ternary SiO2-TiO2/g-C3N4 composite photocatalyst was prepared via the sol-gel method associated with a wet-grinding process.The asprepared composite exhibits photocatalytic hydrogen production and pollutant degradation performance under solar-like irradiation.The effect of SiO2 carrier on the properties of the heterostructure between TiO2 and g-C3N4(CN) was systematically studied.It is found that SiO2 has important effects on promoting the interaction between TiO2 and CN.The particle size of TiO2 and CN was obviously reduced during the calcination process due to the effects of SiO2.Especially,the TiO2 particles exhibit monodispersed state with particle size below 10 nm(quantum dots),resulting in the improvement of the contact area and the interaction betweenTiO2 and CN,and leading to the formation of efficient TiO2/CN Zscheme heterostructure in SiO2-TiO2/CN.Besides,the introduction of SiO2 can increase the specific surface area and light absorption of SiO2-TiO2/CN,further promoting the photocatalytic reaction.As expected,the optimum SiO2-TiO2/CN composite exhibits 12.3,3.1 and 2.9 times higher photocatalytic hydrogen production rate than that of SiO2-TiO2,CN and TiO2/CN under solar-like irradiation,while the photocatalytic active component in SiO2-TiO2/CN is only about 60 wt%.Moreover,the rhodamine B degradation rate of SiO2-TiO2/CN is also higher than that of SiO2-TiO2,CN and TiO2/CN.展开更多
Doping engineering is an effective strategy for graphitic carbon nitride(g-C_(3)N_(4))to improve its photocat-alytic hydrogen evolution reaction(HER)performance.In this work,a novel nitrogen and sulfur co-doped g-C_(3...Doping engineering is an effective strategy for graphitic carbon nitride(g-C_(3)N_(4))to improve its photocat-alytic hydrogen evolution reaction(HER)performance.In this work,a novel nitrogen and sulfur co-doped g-C_(3)N_(4)(N,S-g-C_(3)N_(4))is elaborately designed on the basis of theoretical predictions of first-principle density functional theory(DFT).The calculated Gibbs free energy of adsorbed hydrogen(ΔGH∗)for N,S-g-C_(3)N_(4) at the N-doping active sites is extremely close to zero(0.01 eV).Inspired by the theoretical predictions,the N,S-g-C_(3)N_(4) is successfully fabricated through ammonia-rich pyrolysis synthesis strategy,in which ammonia is in-situ obtained by pyrolyzing melamine.Subsequent characterizations indicate that the N,S-g-C_(3)N_(4) possesses high specific surface area,outstanding light utilization,good hydrophilicity,and efficient carrier transfer efficiency.Consequently,the N,S-g-C_(3)N_(4) displays an extremely high H2 evolution rate of 8269.9μmol g−1 h−1,achieves an apparent quantum efficiency(AQE)of 3.24%,and also possesses outsatnding durability.Theoretical calculations further demonstrate that N and S dopants can not only introduce doping energy level to reduce the band gap,but also induce charge redistribution to facilitate hydrogen adsorption,thus promoting the photocatalytic HER process.Moreover,femtosecond transient absorption(fs-TA)spectroscopy further corroborates the efficient photogenerated carrier transport of N,S-g-C_(3)N_(4).This research highlights a promising and reliable strategy to achieve superior photocatalytic activity,and exhibits significant guidance for precise designing high-efficiency photocatalysts.展开更多
Photocatalytic H_(2)production from water splitting is a promising candidate for solving the increasing energy crisis and environmental issues.Herein we report a novel g-C_(3)N_(4)/Ag In_(x)S_(y)S-scheme heterojunctio...Photocatalytic H_(2)production from water splitting is a promising candidate for solving the increasing energy crisis and environmental issues.Herein we report a novel g-C_(3)N_(4)/Ag In_(x)S_(y)S-scheme heterojunction photocatalyst for water splitting into stoichiometric H_(2)and H_(2)O_(2)under visible light.The catalyst was prepared by depositing 3D bimetallic sulfide(Ag In_(x)S_(y))nanotubes onto 2D g-C_(3)N_(4)nanosheets.Owing to the special 3D-on-2D configuration,the photogenerated carriers could be rapidly transferred and effectively separated through the abundant interfacial heterostructures to avoid recombination,and therefore excellent performance for visible light-driven water splitting could be obtained,with a 24-h H_(2)evolution rate up to 237μmol g^(-1)h^(-1).Furthermore,suitable band alignment enables simultaneous H_(2)and H_(2)O_(2)production in a 1:1 stoichiometric ratio.H_(2)and H_(2)O_(2)were evolved on the conduction band of g-C_(3)N_(4)and on the valance band of Ag In_(x)S_(y),respectively.The novel 3D-on-2D configuration for heterojunction construction proposed in this work provided alternative research ideas toward photocatalytic reaction.展开更多
基金partly supported by the National Natural Science Foundation of China(Nos.21577132,21978276)。
文摘Using low-cost precipitated silica(SiO2) as the carrier,a ternary SiO2-TiO2/g-C3N4 composite photocatalyst was prepared via the sol-gel method associated with a wet-grinding process.The asprepared composite exhibits photocatalytic hydrogen production and pollutant degradation performance under solar-like irradiation.The effect of SiO2 carrier on the properties of the heterostructure between TiO2 and g-C3N4(CN) was systematically studied.It is found that SiO2 has important effects on promoting the interaction between TiO2 and CN.The particle size of TiO2 and CN was obviously reduced during the calcination process due to the effects of SiO2.Especially,the TiO2 particles exhibit monodispersed state with particle size below 10 nm(quantum dots),resulting in the improvement of the contact area and the interaction betweenTiO2 and CN,and leading to the formation of efficient TiO2/CN Zscheme heterostructure in SiO2-TiO2/CN.Besides,the introduction of SiO2 can increase the specific surface area and light absorption of SiO2-TiO2/CN,further promoting the photocatalytic reaction.As expected,the optimum SiO2-TiO2/CN composite exhibits 12.3,3.1 and 2.9 times higher photocatalytic hydrogen production rate than that of SiO2-TiO2,CN and TiO2/CN under solar-like irradiation,while the photocatalytic active component in SiO2-TiO2/CN is only about 60 wt%.Moreover,the rhodamine B degradation rate of SiO2-TiO2/CN is also higher than that of SiO2-TiO2,CN and TiO2/CN.
基金supported by the National Natural Science Foun-dation of China(No.62004143)the Key R&D Program of Hubei Province(No.2022BAA084)the Natural Science Foundation of Hubei Province(No.2021CFB133).
文摘Doping engineering is an effective strategy for graphitic carbon nitride(g-C_(3)N_(4))to improve its photocat-alytic hydrogen evolution reaction(HER)performance.In this work,a novel nitrogen and sulfur co-doped g-C_(3)N_(4)(N,S-g-C_(3)N_(4))is elaborately designed on the basis of theoretical predictions of first-principle density functional theory(DFT).The calculated Gibbs free energy of adsorbed hydrogen(ΔGH∗)for N,S-g-C_(3)N_(4) at the N-doping active sites is extremely close to zero(0.01 eV).Inspired by the theoretical predictions,the N,S-g-C_(3)N_(4) is successfully fabricated through ammonia-rich pyrolysis synthesis strategy,in which ammonia is in-situ obtained by pyrolyzing melamine.Subsequent characterizations indicate that the N,S-g-C_(3)N_(4) possesses high specific surface area,outstanding light utilization,good hydrophilicity,and efficient carrier transfer efficiency.Consequently,the N,S-g-C_(3)N_(4) displays an extremely high H2 evolution rate of 8269.9μmol g−1 h−1,achieves an apparent quantum efficiency(AQE)of 3.24%,and also possesses outsatnding durability.Theoretical calculations further demonstrate that N and S dopants can not only introduce doping energy level to reduce the band gap,but also induce charge redistribution to facilitate hydrogen adsorption,thus promoting the photocatalytic HER process.Moreover,femtosecond transient absorption(fs-TA)spectroscopy further corroborates the efficient photogenerated carrier transport of N,S-g-C_(3)N_(4).This research highlights a promising and reliable strategy to achieve superior photocatalytic activity,and exhibits significant guidance for precise designing high-efficiency photocatalysts.
基金financially supported by the National Natural Science Foundation of China(Nos.52362012,42077162,51978323)Natural Science Foundation of Jiangxi Province(No.2022ACB203014)+4 种基金Major Discipline Academic and Technical Leaders Training Program of Jiangxi Province(Nos.20213BCJ22018,20232BCJ22048)Natural Science Project of the Educational Department in Jiangxi Province(No.GJJ2201121)Natural Science Foundation of Nanchang Hangkong University(No.EA202202256)Educational Reform Project of Jiangxi Province(No.JXYJG-2022-135)Nanchang Hangkong University Educational Reform Project(Nos.sz2214,sz2213,JY22017,KCPY1806)。
文摘Photocatalytic H_(2)production from water splitting is a promising candidate for solving the increasing energy crisis and environmental issues.Herein we report a novel g-C_(3)N_(4)/Ag In_(x)S_(y)S-scheme heterojunction photocatalyst for water splitting into stoichiometric H_(2)and H_(2)O_(2)under visible light.The catalyst was prepared by depositing 3D bimetallic sulfide(Ag In_(x)S_(y))nanotubes onto 2D g-C_(3)N_(4)nanosheets.Owing to the special 3D-on-2D configuration,the photogenerated carriers could be rapidly transferred and effectively separated through the abundant interfacial heterostructures to avoid recombination,and therefore excellent performance for visible light-driven water splitting could be obtained,with a 24-h H_(2)evolution rate up to 237μmol g^(-1)h^(-1).Furthermore,suitable band alignment enables simultaneous H_(2)and H_(2)O_(2)production in a 1:1 stoichiometric ratio.H_(2)and H_(2)O_(2)were evolved on the conduction band of g-C_(3)N_(4)and on the valance band of Ag In_(x)S_(y),respectively.The novel 3D-on-2D configuration for heterojunction construction proposed in this work provided alternative research ideas toward photocatalytic reaction.
