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
Construction of multi-channels of photo-carrier migration in photocatalysts is favor to boost conversion efficiency of solar energy by promoting the charge separation and transfer.Herein,a ternary ZnIn_(2)S_(4)/g-C_(3...Construction of multi-channels of photo-carrier migration in photocatalysts is favor to boost conversion efficiency of solar energy by promoting the charge separation and transfer.Herein,a ternary ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene hybrid composed of S-scheme junction integrated Schottky-junction was fabricated using a simple hydrothermal approach.All the components(g-C_(3)N_(4),ZnIn_(2)S_(4) and Ti_(3)C_(2) MXene)demonstrated two-dimensional(2D)nanosheets structure,leading to the formation of a 2D/2D/2D sandwich-like structure with intimate large interface for carrier migration.Furthermore,the photogenerated carriers on the g-C_(3)N_(4) possessed dual transfer channels,including one route in S-scheme transfer mode between the g-C_(3)N_(4) and ZnIn_(2)S_(4) and the other route in Schottky-junction between g-C_(3)N_(4) and Ti_(3)C_(2) MXene.Consequently,a highly efficient carrier separation and transport was realized in the ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene heterojunction.This ternary sample exhibited wide light response from 200 to 1400 nm and excellent photocatalytic H_(2) evolution of 2452.1μmol∙g^(–1)∙h^(–1),which was 200,3,1.5 and 1.6 times of g-C_(3)N_(4),ZnIn_(2)S_(4),ZnIn_(2)S_(4)/Ti_(3)C_(2) MXene and g-C_(3)N_(4)/ZnIn_(2)S_(4) binary composites.This work offers a paradigm for the rational construction of multi-electron pathways to regulate the charge separation and migration via the introduction of dual-junctions in catalytic system.展开更多
Establishing highly effective charge transfer channels in carbon nitride(g-C_(3)N_(4)) to enhance its photocatalytic activity is still a challenging issue.Herein,the delaminated 2D Ti_(3)C_(2) MXene nanosheets were em...Establishing highly effective charge transfer channels in carbon nitride(g-C_(3)N_(4)) to enhance its photocatalytic activity is still a challenging issue.Herein,the delaminated 2D Ti_(3)C_(2) MXene nanosheets were employed to decorate the P-doped tubular g-C_(3)N_(4)(PTCN)for engineering 1D/2D Schottky heterojunction(PTCN/TC)through electrostatic self-assembly.The optimized PTCN/TC exhibited the highest hydrogen evolution rate(565 μmol h^(-1)g^(-1)),which was 4.3 and 2.0-fold higher than pristine bulk g-C_(3)N_(4) and PTCN,respectively.Such enhancement may be primarily attributed to the phosphorus heteroatom doped and unique structure of 1D/2D g-C_(3)N_(4)/Ti_(3)C_(2) Schottky heterojunction,enhancing the light-harvesting and charges’separation.One-dimensional pathway of g-C_(3)N_(4) tube and built-in electric field of interfacial Schottky effect can significantly facilitate the spatial separation of photogenerated charge carriers,and simultaneously inhibit their recombination via Schottky barrier.In this composite,metallic Ti_(3)C_(2) was served as electrons sink and photons collector.Moreover,ultrathin Ti_(3)C_(2) flake with exposed terminal metal sites as a co-catalyst exhibited higher photocatalytic reactivity in H2 evolution compared to carbon materials(such as reduced graphene oxide).This work not only proposed the mechanism of tubular g-C_(3)N_(4)/Ti_(3)C_(2) Schottky junction in photocatalysis,but also provided a feasible way to load ultrathin Ti_(3)C_(2) as a co-catalyst for designing highly efficient photocatalysts.展开更多
g-C_(3)N_(4) coupled with high specific area TiO_(2)(HSA-TiO_(2))composite was prepared by a simple solvothermal method,which was easy to operate with low energy consumption.Degradation of methyl orange test results s...g-C_(3)N_(4) coupled with high specific area TiO_(2)(HSA-TiO_(2))composite was prepared by a simple solvothermal method,which was easy to operate with low energy consumption.Degradation of methyl orange test results showed that HSA-TiO_(2) effectively improved the photocatalytic activity effectively.Photoelectrochemical test results indicated that the separation of photo-generated carriers and the charge carrier migration speed of TiO_(2) were improved after combination with g-C_(3)N_(4).g-C3N4/HSA-TiO_(2) showed strong photocatalytic ability.The degree of degradation of methyl orange by 6%-g-C_(3)N_(4)/HSA-TiO_(2) could reach up to 92.44%.Furthermore,it revealed good cycle performance.The photocatalytic mechanism of g-C_(3)N_(4)/HSA-TiO_(2) was proposed.展开更多
Carbon nitride(g-C_(3)N_(4))is a promising metal-free and visible-light-responsive photocatalyst.However,its photocatalytic efficiency still suffers from high recombination rates of photoinduced charge carriers,slow k...Carbon nitride(g-C_(3)N_(4))is a promising metal-free and visible-light-responsive photocatalyst.However,its photocatalytic efficiency still suffers from high recombination rates of photoinduced charge carriers,slow kinetics of surface redox reactions,and relatively poor light absorption.Herein,a non-noble metal photocatalyst of MoS_(2) nanodots anchored on P-doped g-C_(3)N_(4) via in situ photodeposition was constructed.With the synergetic effect of the P-doping and MoS_(2) co-catalyst,the as-prepared P-doped g-C_(3)N_(4)/MoS_(2) catalyst has achieved efficient photocatalytic overall water splitting with a hydrogen evolution rate of 121.7μmol h−1 g−1.Experimental results and Density functional theory(DFT)simulations indicate that the enhanced photo-absorption capacity originates from the reduced band gaps by P doping.Meanwhile,the MoS_(2) reduces the overpotential of the water oxidation process and improves hydrogen adsorption capability in the hydrogen evolution reaction.This work can pave a new avenue to design and develop noble-metal-free water-splitting photocatalysts for future large-scale applications.展开更多
CeO_(2)/g-C_(3)N_(4)photocatalysts have attracted tremendous attention in the photocatalytic degradation of organic pollutants.The design and construction of highly active CeO_(2)/g-C_(3)N_(4)photocatalysts without ha...CeO_(2)/g-C_(3)N_(4)photocatalysts have attracted tremendous attention in the photocatalytic degradation of organic pollutants.The design and construction of highly active CeO_(2)/g-C_(3)N_(4)photocatalysts without harsh conditions are still challenging.Herein,highly dispersed CeO_(2-x)nanoparticles with rich oxygen vacancies were successfully precipitated on the surface of g-C_(3)N_(4)under mild conditions.The fabricated CeO_(2-x)/g-C_(3)N_(4)exhibits remarkable activity and stability for photocatalytic degradation of MO pollutant.The optimal rate constant of MO degradation over CeO_(2-x)/g-C_(3)N_(4)is about 0.031 min^(-1),which is three times higher than that of g-C_(3)N_(4).A negligible activity decrease is observed after three cycling runs.The enhanced catalytic performance can be ascribed to the excellent dispersion of CeO_(2-x)with rich oxygen vacancies that benefit O_(2)adsorption and visible light absorption.In addition,the proper band alignment between CeO_(2-x)and gC_(3)N_(4)is conducive to the highly efficient separation of photogenerated electron-hole pairs.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.
文摘Construction of multi-channels of photo-carrier migration in photocatalysts is favor to boost conversion efficiency of solar energy by promoting the charge separation and transfer.Herein,a ternary ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene hybrid composed of S-scheme junction integrated Schottky-junction was fabricated using a simple hydrothermal approach.All the components(g-C_(3)N_(4),ZnIn_(2)S_(4) and Ti_(3)C_(2) MXene)demonstrated two-dimensional(2D)nanosheets structure,leading to the formation of a 2D/2D/2D sandwich-like structure with intimate large interface for carrier migration.Furthermore,the photogenerated carriers on the g-C_(3)N_(4) possessed dual transfer channels,including one route in S-scheme transfer mode between the g-C_(3)N_(4) and ZnIn_(2)S_(4) and the other route in Schottky-junction between g-C_(3)N_(4) and Ti_(3)C_(2) MXene.Consequently,a highly efficient carrier separation and transport was realized in the ZnIn_(2)S_(4)/g-C_(3)N_(4)/Ti_(3)C_(2) MXene heterojunction.This ternary sample exhibited wide light response from 200 to 1400 nm and excellent photocatalytic H_(2) evolution of 2452.1μmol∙g^(–1)∙h^(–1),which was 200,3,1.5 and 1.6 times of g-C_(3)N_(4),ZnIn_(2)S_(4),ZnIn_(2)S_(4)/Ti_(3)C_(2) MXene and g-C_(3)N_(4)/ZnIn_(2)S_(4) binary composites.This work offers a paradigm for the rational construction of multi-electron pathways to regulate the charge separation and migration via the introduction of dual-junctions in catalytic system.
基金the financial supports from the National Natural Science Foundation of China(No.:22002146)Taishan Scholars Foundation of Shandong province(No.:tsqn201909058).
文摘Establishing highly effective charge transfer channels in carbon nitride(g-C_(3)N_(4)) to enhance its photocatalytic activity is still a challenging issue.Herein,the delaminated 2D Ti_(3)C_(2) MXene nanosheets were employed to decorate the P-doped tubular g-C_(3)N_(4)(PTCN)for engineering 1D/2D Schottky heterojunction(PTCN/TC)through electrostatic self-assembly.The optimized PTCN/TC exhibited the highest hydrogen evolution rate(565 μmol h^(-1)g^(-1)),which was 4.3 and 2.0-fold higher than pristine bulk g-C_(3)N_(4) and PTCN,respectively.Such enhancement may be primarily attributed to the phosphorus heteroatom doped and unique structure of 1D/2D g-C_(3)N_(4)/Ti_(3)C_(2) Schottky heterojunction,enhancing the light-harvesting and charges’separation.One-dimensional pathway of g-C_(3)N_(4) tube and built-in electric field of interfacial Schottky effect can significantly facilitate the spatial separation of photogenerated charge carriers,and simultaneously inhibit their recombination via Schottky barrier.In this composite,metallic Ti_(3)C_(2) was served as electrons sink and photons collector.Moreover,ultrathin Ti_(3)C_(2) flake with exposed terminal metal sites as a co-catalyst exhibited higher photocatalytic reactivity in H2 evolution compared to carbon materials(such as reduced graphene oxide).This work not only proposed the mechanism of tubular g-C_(3)N_(4)/Ti_(3)C_(2) Schottky junction in photocatalysis,but also provided a feasible way to load ultrathin Ti_(3)C_(2) as a co-catalyst for designing highly efficient photocatalysts.
基金supported by the National Natural Science Foundation of China(No.61308095,No.21801092,and No.11904128)the Program for the Development of Science and Technology of Jilin province(No.20180520002JH)+1 种基金the Graduate Innovation Project of Jilin Normal University(No.201941)the Key Research Programs in Universities of Henan Province(20A150031).
文摘g-C_(3)N_(4) coupled with high specific area TiO_(2)(HSA-TiO_(2))composite was prepared by a simple solvothermal method,which was easy to operate with low energy consumption.Degradation of methyl orange test results showed that HSA-TiO_(2) effectively improved the photocatalytic activity effectively.Photoelectrochemical test results indicated that the separation of photo-generated carriers and the charge carrier migration speed of TiO_(2) were improved after combination with g-C_(3)N_(4).g-C3N4/HSA-TiO_(2) showed strong photocatalytic ability.The degree of degradation of methyl orange by 6%-g-C_(3)N_(4)/HSA-TiO_(2) could reach up to 92.44%.Furthermore,it revealed good cycle performance.The photocatalytic mechanism of g-C_(3)N_(4)/HSA-TiO_(2) was proposed.
基金supported by Guangdong Basic and Ap-plied Basic Research Foundation(Nos.2021A1515110003 and 2020A1515110332)financial support from the National Natural Science Foundation of China(Nos.51974158 and 21902070)+2 种基金Scientific Research Projects of Key Disciplines in Guangdong Province(No.2019-GDXK-0023)Projects of“Leiyang Scholar”post plan of Lingnan Normal University(2021)Open Project of Key Laboratory of Chean Energy Material Chemistry in Guangdong General University(No.CEMC2022011).
文摘Carbon nitride(g-C_(3)N_(4))is a promising metal-free and visible-light-responsive photocatalyst.However,its photocatalytic efficiency still suffers from high recombination rates of photoinduced charge carriers,slow kinetics of surface redox reactions,and relatively poor light absorption.Herein,a non-noble metal photocatalyst of MoS_(2) nanodots anchored on P-doped g-C_(3)N_(4) via in situ photodeposition was constructed.With the synergetic effect of the P-doping and MoS_(2) co-catalyst,the as-prepared P-doped g-C_(3)N_(4)/MoS_(2) catalyst has achieved efficient photocatalytic overall water splitting with a hydrogen evolution rate of 121.7μmol h−1 g−1.Experimental results and Density functional theory(DFT)simulations indicate that the enhanced photo-absorption capacity originates from the reduced band gaps by P doping.Meanwhile,the MoS_(2) reduces the overpotential of the water oxidation process and improves hydrogen adsorption capability in the hydrogen evolution reaction.This work can pave a new avenue to design and develop noble-metal-free water-splitting photocatalysts for future large-scale applications.
基金Project supported by the Guangdong Provincial Education Department Special Project of Key Research Areas(2020ZDZX2066)the Innovation Team of Universities of Guangdong Province(2020KCXTD011)+2 种基金the Engineering Research Center of Universities of Guangdong Province(2019GCZX002)the Guangdong Key Laboratory for Hydrogen Energy Technologies(2018B030322005)Guangdong Basic and Applied Basic Research Foundation(2019A1515110586,2019A1515110534)。
文摘CeO_(2)/g-C_(3)N_(4)photocatalysts have attracted tremendous attention in the photocatalytic degradation of organic pollutants.The design and construction of highly active CeO_(2)/g-C_(3)N_(4)photocatalysts without harsh conditions are still challenging.Herein,highly dispersed CeO_(2-x)nanoparticles with rich oxygen vacancies were successfully precipitated on the surface of g-C_(3)N_(4)under mild conditions.The fabricated CeO_(2-x)/g-C_(3)N_(4)exhibits remarkable activity and stability for photocatalytic degradation of MO pollutant.The optimal rate constant of MO degradation over CeO_(2-x)/g-C_(3)N_(4)is about 0.031 min^(-1),which is three times higher than that of g-C_(3)N_(4).A negligible activity decrease is observed after three cycling runs.The enhanced catalytic performance can be ascribed to the excellent dispersion of CeO_(2-x)with rich oxygen vacancies that benefit O_(2)adsorption and visible light absorption.In addition,the proper band alignment between CeO_(2-x)and gC_(3)N_(4)is conducive to the highly efficient separation of photogenerated electron-hole pairs.
