Constructing step-scheme(S-scheme)heterojunctions has been confirmed as a promising strategy for enhancing the photocatalytic activity of composite materials.In this work,a series of sulfur-doped g-C3N4(SCN)/TiO2 S-sc...Constructing step-scheme(S-scheme)heterojunctions has been confirmed as a promising strategy for enhancing the photocatalytic activity of composite materials.In this work,a series of sulfur-doped g-C3N4(SCN)/TiO2 S-scheme photocatalysts were synthesized using electrospinning and calcination methods.The as-prepared SCN/TiO2 composites showed superior photocatalytic performance than pure TiO2 and SCN in the photocatalytic degradation of Congo Red(CR)aqueous solution.The significant enhancement in photocatalytic activity benefited not only from the 1D well-distributed nanostructure,but also from the S-scheme heterojunction.Furthermore,the XPS analyses and DFT calculations demonstrated that electrons were transferred from SCN to TiO2 across the interface of the SCN/TiO2 composites.The built-in electric field,band edge bending,and Coulomb interaction synergistically facilitated the recombination of relatively useless electrons and holes in hybrid when the interface was irradiated by simulated solar light.Therefore,the remaining electrons and holes with higher reducibility and oxidizability endowed the composite with supreme redox ability.These results were adequately verified by radical trapping experiments,ESR tests,and in situ XPS analyses,suggesting that the electron immigration in the photocatalyst followed the S-scheme heterojunction mechanism.This work can enrich our knowledge of the design and fabrication of novel S-scheme heterojunction photocatalysts and provide a promising strategy for solving environmental pollution in the future.展开更多
Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate ...Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate photocatalysts.Herein,a novel S-scheme Sb2WO6/g-C3N4 nanocomposite was fabricated by an ultrasound-assisted method,which exhibited excellent performance for photocatalytic ppb-level NO removal.Compared with the pure constituents of the nanocomposite,the as-prepared 15%-Sb2WO6/g-C3N4 photocatalyst could remove more than 68%continuous-flowing NO(initial concentration:400 ppb)under visible-light irradiation in 30 min.The findings of the trapping experiments confirmed that•O2^–and h+were the important active species in the NO oxidation reaction.Meanwhile,the transient photocurrent response and PL spectroscopy analyses proved that the unique S-scheme structure of the samples could enhance the charge separation efficiency.In situ DRIFTS revealed that the photocatalytic reaction pathway of NO removal over the Sb2WO6/g-C3N4 nanocomposite occurred via an oxygen-induced route.The present work proposes a new concept for fabricating efficient photocatalysts for photocatalytic ppb-level NO oxidation and provides deeper insights into the mechanism of photocatalytic NO oxidation.展开更多
Photocatalysis. which utilizes solar energy to trigger chemical reactions, is one of the most desirable solar-energy-conversion approaches. Graphitic carbon nitride （g-C3N4）. as an attractive metal-free photocatalys...Photocatalysis. which utilizes solar energy to trigger chemical reactions, is one of the most desirable solar-energy-conversion approaches. Graphitic carbon nitride （g-C3N4）. as an attractive metal-free photocatalyst, has drawn worldwide research interest in the area of solar energy conversion due to its easy synthesis, earth-abundant nature, physicochemical stability and visible-light-responsive properties. Over the past ten years, g-C3N4 based photocatalysts have experienced intensive exploration, and great progress has been achieved. However, the solar conversion efficiency is still far from industrial applications due to the wide bandgap, severe charge recombination, and lack of surface active sites. Many strategies have been proposed to enhance the light absorption, reduce the recombination of charge carriers and accelerate the surface kinetics. This work makes a crucial review about the main contributions of various strategies to the light harvesting, charge separation and surface kinetics of g-C3N4 photocatalyst. Furthermore, the evaluation measurements for the enhanced light harvesting, reduced charge recombination and accelerated surface kinetics will be discussed. In addition, this review proposes future trends to enhance the photocatalytic performance of g-C3N4 photocatalyst for the solar energy conversion.展开更多
Modification of nickel sulfide cocatalysts is considered to be a promising approach for efficient enhancement of the photocatalytic hydrogen production performance of g-C3N4.Providing more NiS cocatalyst to function a...Modification of nickel sulfide cocatalysts is considered to be a promising approach for efficient enhancement of the photocatalytic hydrogen production performance of g-C3N4.Providing more NiS cocatalyst to function as active sites of g-C3N4 is still highly desirable.To realize this goal,in this work,a facile sulfur-mediated photodeposition approach was developed.Specifically,photogenerated electrons excited by visible light reduce the S molecules absorbed on g-C3N4 surface to S^2‒,and subsequently NiS cocatalyst is formed in situ on the g-C3N4 surface by a combination of Ni2+and S2‒due to their small solubility product constant(Ksp=3.2×10^‒19).This approach has several advantages.The NiS cocatalyst is clearly in situ deposited on the photogenerated electron transfer sites of g-C3N4,and thus provides more active sites for H2 production.In addition,this method utilizes solar energy with mild reaction conditions at room temperature.Consequently,the synthesized NiS/g-C3N4 photocatalyst achieves excellent hydrogen generation performance with the performance of the optimal sample(244μmol h^‒1 g^‒1)close to that of 1 wt%Pt/g-C3N4(316μmol h^‒1 g^‒1,a well-known excellent photocatalyst).More importantly,the present sulfur-mediated photodeposition route is versatile and facile and can be used to deposit various metal sulfides such as CoSx,CuSx and AgSx on the g-C3N4 surface,and all the resulting metal sulfide-modified g-C3N4 photocatalysts exhibit improved H2-production performance.Our study offers a novel insight for the synthesis of high-efficiency photocatalysts.展开更多
A series of Z-scheme TiO2/g-C3N4/RGO ternary heterojunction photocatalysts are successfully constructed via a direct electrospinning technique coupled with an annealing process for the first time. They are investigate...A series of Z-scheme TiO2/g-C3N4/RGO ternary heterojunction photocatalysts are successfully constructed via a direct electrospinning technique coupled with an annealing process for the first time. They are investigated comprehensively in terms of crystal structure, morphology, composition, specific surface area, photoelectrochemical properties, photodegradation performance, etc. Compared with binary TiO2/g-C3N4 and single-component photocatalysts, ternary heterojunction photocatalysts show the best photodegradation performance for RhB under stimulated sunlight. This can be attributed to the enlarged specific surface area (111.41 m2/g), the formation of Z-scheme heterojunction, and the high separation migration efficiency of photoexcited charge carriers. A potential Z-scheme mechanism for ternary heterojunction photocatalysts is proposed to elucidate the remarkably ameliorated photocatalytic performance based on active species trapping experiments, PL detection test of hydroxyl radicals, and photoelectrochemical properties.展开更多
The photoreduction of CO_(2)to achieve high-value-added hydrocarbons under simulated sunlight irradiation is advantageous,but challenging.In this study,a series of MgO and Au nanoparticle-co-modified g-C_(3)N_(4)photo...The photoreduction of CO_(2)to achieve high-value-added hydrocarbons under simulated sunlight irradiation is advantageous,but challenging.In this study,a series of MgO and Au nanoparticle-co-modified g-C_(3)N_(4)photocatalysts were synthesized and subsequently applied for the photocatalytic reduction of CO_(2)with H2O under simulated solar irradiation.The best photocatalytic performance was demonstrated by the Au and 3%MgO-co-modified g-C_(3)N_(4)photocatalysts with CO,CH_(4),CH3OH,and CH3CHO yields of 423.9,83.2,47.2,and 130.4μmol/g,respectively,in a 3-h reaction.We investigated the effects of MgO and Au as cocatalysts on photocatalytic behaviors,respectively.The characterizations and experimental results showed that the enhanced photocatalytic activity was due to the synergistic effect among the components of the ternary photocatalyst.The cocatalyst MgO can activate CO_(2)(adsorbed at the interface between the MgO and Au particles),and the Mg-N bonds formed in the MgO-CN nanosheets played an important role in the charge transfer.Meanwhile,the Au particles that were modified into MgO/g-C_(3)N_(4)can increase the absorption of visible light via the surface plasmon resonance effect and further reduce the activation energies of the photoreduction of CO_(2)using H2O.This study provided an effective method for the modification of traditional primary photocatalysts with promising performance for photocatalytic CO_(2)reduction.展开更多
The CdS/spherical g-C3N4 n-n heterojunction photocatalyst was fabricated via a solvothermal method.The tetracycline was used to characterize the photocatalytic properties of the as-developed hybrids.The photocatalytic...The CdS/spherical g-C3N4 n-n heterojunction photocatalyst was fabricated via a solvothermal method.The tetracycline was used to characterize the photocatalytic properties of the as-developed hybrids.The photocatalytic degradation mechanism of the as-developed heterojunction photocatalyst was also analyzed.Research results show that CdS nanoparticles are well dispersed in the surface layer of spherical g-C3N4.Moreover,the mass ratio of CdS to spherical g-C3N4 will influence the photocatalytic activity of the asdeveloped composites,which shows the trend of first increasing and then decreasing as it increased.When the mass ratio is 7:1,in 25 min,the as-developed heterojunction shows 93.2%of the maximum photocatalytic efficiency and still exhibits 83.6%after 5 times cycle testing.Moreover,the as-developed hybrids can accelerate the electron transport and improve the separation efficiency of photo-generated carriers compared with pure samples.In addition,the holes and superoxide radicals are dominating active species during the photocatalytic degradation process.展开更多
The novel visible light-induced carbon nitride（g-C3N4） and Bi VO4 composite photocatalysts were obtained through a simple mixing-calcination method. The physical and photophysical properties of the Bi VO4-g-C3N4 com...The novel visible light-induced carbon nitride（g-C3N4） and Bi VO4 composite photocatalysts were obtained through a simple mixing-calcination method. The physical and photophysical properties of the Bi VO4-g-C3N4 composites were investigated by X-ray diffraction（XRD）, Fourier transform infrared（FTIR） spectroscopy, UV-vis diffuse reflection spectroscopy, high-resolution transmission electron microscopy（HRTEM）, photoluminescent（PL） spectroscopy, and BET surface area measurements. Photocatalytic oxidation ability of the prepared samples was examined by studying the degradation of rhodamine B（Rh B） as a target pollutant under visible-light irradiation. The composite photocatalysts exhibited an enhanced photocatalytic performance in degrading Rh B. The optimal g-C3N4 content of the composite photocatalysts was determined for the photodegradation activity. The improved photocatalytic activity of the as-prepared composite photocatalyst may be attributed to the enhancement of photo-generated electron-hole separation at the interface.展开更多
文摘Constructing step-scheme(S-scheme)heterojunctions has been confirmed as a promising strategy for enhancing the photocatalytic activity of composite materials.In this work,a series of sulfur-doped g-C3N4(SCN)/TiO2 S-scheme photocatalysts were synthesized using electrospinning and calcination methods.The as-prepared SCN/TiO2 composites showed superior photocatalytic performance than pure TiO2 and SCN in the photocatalytic degradation of Congo Red(CR)aqueous solution.The significant enhancement in photocatalytic activity benefited not only from the 1D well-distributed nanostructure,but also from the S-scheme heterojunction.Furthermore,the XPS analyses and DFT calculations demonstrated that electrons were transferred from SCN to TiO2 across the interface of the SCN/TiO2 composites.The built-in electric field,band edge bending,and Coulomb interaction synergistically facilitated the recombination of relatively useless electrons and holes in hybrid when the interface was irradiated by simulated solar light.Therefore,the remaining electrons and holes with higher reducibility and oxidizability endowed the composite with supreme redox ability.These results were adequately verified by radical trapping experiments,ESR tests,and in situ XPS analyses,suggesting that the electron immigration in the photocatalyst followed the S-scheme heterojunction mechanism.This work can enrich our knowledge of the design and fabrication of novel S-scheme heterojunction photocatalysts and provide a promising strategy for solving environmental pollution in the future.
文摘Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate photocatalysts.Herein,a novel S-scheme Sb2WO6/g-C3N4 nanocomposite was fabricated by an ultrasound-assisted method,which exhibited excellent performance for photocatalytic ppb-level NO removal.Compared with the pure constituents of the nanocomposite,the as-prepared 15%-Sb2WO6/g-C3N4 photocatalyst could remove more than 68%continuous-flowing NO(initial concentration:400 ppb)under visible-light irradiation in 30 min.The findings of the trapping experiments confirmed that•O2^–and h+were the important active species in the NO oxidation reaction.Meanwhile,the transient photocurrent response and PL spectroscopy analyses proved that the unique S-scheme structure of the samples could enhance the charge separation efficiency.In situ DRIFTS revealed that the photocatalytic reaction pathway of NO removal over the Sb2WO6/g-C3N4 nanocomposite occurred via an oxygen-induced route.The present work proposes a new concept for fabricating efficient photocatalysts for photocatalytic ppb-level NO oxidation and provides deeper insights into the mechanism of photocatalytic NO oxidation.
基金the Australian Research Council for the financial support through its DP and FF programsthe Australian Government for the financial support through the Australian Government Research Training Program ScholarshipThe financial support from National Science Foundation of China(No.513228201)
文摘Photocatalysis. which utilizes solar energy to trigger chemical reactions, is one of the most desirable solar-energy-conversion approaches. Graphitic carbon nitride （g-C3N4）. as an attractive metal-free photocatalyst, has drawn worldwide research interest in the area of solar energy conversion due to its easy synthesis, earth-abundant nature, physicochemical stability and visible-light-responsive properties. Over the past ten years, g-C3N4 based photocatalysts have experienced intensive exploration, and great progress has been achieved. However, the solar conversion efficiency is still far from industrial applications due to the wide bandgap, severe charge recombination, and lack of surface active sites. Many strategies have been proposed to enhance the light absorption, reduce the recombination of charge carriers and accelerate the surface kinetics. This work makes a crucial review about the main contributions of various strategies to the light harvesting, charge separation and surface kinetics of g-C3N4 photocatalyst. Furthermore, the evaluation measurements for the enhanced light harvesting, reduced charge recombination and accelerated surface kinetics will be discussed. In addition, this review proposes future trends to enhance the photocatalytic performance of g-C3N4 photocatalyst for the solar energy conversion.
文摘Modification of nickel sulfide cocatalysts is considered to be a promising approach for efficient enhancement of the photocatalytic hydrogen production performance of g-C3N4.Providing more NiS cocatalyst to function as active sites of g-C3N4 is still highly desirable.To realize this goal,in this work,a facile sulfur-mediated photodeposition approach was developed.Specifically,photogenerated electrons excited by visible light reduce the S molecules absorbed on g-C3N4 surface to S^2‒,and subsequently NiS cocatalyst is formed in situ on the g-C3N4 surface by a combination of Ni2+and S2‒due to their small solubility product constant(Ksp=3.2×10^‒19).This approach has several advantages.The NiS cocatalyst is clearly in situ deposited on the photogenerated electron transfer sites of g-C3N4,and thus provides more active sites for H2 production.In addition,this method utilizes solar energy with mild reaction conditions at room temperature.Consequently,the synthesized NiS/g-C3N4 photocatalyst achieves excellent hydrogen generation performance with the performance of the optimal sample(244μmol h^‒1 g^‒1)close to that of 1 wt%Pt/g-C3N4(316μmol h^‒1 g^‒1,a well-known excellent photocatalyst).More importantly,the present sulfur-mediated photodeposition route is versatile and facile and can be used to deposit various metal sulfides such as CoSx,CuSx and AgSx on the g-C3N4 surface,and all the resulting metal sulfide-modified g-C3N4 photocatalysts exhibit improved H2-production performance.Our study offers a novel insight for the synthesis of high-efficiency photocatalysts.
基金supported by the Scientific Research Project from Hubei Provincial Department of Education(Q20181808)the Research and Innovation Initiatives of Wuhan Polytechnic University(2018J04,2018Y07)~~
文摘A series of Z-scheme TiO2/g-C3N4/RGO ternary heterojunction photocatalysts are successfully constructed via a direct electrospinning technique coupled with an annealing process for the first time. They are investigated comprehensively in terms of crystal structure, morphology, composition, specific surface area, photoelectrochemical properties, photodegradation performance, etc. Compared with binary TiO2/g-C3N4 and single-component photocatalysts, ternary heterojunction photocatalysts show the best photodegradation performance for RhB under stimulated sunlight. This can be attributed to the enlarged specific surface area (111.41 m2/g), the formation of Z-scheme heterojunction, and the high separation migration efficiency of photoexcited charge carriers. A potential Z-scheme mechanism for ternary heterojunction photocatalysts is proposed to elucidate the remarkably ameliorated photocatalytic performance based on active species trapping experiments, PL detection test of hydroxyl radicals, and photoelectrochemical properties.
文摘The photoreduction of CO_(2)to achieve high-value-added hydrocarbons under simulated sunlight irradiation is advantageous,but challenging.In this study,a series of MgO and Au nanoparticle-co-modified g-C_(3)N_(4)photocatalysts were synthesized and subsequently applied for the photocatalytic reduction of CO_(2)with H2O under simulated solar irradiation.The best photocatalytic performance was demonstrated by the Au and 3%MgO-co-modified g-C_(3)N_(4)photocatalysts with CO,CH_(4),CH3OH,and CH3CHO yields of 423.9,83.2,47.2,and 130.4μmol/g,respectively,in a 3-h reaction.We investigated the effects of MgO and Au as cocatalysts on photocatalytic behaviors,respectively.The characterizations and experimental results showed that the enhanced photocatalytic activity was due to the synergistic effect among the components of the ternary photocatalyst.The cocatalyst MgO can activate CO_(2)(adsorbed at the interface between the MgO and Au particles),and the Mg-N bonds formed in the MgO-CN nanosheets played an important role in the charge transfer.Meanwhile,the Au particles that were modified into MgO/g-C_(3)N_(4)can increase the absorption of visible light via the surface plasmon resonance effect and further reduce the activation energies of the photoreduction of CO_(2)using H2O.This study provided an effective method for the modification of traditional primary photocatalysts with promising performance for photocatalytic CO_(2)reduction.
基金Funded by the Natural Science Foundation of Hebei Province,China(Nos.E2019210251 and B2019210331).
文摘The CdS/spherical g-C3N4 n-n heterojunction photocatalyst was fabricated via a solvothermal method.The tetracycline was used to characterize the photocatalytic properties of the as-developed hybrids.The photocatalytic degradation mechanism of the as-developed heterojunction photocatalyst was also analyzed.Research results show that CdS nanoparticles are well dispersed in the surface layer of spherical g-C3N4.Moreover,the mass ratio of CdS to spherical g-C3N4 will influence the photocatalytic activity of the asdeveloped composites,which shows the trend of first increasing and then decreasing as it increased.When the mass ratio is 7:1,in 25 min,the as-developed heterojunction shows 93.2%of the maximum photocatalytic efficiency and still exhibits 83.6%after 5 times cycle testing.Moreover,the as-developed hybrids can accelerate the electron transport and improve the separation efficiency of photo-generated carriers compared with pure samples.In addition,the holes and superoxide radicals are dominating active species during the photocatalytic degradation process.
基金Funded by the National Natural Science Foundation of China(No.51208102)
文摘The novel visible light-induced carbon nitride（g-C3N4） and Bi VO4 composite photocatalysts were obtained through a simple mixing-calcination method. The physical and photophysical properties of the Bi VO4-g-C3N4 composites were investigated by X-ray diffraction（XRD）, Fourier transform infrared（FTIR） spectroscopy, UV-vis diffuse reflection spectroscopy, high-resolution transmission electron microscopy（HRTEM）, photoluminescent（PL） spectroscopy, and BET surface area measurements. Photocatalytic oxidation ability of the prepared samples was examined by studying the degradation of rhodamine B（Rh B） as a target pollutant under visible-light irradiation. The composite photocatalysts exhibited an enhanced photocatalytic performance in degrading Rh B. The optimal g-C3N4 content of the composite photocatalysts was determined for the photodegradation activity. The improved photocatalytic activity of the as-prepared composite photocatalyst may be attributed to the enhancement of photo-generated electron-hole separation at the interface.
