The rapid development of the global economy has led to the over-exploitation and burning of fossil fuels,causing a severe energy crisis and continuous CO_(2) emissions.Although solar energy is a clean and renewable re...The rapid development of the global economy has led to the over-exploitation and burning of fossil fuels,causing a severe energy crisis and continuous CO_(2) emissions.Although solar energy is a clean and renewable resource,it faces significant diurnal and seasonal variations and is difficult to store[1-4].Converting solar energy into storable chemical energy through photocatalysis is an effective way to address both energy scarcity and environmental issues.Photocatalytic CO_(2) reduction,with the development of high-efficiency photocatalysts as the key,offers a clean and environmentally friendly method to convert CO_(2) into valuable hydrocarbon fuels,providing a viable solution to the global energy crisis and climate change[5,6].展开更多
Bismuth selenide(Bi_(2)Se_(3))is an attractive visible-light-responsive semiconductor that can absorb a full range of visible and near-infrared light.However,its poor redox capacity and rapid carrier recombination lim...Bismuth selenide(Bi_(2)Se_(3))is an attractive visible-light-responsive semiconductor that can absorb a full range of visible and near-infrared light.However,its poor redox capacity and rapid carrier recombination limit its application in photocatalytic oxidation.In this study,we adopted Bi_(2)Se_(3)as the couple part of graphitic carbon nitride(g-C_(3)N_(4))to construct a Bi_(2)Se_(3)/g-C_(3)N_(4)composite photocatalyst.Through in situ fabrication,the self-developed Bi2O3/g-C_(3)N_(4)precursor was transformed into a Bi_(2)Se_(3)/g-C_(3)N_(4)heterojunction.The as-prepared Bi_(2)Se_(3)/g-C_(3)N_(4)composite exhibited much higher visible-light-driven photocatalytic activity than pristine Bi_(2)Se_(3)and g-C_(3)N_(4)in the removal of phenol.The enhanced photocatalytic activity was ascribed to the S-scheme configuration of Bi_(2)Se_(3)/g-C_(3)N_(4);this was confirmed by the energy-level shift,photoluminescence analysis,computational structure study,and reactive-radical testing.In the S-scheme heterojunction,photo-excited electrons in the conduction band of g-C_(3)N_(4)migrate to the valence band of Bi_(2)Se_(3)and combine with the excited holes therein.By consuming less reactive carriers,the S-scheme heterojunction can not only effectively promote charge separation,but also preserve more reactive photo-generated carriers.This property enhances the photocatalytic activity.展开更多
Photocatalysis is a sunrise technology with great potential for hydrogen production 1,2,carbon dioxide reduction 3,and so on.However,a single-component photocatalyst often exhibits severely limited activity due to rap...Photocatalysis is a sunrise technology with great potential for hydrogen production 1,2,carbon dioxide reduction 3,and so on.However,a single-component photocatalyst often exhibits severely limited activity due to rapid photogenerated carrier recombination and weak redox abilities.展开更多
In this study,a hierarchical Bi2O3/TiO2 fibrous composite was in-situ fabricated on an electrospun TiO2 nanofiber at ambient temperature.In the Bi2O3/TiO2 composite,S-scheme electron migration occurred between Bi2O3 a...In this study,a hierarchical Bi2O3/TiO2 fibrous composite was in-situ fabricated on an electrospun TiO2 nanofiber at ambient temperature.In the Bi2O3/TiO2 composite,S-scheme electron migration occurred between Bi2O3 and TiO2.In the photocatalytic degradation of phenol under simulated sunlight,the asprepared Bi2O3/TiO2 nanofibers considerably outperformed Bi2O3 nanoparticles and TiO2 nanofibers.This improvement is contributed by maintaining and effectively utilizing the useful carriers and consuming the useless holes and electrons,realized by the S-scheme heterojunction and hierarchical structure.This study also provides an alternative design fashion for photocatalysts.展开更多
Surface heterojunction engineering has been extensively studied to promote efficient charge separation in semiconductor materials.Designing an effective heterojunction system to optimize the separation and transport o...Surface heterojunction engineering has been extensively studied to promote efficient charge separation in semiconductor materials.Designing an effective heterojunction system to optimize the separation and transport of photo-induced charges is an appealing strategy to enhance the photocatalytic efficiency.In this work,In_(2)O_(3)-x(OH)y in situ decorated Bi_(2)MoO_(6) two-dimensional step-scheme heterojunctions were synthesized through a controlled dehydroxylation process of indium-based precursors.The charge transfer mechanism of this step-scheme heterojunctions was confirmed by the characterization of electron structures,reactive species,photoelectric properties and DFT theoretical calculation.The band bending and the internal electric field caused by the charge transfer upon hybridization can effectively promote the separation of charges and present the optimal redox capacity.In addition,surface residual hydroxyl groups can regulate the surface energy state and optimize the interfacial charge transfer kinetics of the prepared step-scheme heterojunction.Eventually,the step-scheme heterojunction exhibits superior performance in photocatalytic reduction of hexavalent chromium and degradation of organic pollutants under visible light irradiation.This work provides an innovative perspective to construct photocatalyst with superior activity.展开更多
Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a clean and cost-efficient alternative to the traditional anthraquinone oxidation approach.Herein,a step-scheme(S-scheme)heterojunction photocat-alyst is f...Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a clean and cost-efficient alternative to the traditional anthraquinone oxidation approach.Herein,a step-scheme(S-scheme)heterojunction photocat-alyst is fabricated by coupling TiO_(2)with three dimensionally ordered macroporous sulfur-doped graphitic carbon nitride(3DOM SCN/T)by electrostatic self-assembly.The optimized photocatalyst achieved a high photocatalytic H_(2)O_(2)production activity with a yield of 2128μmol h^(−1)g^(−1)without the addition of hole scavengers.The remarkable performance was attributed to the synergy between the 3DOM framework and the S-scheme heterojunction.The former enhances light harvesting and provides abundant active sites for surface reactions,while the latter promotes the spatial separation of photogenerated carriers and enhances the redox power.Finally,the mechanism of photocatalytic H_(2)O_(2)production over the 3DOM SCN/T S-scheme composite is proposed.This work provides novel insights into the development of effi-cient photocatalysts for H_(2)O_(2)production from water and O_(2).展开更多
As an industrial benign oxidant and alternative clean energy carrier for fuel cells,hydrogen peroxide(H_(2)O_(2))becomes the fo-cus of numerous studies.Photocatalytic H_(2)O_(2) synthesis becomes a sustainable protoco...As an industrial benign oxidant and alternative clean energy carrier for fuel cells,hydrogen peroxide(H_(2)O_(2))becomes the fo-cus of numerous studies.Photocatalytic H_(2)O_(2) synthesis becomes a sustainable protocol[1,2].However,traditional biphase systems suffer from the agglomeration and recycling difficulty of suspended photocatalysts,as well as sluggish delivery of gas reactants,which induces severe charge recombination and slow reaction kinetics[3].展开更多
The strong metal-support interaction(SMSI)plays a pivotal role in regulating electronic properties and activating surface oxygen species.In this work,we report light-irradiation-modulated SMSI for enhanced formaldehyd...The strong metal-support interaction(SMSI)plays a pivotal role in regulating electronic properties and activating surface oxygen species.In this work,we report light-irradiation-modulated SMSI for enhanced formaldehyde(HCHO)oxidation.Specifically,the SMSI between Pt nanoparticles(NPs)and Bi_(2)MoO_(6)cre-ated surface-active oxygen at Pt-Bi_(2)MoO_(6)interfaces to activate HCHO to dioxymethylene(DOM).Notably,light irradiation boosted the SMSI and catalytic activity.Moreover,photogenerated holes in Bi_(2)MoO 6 im-proved HCHO adsorption and activation,while photogenerated electrons migrated from Bi_(2)MoO_(6)to Pt NPs to promote O_(2)adsorption and activation,accelerating the oxidation of DOM to CO_(2)and H_(2)O.The light-modulated SMSI and the synergy between photocatalysis and thermocatalysis lead to enhanced cat-alytic oxidation activity,providing a practical strategy for indoor volatile organic compound(VOC)de-composition under ambient conditions.展开更多
Research on photocatalytic overall water splitting has attracted wide attention.Recently,a work has sys-tematically discussed the challenges for photocatalytic overall water splitting in terms of thermodynam-ics,kinet...Research on photocatalytic overall water splitting has attracted wide attention.Recently,a work has sys-tematically discussed the challenges for photocatalytic overall water splitting in terms of thermodynam-ics,kinetics,dissolved oxygen,and backward and side reactions.The critical analysis of the reaction pro-cess and reaction environment in the work contributes to an in-depth understanding of photocatalytic overall water splitting.展开更多
Although Bi_(7)O_(9)I_(3) is an oxygen-rich bismuth oxyiodide with higher photocatalytic activity than BiOI,its applicability for photocatalytic oxidation is limited by the rapid recombination of photogenerated carrie...Although Bi_(7)O_(9)I_(3) is an oxygen-rich bismuth oxyiodide with higher photocatalytic activity than BiOI,its applicability for photocatalytic oxidation is limited by the rapid recombination of photogenerated carriers and poor reusability.Depositing Bi_(7)O_(9)I_(3) on flexible macro-sized carbonaceous materials is a promising approach for promoting photogenerated electron migration and improving reusability.In this study,a composite consisting of Bi_(7)O_(9)I_(3) supported on graphitic carbon paper(Bi_(7)O_(9)I_(3)-CP)was synthesized via the in situ transformation of a BiOl-deposited carbon paper precursor(BiOl-CP).The as-prepared Bi_(7)O_(9)I_(3)-CP exhibited higher visible-light-driven photocatalytic activity than both Bi_(7)O_(9)I_(3) and BiOI-CP precursor for phenol removal.The improved photocatalytic activity of Bi_(7)O_(9)I_(3)-CP was attributed to its hierarchical structure and promoted carrier separation,as revealed by photoluminescence,pore structure,and reactive radical analyses.Moreover,owing to its macroscale size and flexibility,the Bi_(7)O_(9)I_(3)-CP composite could be easily operated and reused,which are favorable for practical applications.展开更多
文摘The rapid development of the global economy has led to the over-exploitation and burning of fossil fuels,causing a severe energy crisis and continuous CO_(2) emissions.Although solar energy is a clean and renewable resource,it faces significant diurnal and seasonal variations and is difficult to store[1-4].Converting solar energy into storable chemical energy through photocatalysis is an effective way to address both energy scarcity and environmental issues.Photocatalytic CO_(2) reduction,with the development of high-efficiency photocatalysts as the key,offers a clean and environmentally friendly method to convert CO_(2) into valuable hydrocarbon fuels,providing a viable solution to the global energy crisis and climate change[5,6].
文摘Bismuth selenide(Bi_(2)Se_(3))is an attractive visible-light-responsive semiconductor that can absorb a full range of visible and near-infrared light.However,its poor redox capacity and rapid carrier recombination limit its application in photocatalytic oxidation.In this study,we adopted Bi_(2)Se_(3)as the couple part of graphitic carbon nitride(g-C_(3)N_(4))to construct a Bi_(2)Se_(3)/g-C_(3)N_(4)composite photocatalyst.Through in situ fabrication,the self-developed Bi2O3/g-C_(3)N_(4)precursor was transformed into a Bi_(2)Se_(3)/g-C_(3)N_(4)heterojunction.The as-prepared Bi_(2)Se_(3)/g-C_(3)N_(4)composite exhibited much higher visible-light-driven photocatalytic activity than pristine Bi_(2)Se_(3)and g-C_(3)N_(4)in the removal of phenol.The enhanced photocatalytic activity was ascribed to the S-scheme configuration of Bi_(2)Se_(3)/g-C_(3)N_(4);this was confirmed by the energy-level shift,photoluminescence analysis,computational structure study,and reactive-radical testing.In the S-scheme heterojunction,photo-excited electrons in the conduction band of g-C_(3)N_(4)migrate to the valence band of Bi_(2)Se_(3)and combine with the excited holes therein.By consuming less reactive carriers,the S-scheme heterojunction can not only effectively promote charge separation,but also preserve more reactive photo-generated carriers.This property enhances the photocatalytic activity.
文摘Photocatalysis is a sunrise technology with great potential for hydrogen production 1,2,carbon dioxide reduction 3,and so on.However,a single-component photocatalyst often exhibits severely limited activity due to rapid photogenerated carrier recombination and weak redox abilities.
基金financially supported by the National Natural Science Foundation of China(Nos.51872220 and 21871030)the Natural Science Foundation of Hunan Province of China(Nos.2018JJ2456 and 2018JJ2457)the Scientific Research Fund of Hunan Provincial Education Department of China(No.18A370)。
文摘In this study,a hierarchical Bi2O3/TiO2 fibrous composite was in-situ fabricated on an electrospun TiO2 nanofiber at ambient temperature.In the Bi2O3/TiO2 composite,S-scheme electron migration occurred between Bi2O3 and TiO2.In the photocatalytic degradation of phenol under simulated sunlight,the asprepared Bi2O3/TiO2 nanofibers considerably outperformed Bi2O3 nanoparticles and TiO2 nanofibers.This improvement is contributed by maintaining and effectively utilizing the useful carriers and consuming the useless holes and electrons,realized by the S-scheme heterojunction and hierarchical structure.This study also provides an alternative design fashion for photocatalysts.
基金financially supported by National Natural Science Foundation of China(Nos.51875191 and 51272032)Youth Natural Science Foundation of Hunan Province(No.2019JJ50686)+3 种基金the Science and Technology Project of Changsha City(No.k1705056)Talent Introduction Project of Changsha University(No.SF1605)Open Project of Hunan Key Laboratory of Applied Environmental Photocatalysis(No.ccsu-KF-1501)Hunan Provincial Innovation Foundation For Postgraduate(No.CX2018B163)。
文摘Surface heterojunction engineering has been extensively studied to promote efficient charge separation in semiconductor materials.Designing an effective heterojunction system to optimize the separation and transport of photo-induced charges is an appealing strategy to enhance the photocatalytic efficiency.In this work,In_(2)O_(3)-x(OH)y in situ decorated Bi_(2)MoO_(6) two-dimensional step-scheme heterojunctions were synthesized through a controlled dehydroxylation process of indium-based precursors.The charge transfer mechanism of this step-scheme heterojunctions was confirmed by the characterization of electron structures,reactive species,photoelectric properties and DFT theoretical calculation.The band bending and the internal electric field caused by the charge transfer upon hybridization can effectively promote the separation of charges and present the optimal redox capacity.In addition,surface residual hydroxyl groups can regulate the surface energy state and optimize the interfacial charge transfer kinetics of the prepared step-scheme heterojunction.Eventually,the step-scheme heterojunction exhibits superior performance in photocatalytic reduction of hexavalent chromium and degradation of organic pollutants under visible light irradiation.This work provides an innovative perspective to construct photocatalyst with superior activity.
基金supported by the National Natural Science Foundation of China(Nos.22278324,51932007,22238009,U1905215,52073223,52073034,and 22208332)the Natural Science Foundation of Hubei Province of China(No.2022CFA001)the Innovative Research Funds of SKLWUT(No.2022-CL-A1-01).
文摘Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a clean and cost-efficient alternative to the traditional anthraquinone oxidation approach.Herein,a step-scheme(S-scheme)heterojunction photocat-alyst is fabricated by coupling TiO_(2)with three dimensionally ordered macroporous sulfur-doped graphitic carbon nitride(3DOM SCN/T)by electrostatic self-assembly.The optimized photocatalyst achieved a high photocatalytic H_(2)O_(2)production activity with a yield of 2128μmol h^(−1)g^(−1)without the addition of hole scavengers.The remarkable performance was attributed to the synergy between the 3DOM framework and the S-scheme heterojunction.The former enhances light harvesting and provides abundant active sites for surface reactions,while the latter promotes the spatial separation of photogenerated carriers and enhances the redox power.Finally,the mechanism of photocatalytic H_(2)O_(2)production over the 3DOM SCN/T S-scheme composite is proposed.This work provides novel insights into the development of effi-cient photocatalysts for H_(2)O_(2)production from water and O_(2).
基金This work is financially supported by the National Natural Foun-dation of China(Nos.52174238,21871030,21975084,51672089 and 52073034).
文摘As an industrial benign oxidant and alternative clean energy carrier for fuel cells,hydrogen peroxide(H_(2)O_(2))becomes the fo-cus of numerous studies.Photocatalytic H_(2)O_(2) synthesis becomes a sustainable protocol[1,2].However,traditional biphase systems suffer from the agglomeration and recycling difficulty of suspended photocatalysts,as well as sluggish delivery of gas reactants,which induces severe charge recombination and slow reaction kinetics[3].
基金supported by the National Natural Science Foun-dation of China(Nos.52073223,U1905215,52173065,22208332,22278324,and 52073034)the Project funded by China Post-doctoral Science Foundation(Nos.2021TQ0310,2022TQ0317,and 2022M712959)the Natural Science Foundation of Hubei Province of China(No.2022CFA001).
文摘The strong metal-support interaction(SMSI)plays a pivotal role in regulating electronic properties and activating surface oxygen species.In this work,we report light-irradiation-modulated SMSI for enhanced formaldehyde(HCHO)oxidation.Specifically,the SMSI between Pt nanoparticles(NPs)and Bi_(2)MoO_(6)cre-ated surface-active oxygen at Pt-Bi_(2)MoO_(6)interfaces to activate HCHO to dioxymethylene(DOM).Notably,light irradiation boosted the SMSI and catalytic activity.Moreover,photogenerated holes in Bi_(2)MoO 6 im-proved HCHO adsorption and activation,while photogenerated electrons migrated from Bi_(2)MoO_(6)to Pt NPs to promote O_(2)adsorption and activation,accelerating the oxidation of DOM to CO_(2)and H_(2)O.The light-modulated SMSI and the synergy between photocatalysis and thermocatalysis lead to enhanced cat-alytic oxidation activity,providing a practical strategy for indoor volatile organic compound(VOC)de-composition under ambient conditions.
基金financially supported by the National Natural Foun-dation of China(No.52073034).
文摘Research on photocatalytic overall water splitting has attracted wide attention.Recently,a work has sys-tematically discussed the challenges for photocatalytic overall water splitting in terms of thermodynam-ics,kinetics,dissolved oxygen,and backward and side reactions.The critical analysis of the reaction pro-cess and reaction environment in the work contributes to an in-depth understanding of photocatalytic overall water splitting.
基金National Natural Science Foundation of China(Nos.52073034,21871030)Natural Science Foundation of Hunan Province of China(No.2018JJ2457)Scientific Research Foundation of Hunan Provincial Education Department of China(No.18A370).
文摘Although Bi_(7)O_(9)I_(3) is an oxygen-rich bismuth oxyiodide with higher photocatalytic activity than BiOI,its applicability for photocatalytic oxidation is limited by the rapid recombination of photogenerated carriers and poor reusability.Depositing Bi_(7)O_(9)I_(3) on flexible macro-sized carbonaceous materials is a promising approach for promoting photogenerated electron migration and improving reusability.In this study,a composite consisting of Bi_(7)O_(9)I_(3) supported on graphitic carbon paper(Bi_(7)O_(9)I_(3)-CP)was synthesized via the in situ transformation of a BiOl-deposited carbon paper precursor(BiOl-CP).The as-prepared Bi_(7)O_(9)I_(3)-CP exhibited higher visible-light-driven photocatalytic activity than both Bi_(7)O_(9)I_(3) and BiOI-CP precursor for phenol removal.The improved photocatalytic activity of Bi_(7)O_(9)I_(3)-CP was attributed to its hierarchical structure and promoted carrier separation,as revealed by photoluminescence,pore structure,and reactive radical analyses.Moreover,owing to its macroscale size and flexibility,the Bi_(7)O_(9)I_(3)-CP composite could be easily operated and reused,which are favorable for practical applications.
