A novel core–shell TiO2@ZnIn2S4composite has been synthesized successfully by a simple and flexible hydrothermal route using TiO2as precursors.The as-synthesized samples were characterized by X-ray diffraction,UV–vi...A novel core–shell TiO2@ZnIn2S4composite has been synthesized successfully by a simple and flexible hydrothermal route using TiO2as precursors.The as-synthesized samples were characterized by X-ray diffraction,UV–vis diffuse reflectance spectra and transmission electron microscopy.The photocatalytic properties of samples were tested by degradation of aqueous methylene blue（MB）under visible light irradiation.It was found that the as-synthesized TiO2@ZnIn2S4photocatalyst was more effcient than TiO2and ZnIn2S4in the photocatalytic degradation of MB.Moreover,TEM images confrmed the TiO2@ZnIn2S4nanoparticles possessed a well-proportioned core–shell morphology.展开更多
Perfluoroalkyl substances(PFASs)are typical persistent organic pollutants,and their removal is urgently required but challenging.Photocatalysis has shown potential in PFASs degradation due to the redox capabilities of...Perfluoroalkyl substances(PFASs)are typical persistent organic pollutants,and their removal is urgently required but challenging.Photocatalysis has shown potential in PFASs degradation due to the redox capabilities of photoinduced charge carriers in photocatalysts.Herein,hexagonal ZnIn_(2)S_(4)(ZIS)nanosheets were synthesized by a one-pot oil bath method and were well characterized by a series of techniques.In the degradation of sodium p-perfluorous nonenoxybenzenesulfonate(OBS),one kind of representative PFASs,the assynthesized ZIS showed activity superior to P25 TiO_(2) under both simulated sunlight and visible-light irradiation.The good photocatalytic performance was attributed to the enhanced light absorption and facilitated charge separation.The pH conditions were found crucial in the photocatalytic process by influencing the OBS adsorption on the ZIS surface.Photogenerated e−and h+were the main active species involved in OBS degradation in the ZIS system.This work confirmed the feasibility and could provide mechanistic insights into the degradation and defluorination of PFASs by visible-light photocatalysis.展开更多
Rapid carrier recombination and slow charge transfer dynamics have significantly reduced the performance of photocatalytic hydrogen production.Construction of heterojunctions via utilizing the sulfur-edge and metal-ed...Rapid carrier recombination and slow charge transfer dynamics have significantly reduced the performance of photocatalytic hydrogen production.Construction of heterojunctions via utilizing the sulfur-edge and metal-edge sites of metal sulfide semiconductor for improving photocatalytic activity remains a significant challenge.Herein,a novel ZnIn_(2)S_(4)/MnS S-scheme heterojunction was prepared by hydrothermal synthesis to accelerate charge carrier transfer for efficient photocatalysis.Notably,ZnIn_(2)S_(4)/MnS exhibited excellent photocatalytic hydrogen evolution activity(7.95 mmol g^(-1)h^(-1))under visible light irradiation(≥420 nm),up to 4.7 times higher than that of pure ZnIn_(2)S_(4).Additionally,cycling experiments showed that ZM-2 remained high stability after four cycles.Density-functional theory(DFT)calculations and in situ XPS results confirm the formation of S-scheme heterojunction,indicating that the tight interfacial contact between ZnIn_(2)S_(4)and Mn S with the presence of Mn-S bonds(the unsaturated Mn edges of MnS and the uncoordinated S atoms in the edge of ZnIn_(2)S_(4))promoted faster charge transfer.Besides,the unsaturated S atom on the surface of Mn S is an active site with strong H+binding ability,which can effectively reduce the overpotential or activation barrier for hydrogen evolution.This study illustrates the critical influence of the interfacial Mn-S bond on the ZnIn_(2)S_(4)/MnS S-scheme heterojunction to achieve efficient photocatalytic hydrogen production and provides relevant guidance for carrying out rational structural/interfacial modulation.展开更多
ZnIn_(2)S_(4), a typical n-type semiconductor, has received intensive attention due to its suitable bandgap, excellent visible light absorption performance, and simple and fiexible preparation methods. However, its ap...ZnIn_(2)S_(4), a typical n-type semiconductor, has received intensive attention due to its suitable bandgap, excellent visible light absorption performance, and simple and fiexible preparation methods. However, its application is curbed by photo-generated carrier recombination and photo corrosion. Although constructing S-scheme heterojunctions by combining ZnIn_(2)S_(4)with other semiconductors can solve these problems, the photocatalytic activity of S-scheme heterojunctions can be further improved. Therefore, this short review summarizes modification strategies of ZnIn_(2)S_(4)-based S-scheme heterojunctions. This article also introduces the concept, design principles, and characterization methods of ZnIn_(2)S_(4)-based S-scheme heterojunction. Finally, current challenges and future research focuses related to ZnIn_(2)S_(4)-based S-scheme heterojunctions are discussed and summarized, including the utilization of advanced in-situ characterization techniques to further illuminate the photocatalytic mechanism, the DFT-assisted design of catalysts to increase the selectivity of products during photocatalytic CO_(2) reduction, and extending the photoresponse of ZnIn_(2)S_(4)-based S-scheme heterojunction to near-infrared range, etc.展开更多
Efficient photocatalytic water splitting can be significantly enhanced through the careful design of S-scheme heterostructures,which play a pivotal role in optimizing performance.Herein,we report the construction of Z...Efficient photocatalytic water splitting can be significantly enhanced through the careful design of S-scheme heterostructures,which play a pivotal role in optimizing performance.Herein,we report the construction of ZnIn_(2)S_(4)/CdS S-scheme heterojunctions under ambient conditions,based on a sonochemical strategy.This structure is facilitated by the well-matched interface between the(007)plane of layered ZnIn_(2)S_(4)and the(101)plane of CdS,leading to a threshold optical response of 2.12 eV,which optimally aligns with visible light absorption.As a proof of concept,the resulting ZnIn_(2)S_(4)/CdS catalysts demonstrate a remarkable improvement in photocatalytic H_(2) evolution,achieving a rate of 5678.2μmol h^(-1)g^(-1)under visible light irradiation(λ>400 nm).This rate is approximately 10 times higher than that of pristine ZnIn_(2)S_(4)nanosheets(NSs)and about 4.6 times higher than that of CdS nanoparticles(NPs),surpassing the performance of most ZnIn_(2)S_(4)-based photocatalysts reported to date.Moreover,they deliver a robust photocatalytic performance during long-term operation of up to 60 h,showing their potential for use in practical applications.Based on the theoretical calculation and experimental results,it is verified that the movements of electrons and holes in the opposite direction could be induced by the disparity in the work function and the internal electric field within the interfaces,thus facilitating the construction of S-scheme heterojunctions,which fundamentally suppresses carrier recombination while minimizing photocorrosion of ZnIn_(2)S_(4)toward enhanced photocatalytic behaviors.展开更多
Herein we report novel photocatalysts ZnIn_(2)S_(4)-Ag-LaFeO_(3) with the core-shell structured materials prepared by hydrothermal method.In order to improve the efficiency of photocatalytic degradation of pollutants,...Herein we report novel photocatalysts ZnIn_(2)S_(4)-Ag-LaFeO_(3) with the core-shell structured materials prepared by hydrothermal method.In order to improve the efficiency of photocatalytic degradation of pollutants,LaFeO_(3) was prepared by hydrothermal followed by calcination,and further Ag nanoparticle(NP)was loaded onto the spherical structure of LaFeO_(3) by photolysis of silver nitrate,and finally the spherical Znln_(2)S_(4)-Ag-LaFeO_(3) photocatalyst was prepared by hydrothermal method again.The structure and properties of the as-prepared materials were characterized by X-ray photoelectron spectroscopy,ultraviolet-visible absorption spectroscopy,X-ray diffraction,scanning electron microscopy and fluorescence spectra.The results show that the synthesized composite photocatalysts display a significant improvement in photocatalytic efficiency relative to the single LaFeO_(3) and ZnIn_(2)S_(4)and form a core-shell structure.Furthermore,the effect of the ratio of each component on the photocatalytic efficiency was investigated in detail,and it is discovered that at an Methylene Blue(MB)concentration of 0.219 mol/L,the degradation rate of MB is 95%at 120 min using 0.02 g of catalyst with an ideal ZnIn_(2)S_(4):Ag:LaFeO_(3)ratio of 10:0.5:1.The possible mechanisms to improve the photocatalytic efficiency were explored.展开更多
Developing efficient and stable photocatalysts for hydrogen generation still remains a huge challenge.Herein,we adopted Cynanchum fibers as a carbon source and substrate to construct a ternary hollow core-shell carbon...Developing efficient and stable photocatalysts for hydrogen generation still remains a huge challenge.Herein,we adopted Cynanchum fibers as a carbon source and substrate to construct a ternary hollow core-shell carbon microtubes@TiO_(2)/ZnIn_(2)S_(4)(denoted as CMT@TiO_(2)/ZnIn_(2)S_(4))for photothermal-assisted photocatalytic hydrogen evolution(PHE).For the catalyst system,ZnIn_(2)S_(4)is the main visible light absorber,TiO_(2) is introduced to form a heterojunction with ZnIn_(2)S_(4)to facilitate the separation of photogenerated carriers,and hollow CMT derived from Cynanchum fibers serves as a conductive scaffold and a photothermal core to elevate the surface temperature of the localized reaction system.Benefiting from the rationally designed multicomponents and microstructures,the photocatalyst proposed enhanced PHE activity of 9.71 mmol·g^(−1)·h^(−1),which was 30.3,2.7 and 1.5 times higher than those of binary CMT@TiO_(2),pristine ZnIn_(2)S_(4)and TiO_(2)/ZnIn_(2)S_(4)composite,respectively.The outperformed PHE activity of CMT@TiO_(2)/ZnIn_(2)S_(4)could be ascribed to the synergy of the formation of intimate heterointerface,the CMT-induced photothermal effect and the hierarchical core-shell architecture.This work provides a promising approach for constructing efficient and durable photocatalysts for H_(2) evolution.展开更多
The zinc indium sulfide(ZnIn_(2)S_(4))semiconductors have garnered significant interest in photocatalysis due to their environmentally friendly characteristics,appropriate bandgap,and high absorption coefficient.Howev...The zinc indium sulfide(ZnIn_(2)S_(4))semiconductors have garnered significant interest in photocatalysis due to their environmentally friendly characteristics,appropriate bandgap,and high absorption coefficient.However,the exploration of advanced strategies to realize the effective and tailored doping still poses significant challenges in enhancing hydrogen evolution performance.In this work,a mild cation exchange strategy is reported to incorporate Ag cations into flower-like ZnIn_(2)S_(4) microspheres,enabling the selective replacement of Zn atoms by Ag.Remarkably,the as-fabricated Ag-ZnIn_(2)S_(4) exhibited exceptional photocatalytic hydrogen production performance,achieving a rate of 8098μmol·g^(−1)·h^(−1) under visible light irradiation.This is 4 times than that of pristine ZnIn_(2)S_(4)(2002μmol·g^(−1)·h^(−1)),and stands as the highest one among metal-doped-ZnIn_(2)S_(4) photocatalysts ever reported.Along with the theoretical calculations,it has been confirmed that the enhanced photocatalytic hydrogen generation behavior can primarily be attributed to the synergistic effect with improved light absorption,reduced adsorption energy,increased active sites and optimized charge carrier transfer,induced by the cation exchange with Ag in ZnIn_(2)S_(4).This work might provide some valuable insights on the design and development of highly efficient visible light driven photocatalysts for water splitting applications.展开更多
Sodium-ion batteries with ZnIn_(2)S_(4)(ZIS)anodes promise a high capacity and abundant resources.However,their inherent low conductivity,large volume expansion and sluggish Na+diffusion limit the development of the w...Sodium-ion batteries with ZnIn_(2)S_(4)(ZIS)anodes promise a high capacity and abundant resources.However,their inherent low conductivity,large volume expansion and sluggish Na+diffusion limit the development of the wide-temperature sodium storage.This study pioneers a scalable synthesis of hierarchical hollow structural ZIS/C heterostructure through in situ confined growth of ZIS nanosheets in porous hollow carbon spheres(PHCSs)via a hydrothermal method.This unique structure exhibits abundant heterostructures to facilitate charge transport,rich porous structures to promote electrolyte wettability,efficient space utilization to relieve volume expansion,as well as interconnected carbon networks to ensure framework stability.Consequently,ZIS/C exhibits exceptional cycling stability with 92%capacity retention after 1000 cycles.Notably,ZIS/C demonstrates good wide-temperature performance operating at–50∼90°C,especially,at–30°C with a capacity of 208 mA h g^(−1)at 0.3A g^(−1).The full cell of ZIS/C||Na_(3)V_(2)(PO_(4))_(3)exhibits excellent high-rate capability(178 mA h g^(−1)at 6A g^(−1)).展开更多
The synergistic effects of piezoelectric catalysis and plasmonic photocatalysis hold significant promise for achieving high-efficiency solar energy conversion.Herein,SnFe_(2)O_(4)@ZnIn_(2)S_(4)(SFO@ZIS)composites were...The synergistic effects of piezoelectric catalysis and plasmonic photocatalysis hold significant promise for achieving high-efficiency solar energy conversion.Herein,SnFe_(2)O_(4)@ZnIn_(2)S_(4)(SFO@ZIS)composites were prepared by a facile low-temperature water bath method,and an efficient and stable near-infrared(NIR)photothermal-assisted piezoelectric photocatalytic system was successfully constructed.The system achieved a synergistic effect of ultrasonic vibration and NIR illumination,driving a photocatalytic hydrogen(H_(2))production rate of 17.9μmol g^(-1)h^(-1).Related photothermal test results demonstrate that the localized surface plasmon(LSPR)resonance effect of SFO not only significantly broadens the NIR light absorption of ZIS,but also improves the reaction temperature and reduces the activation energy of the reaction by efficiently converting the light energy into heat energy.In addition,photoelectrochemical analyses revealed that the SFO with excellent piezoelectric activity effectively facilitated carrier separation by transferring the energetic hot electrons generated by the LSPR effect to the conduction band of ZIS under external mechanical pressure.This study presents an effective design strategy and theoretical basis for constructing an efficient and robust NIR-driven photothermally assisted piezoelectric photo-catalytic system.展开更多
The modulation of charge transfer pathways within type-I heterojunctions through interfacial electric field(IEF)engineering is of critical importance in promoting photocatalytic hydrogen evolution,effectively facilita...The modulation of charge transfer pathways within type-I heterojunctions through interfacial electric field(IEF)engineering is of critical importance in promoting photocatalytic hydrogen evolution,effectively facilitating the separation of photogenerated charge carriers.In this study,we performed in-situ growth of two-dimensional ZnIn_(2)S_(4)nanosheets on MnCo_(2)O_(4.5)nanorods to construct an ohmic-like type-I ZnIn_(2)S_(4)/MnCo_(2)O_(4.5)heterojunction for efficient photocatalytic hydrogen evolution.This ohmic-like charge transfer mechanism effectively addresses the intrinsic limitations inherent to conventional type-I heterojunctions neglecting IEF effects,particularly through IEF-induced enhancement of charge separation efficiency.Consequently,the optimized ZnIn_(2)S_(4)/MnCo_(2)O_(4.5)photocatalyst demonstrates an outstanding photocatalytic hydrogen evolution rate of 20.9 mmol g^(−1)h^(−1),14.9 times that of the bare ZnIn_(2)S_(4).Furthermore,the ohmic-like charge transport behavior has been rigorously validated by integrated advanced experimental characterizations,including in-situ X-ray photoelectron spectroscopy(XPS),Kelvin probe force microscopy(KPFM),and surface photovoltage(SPV)measurements,which collectively provide robust evidence for the proposed mechanism.This work offers valuable insights into the design of high-efficient ohmic-like type-I heterojunction catalysts for photocatalytic H_(2)evolution.展开更多
基金the financial support of National Natural Science Foundation of China (No. 20976057)Joint Funds of NSFC-Guangdong (No. U0834004)Guangdong Provincial Natural Science Funding (No. 06025657)
文摘A novel core–shell TiO2@ZnIn2S4composite has been synthesized successfully by a simple and flexible hydrothermal route using TiO2as precursors.The as-synthesized samples were characterized by X-ray diffraction,UV–vis diffuse reflectance spectra and transmission electron microscopy.The photocatalytic properties of samples were tested by degradation of aqueous methylene blue（MB）under visible light irradiation.It was found that the as-synthesized TiO2@ZnIn2S4photocatalyst was more effcient than TiO2and ZnIn2S4in the photocatalytic degradation of MB.Moreover,TEM images confrmed the TiO2@ZnIn2S4nanoparticles possessed a well-proportioned core–shell morphology.
基金supported by the National Natural Science Foundation of China (Nos.22206113 and 22376124)the Outstanding Youth Science Fund (Overseas)of Shandong Provincial Natural Science Foundation (No.2022HWYQ-015)+2 种基金the Taishan Scholars Project Special Fund (No.tsqn202211039)the Guangdong Basic and Applied Basic Research Foundation (No.2021A1515111137)Qilu Youth Talent Program of Shandong University (No.61440082163171).
文摘Perfluoroalkyl substances(PFASs)are typical persistent organic pollutants,and their removal is urgently required but challenging.Photocatalysis has shown potential in PFASs degradation due to the redox capabilities of photoinduced charge carriers in photocatalysts.Herein,hexagonal ZnIn_(2)S_(4)(ZIS)nanosheets were synthesized by a one-pot oil bath method and were well characterized by a series of techniques.In the degradation of sodium p-perfluorous nonenoxybenzenesulfonate(OBS),one kind of representative PFASs,the assynthesized ZIS showed activity superior to P25 TiO_(2) under both simulated sunlight and visible-light irradiation.The good photocatalytic performance was attributed to the enhanced light absorption and facilitated charge separation.The pH conditions were found crucial in the photocatalytic process by influencing the OBS adsorption on the ZIS surface.Photogenerated e−and h+were the main active species involved in OBS degradation in the ZIS system.This work confirmed the feasibility and could provide mechanistic insights into the degradation and defluorination of PFASs by visible-light photocatalysis.
基金the National Nature Science Foundation of China(No.22108069)Natural Science Foundation of Hunan Province,China(No.2021JJ40260)for the financial support。
文摘Rapid carrier recombination and slow charge transfer dynamics have significantly reduced the performance of photocatalytic hydrogen production.Construction of heterojunctions via utilizing the sulfur-edge and metal-edge sites of metal sulfide semiconductor for improving photocatalytic activity remains a significant challenge.Herein,a novel ZnIn_(2)S_(4)/MnS S-scheme heterojunction was prepared by hydrothermal synthesis to accelerate charge carrier transfer for efficient photocatalysis.Notably,ZnIn_(2)S_(4)/MnS exhibited excellent photocatalytic hydrogen evolution activity(7.95 mmol g^(-1)h^(-1))under visible light irradiation(≥420 nm),up to 4.7 times higher than that of pure ZnIn_(2)S_(4).Additionally,cycling experiments showed that ZM-2 remained high stability after four cycles.Density-functional theory(DFT)calculations and in situ XPS results confirm the formation of S-scheme heterojunction,indicating that the tight interfacial contact between ZnIn_(2)S_(4)and Mn S with the presence of Mn-S bonds(the unsaturated Mn edges of MnS and the uncoordinated S atoms in the edge of ZnIn_(2)S_(4))promoted faster charge transfer.Besides,the unsaturated S atom on the surface of Mn S is an active site with strong H+binding ability,which can effectively reduce the overpotential or activation barrier for hydrogen evolution.This study illustrates the critical influence of the interfacial Mn-S bond on the ZnIn_(2)S_(4)/MnS S-scheme heterojunction to achieve efficient photocatalytic hydrogen production and provides relevant guidance for carrying out rational structural/interfacial modulation.
基金the Strategic Priority Research Program of the Chinese Academy of Sciences, China (Nos. XDA23010300 and XDA23010000)the National Natural Science Foundation of China (Nos. 51878644 and 41573138)。
文摘ZnIn_(2)S_(4), a typical n-type semiconductor, has received intensive attention due to its suitable bandgap, excellent visible light absorption performance, and simple and fiexible preparation methods. However, its application is curbed by photo-generated carrier recombination and photo corrosion. Although constructing S-scheme heterojunctions by combining ZnIn_(2)S_(4)with other semiconductors can solve these problems, the photocatalytic activity of S-scheme heterojunctions can be further improved. Therefore, this short review summarizes modification strategies of ZnIn_(2)S_(4)-based S-scheme heterojunctions. This article also introduces the concept, design principles, and characterization methods of ZnIn_(2)S_(4)-based S-scheme heterojunction. Finally, current challenges and future research focuses related to ZnIn_(2)S_(4)-based S-scheme heterojunctions are discussed and summarized, including the utilization of advanced in-situ characterization techniques to further illuminate the photocatalytic mechanism, the DFT-assisted design of catalysts to increase the selectivity of products during photocatalytic CO_(2) reduction, and extending the photoresponse of ZnIn_(2)S_(4)-based S-scheme heterojunction to near-infrared range, etc.
基金supported by the National Natural Science Foundation of China(NSFC,Grant No.52372063,62204246 and 52401244)the Young Elite Scientists Sponsorship Program by CAST(Grant No.2023QNRC001)+1 种基金the Postdoctoral Fellowship Program of CPSF(Grant No.GZC20233001,GZC20233006)the China Postdoctoral Science Foundation(Grant No.2024M753526)。
文摘Efficient photocatalytic water splitting can be significantly enhanced through the careful design of S-scheme heterostructures,which play a pivotal role in optimizing performance.Herein,we report the construction of ZnIn_(2)S_(4)/CdS S-scheme heterojunctions under ambient conditions,based on a sonochemical strategy.This structure is facilitated by the well-matched interface between the(007)plane of layered ZnIn_(2)S_(4)and the(101)plane of CdS,leading to a threshold optical response of 2.12 eV,which optimally aligns with visible light absorption.As a proof of concept,the resulting ZnIn_(2)S_(4)/CdS catalysts demonstrate a remarkable improvement in photocatalytic H_(2) evolution,achieving a rate of 5678.2μmol h^(-1)g^(-1)under visible light irradiation(λ>400 nm).This rate is approximately 10 times higher than that of pristine ZnIn_(2)S_(4)nanosheets(NSs)and about 4.6 times higher than that of CdS nanoparticles(NPs),surpassing the performance of most ZnIn_(2)S_(4)-based photocatalysts reported to date.Moreover,they deliver a robust photocatalytic performance during long-term operation of up to 60 h,showing their potential for use in practical applications.Based on the theoretical calculation and experimental results,it is verified that the movements of electrons and holes in the opposite direction could be induced by the disparity in the work function and the internal electric field within the interfaces,thus facilitating the construction of S-scheme heterojunctions,which fundamentally suppresses carrier recombination while minimizing photocorrosion of ZnIn_(2)S_(4)toward enhanced photocatalytic behaviors.
基金Project supported by the National Natural Science Foundation of China(21101107,51173107)State Key Laboratory of Pollution Control and Resource Reuse Foundation(PCRRF19017)。
文摘Herein we report novel photocatalysts ZnIn_(2)S_(4)-Ag-LaFeO_(3) with the core-shell structured materials prepared by hydrothermal method.In order to improve the efficiency of photocatalytic degradation of pollutants,LaFeO_(3) was prepared by hydrothermal followed by calcination,and further Ag nanoparticle(NP)was loaded onto the spherical structure of LaFeO_(3) by photolysis of silver nitrate,and finally the spherical Znln_(2)S_(4)-Ag-LaFeO_(3) photocatalyst was prepared by hydrothermal method again.The structure and properties of the as-prepared materials were characterized by X-ray photoelectron spectroscopy,ultraviolet-visible absorption spectroscopy,X-ray diffraction,scanning electron microscopy and fluorescence spectra.The results show that the synthesized composite photocatalysts display a significant improvement in photocatalytic efficiency relative to the single LaFeO_(3) and ZnIn_(2)S_(4)and form a core-shell structure.Furthermore,the effect of the ratio of each component on the photocatalytic efficiency was investigated in detail,and it is discovered that at an Methylene Blue(MB)concentration of 0.219 mol/L,the degradation rate of MB is 95%at 120 min using 0.02 g of catalyst with an ideal ZnIn_(2)S_(4):Ag:LaFeO_(3)ratio of 10:0.5:1.The possible mechanisms to improve the photocatalytic efficiency were explored.
基金supported by the National Natural Science Foundation of China(No.21701078)the PhD Initiation Foundation of Liaocheng University(No.318052140).
文摘Developing efficient and stable photocatalysts for hydrogen generation still remains a huge challenge.Herein,we adopted Cynanchum fibers as a carbon source and substrate to construct a ternary hollow core-shell carbon microtubes@TiO_(2)/ZnIn_(2)S_(4)(denoted as CMT@TiO_(2)/ZnIn_(2)S_(4))for photothermal-assisted photocatalytic hydrogen evolution(PHE).For the catalyst system,ZnIn_(2)S_(4)is the main visible light absorber,TiO_(2) is introduced to form a heterojunction with ZnIn_(2)S_(4)to facilitate the separation of photogenerated carriers,and hollow CMT derived from Cynanchum fibers serves as a conductive scaffold and a photothermal core to elevate the surface temperature of the localized reaction system.Benefiting from the rationally designed multicomponents and microstructures,the photocatalyst proposed enhanced PHE activity of 9.71 mmol·g^(−1)·h^(−1),which was 30.3,2.7 and 1.5 times higher than those of binary CMT@TiO_(2),pristine ZnIn_(2)S_(4)and TiO_(2)/ZnIn_(2)S_(4)composite,respectively.The outperformed PHE activity of CMT@TiO_(2)/ZnIn_(2)S_(4)could be ascribed to the synergy of the formation of intimate heterointerface,the CMT-induced photothermal effect and the hierarchical core-shell architecture.This work provides a promising approach for constructing efficient and durable photocatalysts for H_(2) evolution.
基金supported by the National Natural Science Foundation of China(Nos.52272085 and 52372063)Zhejiang Provincial Natural Science Foundation of China(No.LY23E020002)+1 种基金Ningbo Youth Science and Technology Innovation Leading Talents Project(No.2023QL031)the Postdoctoral Fellowship Program of CPSF(No.GZC20233006).
文摘The zinc indium sulfide(ZnIn_(2)S_(4))semiconductors have garnered significant interest in photocatalysis due to their environmentally friendly characteristics,appropriate bandgap,and high absorption coefficient.However,the exploration of advanced strategies to realize the effective and tailored doping still poses significant challenges in enhancing hydrogen evolution performance.In this work,a mild cation exchange strategy is reported to incorporate Ag cations into flower-like ZnIn_(2)S_(4) microspheres,enabling the selective replacement of Zn atoms by Ag.Remarkably,the as-fabricated Ag-ZnIn_(2)S_(4) exhibited exceptional photocatalytic hydrogen production performance,achieving a rate of 8098μmol·g^(−1)·h^(−1) under visible light irradiation.This is 4 times than that of pristine ZnIn_(2)S_(4)(2002μmol·g^(−1)·h^(−1)),and stands as the highest one among metal-doped-ZnIn_(2)S_(4) photocatalysts ever reported.Along with the theoretical calculations,it has been confirmed that the enhanced photocatalytic hydrogen generation behavior can primarily be attributed to the synergistic effect with improved light absorption,reduced adsorption energy,increased active sites and optimized charge carrier transfer,induced by the cation exchange with Ag in ZnIn_(2)S_(4).This work might provide some valuable insights on the design and development of highly efficient visible light driven photocatalysts for water splitting applications.
基金supported by the National Natural Science Foundation of China(U23B2075)the Natural Science Foundation of Shandong Province(ZR202111290333)the China Postdoctoral Science Foundation(2023M730640,2024M750490).
文摘Sodium-ion batteries with ZnIn_(2)S_(4)(ZIS)anodes promise a high capacity and abundant resources.However,their inherent low conductivity,large volume expansion and sluggish Na+diffusion limit the development of the wide-temperature sodium storage.This study pioneers a scalable synthesis of hierarchical hollow structural ZIS/C heterostructure through in situ confined growth of ZIS nanosheets in porous hollow carbon spheres(PHCSs)via a hydrothermal method.This unique structure exhibits abundant heterostructures to facilitate charge transport,rich porous structures to promote electrolyte wettability,efficient space utilization to relieve volume expansion,as well as interconnected carbon networks to ensure framework stability.Consequently,ZIS/C exhibits exceptional cycling stability with 92%capacity retention after 1000 cycles.Notably,ZIS/C demonstrates good wide-temperature performance operating at–50∼90°C,especially,at–30°C with a capacity of 208 mA h g^(−1)at 0.3A g^(−1).The full cell of ZIS/C||Na_(3)V_(2)(PO_(4))_(3)exhibits excellent high-rate capability(178 mA h g^(−1)at 6A g^(−1)).
基金financially supported by the National Natural Science Foundation of China(Nos.21906039 and 22006057)China Postdoctoral Science Foundation(No.2023M743178)+6 种基金Jiangsu Province Industry-University-Research Cooperation Project(No.BY20231482)the Open Fund of the Key Laboratory of Solar Cell electrode Materials in China Petroleum and Chemical Industry(No.2024A093)Key Laboratory of Functional Inorganic Material Chemistry(Heilongjiang University)Ministry of EducationExcellent Youth Fund of Basic Research Project of Universities in Shijiazhuang(No.241790627 A)Outstanding Youth Project of Hebei GEO University in 2024(No.JQ202403)PhD Research Startup Foundation of Hebei GEO University in 2024(No.BQ2024026)the National Pre-research Funds of Hebei GEO University in 2024(No.KY2024YB03)。
文摘The synergistic effects of piezoelectric catalysis and plasmonic photocatalysis hold significant promise for achieving high-efficiency solar energy conversion.Herein,SnFe_(2)O_(4)@ZnIn_(2)S_(4)(SFO@ZIS)composites were prepared by a facile low-temperature water bath method,and an efficient and stable near-infrared(NIR)photothermal-assisted piezoelectric photocatalytic system was successfully constructed.The system achieved a synergistic effect of ultrasonic vibration and NIR illumination,driving a photocatalytic hydrogen(H_(2))production rate of 17.9μmol g^(-1)h^(-1).Related photothermal test results demonstrate that the localized surface plasmon(LSPR)resonance effect of SFO not only significantly broadens the NIR light absorption of ZIS,but also improves the reaction temperature and reduces the activation energy of the reaction by efficiently converting the light energy into heat energy.In addition,photoelectrochemical analyses revealed that the SFO with excellent piezoelectric activity effectively facilitated carrier separation by transferring the energetic hot electrons generated by the LSPR effect to the conduction band of ZIS under external mechanical pressure.This study presents an effective design strategy and theoretical basis for constructing an efficient and robust NIR-driven photothermally assisted piezoelectric photo-catalytic system.
基金financial support from the“Lingyan”R&D Plan Project of Zhejiang Province(2025C02218)。
文摘The modulation of charge transfer pathways within type-I heterojunctions through interfacial electric field(IEF)engineering is of critical importance in promoting photocatalytic hydrogen evolution,effectively facilitating the separation of photogenerated charge carriers.In this study,we performed in-situ growth of two-dimensional ZnIn_(2)S_(4)nanosheets on MnCo_(2)O_(4.5)nanorods to construct an ohmic-like type-I ZnIn_(2)S_(4)/MnCo_(2)O_(4.5)heterojunction for efficient photocatalytic hydrogen evolution.This ohmic-like charge transfer mechanism effectively addresses the intrinsic limitations inherent to conventional type-I heterojunctions neglecting IEF effects,particularly through IEF-induced enhancement of charge separation efficiency.Consequently,the optimized ZnIn_(2)S_(4)/MnCo_(2)O_(4.5)photocatalyst demonstrates an outstanding photocatalytic hydrogen evolution rate of 20.9 mmol g^(−1)h^(−1),14.9 times that of the bare ZnIn_(2)S_(4).Furthermore,the ohmic-like charge transport behavior has been rigorously validated by integrated advanced experimental characterizations,including in-situ X-ray photoelectron spectroscopy(XPS),Kelvin probe force microscopy(KPFM),and surface photovoltage(SPV)measurements,which collectively provide robust evidence for the proposed mechanism.This work offers valuable insights into the design of high-efficient ohmic-like type-I heterojunction catalysts for photocatalytic H_(2)evolution.
