The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(...The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.展开更多
The photocatalytic activity of catalysts depends on the energy-harvesting ability and the separation or transport of photogenerated carriers.The light absorption capacity of graphitic carbon nitride(g-C_(3)N_(4))-base...The photocatalytic activity of catalysts depends on the energy-harvesting ability and the separation or transport of photogenerated carriers.The light absorption capacity of graphitic carbon nitride(g-C_(3)N_(4))-based composites can be enhanced by adjusting the surface plasmon resonance(SPR)of noble metal nanoparticles(e.g.,Cu,Au,and Pd)in the entire visible region.Adjustments can be carried out by varying the nanocomponents of the materials.The SPR of noble metals can enhance the local electromagnetic field and improve interband transition,and resonant energy transfer occurs from plasmonic dipoles to electron-hole pairs via near-field electromagnetic interactions.Thus,noble metals have emerged as relevant nanocomponents for g-C_(3)N_(4) used in CO_(2) photoreduction and water splitting.Herein,recent key advances in noble metals(either in single atom,cluster,or nanoparticle forms)and composite photocatalysts based on inorganic or organic nanocomponent-incorporated g-C_(3)N_(4) nanosheets are systematically discussed,including the applications of these photocatalysts,which exhibit improved photoinduced charge mobility in CO_(2) photoconversion and H2 production.Issues related to the different types of multi-nanocomponent heterostructures(involving Schottky junctions,Z-/S-scheme heterostructures,noble metals,and additional semiconductor nanocomponents)and the adjustment of dimensionality of heterostructures(by incorporating noble metal nanoplates on g-C_(3)N_(4) forming 2D/2D heterostructures)are explored.The current prospects and possible challenges of g-C_(3)N_(4) composite photocatalysts incorporated with noble metals(e.g.,Au,Pt,Pd,and Cu),particularly in water splitting,CO_(2) reduction,pollution degradation,and chemical conversion applications,are summarized.展开更多
(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]是新型含能钙钛矿化合物的典型代表,需明确其热分解行为、热分解机制及感度特性,以推动其在配方中的应用。以差示扫描量热-热重分析方法实现了分解放热量、分解温度等参数的获取;以动力学模拟计算...(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]是新型含能钙钛矿化合物的典型代表,需明确其热分解行为、热分解机制及感度特性,以推动其在配方中的应用。以差示扫描量热-热重分析方法实现了分解放热量、分解温度等参数的获取;以动力学模拟计算解析了相关分解机理;以同步热分析-红外-质谱联用技术结合原位红外技术探索了(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]的分解产物及分解历程;以国军标法获得了热感度、摩擦感度与撞击感度参数。结果表明:在10℃·min^(-1)的升温速率下,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]分解放热量为4227 J·g^(-1),分解温度则达到345℃,高于黑索今(RDX)、奥克托今(HMX)、六硝基六氮杂异伍兹烷(CL-20)等多数现役含能材料,显示了优异的热稳定性;分解产物研究表明其立方笼状骨架有效稳定了内部结合的有机物分子,使其热稳定性较高。此外,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]在100℃下加热48 h的放气量约0.04 m L·g^(-1),撞击感度与机械感度分别为32%和80%,优于RDX和HMX。展开更多
Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic a...Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic activity and selectivity.The mobility and accessibility of active sites in Cubased catalysts significantly hinder the development of efficient Cu-based catalysts for CO_(2)electrochemical reduction reaction(CO_(2)RR).Herein,a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride(g-C_(3)N_(4))as the active sites for CO_(2)-to-CH_(4)conversion in CO_(2)RR.By regulating the coordination and density of Cu sites in g-C_(3)N_(4),an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH_(4)Faraday efficiency of 49.04%and produces the products with a high CH_(4)/C_(2)H_(4)ratio over 9.This work provides the first experimental study on g-C_(3)N_(4)-supported single Cu atom catalyst for efficient CH_(4)production from CO_(2)RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO_(2)RR by engineering Cu active sites in 2D materials with porous crystal structures.展开更多
The design and construction of heterojunction photocatalysts,which possess a staggered energy band structure and appropriate interfacial contact,is an effective way to achieve outstanding photocatalytic performance.In...The design and construction of heterojunction photocatalysts,which possess a staggered energy band structure and appropriate interfacial contact,is an effective way to achieve outstanding photocatalytic performance.In this study,2D/2D BiOBr/g‐C_(3)N_(4)heterojunctions were successfully obtained by a convenient in situ self‐assembly route.Under simulated sunlight irradiation,99%of RhB(10 mg·L–1,100 mL)was efficiently degraded by 1.5‐BiOBr/g‐C_(3)N_(4)within 30 min,which is better than the performance of both BiOBr and g‐C_(3)N_(4),and it has superior stability.In addition,the composite also exhibits enhanced photocatalytic activity for H2 production.The enhanced activity can be attributed to the intimate interface contact,the larger surface area,and the highly efficient separation of photoinduced electron–hole pairs.Based on the experimental results,a novel S‐scheme model was proposed to illuminate the transfer process of charge carriers.This study presents a simple way to develop novel step‐scheme photocatalysts for environmental and related applications.展开更多
Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific research.Herein,cobalt phthalocyanine...Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific research.Herein,cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4)(CoPc/OCN) S-scheme heterojunction photocatalyst was designed by coupling multi-step calcination with solvothermal method for enhanced photothermal-assisted photocatalytic H_(2) evolution.The multistep calcined g-C_(3)N_(4) is easier for O-doping formation,and the ethanol solvothermal strategy is utilized to enhance the dispersion of CoPc on OCN nano sheet surface and forms sufficient S-scheme heterojunction through H-bonds.In addition,the active sites and excellent photothermal properties of CoPc itself further improve the integrated photocatalytic activity of CoPc/OCN S-scheme heterojunction.The optimal photocatalytic hydrogen evolution rate of CoPc/OCN S-scheme heterojunction photocatalyst reached 9.56 mmol·g^(-1)·h^(-1),which is 2.69 and 1.23 times higher than that of CN and OCN,respectively.This work provides a valuable design idea and scheme for enhancing the multi-factor co-assisted photocatalytic H_(2) evolution performance.展开更多
To date,extensively high demand for hydrogen peroxide(H_(2)O_(2))has been predominantly supplied by the anthraquinone process for several worldwide applications,encompassing wastewater treatment,environmental remediat...To date,extensively high demand for hydrogen peroxide(H_(2)O_(2))has been predominantly supplied by the anthraquinone process for several worldwide applications,encompassing wastewater treatment,environmental remediation,and chemical synthesis.However,the compacted manufacturing,massive energy input and the release of tremendous wastes have restricted commercialization feasibility.Regards to mitigate such issues,the photocatalytic H_(2)O_(2)production by utilizing g-C_(3)N_(4)catalysts has endowed a greener,sustainable and promising alternative,considering that it involves water and oxygen as reactants in the present of sunlight as energy input.Herein,we have manifested a comprehensive overview of the research progress for g-C_(3)N_(4)-based semiconductors for photocatalytic H_(2)O_(2)generation.This review has systematically elucidated state-of-the-art development of different modifications on g-C_(3)N_(4)to unravel the fundamental mechanism of H_(2)O_(2)evolution via oxygen reduction reaction(ORR)and water oxidation reaction(WOR).In addition,the contribution made by vacancy introduction,doping,heterogenization,and co-catalyst passivation with respect to photoefficiency enhancement have been clarified.Furthermore,the current challenges and perspective of future development directions on photocatalytic H_(2)O_(2)production have also been highlighted.As such,g-C_(3)N_(4)stands as the next step toward advancement in the configuration and modulation of high-efficiency photocatalysts.展开更多
C_(3)N_(4),C_(3)N_(4)@Ti_(3)C_(2)and W_(18)O_(49)@C_(3)N_(4)@Ti_(3)C_(2)hollow spheres were successfully prepared by using SiO_(2)template followed by gradual deposition method.The degradation of phenol solution and p...C_(3)N_(4),C_(3)N_(4)@Ti_(3)C_(2)and W_(18)O_(49)@C_(3)N_(4)@Ti_(3)C_(2)hollow spheres were successfully prepared by using SiO_(2)template followed by gradual deposition method.The degradation of phenol solution and photolysis ability were tested to characterize its photocatalytic activity.Compared with the single-shelled C_(3)N_(4)and C_(3)N_(4)@Ti_(3)C_(2)hollow spheres,double-shelled W_(18)O_(49)@C_(3)N_(4)@Ti_(3)C_(2)hollow spheres possessed larger surface area and fast charge separation efficiency,exhibiting about 8.9 times and 4.0 times higher H_(2)evolution than those of C_(3)N_(4),C_(3)N_(4)@Ti_(3)C_(2)hollow spheres,respectively.The photocatalytic mechanism of the W_(18)O_(49)@C_(3)N_(4)@Ti_(3)C_(2)hollow spheres were carefully investigated according to the results of morphology design and photoelectric performance.A Z scheme mechanism based on the construction of heterojunctions was proposed to explain the improvement of photocatalytic performance.This new charge transfer mechanism appears to greatly inhibit the recombination of electrons/holes during the charge transfer process,while maintaining its strong hydrogen reduction ability,resulting in a higher photocatalytic performance.展开更多
The plasmonic Ag nanoparticles(NPs)loaded g-C_(3)N_(4)photocatalysts(Ag/C_(3)N_(4))were successfully prepared via a conventional procedure.The fully characterized Ag/C_(3)N_(4)photocatalysts exhibited excellent stabil...The plasmonic Ag nanoparticles(NPs)loaded g-C_(3)N_(4)photocatalysts(Ag/C_(3)N_(4))were successfully prepared via a conventional procedure.The fully characterized Ag/C_(3)N_(4)photocatalysts exhibited excellent stability and greatly enhanced visible light-driven photocatalytic performance both in the degradation of methyl orange(MO)and H_(2)evolution from water splitting.The 1.0 wt%Ag/C_(3)N_(4)allowed the highest reaction rate of 0.0294 min^(−1)to be obtained in the MO degradation,which is about 2.3 times higher than the reaction rate of g-C_(3)N_(4)alone of 0.0129 min^(−1).Furthermore,the optimum H_(2)evolution and the k value attained 20μmol and 1.573 h^(−1),respectively,after 12 h of visible light irradiation.The surface plasmon resonance effect of Ag NPs and the charge transfer between the two components of the photocatalyst,strongly promote generation of photoinduced charge carriers while suppressing their recombination.These factors are held responsible for the enhanced visible light photocatalytic performance of Ag/C_(3)N_(4).Our methodology will provide guidance for the design and synthesis of plasmon-enhanced visible light photocatalysts derived from Ag NPs and g-C_(3)N_(4)and their applications in environmental remediation and green energy development.展开更多
文摘The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.
基金supported in part by the projects from the National Natural Science Foundation of China(No.51972145)Jinan Science&Technology Bureau,China(No.2021GXRC109)Science and Technology Program of the University of Jinan,China(No.XKY2118).
文摘The photocatalytic activity of catalysts depends on the energy-harvesting ability and the separation or transport of photogenerated carriers.The light absorption capacity of graphitic carbon nitride(g-C_(3)N_(4))-based composites can be enhanced by adjusting the surface plasmon resonance(SPR)of noble metal nanoparticles(e.g.,Cu,Au,and Pd)in the entire visible region.Adjustments can be carried out by varying the nanocomponents of the materials.The SPR of noble metals can enhance the local electromagnetic field and improve interband transition,and resonant energy transfer occurs from plasmonic dipoles to electron-hole pairs via near-field electromagnetic interactions.Thus,noble metals have emerged as relevant nanocomponents for g-C_(3)N_(4) used in CO_(2) photoreduction and water splitting.Herein,recent key advances in noble metals(either in single atom,cluster,or nanoparticle forms)and composite photocatalysts based on inorganic or organic nanocomponent-incorporated g-C_(3)N_(4) nanosheets are systematically discussed,including the applications of these photocatalysts,which exhibit improved photoinduced charge mobility in CO_(2) photoconversion and H2 production.Issues related to the different types of multi-nanocomponent heterostructures(involving Schottky junctions,Z-/S-scheme heterostructures,noble metals,and additional semiconductor nanocomponents)and the adjustment of dimensionality of heterostructures(by incorporating noble metal nanoplates on g-C_(3)N_(4) forming 2D/2D heterostructures)are explored.The current prospects and possible challenges of g-C_(3)N_(4) composite photocatalysts incorporated with noble metals(e.g.,Au,Pt,Pd,and Cu),particularly in water splitting,CO_(2) reduction,pollution degradation,and chemical conversion applications,are summarized.
文摘(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]是新型含能钙钛矿化合物的典型代表,需明确其热分解行为、热分解机制及感度特性,以推动其在配方中的应用。以差示扫描量热-热重分析方法实现了分解放热量、分解温度等参数的获取;以动力学模拟计算解析了相关分解机理;以同步热分析-红外-质谱联用技术结合原位红外技术探索了(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]的分解产物及分解历程;以国军标法获得了热感度、摩擦感度与撞击感度参数。结果表明:在10℃·min^(-1)的升温速率下,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]分解放热量为4227 J·g^(-1),分解温度则达到345℃,高于黑索今(RDX)、奥克托今(HMX)、六硝基六氮杂异伍兹烷(CL-20)等多数现役含能材料,显示了优异的热稳定性;分解产物研究表明其立方笼状骨架有效稳定了内部结合的有机物分子,使其热稳定性较高。此外,(C_(6)H_(14)N_(2))[Na(ClO_(4))_(3)]在100℃下加热48 h的放气量约0.04 m L·g^(-1),撞击感度与机械感度分别为32%和80%,优于RDX和HMX。
基金This work was supported by the Fundamental Research Funds for the Central Universities(2232021A-02 and 2232023Y-01)the National Natural Science Foundation of China(Nos.52122312,22209024 and 22202183).
文摘Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic activity and selectivity.The mobility and accessibility of active sites in Cubased catalysts significantly hinder the development of efficient Cu-based catalysts for CO_(2)electrochemical reduction reaction(CO_(2)RR).Herein,a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride(g-C_(3)N_(4))as the active sites for CO_(2)-to-CH_(4)conversion in CO_(2)RR.By regulating the coordination and density of Cu sites in g-C_(3)N_(4),an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH_(4)Faraday efficiency of 49.04%and produces the products with a high CH_(4)/C_(2)H_(4)ratio over 9.This work provides the first experimental study on g-C_(3)N_(4)-supported single Cu atom catalyst for efficient CH_(4)production from CO_(2)RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO_(2)RR by engineering Cu active sites in 2D materials with porous crystal structures.
文摘The design and construction of heterojunction photocatalysts,which possess a staggered energy band structure and appropriate interfacial contact,is an effective way to achieve outstanding photocatalytic performance.In this study,2D/2D BiOBr/g‐C_(3)N_(4)heterojunctions were successfully obtained by a convenient in situ self‐assembly route.Under simulated sunlight irradiation,99%of RhB(10 mg·L–1,100 mL)was efficiently degraded by 1.5‐BiOBr/g‐C_(3)N_(4)within 30 min,which is better than the performance of both BiOBr and g‐C_(3)N_(4),and it has superior stability.In addition,the composite also exhibits enhanced photocatalytic activity for H2 production.The enhanced activity can be attributed to the intimate interface contact,the larger surface area,and the highly efficient separation of photoinduced electron–hole pairs.Based on the experimental results,a novel S‐scheme model was proposed to illuminate the transfer process of charge carriers.This study presents a simple way to develop novel step‐scheme photocatalysts for environmental and related applications.
基金financially supported by the National Natural Science Foundation of China (Nos.21906072, 21906039, 21908115 and 22006057)Hebei Province 333 Talents Project (No.A202101020)+3 种基金the Science and Technology Project of Hebei Education Department (No.BJ2021010)the Graduate Student Innovation Ability Training Funding Project of Hebei Province (No.CXZZSS2023129)the Open Fund for Hebei Province Key Laboratory of Sustained Utilization & Development of Water Recourse (No.HSZYL2022002)Instrumental Analysis Center, Jiangsu University of Science and Technology。
文摘Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific research.Herein,cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4)(CoPc/OCN) S-scheme heterojunction photocatalyst was designed by coupling multi-step calcination with solvothermal method for enhanced photothermal-assisted photocatalytic H_(2) evolution.The multistep calcined g-C_(3)N_(4) is easier for O-doping formation,and the ethanol solvothermal strategy is utilized to enhance the dispersion of CoPc on OCN nano sheet surface and forms sufficient S-scheme heterojunction through H-bonds.In addition,the active sites and excellent photothermal properties of CoPc itself further improve the integrated photocatalytic activity of CoPc/OCN S-scheme heterojunction.The optimal photocatalytic hydrogen evolution rate of CoPc/OCN S-scheme heterojunction photocatalyst reached 9.56 mmol·g^(-1)·h^(-1),which is 2.69 and 1.23 times higher than that of CN and OCN,respectively.This work provides a valuable design idea and scheme for enhancing the multi-factor co-assisted photocatalytic H_(2) evolution performance.
基金the Ministry of Higher Education(MOHE)Malaysia under the Fundamental Research Grant Scheme(FRGS)(Ref no:FRGS/1/2020/TK0/XMU/02/1)the Ministry of Science,Technology and Innovation(MOSTI)Malaysia under the Strategic Research Fund(SRF-APP)(S.22015)+4 种基金the National Natural Science Foundation of China(Ref no:22202168)Guangdong Basic and Applied Basic Research Foundation(Ref no:2021A1515111019)Xiamen University Malaysia Investigatorship Grant(Grant no:IENG/0038)Xiamen University Malaysia Research Fund(ICOE/0001,XMUMRF/2021-C8/IENG/0041 and XMUMRF/2019-C3/IENG/0013)Hengyuan International Sdn.Bhd.(Grant no:EENG/0003).
文摘To date,extensively high demand for hydrogen peroxide(H_(2)O_(2))has been predominantly supplied by the anthraquinone process for several worldwide applications,encompassing wastewater treatment,environmental remediation,and chemical synthesis.However,the compacted manufacturing,massive energy input and the release of tremendous wastes have restricted commercialization feasibility.Regards to mitigate such issues,the photocatalytic H_(2)O_(2)production by utilizing g-C_(3)N_(4)catalysts has endowed a greener,sustainable and promising alternative,considering that it involves water and oxygen as reactants in the present of sunlight as energy input.Herein,we have manifested a comprehensive overview of the research progress for g-C_(3)N_(4)-based semiconductors for photocatalytic H_(2)O_(2)generation.This review has systematically elucidated state-of-the-art development of different modifications on g-C_(3)N_(4)to unravel the fundamental mechanism of H_(2)O_(2)evolution via oxygen reduction reaction(ORR)and water oxidation reaction(WOR).In addition,the contribution made by vacancy introduction,doping,heterogenization,and co-catalyst passivation with respect to photoefficiency enhancement have been clarified.Furthermore,the current challenges and perspective of future development directions on photocatalytic H_(2)O_(2)production have also been highlighted.As such,g-C_(3)N_(4)stands as the next step toward advancement in the configuration and modulation of high-efficiency photocatalysts.
基金Supported by the National Natural Science Foundation of China(Nos.91963207 and 12075174)。
文摘C_(3)N_(4),C_(3)N_(4)@Ti_(3)C_(2)and W_(18)O_(49)@C_(3)N_(4)@Ti_(3)C_(2)hollow spheres were successfully prepared by using SiO_(2)template followed by gradual deposition method.The degradation of phenol solution and photolysis ability were tested to characterize its photocatalytic activity.Compared with the single-shelled C_(3)N_(4)and C_(3)N_(4)@Ti_(3)C_(2)hollow spheres,double-shelled W_(18)O_(49)@C_(3)N_(4)@Ti_(3)C_(2)hollow spheres possessed larger surface area and fast charge separation efficiency,exhibiting about 8.9 times and 4.0 times higher H_(2)evolution than those of C_(3)N_(4),C_(3)N_(4)@Ti_(3)C_(2)hollow spheres,respectively.The photocatalytic mechanism of the W_(18)O_(49)@C_(3)N_(4)@Ti_(3)C_(2)hollow spheres were carefully investigated according to the results of morphology design and photoelectric performance.A Z scheme mechanism based on the construction of heterojunctions was proposed to explain the improvement of photocatalytic performance.This new charge transfer mechanism appears to greatly inhibit the recombination of electrons/holes during the charge transfer process,while maintaining its strong hydrogen reduction ability,resulting in a higher photocatalytic performance.
基金supported by LiaoNing Revitalization Talents Pro-gram(XLYC2007166)Joint Funds for Innovation Capability Improve-ment of Natural Science Foundation of Liaoning Province(2021-NLTS-12-08)+1 种基金the Key Task and Local Project in Science&Technology of SYUCT(LDB2019004)the Open Funds of the State Key Laboratory of Rare Earth Resource Utilization(RERU2021018).
文摘The plasmonic Ag nanoparticles(NPs)loaded g-C_(3)N_(4)photocatalysts(Ag/C_(3)N_(4))were successfully prepared via a conventional procedure.The fully characterized Ag/C_(3)N_(4)photocatalysts exhibited excellent stability and greatly enhanced visible light-driven photocatalytic performance both in the degradation of methyl orange(MO)and H_(2)evolution from water splitting.The 1.0 wt%Ag/C_(3)N_(4)allowed the highest reaction rate of 0.0294 min^(−1)to be obtained in the MO degradation,which is about 2.3 times higher than the reaction rate of g-C_(3)N_(4)alone of 0.0129 min^(−1).Furthermore,the optimum H_(2)evolution and the k value attained 20μmol and 1.573 h^(−1),respectively,after 12 h of visible light irradiation.The surface plasmon resonance effect of Ag NPs and the charge transfer between the two components of the photocatalyst,strongly promote generation of photoinduced charge carriers while suppressing their recombination.These factors are held responsible for the enhanced visible light photocatalytic performance of Ag/C_(3)N_(4).Our methodology will provide guidance for the design and synthesis of plasmon-enhanced visible light photocatalysts derived from Ag NPs and g-C_(3)N_(4)and their applications in environmental remediation and green energy development.
