Designing and fabricating highly efficient photocatalysts for water splitting is a promising strategy to address energy and environmental issues.Cadmium sulfide(CdS)has received significant interest as a photocatalyst...Designing and fabricating highly efficient photocatalysts for water splitting is a promising strategy to address energy and environmental issues.Cadmium sulfide(CdS)has received significant interest as a photocatalyst for visible‐light‐induced hydrogen(H2)generation.However,the severe photocorrosion,high overpotential,rapid charge recombination,and sluggish surface reaction kinetics drastically hinder its practical application in water splitting.Herein,uniform zinc cadmium sulfide(Zn_(0.5)Cd_(0.5)S)nanoparticles were anchored on ultrathin Ni(OH)_(2)nanosheets via a facile solution‐phase approach to form an intimate two‐dimensional(2D)/zero‐dimensional(0D)heterojunction.Under visible light irradiation,the 7%Ni(OH)_(2)/Zn_(0.5)Cd_(0.5)S composite exhibited the highest H2 production rate of 6.87 mmol·h^(–1)·g^(–1)with an apparent quantum yield of 16.8%at 420 nm,which is almost 43 times higher than that of pristine Zn_(0.5)Cd_(0.5)S and considerably higher than that of the Pt/Zn_(0.5)Cd_(0.5)S photocatalyst.The high photoactivity of the 2D/0D Ni(OH)_(2)/Zn_(0.5)Cd_(0.5)S heterojunction can be ascribed to its unique and robust structure,wherein the ultrathin Ni(OH)_(2)nanosheets not only provide an excellent platform for the incorporation of Zn_(0.5)Cd_(0.5)S nanoparticles but also serve as an effective cocatalyst to promote photoinduced electron transfer and offer more active sites for photocatalytic H_(2) generation.This work paves the way toward the development of versatile,low‐cost,and highly efficient 2D/0D heterojunction photocatalysts for solar energy conversion.展开更多
Different components of PtPd bimetallic cocatalysts modified Zn_(0.5)Cd_(0.5)S nanorods have already been designed and prepared in this study.The obtained hybrid photocatalysts were tested and characterized by XPS,ICP...Different components of PtPd bimetallic cocatalysts modified Zn_(0.5)Cd_(0.5)S nanorods have already been designed and prepared in this study.The obtained hybrid photocatalysts were tested and characterized by XPS,ICP-OES and UV-Vis spectra,TEM and EDX tools.Such characterizations can prove the formation of PtPd bimetallic alloy particles in hybrid catalysts.Under visible light illumination,an outstanding hydrogen producing rate of 9.689mmol·g^(-1)·h^(-1) and a high AQY efficiency up to 10.43%at 420 nm are achieved in this work.In addition,thermodynamics(DFT calculations)and kinetics(Photoluminescence emission,photocurrent responses,electrochemical impedance spectroscopy and surface photovoltage spectra)investigations illustrate that PtPd bimetallic alloy has similar catalytic thermodynamic properties to Pt,which can greatly boost the charge separation and speed up the charge transfer,and decrease the activation energy of H2 generation.Notably,the calculation data suggests that Pt is thermodynamically favorable,while PtPd alloy is kinetically beneficial to H_(2)production,which can be ascribed to the higher activity of PtPd/Zn_(0.5)Cd_(0.5)S than Pt/Zn_(0.5)Cd_(0.5)S.This work can propose a fresh perspective for preparing high efficiency hybrid photocatalysts.展开更多
In recent years,many effective photocatalysts have been developed to solve the problem of environmental pollution and clean energy shortage.In this paper,non-noble metal cocatalyst Ni_(3)N nanoparticles supported Zn_(...In recent years,many effective photocatalysts have been developed to solve the problem of environmental pollution and clean energy shortage.In this paper,non-noble metal cocatalyst Ni_(3)N nanoparticles supported Zn_(0.5)Cd_(0.5)S(ZCS)nanorods(Ni_(3)N/ZCS)composites were successfully synthesized by ultrasonic method.The hydrogen production efficiencies of the photocatalysts were tested under visible light,which was found that when the loading of Ni_(3)N was 2%of the mass of ZCS,and the Ni_(3)N/ZCS composite had the best hydrogen evolution performance,which could reach 70.3 mmol·h^(-1)·g^(-1).In addition,the quantum efficiency under 420 nm monochromatic light irradiation was 27.2%.Through different characterization analyses,such as X-ray diffraction(XRD),scanning electron microscopy(SEM),and UV-Vis diffuse reflectance spectra(DRS),a possible photocatalytic mechanism was proposed,providing some reference values for non-precious metals as cocatalysts.展开更多
The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal...The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal‐organic frameworks(MOFs)are considered to be potential photocatalytic materials.Herein,monodisperse,small size,non‐precious metal transition metal phosphide Ni2P is encapsulated into a typical MOF(UiO‐66‐NH2)as a hybrid core‐shell cocatalyst to modify Zn_(0.5)Cd_(0.5)S for photocatalytic hydrogen production.Ni2P is wrapped in UiO‐66‐NH_(2)via an in situ solvothermal method,and Zn_(0.5)Cd_(0.5)S sulfide is decorated with a core‐shell Ni_(2)P@UiO‐66‐NH_(2)cocatalyst to obtain ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite materials.Photoelectric and chemical characterization confirms that the ternary composites have good kinetic hydrogen production performance.The hydrogen production rate of 10%10 mg Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S reaches 40.91 mmol·g^(–1)·h^(–1)with an apparent quantum efficiency at 420 nm of 13.57%.The addition of 10 mg Ni_(2)P@UiO‐66‐NH_(2)increases the surface area of the ternary material,providing abundant reaction sites and forming an efficient charge transfer channel,which is conducive to efficient hydrogen production by the ternary photocatalysts.It is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic reaction.This study provides a new perspective for the construction of high‐performance photocatalytic materials.展开更多
The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts...The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.展开更多
文摘Designing and fabricating highly efficient photocatalysts for water splitting is a promising strategy to address energy and environmental issues.Cadmium sulfide(CdS)has received significant interest as a photocatalyst for visible‐light‐induced hydrogen(H2)generation.However,the severe photocorrosion,high overpotential,rapid charge recombination,and sluggish surface reaction kinetics drastically hinder its practical application in water splitting.Herein,uniform zinc cadmium sulfide(Zn_(0.5)Cd_(0.5)S)nanoparticles were anchored on ultrathin Ni(OH)_(2)nanosheets via a facile solution‐phase approach to form an intimate two‐dimensional(2D)/zero‐dimensional(0D)heterojunction.Under visible light irradiation,the 7%Ni(OH)_(2)/Zn_(0.5)Cd_(0.5)S composite exhibited the highest H2 production rate of 6.87 mmol·h^(–1)·g^(–1)with an apparent quantum yield of 16.8%at 420 nm,which is almost 43 times higher than that of pristine Zn_(0.5)Cd_(0.5)S and considerably higher than that of the Pt/Zn_(0.5)Cd_(0.5)S photocatalyst.The high photoactivity of the 2D/0D Ni(OH)_(2)/Zn_(0.5)Cd_(0.5)S heterojunction can be ascribed to its unique and robust structure,wherein the ultrathin Ni(OH)_(2)nanosheets not only provide an excellent platform for the incorporation of Zn_(0.5)Cd_(0.5)S nanoparticles but also serve as an effective cocatalyst to promote photoinduced electron transfer and offer more active sites for photocatalytic H_(2) generation.This work paves the way toward the development of versatile,low‐cost,and highly efficient 2D/0D heterojunction photocatalysts for solar energy conversion.
文摘Different components of PtPd bimetallic cocatalysts modified Zn_(0.5)Cd_(0.5)S nanorods have already been designed and prepared in this study.The obtained hybrid photocatalysts were tested and characterized by XPS,ICP-OES and UV-Vis spectra,TEM and EDX tools.Such characterizations can prove the formation of PtPd bimetallic alloy particles in hybrid catalysts.Under visible light illumination,an outstanding hydrogen producing rate of 9.689mmol·g^(-1)·h^(-1) and a high AQY efficiency up to 10.43%at 420 nm are achieved in this work.In addition,thermodynamics(DFT calculations)and kinetics(Photoluminescence emission,photocurrent responses,electrochemical impedance spectroscopy and surface photovoltage spectra)investigations illustrate that PtPd bimetallic alloy has similar catalytic thermodynamic properties to Pt,which can greatly boost the charge separation and speed up the charge transfer,and decrease the activation energy of H2 generation.Notably,the calculation data suggests that Pt is thermodynamically favorable,while PtPd alloy is kinetically beneficial to H_(2)production,which can be ascribed to the higher activity of PtPd/Zn_(0.5)Cd_(0.5)S than Pt/Zn_(0.5)Cd_(0.5)S.This work can propose a fresh perspective for preparing high efficiency hybrid photocatalysts.
基金supported by the Natural Science Foundation of Jilin Province,China(No.YDZJ202101ZYTS067)the Foundation of Xinzhou Normal University,China(No.2021KY01).
文摘In recent years,many effective photocatalysts have been developed to solve the problem of environmental pollution and clean energy shortage.In this paper,non-noble metal cocatalyst Ni_(3)N nanoparticles supported Zn_(0.5)Cd_(0.5)S(ZCS)nanorods(Ni_(3)N/ZCS)composites were successfully synthesized by ultrasonic method.The hydrogen production efficiencies of the photocatalysts were tested under visible light,which was found that when the loading of Ni_(3)N was 2%of the mass of ZCS,and the Ni_(3)N/ZCS composite had the best hydrogen evolution performance,which could reach 70.3 mmol·h^(-1)·g^(-1).In addition,the quantum efficiency under 420 nm monochromatic light irradiation was 27.2%.Through different characterization analyses,such as X-ray diffraction(XRD),scanning electron microscopy(SEM),and UV-Vis diffuse reflectance spectra(DRS),a possible photocatalytic mechanism was proposed,providing some reference values for non-precious metals as cocatalysts.
文摘The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal‐organic frameworks(MOFs)are considered to be potential photocatalytic materials.Herein,monodisperse,small size,non‐precious metal transition metal phosphide Ni2P is encapsulated into a typical MOF(UiO‐66‐NH2)as a hybrid core‐shell cocatalyst to modify Zn_(0.5)Cd_(0.5)S for photocatalytic hydrogen production.Ni2P is wrapped in UiO‐66‐NH_(2)via an in situ solvothermal method,and Zn_(0.5)Cd_(0.5)S sulfide is decorated with a core‐shell Ni_(2)P@UiO‐66‐NH_(2)cocatalyst to obtain ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite materials.Photoelectric and chemical characterization confirms that the ternary composites have good kinetic hydrogen production performance.The hydrogen production rate of 10%10 mg Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S reaches 40.91 mmol·g^(–1)·h^(–1)with an apparent quantum efficiency at 420 nm of 13.57%.The addition of 10 mg Ni_(2)P@UiO‐66‐NH_(2)increases the surface area of the ternary material,providing abundant reaction sites and forming an efficient charge transfer channel,which is conducive to efficient hydrogen production by the ternary photocatalysts.It is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic reaction.This study provides a new perspective for the construction of high‐performance photocatalytic materials.
文摘The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.
