Inorganic-organic hybrid materials are promising for application in the field of photocatalysis because of their excellent properties.Therefore,their syntheses,mechanisms,and applications are reviewed in this paper.Fi...Inorganic-organic hybrid materials are promising for application in the field of photocatalysis because of their excellent properties.Therefore,their syntheses,mechanisms,and applications are reviewed in this paper.First,we introduce the role of inorganic-organic photocatalysts,their advantages and disadvantages,and their design principles.Second,we present the top-down and bottom-up synthesis methods of the hybrid materials.The interaction between inorganic and organic components in hybrid materials is discussed,followed by how to improve inorganic-organic photocatalysts.Third,the applications of hybrid materials in the field of photocatalysis,such as realizing hydrogen evolution,organic pollutant degradation,heavy metals and CO_(2) reduction,sterilization,and nitrogen fixation,are examined.Finally,the application prospects and development directions of inorganic-organic hybrid materials are explored and the unsolved problems are described.展开更多
In this work, an efficient AgVO3/MoS 2 composite photocatalyst was successfully synthesized via a hydrothermal method. The photocatalytic activity of the as-prepared photocatalyst was evaluated by using it for assessi...In this work, an efficient AgVO3/MoS 2 composite photocatalyst was successfully synthesized via a hydrothermal method. The photocatalytic activity of the as-prepared photocatalyst was evaluated by using it for assessing the degradation of different organic pollutants under visible-light irradiation. The composite 3%-AgVO3/MoS 2 catalyst demonstrated a significantly enhanced photocatalytic activity compared to the pure compounds(AgVO3 and MoS2). The reason behind the excellent photocatalytic performance was the modification of MoS 2 by AgVO3 to facilitate O2 adsorption/activation. In addition, the composite catalyst facilitates the two-electron oxygen reduction reaction whereby H2O2 is generated on the surface of MoS 2 to produce additional reactive oxygen species(ROSs). ESR coupled with the POPHA fluorescence detection method and a free radical capture experiment were used to elucidate the mechanism of formation of the ROSs, including ·OH, ·O2- and H2O2. Furthermore, the generation of additional ROSs could accelerate electron consumption, leaving behind more holes for the oxidation of organic pollutants. A possible photocatalytic mechanism of the composite is also discussed.展开更多
TiO2 and TiO2-SiO2 photocatalysts were prepared by sol-gel and supercritical CO2 fluid drying method and characterized by X-ray diffraction (XRD), transmission electron microscope (TEM), etc. Their catalytic propertie...TiO2 and TiO2-SiO2 photocatalysts were prepared by sol-gel and supercritical CO2 fluid drying method and characterized by X-ray diffraction (XRD), transmission electron microscope (TEM), etc. Their catalytic properties were tested through the photocatalytic degradation of phenol and aniline in wastewater. The results show that the developed fluidized photocatalytic reactor (FPR) and TiO2 catalyst had better performance in degrading pollutants as compared with slurry photocatalytic reactor (SPR) and commercial TiO2 catalyst. The composition and crystal form of TiO2-SiO2 composite oxide had obvious influence on catalytic effect and TiO2-SiO2 photocatalysts showed better catalytic activity and stability.展开更多
Molecular catalysts for H2-evolution are of interest for their integration into light-harvesting complexes for photocatalytic water splitting.Here,we report the meso-tetra(4-carboxyphenyl)porphine[(TCPP)Pt^(Ⅱ)]comple...Molecular catalysts for H2-evolution are of interest for their integration into light-harvesting complexes for photocatalytic water splitting.Here,we report the meso-tetra(4-carboxyphenyl)porphine[(TCPP)Pt^(Ⅱ)]complex as a molecular H2-evolving photocatalyst using chloranilic acid(CA)as a sacrificial electron donor,the choice of which is critical to the stability of the photocatalyst.When triethanolamine was used,[(TCPP)Pt^(Ⅱ)]decomposed to form Pt nanoparticles.Density functional theory calculations together with evidence from electrochemical and spectroscopic analyses suggested that the catalysis was possibly initiated by a proton-coupled electron transfer(PCET)to form[(TCPP)Pt^(Ⅰ)]-N-H,followed by another electron injection and protonation to form a[(TCPP)Pt^(Ⅱ)-hydride]-N-H intermediate that can release H2.As the whole catalytic cycle involves the injection of multiple electrons,a light-harvesting network should be helpful by providing multiple photo-induced electrons.Thus,we integrated this molecular catalyst into a light-harvesting metal-organic framework to boost its activity by~830 times.This work presents a mechanistic study of the photocatalytic H2 evolution and energy transfer and highlights the importance of a light-harvesting network for multiple electron injections.展开更多
In the present work, a novel porous, and chemically stable amine-based covalent organic polymer (POP-1) was designed and synthesized under solvothermal conditions. The porosity, crystallinity, chemical stability, el...In the present work, a novel porous, and chemically stable amine-based covalent organic polymer (POP-1) was designed and synthesized under solvothermal conditions. The porosity, crystallinity, chemical stability, electrochemical properties, and diffuse reflectance of POP-1 were investigated via N2 sorp- tion experiment, power X-ray diffraction, thermogravimetric analysis, cyclic voltammetry, and ultraviolet visible near infrared spectrometry, respectively. POP-I exhibits good chemical stability in both acidic and alkaline aqueous solutions, as well as in organic solvents. Undoped POP-1 can be directly used as a pho- tocatalyst for rhodamine B irradiation degradation under light-emitting diode and natural light. The Ea of POP-1 for RhB degradation is 82.37 kJ/mol. Furthermore, POP-1 can be reused as a catalyst in RhB degra- dation without degraded catalytic activity.展开更多
文摘Inorganic-organic hybrid materials are promising for application in the field of photocatalysis because of their excellent properties.Therefore,their syntheses,mechanisms,and applications are reviewed in this paper.First,we introduce the role of inorganic-organic photocatalysts,their advantages and disadvantages,and their design principles.Second,we present the top-down and bottom-up synthesis methods of the hybrid materials.The interaction between inorganic and organic components in hybrid materials is discussed,followed by how to improve inorganic-organic photocatalysts.Third,the applications of hybrid materials in the field of photocatalysis,such as realizing hydrogen evolution,organic pollutant degradation,heavy metals and CO_(2) reduction,sterilization,and nitrogen fixation,are examined.Finally,the application prospects and development directions of inorganic-organic hybrid materials are explored and the unsolved problems are described.
基金supported by the National Natural Science Foundation of China(21706104)the Natural Science Foundation of Jiangsu Province(BK20150484)+1 种基金the China Postdoctoral Science Foundation(2015M570416)the financial support of the Research Foundation of Jiangsu University,China(14JDG148)~~
文摘In this work, an efficient AgVO3/MoS 2 composite photocatalyst was successfully synthesized via a hydrothermal method. The photocatalytic activity of the as-prepared photocatalyst was evaluated by using it for assessing the degradation of different organic pollutants under visible-light irradiation. The composite 3%-AgVO3/MoS 2 catalyst demonstrated a significantly enhanced photocatalytic activity compared to the pure compounds(AgVO3 and MoS2). The reason behind the excellent photocatalytic performance was the modification of MoS 2 by AgVO3 to facilitate O2 adsorption/activation. In addition, the composite catalyst facilitates the two-electron oxygen reduction reaction whereby H2O2 is generated on the surface of MoS 2 to produce additional reactive oxygen species(ROSs). ESR coupled with the POPHA fluorescence detection method and a free radical capture experiment were used to elucidate the mechanism of formation of the ROSs, including ·OH, ·O2- and H2O2. Furthermore, the generation of additional ROSs could accelerate electron consumption, leaving behind more holes for the oxidation of organic pollutants. A possible photocatalytic mechanism of the composite is also discussed.
文摘TiO2 and TiO2-SiO2 photocatalysts were prepared by sol-gel and supercritical CO2 fluid drying method and characterized by X-ray diffraction (XRD), transmission electron microscope (TEM), etc. Their catalytic properties were tested through the photocatalytic degradation of phenol and aniline in wastewater. The results show that the developed fluidized photocatalytic reactor (FPR) and TiO2 catalyst had better performance in degrading pollutants as compared with slurry photocatalytic reactor (SPR) and commercial TiO2 catalyst. The composition and crystal form of TiO2-SiO2 composite oxide had obvious influence on catalytic effect and TiO2-SiO2 photocatalysts showed better catalytic activity and stability.
文摘Molecular catalysts for H2-evolution are of interest for their integration into light-harvesting complexes for photocatalytic water splitting.Here,we report the meso-tetra(4-carboxyphenyl)porphine[(TCPP)Pt^(Ⅱ)]complex as a molecular H2-evolving photocatalyst using chloranilic acid(CA)as a sacrificial electron donor,the choice of which is critical to the stability of the photocatalyst.When triethanolamine was used,[(TCPP)Pt^(Ⅱ)]decomposed to form Pt nanoparticles.Density functional theory calculations together with evidence from electrochemical and spectroscopic analyses suggested that the catalysis was possibly initiated by a proton-coupled electron transfer(PCET)to form[(TCPP)Pt^(Ⅰ)]-N-H,followed by another electron injection and protonation to form a[(TCPP)Pt^(Ⅱ)-hydride]-N-H intermediate that can release H2.As the whole catalytic cycle involves the injection of multiple electrons,a light-harvesting network should be helpful by providing multiple photo-induced electrons.Thus,we integrated this molecular catalyst into a light-harvesting metal-organic framework to boost its activity by~830 times.This work presents a mechanistic study of the photocatalytic H2 evolution and energy transfer and highlights the importance of a light-harvesting network for multiple electron injections.
基金supported by the National Natural Science Foundation of China(21601109 and 21403130)the Natural Science Foundation of Shandong Province(ZR2014BQ028)
文摘In the present work, a novel porous, and chemically stable amine-based covalent organic polymer (POP-1) was designed and synthesized under solvothermal conditions. The porosity, crystallinity, chemical stability, electrochemical properties, and diffuse reflectance of POP-1 were investigated via N2 sorp- tion experiment, power X-ray diffraction, thermogravimetric analysis, cyclic voltammetry, and ultraviolet visible near infrared spectrometry, respectively. POP-I exhibits good chemical stability in both acidic and alkaline aqueous solutions, as well as in organic solvents. Undoped POP-1 can be directly used as a pho- tocatalyst for rhodamine B irradiation degradation under light-emitting diode and natural light. The Ea of POP-1 for RhB degradation is 82.37 kJ/mol. Furthermore, POP-1 can be reused as a catalyst in RhB degra- dation without degraded catalytic activity.