In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using...In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 （EO20PO70EO20） as template. Scanning electron microscopy （SEM）, X-ray diffraction （XRD）, nitrogen adsorption-desorption measurements, and UV-visible spectroscopy （UV-Vis） were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange （MO） in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.展开更多
A heterojunction photocatalyst based on porous tubular g-C3N4 decorated with CdS nanoparticles was fabricated by a facile hydrothermal co-deposition method.The one-dimensional porous structure of g-C3N4 provides a hig...A heterojunction photocatalyst based on porous tubular g-C3N4 decorated with CdS nanoparticles was fabricated by a facile hydrothermal co-deposition method.The one-dimensional porous structure of g-C3N4 provides a higher specific surface area,enhanced light absorption,and better separation and transport performance of charge carriers along the longitudinal direction,all of which synergistically contribute to the superior photocatalytic activity observed.The significantly enhanced catalytic efficiency is also a benefit originating from the fast transfer of photogenerated electrons and holes between g-C3N4 and CdS through a built-in electric field,which was confirmed by investigating the morphology,structure,optical properties,electrochemical properties,and photocatalytic activities.Photocatalytic degradation of rhodamine B(RhB)and photocatalytic hydrogen evolution reaction were also carried out to investigate its photocatalytic performance.RhB can be degraded completely within 60 min,and the optimum H2 evolution rate of tubular g-C3N4/CdS composite is as high as 71.6μmol h^–1,which is about 16.3 times higher than that of pure bulk g-C3N4.The as-prepared nanostructure would be suitable for treating environmental pollutants as well as for water splitting.展开更多
Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most de...Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most developed co-catalysts for semiconductor-based photocatalysis are inorganic materials;the employment of a specific organic molecule as a co-catalyst for photocatalytic hydrogen evolution and pollutant photodegradation is rare and still remains a challenging task. Herein, we report on the use of an organic molecule, oxamide (OA), as a novel co-catalyst to enhance electron- hole separation, photocatalytic H2 evolution, and dye degradation over TiO2 nanosheets. OA-modified TiO2 samples were prepared by a wet chemical route and demonstrated improved light absorption in the visible-light region and more efficient charge transport. The photocatalytic performance of H2 evolution from water splitting and rhodamine B (RhB) degradation for an optimal OA-modified TiO2 photocatalyst reached 2.37 mmol g^–1 h^–1 and 1.43 × 10^-2 min^-1, respectively, which were 2.4 and 3.8 times higher than those of pristine TiO2, respectively. A possible mechanism is proposed, in which the specific π-conjugated structure of OA is suggested to play a key role in the enhancement of the charge transfer and catalytic capability of TiO2. This work may provide advanced insight into the development of a variety of metal-free organic molecules as functional co-catalysts for improved solar-to-fuel conversion and environmental remediation.展开更多
Nanosize TiO 2,Y 2 O 3/TiO 2 particles were prepared by the sol-gel process. The structur e was characterized by means of XRD,TEM. The photoelectric properties of the nan oparticles were studied by PL. The thickness a...Nanosize TiO 2,Y 2 O 3/TiO 2 particles were prepared by the sol-gel process. The structur e was characterized by means of XRD,TEM. The photoelectric properties of the nan oparticles were studied by PL. The thickness and the surface of the carboxymethy l cellulose film was measured by SEM. Based on a model reaction, the photocataly tic degradation of methylene blue with positive charge was investigated in TiO 2, Y2O3/TiO 2 nanopowder composite films irradiated by UV lamp. The results revealed that the degradation process belonged to the first-order k inetic reaction.展开更多
Molecular doping has been proven to be an effective approach to adjusting the electronic structure of polymeric carbon nitride(PCN)and thus improving its optical properties and photocatalytic activity.Herein,theobromi...Molecular doping has been proven to be an effective approach to adjusting the electronic structure of polymeric carbon nitride(PCN)and thus improving its optical properties and photocatalytic activity.Herein,theobromine,a compound composed of an imidazole ring and a pyrimidine ring,was first copolymerized with urea to prepared doped PCN.Experimental investigations and theoretical calculations indicate that,a narrowing in band gap and a positive shift in valence band positon happened to the theobromine doped PCN,owing to the synergistic effect between the pyrimidine ring and the imidazole ring in the theobromine molecule.Moreover,it is shown that the doping with theobromine at a suitable mass fraction makes the obtained sample exhibit decreased photoluminescent emission,enhanced photocurrent density,and reduced charge-transport resistance.Consequently,an enhancement in the photocatalytic activity for water oxidation is found for the sample,which oxygen evolution rate is 4.43 times higher than that of the undoped PCN.This work sheds light on the choice of the molecular dopants for PCN to improve its photocatalytic performance.展开更多
The photodegradation has been widely used in water and waste water treatment of all the methods like froth flotation coagulation etc., photodegradation appears to offer the best prospects for overall treatment of dyes...The photodegradation has been widely used in water and waste water treatment of all the methods like froth flotation coagulation etc., photodegradation appears to offer the best prospects for overall treatment of dyestuff effulent. Photodegradation of aniline blue and crystal violet dyes from aqueous solutions of their binary mixture was carried out using TiO2 as photocatalyst. By carrying out photodegradation, varying the experimental parameters, the optimum conditions required for maximum degradation was found out. The photodegradation of dye was carried out using different sources of energy like solar radiation and microwave radiation. The degradation studies were carried out at temperatures 25 ℃, 35 ℃ and 45 ℃ so as to calculate the rate constant and activation parameters. Both energy sources are equivalent in causing degradation in all respects except time and dose of photo catalyst. Time required is less for microwave than solar radiation, but dose of photo catalyst needed was high for microwave radiation. These results will be helpful in designing effluent treatment plants in industries.展开更多
Semiconductor photocatalysts play an indispensable role in the photocatalytic process.Two-dimensional covalent organic frameworks(2D-COFs),as a kind of innovative photocatalyst,have garnered tremendous attention.Herei...Semiconductor photocatalysts play an indispensable role in the photocatalytic process.Two-dimensional covalent organic frameworks(2D-COFs),as a kind of innovative photocatalyst,have garnered tremendous attention.Herein,we report an amide-linked 2D-COF(COF-JLU19)with outstanding photocatalytic performance in water,designed through a multi-synergistic approach.The synergistic effects of the high porosity,photoactive framework,high wettability,and stability of COF-JLU19 led to an unprecedented enhancement in the photocatalytic activity and recyclability in water upon illumination by visible light.More importantly,amide-linked 2D-COF based electrospinning membranes were prepared,which also exhibited superior photocatalytic activity for the degradation of Rhodamine B in water with sunlight.This study highlights the potential of the multi-synergistic approach as a universal rule for developing COF-based photocatalysts to address environmental and energy challenges.展开更多
Zinc oxide （ZnO） has been used as heterogeneous catalyst for the degradation of Acid Alizarin Black S dye （AAB） in aqueous solutions using UV light irradiation. Experiments were conducted at various operating para...Zinc oxide （ZnO） has been used as heterogeneous catalyst for the degradation of Acid Alizarin Black S dye （AAB） in aqueous solutions using UV light irradiation. Experiments were conducted at various operating parameters. The operating parameters were amount of catalyst （50 rag, 100 mg and 150 mg）, initial concentration of dye （30 mg/L, 50 mg/L and 70 mg/L）, the pH of solution （2, 4, 6, 8, l0 and 12） and the UV light intensity （6 watt and 12 watt）. The progress of the degradation reaction was monitored spectrophotometrically. It was found that the degradation process of AAB solution was accelerated with increased catalyst dosage and decreased initial concentration of AAB. It was also found that the removal efficiency of AAB significantly depend on pH value of solution. The results show that the degradation percent reaches the highest values with pH close to neutral. The data proved that removal percent of dye decreased when 6 watt lamp used instead of 12 watt lamp. The kinetic study confirmed that photocatalytic degradation of AAB dye follows a pseudo first order reaction rate.展开更多
Perylene tetracarboxylic diimide (PTCDI),widely used in organic photovoltaic devices,is an n-type semiconductor with strong absorption in the visible-light spectrum.There has been almost no study of the PTCDI-sensitiz...Perylene tetracarboxylic diimide (PTCDI),widely used in organic photovoltaic devices,is an n-type semiconductor with strong absorption in the visible-light spectrum.There has been almost no study of the PTCDI-sensitized TiO2 composite used to photocatalytically degrade pollutants.In this study,PTCDIand copper phthalocyanine tetrasulfonic acid (CuPcTs)-sensitized TiO2 composites were prepared using a hydrothermal method.The morphologies and structures of the two composites were characterized by X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,and fluorescence spectroscopy.The visible-light photocatalytic activities of the composites were evaluated using the degradation of rhodamine B as a model reaction.Results showed that dye-sensitized TiO2 samples had a wider absorption spectrum range and higher visiblelight photocatalytic activity compared to TiO2 samples.The double dye-sensitized (or co-sensitized) TiO2 composite with efficient electron collection exhibited higher photocatalytic activity than did the single dye-sensitized TiO2 composite.The electron transfer processes of single and double dye-sensitized TiO2 composites were illustrated according to band theory.展开更多
Low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O nanopowders(NPs)would determine their practical application in purifying wastewater.In this contribution,ZnO NPs were scala...Low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O nanopowders(NPs)would determine their practical application in purifying wastewater.In this contribution,ZnO NPs were scalably synthesized via the simple reaction of Zn powder with H_2O vapor in autoclave.The structural,morphological and optical properties of the samples were systematically characterized by X-ray diffraction,scanning electron microscopy,Fourier transform infrared spectra,transmission electron microscopy,Micro-Raman,photoluminescence,and ultraviolet-visible spectroscopy.The as-prepared Zn O NPs are composed of nanoparticles with 100–150 nm in diameter,and have a small Brunauer-Emmett-Teller surface area of 6.85 m^2/g.The formation of Zn O nanoparticles is relative to the peeling of H_2 release.Furthermore,the product has big strain-stress leading to the red-shift in the band gap of product,and shows a strong green emission centered at 515 nm revealing enough atomic defects in Zn O NPs.As a comparison with P25,the obtained dust gray Zn O NPs have a strong absorbance in the region of 200–700 nm,suggesting the wide wave-band utilization in sunlight.Based on the traits above,the Zn O NPs show excellent photocatalytic activity on the degradation of rhodamine B(Rh-B)under solar light irradiation,close to that under UV irradiation.Importantly,the Zn O NPs could be well recycled in water due to the quick sedimentation in themselves in solution.The low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O NPs endow themselves with promising application in purifying wastewater.展开更多
基金This work was supported by the National Natural Sci- ence Foundation of China （No.41373127） and the Liaoning Provincial Natural Science Foundation of China （No.2013020121）.
文摘In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 （EO20PO70EO20） as template. Scanning electron microscopy （SEM）, X-ray diffraction （XRD）, nitrogen adsorption-desorption measurements, and UV-visible spectroscopy （UV-Vis） were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange （MO） in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.
基金support from the National Natural Science Foundation of China(51602297 and U1510109)Major Research Project of Shandong Province(2016ZDJS11A04)+3 种基金Fundamental Research Funds for the Central Universities(201612007)Postdoctoral Innovation Program of Shandong Province(201603043)Australia Research Council(ARC)under the Project DP160104089Start-up Foundation for Advanced Talents of Qingdao University of Science and Technology(010022919)~~
文摘A heterojunction photocatalyst based on porous tubular g-C3N4 decorated with CdS nanoparticles was fabricated by a facile hydrothermal co-deposition method.The one-dimensional porous structure of g-C3N4 provides a higher specific surface area,enhanced light absorption,and better separation and transport performance of charge carriers along the longitudinal direction,all of which synergistically contribute to the superior photocatalytic activity observed.The significantly enhanced catalytic efficiency is also a benefit originating from the fast transfer of photogenerated electrons and holes between g-C3N4 and CdS through a built-in electric field,which was confirmed by investigating the morphology,structure,optical properties,electrochemical properties,and photocatalytic activities.Photocatalytic degradation of rhodamine B(RhB)and photocatalytic hydrogen evolution reaction were also carried out to investigate its photocatalytic performance.RhB can be degraded completely within 60 min,and the optimum H2 evolution rate of tubular g-C3N4/CdS composite is as high as 71.6μmol h^–1,which is about 16.3 times higher than that of pure bulk g-C3N4.The as-prepared nanostructure would be suitable for treating environmental pollutants as well as for water splitting.
基金supported by the National Natural Science Foundation of China(51672113,51602132)the Six Talent Peaks Project in Jiangsu Province(2015-XCL-026)+2 种基金the Natural Science Foundation of Jiangsu Province(BK20171299)the Training Project of Jiangsu University for Young Cadre Teachers(5521220009)the Youth Research Project of Jiangsu Health and Family Planning Commission in 2016(Q201609)~~
文摘Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most developed co-catalysts for semiconductor-based photocatalysis are inorganic materials;the employment of a specific organic molecule as a co-catalyst for photocatalytic hydrogen evolution and pollutant photodegradation is rare and still remains a challenging task. Herein, we report on the use of an organic molecule, oxamide (OA), as a novel co-catalyst to enhance electron- hole separation, photocatalytic H2 evolution, and dye degradation over TiO2 nanosheets. OA-modified TiO2 samples were prepared by a wet chemical route and demonstrated improved light absorption in the visible-light region and more efficient charge transport. The photocatalytic performance of H2 evolution from water splitting and rhodamine B (RhB) degradation for an optimal OA-modified TiO2 photocatalyst reached 2.37 mmol g^–1 h^–1 and 1.43 × 10^-2 min^-1, respectively, which were 2.4 and 3.8 times higher than those of pristine TiO2, respectively. A possible mechanism is proposed, in which the specific π-conjugated structure of OA is suggested to play a key role in the enhancement of the charge transfer and catalytic capability of TiO2. This work may provide advanced insight into the development of a variety of metal-free organic molecules as functional co-catalysts for improved solar-to-fuel conversion and environmental remediation.
基金Support Foundation of Fujian Education Bureau( K04026) Support Foundation of Fujian Development &Reformation Committee(04FJSD)
文摘Nanosize TiO 2,Y 2 O 3/TiO 2 particles were prepared by the sol-gel process. The structur e was characterized by means of XRD,TEM. The photoelectric properties of the nan oparticles were studied by PL. The thickness and the surface of the carboxymethy l cellulose film was measured by SEM. Based on a model reaction, the photocataly tic degradation of methylene blue with positive charge was investigated in TiO 2, Y2O3/TiO 2 nanopowder composite films irradiated by UV lamp. The results revealed that the degradation process belonged to the first-order k inetic reaction.
基金supported by the National Natural Science Foundation of China(21276088,U1507201)Natural Science Foundation of Guangdong Province(2014A030312009)China Postdoctoral Science Foundation(2018M640784)~~
文摘Molecular doping has been proven to be an effective approach to adjusting the electronic structure of polymeric carbon nitride(PCN)and thus improving its optical properties and photocatalytic activity.Herein,theobromine,a compound composed of an imidazole ring and a pyrimidine ring,was first copolymerized with urea to prepared doped PCN.Experimental investigations and theoretical calculations indicate that,a narrowing in band gap and a positive shift in valence band positon happened to the theobromine doped PCN,owing to the synergistic effect between the pyrimidine ring and the imidazole ring in the theobromine molecule.Moreover,it is shown that the doping with theobromine at a suitable mass fraction makes the obtained sample exhibit decreased photoluminescent emission,enhanced photocurrent density,and reduced charge-transport resistance.Consequently,an enhancement in the photocatalytic activity for water oxidation is found for the sample,which oxygen evolution rate is 4.43 times higher than that of the undoped PCN.This work sheds light on the choice of the molecular dopants for PCN to improve its photocatalytic performance.
文摘The photodegradation has been widely used in water and waste water treatment of all the methods like froth flotation coagulation etc., photodegradation appears to offer the best prospects for overall treatment of dyestuff effulent. Photodegradation of aniline blue and crystal violet dyes from aqueous solutions of their binary mixture was carried out using TiO2 as photocatalyst. By carrying out photodegradation, varying the experimental parameters, the optimum conditions required for maximum degradation was found out. The photodegradation of dye was carried out using different sources of energy like solar radiation and microwave radiation. The degradation studies were carried out at temperatures 25 ℃, 35 ℃ and 45 ℃ so as to calculate the rate constant and activation parameters. Both energy sources are equivalent in causing degradation in all respects except time and dose of photo catalyst. Time required is less for microwave than solar radiation, but dose of photo catalyst needed was high for microwave radiation. These results will be helpful in designing effluent treatment plants in industries.
文摘Semiconductor photocatalysts play an indispensable role in the photocatalytic process.Two-dimensional covalent organic frameworks(2D-COFs),as a kind of innovative photocatalyst,have garnered tremendous attention.Herein,we report an amide-linked 2D-COF(COF-JLU19)with outstanding photocatalytic performance in water,designed through a multi-synergistic approach.The synergistic effects of the high porosity,photoactive framework,high wettability,and stability of COF-JLU19 led to an unprecedented enhancement in the photocatalytic activity and recyclability in water upon illumination by visible light.More importantly,amide-linked 2D-COF based electrospinning membranes were prepared,which also exhibited superior photocatalytic activity for the degradation of Rhodamine B in water with sunlight.This study highlights the potential of the multi-synergistic approach as a universal rule for developing COF-based photocatalysts to address environmental and energy challenges.
文摘Zinc oxide （ZnO） has been used as heterogeneous catalyst for the degradation of Acid Alizarin Black S dye （AAB） in aqueous solutions using UV light irradiation. Experiments were conducted at various operating parameters. The operating parameters were amount of catalyst （50 rag, 100 mg and 150 mg）, initial concentration of dye （30 mg/L, 50 mg/L and 70 mg/L）, the pH of solution （2, 4, 6, 8, l0 and 12） and the UV light intensity （6 watt and 12 watt）. The progress of the degradation reaction was monitored spectrophotometrically. It was found that the degradation process of AAB solution was accelerated with increased catalyst dosage and decreased initial concentration of AAB. It was also found that the removal efficiency of AAB significantly depend on pH value of solution. The results show that the degradation percent reaches the highest values with pH close to neutral. The data proved that removal percent of dye decreased when 6 watt lamp used instead of 12 watt lamp. The kinetic study confirmed that photocatalytic degradation of AAB dye follows a pseudo first order reaction rate.
基金supported by the National Natural Science Foundation of China (20407002)National Basic Research Program of China (2002CB410802)Special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control
文摘Perylene tetracarboxylic diimide (PTCDI),widely used in organic photovoltaic devices,is an n-type semiconductor with strong absorption in the visible-light spectrum.There has been almost no study of the PTCDI-sensitized TiO2 composite used to photocatalytically degrade pollutants.In this study,PTCDIand copper phthalocyanine tetrasulfonic acid (CuPcTs)-sensitized TiO2 composites were prepared using a hydrothermal method.The morphologies and structures of the two composites were characterized by X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,and fluorescence spectroscopy.The visible-light photocatalytic activities of the composites were evaluated using the degradation of rhodamine B as a model reaction.Results showed that dye-sensitized TiO2 samples had a wider absorption spectrum range and higher visiblelight photocatalytic activity compared to TiO2 samples.The double dye-sensitized (or co-sensitized) TiO2 composite with efficient electron collection exhibited higher photocatalytic activity than did the single dye-sensitized TiO2 composite.The electron transfer processes of single and double dye-sensitized TiO2 composites were illustrated according to band theory.
基金the National Natural Science Foundation of China (21161016)the Natural Science Foundation of Jiangxi Province (20142BAB216013)+1 种基金Jiangxi Education Department Fund (KJLD14087, GJJ14714)Jiangxi Environmental Protection Department Fund ([2013]370)
文摘Low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O nanopowders(NPs)would determine their practical application in purifying wastewater.In this contribution,ZnO NPs were scalably synthesized via the simple reaction of Zn powder with H_2O vapor in autoclave.The structural,morphological and optical properties of the samples were systematically characterized by X-ray diffraction,scanning electron microscopy,Fourier transform infrared spectra,transmission electron microscopy,Micro-Raman,photoluminescence,and ultraviolet-visible spectroscopy.The as-prepared Zn O NPs are composed of nanoparticles with 100–150 nm in diameter,and have a small Brunauer-Emmett-Teller surface area of 6.85 m^2/g.The formation of Zn O nanoparticles is relative to the peeling of H_2 release.Furthermore,the product has big strain-stress leading to the red-shift in the band gap of product,and shows a strong green emission centered at 515 nm revealing enough atomic defects in Zn O NPs.As a comparison with P25,the obtained dust gray Zn O NPs have a strong absorbance in the region of 200–700 nm,suggesting the wide wave-band utilization in sunlight.Based on the traits above,the Zn O NPs show excellent photocatalytic activity on the degradation of rhodamine B(Rh-B)under solar light irradiation,close to that under UV irradiation.Importantly,the Zn O NPs could be well recycled in water due to the quick sedimentation in themselves in solution.The low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O NPs endow themselves with promising application in purifying wastewater.
