In this study,the Cr2O3/C@TiO2 composite was synthesized via the calcination of yolk–shell MIL-101@TiO2.The composite presented core–shell structure,where Cr-doped TiO2 and Cr2O3/C were the shell and core,respective...In this study,the Cr2O3/C@TiO2 composite was synthesized via the calcination of yolk–shell MIL-101@TiO2.The composite presented core–shell structure,where Cr-doped TiO2 and Cr2O3/C were the shell and core,respectively.The introduction of Cr^3+and Cr2O3/C,which were derived from the calcination of MIL-101,in the composite enhanced its visible light absorbing ability and lowered the recombination rate of the photogenerated electrons and holes.The large surface area of the Cr2O3/C@TiO2 composite provided numerous active sites for the photoreduction reaction.Consequently,the photocatalytic performance of the composite for the production of H2 was better than that of pure TiO2.Under the irradiation of a 300 W Xe arc lamp,the H2 production rate of the Cr2O3/C@TiO2 composite that was calcined at 500°C was 446μmol h−1 g−1,which was approximately four times higher than that of pristine TiO2 nanoparticles.Moreover,the composite exhibited the high H2 production rate of 25.5μmol h−1 g−1 under visible light irradiation(λ>420 nm).The high photocatalytic performance of Cr2O3/C@TiO2 could be attributed to its wide visible light photoresponse range and efficient separation of photogenerated electrons and holes.This paper offers some insights into the design of a novel efficient photocatalyst for water-splitting applications.展开更多
TiO2-WO3 hybrid photocatalysts were prepared using wet-chemical technique, and their energy storage performance was characterized by electrochemical galvanostatic method. TiO2 powder was coupled with WO3 powder, which...TiO2-WO3 hybrid photocatalysts were prepared using wet-chemical technique, and their energy storage performance was characterized by electrochemical galvanostatic method. TiO2 powder was coupled with WO3 powder, which was used as electron pool and the reductive energy could be stored in. As a result, the prepared TiO2-WO3 had good energy storage ability while pure TiO2 showed no capacity and pure WO3 showed quite low performance. The energy storage ability was affected by the crystal structure of WO3 and calcination temperature. The photocatalyst had better capacity when WO3 had low degree of crystallinity, since its loose structure made it easier for electrons and cations to pass through. The photocatalytic energy storage performance was also affected by the molar ratio of TiO2 to WO3. Energy storage capacity was significantly dependent on the composition, reaching the maximum value at TiO2/WO3 1:1 (mol/mol).展开更多
According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equatio...According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.展开更多
Photodegradation has emerged as an environmentally friendly method of decomposing harmful dyes in wastewater. In this study, core-shell Fe3O4/SiO2/ TiO2 nanospheres with magnetic cores were obtained from synthesised m...Photodegradation has emerged as an environmentally friendly method of decomposing harmful dyes in wastewater. In this study, core-shell Fe3O4/SiO2/ TiO2 nanospheres with magnetic cores were obtained from synthesised magnetic Fe3O4 nanoparticles through the precipitation method, the surface of the magnetic Fe3O4 nanoparticles was coated with a silica (SiO2) layer by hydrolysis of tetramethoxysilane (TMOS) as a silica source, and finally, Fe3O4/SiO2 nanospheres were coated with titanium (TiO2) layer using tetrabutyltitanate (TBT) as a precursor through the sol-gel process. The morphology and structure of the prepared materials were characterised by X-ray diffraction (XRD) analysis, scanning electron microscopy (SEM), X-ray energy dispersive spectrometry (EDAX), Fourier transform infrared spectroscopy (FT-IR), and atomic force microscopy (AFM). The photocatalytic activities of the prepared core-shell nanospheres were studied using binary azo dyes, namely methyl orange (anionic dye, MO) and methylene blue (cationic dye, MB) in aqueous solution under UV light irradiation (365 nm), and UV-Vis spectrophotometer was utilised to monitor the amount of each dye in the mixture. It was found that 90.2% and 100% of binary MO and MB were removed for 5 h, respectively. The results revealed that the efficiency of the photocatalytic degradation of the core-shell nanospheres was not degreased after five runs that can be used as recyclable photocatalysts. The results show that the performance of the prepared core-shell nanospheres was better than that of commercial TiO2 nanoparticles. Moreover, the magnetic separation properties of the core-shell Fe3O4/SiO2/TiO2 nanospheres can enable the prepared materials to have wider application prospects.展开更多
Conventional titanium dioxide(TiO2)photocatalyst could absorb only ultraviolet light due to its wide bandgap.In this paper,black TiO2 with narrow bandgap was prepared by introducing oxygen vacancies.Meanwhile.nitrogen...Conventional titanium dioxide(TiO2)photocatalyst could absorb only ultraviolet light due to its wide bandgap.In this paper,black TiO2 with narrow bandgap was prepared by introducing oxygen vacancies.Meanwhile.nitrogen(N)and sulfur(S)elements were doped to further broaden the visible light response range of TiOx(NS-BT),and then heterostructured N.S-doped black TiOz/g-C3Na(CN/NS-BT)was successfully constructed by easily accessible route.The formation of CN/NS-BT heteroiunction structure increased the generation and separation efficiency of photogenerated electron-hole pairs,as well as accelerated the transfer rate of the carriers.The as-prepared CN/NS-BT exhibited excellent photocatalytic performance towards the degradation of Rhodamine B(RhB)under visible light irradiation with satisfactory stability.The apparent reaction rate constant of CN/NS-BT(0.0079)was 15.8-fold higher than that of commercial P25(0.0005),The structure,morphology,chemical composition and optical properties of the as-prepared CN/NS-BT were characterized by various analytical methods,and possible photocatalytic enhancement mechanism was proposed.Overall,CN/NS-BT composites look promising as photocatalytic material for future environmental treatment.展开更多
Using low-cost precipitated silica(SiO2) as the carrier,a ternary SiO2-TiO2/g-C3N4 composite photocatalyst was prepared via the sol-gel method associated with a wet-grinding process.The asprepared composite exhibits p...Using low-cost precipitated silica(SiO2) as the carrier,a ternary SiO2-TiO2/g-C3N4 composite photocatalyst was prepared via the sol-gel method associated with a wet-grinding process.The asprepared composite exhibits photocatalytic hydrogen production and pollutant degradation performance under solar-like irradiation.The effect of SiO2 carrier on the properties of the heterostructure between TiO2 and g-C3N4(CN) was systematically studied.It is found that SiO2 has important effects on promoting the interaction between TiO2 and CN.The particle size of TiO2 and CN was obviously reduced during the calcination process due to the effects of SiO2.Especially,the TiO2 particles exhibit monodispersed state with particle size below 10 nm(quantum dots),resulting in the improvement of the contact area and the interaction betweenTiO2 and CN,and leading to the formation of efficient TiO2/CN Zscheme heterostructure in SiO2-TiO2/CN.Besides,the introduction of SiO2 can increase the specific surface area and light absorption of SiO2-TiO2/CN,further promoting the photocatalytic reaction.As expected,the optimum SiO2-TiO2/CN composite exhibits 12.3,3.1 and 2.9 times higher photocatalytic hydrogen production rate than that of SiO2-TiO2,CN and TiO2/CN under solar-like irradiation,while the photocatalytic active component in SiO2-TiO2/CN is only about 60 wt%.Moreover,the rhodamine B degradation rate of SiO2-TiO2/CN is also higher than that of SiO2-TiO2,CN and TiO2/CN.展开更多
Photocatalysis is considered to be a clean, green and efficient method to purify water. In this report, we first developed a highly efficient ultrafine TiO2 nanorods/g-C3N4 nanosheets (TiO2 NR/CN NS) composites via ...Photocatalysis is considered to be a clean, green and efficient method to purify water. In this report, we first developed a highly efficient ultrafine TiO2 nanorods/g-C3N4 nanosheets (TiO2 NR/CN NS) composites via a simple hydrothermal method. Tiny TiO2 nanorods (diameter: ~1.5 nm and length: ~8.3 nm) were first loaded in situ on the CN NS by adding graphitic carbon nitride (g-C3N4) to the reaction solution. The TiO2 NR/CN NS composites present high charge separation efficiency and broader light absorbance than P25 TiO2. Furthermore, we illustrate that the TiO2 NR/CN NS catalyst possesses high performance for the photocatalytic degradation of the common and stubborn pollutants in water, such as the rhodamine B (RhB) dye and phenol. Under visible light (λ 〉 420 nm) irradiation, the apparent rate of the TiO2 NR/CN NR is 172 and 41 times higher than that of the P25 TiO2 and TiO2 NR, respectively. Additionally, we speculated that the heterojunction formed between TiO2 NR and CN NS, which is the basis for the experiments we have designed and the corresponding results. We demonstrated that reactive oxidative species such as superoxide anion radical and holes play critical roles in the degradation, and the hydroxyl radical contributes nothing to the degradation.展开更多
A nanoheterojunction composite photocatalyst Bi2O3/TiO2 working under visible-light (λ≥ 420 nm) was prepared by combining two semiconductors Bi2O3 and TiO2 varying the Bi2O3/TiO2 molar ratio. Maleic acid was emplo...A nanoheterojunction composite photocatalyst Bi2O3/TiO2 working under visible-light (λ≥ 420 nm) was prepared by combining two semiconductors Bi2O3 and TiO2 varying the Bi2O3/TiO2 molar ratio. Maleic acid was employed as an organic binder to unite Bi2O3 and TiO2 nanoparticles. The SEM, TEM, XRD and diffuse reflectance spectra were utilized to characterize the prepared Bi2O3/TiO2 nanoheterojunction. The nanocomposite exhibited unusual high photocatalytic activity in decomposing 2-propanol in gas phase and phenol in aqueous phase and, evolution of CO2 under visible light irradiation while the end members exhibited low photocatalytic activity. The composite was optimized to 5 mol% Bi2O3/TiO2. The remarkable high photocatalytic efficiency originates from the unique relative energy band position of Bi2O3 and TiO2 as well as the absorption of visible light by Bi2O3.展开更多
A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles(NPs)were produced through single-step pyrolysis of FeCl_3–Ti(OBu)_4 laden agar biomass under NH_3 environment...A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles(NPs)were produced through single-step pyrolysis of FeCl_3–Ti(OBu)_4 laden agar biomass under NH_3 environment.The physiochemical properties of composites were characterized thoroughly.It has found that heating temperature and N-doping through NH_3-ambiance pyrolysis significantly influence the visible-light sensitivity and bandgap energy of composites.The catalytic activities of composites were measured by degradation of Methylene Blue(MB)in the presence or absence of H_2O_2 and visible-light irradiation.Our best catalyst(N–TiO_2–Fe_3O_4-biochar)exhibits rapid and high MB removal competency(99.99%)via synergism of adsorption,photodegradation,and Fenton-like reaction.Continuous production of O_2U^-and UOH radicles performs MB degradation and mineralization,confirmed by scavenging experiments and degradation product analysis.The local trap state Ti^(3+),Fe_3O_4,and N-carbon of the catalyst acted as active sites.It has suggested that the Ti^(3+)and N-doped dense carbon layer improve charge separation and shuttle that prolonged photo-Fenton like reaction.Moreover,the catalyst is highly stable,collectible,and recyclable up to 5 cycles with high MB degradation efficiency.This work provides a new insight into the synthesis of highly visible-light sensitized biocharsupported photocatalyst through NH_3-ambiance pyrolysis of NPs-laden biomass.展开更多
文摘In this study,the Cr2O3/C@TiO2 composite was synthesized via the calcination of yolk–shell MIL-101@TiO2.The composite presented core–shell structure,where Cr-doped TiO2 and Cr2O3/C were the shell and core,respectively.The introduction of Cr^3+and Cr2O3/C,which were derived from the calcination of MIL-101,in the composite enhanced its visible light absorbing ability and lowered the recombination rate of the photogenerated electrons and holes.The large surface area of the Cr2O3/C@TiO2 composite provided numerous active sites for the photoreduction reaction.Consequently,the photocatalytic performance of the composite for the production of H2 was better than that of pure TiO2.Under the irradiation of a 300 W Xe arc lamp,the H2 production rate of the Cr2O3/C@TiO2 composite that was calcined at 500°C was 446μmol h−1 g−1,which was approximately four times higher than that of pristine TiO2 nanoparticles.Moreover,the composite exhibited the high H2 production rate of 25.5μmol h−1 g−1 under visible light irradiation(λ>420 nm).The high photocatalytic performance of Cr2O3/C@TiO2 could be attributed to its wide visible light photoresponse range and efficient separation of photogenerated electrons and holes.This paper offers some insights into the design of a novel efficient photocatalyst for water-splitting applications.
基金supported by the National Basic Research Program of China (973 Program) (No. 2007CB613305)the National High Technology Research and Development Program of China (863 Program) (No. 2007AA061405)the Special Foundation of Nanometer Technology(No. 0752nm005) from Shanghai Municipal Science and Technology Commission (STCSM) of China
文摘TiO2-WO3 hybrid photocatalysts were prepared using wet-chemical technique, and their energy storage performance was characterized by electrochemical galvanostatic method. TiO2 powder was coupled with WO3 powder, which was used as electron pool and the reductive energy could be stored in. As a result, the prepared TiO2-WO3 had good energy storage ability while pure TiO2 showed no capacity and pure WO3 showed quite low performance. The energy storage ability was affected by the crystal structure of WO3 and calcination temperature. The photocatalyst had better capacity when WO3 had low degree of crystallinity, since its loose structure made it easier for electrons and cations to pass through. The photocatalytic energy storage performance was also affected by the molar ratio of TiO2 to WO3. Energy storage capacity was significantly dependent on the composition, reaching the maximum value at TiO2/WO3 1:1 (mol/mol).
基金Sponsored by the National Natural Science Foundation of China (Grant No. 51078100)the National Creative Research Groups granted by NSFC(Grant No. 50821002)+1 种基金Excellent Youth Foundation of Heilongjiang Scientific Committee(Grant No. JC2010-03)State Key Laboratory of Urban Water Resource and Environment(Grant No. 2010DX11)
文摘According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.
文摘Photodegradation has emerged as an environmentally friendly method of decomposing harmful dyes in wastewater. In this study, core-shell Fe3O4/SiO2/ TiO2 nanospheres with magnetic cores were obtained from synthesised magnetic Fe3O4 nanoparticles through the precipitation method, the surface of the magnetic Fe3O4 nanoparticles was coated with a silica (SiO2) layer by hydrolysis of tetramethoxysilane (TMOS) as a silica source, and finally, Fe3O4/SiO2 nanospheres were coated with titanium (TiO2) layer using tetrabutyltitanate (TBT) as a precursor through the sol-gel process. The morphology and structure of the prepared materials were characterised by X-ray diffraction (XRD) analysis, scanning electron microscopy (SEM), X-ray energy dispersive spectrometry (EDAX), Fourier transform infrared spectroscopy (FT-IR), and atomic force microscopy (AFM). The photocatalytic activities of the prepared core-shell nanospheres were studied using binary azo dyes, namely methyl orange (anionic dye, MO) and methylene blue (cationic dye, MB) in aqueous solution under UV light irradiation (365 nm), and UV-Vis spectrophotometer was utilised to monitor the amount of each dye in the mixture. It was found that 90.2% and 100% of binary MO and MB were removed for 5 h, respectively. The results revealed that the efficiency of the photocatalytic degradation of the core-shell nanospheres was not degreased after five runs that can be used as recyclable photocatalysts. The results show that the performance of the prepared core-shell nanospheres was better than that of commercial TiO2 nanoparticles. Moreover, the magnetic separation properties of the core-shell Fe3O4/SiO2/TiO2 nanospheres can enable the prepared materials to have wider application prospects.
基金Supported by the National Natural Science Foundation of China(No.51472106)the Natural Science Foundation of Jilin Province,China(Nos.20180101065JC,20190201129JC)+1 种基金the International Science and Technology Cooperation Project of Jilit Province,China(No.20200801059GH)the Industrial Technology Research and Development Project of Development and Reform Commission of Jilin Province,China(Nos.2019C045-3,2019C42-6)。
文摘Conventional titanium dioxide(TiO2)photocatalyst could absorb only ultraviolet light due to its wide bandgap.In this paper,black TiO2 with narrow bandgap was prepared by introducing oxygen vacancies.Meanwhile.nitrogen(N)and sulfur(S)elements were doped to further broaden the visible light response range of TiOx(NS-BT),and then heterostructured N.S-doped black TiOz/g-C3Na(CN/NS-BT)was successfully constructed by easily accessible route.The formation of CN/NS-BT heteroiunction structure increased the generation and separation efficiency of photogenerated electron-hole pairs,as well as accelerated the transfer rate of the carriers.The as-prepared CN/NS-BT exhibited excellent photocatalytic performance towards the degradation of Rhodamine B(RhB)under visible light irradiation with satisfactory stability.The apparent reaction rate constant of CN/NS-BT(0.0079)was 15.8-fold higher than that of commercial P25(0.0005),The structure,morphology,chemical composition and optical properties of the as-prepared CN/NS-BT were characterized by various analytical methods,and possible photocatalytic enhancement mechanism was proposed.Overall,CN/NS-BT composites look promising as photocatalytic material for future environmental treatment.
基金partly supported by the National Natural Science Foundation of China(Nos.21577132,21978276)。
文摘Using low-cost precipitated silica(SiO2) as the carrier,a ternary SiO2-TiO2/g-C3N4 composite photocatalyst was prepared via the sol-gel method associated with a wet-grinding process.The asprepared composite exhibits photocatalytic hydrogen production and pollutant degradation performance under solar-like irradiation.The effect of SiO2 carrier on the properties of the heterostructure between TiO2 and g-C3N4(CN) was systematically studied.It is found that SiO2 has important effects on promoting the interaction between TiO2 and CN.The particle size of TiO2 and CN was obviously reduced during the calcination process due to the effects of SiO2.Especially,the TiO2 particles exhibit monodispersed state with particle size below 10 nm(quantum dots),resulting in the improvement of the contact area and the interaction betweenTiO2 and CN,and leading to the formation of efficient TiO2/CN Zscheme heterostructure in SiO2-TiO2/CN.Besides,the introduction of SiO2 can increase the specific surface area and light absorption of SiO2-TiO2/CN,further promoting the photocatalytic reaction.As expected,the optimum SiO2-TiO2/CN composite exhibits 12.3,3.1 and 2.9 times higher photocatalytic hydrogen production rate than that of SiO2-TiO2,CN and TiO2/CN under solar-like irradiation,while the photocatalytic active component in SiO2-TiO2/CN is only about 60 wt%.Moreover,the rhodamine B degradation rate of SiO2-TiO2/CN is also higher than that of SiO2-TiO2,CN and TiO2/CN.
基金supported by the Beijing Municipal High Level Innovative Team Building Program(IDHT20180504)the National Natural Science Foundation of China(21671011)+4 种基金Beijing High Talent ProgramBeijing Natural Science Foundation(KZ201710005002)the Large-scale Instrument and Equipment Platform of Beijing University of TechnologyChina Postdoctoral Science FoundationBeijing Postdoctoral Research Foundation
文摘Photocatalysis is considered to be a clean, green and efficient method to purify water. In this report, we first developed a highly efficient ultrafine TiO2 nanorods/g-C3N4 nanosheets (TiO2 NR/CN NS) composites via a simple hydrothermal method. Tiny TiO2 nanorods (diameter: ~1.5 nm and length: ~8.3 nm) were first loaded in situ on the CN NS by adding graphitic carbon nitride (g-C3N4) to the reaction solution. The TiO2 NR/CN NS composites present high charge separation efficiency and broader light absorbance than P25 TiO2. Furthermore, we illustrate that the TiO2 NR/CN NS catalyst possesses high performance for the photocatalytic degradation of the common and stubborn pollutants in water, such as the rhodamine B (RhB) dye and phenol. Under visible light (λ 〉 420 nm) irradiation, the apparent rate of the TiO2 NR/CN NR is 172 and 41 times higher than that of the P25 TiO2 and TiO2 NR, respectively. Additionally, we speculated that the heterojunction formed between TiO2 NR and CN NS, which is the basis for the experiments we have designed and the corresponding results. We demonstrated that reactive oxidative species such as superoxide anion radical and holes play critical roles in the degradation, and the hydroxyl radical contributes nothing to the degradation.
文摘A nanoheterojunction composite photocatalyst Bi2O3/TiO2 working under visible-light (λ≥ 420 nm) was prepared by combining two semiconductors Bi2O3 and TiO2 varying the Bi2O3/TiO2 molar ratio. Maleic acid was employed as an organic binder to unite Bi2O3 and TiO2 nanoparticles. The SEM, TEM, XRD and diffuse reflectance spectra were utilized to characterize the prepared Bi2O3/TiO2 nanoheterojunction. The nanocomposite exhibited unusual high photocatalytic activity in decomposing 2-propanol in gas phase and phenol in aqueous phase and, evolution of CO2 under visible light irradiation while the end members exhibited low photocatalytic activity. The composite was optimized to 5 mol% Bi2O3/TiO2. The remarkable high photocatalytic efficiency originates from the unique relative energy band position of Bi2O3 and TiO2 as well as the absorption of visible light by Bi2O3.
基金supported by the National Basic Research Program of China (973 Program, 2014CB238903)the National Natural Science Foundation of China (Nos. 41672144, 41173032, and 41373110)
文摘A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles(NPs)were produced through single-step pyrolysis of FeCl_3–Ti(OBu)_4 laden agar biomass under NH_3 environment.The physiochemical properties of composites were characterized thoroughly.It has found that heating temperature and N-doping through NH_3-ambiance pyrolysis significantly influence the visible-light sensitivity and bandgap energy of composites.The catalytic activities of composites were measured by degradation of Methylene Blue(MB)in the presence or absence of H_2O_2 and visible-light irradiation.Our best catalyst(N–TiO_2–Fe_3O_4-biochar)exhibits rapid and high MB removal competency(99.99%)via synergism of adsorption,photodegradation,and Fenton-like reaction.Continuous production of O_2U^-and UOH radicles performs MB degradation and mineralization,confirmed by scavenging experiments and degradation product analysis.The local trap state Ti^(3+),Fe_3O_4,and N-carbon of the catalyst acted as active sites.It has suggested that the Ti^(3+)and N-doped dense carbon layer improve charge separation and shuttle that prolonged photo-Fenton like reaction.Moreover,the catalyst is highly stable,collectible,and recyclable up to 5 cycles with high MB degradation efficiency.This work provides a new insight into the synthesis of highly visible-light sensitized biocharsupported photocatalyst through NH_3-ambiance pyrolysis of NPs-laden biomass.