Photocatalytic processes are efficient methods to solve water contamination problems,especially considering dyeing wastewater disposal.However,high-efficiency photocatalysts are usually very expensive and have the ris...Photocatalytic processes are efficient methods to solve water contamination problems,especially considering dyeing wastewater disposal.However,high-efficiency photocatalysts are usually very expensive and have the risk of heavy metal pollution.Recently,an iron oxides@hydrothermal carbonation carbon(HTCC)heterogeneous catalyst was prepared by our group through co-hydrothermal treatment of carbohydrates and zinc extraction tailings of converter dust.Herein,the catalytic performance of the iron oxides@HTCC was verified by a nonbiodegradable dye,methylene blue(MB),and the catalytic mechanism was deduced from theoretical simulations and spectroscopic measurements.The iron oxides@HTCC showed an excellent synergy between photocatalysis and Fenton-like reactions.Under visible-light illumination,the iron oxides@HTCC could be excited to generate electrons and holes,reacting with H_(2)O_(2)to produce·OH radicals to oxidize and decompose organic pollutants.The removal efficiency of methylene blue over iron oxides@HTCC at 140 min was 2.86 times that of HTCC.The enhanced catalytic performance was attributed to the advantages of iron oxides modification:(1)promoting the excitation induced by photons;(2)improving the charge transfer.Furthermore,the iron oxides@HTCC showed high catalytic activity in a wide pH value range of 2.3-10.4,and the MB removal efficiency remained higher than 95% after the iron oxides@HTCC was recycled 4 times.The magnetically recyclable iron oxides@HTCC may provide a solution for the treatment of wastewater from the textile industry.展开更多
The photocatalytic performance of mechano-thermally synthesized Fe/FeS nanostructures formed from micron-sized starting materials was compared with that of a thermally synthesized nanostructure with nano-sized precurs...The photocatalytic performance of mechano-thermally synthesized Fe/FeS nanostructures formed from micron-sized starting materials was compared with that of a thermally synthesized nanostructure with nano-sized precursors in this paper. The properties of as-synthesized materials were studied by X-ray diffraction(XRD), transmission electron microscopy(TEM), vibrating sample magnetometry(VSM), diffuse reflectance spectroscopy(DRS), and ultraviolet–visible(UV-Vis) spectroscopy. The effects of irradiation time, methylene blue(MB) concentration, catalyst dosage, and p H value upon the degradation of MB were studied. Magnetic properties of the samples showed that both as-synthesized Fe/FeS photocatalysts are magnetically recoverable, eliminating the need for conventional filtration steps. Degradation of 5 ppm of the MB solution by mechano-thermally synthesized Fe/FeS with a photocatalyst dosage of 1 kg/m^3 at pH 11 can reach 96% after 12 ks irradiation under visible light. The photocatalytic efficiency is higher in alkaline solution. The kinetics of photocatalytic degradation in both samples is controlled by a first-order reaction. However, the rate-constant value in the thermally synthesized Fe/FeS photocatalyst sample is only 1.5 times greater than that of the mechano-thermally synthesized one.展开更多
Porous S-doped bismuth vanadate with an olive-like morphology and its supported iron oxide (y wt.% FeOx/BiVO4-δS0.08, y = 0.06, 0.76, and 1.40) photocatalysts were fabricated using the dodecylamine-assisted alcohol...Porous S-doped bismuth vanadate with an olive-like morphology and its supported iron oxide (y wt.% FeOx/BiVO4-δS0.08, y = 0.06, 0.76, and 1.40) photocatalysts were fabricated using the dodecylamine-assisted alcohol-hydrothermal and incipient wetness impregnation methods, respectively. It is shown that the y wt.% FeOx/BiVO4-δS0.08 photocatalysts contained a monoclinic scheetlite BiVO4 phase with a porous olive-like morphology, a surface area of 8.8-9.2 m^2/g, and a bandgap energy of 2.38-2.42 eV. There was co-presence of surface Bi^5+, Bi^3+, V^5+, V^3+, Fe^3+, and Fe^2+ species in y wt.% FeOx/BiVO4-δS0.08. The 1.40 wt.% FeOx/BiVO4-δS0.08 sample performed the best for Methylene Blue degradation under visible-light illumination. The photocatalytic mechanism was also discussed. We believe that the sulfur and FeOx co-doping, higher oxygen adspecies concentration, and lower baudgap energy were responsible for the excellent visible-light-driven catalytic activity of 1.40 wt.% FeOx/BiVO4-δS0.08.展开更多
Metallic glasses have recently attracted great attention in terms of degrading dyes and other organic pollutants as an environmentally friendly material for wastewater remediation.Herein,we report a new type of amorph...Metallic glasses have recently attracted great attention in terms of degrading dyes and other organic pollutants as an environmentally friendly material for wastewater remediation.Herein,we report a new type of amorphous catalyst Fe_(41)Co_(7)Cr_(15)Mo_(14)C_(15)B_(6)Y_(2) hollow balls.Results demonstrate that the catalyst can still completely decolorize the 20 mg/L methylene blue(MB)solution after reused for 50 times under conditions of pH=5,catalyst content 0.5 g/L,and temperature 80°C.The catalyst is easily broken during degradation,so the inner surface also provides additional active sites.The Fe_(41)Co_(7)Cr_(15)Mo_(14)C_(15)B_(6)Y_(2) amorphous alloy hollow balls were characterized by energy dispersive X-ray specroscopy(EDS),scanning electron microscopy(SEM)and X-ray photoelectron spectroscopy(XPS),respectively.The elements in the catalytic system have a synergistic catalytic effect.Redox cycle Fe^(2+)/Fe^(3+),Co^(2+)/Co^(3+)and Mo^(4+)/Mo^(6+) promote mutual conversion and accelerate the catalytic process of their reaction with H_(2)O_(2),forming a self-stable redox cycle process.Among them,Fe^(2+)promotes the conversion of Co^(3+)to Co^(2+),and Mo^(4+) promotes the conversion of Fe^(3+)to Fe^(2+),mainly Fe^(2+)and Co^(2+)react with H_(2)O_(2) to generate•OH.Mo and Cr elements form MoO_(2) and Cr_(2)O_(3) plasma compounds on the surface,which act as a protective film to make the catalyst more stable and be repeated used more frequently.展开更多
We report the fabrication and photocatalytic property of a composite of C/CaFe2O4nanorods(NRs)in an effort to reveal the influence of carbon modification.It is demonstrated that the photocatalytic degradation activity...We report the fabrication and photocatalytic property of a composite of C/CaFe2O4nanorods(NRs)in an effort to reveal the influence of carbon modification.It is demonstrated that the photocatalytic degradation activity is dependent on the mass ratio of C to CaFe2O4.The optimal carbon content is determined to be58wt%to yield a methylene blue(MB)degradation rate of0.0058min.1,which is4.8times higher than that of the pristine CaFe2O4NRs.The decoration of carbon on the surface of CaFe2O4NRs improves its adsorption capacity of the MB dye,which is specifically adsorbed on the surface as a monolayer according to the adsorption isotherm analysis.The trapping experiments of the reactive species indicate that superoxide radicals(.O2)are the main active species responsible for the removal of MB under visible‐light irradiation.Overall,the unique feature of carbon coating enables the efficient separation and transfer of photogenerated electrons and holes,strengthens the adsorption capacity of MB,and improves the light harvesting capability,hence enhancing the overall photocatalytic degradation of MB.展开更多
Environmental pollution jeopardizes our existence. For this purpose, research is moving more and more towards the search for economic means and green chemistry to curb this phenomenon. In this context, the photocataly...Environmental pollution jeopardizes our existence. For this purpose, research is moving more and more towards the search for economic means and green chemistry to curb this phenomenon. In this context, the photocatalytic activity of zinc sulfide nanoparticles (ZnS NPs) and nanostructured composite ZnS/carbon dots (ZnS/CDs) was evaluated after their synthesis. The results of X-ray diffraction (XRD) analysis indicate that the crystal structure of ZnS/CDs is identical to that of the cubic phase structure of ZnS, revealing that the cubic phase structure of ZnS was not altered in the presence of CDs. Indeed, there is no additional peak in the crystal structure of ZnS/CDs, revealing that the crystalline structure of ZnS is not responsible for the difference in photocatalytic activity between ZnS/CDs and ZnS NPs. Moreover, analysis performed by transmission electron microscopy (TEM) shows aggregation of the synthesized ZnS and ZnS/CDs nanoparticles with an average size estimated around 10 nm and 12 nm, respectively. In addition, the reflectance study in the visible range shows a reduction in the sunlight reflection intensity using ZnS/CDs compared to the capability of ZnS NPs. Photocatalytic degradation tests reveal that ZnS/CDs have the best methylene blue (MB) degradation rate. Indeed, under the optimal conditions, the photocatalytic activity can reach 100% efficiency within 100 min and 240 min of sunlight exposure for the degradation of 7.5 mg/L MB using ZnS/CDs and ZnS, respectively. This improvement in photocatalytic activity of ZnS/CDs may be due to the presence of CDs which can permit to undergo a reduction of reflection properties of ZnS NPs in the visible range. These results show that CDs can play a key role in enhancing the photocatalytic activity of ZnS, and suggest that ZnS/CDs could be used as eco-friendly composite materials for the degradation of organic pollutants of similar structures in the aquatic environment under solar irradiation.展开更多
基金financially supported by the National Natural Science Foundation of China(No.52074035)the Fundamental Research Funds for the Central Universities,China(No.00007720)the National Key Research and Development Program of China(No.2020YFC1910000)。
文摘Photocatalytic processes are efficient methods to solve water contamination problems,especially considering dyeing wastewater disposal.However,high-efficiency photocatalysts are usually very expensive and have the risk of heavy metal pollution.Recently,an iron oxides@hydrothermal carbonation carbon(HTCC)heterogeneous catalyst was prepared by our group through co-hydrothermal treatment of carbohydrates and zinc extraction tailings of converter dust.Herein,the catalytic performance of the iron oxides@HTCC was verified by a nonbiodegradable dye,methylene blue(MB),and the catalytic mechanism was deduced from theoretical simulations and spectroscopic measurements.The iron oxides@HTCC showed an excellent synergy between photocatalysis and Fenton-like reactions.Under visible-light illumination,the iron oxides@HTCC could be excited to generate electrons and holes,reacting with H_(2)O_(2)to produce·OH radicals to oxidize and decompose organic pollutants.The removal efficiency of methylene blue over iron oxides@HTCC at 140 min was 2.86 times that of HTCC.The enhanced catalytic performance was attributed to the advantages of iron oxides modification:(1)promoting the excitation induced by photons;(2)improving the charge transfer.Furthermore,the iron oxides@HTCC showed high catalytic activity in a wide pH value range of 2.3-10.4,and the MB removal efficiency remained higher than 95% after the iron oxides@HTCC was recycled 4 times.The magnetically recyclable iron oxides@HTCC may provide a solution for the treatment of wastewater from the textile industry.
基金financial support of University of Tehran for this researchfinancial support of Iran Nanotechnology Initiative Council
文摘The photocatalytic performance of mechano-thermally synthesized Fe/FeS nanostructures formed from micron-sized starting materials was compared with that of a thermally synthesized nanostructure with nano-sized precursors in this paper. The properties of as-synthesized materials were studied by X-ray diffraction(XRD), transmission electron microscopy(TEM), vibrating sample magnetometry(VSM), diffuse reflectance spectroscopy(DRS), and ultraviolet–visible(UV-Vis) spectroscopy. The effects of irradiation time, methylene blue(MB) concentration, catalyst dosage, and p H value upon the degradation of MB were studied. Magnetic properties of the samples showed that both as-synthesized Fe/FeS photocatalysts are magnetically recoverable, eliminating the need for conventional filtration steps. Degradation of 5 ppm of the MB solution by mechano-thermally synthesized Fe/FeS with a photocatalyst dosage of 1 kg/m^3 at pH 11 can reach 96% after 12 ks irradiation under visible light. The photocatalytic efficiency is higher in alkaline solution. The kinetics of photocatalytic degradation in both samples is controlled by a first-order reaction. However, the rate-constant value in the thermally synthesized Fe/FeS photocatalyst sample is only 1.5 times greater than that of the mechano-thermally synthesized one.
基金supported by the National Natural Science Foundation of China(No.21077007)the Natural Science Foundation of Beijing Municipality(No.2102008)+3 种基金the Discipline and Postgraduate Education Foundation(No.PXM2013 014204 07 000261,005000542513551)the Creative Research Foundation of Beijing University of Technology(No.00500054R4003,005000543111501)the Funding Project for Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality(No.PHR201007105,PHR201107104)the Hong Kong Baptist University for financial support(No.FRG2/09-10/023)
文摘Porous S-doped bismuth vanadate with an olive-like morphology and its supported iron oxide (y wt.% FeOx/BiVO4-δS0.08, y = 0.06, 0.76, and 1.40) photocatalysts were fabricated using the dodecylamine-assisted alcohol-hydrothermal and incipient wetness impregnation methods, respectively. It is shown that the y wt.% FeOx/BiVO4-δS0.08 photocatalysts contained a monoclinic scheetlite BiVO4 phase with a porous olive-like morphology, a surface area of 8.8-9.2 m^2/g, and a bandgap energy of 2.38-2.42 eV. There was co-presence of surface Bi^5+, Bi^3+, V^5+, V^3+, Fe^3+, and Fe^2+ species in y wt.% FeOx/BiVO4-δS0.08. The 1.40 wt.% FeOx/BiVO4-δS0.08 sample performed the best for Methylene Blue degradation under visible-light illumination. The photocatalytic mechanism was also discussed. We believe that the sulfur and FeOx co-doping, higher oxygen adspecies concentration, and lower baudgap energy were responsible for the excellent visible-light-driven catalytic activity of 1.40 wt.% FeOx/BiVO4-δS0.08.
基金Project supported by the Research Fund of State Key Laboratory for Marine Corrosion and Protection of Luoyang Ship Material Research Institute (LSMRI)(KF190413)。
文摘Metallic glasses have recently attracted great attention in terms of degrading dyes and other organic pollutants as an environmentally friendly material for wastewater remediation.Herein,we report a new type of amorphous catalyst Fe_(41)Co_(7)Cr_(15)Mo_(14)C_(15)B_(6)Y_(2) hollow balls.Results demonstrate that the catalyst can still completely decolorize the 20 mg/L methylene blue(MB)solution after reused for 50 times under conditions of pH=5,catalyst content 0.5 g/L,and temperature 80°C.The catalyst is easily broken during degradation,so the inner surface also provides additional active sites.The Fe_(41)Co_(7)Cr_(15)Mo_(14)C_(15)B_(6)Y_(2) amorphous alloy hollow balls were characterized by energy dispersive X-ray specroscopy(EDS),scanning electron microscopy(SEM)and X-ray photoelectron spectroscopy(XPS),respectively.The elements in the catalytic system have a synergistic catalytic effect.Redox cycle Fe^(2+)/Fe^(3+),Co^(2+)/Co^(3+)and Mo^(4+)/Mo^(6+) promote mutual conversion and accelerate the catalytic process of their reaction with H_(2)O_(2),forming a self-stable redox cycle process.Among them,Fe^(2+)promotes the conversion of Co^(3+)to Co^(2+),and Mo^(4+) promotes the conversion of Fe^(3+)to Fe^(2+),mainly Fe^(2+)and Co^(2+)react with H_(2)O_(2) to generate•OH.Mo and Cr elements form MoO_(2) and Cr_(2)O_(3) plasma compounds on the surface,which act as a protective film to make the catalyst more stable and be repeated used more frequently.
基金supported by the National Natural Science Foundation of China(21503100)Natural Science Foundation of Jiangxi Province(20161BAB213071,20151BAB213010)+1 种基金Project of Education Department of Jiangxi Province(GJJ150325)Sponsored Program for Cultivating Youths of Outstanding Ability in Jiangxi Normal University~~
文摘We report the fabrication and photocatalytic property of a composite of C/CaFe2O4nanorods(NRs)in an effort to reveal the influence of carbon modification.It is demonstrated that the photocatalytic degradation activity is dependent on the mass ratio of C to CaFe2O4.The optimal carbon content is determined to be58wt%to yield a methylene blue(MB)degradation rate of0.0058min.1,which is4.8times higher than that of the pristine CaFe2O4NRs.The decoration of carbon on the surface of CaFe2O4NRs improves its adsorption capacity of the MB dye,which is specifically adsorbed on the surface as a monolayer according to the adsorption isotherm analysis.The trapping experiments of the reactive species indicate that superoxide radicals(.O2)are the main active species responsible for the removal of MB under visible‐light irradiation.Overall,the unique feature of carbon coating enables the efficient separation and transfer of photogenerated electrons and holes,strengthens the adsorption capacity of MB,and improves the light harvesting capability,hence enhancing the overall photocatalytic degradation of MB.
文摘Environmental pollution jeopardizes our existence. For this purpose, research is moving more and more towards the search for economic means and green chemistry to curb this phenomenon. In this context, the photocatalytic activity of zinc sulfide nanoparticles (ZnS NPs) and nanostructured composite ZnS/carbon dots (ZnS/CDs) was evaluated after their synthesis. The results of X-ray diffraction (XRD) analysis indicate that the crystal structure of ZnS/CDs is identical to that of the cubic phase structure of ZnS, revealing that the cubic phase structure of ZnS was not altered in the presence of CDs. Indeed, there is no additional peak in the crystal structure of ZnS/CDs, revealing that the crystalline structure of ZnS is not responsible for the difference in photocatalytic activity between ZnS/CDs and ZnS NPs. Moreover, analysis performed by transmission electron microscopy (TEM) shows aggregation of the synthesized ZnS and ZnS/CDs nanoparticles with an average size estimated around 10 nm and 12 nm, respectively. In addition, the reflectance study in the visible range shows a reduction in the sunlight reflection intensity using ZnS/CDs compared to the capability of ZnS NPs. Photocatalytic degradation tests reveal that ZnS/CDs have the best methylene blue (MB) degradation rate. Indeed, under the optimal conditions, the photocatalytic activity can reach 100% efficiency within 100 min and 240 min of sunlight exposure for the degradation of 7.5 mg/L MB using ZnS/CDs and ZnS, respectively. This improvement in photocatalytic activity of ZnS/CDs may be due to the presence of CDs which can permit to undergo a reduction of reflection properties of ZnS NPs in the visible range. These results show that CDs can play a key role in enhancing the photocatalytic activity of ZnS, and suggest that ZnS/CDs could be used as eco-friendly composite materials for the degradation of organic pollutants of similar structures in the aquatic environment under solar irradiation.