The development of new catalytic techniques for wastewater treatment has long attracted much attention from industrial and academic communities.However,because of catalyst leaching during degradation,catalysts can be ...The development of new catalytic techniques for wastewater treatment has long attracted much attention from industrial and academic communities.However,because of catalyst leaching during degradation,catalysts can be short lived,and therefore expensive,and unsuitable for use in wastewater treatment.In this work,we developed a bimetallic CuO-Co3O4@γ-Al2O3 catalyst for phenol degradation with bicarbonate-activated H2O2.The weakly basic environment provided by the bicarbonate buffer greatly suppresses leaching of active Cu and Co metal ions from the catalyst.X-ray diffraction and X-ray photoelectron spectroscopy results showed interactions between Cu and Co ions in the CuO-Co3O4@γ-Al2O3 catalyst,and these improve the catalytic activity in phenol degradation.Mechanistic studies using different radical scavengers showed that superoxide and hydroxyl radicals both played significant roles in phenol degradation,whereas singlet oxygen was less important.展开更多
In this work,the gold nanoparticles（Au-NPs）were in-situ generated on the surface of MnO2nanosheets to form MnO2/Au-NPs nanocomposite in a simple and cost-effective way.Multiple experiments were carried out to optimi...In this work,the gold nanoparticles（Au-NPs）were in-situ generated on the surface of MnO2nanosheets to form MnO2/Au-NPs nanocomposite in a simple and cost-effective way.Multiple experiments were carried out to optimize the oxidation of basic dye（Methylene Blue（MB））,including the molar ratio of MnO2to chloroauric acid（HAu Cl4）,the p H of the solution and the effect of initial material.Under the optimal condition,the highest degradation efficiency for MB achieved to 98.9%within 60 min,which was obviously better than commercial MnO2powders（4.3%）and MnO2nanosheets（74.2%）.The enhanced oxidative degradation might attribute to the in-situ generation of ultra-small and highly-dispersed Au-NPs which enlarged the synergistic effect and/or interfacial effect between MnO2nanosheets and Au-NPs and facilitated the uptake of electrons by MnO2from MB during the oxidation,thus validating the application of MnO2/Au-NPs nanocomposite for direct removal of organic dyes from wastewater in a simple and convenient fashion.展开更多
A series of metal oxide catalysts for catalytic oxidative degradation of 2-chlorophenol （2-CP） and 4-chlorophenol （4-CP） were prepared, and the supported CuO catalysts were studied particularly. The supported CuO ...A series of metal oxide catalysts for catalytic oxidative degradation of 2-chlorophenol （2-CP） and 4-chlorophenol （4-CP） were prepared, and the supported CuO catalysts were studied particularly. The supported CuO catalysts were characterized by XRD and NH3-TPD techniques, in which CuO/γ-Al2O3 exhibited high degradation activity. The addition of Na2O or K2O into CuO/γ-Al2O3 improved the oxidative degradation of CPs remarkably, in which Na2O was more efficient than K2O. Over CuO/γ-Al2O3-Na2O, CPs were completely converted and the liberation of the inorganic chloride from 2-CP or 4-CP reached 97% or 100% respectively at 30 ？C for 2 h. The supported CuO catalysts with good dispersion of CuO particles and less acid sites were favorable for the efficient oxidative degradation of CPs. In addition, the initial pH of the reaction solution was found to be an important factor which influenced the catalytic oxidative degradation of CPs and the initial pH of 11.2 and 9.8 was preferred for the oxidative degradation of 2-CP and 4-CP respectively over CuO/γ-Al2O3 catalyst.展开更多
A series of(Ce,Cr)xO2/Nb2O5 catalysts with different(Ce,Cr)xO2 to Nb2O5 mass ratios were synthesized by the deposition-precipitation method for use in deep catalytic oxidation of 1,2-dichloroethane(DCE), which is one ...A series of(Ce,Cr)xO2/Nb2O5 catalysts with different(Ce,Cr)xO2 to Nb2O5 mass ratios were synthesized by the deposition-precipitation method for use in deep catalytic oxidation of 1,2-dichloroethane(DCE), which is one of the typical chlorinated volatile organic compound pollutants. The textural properties were characterized by X-ray diffraction, N2 adsorption/desorption isotherms, UV-Raman spectroscopy, and scanning electron microscopy. The surface acidity and the redox properties were characterized by ammonia temperature-programmed desorption and H2 temperature-programmed reduction, respectively. The results show that the addition of a proper amount of(Ce,Cr)xO2 over Nb2O5 significantly improves the intrinsic catalytic activity towards the deep oxidation of DCE, and only a very small amount of C2H3Cl is detected as the byproduct of the oxidation process. Further study reveals the existence of an obvious synergistic effect between Nb2O5, with abundant strong acid sites, and(Ce,Cr)xO2, with strong oxidation sites, as the strong acid sites of Nb2O5 promote the adsorption and dehydrochlorination of DCE, while the strong oxidation sites of(Ce,Cr)xO2 contribute to the deep oxidation of the reactant, intermediates, and byproducts.展开更多
For CO catalytic oxidation,Cu and Ce species are of great importance,between which the synergistic effect is worth investigating.In this work,CeO_(2)/Cu_(2)O with Cu_(2)O{111}and{100}planes were comparatively explored...For CO catalytic oxidation,Cu and Ce species are of great importance,between which the synergistic effect is worth investigating.In this work,CeO_(2)/Cu_(2)O with Cu_(2)O{111}and{100}planes were comparatively explored on CO catalytic oxidation to reveal the effects of interfacial electronic interactions and oxygen defects.The activity result demonstrates that CeO_(2)/o-Cu_(2)O{111}has superior performance compared with CeO_(2)/c-Cu_(2)O{100}.Credit to the coordination unsaturated copper atoms(Cu_(CUS))on oCu_(2)O{111}surface,the interfacial electronic interactions on CeO_(2)/o-Cu_(2)O{111}are more obvious than those on CeO_(2)/c-Cu_(2)O{100},leading to richer oxygen defect generation,better redox and activation abilities of CO and O_(2)reactants.Furthermore,the reaction mechanism of CeO_(2)/o-Cu_(2)O{111}on CO oxidation is revealed,i.e.,CO and O_(2)are adsorbed on the Cucus on Cu_(2)O{111}and oxygen defect of CeO_(2),respectively,and then synergistically promote the CO oxidation to CO_(2).The work sheds light on the designing optimized ceria and copper-based catalysts and the mechanism of CO oxidation.展开更多
The extensive use of tetracycline hydrochloride(TCH)poses a threat to human health and the aquatic environment.Here,magnetic p-n Bi2WO6/CuFe2O4 catalyst was fabricated to efficiently remove TCH.The obtained Bi2WO6/CuF...The extensive use of tetracycline hydrochloride(TCH)poses a threat to human health and the aquatic environment.Here,magnetic p-n Bi2WO6/CuFe2O4 catalyst was fabricated to efficiently remove TCH.The obtained Bi2WO6/CuFe2O4 exhibited 92.1%TCH degradation efficiency and 50.7%and 35.1%mineralization performance for TCH and raw secondary effluent from a wastewater treatment plant in a photo-Fenton-like system,respectively.The remarkable performance was attributed to the fact that photogenerated electrons accelerated the Fe(III)/Fe(II)and Cu(II)/Cu(I)conversion for the Fenton-like reaction between Fe(II)/Cu(I)and H2O2,thereby generating abundant·OH for pollutant oxidation.Various environmental factors including H2O2 concentration,initial pH,catalyst dosage,TCH concentration and inorganic ions were explored.The reactive oxidation species(ROS)quenching results and electron spin resonance(ESR)spectra confirmed that·O2-and·OH were responsible for the dark and photo-Fenton-like systems,respectively.The degradation mechanisms and pathways of TCH were proposed,and the toxicity of products was evaluated.This work contributes a highly efficient and environmentally friendly catalyst and provides a clear mechanistic explanation for the removal of antibiotic pollutants in environmental remediation.展开更多
The characteristics of water quality had significant effects on the oxidative degradation of O_3/H_2O_2 system.In this study,iron supported on activated carbon catalyst was prepared firstly,and then the treatment of l...The characteristics of water quality had significant effects on the oxidative degradation of O_3/H_2O_2 system.In this study,iron supported on activated carbon catalyst was prepared firstly,and then the treatment of landfill leachate by O_3/H_2O_2/catalyst system was analyzed,especially the roles of H_2O_2 in the oxidation of landfill leachate by O_3/H_2O_2 system.The results showed that at room temperature,when the dosage of the catalyst was 1.0g,the removal rate of COD from the landfill leachate reached 79.8% after 50 ml of the landfill leachate(pH=3)was oxidized by O_3(its flow rate was 5g/h)for 50 min.If 0.3ml of H_2O_2 was added to the landfill leachate,the removal rate of COD increased from 79.8%to 88.7%.It showed that the landfill leachate with the characteristics of complex composition and difficult biodegradation could be effectively degraded by the O_3/H_2O_2 system.展开更多
Three-dimensionally ordered mesoporous Fe2O3（meso-Fe2O3） and its supported Au, Pd,and Au-Pd alloy（xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio（y） = 1.48–1.85）photocatalysts have been prepared via...Three-dimensionally ordered mesoporous Fe2O3（meso-Fe2O3） and its supported Au, Pd,and Au-Pd alloy（xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio（y） = 1.48–1.85）photocatalysts have been prepared via the KIT-6-templating and polyvinyl alcohol-protected reduction routes, respectively. Physical properties of the samples were characterized, and their photocatalytic activities were evaluated for the photocatalytic oxidation of acetone in the presence of a small amount of H2O2 under visible-light illumination. It was found that the meso-Fe2O3 was rhombohedral in crystal structure. The as-obtained samples displayed a high surface area of 111.0–140.8 m^2/g and a bandgap energy of 1.98–2.12 eV. The Au, Pd and/or Au–Pd alloy nanoparticles（NPs） with a size of 3–4 nm were uniformly dispersed on the surface of the meso-Fe2O3 support. The 0.72 wt.% AuP d1.48/meso-Fe2O3 sample performed the best in the presence of 0.06 mol/L H2O2 aqueous solution, showing a 100% acetone conversion within4 hr of visible-light illumination. It was concluded that the good performance of 0.72 wt.%AuPd（1.48）/meso-Fe2O3 for photocatalytic acetone oxidation was associated with its ordered mesoporous structure, high adsorbed oxygen species concentration, plasmonic resonance effect between AuPd（1.48） NPs and meso-Fe2O3, and effective separation of the photogenerated charge carriers. In addition, the introduction of H2O2 and the involvement of the photo-Fenton process also played important roles in enhancing the photocatalytic activity of 0.72 wt.%AuPd（1.48）/meso-Fe2O3.展开更多
Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled inte...Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled interface constructed betweenα-MnO2 and Co3O4 is responsible for the enhanced catalytic activity.The resultantα-MnO2@Co3O4 catalyst exhibits excellent catalytic activity at a T90%(temperature required to achieve a toluene conversion of 90%)of approximately 229℃,which is 47 and 28℃ lower than those of the pureα-MnO2 nanowire and Co3O4-b obtained via pyrolysis of ZIF-67,respectively.This activity is attributed to the increase in the number of surface-adsorbed oxygen species,which accelerate the oxygen mobility and enhance the redox pairs of Mn^4+/Mn^3+ and Co^2+/Co^3+.Moreover,the result of in situ diffuse reflectance infrared Fourier transform spectroscopy suggests that the gaseous oxygen could be more easily activated to adsorbed oxygen species on the surface of α-MnO2@Co3O4 than on that of α-MnO2.The catalytic reaction route of toluene oxidation over theα-MnO2@Co3O4 catalyst is as follows:toluene→benzoate species→alkanes containing oxygen functional group→CO2 and H2O.In addition,the α-MnO2@Co3O4 catalyst shows excellent stability and good water resistance for toluene oxidation.Furthermore,the preparation method can be extended to other 1D MnO2 materials.A new strategy for the development of high-performance catalysts of practical significance is provided.展开更多
The La2O3/Fe2O3-CeO2 composite oxide catalysts were prepared by coprecipitation method, sol-gel method and hydrothermal method. The effect of preparation methods on structure morphology and photocatalytic properties o...The La2O3/Fe2O3-CeO2 composite oxide catalysts were prepared by coprecipitation method, sol-gel method and hydrothermal method. The effect of preparation methods on structure morphology and photocatalytic properties of La2O3/Fe2O3-CeO2 samples was investigated. The results show that the cubic CeO2 structure can be obtained at 600℃. The rod-shaped sample prepared by coprecipitation method, displays the highest crystalline and the strongest diffraction peak intensity. The spherical sample is acquired from sol-gel method, while the small granular sample prepared by hydrothermal method tends to aggregate. The maximum specific surface area of the sample prepared by coprecipitation method is 76.21 m2/g, the minimum specific area of the sample from sol-gel method is 32.66 m2/g and the maximum pore size is 13.84 nm, while the minimum pore volume and pore size of the sample by hydrothermal method are 0.038 cm3/g and 3.95 nm respectively. The band gap energy of catalyst samples is in the following order: sample-CP < sample-SG < sample-HT. The sample obtained by coprecipitation method has the best catalytic degradation performance for methylene blue. Under the excitation of visible light, the degradation rate was 99.58% at 50 minutes, which was higher than those of sol-gel method and hydrothermal method by 5.58% and 9.54% respectively. The catalytic degradation reaction is a first-order kinetic model: ln (c0/ct) = kt + qe. The maximum k-value of the sample degradation process obtained by coprecipitation method is 0.074 min-1.展开更多
The effects of eleven flavonoids on lipid peroxidation, protein degradation, deformability and osmotic fragility of human erythrocytes exposed in vitro to 10 mM H2O2 for 60 min at 37 oC have been studied. The followin...The effects of eleven flavonoids on lipid peroxidation, protein degradation, deformability and osmotic fragility of human erythrocytes exposed in vitro to 10 mM H2O2 for 60 min at 37 oC have been studied. The following flavonoids;quercetin, rutin and morin significantly protected eryt-hrocytes against lipid peroxidation caused by H2O2. This inhibition of lipid peroxidation could be explained by the presence of at least two hydroxyl groups in ring B of the flavonoid structure, regardless of their positions. However, the flavonoids;quercetin, 3,5,7-trihy- droxy-4'-methoxy flavone-7-rutinoside and 3- hydroxy flavone significantly protected eryt-hrocytes against protein degradation. This inhibition could also be explained by the presence of a hydroxyl group at C-3 in ring C of the flavonoid structure. Quercetin and 3,5,7-trihydroxy-4'- methoxy flvone-7-rutinoside significantly protected erythrocytes against loss of deformability and increased osmotic fragility, indicating that the loss of erythrocyte deformability and the increase in osmotic fragility of erythrocytes exposed to H2O2 are related to protein degradation rather than to lipid peroxidation. The other flavonoids (chrysin, 2-carboxy ethyl dihydroxy flavone, apigenin, cirsimaritin, α-naphto flavone and flavanone) failed to protect erythrocytes against the observed oxidative damages. The results demonstrate the importance of the chemical groups substituted on the basic skeleton of the flavonoids in dictating the type of antioxidant activity, and also demonstrate the hemorheological potentials of flavonoids that have particular protein-antioxidant activities.展开更多
In this study, Co3O4@CeO2 core@shell nanowires were successfully prepared via thermal decomposition of Co（CO3）0.5（OH）.0.11H2O@CeO2 core@shell nanowire precursors. As a CO oxidation catalyst, Co3O4@CeO2 shows remar...In this study, Co3O4@CeO2 core@shell nanowires were successfully prepared via thermal decomposition of Co（CO3）0.5（OH）.0.11H2O@CeO2 core@shell nanowire precursors. As a CO oxidation catalyst, Co3O4@CeO2 shows remarkably enhanced catalytic performance compared to Co3O4 nanowires and CeO2 nanoparticles （NPs）, indicating obvious synergistic effects between the two components. It also suggests that the CeO2 shell coating can effectively prevent Co3O4 nanowires from agglomerating, hence effecting a substantial improvement in the structural stability of the Co3O4 catalyst. Furthermore, the fabrication of the welbdisperse4 core@shell structure results in a maximized interface area between Co3O4 and CeO2, as well as a reduced Co3O4 size, which may be responsible for the enhanced catalytic activity of Co3O4@CeO2. Further examination revealed that CO oxidation may occur at the interface of Co3O4 and CeO2. The influence of calcination temperatures and the component ratio between Co3O4 and CeO2 were then investigated in detail to determine the catalytic performance of Co3O4@CeO2 core@shell nanowires, the best of which was obtained by calcination at 250 ℃ for 3 h with a Ce molar concentration of about 38.5%. This sample achieved 100% CO conversion at a reduced temperature of 160 ℃. More importantly, more than 2.5 g of the Co3O4@CeO2 core@shell nanowires were produced in one pot by this simple process, which may be beneficial for practical applications as automobile-exhaust gas-treatment catalysts.展开更多
基金supported by the National Natural Science Foundation of China(21273086)Chutian Scholar Foundation from Hubei Province,China~~
文摘The development of new catalytic techniques for wastewater treatment has long attracted much attention from industrial and academic communities.However,because of catalyst leaching during degradation,catalysts can be short lived,and therefore expensive,and unsuitable for use in wastewater treatment.In this work,we developed a bimetallic CuO-Co3O4@γ-Al2O3 catalyst for phenol degradation with bicarbonate-activated H2O2.The weakly basic environment provided by the bicarbonate buffer greatly suppresses leaching of active Cu and Co metal ions from the catalyst.X-ray diffraction and X-ray photoelectron spectroscopy results showed interactions between Cu and Co ions in the CuO-Co3O4@γ-Al2O3 catalyst,and these improve the catalytic activity in phenol degradation.Mechanistic studies using different radical scavengers showed that superoxide and hydroxyl radicals both played significant roles in phenol degradation,whereas singlet oxygen was less important.
基金supported by the National Natural Science Foundation of China (Nos. 21277048 and 21505046)the China Postdoctoral Science Foundation (No. 2016 M590336)+1 种基金the "Chenguang Program" funded by Shanghai Education Development FoundationShanghai Municipal Education Commission (No. 15CG21)
文摘In this work,the gold nanoparticles（Au-NPs）were in-situ generated on the surface of MnO2nanosheets to form MnO2/Au-NPs nanocomposite in a simple and cost-effective way.Multiple experiments were carried out to optimize the oxidation of basic dye（Methylene Blue（MB））,including the molar ratio of MnO2to chloroauric acid（HAu Cl4）,the p H of the solution and the effect of initial material.Under the optimal condition,the highest degradation efficiency for MB achieved to 98.9%within 60 min,which was obviously better than commercial MnO2powders（4.3%）and MnO2nanosheets（74.2%）.The enhanced oxidative degradation might attribute to the in-situ generation of ultra-small and highly-dispersed Au-NPs which enlarged the synergistic effect and/or interfacial effect between MnO2nanosheets and Au-NPs and facilitated the uptake of electrons by MnO2from MB during the oxidation,thus validating the application of MnO2/Au-NPs nanocomposite for direct removal of organic dyes from wastewater in a simple and convenient fashion.
基金financially supported by the Education Department of Liaoning Province(No.2009A421)
文摘A series of metal oxide catalysts for catalytic oxidative degradation of 2-chlorophenol （2-CP） and 4-chlorophenol （4-CP） were prepared, and the supported CuO catalysts were studied particularly. The supported CuO catalysts were characterized by XRD and NH3-TPD techniques, in which CuO/γ-Al2O3 exhibited high degradation activity. The addition of Na2O or K2O into CuO/γ-Al2O3 improved the oxidative degradation of CPs remarkably, in which Na2O was more efficient than K2O. Over CuO/γ-Al2O3-Na2O, CPs were completely converted and the liberation of the inorganic chloride from 2-CP or 4-CP reached 97% or 100% respectively at 30 ？C for 2 h. The supported CuO catalysts with good dispersion of CuO particles and less acid sites were favorable for the efficient oxidative degradation of CPs. In addition, the initial pH of the reaction solution was found to be an important factor which influenced the catalytic oxidative degradation of CPs and the initial pH of 11.2 and 9.8 was preferred for the oxidative degradation of 2-CP and 4-CP respectively over CuO/γ-Al2O3 catalyst.
基金supported by the National Key R&D Program of China(2016YFC0204300)the National Natural Science Foundation of China(21477109)~~
文摘A series of(Ce,Cr)xO2/Nb2O5 catalysts with different(Ce,Cr)xO2 to Nb2O5 mass ratios were synthesized by the deposition-precipitation method for use in deep catalytic oxidation of 1,2-dichloroethane(DCE), which is one of the typical chlorinated volatile organic compound pollutants. The textural properties were characterized by X-ray diffraction, N2 adsorption/desorption isotherms, UV-Raman spectroscopy, and scanning electron microscopy. The surface acidity and the redox properties were characterized by ammonia temperature-programmed desorption and H2 temperature-programmed reduction, respectively. The results show that the addition of a proper amount of(Ce,Cr)xO2 over Nb2O5 significantly improves the intrinsic catalytic activity towards the deep oxidation of DCE, and only a very small amount of C2H3Cl is detected as the byproduct of the oxidation process. Further study reveals the existence of an obvious synergistic effect between Nb2O5, with abundant strong acid sites, and(Ce,Cr)xO2, with strong oxidation sites, as the strong acid sites of Nb2O5 promote the adsorption and dehydrochlorination of DCE, while the strong oxidation sites of(Ce,Cr)xO2 contribute to the deep oxidation of the reactant, intermediates, and byproducts.
基金Project supported by the National Natural Science Foundation of China(21707066,21677069)。
文摘For CO catalytic oxidation,Cu and Ce species are of great importance,between which the synergistic effect is worth investigating.In this work,CeO_(2)/Cu_(2)O with Cu_(2)O{111}and{100}planes were comparatively explored on CO catalytic oxidation to reveal the effects of interfacial electronic interactions and oxygen defects.The activity result demonstrates that CeO_(2)/o-Cu_(2)O{111}has superior performance compared with CeO_(2)/c-Cu_(2)O{100}.Credit to the coordination unsaturated copper atoms(Cu_(CUS))on oCu_(2)O{111}surface,the interfacial electronic interactions on CeO_(2)/o-Cu_(2)O{111}are more obvious than those on CeO_(2)/c-Cu_(2)O{100},leading to richer oxygen defect generation,better redox and activation abilities of CO and O_(2)reactants.Furthermore,the reaction mechanism of CeO_(2)/o-Cu_(2)O{111}on CO oxidation is revealed,i.e.,CO and O_(2)are adsorbed on the Cucus on Cu_(2)O{111}and oxygen defect of CeO_(2),respectively,and then synergistically promote the CO oxidation to CO_(2).The work sheds light on the designing optimized ceria and copper-based catalysts and the mechanism of CO oxidation.
基金supported by the National Natural Science Foundation of China(Nos.51678270,21872063)111 Project of Jilin University,China(No.B16020)。
文摘The extensive use of tetracycline hydrochloride(TCH)poses a threat to human health and the aquatic environment.Here,magnetic p-n Bi2WO6/CuFe2O4 catalyst was fabricated to efficiently remove TCH.The obtained Bi2WO6/CuFe2O4 exhibited 92.1%TCH degradation efficiency and 50.7%and 35.1%mineralization performance for TCH and raw secondary effluent from a wastewater treatment plant in a photo-Fenton-like system,respectively.The remarkable performance was attributed to the fact that photogenerated electrons accelerated the Fe(III)/Fe(II)and Cu(II)/Cu(I)conversion for the Fenton-like reaction between Fe(II)/Cu(I)and H2O2,thereby generating abundant·OH for pollutant oxidation.Various environmental factors including H2O2 concentration,initial pH,catalyst dosage,TCH concentration and inorganic ions were explored.The reactive oxidation species(ROS)quenching results and electron spin resonance(ESR)spectra confirmed that·O2-and·OH were responsible for the dark and photo-Fenton-like systems,respectively.The degradation mechanisms and pathways of TCH were proposed,and the toxicity of products was evaluated.This work contributes a highly efficient and environmentally friendly catalyst and provides a clear mechanistic explanation for the removal of antibiotic pollutants in environmental remediation.
基金Supported by the Natural Science Foundation of Ningbo City,Zhejiang Province(2013A610188)the Self-designed Subject of "Modern Microorganism Technology and Application",the Priority Discipline of Zhejiang Province,China(ZS2013011)
文摘The characteristics of water quality had significant effects on the oxidative degradation of O_3/H_2O_2 system.In this study,iron supported on activated carbon catalyst was prepared firstly,and then the treatment of landfill leachate by O_3/H_2O_2/catalyst system was analyzed,especially the roles of H_2O_2 in the oxidation of landfill leachate by O_3/H_2O_2 system.The results showed that at room temperature,when the dosage of the catalyst was 1.0g,the removal rate of COD from the landfill leachate reached 79.8% after 50 ml of the landfill leachate(pH=3)was oxidized by O_3(its flow rate was 5g/h)for 50 min.If 0.3ml of H_2O_2 was added to the landfill leachate,the removal rate of COD increased from 79.8%to 88.7%.It showed that the landfill leachate with the characteristics of complex composition and difficult biodegradation could be effectively degraded by the O_3/H_2O_2 system.
基金supported by the National Natural Science Foundation of China (No. 21377008)the National High Technology Research and Development Program of China ("863"Program)(No. 2015AA034603)the Foundation of the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions
文摘Three-dimensionally ordered mesoporous Fe2O3（meso-Fe2O3） and its supported Au, Pd,and Au-Pd alloy（xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio（y） = 1.48–1.85）photocatalysts have been prepared via the KIT-6-templating and polyvinyl alcohol-protected reduction routes, respectively. Physical properties of the samples were characterized, and their photocatalytic activities were evaluated for the photocatalytic oxidation of acetone in the presence of a small amount of H2O2 under visible-light illumination. It was found that the meso-Fe2O3 was rhombohedral in crystal structure. The as-obtained samples displayed a high surface area of 111.0–140.8 m^2/g and a bandgap energy of 1.98–2.12 eV. The Au, Pd and/or Au–Pd alloy nanoparticles（NPs） with a size of 3–4 nm were uniformly dispersed on the surface of the meso-Fe2O3 support. The 0.72 wt.% AuP d1.48/meso-Fe2O3 sample performed the best in the presence of 0.06 mol/L H2O2 aqueous solution, showing a 100% acetone conversion within4 hr of visible-light illumination. It was concluded that the good performance of 0.72 wt.%AuPd（1.48）/meso-Fe2O3 for photocatalytic acetone oxidation was associated with its ordered mesoporous structure, high adsorbed oxygen species concentration, plasmonic resonance effect between AuPd（1.48） NPs and meso-Fe2O3, and effective separation of the photogenerated charge carriers. In addition, the introduction of H2O2 and the involvement of the photo-Fenton process also played important roles in enhancing the photocatalytic activity of 0.72 wt.%AuPd（1.48）/meso-Fe2O3.
文摘Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled interface constructed betweenα-MnO2 and Co3O4 is responsible for the enhanced catalytic activity.The resultantα-MnO2@Co3O4 catalyst exhibits excellent catalytic activity at a T90%(temperature required to achieve a toluene conversion of 90%)of approximately 229℃,which is 47 and 28℃ lower than those of the pureα-MnO2 nanowire and Co3O4-b obtained via pyrolysis of ZIF-67,respectively.This activity is attributed to the increase in the number of surface-adsorbed oxygen species,which accelerate the oxygen mobility and enhance the redox pairs of Mn^4+/Mn^3+ and Co^2+/Co^3+.Moreover,the result of in situ diffuse reflectance infrared Fourier transform spectroscopy suggests that the gaseous oxygen could be more easily activated to adsorbed oxygen species on the surface of α-MnO2@Co3O4 than on that of α-MnO2.The catalytic reaction route of toluene oxidation over theα-MnO2@Co3O4 catalyst is as follows:toluene→benzoate species→alkanes containing oxygen functional group→CO2 and H2O.In addition,the α-MnO2@Co3O4 catalyst shows excellent stability and good water resistance for toluene oxidation.Furthermore,the preparation method can be extended to other 1D MnO2 materials.A new strategy for the development of high-performance catalysts of practical significance is provided.
文摘The La2O3/Fe2O3-CeO2 composite oxide catalysts were prepared by coprecipitation method, sol-gel method and hydrothermal method. The effect of preparation methods on structure morphology and photocatalytic properties of La2O3/Fe2O3-CeO2 samples was investigated. The results show that the cubic CeO2 structure can be obtained at 600℃. The rod-shaped sample prepared by coprecipitation method, displays the highest crystalline and the strongest diffraction peak intensity. The spherical sample is acquired from sol-gel method, while the small granular sample prepared by hydrothermal method tends to aggregate. The maximum specific surface area of the sample prepared by coprecipitation method is 76.21 m2/g, the minimum specific area of the sample from sol-gel method is 32.66 m2/g and the maximum pore size is 13.84 nm, while the minimum pore volume and pore size of the sample by hydrothermal method are 0.038 cm3/g and 3.95 nm respectively. The band gap energy of catalyst samples is in the following order: sample-CP < sample-SG < sample-HT. The sample obtained by coprecipitation method has the best catalytic degradation performance for methylene blue. Under the excitation of visible light, the degradation rate was 99.58% at 50 minutes, which was higher than those of sol-gel method and hydrothermal method by 5.58% and 9.54% respectively. The catalytic degradation reaction is a first-order kinetic model: ln (c0/ct) = kt + qe. The maximum k-value of the sample degradation process obtained by coprecipitation method is 0.074 min-1.
文摘The effects of eleven flavonoids on lipid peroxidation, protein degradation, deformability and osmotic fragility of human erythrocytes exposed in vitro to 10 mM H2O2 for 60 min at 37 oC have been studied. The following flavonoids;quercetin, rutin and morin significantly protected eryt-hrocytes against lipid peroxidation caused by H2O2. This inhibition of lipid peroxidation could be explained by the presence of at least two hydroxyl groups in ring B of the flavonoid structure, regardless of their positions. However, the flavonoids;quercetin, 3,5,7-trihy- droxy-4'-methoxy flavone-7-rutinoside and 3- hydroxy flavone significantly protected eryt-hrocytes against protein degradation. This inhibition could also be explained by the presence of a hydroxyl group at C-3 in ring C of the flavonoid structure. Quercetin and 3,5,7-trihydroxy-4'- methoxy flvone-7-rutinoside significantly protected erythrocytes against loss of deformability and increased osmotic fragility, indicating that the loss of erythrocyte deformability and the increase in osmotic fragility of erythrocytes exposed to H2O2 are related to protein degradation rather than to lipid peroxidation. The other flavonoids (chrysin, 2-carboxy ethyl dihydroxy flavone, apigenin, cirsimaritin, α-naphto flavone and flavanone) failed to protect erythrocytes against the observed oxidative damages. The results demonstrate the importance of the chemical groups substituted on the basic skeleton of the flavonoids in dictating the type of antioxidant activity, and also demonstrate the hemorheological potentials of flavonoids that have particular protein-antioxidant activities.
基金This work was supported by the financial aid from the National Natural Science Foundation of China （Nos. 91122030, 51272249, 21210001, 21221061 and 21401186）, and the National Key Basic Research Program of China （No. 2014CB643802）.
文摘In this study, Co3O4@CeO2 core@shell nanowires were successfully prepared via thermal decomposition of Co（CO3）0.5（OH）.0.11H2O@CeO2 core@shell nanowire precursors. As a CO oxidation catalyst, Co3O4@CeO2 shows remarkably enhanced catalytic performance compared to Co3O4 nanowires and CeO2 nanoparticles （NPs）, indicating obvious synergistic effects between the two components. It also suggests that the CeO2 shell coating can effectively prevent Co3O4 nanowires from agglomerating, hence effecting a substantial improvement in the structural stability of the Co3O4 catalyst. Furthermore, the fabrication of the welbdisperse4 core@shell structure results in a maximized interface area between Co3O4 and CeO2, as well as a reduced Co3O4 size, which may be responsible for the enhanced catalytic activity of Co3O4@CeO2. Further examination revealed that CO oxidation may occur at the interface of Co3O4 and CeO2. The influence of calcination temperatures and the component ratio between Co3O4 and CeO2 were then investigated in detail to determine the catalytic performance of Co3O4@CeO2 core@shell nanowires, the best of which was obtained by calcination at 250 ℃ for 3 h with a Ce molar concentration of about 38.5%. This sample achieved 100% CO conversion at a reduced temperature of 160 ℃. More importantly, more than 2.5 g of the Co3O4@CeO2 core@shell nanowires were produced in one pot by this simple process, which may be beneficial for practical applications as automobile-exhaust gas-treatment catalysts.
