Series Li-Sb-Mn composite oxides with different Sb/Mn molar ratios were obtained by solid state reaction.Their structure,morphology and Li^＋ extraction/adsorption properties were characterized by X-ray diffractometry...Series Li-Sb-Mn composite oxides with different Sb/Mn molar ratios were obtained by solid state reaction.Their structure,morphology and Li^＋ extraction/adsorption properties were characterized by X-ray diffractometry （XRD）,scanning electron microscopy （SEM） and atomic absorption spectrophotometry （AAS）,respectively.XRD and SEM analyses reveal that the crystal of the products transfers from spinel to orthorhombic phase with the increase of molar ratio of Sb to Mn from 0.05 to 1.00.The Li^＋ extraction and adsorption experiments for these Li-Sb-Mn composite oxides demonstrate that the composite oxides can all be used as lithium inorganic adsorbents.The acid treated spinel Li-Sb-Mn composite oxide with Sb/Mn molar ratio of 0.05 has a high Li^＋ adsorption capacity of 33.23mg/g in lithium solution.The Sb/Mn molar ratio of these Li-Sb-Mn composite oxides should be a crucial factor in determining their structure and Li^＋ extraction and adsorption properties.展开更多
The composite oxides xAg/Co_（0.93）Ce_（0.07）（x=Ag/（Co＋Ce） molar ratio）,intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on ...The composite oxides xAg/Co_（0.93）Ce_（0.07）（x=Ag/（Co＋Ce） molar ratio）,intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on the performance of these substances during soot combustion were subsequently investigated.Under O_2,the 0.3Ag/Co_（0.93）Ce_（0.07） catalyst resulted in the lowest ignition temperature,T_（10）,of197 ℃,while the minimum light-off temperature was obtained from both 0.2Ag/Co_（0.93）Ce_（0.07） and0.3Ag/Co_（0.93）Ce_（0.07） in the NO_x atmosphere.These materials were also characterized by various techniques,including H_2,soot and NO_x temperature programmed reduction,X-ray diffraction,and electron paramagnetic resonance,Raman,X-ray photoelectron,and Fourier transform infrared spectroscopic analyses.The results demonstrated that silver significantly alters the catalytic behavior under both O_2 and NO_x,even though the lattice structure of the mixed oxide is not affected.Surface silver oxides generated under the O_2 atmosphere favor soot combustion by participating in the redox cycles between soot and the silver oxide,whereas the AgNO_3 that forms in a NO_x-rich atmosphere facilitates soot abatement at a lower temperature.The inferior activity of AgNO_3 relative to that of Ag_2O results in the different catalytic performance in the presence of NO_x or O_2.展开更多
Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product...Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product fraction in hydrocarbon distribution was rather low, demonstrating a promising potential in higher alcohols synthesis from syngas. The distribution of alcohols and hydrocarbons approximately obeyed Anderson-Schulz-Flory distribution with similar chain growth probability, indicating alcohols and hydrocarbons derived from the same intermediates. The effects of Cu/Fe molar ratio, reaction temperature and gas hourly space velocity （GHSV） on catalytic performance were studied in detail. The sample with a Cu/Fe molar ratio of 10/1 exhibited the best catalytic performance. Higher reaction temperature accelerated water-gas-shift reaction and led to lower total alcohols selectivity. GHSV showed great effect on catalytic performance and higher GHSV increased the total alcohol selectivity, indicating there existed visible dehydration reaction of alcohol into hydrocarbon.展开更多
The nano-crystalline Cu-Ce-Zr-O composite oxides were successfully prepared by the supercritical anti-solvent （SAS） process. The physicochemical properties and catalytic performances were investigated by X-ray diffr...The nano-crystalline Cu-Ce-Zr-O composite oxides were successfully prepared by the supercritical anti-solvent （SAS） process. The physicochemical properties and catalytic performances were investigated by X-ray diffraction （XRD）, Raman spectroscopy, H2 temperature-programmed reduction （H2 -TPR）, oxygen storage capacity （OSC） measurement and catalytic activity evaluation. It was found that Cu2＋ ions incorporated into CeO2 -ZrO2 lattice to form Cu-Ce-Zr-O solid solution associated with the formation of oxygen vacancies. The Cu-Ce-Zr-O catalysts prepared via the SAS process with the Cu content 2.63 mol.% showed the highest OSC index of 636.9 μmol/g. Compared with the samples prepared by impregnation method, Cu doping using SAS process could improve the dispersion of Cu2＋ in the composite oxide, enhance the interaction between Cu2＋ and CeO2-ZrO2 , improve the reducibility of catalyst, and thus improve the OSC performance and increase the catalytic activity for CO oxidation at low temperature.展开更多
Cerium-zirconium composite oxides with high performance were synthesized by a co-precipitation method, using zirconium oxychloride and rare earth chloride as raw materials. The effects of precipitate aging time on the...Cerium-zirconium composite oxides with high performance were synthesized by a co-precipitation method, using zirconium oxychloride and rare earth chloride as raw materials. The effects of precipitate aging time on the properties of cerium-zirconium composite oxides were investigated. The prepared cerium-zirconium composite oxides were characterized by X-ray diffraction（XRD）, BET specific surface area, pulsed oxygen chemical adsorption, H2 temperature-programmed-reduction（H2-TPR）, scanning electron microscopy（SEM）, etc. The results showed that the precipitate aging time caused great effects on the properties of cerium zirconium composite oxides. With the increase of aging time, the cerium zirconium composite oxides showed enhanced specific surface area, good thermal stability, and high oxygen storage capacity（OSC）. The best performance sample was obtained while the precipitate aging time up to 48 h, with the specific surface area of 140.7 m2/g, and OSC of 657.24 μmolO2/g for the fresh sample. Even after thermal aged under 1000 oC for 4 h, the aged specific surface area was 41.6 m2/g, moreover with a good OSC of 569.9 μmolO2/g.展开更多
With sol-gel method,nanometer La-Ti composite oxides were prepared.By means of atomic force microscope,the surface pattern,particle size distribution and specific surface area were studied.The newly prepared nanocryst...With sol-gel method,nanometer La-Ti composite oxides were prepared.By means of atomic force microscope,the surface pattern,particle size distribution and specific surface area were studied.The newly prepared nanocrystals of La-Ti composite oxides were used as the catalysts to catalyze the dehydration of external compensated lactic acid to lactide.The lactide product was measured by polarimeter and micropolariscope.The results demonstrate that the ratio between D-lactide and L-lactide will not be equal to 1-1 if nanocrystals of La-Ti composite oxides are used as the catalysts,which implies,that nanocrystals of La-Ti composite oxides may be potential catalysts with a good selectivity.展开更多
The composition,structure and micro-morphology of magnesium- iron- aluminum composite oxides were investigated using various methods such as XRF,SEM,EDS,XRD and KMn O4-titration. Compared to hercynite,the composite ox...The composition,structure and micro-morphology of magnesium- iron- aluminum composite oxides were investigated using various methods such as XRF,SEM,EDS,XRD and KMn O4-titration. Compared to hercynite,the composite oxides have completely different phases including solid solution（ Mg O）0. 77（ Fe O）0. 23,composite spinel Mg Fe0. 2Al1. 8O4 and a small amount of Mg Fe2O4. The composite oxides exhibit excellent corrosion resistance to cement clinker and potassium salts.The products produced by magnesite and the composite oxides show better performance than magnesia- hercynite bricks,especially the corrosion resistance and thermal shock resistance.展开更多
Vanadium‐chromium oxides(VCrO)were usually prepared by high‐temperature solid‐state reactions;however,mixed phases were frequently produced and the morphology of the products was not well controlled.In this work,we...Vanadium‐chromium oxides(VCrO)were usually prepared by high‐temperature solid‐state reactions;however,mixed phases were frequently produced and the morphology of the products was not well controlled.In this work,we prepared amorphous VCrO precursors by using V2O5 and CrO3 and alcohols or mixtures of alcohol and water via solvothermal reaction at 180°C.The precursors were then calcined under nitrogen at various temperatures.The products were characterized by powder X‐ray diffraction,transmission electron microscopy,and X‐ray photoelectron spectroscopy.It was revealed that pure‐phase nanocrystalline orthorhombic CrVO4 was obtained when methanol or methanol/water was used as the solvothermal medium and the precursor was calcined at 700°C.The size of the CrVO4 crystals was around 500 nm when methanol was used,whereas it reduced significantly to less than 50 nm when a mixture of methanol and water was used.The sizes could be effectively tuned from 10 to 50 nm by varying the methanol/water volume ratio.To the best of our knowledge,this is the first report on the synthesis of pure‐phase CrVO4 nanocrystals.The nano‐CrVO4 showed almost the highest catalytic activity for the ammoxidation of 2,6‐dichlorotoluene to 2,6‐dichlorobenzonitrile among the reported bi‐component composite oxides,owing to its smaller particle size,larger specific surface area,and more exposed active centers.展开更多
Three La-doped CeO2-ZrO2-Al2O3(CZA)composite oxide samples,namely,CZA-I,CZA-II and CZA-III,were prepared following a co-precipitation method in the presence of La2O3,La(NO3)3-6H2O and H[La(EDTA)]-16H2O precursors,resp...Three La-doped CeO2-ZrO2-Al2O3(CZA)composite oxide samples,namely,CZA-I,CZA-II and CZA-III,were prepared following a co-precipitation method in the presence of La2O3,La(NO3)3-6H2O and H[La(EDTA)]-16H2O precursors,respectively.When the precursor samples are sintered at 1000°C,the as-prepared composite oxides mainly exhibit the CeO2-ZrO2 cubic fluorite phase,while theγ-Al2O3 andδ-Al2O3 phases appear when the precursor samples are subjected to sintering at 1100 and 1200°C.CZA-III exhibits improved redox properties after high-temperature treatment compared with CZA-I and CZA-II.CZA-III presents the largest surface area of 97.46 m2/g among the three CZAs when the CZA-III precursor sample is sintered at 1000°C.Furthermore,the corresponding oxygen storage capacity(OSC)is the largest with value of 400.27μmol/g when CZA-III precursor sample is sintered at 1000°C.Additionally,CZA-III exhibits the best thermal stability and the highest reduction temperature.However,by increasing the sintering temperature to 1200°C,there is a dramatic decline in the properties of surface area and OSC.And a decrease for CZA-III in surface area by 58.94%and a decrease of the OSC value by 74.56%are observed.展开更多
CO2-TPD was demonstrated an effective way to investigate the phase formation during pyrolysis for the preparation of composite oxides using metal-organic molecules as precursors.Based on the CO2-TPD results, it was f...CO2-TPD was demonstrated an effective way to investigate the phase formation during pyrolysis for the preparation of composite oxides using metal-organic molecules as precursors.Based on the CO2-TPD results, it was found that calcination condition had deep effect on the carbonate formation and the minimum firing temperature to acquire pure phase composite oxide.An optimized calcination schedule was then developed.展开更多
A series of spinel Li-Mn-Ni composite oxides with theoretical chemical formula of LiNixMn2-xO4 （0〈_x〈_1.0） were synthesized by liquid phase method. Their structure and morphology were characterized by X-ray diffra...A series of spinel Li-Mn-Ni composite oxides with theoretical chemical formula of LiNixMn2-xO4 （0〈_x〈_1.0） were synthesized by liquid phase method. Their structure and morphology were characterized by X-ray diffractometry （XRD） and scanning electron microscopy （SEM）, respectively. The stability of these Ni-substituted spinel oxides prepared at different temperatures was investigated in acidic medium as well. The results show that Ni can be brought into the spinel framework completely to form well-crystallized product when x〈_0.5 and the optimized synthesis temperature is 800℃. LiNi0.4Mn1.6O4 prepared at 800℃ can maintain the spinel structure and morphology with Li extraction ratio of 30.37%, Mn extraction ratio of 8.78% and Ni extraction ratio of 1,82% during acid treatment. The incorporated Ni not only inhibits the dissolution of Mn, but also reduces the extraction of Li due to the lattice contraction展开更多
Plasma-coupled catalysis is a promising volatile organic co mpounds(VOCs) removal technology because of its interactional principles of plasma decomposition and catalytic oxidation.However,the problem of harmful by-pr...Plasma-coupled catalysis is a promising volatile organic co mpounds(VOCs) removal technology because of its interactional principles of plasma decomposition and catalytic oxidation.However,the problem of harmful by-products is still in trouble.A series of rare earth doped RE-NiO_(x)(RE=Ce,Y,La) composite oxides were synthesized by metal organic frameworks(MOFs)-derived method for coupled plasma oxidation of benzene and by-product ozone removal.Compared with plasma alone,the 1%La-NiO_(x)catalyst shows the best enhancement of 50% for benzene conversion with complete removal of a maximum of 800 ppm ozone.The energy consumption for 90% benzene removal efficiency(η90%) is also reduced from 3600 to 1200 J/L.Characterization re sults of RE-NiO_(x) catalysts indicate that the doping of La causes interaction and synergistic effect between La and Ni,and the surface oxygen and lattice oxygen with defects play crucial roles in benzene oxidation and ozone decomposition,respectively.In addition,the decomposition mechanism of benzene and ozone under plasma is proposed.Plasma is responsible for the indiscriminate bond breaking in benzene and oxygen to form a variety of organic intermediates and ozone,while the La-NiO_(x) catalyst selectively oxidizes the intermediates to CO_(x)/H2O and decomposes the ozone into oxygen.展开更多
A novel type of microcapsule-encapsulated corrosion inhibitor was prepared in a water-based solution with a pH range of 7-8,and it was applied to the composite organic coating of magnesium alloy plasma electrolytic ox...A novel type of microcapsule-encapsulated corrosion inhibitor was prepared in a water-based solution with a pH range of 7-8,and it was applied to the composite organic coating of magnesium alloy plasma electrolytic oxidation to enhance its corrosion resistance and self-healing properties.The morphology,chemical composition,structure,and functional properties of the composite coating were investigated by scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDS),Fourier transform infrared spectroscopy(FTIR),polarization curve,alternating current impedance,and salt immersion test.The experimental results showed that,after immersion in a 3.5 wt%NaCl solution for 12 h,the coating could effectively protect AZ91D from corrosion.When the coating was damaged,the exposed alloy surface would release metal ions in the corrosive environment and react with the corrosion inhibitor 8-hydroxyquinoline to form a Mg(8-HQ)_(2) chelate,exhibiting significant self-healing behavior.The study results demonstrate the broad application prospects of microcapsule technology in the coating field,providing new ideas for the development of efficient anti-corrosion coatings.展开更多
Sodium-ion batteries have garnered significant attention as a cost-effective alternative to lithium-ion batteries due to the abundance and affordability of sodium precursors.However,the lack of suitable electrode mate...Sodium-ion batteries have garnered significant attention as a cost-effective alternative to lithium-ion batteries due to the abundance and affordability of sodium precursors.However,the lack of suitable electrode materials with both high capacity and excellent stability continues to hinder their practical viability.Herein,we couple lattice strain and sulfur deficiency effects in a tin monosulfide/reduced graphene oxide composite to enhance sodium storage performance.Experimental results and theoretical calculations reveal that the synergistic effects of lattice strain and sulfur vacancies in tin monosulfide promote rapid(de)intercalation near the surface/edge of the material,thereby enhancing its pseudocapacitive sodium storage properties.Consequently,the strained and defective tin monosulfide/reduced graphene oxide composite demonstrates a high reversible capacity of 511.82 mAh g^(-1) at 1 A g^(-1) and an outstanding rate capability of 450.60 mAh g^(-1) at 3 A g^(-1).This study offers an effective strategy for improving sodium storage performance through lattice strain and defect engineering.展开更多
The high band gap of zinc oxide(ZnO)has significantly limited its potential application for organic contaminant removal in photocatalysis.In this study,ZnO/halloysites(HNTs)composites(ZnO/HNTs)were prepared using a hi...The high band gap of zinc oxide(ZnO)has significantly limited its potential application for organic contaminant removal in photocatalysis.In this study,ZnO/halloysites(HNTs)composites(ZnO/HNTs)were prepared using a high-temperature calcination method to enhance the removal of tetracycline hydrochloride(TCH).The experimental results demonstrated that the band gap of ZnO/HNTs decreased to 3.12 eV,compared to 3.21 eV for pure ZnO.The observed removal rate(k_(obs))of TCH in the ZnO/HNTs/vis system was 1.90×10^(-2) min^(-1),significantly higher than the rates in the HNTs/vis(1.25×10^(-3)min^(-1))and ZnO/vis(1.13×10^(-2) min^(-1))systems.Additionally,ZnO/HNTs exhibited strong resistance to coexisting natural organic and inorganic matter,maintaining high pollutant removal efficiency in natural water samples.The ZnO/HNTs/vis system also effectively removed other common organic pollutants,such as ciprofloxacin and methylene blue.Cycle tests indicated that the ZnO/HNTs/vis system retained 65.57%of its original efficiency,demonstrating good reusability and versatility.Scavenging and electron paramagnetic resonance experiments identified that h+was the primary species in the ZnO/HNTs/vis system,with other species playing auxiliary roles in TCH degradation.This study provides valuable insights into the design of novel ZnO-based photocatalysts for the degradation of organic pollutants in water.展开更多
The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging.Therefore,an efficient and low-cost catalys...The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging.Therefore,an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process.In this study,a Co_(3)O_(4)–CeO2 composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation.This catalyst exhibited a higher selectivity to KA-oil,which was benefited from the synergistic effects between Co^(3+))/Co^(2+))and Ce^(4+)/Ce^(3+)redox pairs,than bulk CeO2 and/or Co_(3)O_(4).Under the optimum reaction conditions,89.6%selectivity to KA-oil with a cyclohexane conversion of 5.8%was achieved over Co_(3)O_(4)–CeO2.Its catalytic performance remained unchanged after five runs.Using the synergistic effects between the redox pairs of different transition metals,this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.展开更多
Emission of volatile organic compounds has important influence on complex air pollution and human health.In this paper,a series of tungsten-iron composite oxides with different proportions and preparation methods were...Emission of volatile organic compounds has important influence on complex air pollution and human health.In this paper,a series of tungsten-iron composite oxides with different proportions and preparation methods were synthesized and first used for catalytic combustion of chlorobenzene and toluene,as typical polluting gas sources.These WO_(3)-based solid catalytic materials were systematically characterized by modern analytical methods,and the results showed that there was strong electron interaction between W and Fe elements in the composite oxides,and the presence of a certain amount of tungsten oxide inhibited the crystallization of iron oxide,and vice versa,which were beneficial to the uniform dispersion of tungsten-iron components into each other and the improvement of redox properties.Compared with single-component oxide,the formation of tungsten-iron composite oxide affected the micro-structure,improved the specific surface area and optimized the pore structure of materials.The performance test results showed that the tungsten-iron composite oxide(FeWO_4-0.5 Fe_(2)O_(3),molar ratio of tungsten and iron was 1/2)prepared using citric acid-based sol-gel method was the optimal,and its catalytic degradation efficiency could reach 90%for chlorobenzene and 83%for toluene at 320℃,and maintain at least 60 h without obvious deactivation,with high selectivity to the formation of HCl and CO_(2).展开更多
This review provides insight into the current research trend in transition metal oxides(TMOs)-based photocatalysis in removing the organic colouring matters from water.For easy understanding,the research progress has ...This review provides insight into the current research trend in transition metal oxides(TMOs)-based photocatalysis in removing the organic colouring matters from water.For easy understanding,the research progress has been presented in four generations according to the catalyst composition and mode of application,viz:single component TMOs(the firstgeneration),doped TMOs/binary TMOs/doped binary TMOs(the second-generation),inactive/active support-immobilized TMOs(the third-generation),and ternary/quaternary compositions(the fourth-generation).The first two generations represent suspended catalysts,the third generation is supported catalysts,and the fourth generation can be suspended or supported.The review provides an elaborated comparison between suspended and supported catalysts,their general/specific requirements,key factors controlling degradation,and the methodologies for performance evaluation.All the plausible fundamental and advanced dye degradation mechanisms involved in each generation of catalysts were demonstrated.The existing challenges in TMOs-based photocatalysis and how the researchers approach the hitch to resolve it effectively are discussed.Future research trends are also presented.展开更多
p-block metal composite oxides Sr_(1.36)Sb_(2)O_(6) and Sr_(2)Sb_(2)O_(7) synthesized by a hydrothermal method as photocatalysts in the degradation of tetracycline hydrochloride under UV light irradiation have been ex...p-block metal composite oxides Sr_(1.36)Sb_(2)O_(6) and Sr_(2)Sb_(2)O_(7) synthesized by a hydrothermal method as photocatalysts in the degradation of tetracycline hydrochloride under UV light irradiation have been extensively studied.The effects of synthesis conditions on the photocatalytic activity were discussed.The Sr_(1.36)Sb_(2)O_(6)-100°C-24 h-5 and Sr_(2)Sb_(2)O_(7)-150℃-24 h^(-2) samples prepared under optimal conditions exhibited remarkably different photocatalytic activities.The essential factors influencing the difference of photocatalytic performance were revealed.The results showed that the different photocatalytic activities observed for Sr_(1.36)Sb_(2)O_(6)and Sr_(2)Sb_(2)O_(7) could be attributed to their different electronic and crystal structures.Our work will provide a new perspective for the screening and design of p-block metal composite oxide photocatalysts to enhance the removal of organic pollutants in the environment.展开更多
Mesoporous CeO2-MnOx binary oxides with different Mn/Ce molar ratios were prepared by hydrothermal synthesis and characterized by scanning electron microscopy （SEM）, N2 sorption, X-ray diffraction （XRD）, X-ray pho...Mesoporous CeO2-MnOx binary oxides with different Mn/Ce molar ratios were prepared by hydrothermal synthesis and characterized by scanning electron microscopy （SEM）, N2 sorption, X-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and H2 temperature-programmed reduction （H2-TPR）. The characterization results indicated that the CeO2-MnOx catalysts exhibited flower-like microspheres with high specific surface areas, and partial Mn cations could be incorporated into CeO2 lattice to form solid solution. The CeO2-MnOx catalysts showed better catalytic activity for CO oxidation than that prepared by the coprecipitation method. Furthermore, the CeO2-MnOx catalyst with Mn/Ce molar ratio of 1 in the synthesis gel （Ce-Mn-1） exhibited the best catalytic activity, over which the conversion of CO could achieve 90% at 135 ℃. This was ascribed to presence of more Mn species with higher oxida- tion state on the surface and the better reducibility over the Ce-Mn-I catalyst than other CeO2-MnOx catalysts.展开更多
基金Project(2008BAB35B04) supported by the National Key Technology R&D Program of China
文摘Series Li-Sb-Mn composite oxides with different Sb/Mn molar ratios were obtained by solid state reaction.Their structure,morphology and Li^＋ extraction/adsorption properties were characterized by X-ray diffractometry （XRD）,scanning electron microscopy （SEM） and atomic absorption spectrophotometry （AAS）,respectively.XRD and SEM analyses reveal that the crystal of the products transfers from spinel to orthorhombic phase with the increase of molar ratio of Sb to Mn from 0.05 to 1.00.The Li^＋ extraction and adsorption experiments for these Li-Sb-Mn composite oxides demonstrate that the composite oxides can all be used as lithium inorganic adsorbents.The acid treated spinel Li-Sb-Mn composite oxide with Sb/Mn molar ratio of 0.05 has a high Li^＋ adsorption capacity of 33.23mg/g in lithium solution.The Sb/Mn molar ratio of these Li-Sb-Mn composite oxides should be a crucial factor in determining their structure and Li^＋ extraction and adsorption properties.
基金supported by the National Natural Science Foundation of China(21577088)~~
文摘The composite oxides xAg/Co_（0.93）Ce_（0.07）（x=Ag/（Co＋Ce） molar ratio）,intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on the performance of these substances during soot combustion were subsequently investigated.Under O_2,the 0.3Ag/Co_（0.93）Ce_（0.07） catalyst resulted in the lowest ignition temperature,T_（10）,of197 ℃,while the minimum light-off temperature was obtained from both 0.2Ag/Co_（0.93）Ce_（0.07） and0.3Ag/Co_（0.93）Ce_（0.07） in the NO_x atmosphere.These materials were also characterized by various techniques,including H_2,soot and NO_x temperature programmed reduction,X-ray diffraction,and electron paramagnetic resonance,Raman,X-ray photoelectron,and Fourier transform infrared spectroscopic analyses.The results demonstrated that silver significantly alters the catalytic behavior under both O_2 and NO_x,even though the lattice structure of the mixed oxide is not affected.Surface silver oxides generated under the O_2 atmosphere favor soot combustion by participating in the redox cycles between soot and the silver oxide,whereas the AgNO_3 that forms in a NO_x-rich atmosphere facilitates soot abatement at a lower temperature.The inferior activity of AgNO_3 relative to that of Ag_2O results in the different catalytic performance in the presence of NO_x or O_2.
基金the State Key Fundamental Research Program(Ministry of Science and Technology of China,No.2011CBA00501)Shanghai Municipal Science and Technology Commission,China(Grant No:11DZ1200300)the Foundation of State Key Laboratory of Coal Conversion(Grant No:1112610)
文摘Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product fraction in hydrocarbon distribution was rather low, demonstrating a promising potential in higher alcohols synthesis from syngas. The distribution of alcohols and hydrocarbons approximately obeyed Anderson-Schulz-Flory distribution with similar chain growth probability, indicating alcohols and hydrocarbons derived from the same intermediates. The effects of Cu/Fe molar ratio, reaction temperature and gas hourly space velocity （GHSV） on catalytic performance were studied in detail. The sample with a Cu/Fe molar ratio of 10/1 exhibited the best catalytic performance. Higher reaction temperature accelerated water-gas-shift reaction and led to lower total alcohols selectivity. GHSV showed great effect on catalytic performance and higher GHSV increased the total alcohol selectivity, indicating there existed visible dehydration reaction of alcohol into hydrocarbon.
基金Project supported by National Natural Science Foundation of China(20976120)Natural Science Foundation of Tianjin(09JCYBJC06200)
文摘The nano-crystalline Cu-Ce-Zr-O composite oxides were successfully prepared by the supercritical anti-solvent （SAS） process. The physicochemical properties and catalytic performances were investigated by X-ray diffraction （XRD）, Raman spectroscopy, H2 temperature-programmed reduction （H2 -TPR）, oxygen storage capacity （OSC） measurement and catalytic activity evaluation. It was found that Cu2＋ ions incorporated into CeO2 -ZrO2 lattice to form Cu-Ce-Zr-O solid solution associated with the formation of oxygen vacancies. The Cu-Ce-Zr-O catalysts prepared via the SAS process with the Cu content 2.63 mol.% showed the highest OSC index of 636.9 μmol/g. Compared with the samples prepared by impregnation method, Cu doping using SAS process could improve the dispersion of Cu2＋ in the composite oxide, enhance the interaction between Cu2＋ and CeO2-ZrO2 , improve the reducibility of catalyst, and thus improve the OSC performance and increase the catalytic activity for CO oxidation at low temperature.
基金Project supported by the Twelfth Five-Year National Science and Technology Pillar Program(2012BAE01B02)National Development and Reform Commission Fund:Development and commercialization of the rare earth based automotive catalytic converter for national V automotive emission standard
文摘Cerium-zirconium composite oxides with high performance were synthesized by a co-precipitation method, using zirconium oxychloride and rare earth chloride as raw materials. The effects of precipitate aging time on the properties of cerium-zirconium composite oxides were investigated. The prepared cerium-zirconium composite oxides were characterized by X-ray diffraction（XRD）, BET specific surface area, pulsed oxygen chemical adsorption, H2 temperature-programmed-reduction（H2-TPR）, scanning electron microscopy（SEM）, etc. The results showed that the precipitate aging time caused great effects on the properties of cerium zirconium composite oxides. With the increase of aging time, the cerium zirconium composite oxides showed enhanced specific surface area, good thermal stability, and high oxygen storage capacity（OSC）. The best performance sample was obtained while the precipitate aging time up to 48 h, with the specific surface area of 140.7 m2/g, and OSC of 657.24 μmolO2/g for the fresh sample. Even after thermal aged under 1000 oC for 4 h, the aged specific surface area was 41.6 m2/g, moreover with a good OSC of 569.9 μmolO2/g.
基金Project(50174059)supported by the National Natural Science Foundation of ChinaProject(Y406469)supported by Natural Science Foundation of Zhejiang Province
文摘With sol-gel method,nanometer La-Ti composite oxides were prepared.By means of atomic force microscope,the surface pattern,particle size distribution and specific surface area were studied.The newly prepared nanocrystals of La-Ti composite oxides were used as the catalysts to catalyze the dehydration of external compensated lactic acid to lactide.The lactide product was measured by polarimeter and micropolariscope.The results demonstrate that the ratio between D-lactide and L-lactide will not be equal to 1-1 if nanocrystals of La-Ti composite oxides are used as the catalysts,which implies,that nanocrystals of La-Ti composite oxides may be potential catalysts with a good selectivity.
文摘The composition,structure and micro-morphology of magnesium- iron- aluminum composite oxides were investigated using various methods such as XRF,SEM,EDS,XRD and KMn O4-titration. Compared to hercynite,the composite oxides have completely different phases including solid solution（ Mg O）0. 77（ Fe O）0. 23,composite spinel Mg Fe0. 2Al1. 8O4 and a small amount of Mg Fe2O4. The composite oxides exhibit excellent corrosion resistance to cement clinker and potassium salts.The products produced by magnesite and the composite oxides show better performance than magnesia- hercynite bricks,especially the corrosion resistance and thermal shock resistance.
基金supported by the National Natural Science Foundation of China(21172269)Innovation Group of Hubei Natural Science Foundation(2018CFA023)Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices,Ministry of Education,Jianghan University(JDGD-201809)~~
文摘Vanadium‐chromium oxides(VCrO)were usually prepared by high‐temperature solid‐state reactions;however,mixed phases were frequently produced and the morphology of the products was not well controlled.In this work,we prepared amorphous VCrO precursors by using V2O5 and CrO3 and alcohols or mixtures of alcohol and water via solvothermal reaction at 180°C.The precursors were then calcined under nitrogen at various temperatures.The products were characterized by powder X‐ray diffraction,transmission electron microscopy,and X‐ray photoelectron spectroscopy.It was revealed that pure‐phase nanocrystalline orthorhombic CrVO4 was obtained when methanol or methanol/water was used as the solvothermal medium and the precursor was calcined at 700°C.The size of the CrVO4 crystals was around 500 nm when methanol was used,whereas it reduced significantly to less than 50 nm when a mixture of methanol and water was used.The sizes could be effectively tuned from 10 to 50 nm by varying the methanol/water volume ratio.To the best of our knowledge,this is the first report on the synthesis of pure‐phase CrVO4 nanocrystals.The nano‐CrVO4 showed almost the highest catalytic activity for the ammoxidation of 2,6‐dichlorotoluene to 2,6‐dichlorobenzonitrile among the reported bi‐component composite oxides,owing to its smaller particle size,larger specific surface area,and more exposed active centers.
基金Project(14JJ4043)supported by the Natural Science Foundation of Hunan Province,China
文摘Three La-doped CeO2-ZrO2-Al2O3(CZA)composite oxide samples,namely,CZA-I,CZA-II and CZA-III,were prepared following a co-precipitation method in the presence of La2O3,La(NO3)3-6H2O and H[La(EDTA)]-16H2O precursors,respectively.When the precursor samples are sintered at 1000°C,the as-prepared composite oxides mainly exhibit the CeO2-ZrO2 cubic fluorite phase,while theγ-Al2O3 andδ-Al2O3 phases appear when the precursor samples are subjected to sintering at 1100 and 1200°C.CZA-III exhibits improved redox properties after high-temperature treatment compared with CZA-I and CZA-II.CZA-III presents the largest surface area of 97.46 m2/g among the three CZAs when the CZA-III precursor sample is sintered at 1000°C.Furthermore,the corresponding oxygen storage capacity(OSC)is the largest with value of 400.27μmol/g when CZA-III precursor sample is sintered at 1000°C.Additionally,CZA-III exhibits the best thermal stability and the highest reduction temperature.However,by increasing the sintering temperature to 1200°C,there is a dramatic decline in the properties of surface area and OSC.And a decrease for CZA-III in surface area by 58.94%and a decrease of the OSC value by 74.56%are observed.
文摘CO2-TPD was demonstrated an effective way to investigate the phase formation during pyrolysis for the preparation of composite oxides using metal-organic molecules as precursors.Based on the CO2-TPD results, it was found that calcination condition had deep effect on the carbonate formation and the minimum firing temperature to acquire pure phase composite oxide.An optimized calcination schedule was then developed.
基金Project(2008BAB35B04) supported by the National Key Technology R&D Program of ChinaProject(CX2010B111) supported by the Innovation Program of Doctoral Research of Hunan Province, ChinaProject(2010QZZD003) supported by Advanced Research Program of Central South University, China
文摘A series of spinel Li-Mn-Ni composite oxides with theoretical chemical formula of LiNixMn2-xO4 （0〈_x〈_1.0） were synthesized by liquid phase method. Their structure and morphology were characterized by X-ray diffractometry （XRD） and scanning electron microscopy （SEM）, respectively. The stability of these Ni-substituted spinel oxides prepared at different temperatures was investigated in acidic medium as well. The results show that Ni can be brought into the spinel framework completely to form well-crystallized product when x〈_0.5 and the optimized synthesis temperature is 800℃. LiNi0.4Mn1.6O4 prepared at 800℃ can maintain the spinel structure and morphology with Li extraction ratio of 30.37%, Mn extraction ratio of 8.78% and Ni extraction ratio of 1,82% during acid treatment. The incorporated Ni not only inhibits the dissolution of Mn, but also reduces the extraction of Li due to the lattice contraction
基金Project supported by the National Natural Science Foundation of China(22176123,U1832155)the National Key Research&Development Plan(2017YFC0211804).
文摘Plasma-coupled catalysis is a promising volatile organic co mpounds(VOCs) removal technology because of its interactional principles of plasma decomposition and catalytic oxidation.However,the problem of harmful by-products is still in trouble.A series of rare earth doped RE-NiO_(x)(RE=Ce,Y,La) composite oxides were synthesized by metal organic frameworks(MOFs)-derived method for coupled plasma oxidation of benzene and by-product ozone removal.Compared with plasma alone,the 1%La-NiO_(x)catalyst shows the best enhancement of 50% for benzene conversion with complete removal of a maximum of 800 ppm ozone.The energy consumption for 90% benzene removal efficiency(η90%) is also reduced from 3600 to 1200 J/L.Characterization re sults of RE-NiO_(x) catalysts indicate that the doping of La causes interaction and synergistic effect between La and Ni,and the surface oxygen and lattice oxygen with defects play crucial roles in benzene oxidation and ozone decomposition,respectively.In addition,the decomposition mechanism of benzene and ozone under plasma is proposed.Plasma is responsible for the indiscriminate bond breaking in benzene and oxygen to form a variety of organic intermediates and ozone,while the La-NiO_(x) catalyst selectively oxidizes the intermediates to CO_(x)/H2O and decomposes the ozone into oxygen.
基金Funded by the National Natural Science Foundation of China(No.52271066)Basic Research and Innovation Project for Vehicle Power+1 种基金Key Project of"Two-Chain Integration"in Shaanxi Province(No.2023-LL-QY-33-3)Xi'an Key Laboratory of Corrosion Protection and Functional Coating Technology for Military and Civil Light Alloy and Key Project of Shaanxi Natural Science Foundation Research Program(No.2021JZ-54)。
文摘A novel type of microcapsule-encapsulated corrosion inhibitor was prepared in a water-based solution with a pH range of 7-8,and it was applied to the composite organic coating of magnesium alloy plasma electrolytic oxidation to enhance its corrosion resistance and self-healing properties.The morphology,chemical composition,structure,and functional properties of the composite coating were investigated by scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDS),Fourier transform infrared spectroscopy(FTIR),polarization curve,alternating current impedance,and salt immersion test.The experimental results showed that,after immersion in a 3.5 wt%NaCl solution for 12 h,the coating could effectively protect AZ91D from corrosion.When the coating was damaged,the exposed alloy surface would release metal ions in the corrosive environment and react with the corrosion inhibitor 8-hydroxyquinoline to form a Mg(8-HQ)_(2) chelate,exhibiting significant self-healing behavior.The study results demonstrate the broad application prospects of microcapsule technology in the coating field,providing new ideas for the development of efficient anti-corrosion coatings.
基金supported by the National Natural Science Foundation of China(no.22109023,no.22179022,and no.22209027)the Youth Innovation Fund of Fujian Province(no.2021J05043 and no.2022J05046)+5 种基金the National Key Research and Development Program of China(2023YFC3906300)the FuXiaQuan National Independent Innovation Demonstration Zone Collaborative Innovation Platform(no.2022-P-027)the·“Hundred Talents·Plan”of Fujian Provincethe“Top Young Talents of Young Eagle”Program of Fujian Provincethe Award Program for Fujian Minjiang Scholar Professorshipthe Talent Fund Program of Fujian Normal University.
文摘Sodium-ion batteries have garnered significant attention as a cost-effective alternative to lithium-ion batteries due to the abundance and affordability of sodium precursors.However,the lack of suitable electrode materials with both high capacity and excellent stability continues to hinder their practical viability.Herein,we couple lattice strain and sulfur deficiency effects in a tin monosulfide/reduced graphene oxide composite to enhance sodium storage performance.Experimental results and theoretical calculations reveal that the synergistic effects of lattice strain and sulfur vacancies in tin monosulfide promote rapid(de)intercalation near the surface/edge of the material,thereby enhancing its pseudocapacitive sodium storage properties.Consequently,the strained and defective tin monosulfide/reduced graphene oxide composite demonstrates a high reversible capacity of 511.82 mAh g^(-1) at 1 A g^(-1) and an outstanding rate capability of 450.60 mAh g^(-1) at 3 A g^(-1).This study offers an effective strategy for improving sodium storage performance through lattice strain and defect engineering.
基金financially supported by the National Natural Science Foundation of China(Nos.52270149,51908528,2200013)Natural Science Foundation of Henan Province,China(No.242300421443)+1 种基金The Science and Technology Key Project of Henan Province,China(No.242102321073)Doctoral Fund Project of Henan University of Technology,China(Nos.2020BS005,2023BS004).
文摘The high band gap of zinc oxide(ZnO)has significantly limited its potential application for organic contaminant removal in photocatalysis.In this study,ZnO/halloysites(HNTs)composites(ZnO/HNTs)were prepared using a high-temperature calcination method to enhance the removal of tetracycline hydrochloride(TCH).The experimental results demonstrated that the band gap of ZnO/HNTs decreased to 3.12 eV,compared to 3.21 eV for pure ZnO.The observed removal rate(k_(obs))of TCH in the ZnO/HNTs/vis system was 1.90×10^(-2) min^(-1),significantly higher than the rates in the HNTs/vis(1.25×10^(-3)min^(-1))and ZnO/vis(1.13×10^(-2) min^(-1))systems.Additionally,ZnO/HNTs exhibited strong resistance to coexisting natural organic and inorganic matter,maintaining high pollutant removal efficiency in natural water samples.The ZnO/HNTs/vis system also effectively removed other common organic pollutants,such as ciprofloxacin and methylene blue.Cycle tests indicated that the ZnO/HNTs/vis system retained 65.57%of its original efficiency,demonstrating good reusability and versatility.Scavenging and electron paramagnetic resonance experiments identified that h+was the primary species in the ZnO/HNTs/vis system,with other species playing auxiliary roles in TCH degradation.This study provides valuable insights into the design of novel ZnO-based photocatalysts for the degradation of organic pollutants in water.
基金supported by Key Research and Development Program in Hunan Province(Grant No.2019GK2041)Hunan Provincial Natural Science Foundation of China(Grant No.2019JJ50579)+3 种基金Scientific Research Fund of Hunan Provincial Education Department(Grant Nos.18C0106 and 20B550)the fund of the Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education&Hubei Key Laboratory of Catalysis and Materials Science(Grant No.CHCL21004)National Training Program of Innovation and Entrepreneurship for Undergraduates(Grant No.S202010530022)and Hunan Key Laboratory of Environment Friendly Chemical Process Integrated Technology and Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization.
文摘The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging.Therefore,an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process.In this study,a Co_(3)O_(4)–CeO2 composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation.This catalyst exhibited a higher selectivity to KA-oil,which was benefited from the synergistic effects between Co^(3+))/Co^(2+))and Ce^(4+)/Ce^(3+)redox pairs,than bulk CeO2 and/or Co_(3)O_(4).Under the optimum reaction conditions,89.6%selectivity to KA-oil with a cyclohexane conversion of 5.8%was achieved over Co_(3)O_(4)–CeO2.Its catalytic performance remained unchanged after five runs.Using the synergistic effects between the redox pairs of different transition metals,this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.
基金financially supported by the Zhejiang Provincial Natural Science Foundation(Grant No.LQ19B030004)the National Natural Science Foundation of China(NSFC,Grant Nos.21906106 and 21808048)the soft science research project of Shaoxing Association of Science and Technology。
文摘Emission of volatile organic compounds has important influence on complex air pollution and human health.In this paper,a series of tungsten-iron composite oxides with different proportions and preparation methods were synthesized and first used for catalytic combustion of chlorobenzene and toluene,as typical polluting gas sources.These WO_(3)-based solid catalytic materials were systematically characterized by modern analytical methods,and the results showed that there was strong electron interaction between W and Fe elements in the composite oxides,and the presence of a certain amount of tungsten oxide inhibited the crystallization of iron oxide,and vice versa,which were beneficial to the uniform dispersion of tungsten-iron components into each other and the improvement of redox properties.Compared with single-component oxide,the formation of tungsten-iron composite oxide affected the micro-structure,improved the specific surface area and optimized the pore structure of materials.The performance test results showed that the tungsten-iron composite oxide(FeWO_4-0.5 Fe_(2)O_(3),molar ratio of tungsten and iron was 1/2)prepared using citric acid-based sol-gel method was the optimal,and its catalytic degradation efficiency could reach 90%for chlorobenzene and 83%for toluene at 320℃,and maintain at least 60 h without obvious deactivation,with high selectivity to the formation of HCl and CO_(2).
基金supporting us by providing technical facilities(access to journals)。
文摘This review provides insight into the current research trend in transition metal oxides(TMOs)-based photocatalysis in removing the organic colouring matters from water.For easy understanding,the research progress has been presented in four generations according to the catalyst composition and mode of application,viz:single component TMOs(the firstgeneration),doped TMOs/binary TMOs/doped binary TMOs(the second-generation),inactive/active support-immobilized TMOs(the third-generation),and ternary/quaternary compositions(the fourth-generation).The first two generations represent suspended catalysts,the third generation is supported catalysts,and the fourth generation can be suspended or supported.The review provides an elaborated comparison between suspended and supported catalysts,their general/specific requirements,key factors controlling degradation,and the methodologies for performance evaluation.All the plausible fundamental and advanced dye degradation mechanisms involved in each generation of catalysts were demonstrated.The existing challenges in TMOs-based photocatalysis and how the researchers approach the hitch to resolve it effectively are discussed.Future research trends are also presented.
基金financially supported by the National Natural Science Foundation of China(21875037,51502036)the National Key Research and Development Program of China(2016YFB0302303,2019YFC1908203)the Natural Science Foundation of Distinguished Young Scholars of Fujian Province(2019J06015)。
文摘p-block metal composite oxides Sr_(1.36)Sb_(2)O_(6) and Sr_(2)Sb_(2)O_(7) synthesized by a hydrothermal method as photocatalysts in the degradation of tetracycline hydrochloride under UV light irradiation have been extensively studied.The effects of synthesis conditions on the photocatalytic activity were discussed.The Sr_(1.36)Sb_(2)O_(6)-100°C-24 h-5 and Sr_(2)Sb_(2)O_(7)-150℃-24 h^(-2) samples prepared under optimal conditions exhibited remarkably different photocatalytic activities.The essential factors influencing the difference of photocatalytic performance were revealed.The results showed that the different photocatalytic activities observed for Sr_(1.36)Sb_(2)O_(6)and Sr_(2)Sb_(2)O_(7) could be attributed to their different electronic and crystal structures.Our work will provide a new perspective for the screening and design of p-block metal composite oxide photocatalysts to enhance the removal of organic pollutants in the environment.
基金supported by National Basic Research Program of China(2010CB732300,2013CB933201)National High Technology Research and Development Program of China(2011AA03A406,2012AA062703)+2 种基金the National Natural Science Foundation of China(21103048,21273150)Shu Guang Project of Shanghai Municipal Education CommissionShanghai Education Development Foundation(10SG30)
文摘Mesoporous CeO2-MnOx binary oxides with different Mn/Ce molar ratios were prepared by hydrothermal synthesis and characterized by scanning electron microscopy （SEM）, N2 sorption, X-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and H2 temperature-programmed reduction （H2-TPR）. The characterization results indicated that the CeO2-MnOx catalysts exhibited flower-like microspheres with high specific surface areas, and partial Mn cations could be incorporated into CeO2 lattice to form solid solution. The CeO2-MnOx catalysts showed better catalytic activity for CO oxidation than that prepared by the coprecipitation method. Furthermore, the CeO2-MnOx catalyst with Mn/Ce molar ratio of 1 in the synthesis gel （Ce-Mn-1） exhibited the best catalytic activity, over which the conversion of CO could achieve 90% at 135 ℃. This was ascribed to presence of more Mn species with higher oxida- tion state on the surface and the better reducibility over the Ce-Mn-I catalyst than other CeO2-MnOx catalysts.
