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
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
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
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
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
The hydrogen permeation resistance of Si–Zr(SZ) and Si–Al(SA) composite sol oxide coating on zirconium hydride blocks(Zr H) was studied. SZ and SA composite sol were prepared by sol–gel method. SZ and SA composite ...The hydrogen permeation resistance of Si–Zr(SZ) and Si–Al(SA) composite sol oxide coating on zirconium hydride blocks(Zr H) was studied. SZ and SA composite sol were prepared by sol–gel method. SZ and SA composite oxide coatings were prepared on the surface of Zr H(in situ oxidized or not) in turns by dip-coating and heat treatment. Hydrogen permeation of Zr Hwith and without composite oxide coating was compared.Hydrogen desorption experiments in thermal vacuum show that hydrogen permeation resistance of SA composite oxide coating is better than that of SZ, to a certain extent,which could decrease hydrogen thermal loss. Experimental results in the working condition show that the SA composite oxide coating can not only prevent hydrogen permeation, but also retard contact and reaction between COand Zr Hmatrix, which could mitigate excessive oxidation of in situ oxide film. Differential scanning calorimetry and thermogravimetry(DSC–TG) analysis was performed to investigate the decomposition behavior of SA and SZ liquid sol in heat treatment process. X-ray diffraction(XRD) and scanning electron microscopy(SEM) analysis were employed to characterize the phase composition,surface and cross-section morphology of the coatings.展开更多
Iron-manganese composited oxide（FeMnO） was prepared with potassium permanganate and ferrous salt. Interface performance, charge property and structure topography of the FeMnO were investigated. Coagulation efficienc...Iron-manganese composited oxide（FeMnO） was prepared with potassium permanganate and ferrous salt. Interface performance, charge property and structure topography of the FeMnO were investigated. Coagulation efficiency and pollution removal mechanism of the FeMnO were approached. Results show that the main compositions of the FeMnO are δ-manganese dioxide and ferric hydroxide. The specific surface area is about 146.22 m^2/g. The FeMnO contains rich hydroxyl with extremely strong adsorption action and chemical adsorption activity. The zero charge point of the oxide in pure water is about 8.0 of pH value. Under neutral pH value conditions, the FeMnO particle surface carried positive charges. The FeMnO particles are quasi-spherical micro-particles with irregular sizes adjoined each other to form net construction. Phosphorus removal efficiency of the FeMnO is remarkable, the total dissoluble phosphorus of settled water can be reduced below detecting level（0.3 μtg/L） at a FeMnO dosage of 6 mg/L, and total phosphorus below detecting level at a FeMnO dosage of 10 mg/L, for water samples containing total phos- phorus of 1281.70 μg/L and total dissoluble phosphorus of 1187.91 μtg/L. The mechanism of effective coagulation for phosphorus removal is combined results of multiple actions of adsorption, charge neutralization, adsorption/bridging and so on.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
In this work,p-type Co3O4 decorated n-type ZnO(Co3O4/ZnO)nanocomposite was designed with the assistance of bacterial cellulose template.Phase composition,morphology and element distribution were investigated by XRD,SE...In this work,p-type Co3O4 decorated n-type ZnO(Co3O4/ZnO)nanocomposite was designed with the assistance of bacterial cellulose template.Phase composition,morphology and element distribution were investigated by XRD,SEM,HRTEM,EDS mapping and XPS.Volatile organic compounds(VOCs)sensing measurements indicated a noticeable improvement of response and decrease of working temperature for Co3O4/ZnO sensor,in comparison with pure ZnO,i.e.,the response towards 100 ppm acetone was 63.7(at a low working temperature of 180℃),which was 26 times higher than pure ZnO(response of 2.3 at 240℃).Excellent VOCs response characteristics could be ascribed to increased surface oxygen vacancy concentration(revealed by defect characterizations),catalytic activity of Co3O4 and the special p-n heterojunction structure,and bacterial cellulose provides a facile template for designing diverse functional heterojunctions for VOCs detection and other applications.展开更多
A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation.It was ...A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation.It was demonstrated that Co3O_(4)phase was the main component in regulation.The combined results of X-ray photoelectron spectroscopy (XPS),temperature-programmed desorption of oxygen (O_(2)-TPD),temperature-programmed reduction of hydrogen (H_(2)-TPR),temperature-programmed desorption of ammonia/carbon dioxide (NH_(3)/CO_(2)-TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co_(2)+,lower surface basicity and optimized acidity,which were beneficial for adsorption of active oxygen species and activation of methane molecules,resulting in the excellent catalytic oxidation performance.Especially,the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T50and T90(the temperature at which the CH_(4)conversion rate was 50%and 90%,respectively) were 318 and 367℃,respectively.Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization,it was also found that the catalytic mechanism changes from the “Rideal-Eley” mechanism to the “Two-term” mechanism depending on the temperature windows in which the reaction takes place.Besides,the use of the “Flynn-Wall-Ozawa” model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy,further expanding the application scope of carboncontaining composites.展开更多
A coating of composition Si-40Mo (wt pct) was prepared by fused slurry coating method on the two-dimensional carbon/carbon (2D-C/C) composite to improve oxidation resistance. In the procedure of the fabrication, pure ...A coating of composition Si-40Mo (wt pct) was prepared by fused slurry coating method on the two-dimensional carbon/carbon (2D-C/C) composite to improve oxidation resistance. In the procedure of the fabrication, pure St slurry inner layer in the pre-coating was necessary to apply because of infiltration of liquid Si into the substrate during the sintering. The coating consists of Si continuous phase and MoSi2 particles. In addition, the infiltration of Si into the substrate and the SiC reaction layer between the coating and the C/C composite were observed. Oxidation behavior of coated and uncoated C/C composites was studied in cyclic mode. The oxidation resistance and the thermal shock resistance of the Si-Mo fused slurry coating were quite excellent at 1370℃.展开更多
Pt-free counter electrode(CE) composed of La2 MoO(LaO-MoO) was successfully synthesized by simple pyrolysis of lanthanum acetate(CHOLa·xHO) and hexaammonium heptamolybdate tetrahydrate((NH4)6 MoO·4 HO). Furt...Pt-free counter electrode(CE) composed of La2 MoO(LaO-MoO) was successfully synthesized by simple pyrolysis of lanthanum acetate(CHOLa·xHO) and hexaammonium heptamolybdate tetrahydrate((NH4)6 MoO·4 HO). Furthermore,three proportions composites catalysts of La2 MoO@MWCNTs based on La2 MoOand multiwall carbon nanotubes(MWCNTs) were prepared and characterized as Ptfree catalyst for CE in dye-sensitized solar cells(DSSCs). The morphology and structure of La2 MoO@MWCNTs composites were determined by scanning electron microscopy, transmission electron microscope and X-ray diffraction. The electrochemical performance of La2 MoO@MWCNTs composite catalysts for CEs was determined by photocurrent-voltage measurements, cyclic voltammetry,electrochemical impedance spectroscopy, and Tafel polarization. The power conversion efficiencies of4.68%, 4.87% and 5.06% are obtained for La2 MoO:MWCNTs with the mass ratios of 5:1, 3:1 and 1:1 towards the reduction of I~-to I~-under the same conditions,respectively,which are superior to those of MWCNTs(3,94%) and La2 MoO(1.71%) electrodes. The experimental results reveal that the presence of MWCNTs results in an augmented active catalytic surface area and enhanced charge transfer from CE to the electrolyte.展开更多
Al specimens were covered with TiO2 film by sol-gel dip-coating and then anodized in ammonium adipate solution.The structure,composition and capacitance properties of the anodic oxide film were investigated by transmi...Al specimens were covered with TiO2 film by sol-gel dip-coating and then anodized in ammonium adipate solution.The structure,composition and capacitance properties of the anodic oxide film were investigated by transmission electron microscopy (TEM),Auger electron spectroscopy (AES),X-ray diffractometry (XRD) and electrochemical impedance spectroscopy (EIS).It was found that an anodic oxide film with a dual-layer structure formed between TiO2 coating and Al substrate.The film consisted of an inner Al2O3 layer and an outer Ti-Al composite oxide layer.The thickness of layers varied with the number of times of sol-gel dip-coating.The capacitance of anodic oxide films formed on coated specimens was at most 80% higher than that without TiO2.In film formation mechanism,it was claimed that the formation of composite oxide film was mainly affected by the structure of micro-pores network in TiO2 coating which had an influence on Al3+ and O2? ions transport during the anodizing.展开更多
A series of novel Ni/CeOe-Al2O3 composite catalysts were synthesized by one-step citric acid complex method, The as-synthesized catalysts were characterized by N2 physical adsorption/desorption, X-ray diffraction （XR...A series of novel Ni/CeOe-Al2O3 composite catalysts were synthesized by one-step citric acid complex method, The as-synthesized catalysts were characterized by N2 physical adsorption/desorption, X-ray diffraction （XRD）, Fourier transform infrared （FT-IR） spectroscopy, hydrogen temperature-programmed reduction （Hz-TPR）, X-ray photoelectron spectroscopy （XPS） and thermogravimetry analysis （TGA）. The effects of nickel content, calcination and reaction temperatures, gas hourly space velocity （GHSV） and inert gas dilution of N2 on their performance of catalytic partial oxidation of methane （CPOM） were investigated. Catalytic activity test results show that the highest methane conversion （〉85%）, the best selectivities to carbon monoxide （〉87%） and to hydrogen （〉95%）, the excellent stability and perfect Hz/CO ratio （2.0） can be obtained over Ni/CeO2-Al2O3 with 8 wt% Ni content calcined at 700 ℃ under the reaction condition of 750 ℃, CH4/O2 ratio of 2 ： 1 and gas hourly space velocity of 12000 mL.h-1 .g-1. Characterization results show that the good catalytic performance of this composite catalyst can be contributed to its large specific surface area （~108 m2.g-1）, small crystallite size, easy reducibility and low coking rate.展开更多
The present paper discussed some fundamental aspects on composite oxide scales and coatings for protection of alloys from high temperature oxidation, the related thermodynamic conditions, special mechanical characteri...The present paper discussed some fundamental aspects on composite oxide scales and coatings for protection of alloys from high temperature oxidation, the related thermodynamic conditions, special mechanical characteristics and a sealing mechanism. It was proposed that the oxide scales and coatings with a composite structure should possess superior mechanical properties than that with a single phase oxide. It also showed that the A1203 scales or coatings doped with 3（203 and ZrO2 （or YSZ）-A1203 composite coatings possessed superior properties at high temperatures. In such composite oxide scales and coatings, the fracture resistance of the scales was increased by the toughening effect, the thermal stress was decreased owing to the increase of thermal-expansion coefficients, and A1203 phase could seal the alloy substrate well In addition, the kinetic equation of thermal growth oxide on alloy covered with composite oxide coatings was derived.展开更多
Ammonia borane(NH_(3)BH_(3),AB)has been regarded as a promising chemical hydrogen storage material owing to its high hydrogen density and superior stability.Thus,the development of low-cost and high-efficient heteroge...Ammonia borane(NH_(3)BH_(3),AB)has been regarded as a promising chemical hydrogen storage material owing to its high hydrogen density and superior stability.Thus,the development of low-cost and high-efficient heterogeneous catalysts for the dehydrogenation of AB has attracted considerable scholarly attention.In this study,heterostructured Co_(3)O_(4)-SnO_(2)catalysts containing oxygen vacancy(V_(o))with different Co/Sn atomic ratios(designated as V_(o)-Co-Sn_(5:x))were synthesized via a simple coprecipitation-calcination method under mild reaction conditions.The catalyst containing an optimized Co/Sn atomic ratio of 5:2(V_(o)-Co-Sn_(5:2))exhibited robust catalytic performance with a turnover frequency value of 17.6mol_(H2)·mol^(-1)_(metal)·min^(-1).Moreover,82.6%of the original activity of the catalyst was retained after 14 catalytic cycles,indicating the high stability of the catalyst.Diversified characterization combined with the density functional theory(DFT)calculation confirmed the transfer of electrons from Co_(3)O_(4)to Sn O_(2)and the distribution of the separated charges on SnO_(2)-Co_(3)O_(4)interface.The transfer of electrons and the distribution of charges facilitated the adsorption and activation of water on the catalyst,thus accelerating the dissociation of H_(2)O molecule(the ratedetermining step of AB hydrolysis).It was found that the V_(o)adjusted the electron structure of the catalysts rather than acted as active sites.These findings will provide researchers with useful information for designing cheap and highly efficient catalysts for catalytic AB hydrolysis.展开更多
The lanthanum aluminum mesoporous materials were synthesized using sodium dodecyl sulfate as a template agent by ultrasonic hydrothermal method.The resulting samples were characterized by low angle X-ray diffraction（...The lanthanum aluminum mesoporous materials were synthesized using sodium dodecyl sulfate as a template agent by ultrasonic hydrothermal method.The resulting samples were characterized by low angle X-ray diffraction（XRD）,N2 adsorption-desorption studies,transmission electron microscopy（TEM）and surface morphology analysis（SEM）,surface acid（NH3-TPD）,reducibility properties（TPR）,X-ray energy dispersive spectrometer（EDS）and thermogravimetric analysis（TG/DTG）.A l/La composite mesoporous material were synthesized with n（Al）︰n（La）=70︰1.0,80°C of reaction temperature,20 h of reaction time,12 h of crystallization time,650°C of calcination temperature.The specific surface area of the sample is 273.90 m 2 ·g ？1 ,with the average diameter 5.642 nm and pore volume 0.2354 cm 3 ·g ？1 .The samples have mesoporous structure and its particles are similar to a worm-shaped tubular structure.The influence of calcination temperature on the surface physical and chemical properties of Al/La composited mesoporous materials was examined,and the results showed that the acid strength was increased but the amount of acidic sites is decreased as the calcination temperature increased.It was found that the sample calcined at 650°C had appropriate acid content,acid strength and better reducibility.展开更多
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financially supported by the National Natural Science Foundation of China (No. 51404034)
文摘The hydrogen permeation resistance of Si–Zr(SZ) and Si–Al(SA) composite sol oxide coating on zirconium hydride blocks(Zr H) was studied. SZ and SA composite sol were prepared by sol–gel method. SZ and SA composite oxide coatings were prepared on the surface of Zr H(in situ oxidized or not) in turns by dip-coating and heat treatment. Hydrogen permeation of Zr Hwith and without composite oxide coating was compared.Hydrogen desorption experiments in thermal vacuum show that hydrogen permeation resistance of SA composite oxide coating is better than that of SZ, to a certain extent,which could decrease hydrogen thermal loss. Experimental results in the working condition show that the SA composite oxide coating can not only prevent hydrogen permeation, but also retard contact and reaction between COand Zr Hmatrix, which could mitigate excessive oxidation of in situ oxide film. Differential scanning calorimetry and thermogravimetry(DSC–TG) analysis was performed to investigate the decomposition behavior of SA and SZ liquid sol in heat treatment process. X-ray diffraction(XRD) and scanning electron microscopy(SEM) analysis were employed to characterize the phase composition,surface and cross-section morphology of the coatings.
基金Supported by National Natural Science Foundation of China(Nos.50378004 and 50678007)Beijing Natural Science Foun-dation(No.8082009)+1 种基金Science & Technology Development Programme of Beijing Municipal Commission of Education (No.KM200610005025)Academic Human Resources Development in Institutions of Higher Learning Under the Jurisdiction of Beijing Municipality(No. 05004014200701).
文摘Iron-manganese composited oxide（FeMnO） was prepared with potassium permanganate and ferrous salt. Interface performance, charge property and structure topography of the FeMnO were investigated. Coagulation efficiency and pollution removal mechanism of the FeMnO were approached. Results show that the main compositions of the FeMnO are δ-manganese dioxide and ferric hydroxide. The specific surface area is about 146.22 m^2/g. The FeMnO contains rich hydroxyl with extremely strong adsorption action and chemical adsorption activity. The zero charge point of the oxide in pure water is about 8.0 of pH value. Under neutral pH value conditions, the FeMnO particle surface carried positive charges. The FeMnO particles are quasi-spherical micro-particles with irregular sizes adjoined each other to form net construction. Phosphorus removal efficiency of the FeMnO is remarkable, the total dissoluble phosphorus of settled water can be reduced below detecting level（0.3 μtg/L） at a FeMnO dosage of 6 mg/L, and total phosphorus below detecting level at a FeMnO dosage of 10 mg/L, for water samples containing total phos- phorus of 1281.70 μg/L and total dissoluble phosphorus of 1187.91 μtg/L. The mechanism of effective coagulation for phosphorus removal is combined results of multiple actions of adsorption, charge neutralization, adsorption/bridging and so on.
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In this work,p-type Co3O4 decorated n-type ZnO(Co3O4/ZnO)nanocomposite was designed with the assistance of bacterial cellulose template.Phase composition,morphology and element distribution were investigated by XRD,SEM,HRTEM,EDS mapping and XPS.Volatile organic compounds(VOCs)sensing measurements indicated a noticeable improvement of response and decrease of working temperature for Co3O4/ZnO sensor,in comparison with pure ZnO,i.e.,the response towards 100 ppm acetone was 63.7(at a low working temperature of 180℃),which was 26 times higher than pure ZnO(response of 2.3 at 240℃).Excellent VOCs response characteristics could be ascribed to increased surface oxygen vacancy concentration(revealed by defect characterizations),catalytic activity of Co3O4 and the special p-n heterojunction structure,and bacterial cellulose provides a facile template for designing diverse functional heterojunctions for VOCs detection and other applications.
基金supported by the National Natural Science Foundation of China (No.U20A201714)Hebei Education Department (No.QN2021059)Natural Science Foundation of Hebei Province (Nos.B2021208033 and B2021208040)。
文摘A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation.It was demonstrated that Co3O_(4)phase was the main component in regulation.The combined results of X-ray photoelectron spectroscopy (XPS),temperature-programmed desorption of oxygen (O_(2)-TPD),temperature-programmed reduction of hydrogen (H_(2)-TPR),temperature-programmed desorption of ammonia/carbon dioxide (NH_(3)/CO_(2)-TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co_(2)+,lower surface basicity and optimized acidity,which were beneficial for adsorption of active oxygen species and activation of methane molecules,resulting in the excellent catalytic oxidation performance.Especially,the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T50and T90(the temperature at which the CH_(4)conversion rate was 50%and 90%,respectively) were 318 and 367℃,respectively.Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization,it was also found that the catalytic mechanism changes from the “Rideal-Eley” mechanism to the “Two-term” mechanism depending on the temperature windows in which the reaction takes place.Besides,the use of the “Flynn-Wall-Ozawa” model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy,further expanding the application scope of carboncontaining composites.
文摘A coating of composition Si-40Mo (wt pct) was prepared by fused slurry coating method on the two-dimensional carbon/carbon (2D-C/C) composite to improve oxidation resistance. In the procedure of the fabrication, pure St slurry inner layer in the pre-coating was necessary to apply because of infiltration of liquid Si into the substrate during the sintering. The coating consists of Si continuous phase and MoSi2 particles. In addition, the infiltration of Si into the substrate and the SiC reaction layer between the coating and the C/C composite were observed. Oxidation behavior of coated and uncoated C/C composites was studied in cyclic mode. The oxidation resistance and the thermal shock resistance of the Si-Mo fused slurry coating were quite excellent at 1370℃.
基金Project supported by the National Natural Science Foundation of China(21473048 and 21303039)the Natural Science Foundation of Hebei Province(B2015205163,B2016205161)the 2015 Hebei Province Undergraduate Training Programs for Innovation and Entrepreneurship
文摘Pt-free counter electrode(CE) composed of La2 MoO(LaO-MoO) was successfully synthesized by simple pyrolysis of lanthanum acetate(CHOLa·xHO) and hexaammonium heptamolybdate tetrahydrate((NH4)6 MoO·4 HO). Furthermore,three proportions composites catalysts of La2 MoO@MWCNTs based on La2 MoOand multiwall carbon nanotubes(MWCNTs) were prepared and characterized as Ptfree catalyst for CE in dye-sensitized solar cells(DSSCs). The morphology and structure of La2 MoO@MWCNTs composites were determined by scanning electron microscopy, transmission electron microscope and X-ray diffraction. The electrochemical performance of La2 MoO@MWCNTs composite catalysts for CEs was determined by photocurrent-voltage measurements, cyclic voltammetry,electrochemical impedance spectroscopy, and Tafel polarization. The power conversion efficiencies of4.68%, 4.87% and 5.06% are obtained for La2 MoO:MWCNTs with the mass ratios of 5:1, 3:1 and 1:1 towards the reduction of I~-to I~-under the same conditions,respectively,which are superior to those of MWCNTs(3,94%) and La2 MoO(1.71%) electrodes. The experimental results reveal that the presence of MWCNTs results in an augmented active catalytic surface area and enhanced charge transfer from CE to the electrolyte.
文摘Al specimens were covered with TiO2 film by sol-gel dip-coating and then anodized in ammonium adipate solution.The structure,composition and capacitance properties of the anodic oxide film were investigated by transmission electron microscopy (TEM),Auger electron spectroscopy (AES),X-ray diffractometry (XRD) and electrochemical impedance spectroscopy (EIS).It was found that an anodic oxide film with a dual-layer structure formed between TiO2 coating and Al substrate.The film consisted of an inner Al2O3 layer and an outer Ti-Al composite oxide layer.The thickness of layers varied with the number of times of sol-gel dip-coating.The capacitance of anodic oxide films formed on coated specimens was at most 80% higher than that without TiO2.In film formation mechanism,it was claimed that the formation of composite oxide film was mainly affected by the structure of micro-pores network in TiO2 coating which had an influence on Al3+ and O2? ions transport during the anodizing.
基金supported by the National Natural Science Foundation of China(Grants No.21067004 and No.21263005)the Technological Foundation of Jiangxi Province Education Office(No.GJJ12344)+1 种基金the Young Science and Technolgy Project of Jiangxi Province(No.20133BAB21003)the Young Scientist Training Project of Jiangxi Province(No.20122BCB23015)
文摘A series of novel Ni/CeOe-Al2O3 composite catalysts were synthesized by one-step citric acid complex method, The as-synthesized catalysts were characterized by N2 physical adsorption/desorption, X-ray diffraction （XRD）, Fourier transform infrared （FT-IR） spectroscopy, hydrogen temperature-programmed reduction （Hz-TPR）, X-ray photoelectron spectroscopy （XPS） and thermogravimetry analysis （TGA）. The effects of nickel content, calcination and reaction temperatures, gas hourly space velocity （GHSV） and inert gas dilution of N2 on their performance of catalytic partial oxidation of methane （CPOM） were investigated. Catalytic activity test results show that the highest methane conversion （〉85%）, the best selectivities to carbon monoxide （〉87%） and to hydrogen （〉95%）, the excellent stability and perfect Hz/CO ratio （2.0） can be obtained over Ni/CeO2-Al2O3 with 8 wt% Ni content calcined at 700 ℃ under the reaction condition of 750 ℃, CH4/O2 ratio of 2 ： 1 and gas hourly space velocity of 12000 mL.h-1 .g-1. Characterization results show that the good catalytic performance of this composite catalyst can be contributed to its large specific surface area （~108 m2.g-1）, small crystallite size, easy reducibility and low coking rate.
基金supported by National Natural Science Foundation of China(51071030)
文摘The present paper discussed some fundamental aspects on composite oxide scales and coatings for protection of alloys from high temperature oxidation, the related thermodynamic conditions, special mechanical characteristics and a sealing mechanism. It was proposed that the oxide scales and coatings with a composite structure should possess superior mechanical properties than that with a single phase oxide. It also showed that the A1203 scales or coatings doped with 3（203 and ZrO2 （or YSZ）-A1203 composite coatings possessed superior properties at high temperatures. In such composite oxide scales and coatings, the fracture resistance of the scales was increased by the toughening effect, the thermal stress was decreased owing to the increase of thermal-expansion coefficients, and A1203 phase could seal the alloy substrate well In addition, the kinetic equation of thermal growth oxide on alloy covered with composite oxide coatings was derived.
基金financially supported by the Professorial and Doctoral Scientific Research Foundation of Huizhou University(Nos.2018JB036,2020JB046 and 2022JB009)the Major and Special Project in the Field of Intelligent Manufacturing of the Universities in Guangdong Province(No.2020ZDZX2067)+3 种基金the Natural Science Foundation of Huizhou University(No.HZU202004)Open Project Program of Guangdong Provincial Key Laboratory of Electronic Functional Materials and Devices,Huizhou University(Nos.EFMDN2021001Z and EFMDN2021004M)Youth Innovative Talents Project in Collegesand Universities in Guangdong Province(No.2019KQNCX151)Basic and Applied Basic Research Fund of Guangdong Province(No.2020A1515110038)。
文摘Ammonia borane(NH_(3)BH_(3),AB)has been regarded as a promising chemical hydrogen storage material owing to its high hydrogen density and superior stability.Thus,the development of low-cost and high-efficient heterogeneous catalysts for the dehydrogenation of AB has attracted considerable scholarly attention.In this study,heterostructured Co_(3)O_(4)-SnO_(2)catalysts containing oxygen vacancy(V_(o))with different Co/Sn atomic ratios(designated as V_(o)-Co-Sn_(5:x))were synthesized via a simple coprecipitation-calcination method under mild reaction conditions.The catalyst containing an optimized Co/Sn atomic ratio of 5:2(V_(o)-Co-Sn_(5:2))exhibited robust catalytic performance with a turnover frequency value of 17.6mol_(H2)·mol^(-1)_(metal)·min^(-1).Moreover,82.6%of the original activity of the catalyst was retained after 14 catalytic cycles,indicating the high stability of the catalyst.Diversified characterization combined with the density functional theory(DFT)calculation confirmed the transfer of electrons from Co_(3)O_(4)to Sn O_(2)and the distribution of the separated charges on SnO_(2)-Co_(3)O_(4)interface.The transfer of electrons and the distribution of charges facilitated the adsorption and activation of water on the catalyst,thus accelerating the dissociation of H_(2)O molecule(the ratedetermining step of AB hydrolysis).It was found that the V_(o)adjusted the electron structure of the catalysts rather than acted as active sites.These findings will provide researchers with useful information for designing cheap and highly efficient catalysts for catalytic AB hydrolysis.
文摘The lanthanum aluminum mesoporous materials were synthesized using sodium dodecyl sulfate as a template agent by ultrasonic hydrothermal method.The resulting samples were characterized by low angle X-ray diffraction（XRD）,N2 adsorption-desorption studies,transmission electron microscopy（TEM）and surface morphology analysis（SEM）,surface acid（NH3-TPD）,reducibility properties（TPR）,X-ray energy dispersive spectrometer（EDS）and thermogravimetric analysis（TG/DTG）.A l/La composite mesoporous material were synthesized with n（Al）︰n（La）=70︰1.0,80°C of reaction temperature,20 h of reaction time,12 h of crystallization time,650°C of calcination temperature.The specific surface area of the sample is 273.90 m 2 ·g ？1 ,with the average diameter 5.642 nm and pore volume 0.2354 cm 3 ·g ？1 .The samples have mesoporous structure and its particles are similar to a worm-shaped tubular structure.The influence of calcination temperature on the surface physical and chemical properties of Al/La composited mesoporous materials was examined,and the results showed that the acid strength was increased but the amount of acidic sites is decreased as the calcination temperature increased.It was found that the sample calcined at 650°C had appropriate acid content,acid strength and better reducibility.
