In order to investigate the effect of solid particles dopants on physicochemical properties of α-PbO2 electrodes, a-PbO2 composite electrodes doped with nano-TiO2 and nano-CeO2 particles were respectively prepared on...In order to investigate the effect of solid particles dopants on physicochemical properties of α-PbO2 electrodes, a-PbO2 composite electrodes doped with nano-TiO2 and nano-CeO2 particles were respectively prepared on A1/conductive coating electrodes in 4 mol/L NaOH solution with addition of PbO until saturation by anodic codeposition. The electrodeposition mechanism, morphology, composition and structure of the composite electrodes were characterized by cyclic voltarnmogram (CV), SEM, EDAX and XRD. Results show that the doping solid particles can not change reaction mechanism of α-PbO2 electrode in alkaline or acid plating bath, but can improve deposition rate and reduce oxygen evolution potential. The doping solid particles can inhibit the growth of a-PbO2 unit cell and improve specific surface area. The diffraction peak intensity of a-PbO2-CeO2-TiO2 composite electrode is lower than that of pure a-PbO2 electrode. The electrocatalytic activity of a-PbO2-2.12%CEO2-3.71%TIO2 composite electrode is the best. The Guglielmi model for CeO2 and TiO2 codeposition with a-PbO2 is also pronosed.展开更多
A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides ...A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides are modulated by changing the Mg/Al ratios,calcination temperature and treatment with probe molecules.Detailed characterization,including X‐ray diffraction,27Al magic angle spinning nuclear magnetic resonance spectroscopy,N2‐adsorption,NH3‐temperature‐programmed desorption,CO2‐temperature‐programmed desorption and X‐ray photoelectron spectroscopy are carried out to determine the physicochemical properties of these catalysts.The Mg‐Al oxides with Mg/Al=3exhibit the highest activity in the reaction,which possess a large number of surface weak basic sites and a relatively small number of weak acidic sites.The role of the acidic and basic sites in the reaction process is systematically investigated,and are shown to serve as adsorption and activation sites for amines and alcohols,respectively.Under the synergistic effect of these acid‐base centers,the oxidative coupling process successfully occurs on the surface of Mg‐Al mixed oxides.Compared with the acidic sites,the weak basic sites play a more important role in the catalytic process.The acidic sites are the catalytic centers for the benzyl alcohol activation,which control the reaction rate of the oxidative coupling reaction.展开更多
Zr‐Al mixed oxide supported Pt catalysts with different Zr/Al mole ratios(2.5%Pt/ZrxAl(1–x)Oy) were synthesized by an impregnation method and used for the selective hydrogenolysis of glycerol to n‐propanol in a...Zr‐Al mixed oxide supported Pt catalysts with different Zr/Al mole ratios(2.5%Pt/ZrxAl(1–x)Oy) were synthesized by an impregnation method and used for the selective hydrogenolysis of glycerol to n‐propanol in an autoclave reactor. The catalysts were fully characterized by X‐ray powder diffrac‐tion, Brunauer‐Emmett‐Teller surface area analysis, CO chemisorption, H2 temperature‐ pro‐grammed reduction, pyridine‐infrared spectroscopy, and NH3‐temperature‐programmed desorp‐tion. The results revealed that the Zr/Al ratio on the support significantly affected the size of the platinum particles and the properties of the acid sites on the catalysts. The catalytic performance was well correlated with the acidic properties of the catalyst; specifically, more acid sites contrib‐uted to the conversion and strong acid sites with a specific intensity contributed to the deep dehy‐dration of glycerol to form n‐propanol. Among the tested catalysts, 2.5 wt% Pt/Zr(0.7)Al(0.3)Oy exhibited excellent selectivity for n‐propanol with 81.2% glycerol conversion at 240 °C and 6.0 MPa H2 pres‐sure when 10% aqueous glycerol solution was used as the substrate. In addition, the effect of vari‐ous reaction parameters, such as H2 content, reaction temperature, reaction time, and number of experimental cycles were studied to determine the optimized reaction conditions and to evaluate the stability of the catalyst.展开更多
As an important anthropogenic volatile organic compound(VOC), m-xylene has attracted numerous attentions due to its potential in secondary organic aerosol(SOA) formation. In this study, effects of aluminium dust seeds...As an important anthropogenic volatile organic compound(VOC), m-xylene has attracted numerous attentions due to its potential in secondary organic aerosol(SOA) formation. In this study, effects of aluminium dust seeds(boehmite and alumina) on SOA yield and aerosol size in m-xylene/NOx photo-oxidation were investigated in a 2 m3 smog chamber at 30°C and 50% relative humidity. Compared to the seed-free system, the presence of aluminium seeds resulted in an increase in the SOA yield, and also enhanced the O3 concentration in the chamber. The photolysis of O3 is a major source of OH radical, which is the most important oxidant of m-xylene. The increase in O3 concentration could result in the generation of more OH radicals, and finally contribute to the SOA formation. Seed particles influence the SOA size mainly by acting as condensation nuclei. Semi-volatile organic compounds(SVOCs) were condensed onto these nuclei, resulting in the increase in SOA size. However, when aluminium seeds with high concentrations were introduced into the system, SVOCs that had been condensed onto each particle were dispersed by these seeds, leading to the reduction in aerosol size.展开更多
There has been increasing interest in devel- oping micro/nanostructured aluminum-based materials for sustainable, dependable and high-efficiency electro- chemical energy storage. This review chiefly discusses the alum...There has been increasing interest in devel- oping micro/nanostructured aluminum-based materials for sustainable, dependable and high-efficiency electro- chemical energy storage. This review chiefly discusses the aluminum-based electrode materials mainly including A1203, AIF3, AIPO4, AI(OH)3, as well as the composites (carbons, silicons, metals and transition metal oxides) for lithium-ion batteries, the development of aluminum-ion batteries, and nickel-metal hydride alkaline secondary batteries, which summarizes the methodologies, related charge-storage mechanisms, the relationship between nanos- tructures and electrochemical properties found in recent years, latest research achievements and their potential ap- plications. In addition, we raise the relevant challenges in recently developed electrode materials and put forward new ideas for further development of micro/nanostructured aluminum-based materials in advanced battery systems.展开更多
基金Project(51004056) supported by the National Natural Science Foundation of ChinaProject(KKZ6201152009) supported by the Opening Foundation of Key Laboratory of Inorganic Coating Materials,Chinese Academy of Sciences+2 种基金Project(2010ZC052) supported by the Applied Basic Research Foundation of Yunnan Province,ChinaProject(20125314110011) supported by the Specialized Research Fund for the Doctoral Program of Higher EducationProject(2010247) supported by Analysis & Testing Foundation of Kunming University of Science and Technology,China
文摘In order to investigate the effect of solid particles dopants on physicochemical properties of α-PbO2 electrodes, a-PbO2 composite electrodes doped with nano-TiO2 and nano-CeO2 particles were respectively prepared on A1/conductive coating electrodes in 4 mol/L NaOH solution with addition of PbO until saturation by anodic codeposition. The electrodeposition mechanism, morphology, composition and structure of the composite electrodes were characterized by cyclic voltarnmogram (CV), SEM, EDAX and XRD. Results show that the doping solid particles can not change reaction mechanism of α-PbO2 electrode in alkaline or acid plating bath, but can improve deposition rate and reduce oxygen evolution potential. The doping solid particles can inhibit the growth of a-PbO2 unit cell and improve specific surface area. The diffraction peak intensity of a-PbO2-CeO2-TiO2 composite electrode is lower than that of pure a-PbO2 electrode. The electrocatalytic activity of a-PbO2-2.12%CEO2-3.71%TIO2 composite electrode is the best. The Guglielmi model for CeO2 and TiO2 codeposition with a-PbO2 is also pronosed.
文摘A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides are modulated by changing the Mg/Al ratios,calcination temperature and treatment with probe molecules.Detailed characterization,including X‐ray diffraction,27Al magic angle spinning nuclear magnetic resonance spectroscopy,N2‐adsorption,NH3‐temperature‐programmed desorption,CO2‐temperature‐programmed desorption and X‐ray photoelectron spectroscopy are carried out to determine the physicochemical properties of these catalysts.The Mg‐Al oxides with Mg/Al=3exhibit the highest activity in the reaction,which possess a large number of surface weak basic sites and a relatively small number of weak acidic sites.The role of the acidic and basic sites in the reaction process is systematically investigated,and are shown to serve as adsorption and activation sites for amines and alcohols,respectively.Under the synergistic effect of these acid‐base centers,the oxidative coupling process successfully occurs on the surface of Mg‐Al mixed oxides.Compared with the acidic sites,the weak basic sites play a more important role in the catalytic process.The acidic sites are the catalytic centers for the benzyl alcohol activation,which control the reaction rate of the oxidative coupling reaction.
基金supported by the National Natural Science Foundation of China (21573031, 21373038)the Program for Excellent Talents in Dalian City (2016RD09)the Doctoral Scientific Research Foundation of Liao Ning Province (20170520395)~~
文摘Zr‐Al mixed oxide supported Pt catalysts with different Zr/Al mole ratios(2.5%Pt/ZrxAl(1–x)Oy) were synthesized by an impregnation method and used for the selective hydrogenolysis of glycerol to n‐propanol in an autoclave reactor. The catalysts were fully characterized by X‐ray powder diffrac‐tion, Brunauer‐Emmett‐Teller surface area analysis, CO chemisorption, H2 temperature‐ pro‐grammed reduction, pyridine‐infrared spectroscopy, and NH3‐temperature‐programmed desorp‐tion. The results revealed that the Zr/Al ratio on the support significantly affected the size of the platinum particles and the properties of the acid sites on the catalysts. The catalytic performance was well correlated with the acidic properties of the catalyst; specifically, more acid sites contrib‐uted to the conversion and strong acid sites with a specific intensity contributed to the deep dehy‐dration of glycerol to form n‐propanol. Among the tested catalysts, 2.5 wt% Pt/Zr(0.7)Al(0.3)Oy exhibited excellent selectivity for n‐propanol with 81.2% glycerol conversion at 240 °C and 6.0 MPa H2 pres‐sure when 10% aqueous glycerol solution was used as the substrate. In addition, the effect of vari‐ous reaction parameters, such as H2 content, reaction temperature, reaction time, and number of experimental cycles were studied to determine the optimized reaction conditions and to evaluate the stability of the catalyst.
基金supported by the National Natural Science Foundation of China(Grant No.41305116)the National Basic Research Program of China(Grant No.2011CB403401)the Specific Team Fund of Chinese Academy of Meteorological Sciences(Grant No.2010Z002)
文摘As an important anthropogenic volatile organic compound(VOC), m-xylene has attracted numerous attentions due to its potential in secondary organic aerosol(SOA) formation. In this study, effects of aluminium dust seeds(boehmite and alumina) on SOA yield and aerosol size in m-xylene/NOx photo-oxidation were investigated in a 2 m3 smog chamber at 30°C and 50% relative humidity. Compared to the seed-free system, the presence of aluminium seeds resulted in an increase in the SOA yield, and also enhanced the O3 concentration in the chamber. The photolysis of O3 is a major source of OH radical, which is the most important oxidant of m-xylene. The increase in O3 concentration could result in the generation of more OH radicals, and finally contribute to the SOA formation. Seed particles influence the SOA size mainly by acting as condensation nuclei. Semi-volatile organic compounds(SVOCs) were condensed onto these nuclei, resulting in the increase in SOA size. However, when aluminium seeds with high concentrations were introduced into the system, SVOCs that had been condensed onto each particle were dispersed by these seeds, leading to the reduction in aerosol size.
基金supported by the Program for New Century Excellent Talents of the University in China (NCET-13-0645)the National Natural Science Foundation of China (21201010, 21671170 and 21673203)+5 种基金the Innovation Scientists and Technicians Troop Construction Projects of Henan Province (164200510018)the Program for Innovative Research Team (in Science and Technology) in the University of Henan Province (14IRTSTHN004)the Six Talent Plan (2015-XCL030)Qinglan Projectthe Priority Academic Program Development of Jiangsu Higher Education Institutionsthe Undergraduate Scientific Research Innovation Projects in Jiangsu province (201611117047Y)
文摘There has been increasing interest in devel- oping micro/nanostructured aluminum-based materials for sustainable, dependable and high-efficiency electro- chemical energy storage. This review chiefly discusses the aluminum-based electrode materials mainly including A1203, AIF3, AIPO4, AI(OH)3, as well as the composites (carbons, silicons, metals and transition metal oxides) for lithium-ion batteries, the development of aluminum-ion batteries, and nickel-metal hydride alkaline secondary batteries, which summarizes the methodologies, related charge-storage mechanisms, the relationship between nanos- tructures and electrochemical properties found in recent years, latest research achievements and their potential ap- plications. In addition, we raise the relevant challenges in recently developed electrode materials and put forward new ideas for further development of micro/nanostructured aluminum-based materials in advanced battery systems.