An efficient method for the synthesis of α-phenylcinnamates via silver catalyzed C—C bond activation reaction of cyclopropenone and alcohol was developed.This protocol features a simple reaction system,specific regi...An efficient method for the synthesis of α-phenylcinnamates via silver catalyzed C—C bond activation reaction of cyclopropenone and alcohol was developed.This protocol features a simple reaction system,specific regioselectivity,good functional group compatibility and good yields.It is of great significance for the later modification of natural products.展开更多
Due to their outstanding electrical contact properties,Cd-containing silver-matrix electrical contact materials can meet the requirements of high stability and long life for military defense and aerospace applications...Due to their outstanding electrical contact properties,Cd-containing silver-matrix electrical contact materials can meet the requirements of high stability and long life for military defense and aerospace applications.In order to further reduce the Cd content under the premise of meeting the high-performance requirements,in this study,high-purity intermediate Ti_(2)Cd powder of MAX phase(Ti_(2)CdC)was synthesized with a pressureless technique and then applied to reinforce the Ag matrix.The Cd content of the as-prepared Ag/Ti_(2)Cd composites was actually reduced by 38.31%compared with conventional Ag/CdO material.Based on the systematic study of the effect of heat treatment temperature on the physical phase,morphology,interface and comprehensive physical properties of Ag/Ti_(2)Cd composites,the preferred samples(heat treated at 400°C for 1 h)showed high density(97.77%),low resistivity(2.34μΩ·cm),moderate hardness(90.8HV),high tensile strength(189.9 MPa),and exhibited good electrical contact performance after 40000 cycles of arc discharging under severe conditions(DC 28 V/20 A).The results of microscopic morphological evolution,phase change and elemental distribution of the electrical contact surface show that the combination of high stability of Ti_(2)Cd reinforcing phase,good interfacial bonding with Ag matrix and improved melt pool viscosity in the primary stage of arc erosion,results in low and stable contact resistance(average value 13.20 mΩ)and welding force(average value 0.6 N),low fluctuation of static force(2.2-2.5 N).The decomposition and absorption energy of Ti_(2)Cd and the arc extinguishing effect of Cd vapor are the main reasons for the stable arcing energy and arcing time of electric contacts in the late stage of arc erosion.展开更多
Microcystin-RR(MC-RR),a form of microcystin with two arginine moieties,is a cyanobacterial toxin that has been detected across a wide geographic range.It is a great concern globally because of its potential liver to...Microcystin-RR(MC-RR),a form of microcystin with two arginine moieties,is a cyanobacterial toxin that has been detected across a wide geographic range.It is a great concern globally because of its potential liver toxicity.Herein,the abilities of BiVO4,Ag-BiVO4,Ag2O-BiVO4 and Ag/Ag2O-BiVO4 to photocatalytically degrade MC-RR under visible-light irradiation(λ≥420 nm) were investigated and compared.The possible degradation pathways were explored through analysis of the reaction intermediates by high-performance liquid chromatography-mass spectrometry.The results showed that the presence of Ag^0 enhanced the photocatalytic efficiency of Ag/Ag2O-BiVO4 via a synergetic effect between Ag2O and Ag^0 at the p-n heterojunction.Moreover,the presence of Ag^0 also greatly promoted the adsorption of MC-RR on the photocatalyst surface.Toxicological experiments on mice showed that the toxicity of MC-RR was significantly reduced after photocatalytic degradation.展开更多
Ternary Ag/AgC l/BiO IO3 composite photocatalysts are prepared by a facile method. Enhanced visible-light absorption and charge carrier separation are achieved after the introduction of Ag/AgC l particles into BiO IO3...Ternary Ag/AgC l/BiO IO3 composite photocatalysts are prepared by a facile method. Enhanced visible-light absorption and charge carrier separation are achieved after the introduction of Ag/AgC l particles into BiO IO3 systems,as revealed by ultraviolet-visible diffuse-reflectance spectrometry,photocurrent response and electrochemical impedance spectroscopy. The Ag/AgC l/BiO IO3 composites are applied to the visible-light photocatalytic oxidization of NO in air and exhibit an enhanced activity for NO removal in comparison with Ag/AgC l and pure BiO IO3. A possible photocatalytic mechanism for Ag/AgC l/BiO IO3 is proposed,which is related to the surface plasmon resonance effects of Ag metal and the effective carrier separation ability of BiO IO3. This work provides insight into the design and preparation of BiO IO3-based materials with enhanced visible-light photocatalysis ability.展开更多
Ag2O-TiO 2/sepiolite heterostructure composites were synthesized by a simple two-step method at low temperatures(100–450 °C). Acid red G aqueous solution and gaseous formaldehyde were chosen as model organic p...Ag2O-TiO 2/sepiolite heterostructure composites were synthesized by a simple two-step method at low temperatures(100–450 °C). Acid red G aqueous solution and gaseous formaldehyde were chosen as model organic pollutants to evaluate the photocatalytic performance of the as-prepared composites. The results showed that the Ag2O-TiO 2/sepiolite exhibited enhanced photocatalytic activity over pure Ag2O-TiO 2,TiO 2/sepiolite,and Ag2O/sepiolite under visible-light irradiation(λ 420 nm). The excellent photocatalytic efficiency of these composites can be ascribed to the synergistic effect between the heterojunction and the porous structure of the clay layers,which induced high adsorption and efficient charge separation. In addition,the active species involved in the degradation reaction have been investigated by photoluminescence spectroscopy and quenching experiments. A possible photocatalytic degradation mechanism of acid red G dye by the Ag2O-TiO 2/sepiolite composite is also discussed.展开更多
Ag2S/Ag2WO4 composite microrods,with lengths of 0.2-1μm and diameters of 20-30 nm,were fabricated by a facile sonochemical route.The as-synthesized products were intensively investigated by a series of physicochemica...Ag2S/Ag2WO4 composite microrods,with lengths of 0.2-1μm and diameters of 20-30 nm,were fabricated by a facile sonochemical route.The as-synthesized products were intensively investigated by a series of physicochemical characterizations,such as N2 physical adsorption,X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Fourier transform infrared spectroscopy,diffuser reflectance spectroscopy,X-ray photoelectron spectroscopy,photoluminescence spectroscopy and photocurrent response measurements.Ultrasonic irradiation yields an obvious improvement in the photocatalyst texture,for example,an increase in crystallinity and surface area.Moreover,sonochemically fabricated Ag2S/Ag2WO4 microrods display strong visible light absorption and a high transient photocurrent response.The produced intimate Ag2S/Ag2WO4interface between Ag2S and Ag2WO4 crystal phases largely promotes the separation of photogenerated holes and electrons.High photocatalytic activity and stability were obtained over Ag2S/Ag2WO4composite microrods.The dye degradation rate constant of Ag2S/Ag2WO4 was 4.7 times and 29.8times higher than that of bare Ag2WO4 and Ag2S,respectively.展开更多
Noble metal/titania hollow nanomaterials usually exhibit excellent photocatalytic activity because of their high specific surface area,low density,good surface permeability,strong light-harvesting capacity,and rapid i...Noble metal/titania hollow nanomaterials usually exhibit excellent photocatalytic activity because of their high specific surface area,low density,good surface permeability,strong light-harvesting capacity,and rapid interfacial charge transfer. However,the present preparation methods usually include complicated and multistep procedures,which can cause damage to the hollow nanostructures. In this paper,a facile template-induced synthesis,based on a template-directed deposition and in situ template-sacrificial dissolution,was employed to prepare Ag-modified TiO 2(Ag/TiO 2) hollow octahedra using Ag2 O octahedra as templates and TiF 4 as the precursor. In the synthetic strategy,the shells of TiO 2 hollow octahedra were formed by coating TiO 2 nanoparticles on the surface of Ag2 O templates based on the template-directed deposition. Simultaneously,the Ag2 O templates can be in situ removed by dissolving the Ag2 O octahedral template in HF solution produced via the hydrolysis reaction of TiF 4 in the reaction system. In addition,Ag nanoparticles were deposited on the inside and outside surfaces of TiO 2 shells by effectively using the photosensitive properties of Ag2 O and Ag+ ions under light irradiation,along with the formation of TiO 2 hollow octahedra. The Ag/TiO 2 hollow octahedra exhibited high photocatalytic activity because of their(1) short diffusion distances between photogenerated electrons and holes because of the thin shells of Ag/TiO 2 hollow octahedral,(2) deposition of Ag nanoparticles on the inside and outside surfaces of TiO 2 shells,and(3) rapid interfacial charge transfer between TiO 2 shells and Ag nanoparticles. This work may also provide new insights into preparing other Ag-modified and hollow nanostructured photocatalysts.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
The effect of preparation routes on the physical characteristics and activity of the Ag-MnOx/C composites toward the oxygen reduction reaction (ORR) in alkaline media were studied by X-ray diffraction (XRD), X-ray...The effect of preparation routes on the physical characteristics and activity of the Ag-MnOx/C composites toward the oxygen reduction reaction (ORR) in alkaline media were studied by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), energy-dispersion spectroscopy (EDS) as well as scanning electron microscopy (SEM) and electrochemical techniques. The results show that more Ag and Mn species present on the surface of the Ag-MnOx/C composite prepared by two-step route (Ag-MnOx/C-2) compared to the one prepared by one-step route (Ag-MnOx/C-1), which contributes to its superior activity toward the ORR. The higher electron transfer number involved in the ORR can be observed on the Ag-MnOx/C-2 composite and its specific mass kinetic current at -0.6 V (vs Hg/HgO) is 46 mA/μg, which is 23 times that on the Ag/C. The peak power density of zinc-air battery with the Ag-MnOx/C-2 air electrode reaches up to 117 mW/cm^2.展开更多
TiO2/γ-Al2O3 supported In/Ag catalysts were prepared by impregnation method,and investigated for NO reduction with CO as the reducing agent under lean burn conditions.The microscopic structure and surface properties ...TiO2/γ-Al2O3 supported In/Ag catalysts were prepared by impregnation method,and investigated for NO reduction with CO as the reducing agent under lean burn conditions.The microscopic structure and surface properties of the catalysts were studied by N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,X-ray photoelectron spectroscopy,ultraviolet-visible spectroscopy,H2 temperature-programmed reduction and Fourier transform infrared spectroscopy.TiO2/γ-Al2O3 supported In/Ag is a good catalyst for the reduction of NO to N2.It displayed high dispersion,large amounts of surface active components and high NO adsorption capacity,which gave good catalytic performance and stability for the reduction of NO with CO under lean burn conditions.The silver species stabilized and improved the dispersion of the indium species.The introduction of TiO2 into the γ-Al2O3 support promoted NO adsorption and improved the dispersion of the indium species and silver species.展开更多
基金Project supported by the National Natural Science Foundation of China(No.21702160)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(No.KF2311)。
文摘An efficient method for the synthesis of α-phenylcinnamates via silver catalyzed C—C bond activation reaction of cyclopropenone and alcohol was developed.This protocol features a simple reaction system,specific regioselectivity,good functional group compatibility and good yields.It is of great significance for the later modification of natural products.
基金This work was financially supported by the National Natural Science Foundation of China(52101064)Jiangsu Planned Projects for Postdoctoral Research Funds(2020Z158)Industry-University-Research Cooperation Projects(RH2000002728,RH2000002332,RH2100000263).
文摘Due to their outstanding electrical contact properties,Cd-containing silver-matrix electrical contact materials can meet the requirements of high stability and long life for military defense and aerospace applications.In order to further reduce the Cd content under the premise of meeting the high-performance requirements,in this study,high-purity intermediate Ti_(2)Cd powder of MAX phase(Ti_(2)CdC)was synthesized with a pressureless technique and then applied to reinforce the Ag matrix.The Cd content of the as-prepared Ag/Ti_(2)Cd composites was actually reduced by 38.31%compared with conventional Ag/CdO material.Based on the systematic study of the effect of heat treatment temperature on the physical phase,morphology,interface and comprehensive physical properties of Ag/Ti_(2)Cd composites,the preferred samples(heat treated at 400°C for 1 h)showed high density(97.77%),low resistivity(2.34μΩ·cm),moderate hardness(90.8HV),high tensile strength(189.9 MPa),and exhibited good electrical contact performance after 40000 cycles of arc discharging under severe conditions(DC 28 V/20 A).The results of microscopic morphological evolution,phase change and elemental distribution of the electrical contact surface show that the combination of high stability of Ti_(2)Cd reinforcing phase,good interfacial bonding with Ag matrix and improved melt pool viscosity in the primary stage of arc erosion,results in low and stable contact resistance(average value 13.20 mΩ)and welding force(average value 0.6 N),low fluctuation of static force(2.2-2.5 N).The decomposition and absorption energy of Ti_(2)Cd and the arc extinguishing effect of Cd vapor are the main reasons for the stable arcing energy and arcing time of electric contacts in the late stage of arc erosion.
基金supported by the National Natural Science Foundation of China (21677086, 21407092, 21377067, 21577078)the Natural Science Foundation for Innovation Group of Hubei Province, China (2015CFA021)~~
文摘Microcystin-RR(MC-RR),a form of microcystin with two arginine moieties,is a cyanobacterial toxin that has been detected across a wide geographic range.It is a great concern globally because of its potential liver toxicity.Herein,the abilities of BiVO4,Ag-BiVO4,Ag2O-BiVO4 and Ag/Ag2O-BiVO4 to photocatalytically degrade MC-RR under visible-light irradiation(λ≥420 nm) were investigated and compared.The possible degradation pathways were explored through analysis of the reaction intermediates by high-performance liquid chromatography-mass spectrometry.The results showed that the presence of Ag^0 enhanced the photocatalytic efficiency of Ag/Ag2O-BiVO4 via a synergetic effect between Ag2O and Ag^0 at the p-n heterojunction.Moreover,the presence of Ag^0 also greatly promoted the adsorption of MC-RR on the photocatalyst surface.Toxicological experiments on mice showed that the toxicity of MC-RR was significantly reduced after photocatalytic degradation.
基金supported by the National Natural Science Foundation of China(5147807051108487)the Science and Technology Project from Chongqing Education Commission(KJ1400617)~~
文摘Ternary Ag/AgC l/BiO IO3 composite photocatalysts are prepared by a facile method. Enhanced visible-light absorption and charge carrier separation are achieved after the introduction of Ag/AgC l particles into BiO IO3 systems,as revealed by ultraviolet-visible diffuse-reflectance spectrometry,photocurrent response and electrochemical impedance spectroscopy. The Ag/AgC l/BiO IO3 composites are applied to the visible-light photocatalytic oxidization of NO in air and exhibit an enhanced activity for NO removal in comparison with Ag/AgC l and pure BiO IO3. A possible photocatalytic mechanism for Ag/AgC l/BiO IO3 is proposed,which is related to the surface plasmon resonance effects of Ag metal and the effective carrier separation ability of BiO IO3. This work provides insight into the design and preparation of BiO IO3-based materials with enhanced visible-light photocatalysis ability.
基金supported by the National Key Technology R&D Program of China(2012BAJ25B02-03)~~
文摘Ag2O-TiO 2/sepiolite heterostructure composites were synthesized by a simple two-step method at low temperatures(100–450 °C). Acid red G aqueous solution and gaseous formaldehyde were chosen as model organic pollutants to evaluate the photocatalytic performance of the as-prepared composites. The results showed that the Ag2O-TiO 2/sepiolite exhibited enhanced photocatalytic activity over pure Ag2O-TiO 2,TiO 2/sepiolite,and Ag2O/sepiolite under visible-light irradiation(λ 420 nm). The excellent photocatalytic efficiency of these composites can be ascribed to the synergistic effect between the heterojunction and the porous structure of the clay layers,which induced high adsorption and efficient charge separation. In addition,the active species involved in the degradation reaction have been investigated by photoluminescence spectroscopy and quenching experiments. A possible photocatalytic degradation mechanism of acid red G dye by the Ag2O-TiO 2/sepiolite composite is also discussed.
基金supported by the National Natural Science Foundation of China(21567008,21263005)the Yangfan Project of Guangdong Province+2 种基金the Natural Science Foundation of Jiangxi Province(20133BAB21003,20161BAB203090)the Landing Project of Science and Technology of Colleges and Universities in Jiangxi Province(KJLD14046)the Graduate Innovation Project of Jiangxi Province(YC2015-S293)~~
文摘Ag2S/Ag2WO4 composite microrods,with lengths of 0.2-1μm and diameters of 20-30 nm,were fabricated by a facile sonochemical route.The as-synthesized products were intensively investigated by a series of physicochemical characterizations,such as N2 physical adsorption,X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Fourier transform infrared spectroscopy,diffuser reflectance spectroscopy,X-ray photoelectron spectroscopy,photoluminescence spectroscopy and photocurrent response measurements.Ultrasonic irradiation yields an obvious improvement in the photocatalyst texture,for example,an increase in crystallinity and surface area.Moreover,sonochemically fabricated Ag2S/Ag2WO4 microrods display strong visible light absorption and a high transient photocurrent response.The produced intimate Ag2S/Ag2WO4interface between Ag2S and Ag2WO4 crystal phases largely promotes the separation of photogenerated holes and electrons.High photocatalytic activity and stability were obtained over Ag2S/Ag2WO4composite microrods.The dye degradation rate constant of Ag2S/Ag2WO4 was 4.7 times and 29.8times higher than that of bare Ag2WO4 and Ag2S,respectively.
基金supported by the National Natural Science Foundation of China(5120839621277107+5 种基金21477094and 51472192)the Program for New Century Excellent Talents in University(NCET-13-0944)the Fundamental Research Funds for the Central Universities(WUT 2014-1a-0032014-VII-037and 2015IB002)~~
文摘Noble metal/titania hollow nanomaterials usually exhibit excellent photocatalytic activity because of their high specific surface area,low density,good surface permeability,strong light-harvesting capacity,and rapid interfacial charge transfer. However,the present preparation methods usually include complicated and multistep procedures,which can cause damage to the hollow nanostructures. In this paper,a facile template-induced synthesis,based on a template-directed deposition and in situ template-sacrificial dissolution,was employed to prepare Ag-modified TiO 2(Ag/TiO 2) hollow octahedra using Ag2 O octahedra as templates and TiF 4 as the precursor. In the synthetic strategy,the shells of TiO 2 hollow octahedra were formed by coating TiO 2 nanoparticles on the surface of Ag2 O templates based on the template-directed deposition. Simultaneously,the Ag2 O templates can be in situ removed by dissolving the Ag2 O octahedral template in HF solution produced via the hydrolysis reaction of TiF 4 in the reaction system. In addition,Ag nanoparticles were deposited on the inside and outside surfaces of TiO 2 shells by effectively using the photosensitive properties of Ag2 O and Ag+ ions under light irradiation,along with the formation of TiO 2 hollow octahedra. The Ag/TiO 2 hollow octahedra exhibited high photocatalytic activity because of their(1) short diffusion distances between photogenerated electrons and holes because of the thin shells of Ag/TiO 2 hollow octahedral,(2) deposition of Ag nanoparticles on the inside and outside surfaces of TiO 2 shells,and(3) rapid interfacial charge transfer between TiO 2 shells and Ag nanoparticles. This work may also provide new insights into preparing other Ag-modified and hollow nanostructured photocatalysts.
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Project(21406273)supported by the National Natural Science Foundation of China
文摘The effect of preparation routes on the physical characteristics and activity of the Ag-MnOx/C composites toward the oxygen reduction reaction (ORR) in alkaline media were studied by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), energy-dispersion spectroscopy (EDS) as well as scanning electron microscopy (SEM) and electrochemical techniques. The results show that more Ag and Mn species present on the surface of the Ag-MnOx/C composite prepared by two-step route (Ag-MnOx/C-2) compared to the one prepared by one-step route (Ag-MnOx/C-1), which contributes to its superior activity toward the ORR. The higher electron transfer number involved in the ORR can be observed on the Ag-MnOx/C-2 composite and its specific mass kinetic current at -0.6 V (vs Hg/HgO) is 46 mA/μg, which is 23 times that on the Ag/C. The peak power density of zinc-air battery with the Ag-MnOx/C-2 air electrode reaches up to 117 mW/cm^2.
基金supported by the National Science & Technology Pillar Program(2012BAF03B02)National Natural Science Foundation of China(21101085,U1162203)+3 种基金Natural Science Foundation of Liaoning Province(2015020196)Doctoral Fund of Shandong Province(BS2015HZ003)Fushun Science & Technology Program(FSKJHT 201423)Liaoning Excellent Talents Program in University(LJQ2012031)~~
文摘TiO2/γ-Al2O3 supported In/Ag catalysts were prepared by impregnation method,and investigated for NO reduction with CO as the reducing agent under lean burn conditions.The microscopic structure and surface properties of the catalysts were studied by N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,X-ray photoelectron spectroscopy,ultraviolet-visible spectroscopy,H2 temperature-programmed reduction and Fourier transform infrared spectroscopy.TiO2/γ-Al2O3 supported In/Ag is a good catalyst for the reduction of NO to N2.It displayed high dispersion,large amounts of surface active components and high NO adsorption capacity,which gave good catalytic performance and stability for the reduction of NO with CO under lean burn conditions.The silver species stabilized and improved the dispersion of the indium species.The introduction of TiO2 into the γ-Al2O3 support promoted NO adsorption and improved the dispersion of the indium species and silver species.