Zeolite-13X-supported Fe（Fe/zeolite-13X） catalysts with various Fe contents were prepared by the wet impregnation method.The catalysts were characterized by N2 adsorption-desorption isotherms to estimate the Brunaue...Zeolite-13X-supported Fe（Fe/zeolite-13X） catalysts with various Fe contents were prepared by the wet impregnation method.The catalysts were characterized by N2 adsorption-desorption isotherms to estimate the Brunauer-Emmett-Teller surface areas and Barrett-Joyner-Hanlenda pore size distributions.X-ray diffraction,scanning electron microscopy,temperature-programmed reduction,and temperature-programmed desorption of NH3 were used to investigate the textural properties of the Fe/zeolite-13 X catalysts.Their catalytic activities were determined for the complete oxidation of1,4-dioxane using air as the oxidant in a fixed-bed flow reactor in the temperature range 100-400℃.The influences of various process parameters,such as reaction temperature,metal loading,and gas hourly space velocity（GHSV）,on the dioxane removal efficiency by catalytic oxidation were investigated.The stability of the catalyst was tested at 400℃ by performing time-on-stream analysis for 50 h.The Fe/zeolite-13 X catalyst with 6 wt%Fe exhibited the best catalytic activity among the Fe/zeolite-13 X catalysts at 400℃ and a GHSV of 24000 h^（-1）,with 97%dioxane conversion and95%selectivity for the formation of carbon oxides（CO and CO2）.Trace amounts（ 3%） of acetaldehyde,ethylene glycol monoformate,ethylene glycol diformate,1,4-dioxane-2-ol,1,4-dioxane-2-one,and 2-methoxy-1,3-dioxalane were also formed as degradation products.A plausible degradation mechanism is proposed based on the products identified by GC-MS analysis.展开更多
1,4-dioxane pollution is characterized by its early identification, widespread sources and extensive distribution. The pollutant is highly mobile and persistent in the water environment and is classified as a B2(proba...1,4-dioxane pollution is characterized by its early identification, widespread sources and extensive distribution. The pollutant is highly mobile and persistent in the water environment and is classified as a B2(probable) human carcinogen. After reviewing recent researches on the pollution status,transport and transformation characteristics of 1,4-dioxane in the water environment, as well as the environmental pollution remediation and treatment technologies, and the status of environmental regulation,this paper addresses that the distribution of 1,4-dioxane in water bodies is significantly correlated with chlorinated hydrocarbon pollutants such as 1,1,1-trichloroethane(1,1,1-TCA) and trichloroethylene(TCE).It is noteworthy that 1,4-dioxane often occurs in symbiosis with 1,1,1-TCA and has a similarity contamination plume distribution to 1,1,1-TCA. The natural attenuation of 1,4-dioxane in groundwater environment is weak, but there is a certain degree of biological oxidation attenuation. Current methods for treating 1,4-dioxane pollution mainly include extraction-treatment technology, advanced oxidation treatment technology, modified biological treatment technology and phytoremediation technology, all of which have their limitations in practical application. Currently, there is no environmental regulation available for the 1,4-dioxane pollution worldwide, and no enforceable standard established for defining the health trigger levels of 1,4-dioxane in drinking water. Research on this contaminant in China is generally limited to the site or laboratory scale, and there are no studies on the environmental risk and quality standards for 1,4-dioxane in the water environment.展开更多
1,4-dioxane （DOA） was originally used to pretreat the lithium metal electrode in order to improve its interface stability. Electrochemical impedance spectra （EIS） measurements reveal that with DOA pretreatment, li...1,4-dioxane （DOA） was originally used to pretreat the lithium metal electrode in order to improve its interface stability. Electrochemical impedance spectra （EIS） measurements reveal that with DOA pretreatment, lithium electrode has a low and stable interfacial resistance during the storage in electrolyte for a long time. And it is also found that the pretreated lithium electrode has an improved interfacial performance in repeated charge/discharge cycles. Furthermore, it is proved by SEM that the pretreated one has smooth morphology after long-time storage or repeated charge/discharge cycles. Consequentially, because of more stable interface characteristics of lithium electrode, the rechargeable lithium cell with DOA pretreated lithium anode has an obviously enhanced discharging performance and a better cycleability, compared with that of the cell using the untreated lithium anode.展开更多
A method for oxidative degradation of 1,4-dioxane （1,4-D） in waste water using a combination of ozone oxidation with UV irradiation （ozone/UV） treatment was investigated. The results showed that 1,4-D was degraded...A method for oxidative degradation of 1,4-dioxane （1,4-D） in waste water using a combination of ozone oxidation with UV irradiation （ozone/UV） treatment was investigated. The results showed that 1,4-D was degraded by ozone/UV treatment up to 90 min. The optimum concentration for the injected ozone gas was about 40 g·m^3 under a constant level of UV irradiation. Furthermore, solid phase extraction and GC-MS analysis showed no specific or reproducible peaks due to by-products of 1,4-D. It was therefore concluded that 1,4-D was completely degraded by ozone/UV treatment. In contrast, the amount of 1,4-D remaining decreased slowly in the presence of HCOf or CI. It was suggested that the degradation of 1,4-D, which results from .OH oxidation, was retarded by the presence of HCO3 or CI, which act as radical scavengers.展开更多
The copolymerization of DL-LA and 3-BMG was carried out in bulk with stannous 2-ethythexanoate as the catalyst. A series of copolymers with pendant protected groups were obtained and characterized by H-1-NMR and GPC a...The copolymerization of DL-LA and 3-BMG was carried out in bulk with stannous 2-ethythexanoate as the catalyst. A series of copolymers with pendant protected groups were obtained and characterized by H-1-NMR and GPC analysis. The monomer reactivity ratios were evaluated by the Fineman-Ross method and the Kelen-Tudos method and found to be r(BMG)=1.96 and r(LA)=0.37, respectively.展开更多
Density,viscosity and ultrasonic v elocity of solutions of four Schiff bases in 1,4-dioxane and dimethylfor -mamide(DMF )were measured at 308.15K.Various acoustical properties such as specific impedance(Z),adiabatic c...Density,viscosity and ultrasonic v elocity of solutions of four Schiff bases in 1,4-dioxane and dimethylfor -mamide(DMF )were measured at 308.15K.Various acoustical properties such as specific impedance(Z),adiabatic compressibility(κ s ),Rao’s molar sound function(R m ),the van der Waals constant (b),molar compressibility(W),intermolecular free length(L f ),relaxation strength(r),solvation number(S n ),were calculated.The results are in terpret-ed in terms of molecular interactions occurring in the solutions.展开更多
The Ni/SBA-15 catalysts were synthesized using the in situ method and the influence of crystallization temperature on nickel utilization efficiency-a critical factor in mesoporous material design-was systematically in...The Ni/SBA-15 catalysts were synthesized using the in situ method and the influence of crystallization temperature on nickel utilization efficiency-a critical factor in mesoporous material design-was systematically investigated.The structural characteristics and nickel anchoring capacity were analyzed using XRD,BET,FT-IR,H2-TPR,and ICP-OES.The results demonstrated that the crystallization temperature significantly affected the framework order of SBA-15 and the surface anchoring efficiency of Ni ions.The nickel utilization efficiency increased from 8.4%at 80℃to 60.49%at 140℃,but then decreased to 47.25%at 160℃,indicating an optimal crystallization temperature window.This provides crucial guidance for tailoring high-performance metal-doped molecular sieves.The optimal catalyst exhibited excellent performance in the hydrogenation of 1,4-butynediol(BYD):the BYD conversion reached 97.25%with 88.99%selectivity of 1,4-butenediol(BED)within 5 h,and reached 99.73%with 87.34%selectivity of 1,4-butanediol(BDO)after 20 h reaction.These results revealed the critical role of crystallization temperature in metal utilization and provided theoretical support for designing highly active molecular sieve catalysts.展开更多
基金supported by the Director,DRDE(DRDO),Ministry of Defence,India~~
文摘Zeolite-13X-supported Fe（Fe/zeolite-13X） catalysts with various Fe contents were prepared by the wet impregnation method.The catalysts were characterized by N2 adsorption-desorption isotherms to estimate the Brunauer-Emmett-Teller surface areas and Barrett-Joyner-Hanlenda pore size distributions.X-ray diffraction,scanning electron microscopy,temperature-programmed reduction,and temperature-programmed desorption of NH3 were used to investigate the textural properties of the Fe/zeolite-13 X catalysts.Their catalytic activities were determined for the complete oxidation of1,4-dioxane using air as the oxidant in a fixed-bed flow reactor in the temperature range 100-400℃.The influences of various process parameters,such as reaction temperature,metal loading,and gas hourly space velocity（GHSV）,on the dioxane removal efficiency by catalytic oxidation were investigated.The stability of the catalyst was tested at 400℃ by performing time-on-stream analysis for 50 h.The Fe/zeolite-13 X catalyst with 6 wt%Fe exhibited the best catalytic activity among the Fe/zeolite-13 X catalysts at 400℃ and a GHSV of 24000 h^（-1）,with 97%dioxane conversion and95%selectivity for the formation of carbon oxides（CO and CO2）.Trace amounts（ 3%） of acetaldehyde,ethylene glycol monoformate,ethylene glycol diformate,1,4-dioxane-2-ol,1,4-dioxane-2-one,and 2-methoxy-1,3-dioxalane were also formed as degradation products.A plausible degradation mechanism is proposed based on the products identified by GC-MS analysis.
文摘1,4-dioxane pollution is characterized by its early identification, widespread sources and extensive distribution. The pollutant is highly mobile and persistent in the water environment and is classified as a B2(probable) human carcinogen. After reviewing recent researches on the pollution status,transport and transformation characteristics of 1,4-dioxane in the water environment, as well as the environmental pollution remediation and treatment technologies, and the status of environmental regulation,this paper addresses that the distribution of 1,4-dioxane in water bodies is significantly correlated with chlorinated hydrocarbon pollutants such as 1,1,1-trichloroethane(1,1,1-TCA) and trichloroethylene(TCE).It is noteworthy that 1,4-dioxane often occurs in symbiosis with 1,1,1-TCA and has a similarity contamination plume distribution to 1,1,1-TCA. The natural attenuation of 1,4-dioxane in groundwater environment is weak, but there is a certain degree of biological oxidation attenuation. Current methods for treating 1,4-dioxane pollution mainly include extraction-treatment technology, advanced oxidation treatment technology, modified biological treatment technology and phytoremediation technology, all of which have their limitations in practical application. Currently, there is no environmental regulation available for the 1,4-dioxane pollution worldwide, and no enforceable standard established for defining the health trigger levels of 1,4-dioxane in drinking water. Research on this contaminant in China is generally limited to the site or laboratory scale, and there are no studies on the environmental risk and quality standards for 1,4-dioxane in the water environment.
基金the Foundation of Science-Technology Research Program of Guangdong Province (No.2003C105006) the Foundation of Key Science-Technology Program of Guangdong Province (No.2003A1100101)
文摘1,4-dioxane （DOA） was originally used to pretreat the lithium metal electrode in order to improve its interface stability. Electrochemical impedance spectra （EIS） measurements reveal that with DOA pretreatment, lithium electrode has a low and stable interfacial resistance during the storage in electrolyte for a long time. And it is also found that the pretreated lithium electrode has an improved interfacial performance in repeated charge/discharge cycles. Furthermore, it is proved by SEM that the pretreated one has smooth morphology after long-time storage or repeated charge/discharge cycles. Consequentially, because of more stable interface characteristics of lithium electrode, the rechargeable lithium cell with DOA pretreated lithium anode has an obviously enhanced discharging performance and a better cycleability, compared with that of the cell using the untreated lithium anode.
文摘A method for oxidative degradation of 1,4-dioxane （1,4-D） in waste water using a combination of ozone oxidation with UV irradiation （ozone/UV） treatment was investigated. The results showed that 1,4-D was degraded by ozone/UV treatment up to 90 min. The optimum concentration for the injected ozone gas was about 40 g·m^3 under a constant level of UV irradiation. Furthermore, solid phase extraction and GC-MS analysis showed no specific or reproducible peaks due to by-products of 1,4-D. It was therefore concluded that 1,4-D was completely degraded by ozone/UV treatment. In contrast, the amount of 1,4-D remaining decreased slowly in the presence of HCOf or CI. It was suggested that the degradation of 1,4-D, which results from .OH oxidation, was retarded by the presence of HCO3 or CI, which act as radical scavengers.
基金This work was supported by the Major State Basic Research Program of China (Grant No. G1999064704).
文摘The copolymerization of DL-LA and 3-BMG was carried out in bulk with stannous 2-ethythexanoate as the catalyst. A series of copolymers with pendant protected groups were obtained and characterized by H-1-NMR and GPC analysis. The monomer reactivity ratios were evaluated by the Fineman-Ross method and the Kelen-Tudos method and found to be r(BMG)=1.96 and r(LA)=0.37, respectively.
文摘Density,viscosity and ultrasonic v elocity of solutions of four Schiff bases in 1,4-dioxane and dimethylfor -mamide(DMF )were measured at 308.15K.Various acoustical properties such as specific impedance(Z),adiabatic compressibility(κ s ),Rao’s molar sound function(R m ),the van der Waals constant (b),molar compressibility(W),intermolecular free length(L f ),relaxation strength(r),solvation number(S n ),were calculated.The results are in terpret-ed in terms of molecular interactions occurring in the solutions.
文摘The Ni/SBA-15 catalysts were synthesized using the in situ method and the influence of crystallization temperature on nickel utilization efficiency-a critical factor in mesoporous material design-was systematically investigated.The structural characteristics and nickel anchoring capacity were analyzed using XRD,BET,FT-IR,H2-TPR,and ICP-OES.The results demonstrated that the crystallization temperature significantly affected the framework order of SBA-15 and the surface anchoring efficiency of Ni ions.The nickel utilization efficiency increased from 8.4%at 80℃to 60.49%at 140℃,but then decreased to 47.25%at 160℃,indicating an optimal crystallization temperature window.This provides crucial guidance for tailoring high-performance metal-doped molecular sieves.The optimal catalyst exhibited excellent performance in the hydrogenation of 1,4-butynediol(BYD):the BYD conversion reached 97.25%with 88.99%selectivity of 1,4-butenediol(BED)within 5 h,and reached 99.73%with 87.34%selectivity of 1,4-butanediol(BDO)after 20 h reaction.These results revealed the critical role of crystallization temperature in metal utilization and provided theoretical support for designing highly active molecular sieve catalysts.
