An innovative green process of producing ε-caprolactam was proposed by integrating ammoximation and Beckmann rearrangement effectively. As a first part of the new process, TS-1 molecular sieve-catalyzed synthesis of ...An innovative green process of producing ε-caprolactam was proposed by integrating ammoximation and Beckmann rearrangement effectively. As a first part of the new process, TS-1 molecular sieve-catalyzed synthesis of cyclohexanone oxime from cyclohexanone, ammonia and hydrogen peroxide was carried out in a batch plant. Cyclohexane was used as the solvent in the three-phase reaction system. The influences of essential process parameters on ammoximation were investigated. Under the reaction conditions as catalyst content of 2.5% (by mass); H 2 O 2 /yclohexanone molar ratio of 1.10; NH 3 /cyclohexanone molar ratio of 2.20; reaction temperature of 343 K; reaction time of 5 h, high conversion of cyclohexanone and selectivity to oxime (both>99%) were obtained. Thus, the three-phase ammoximation process showed equal catalytic activity as TS-1 but much more convenient and simpler for the separation of catalyst in comparison to the industrial two-phase system with t-butanol used as solvent.展开更多
Silicon carbide(SiC)was used as a support for SSZ‐13zeolite in an attempt to improve the high‐temperature stability and activity of Cu/SSZ‐13in the selective catalytic reduction(SCR)of NO with NH3.SSZ‐13was grown ...Silicon carbide(SiC)was used as a support for SSZ‐13zeolite in an attempt to improve the high‐temperature stability and activity of Cu/SSZ‐13in the selective catalytic reduction(SCR)of NO with NH3.SSZ‐13was grown via a hydrothermal method using the silicon and silica contained in SiC as the source of silicon,which led to the formation of a chemically bonded SSZ‐13layer on SiC.Characterization using X‐ray diffraction,scanning electron microscopy,and N2adsorption‐desorption isotherms revealed that the alkali content strongly affected the purity of zeolite and the crystallization time affected the coverage and crystallinity of the zeolite layer.Upon ion exchange,the resulting Cu/SSZ‐13@SiC catalyst exhibited enhanced activity in NH3‐SCR in the high‐temperature region compared with the unsupported Cu/SSZ‐13.Thus,the application temperature was extended with the use of SiC as the support.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
A new catalytic chemical vapor process for depositing silicon nitride films using silane hydrazine gaseous mixture is described. This system can be useful at a temperature of lower than 400 ℃. The catalytic process ...A new catalytic chemical vapor process for depositing silicon nitride films using silane hydrazine gaseous mixture is described. This system can be useful at a temperature of lower than 400 ℃. The catalytic process gives more rapid deposition rate than 10 nm/min. The atomic composition ratio, N/Si, which is evaluated by Rutherfold backscattering method is about 1.4 under a given experimental conditions more than the stoichiometric value of 1.33 in Si 3N 4. The infrared transmission spectra show a large dip at 850 cm -1 due to Si-N bonds and no clear dip due to Si-O bonds. High N-H bond density is the evidence that the deposition mechanism is limited by N-N bond breaking of the hydrazine. The H contents, evaluated from Si-H and N-H bonds in the infrared absorption spectra, and the deposition rate are measured as a function of the substrate temperature. In addition some film properties such as the resistivity and the breakdown electric field are presented.展开更多
Magnesium hydroxide(MH),which is commonly used as a halogen-free flame retardant filler in composite materials,was modified by silanization reaction with γ-aminopropyltriethoxysilane (γ-APS) in aqueous solution at d...Magnesium hydroxide(MH),which is commonly used as a halogen-free flame retardant filler in composite materials,was modified by silanization reaction with γ-aminopropyltriethoxysilane (γ-APS) in aqueous solution at different pH values (pH range from 8.0 to 12.0). The surface properties of grafted γ-APS on MH surface as a function of solution pH value were studied using elemental analysis,Fourier transform infrared spectroscopy and zeta potential measurement. The results show that hydrolysis and condensation of γ-APS are activated in alkaline solution and lead to multilayer adsorption of γ-APS molecules on the surface of MH. The type of adsorption orientation of γ-APS on MH surface is a function of coverage density that is altered by changing solution pH value. At low coverage density (e.g. 55 nm-2),γ-APS molecules are preferentially adsorbed to the surface with the silicon moiety towards the surface,and increasing coverage density (e.g. 90 nm-2) leads to parallel orientation. At an even higher coverage density (e.g. 115 nm-2),γ-APS molecules bond to the surface with the amino moiety towards the surface.展开更多
A new and an inexpensive adsorbent of chitosan coated silica for immobilized metal affinity chromatography (IMIC) was studied. After a double coating, the chitosan coated on silica beads could be up to 53. 4 mg/g sili...A new and an inexpensive adsorbent of chitosan coated silica for immobilized metal affinity chromatography (IMIC) was studied. After a double coating, the chitosan coated on silica beads could be up to 53. 4 mg/g silica beads.When pH＞3. 8, the metal ligand Cu2+ was chelated on the coated chitosan witha bound capacity of 14. 6 mg/g chitosan without introducing iminodiacetic acid(IDA).展开更多
基金Supported by the National Natural Science Foundation of China and Sinopec (20736009)
文摘An innovative green process of producing ε-caprolactam was proposed by integrating ammoximation and Beckmann rearrangement effectively. As a first part of the new process, TS-1 molecular sieve-catalyzed synthesis of cyclohexanone oxime from cyclohexanone, ammonia and hydrogen peroxide was carried out in a batch plant. Cyclohexane was used as the solvent in the three-phase reaction system. The influences of essential process parameters on ammoximation were investigated. Under the reaction conditions as catalyst content of 2.5% (by mass); H 2 O 2 /yclohexanone molar ratio of 1.10; NH 3 /cyclohexanone molar ratio of 2.20; reaction temperature of 343 K; reaction time of 5 h, high conversion of cyclohexanone and selectivity to oxime (both>99%) were obtained. Thus, the three-phase ammoximation process showed equal catalytic activity as TS-1 but much more convenient and simpler for the separation of catalyst in comparison to the industrial two-phase system with t-butanol used as solvent.
基金supported by the INCOEmission project coordinated by BASF SE,Germanythe support from the Fundamental Research Funds for the Central Universities(DC201502080409)~~
文摘Silicon carbide(SiC)was used as a support for SSZ‐13zeolite in an attempt to improve the high‐temperature stability and activity of Cu/SSZ‐13in the selective catalytic reduction(SCR)of NO with NH3.SSZ‐13was grown via a hydrothermal method using the silicon and silica contained in SiC as the source of silicon,which led to the formation of a chemically bonded SSZ‐13layer on SiC.Characterization using X‐ray diffraction,scanning electron microscopy,and N2adsorption‐desorption isotherms revealed that the alkali content strongly affected the purity of zeolite and the crystallization time affected the coverage and crystallinity of the zeolite layer.Upon ion exchange,the resulting Cu/SSZ‐13@SiC catalyst exhibited enhanced activity in NH3‐SCR in the high‐temperature region compared with the unsupported Cu/SSZ‐13.Thus,the application temperature was extended with the use of SiC as the support.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
文摘A new catalytic chemical vapor process for depositing silicon nitride films using silane hydrazine gaseous mixture is described. This system can be useful at a temperature of lower than 400 ℃. The catalytic process gives more rapid deposition rate than 10 nm/min. The atomic composition ratio, N/Si, which is evaluated by Rutherfold backscattering method is about 1.4 under a given experimental conditions more than the stoichiometric value of 1.33 in Si 3N 4. The infrared transmission spectra show a large dip at 850 cm -1 due to Si-N bonds and no clear dip due to Si-O bonds. High N-H bond density is the evidence that the deposition mechanism is limited by N-N bond breaking of the hydrazine. The H contents, evaluated from Si-H and N-H bonds in the infrared absorption spectra, and the deposition rate are measured as a function of the substrate temperature. In addition some film properties such as the resistivity and the breakdown electric field are presented.
基金Projects(50574104 50574102) supported by the National Natural Science Foundation of China
文摘Magnesium hydroxide(MH),which is commonly used as a halogen-free flame retardant filler in composite materials,was modified by silanization reaction with γ-aminopropyltriethoxysilane (γ-APS) in aqueous solution at different pH values (pH range from 8.0 to 12.0). The surface properties of grafted γ-APS on MH surface as a function of solution pH value were studied using elemental analysis,Fourier transform infrared spectroscopy and zeta potential measurement. The results show that hydrolysis and condensation of γ-APS are activated in alkaline solution and lead to multilayer adsorption of γ-APS molecules on the surface of MH. The type of adsorption orientation of γ-APS on MH surface is a function of coverage density that is altered by changing solution pH value. At low coverage density (e.g. 55 nm-2),γ-APS molecules are preferentially adsorbed to the surface with the silicon moiety towards the surface,and increasing coverage density (e.g. 90 nm-2) leads to parallel orientation. At an even higher coverage density (e.g. 115 nm-2),γ-APS molecules bond to the surface with the amino moiety towards the surface.
文摘A new and an inexpensive adsorbent of chitosan coated silica for immobilized metal affinity chromatography (IMIC) was studied. After a double coating, the chitosan coated on silica beads could be up to 53. 4 mg/g silica beads.When pH＞3. 8, the metal ligand Cu2+ was chelated on the coated chitosan witha bound capacity of 14. 6 mg/g chitosan without introducing iminodiacetic acid(IDA).
