A simple and general strategy is described for preparing network supported catalyst through a one-pot synthetic procedure using supramolecular gel as template.This procedure directly attaches ligand to support during ...A simple and general strategy is described for preparing network supported catalyst through a one-pot synthetic procedure using supramolecular gel as template.This procedure directly attaches ligand to support during fabricating the support.Using this strategy,supported CuBr/di-（2-picolyl） amine catalyst with U-shaped fibrillar network was prepared and used in atom transfer radical polymerization of methyl methacrylate.XPS and SEM characterization of the catalyst revealed homogeneous distribution of ligand,sufficient reactive sites,adequate mechanical strength and macroporosity.The polymerization results demonstrated high activity and reusability of such catalyst.This strategy might be extended to other supported catalysts used in column reactors.展开更多
CeO2-promoted Ni/Al2O3-ZrO2 （Ni/Al2O3-ZrO2-CeO2） catalysts were prepared by a direct sol-gel process with citric acid as gelling agent. The catalysts used for the methane reforming with CO2 was studied by infrared s...CeO2-promoted Ni/Al2O3-ZrO2 （Ni/Al2O3-ZrO2-CeO2） catalysts were prepared by a direct sol-gel process with citric acid as gelling agent. The catalysts used for the methane reforming with CO2 was studied by infrared spectroscopy （IR）, thermal gravimetric analysis （TGA）, microscopic analysis, X-ray diffraction （XRD） and temperature-programmed reduction （TPR）. The catalytic performance for CO2 reforming of methane to synthesis gas was investigated in a continuous-flow micro-reactor under atmospheric pressure. TGA, IR, XRD and microscopic analysis show that the catalysts prepared by the direct sol-gel process consist of Ni particles with a nanostructure of around 5 nm and an amorphous-phase composite oxide support. There exists a chemical interaction between metallic Ni particles and supports, which makes metallic Ni well dispersed, highly active and stable. The addition of CeO2 effectively improves the dispersion and the stability of Ni particles of the prepared catalysts, and enhances the adsorption of CO2 on the surface of catalysts. The catalytic tests for methane reforming with CO2 to synthesis gas show that the Ni/Al2O3-ZrO2-CeO2 catalysts show excellent activity and stability compared with the Ni/Al2O3 catalyst. The excellent catalytic activity and stability of the Ni/Al2O3-ZrO2-CeO2 are attributed to the highly, uniformly and stably dispersed small metallic Ni particles, the high reducibility of the Ni oxides and the interaction between metallic Ni particles and the composite oxide supports.展开更多
Three new catalysts based on the silica gel supported polyether ionic liquids(ILs), i.e., [HO-PECH-MIM]ClSi, [H2N-PECH-MIM]Cl-Si, and [HOOC-PECH-MIM]Cl-Si, were prepared, and their chemical structures were characteriz...Three new catalysts based on the silica gel supported polyether ionic liquids(ILs), i.e., [HO-PECH-MIM]ClSi, [H2N-PECH-MIM]Cl-Si, and [HOOC-PECH-MIM]Cl-Si, were prepared, and their chemical structures were characterized by infrared(IR) spectroscopy and nuclear magnetic resonance(NMR) spectroscopy. Thermogravimetric analyzer(TG), X-ray diffractometer(XRD) and scanning electron microscope(SEM) were used to evaluate their thermal stability,crystalline structure and apparent morphology, respectively. Surface areas of the prepared catalysts were calculated by the Brunauer-Emmett-Teller(BET) method. The catalytic reaction for the synthesis of propylene carbonate(PC) using CO_2 and propylene oxide(PO) in the presence of the prepared catalysts was studied. The influences of times of recycling and catalyst structure on catalytic performance were also investigated. The experimental results showed that the silica gel supported polyether ILs catalysts successfully prepared under mild condition could possess the advantages of high activity, excellent thermal stability, good selectivity and easy recycling, while the phase transition of the liquid polyether ILs catalysts was also achieved. When the reaction temperature was 90 °C, the CO_2 pressure was 2.0 MPa and the dosage of the catalyst was 2.5%, [HOOC-PECH-MIM]Cl-Si was found to have the best catalytic performance in the catalytic process, with the conversion rate reaching 100% and the selectivity equating to 98.2%. The conversion rate and selectivity still could reach more than 90% even after the catalyst was reused for 15 times.展开更多
The nickel-based catalysts were prepared by the sol-gel method and used for the CH4 reforming with CO2. The effects of the sol-gel method on the specific surface area, catalytic activity, desorption, and reduction per...The nickel-based catalysts were prepared by the sol-gel method and used for the CH4 reforming with CO2. The effects of the sol-gel method on the specific surface area, catalytic activity, desorption, and reduction performances of catalysts were investigated with BET, TPR, and TPD. Compared with the catalyst prepared by the impregnation method, the results indicated that the catalysts prepared by the sol-gel method had larger specific surface area, showing higher catalytic activities and exhibiting perfect desorption and reduction performances. In addition, the modification effects of adding La were studied, and it was found that the 0.75NLBT catalyst constituted of 5wt.%Ni-0.75wt.%La was optimal.展开更多
This paper reports that by using the hydrofluoric acid （HF） as the acid catalyst, F doped nanoporous low-k SiO2 thin films have been prepared by means of sol-gel method. The characterization of atomic force microsco...This paper reports that by using the hydrofluoric acid （HF） as the acid catalyst, F doped nanoporous low-k SiO2 thin films have been prepared by means of sol-gel method. The characterization of atomic force microscopy and Fourier transform infrared spectroscopy demonstrates that the HF catalyzed films are more hydrophobic. The N2 adsorption/desorption experiments show that the suited introduction of HF increases the porosity and decreases the pore size distribution （about 10 nm） in the films. The above results indicate that the hydrofluoric acid is the more suitable acid catalyst than the hydrochloric one for preparing nanoporous ultra low-k SiO2 thin films.展开更多
In this research work silica coating was produced on nickel substrates by a sol-gel process. In order to increase the rate of hydrolysis and to reduce the rate of polymerization several acid catalysts including nitric...In this research work silica coating was produced on nickel substrates by a sol-gel process. In order to increase the rate of hydrolysis and to reduce the rate of polymerization several acid catalysts including nitric acid-hydrochloric acid, acetic acid, hydrochloric acid and nitric acid were add to silica sol. Conversely, in order to control the rate of hydrolysis and to increase the rate of polymerization, basic catalyst of ammonia and ammonia hydroxyl were introduced in to the solution. Nickel specimens of known surface roughness were chemically cleaned and prepared by dipping in the sols. In order to produce a suitable silica coating the drying and firing cycles were optimized on these substrates. The structure and uniformity of the coatings produced were examined by scanning electron microscopy. Coatings composition was determined using glow discharge optical spectroscopy and EDAX microanalysis. Experimental result showed that hydrochloric acid, acetic acid, ammonia and acetic acid - ammonia are suitable catalytic agents for silica coating formation on nickel type substrate.展开更多
Carbon aerogels (CAG) were synthesized by the pyrolysis of resorcinol-furfural based organic aerogels, derived from sol-gel polymerization of resorcinol and furfural using different catalysts followed by supercritical...Carbon aerogels (CAG) were synthesized by the pyrolysis of resorcinol-furfural based organic aerogels, derived from sol-gel polymerization of resorcinol and furfural using different catalysts followed by supercritical drying of as-prepared gels. Different catalysts viz. hydrochloric acid (HA), acetic acid (AcH) and hexamethylenetetramine (HMTA) of different concentrations were used for this purpose in order to study the role of different catalysts and the effect of R/C ratio (reactant to catalyst molar ratio) on the formation of organic gel monolith and their physical properties were investigated. Aerogels were thoroughly characterized by using CHN, FTIR, TG-DSC, XRD and SEM. A considerable reduction of gelation time and the formation of relatively denser organic gel were observed in the case of HMTA, which indicated the dual role (catalyst & cross-linking agent) of HMTA during the polymerization/polycondensation of resorcinol and furfural. Carbon aerogels obtained by using different catalysts showed BET surface area, average pore size, total pore volumes in the range of 438 496 m2/g, 17.9 22.4 ? and 0.20 0.27 cm3/g, respectively. The SEM images and results revealed the presence of different morphologies of carbon aerogels, obtained by using different catalysts. The HMTA catalyzed samples were found to have highest surface area with particles in smaller in size and well interconnected 3D carbon network.展开更多
Bi2O3· 3MoO3 oxide catalyst has been prepared by the sol gel pr℃ ess at lower temperature. The influences of preparation conditions and thermal treatment conditions on the morphology and structure of the catalys...Bi2O3· 3MoO3 oxide catalyst has been prepared by the sol gel pr℃ ess at lower temperature. The influences of preparation conditions and thermal treatment conditions on the morphology and structure of the catalyst have been studied by using TEM, DTA TG, FT IR, XRD and BET surface area measurement methods. It is shown that the BET surface area of Bi2O3· 3MoO3 prepared by sol gel method is larger than that of Bi2O3· 3MoO3 prepared by coprecipitation method. For the preparation of the well distribuated Bi2O3· 3MoO3 catalyst has a BET surface area of 13.2m2· g－ 1, the optimum conditions for the catalyst are :展开更多
The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed...The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed that the Ni/TiO2-SiO2 catalyst calcined at 700 ℃ had high and stable activity while the catalysts calcined at 550 and 850 ℃ had low and unstable activity. Depending on the calcination temperature, one, two, or three of the following Ni-containing species, NiO, Ni2.44Ti0.72Si0.07O4, and NiTiO3 were identified by combining the temperature programmed reduction （TPR） and X-ray diffraction （XRD） results. Their reducibility decreased in the sequence： NiO〉Ni2.44Ti0.72Si0.07O4〉NiTiO3. It suggests that high and stable activities observed over the Ni/TiO2-SiO2 catalyst calcined at 700 ~C were induced by the formation of Ni2.44Ti0.72Si0.07O4 and smaller NiO species crystallite size.展开更多
FeOx-SiO2 catalysts prepared by a sol-gel method were studied for the selective oxidation of methane by oxygen. A single-pass formaldehyde yield of 2.0% was obtained over the FeOx-SiO2 with an iron content of 0.5 wt% ...FeOx-SiO2 catalysts prepared by a sol-gel method were studied for the selective oxidation of methane by oxygen. A single-pass formaldehyde yield of 2.0% was obtained over the FeOx-SiO2 with an iron content of 0.5 wt% at 898 K. This 0.5 wt% FeOx-SiO2 catalyst demonstrated significantly higher catalytic performances than the 0.5 wt% FeOx/SiO2 prepared by an impregnation method. The correlation between the catalytic performances and the characterizations with UV-Vis and H2-TPR suggested that the higher dispersion of iron species in the catalyst prepared by the sol-gel method was responsible for its higher catalytic activity for formaldehyde formation. The modification of the FeOx-SiO2 by phosphorus enhanced the formaldehyde selectivity, and a single-pass formaldehyde yield of 2.4% could be attained over a P-FeOx-SiO2 catalyst （P/Fe = 0.5） at 898 K. Raman spectroscopic measurements indicated the formation of FePO4 nanoclusters in this catalyst, which were more selective toward formaldehyde formation.展开更多
基金support from the National Natural Science Foundation of China(Nos.20574041 and 20874055)Hi-tech Research and Development Program(863 plan) of China(No.2009AA062903)
文摘A simple and general strategy is described for preparing network supported catalyst through a one-pot synthetic procedure using supramolecular gel as template.This procedure directly attaches ligand to support during fabricating the support.Using this strategy,supported CuBr/di-（2-picolyl） amine catalyst with U-shaped fibrillar network was prepared and used in atom transfer radical polymerization of methyl methacrylate.XPS and SEM characterization of the catalyst revealed homogeneous distribution of ligand,sufficient reactive sites,adequate mechanical strength and macroporosity.The polymerization results demonstrated high activity and reusability of such catalyst.This strategy might be extended to other supported catalysts used in column reactors.
基金supported by the National Natural Science Foundation of China (NO. 20976013, 21006057)
文摘CeO2-promoted Ni/Al2O3-ZrO2 （Ni/Al2O3-ZrO2-CeO2） catalysts were prepared by a direct sol-gel process with citric acid as gelling agent. The catalysts used for the methane reforming with CO2 was studied by infrared spectroscopy （IR）, thermal gravimetric analysis （TGA）, microscopic analysis, X-ray diffraction （XRD） and temperature-programmed reduction （TPR）. The catalytic performance for CO2 reforming of methane to synthesis gas was investigated in a continuous-flow micro-reactor under atmospheric pressure. TGA, IR, XRD and microscopic analysis show that the catalysts prepared by the direct sol-gel process consist of Ni particles with a nanostructure of around 5 nm and an amorphous-phase composite oxide support. There exists a chemical interaction between metallic Ni particles and supports, which makes metallic Ni well dispersed, highly active and stable. The addition of CeO2 effectively improves the dispersion and the stability of Ni particles of the prepared catalysts, and enhances the adsorption of CO2 on the surface of catalysts. The catalytic tests for methane reforming with CO2 to synthesis gas show that the Ni/Al2O3-ZrO2-CeO2 catalysts show excellent activity and stability compared with the Ni/Al2O3 catalyst. The excellent catalytic activity and stability of the Ni/Al2O3-ZrO2-CeO2 are attributed to the highly, uniformly and stably dispersed small metallic Ni particles, the high reducibility of the Ni oxides and the interaction between metallic Ni particles and the composite oxide supports.
基金supported by the National Natural Science Foundation of China (NSFC 21706163)the Liaoning Province Department of Education Foundation (LQGD2017020)
文摘Three new catalysts based on the silica gel supported polyether ionic liquids(ILs), i.e., [HO-PECH-MIM]ClSi, [H2N-PECH-MIM]Cl-Si, and [HOOC-PECH-MIM]Cl-Si, were prepared, and their chemical structures were characterized by infrared(IR) spectroscopy and nuclear magnetic resonance(NMR) spectroscopy. Thermogravimetric analyzer(TG), X-ray diffractometer(XRD) and scanning electron microscope(SEM) were used to evaluate their thermal stability,crystalline structure and apparent morphology, respectively. Surface areas of the prepared catalysts were calculated by the Brunauer-Emmett-Teller(BET) method. The catalytic reaction for the synthesis of propylene carbonate(PC) using CO_2 and propylene oxide(PO) in the presence of the prepared catalysts was studied. The influences of times of recycling and catalyst structure on catalytic performance were also investigated. The experimental results showed that the silica gel supported polyether ILs catalysts successfully prepared under mild condition could possess the advantages of high activity, excellent thermal stability, good selectivity and easy recycling, while the phase transition of the liquid polyether ILs catalysts was also achieved. When the reaction temperature was 90 °C, the CO_2 pressure was 2.0 MPa and the dosage of the catalyst was 2.5%, [HOOC-PECH-MIM]Cl-Si was found to have the best catalytic performance in the catalytic process, with the conversion rate reaching 100% and the selectivity equating to 98.2%. The conversion rate and selectivity still could reach more than 90% even after the catalyst was reused for 15 times.
基金supported by the Jiangxi Provincial Department of Education
文摘The nickel-based catalysts were prepared by the sol-gel method and used for the CH4 reforming with CO2. The effects of the sol-gel method on the specific surface area, catalytic activity, desorption, and reduction performances of catalysts were investigated with BET, TPR, and TPD. Compared with the catalyst prepared by the impregnation method, the results indicated that the catalysts prepared by the sol-gel method had larger specific surface area, showing higher catalytic activities and exhibiting perfect desorption and reduction performances. In addition, the modification effects of adding La were studied, and it was found that the 0.75NLBT catalyst constituted of 5wt.%Ni-0.75wt.%La was optimal.
文摘This paper reports that by using the hydrofluoric acid （HF） as the acid catalyst, F doped nanoporous low-k SiO2 thin films have been prepared by means of sol-gel method. The characterization of atomic force microscopy and Fourier transform infrared spectroscopy demonstrates that the HF catalyzed films are more hydrophobic. The N2 adsorption/desorption experiments show that the suited introduction of HF increases the porosity and decreases the pore size distribution （about 10 nm） in the films. The above results indicate that the hydrofluoric acid is the more suitable acid catalyst than the hydrochloric one for preparing nanoporous ultra low-k SiO2 thin films.
基金supported by electroceramics research center in Malek Ashtar university of Technology(Shahin-Shahr)and Isfahan university of Technology
文摘In this research work silica coating was produced on nickel substrates by a sol-gel process. In order to increase the rate of hydrolysis and to reduce the rate of polymerization several acid catalysts including nitric acid-hydrochloric acid, acetic acid, hydrochloric acid and nitric acid were add to silica sol. Conversely, in order to control the rate of hydrolysis and to increase the rate of polymerization, basic catalyst of ammonia and ammonia hydroxyl were introduced in to the solution. Nickel specimens of known surface roughness were chemically cleaned and prepared by dipping in the sols. In order to produce a suitable silica coating the drying and firing cycles were optimized on these substrates. The structure and uniformity of the coatings produced were examined by scanning electron microscopy. Coatings composition was determined using glow discharge optical spectroscopy and EDAX microanalysis. Experimental result showed that hydrochloric acid, acetic acid, ammonia and acetic acid - ammonia are suitable catalytic agents for silica coating formation on nickel type substrate.
文摘Carbon aerogels (CAG) were synthesized by the pyrolysis of resorcinol-furfural based organic aerogels, derived from sol-gel polymerization of resorcinol and furfural using different catalysts followed by supercritical drying of as-prepared gels. Different catalysts viz. hydrochloric acid (HA), acetic acid (AcH) and hexamethylenetetramine (HMTA) of different concentrations were used for this purpose in order to study the role of different catalysts and the effect of R/C ratio (reactant to catalyst molar ratio) on the formation of organic gel monolith and their physical properties were investigated. Aerogels were thoroughly characterized by using CHN, FTIR, TG-DSC, XRD and SEM. A considerable reduction of gelation time and the formation of relatively denser organic gel were observed in the case of HMTA, which indicated the dual role (catalyst & cross-linking agent) of HMTA during the polymerization/polycondensation of resorcinol and furfural. Carbon aerogels obtained by using different catalysts showed BET surface area, average pore size, total pore volumes in the range of 438 496 m2/g, 17.9 22.4 ? and 0.20 0.27 cm3/g, respectively. The SEM images and results revealed the presence of different morphologies of carbon aerogels, obtained by using different catalysts. The HMTA catalyzed samples were found to have highest surface area with particles in smaller in size and well interconnected 3D carbon network.
文摘Bi2O3· 3MoO3 oxide catalyst has been prepared by the sol gel pr℃ ess at lower temperature. The influences of preparation conditions and thermal treatment conditions on the morphology and structure of the catalyst have been studied by using TEM, DTA TG, FT IR, XRD and BET surface area measurement methods. It is shown that the BET surface area of Bi2O3· 3MoO3 prepared by sol gel method is larger than that of Bi2O3· 3MoO3 prepared by coprecipitation method. For the preparation of the well distribuated Bi2O3· 3MoO3 catalyst has a BET surface area of 13.2m2· g－ 1, the optimum conditions for the catalyst are :
文摘The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed that the Ni/TiO2-SiO2 catalyst calcined at 700 ℃ had high and stable activity while the catalysts calcined at 550 and 850 ℃ had low and unstable activity. Depending on the calcination temperature, one, two, or three of the following Ni-containing species, NiO, Ni2.44Ti0.72Si0.07O4, and NiTiO3 were identified by combining the temperature programmed reduction （TPR） and X-ray diffraction （XRD） results. Their reducibility decreased in the sequence： NiO〉Ni2.44Ti0.72Si0.07O4〉NiTiO3. It suggests that high and stable activities observed over the Ni/TiO2-SiO2 catalyst calcined at 700 ~C were induced by the formation of Ni2.44Ti0.72Si0.07O4 and smaller NiO species crystallite size.
基金supported by the National Natural Science Foundation of China (Nos.20625310,20773099 and 20873110)the National Basic Programof China (No. 2005CB221408)the National Science Fund for Talent Training in Basic Science (No.J0630429)
文摘FeOx-SiO2 catalysts prepared by a sol-gel method were studied for the selective oxidation of methane by oxygen. A single-pass formaldehyde yield of 2.0% was obtained over the FeOx-SiO2 with an iron content of 0.5 wt% at 898 K. This 0.5 wt% FeOx-SiO2 catalyst demonstrated significantly higher catalytic performances than the 0.5 wt% FeOx/SiO2 prepared by an impregnation method. The correlation between the catalytic performances and the characterizations with UV-Vis and H2-TPR suggested that the higher dispersion of iron species in the catalyst prepared by the sol-gel method was responsible for its higher catalytic activity for formaldehyde formation. The modification of the FeOx-SiO2 by phosphorus enhanced the formaldehyde selectivity, and a single-pass formaldehyde yield of 2.4% could be attained over a P-FeOx-SiO2 catalyst （P/Fe = 0.5） at 898 K. Raman spectroscopic measurements indicated the formation of FePO4 nanoclusters in this catalyst, which were more selective toward formaldehyde formation.
