With the aim of deep desulfurization, silica-supported polyoxometalate-based ionic liquids were successfully prepared by a one-pot hydrothermal process and employed in heterogeneous oxidative desulfurization of variou...With the aim of deep desulfurization, silica-supported polyoxometalate-based ionic liquids were successfully prepared by a one-pot hydrothermal process and employed in heterogeneous oxidative desulfurization of various sulfur compounds. The compositions and structures of the hybrid samples were characterized by various methods such as FT-IR, XPS, Raman,UV–Vis, wide-angle XRD and N2adsorption–desorption. The experimental results indicated that the hybrid materials presented a high dispersion of tungsten species and excellent catalytic activity for the removal of 4,6-dimethyldibenzothiophene without any organic solvent as extractant, and the sulfur removal could reach 100.0% under mild conditions.The catalytic performance on various substrates was also investigated in detail. After cycling seven cycles, the sulfur removal of the heterogeneous system still reached 93.0%. The GC-MS analysis results demonstrated that the sulfur compound was first adsorbed by the catalyst and subsequently oxidized to its corresponding sulfone.展开更多
Silica-supported tin chloride and titanium tetrachloride were prepared by the reaction of tin chloride and titanium tetrachloride with activated silica gel in refluxing toluene.These solid acids have been employed as ...Silica-supported tin chloride and titanium tetrachloride were prepared by the reaction of tin chloride and titanium tetrachloride with activated silica gel in refluxing toluene.These solid acids have been employed as the catalysts for the synthesis of bisdihydropyrimidin -2(1H)-ones from aromatic dialdehydes,1,3-dicarbonyl compounds and urea at 90℃under solvent-free conditions.展开更多
The hydrogenation of toluidines catalyzed by silica-supported carboxymethyl cellulose platinum complex forms methylcyclohexlamines in high yields, such as m-toluidine to 3-methylcyclohexylamine, o-toluidine to 2-methy...The hydrogenation of toluidines catalyzed by silica-supported carboxymethyl cellulose platinum complex forms methylcyclohexlamines in high yields, such as m-toluidine to 3-methylcyclohexylamine, o-toluidine to 2-methylcyclohexylamine, and p-toluidine to 4-methylcyclohexylamine in 97%, 96.7% and 98.2% yields, respectively, at 30 ℃ and under atmospheric hydrogen pressure. The yields were remarkably affected by the Pt content in the complex, the kind of solvent and the reaction temperature. The catalyst was very stable and could be reused several times without remarkable change in the catalytic activity.展开更多
A silica-supported carboxymethylcellulose platinum complex (abbreviated as SiO_2-CMC-Pt) has been prepared and characterized by XPS. Its catalytic properties for hydro-genation of aromatic compounds were studied. The ...A silica-supported carboxymethylcellulose platinum complex (abbreviated as SiO_2-CMC-Pt) has been prepared and characterized by XPS. Its catalytic properties for hydro-genation of aromatic compounds were studied. The results showed that this catalystcould catalyze the hydrogenation of phenol, anisol, p-cresol, benzene and toluene to cyclo-hexanol, cyclohexyl methyl ether, p-methyl cyclohexanol, cyclohexane and methylcyclo-hexane, respectively in 100% yield at 30℃ and 1 atm. In the hydrogenation of phenol,COO/Pt ratio in SiO_2-CMC-Pt has much influence on the initial hydrogenation rate andthe selectivity for the intermediate product, cyclohexanone. The highest initial rate andthe highest yield of cyclohexanone both occur at COO/Pt ratio of 6. The complex is stableduring the reaction and can be used repeatedly.展开更多
A silica-supported poly-γ- aminopropylsiloxane-rhodium-cobalt bimetallic complex(abbreviated as SiO_2-NH_2-Rh-Co)has been prepared and used as catalyst for hydroformylationof methyl methacrylate. The results showed t...A silica-supported poly-γ- aminopropylsiloxane-rhodium-cobalt bimetallic complex(abbreviated as SiO_2-NH_2-Rh-Co)has been prepared and used as catalyst for hydroformylationof methyl methacrylate. The results showed that the catalyst could catalyze the reaction in95.6% conversion with 92.8% selectivity for the normal aldehyde, methyl β-formylisobu-tyrate. Such catalyst also showed high stability during the reaction and could be used repeat-edly.展开更多
Methyl-(γ-chloropropyl)dichlorosilane was synthesized under the catalysis of a silicasupported Karstedt-type catalyst. By orthogonal experimental design method, the optimum reaction parameters such as reactants rat...Methyl-(γ-chloropropyl)dichlorosilane was synthesized under the catalysis of a silicasupported Karstedt-type catalyst. By orthogonal experimental design method, the optimum reaction parameters such as reactants ratio, reaction temperature and time, and the dosage of catalyst, were determined. At the optimum reaction condition the product yield reached 78.42%, which is higher than that reported in the literatures.展开更多
A natural polymer catalyst, silica-supported chitosan palladium complex (abbr. as SiO2-CS-Pd) was found to catalyze the hydrogenation of phenol and cresols to corresponding cyclohexanones in high yield and 100% select...A natural polymer catalyst, silica-supported chitosan palladium complex (abbr. as SiO2-CS-Pd) was found to catalyze the hydrogenation of phenol and cresols to corresponding cyclohexanones in high yield and 100% selectivity at 70 degrees C and 1.01325 x 10(5) Pa mild conditions. N/Pd molar ratio in the complex, temperature and solvents have much influence on the reaction. The reactivity order of reactants was found to be: phenol >m->p->o- The catalyst is stable during the reaction and could be repeatedly used for several times without much decrease in its catalytic activity.展开更多
Supported catalysts based on metal nanoparticles are a class of widely used heterogeneous catalysts in industry.The catalytic performances of supported metal catalysts are highly determined by many parameters of metal...Supported catalysts based on metal nanoparticles are a class of widely used heterogeneous catalysts in industry.The catalytic performances of supported metal catalysts are highly determined by many parameters of metal nanoparticles such as their particle size,composition,surface structure and also interfacial interaction with supports[1].Supported metal catalysts are展开更多
Application of sulfuric acid immobilized on silica gel as an efficient and benign catalyst has been explored in the syn-thesis of 2,4,5-Triaryl-1H-imidazoles via condensation reaction of benzil or benzoin, aldehyde an...Application of sulfuric acid immobilized on silica gel as an efficient and benign catalyst has been explored in the syn-thesis of 2,4,5-Triaryl-1H-imidazoles via condensation reaction of benzil or benzoin, aldehyde and ammonium acetate. The key advantages of this process are high yields, cost effectiveness of catalyst, easy work-up, purification of products by non-chromatographic method and the reusability of the H2SO4.SiO2 catalyst.展开更多
基金financially supported by the National Nature Science Foundation of China (Nos. 21776116, 21576122, 21722604)Postdoctoral Foundation of China (No. 2017M621646)+1 种基金Postdoctoral Foundation of Jiangsu Province (No. 2018K083C)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
文摘With the aim of deep desulfurization, silica-supported polyoxometalate-based ionic liquids were successfully prepared by a one-pot hydrothermal process and employed in heterogeneous oxidative desulfurization of various sulfur compounds. The compositions and structures of the hybrid samples were characterized by various methods such as FT-IR, XPS, Raman,UV–Vis, wide-angle XRD and N2adsorption–desorption. The experimental results indicated that the hybrid materials presented a high dispersion of tungsten species and excellent catalytic activity for the removal of 4,6-dimethyldibenzothiophene without any organic solvent as extractant, and the sulfur removal could reach 100.0% under mild conditions.The catalytic performance on various substrates was also investigated in detail. After cycling seven cycles, the sulfur removal of the heterogeneous system still reached 93.0%. The GC-MS analysis results demonstrated that the sulfur compound was first adsorbed by the catalyst and subsequently oxidized to its corresponding sulfone.
文摘Silica-supported tin chloride and titanium tetrachloride were prepared by the reaction of tin chloride and titanium tetrachloride with activated silica gel in refluxing toluene.These solid acids have been employed as the catalysts for the synthesis of bisdihydropyrimidin -2(1H)-ones from aromatic dialdehydes,1,3-dicarbonyl compounds and urea at 90℃under solvent-free conditions.
文摘The hydrogenation of toluidines catalyzed by silica-supported carboxymethyl cellulose platinum complex forms methylcyclohexlamines in high yields, such as m-toluidine to 3-methylcyclohexylamine, o-toluidine to 2-methylcyclohexylamine, and p-toluidine to 4-methylcyclohexylamine in 97%, 96.7% and 98.2% yields, respectively, at 30 ℃ and under atmospheric hydrogen pressure. The yields were remarkably affected by the Pt content in the complex, the kind of solvent and the reaction temperature. The catalyst was very stable and could be reused several times without remarkable change in the catalytic activity.
文摘A silica-supported carboxymethylcellulose platinum complex (abbreviated as SiO_2-CMC-Pt) has been prepared and characterized by XPS. Its catalytic properties for hydro-genation of aromatic compounds were studied. The results showed that this catalystcould catalyze the hydrogenation of phenol, anisol, p-cresol, benzene and toluene to cyclo-hexanol, cyclohexyl methyl ether, p-methyl cyclohexanol, cyclohexane and methylcyclo-hexane, respectively in 100% yield at 30℃ and 1 atm. In the hydrogenation of phenol,COO/Pt ratio in SiO_2-CMC-Pt has much influence on the initial hydrogenation rate andthe selectivity for the intermediate product, cyclohexanone. The highest initial rate andthe highest yield of cyclohexanone both occur at COO/Pt ratio of 6. The complex is stableduring the reaction and can be used repeatedly.
文摘A silica-supported poly-γ- aminopropylsiloxane-rhodium-cobalt bimetallic complex(abbreviated as SiO_2-NH_2-Rh-Co)has been prepared and used as catalyst for hydroformylationof methyl methacrylate. The results showed that the catalyst could catalyze the reaction in95.6% conversion with 92.8% selectivity for the normal aldehyde, methyl β-formylisobu-tyrate. Such catalyst also showed high stability during the reaction and could be used repeat-edly.
基金support from the National Natural Science Foundation of China(No.50473036)
文摘Methyl-(γ-chloropropyl)dichlorosilane was synthesized under the catalysis of a silicasupported Karstedt-type catalyst. By orthogonal experimental design method, the optimum reaction parameters such as reactants ratio, reaction temperature and time, and the dosage of catalyst, were determined. At the optimum reaction condition the product yield reached 78.42%, which is higher than that reported in the literatures.
文摘A natural polymer catalyst, silica-supported chitosan palladium complex (abbr. as SiO2-CS-Pd) was found to catalyze the hydrogenation of phenol and cresols to corresponding cyclohexanones in high yield and 100% selectivity at 70 degrees C and 1.01325 x 10(5) Pa mild conditions. N/Pd molar ratio in the complex, temperature and solvents have much influence on the reaction. The reactivity order of reactants was found to be: phenol >m->p->o- The catalyst is stable during the reaction and could be repeatedly used for several times without much decrease in its catalytic activity.
文摘Supported catalysts based on metal nanoparticles are a class of widely used heterogeneous catalysts in industry.The catalytic performances of supported metal catalysts are highly determined by many parameters of metal nanoparticles such as their particle size,composition,surface structure and also interfacial interaction with supports[1].Supported metal catalysts are
文摘Application of sulfuric acid immobilized on silica gel as an efficient and benign catalyst has been explored in the syn-thesis of 2,4,5-Triaryl-1H-imidazoles via condensation reaction of benzil or benzoin, aldehyde and ammonium acetate. The key advantages of this process are high yields, cost effectiveness of catalyst, easy work-up, purification of products by non-chromatographic method and the reusability of the H2SO4.SiO2 catalyst.