A sustainable process was explored for the preparation of 5-hydroxymethylfurfural(HMF) by catalytic degradation of the waste cotton stalk. Solid super-acid(SO_4^(2-)/ZrO_2) was used as an efficient catalyst for the de...A sustainable process was explored for the preparation of 5-hydroxymethylfurfural(HMF) by catalytic degradation of the waste cotton stalk. Solid super-acid(SO_4^(2-)/ZrO_2) was used as an efficient catalyst for the degradation of cotton stalk. Both decomposition experiments and kinetic study were conducted for the exploration of degradation condition and kinetics mechanism. The optimized experimental conditions are reaction temperature 503 K, reaction time 75 min and dosage of catalyst 30%(mass fraction) based on the decomposition experiments, under which a maximum yield of 27.2% for HMF could be achieved. Kinetic study was then carried out in the presence of SO_4^(2-)/ZrO_2. The theoretical results indicate that the activation energies for reducing sugar and HMF with catalyst are 96.71 k J/mol, 84.21 kJ/mol in the presence of SO_4^(2-)/ZrO_2, and they are 105.96 k J/mol and 119.37 k J/mol in the absence of SO_4^(2-)/ZrO_2.展开更多
Sulfated zirconia-lanthana （SO4^2-/ZrO2-La2O3） precursors were prepared by ultrasonic coprecipitation method and followed by aging at different temperature. The precursors were treated by 0.5 mol/L H2SO4. Samples of...Sulfated zirconia-lanthana （SO4^2-/ZrO2-La2O3） precursors were prepared by ultrasonic coprecipitation method and followed by aging at different temperature. The precursors were treated by 0.5 mol/L H2SO4. Samples of SO4^2-/ZrO2-La2O3 nano-crystalline catalysts were obtained by baking the treated precursors at different temperatures. The acidic properties of SO4^2-/ZrO2-La2O3 were tested by the Hammett indicator method. The phase composition, specific area, particle structure, and surface state were characterized by X-ray diffraction, BET, transmission electron microscopy, infrared spectrum, and X-ray photoelectron spec- troscopy. The catalytic activities were estimated by esterification of acetic acid with glycerin. It was shown that the catalyst prepared by ultrasonic stirring and low temperature （-15 ℃） exhibited highly active sites and high catalytic property.展开更多
Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts wer...Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.展开更多
A novel solid superacid catalyst S2O8^2-/ZrO2-CeO2 was prepared by a coprecipitation method and characterized by means of XRD FTIR, BET, TEM and DSC/TG analysis methods. The results indicated that incorporation of app...A novel solid superacid catalyst S2O8^2-/ZrO2-CeO2 was prepared by a coprecipitation method and characterized by means of XRD FTIR, BET, TEM and DSC/TG analysis methods. The results indicated that incorporation of appropriate amounts of Ce into the catalyst was beneficial to the formation of sole tetragonal ZrO2 and effectively prevented from the formation of monoclinic ZrO〉 and restrained the loss of sulfated species. XRD revealed the presence of tetragonal Ce0.16Zr0.84O2phase in the case of S2O8^2-/ZrO2-CeO2 calcined above 500 ℃. Catalytic activities of S2O8^2-/ZrO2-CeO2 for the esterification of lactic acid with n-butanol was studied. The results showed that the optimum conditions were as follows： calcination temperature of the catalyst 600 ℃, n（lactic acid）：n（n-butyl alcohol）=1.0：3.0, w（S2O8^2-/ZrO2- CeO2）=12.0%, reaction temperature 145 ℃, and reaction time 2 h. The esterification efficiency of lactic acid was about 96.6%.展开更多
SO4^2-/TiO2-MoO3, a novel solid superacid, has been prepared and its catalytic activity at different synthetic conditions was examined with esterification of n-butanoic acid and n-butyl alcohol as probing reaction.The...SO4^2-/TiO2-MoO3, a novel solid superacid, has been prepared and its catalytic activity at different synthetic conditions was examined with esterification of n-butanoic acid and n-butyl alcohol as probing reaction.The optimum conditions were also found, that is, the mass ratio of MoO3 used in the compound is 25%, the calcination temperature 450℃, and the soaked consistency of H2SO4 is 0.5mol.L^-1. Then it was applied in the catalytic synthesis of six similar important ketals and acetals as catalyst and revealed high catalytic activity. Under the condition that the molar ratio of aldehyde/ketone to glycol was 1:1.5, the mass ratio of the catalyst to the reactants was 0.5% and the reaction time 1.0 h, the yield of ketals and acetals reached up to 63.2%. The catalyst can be easily recovered and reused.展开更多
SO4^2- / TiO2-La2O3, a novel solid superacid, was prepared and its catalytic activities at different synthetic conditions are discussed with esterification of n-butanoic acid and n-butyl alcohol as probing reaction. T...SO4^2- / TiO2-La2O3, a novel solid superacid, was prepared and its catalytic activities at different synthetic conditions are discussed with esterification of n-butanoic acid and n-butyl alcohol as probing reaction. The optimum conditions have also been found, mole ratio of n（La^3＋）：n（Ti^4＋） is 1：34, the soaked consistency of H2SO4 is 0.8 tool/L, the soaked time of HESO4 is 24 h, the calcining temperature is 480 ℃, the calcining time is 3 h. Then it was applied in the catalytic synthesis often important ketals and acetals as catalyst and revealed high catalytic activity. Under these conditions on which the molar ratio of aldehyde/ketone to glycol is l： 1.5, the mass ratio of the catalyst used in the reactants is 0.5%, and the reaction time is 1.0 h, the yields of ketals and acetals can reach 41.4%-95.8%.展开更多
An efficient synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one is achieved via a reaction of acenaphthe-nequinone and indoles catalyzed by solid superacid SO4^2-/TiO2 under solvent-free conditions...An efficient synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one is achieved via a reaction of acenaphthe-nequinone and indoles catalyzed by solid superacid SO4^2-/TiO2 under solvent-free conditions at room temperature by grinding, which provides an efficient route to the synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one.This procedure offers several advantages including solvent-free conditions,excellent yields of products,simple work-up as well as reuse of catalysts which makes it a useful and attractive protocol for the synthesis of these compounds.展开更多
基金Project(2010DFA41440)supported by China-Japan International CooperationProject(2016TP1007)supported by the Hunan Provincial Science and Technology Plan,ChinaProject(21376269)supported by the National Natural Science Foundation of China
文摘A sustainable process was explored for the preparation of 5-hydroxymethylfurfural(HMF) by catalytic degradation of the waste cotton stalk. Solid super-acid(SO_4^(2-)/ZrO_2) was used as an efficient catalyst for the degradation of cotton stalk. Both decomposition experiments and kinetic study were conducted for the exploration of degradation condition and kinetics mechanism. The optimized experimental conditions are reaction temperature 503 K, reaction time 75 min and dosage of catalyst 30%(mass fraction) based on the decomposition experiments, under which a maximum yield of 27.2% for HMF could be achieved. Kinetic study was then carried out in the presence of SO_4^(2-)/ZrO_2. The theoretical results indicate that the activation energies for reducing sugar and HMF with catalyst are 96.71 k J/mol, 84.21 kJ/mol in the presence of SO_4^(2-)/ZrO_2, and they are 105.96 k J/mol and 119.37 k J/mol in the absence of SO_4^(2-)/ZrO_2.
文摘Sulfated zirconia-lanthana （SO4^2-/ZrO2-La2O3） precursors were prepared by ultrasonic coprecipitation method and followed by aging at different temperature. The precursors were treated by 0.5 mol/L H2SO4. Samples of SO4^2-/ZrO2-La2O3 nano-crystalline catalysts were obtained by baking the treated precursors at different temperatures. The acidic properties of SO4^2-/ZrO2-La2O3 were tested by the Hammett indicator method. The phase composition, specific area, particle structure, and surface state were characterized by X-ray diffraction, BET, transmission electron microscopy, infrared spectrum, and X-ray photoelectron spec- troscopy. The catalytic activities were estimated by esterification of acetic acid with glycerin. It was shown that the catalyst prepared by ultrasonic stirring and low temperature （-15 ℃） exhibited highly active sites and high catalytic property.
文摘Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.
基金supported by the Science and Technique Foundation of Shaaxi Province of China (2008K07-32)the Foundation of Shaanxi Educa- tional Committee of China (08JK228)the Graduate Innovation Fund of Shaanxi University of Science and Technology
文摘A novel solid superacid catalyst S2O8^2-/ZrO2-CeO2 was prepared by a coprecipitation method and characterized by means of XRD FTIR, BET, TEM and DSC/TG analysis methods. The results indicated that incorporation of appropriate amounts of Ce into the catalyst was beneficial to the formation of sole tetragonal ZrO2 and effectively prevented from the formation of monoclinic ZrO〉 and restrained the loss of sulfated species. XRD revealed the presence of tetragonal Ce0.16Zr0.84O2phase in the case of S2O8^2-/ZrO2-CeO2 calcined above 500 ℃. Catalytic activities of S2O8^2-/ZrO2-CeO2 for the esterification of lactic acid with n-butanol was studied. The results showed that the optimum conditions were as follows： calcination temperature of the catalyst 600 ℃, n（lactic acid）：n（n-butyl alcohol）=1.0：3.0, w（S2O8^2-/ZrO2- CeO2）=12.0%, reaction temperature 145 ℃, and reaction time 2 h. The esterification efficiency of lactic acid was about 96.6%.
文摘SO4^2-/TiO2-MoO3, a novel solid superacid, has been prepared and its catalytic activity at different synthetic conditions was examined with esterification of n-butanoic acid and n-butyl alcohol as probing reaction.The optimum conditions were also found, that is, the mass ratio of MoO3 used in the compound is 25%, the calcination temperature 450℃, and the soaked consistency of H2SO4 is 0.5mol.L^-1. Then it was applied in the catalytic synthesis of six similar important ketals and acetals as catalyst and revealed high catalytic activity. Under the condition that the molar ratio of aldehyde/ketone to glycol was 1:1.5, the mass ratio of the catalyst to the reactants was 0.5% and the reaction time 1.0 h, the yield of ketals and acetals reached up to 63.2%. The catalyst can be easily recovered and reused.
基金Project supported by the National Natural Science Foundation of China (No. 20471044), and the Natural Science Foundation of Hubei Province (No. 2005ABA053), China
文摘SO4^2- / TiO2-La2O3, a novel solid superacid, was prepared and its catalytic activities at different synthetic conditions are discussed with esterification of n-butanoic acid and n-butyl alcohol as probing reaction. The optimum conditions have also been found, mole ratio of n（La^3＋）：n（Ti^4＋） is 1：34, the soaked consistency of H2SO4 is 0.8 tool/L, the soaked time of HESO4 is 24 h, the calcining temperature is 480 ℃, the calcining time is 3 h. Then it was applied in the catalytic synthesis often important ketals and acetals as catalyst and revealed high catalytic activity. Under these conditions on which the molar ratio of aldehyde/ketone to glycol is l： 1.5, the mass ratio of the catalyst used in the reactants is 0.5%, and the reaction time is 1.0 h, the yields of ketals and acetals can reach 41.4%-95.8%.
基金supported by the research foundation of Hebei University of Science and Technology
文摘An efficient synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one is achieved via a reaction of acenaphthe-nequinone and indoles catalyzed by solid superacid SO4^2-/TiO2 under solvent-free conditions at room temperature by grinding, which provides an efficient route to the synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one.This procedure offers several advantages including solvent-free conditions,excellent yields of products,simple work-up as well as reuse of catalysts which makes it a useful and attractive protocol for the synthesis of these compounds.
