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
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
通过水热改性氢氧化锆制备了SO42-/ZrO2固体酸催化剂。以冰乙酸和正丁醇的酯化反应为探针反应,确定了固体超强酸的最佳制备条件。分别考察了浸渍硫酸浓度、硫酸浸渍时间和焙烧温度等对催化活性的影响。并以水热改性和未经水热改性氢氧...通过水热改性氢氧化锆制备了SO42-/ZrO2固体酸催化剂。以冰乙酸和正丁醇的酯化反应为探针反应,确定了固体超强酸的最佳制备条件。分别考察了浸渍硫酸浓度、硫酸浸渍时间和焙烧温度等对催化活性的影响。并以水热改性和未经水热改性氢氧化锆制备SO42-/ZrO2固体超强酸做了对比实验,采用XRD、BET对催化剂进行了表征。实验结果表明:水热改性氢氧化锆制备SO42-/ZrO2固体酸催化剂的最佳条件是:浸渍硫酸浓度为0.5mol/L,浸渍时间是120 m in,焙烧温度500℃。乙酸正丁酯较佳的合成工艺条件是:反应温度105~110℃,反应时间2 h,n(正丁醇)∶n(冰乙酸)=2∶1,催化剂用量占反应投料总质量的0.27%,冰乙酸的酯化率达99.1%。催化剂重复使用4次后催化活性降低5%。展开更多
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.
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.
文摘通过水热改性氢氧化锆制备了SO42-/ZrO2固体酸催化剂。以冰乙酸和正丁醇的酯化反应为探针反应,确定了固体超强酸的最佳制备条件。分别考察了浸渍硫酸浓度、硫酸浸渍时间和焙烧温度等对催化活性的影响。并以水热改性和未经水热改性氢氧化锆制备SO42-/ZrO2固体超强酸做了对比实验,采用XRD、BET对催化剂进行了表征。实验结果表明:水热改性氢氧化锆制备SO42-/ZrO2固体酸催化剂的最佳条件是:浸渍硫酸浓度为0.5mol/L,浸渍时间是120 m in,焙烧温度500℃。乙酸正丁酯较佳的合成工艺条件是:反应温度105~110℃,反应时间2 h,n(正丁醇)∶n(冰乙酸)=2∶1,催化剂用量占反应投料总质量的0.27%,冰乙酸的酯化率达99.1%。催化剂重复使用4次后催化活性降低5%。
