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
LuFeO3 crystallites of different sizes and morphologies were synthesized via a hydrothermal route. The sonocatalytic properties of the as-synthesized samples were investigated by degrading various organic dyes, includ...LuFeO3 crystallites of different sizes and morphologies were synthesized via a hydrothermal route. The sonocatalytic properties of the as-synthesized samples were investigated by degrading various organic dyes, including acid orange 7 （AOT）, rhodamine B （RhB）, methyl orange （MO）, and methylene blue （MB）, under ultrasonic irradiation, revealing that they exhibit excellent sonocatalytic activity toward the degradation of these dyes. Particularly, the synthesized bar-like particles with lengths of-3 μm and widths of-1μm have the highest sonocatalytic activity, and the degradation percentage of AO7 reaches 89% after 30 min of sonocatalysis. The effects of inorganic anions such as CI-, NO3-, SO42-, PO43-, and HCO3- on the sonocatalysis efficiency were investigated. Hydroxyl radicals （·OH） detected by fiuorimetry using terephthalic acid as a probe molecule were found to be produced over the ultrasonic-irradiated LuFeO3 particles. The addition of ethanol, which acts as a· OH scavenger, leads to quenching of ＂OH radicals and a simultaneous decrease in the dye degrada- tion. This suggests that ＂OH is the dominant active species responsible for the dye degradation.展开更多
This paper reports a new strategy for the structural reconstruction of biomass carbon sulfonic acid(BCSA)to its solid superacid counterpart.In this approach,a cheap layered biomass carbon(BC)source is chemically exfol...This paper reports a new strategy for the structural reconstruction of biomass carbon sulfonic acid(BCSA)to its solid superacid counterpart.In this approach,a cheap layered biomass carbon(BC)source is chemically exfoliated by cetyltrimethyl ammonium bromide and then converted to silica-isolated carbon nanosheets(CNSs)by a series of conversion steps.The state of the silica-isolated CNSs and the stacking density of their nanoparticles are regulated by the dehydration temperature.Only the highly isolated and non-crosslinked CNSs with loose particle stacking structures obtained upon dehydration at 250℃ can be turned into superacid sites(with stronger acidity than that of 100%H2 SO4)after sulfonation.This is accompanied by the creation of abundant hierarchical slit pores with high external surface area,mainly driven by the strong hydrogen bonding interactions between the introduced sulfonic acid groups.In typical acid-catalyzed esterification,etherification,and hydrolysis reactions,the newly formed superacid exhibits superior catalytic activity and stability compared to those of common BCSA and commercial Amberlyst-15 catalysts,owing to its good structural stability,highly exposed stable superacidic sites,and abundance of mesoporous/macroporous channels with excellent mass transfer rate.This groundbreaking work not only provides a novel strategy for fabricating bio-based solid superacids,but also overcomes the drawbacks of BCSA,i.e.,unsatisfactory structural stability,acidity,and porosity.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
A solid superacid was prepared as a catalyst. The catalyst was characterized by ammonia temperature- programmed desorption, surface property measurement, and analyses with scanning electron micros- copy and Fourier tr...A solid superacid was prepared as a catalyst. The catalyst was characterized by ammonia temperature- programmed desorption, surface property measurement, and analyses with scanning electron micros- copy and Fourier transform infrared spectrometry. A extraction residue from Lingwu subbituminous coal was subject to non-catalytic and catalytic hydroconversion using cyclohexane as the solvent under pres- surized hydrogen at 300 ℃ for 3 h. The results show that the total yield of petroleum ether-extractable arenes from catalytic hydroconversion is much higher than that from non-catalytic hydroconversion. The cleavage of Car-Cask bonds in the residue could significantly proceed during catalytic hvdrncnnvarsion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supported by the National Natural Science Foundation of China(51262018)the Fundamental Research Funds for Universities of Gansu Province(056003)the Hongliu Outstanding Talents Foundation of Lanzhou University of Technology(J201205)~~
文摘LuFeO3 crystallites of different sizes and morphologies were synthesized via a hydrothermal route. The sonocatalytic properties of the as-synthesized samples were investigated by degrading various organic dyes, including acid orange 7 （AOT）, rhodamine B （RhB）, methyl orange （MO）, and methylene blue （MB）, under ultrasonic irradiation, revealing that they exhibit excellent sonocatalytic activity toward the degradation of these dyes. Particularly, the synthesized bar-like particles with lengths of-3 μm and widths of-1μm have the highest sonocatalytic activity, and the degradation percentage of AO7 reaches 89% after 30 min of sonocatalysis. The effects of inorganic anions such as CI-, NO3-, SO42-, PO43-, and HCO3- on the sonocatalysis efficiency were investigated. Hydroxyl radicals （·OH） detected by fiuorimetry using terephthalic acid as a probe molecule were found to be produced over the ultrasonic-irradiated LuFeO3 particles. The addition of ethanol, which acts as a· OH scavenger, leads to quenching of ＂OH radicals and a simultaneous decrease in the dye degrada- tion. This suggests that ＂OH is the dominant active species responsible for the dye degradation.
基金financial support for this work by the National Natural Science Foundation of China(21690080,21676079,21546010,21690083,21878288)the Strategic Priority Research Program of Chinese Academy of Sciences(XDB17020100)+2 种基金DNL Cooperation Fund CAS(DNL180302)the Natural Science Foundation of Hunan Province(2018JJ3335)the Innovation Platform Open Fund of Hunan College(18K016)~~
文摘This paper reports a new strategy for the structural reconstruction of biomass carbon sulfonic acid(BCSA)to its solid superacid counterpart.In this approach,a cheap layered biomass carbon(BC)source is chemically exfoliated by cetyltrimethyl ammonium bromide and then converted to silica-isolated carbon nanosheets(CNSs)by a series of conversion steps.The state of the silica-isolated CNSs and the stacking density of their nanoparticles are regulated by the dehydration temperature.Only the highly isolated and non-crosslinked CNSs with loose particle stacking structures obtained upon dehydration at 250℃ can be turned into superacid sites(with stronger acidity than that of 100%H2 SO4)after sulfonation.This is accompanied by the creation of abundant hierarchical slit pores with high external surface area,mainly driven by the strong hydrogen bonding interactions between the introduced sulfonic acid groups.In typical acid-catalyzed esterification,etherification,and hydrolysis reactions,the newly formed superacid exhibits superior catalytic activity and stability compared to those of common BCSA and commercial Amberlyst-15 catalysts,owing to its good structural stability,highly exposed stable superacidic sites,and abundance of mesoporous/macroporous channels with excellent mass transfer rate.This groundbreaking work not only provides a novel strategy for fabricating bio-based solid superacids,but also overcomes the drawbacks of BCSA,i.e.,unsatisfactory structural stability,acidity,and porosity.
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.
基金subsidized by the Special Fund for Major State Basic Research Project (No. 2011CB201302)the Fund from the National Natural Science Foundation of China for Innovative Research Group (No. 50921002)+4 种基金the Key Project of Natural Science Foundation of China (No. 20936007)the Key Project of Coal Joint Fund from National Natural Science Foundation of China and Shenhua Group Corporation Limited (No. 51134021)National Natural Science Foundation of China (No. 51074153)the Program of the Universities in Jiangsu Province for Development of High-Tech Industries (No. JHB05-33)the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘A solid superacid was prepared as a catalyst. The catalyst was characterized by ammonia temperature- programmed desorption, surface property measurement, and analyses with scanning electron micros- copy and Fourier transform infrared spectrometry. A extraction residue from Lingwu subbituminous coal was subject to non-catalytic and catalytic hydroconversion using cyclohexane as the solvent under pres- surized hydrogen at 300 ℃ for 3 h. The results show that the total yield of petroleum ether-extractable arenes from catalytic hydroconversion is much higher than that from non-catalytic hydroconversion. The cleavage of Car-Cask bonds in the residue could significantly proceed during catalytic hvdrncnnvarsion
