In solid basic catalysis field,how to achieve optimized activity and desired stability through elaborate control over basic site properties remains a challenge.In this work,taking advantage of the structure memory eff...In solid basic catalysis field,how to achieve optimized activity and desired stability through elaborate control over basic site properties remains a challenge.In this work,taking advantage of the structure memory effect of layered double hydroxides(LDHs),rehydrated Ca4 Al1-x Gax-LDHs and Ca4 Al1-x Inx-LDHs catalysts were prepared and applied in aldol condensation reaction that isobutyraldehyde(IBD)reacts with formaldehyde(FA)to obtain hydroxypivalaldehyde(HPA).Notably,the resulting re-Ca4 Al0.90Ga0.10-LDHs exhibits an extraordinarily-high catalytic activity(HPA yield:72%),which is to our best knowledge the highest level in this reaction.The weak Br?nsted basic site,7-coordinated Ca-OH group,which serves as an active site,catalyzes the condensation process and promotes the product desorption.Studies on structure-property correlations demonstrate that Ga as a structural promoter induces a moderate expansion of the laminate lattice,which results in a significant increase in the concentration of weak basic sites in re-Ca4Al0.90Ga0.10-LDHs,accounting for its high catalytic activity.This work illuminates that geometric structure of basic active sites can be tuned via introducing catalyst additive,which leads to a largely improved performance of hydrotalcite solid basic catalysts towards aldol condensation reaction.展开更多
A basic ionic liquid, namely 1,1'-(butane-1,4-diyl)bis(1,4-diazabicyclo [2.2.2]octan-1-ium) hydrox-ide, was prepared and characterized using Fourier-transform infrared spectroscopy, XH nuclear magnetic...A basic ionic liquid, namely 1,1'-(butane-1,4-diyl)bis(1,4-diazabicyclo [2.2.2]octan-1-ium) hydrox-ide, was prepared and characterized using Fourier-transform infrared spectroscopy, XH nuclear magnetic resonance spectroscopy, and pH measurements. The ionic liquid was used for efficient promotion of the synthesis of pyrano[2,3-d]pyrimidinone and pyrido[2,3-d]pyrimidine derivatives at room temperature under grinding conditions. A simple procedure, short reaction time, high yields, non-column chromatographic separation, commercial availability of the starting materials, and recyclability of the catalyst are attractive features of this process.展开更多
A new method for the fabrication of carbon aerogels is reported in this paper. Resorcinol and furfural were gelated in isopropanol with basic catalysts and then dried directly under isopropanol supercritical condition...A new method for the fabrication of carbon aerogels is reported in this paper. Resorcinol and furfural were gelated in isopropanol with basic catalysts and then dried directly under isopropanol supercritical condition, followed by carbonization under nitrogen atmosphere. The bulk densities of carbon aerogels obtained are in the range of 0.21g/cm3~0.27g/cm3 and the sizes of the interconnected carbon nano-particles are in the range of 20nm^30nm. All of the aerogel samples exhibit high BET surface areas in the range of 730m2/g^900m2/g. The bulk density, micro-pore volume, meso-pore volume and meso-pore diameter can be controlled by gelation conditions such as R/I ratio and R/C ratio.展开更多
The Co3O4 and Zr-,Ce-,and La-Co3O4 catalysts were prepared,characterized,and applied to produce CH4 from CO2 catalytic hydrogenation in low temperature as 140–220℃.The results indicated that the addition of Zr,Ce,or...The Co3O4 and Zr-,Ce-,and La-Co3O4 catalysts were prepared,characterized,and applied to produce CH4 from CO2 catalytic hydrogenation in low temperature as 140–220℃.The results indicated that the addition of Zr,Ce,or La to the Co3O4 decreased the crystallite sizes of Co and the outer-shell electron density of Co^3+,and increased the specific surface area,which would provide more active sites for the CO2 methanation.Especially,the addition of Zr also changed the reducing state of Co3O4 via an obvious change in the interaction between Co3O4 and ZrO2.Furthermore,Zr doped into the Co3O4 increased the basic intensity of the weak and medium basic sites,as well as the amount of Lewis acid sites,and Bronsted acid sites were also found on the Zr-Co3O4 surface.The introduction of Zr,Ce,or La favored the production of CH4,and the Zr-Co3O4catalyst exhibited the highest CO2 conversion(58.2%)and CH4 selectivity(100%)at 200℃,and 0.5 MPa with a gaseous hourly space velocity of 18,000 ml·g^-1(cat)·h^-1,and the catalytic activity of CO2methanation for the Zr-,Ce-,and La-Co3O4 exhibited more stable than Co3O4 in a 20-h reaction.展开更多
Red mud was investigated in triglyceride transesterification with a view to determine its viability as a basic catalyst for use in biodiesel synthesis. The effect of calcination temperature on the structure and activi...Red mud was investigated in triglyceride transesterification with a view to determine its viability as a basic catalyst for use in biodiesel synthesis. The effect of calcination temperature on the structure and activity of red mud catalysts was investigated. It was found that highly active catalyst was obtained by simply drying red mud at 200℃. Utilization of red mud as a catalyst for biodiesel production not only provides a cost-effective and environmentally friendly way of recycling this solid red mud waste, significantly reducing its environmental effects, but also reduces the price of biodiesel to make biodiesel competitive with petroleum diesel.展开更多
Renewable biofuels have gained increasing attention as a potential alternative fuel to decrease CO_(2) emission from combustion of fossil fuels.The aims of the work were to modify Thai dolomite by adding magnesium car...Renewable biofuels have gained increasing attention as a potential alternative fuel to decrease CO_(2) emission from combustion of fossil fuels.The aims of the work were to modify Thai dolomite by adding magnesium carbonate(MgCO_(3))at various contents(0-30 wt%),and used as catalyst in pyrolytic catalysis cracking(PCC)process to produce light biofuels including gasoline and kerosene.All catalysts were calcined at 600℃ for 4 h prior to the characterization and experiments.The physicochemical properties were done by various techniques such as X-ray diffractometer(XRD),N2 adsorption-desorption,thermogravimetric analyzer and differential thermal analyzer(TGA-DTA),Field-emission scanning electron microscope(FE-SEM),and energy dispersive X-ray spectroscopy(EDX).The experiments of PCC process were carried out at different reaction temperatures of 450-550℃.The results from XRD and SEM-EDX confirmed that the Mg was successfully added in Thai dolomite.The Mg content in the catalysts increased with increasing MgCO_(3) loadings.The calcination temperature of 600℃ cannot completely convert CaCO3 to CaO form.The pyrolytic oil and distilled oil yields and quality were affected by both Mg content and reaction temperature.In addition,pyrolytic oil was completely distillated according to ASTM D86 to separate into gasoline,kerosene,and diesel.The light biofuel production was enhanced with increasing Mg content in the reaction temperatures of 500 and 550℃.The appropriate condition was suggested at reaction temperature of 500℃ with 20 wt%Mg/dolomite catalyst as it showed the highest production yield of about 84 vol%and light biofuel yield of about 65 vol%.展开更多
文摘In solid basic catalysis field,how to achieve optimized activity and desired stability through elaborate control over basic site properties remains a challenge.In this work,taking advantage of the structure memory effect of layered double hydroxides(LDHs),rehydrated Ca4 Al1-x Gax-LDHs and Ca4 Al1-x Inx-LDHs catalysts were prepared and applied in aldol condensation reaction that isobutyraldehyde(IBD)reacts with formaldehyde(FA)to obtain hydroxypivalaldehyde(HPA).Notably,the resulting re-Ca4 Al0.90Ga0.10-LDHs exhibits an extraordinarily-high catalytic activity(HPA yield:72%),which is to our best knowledge the highest level in this reaction.The weak Br?nsted basic site,7-coordinated Ca-OH group,which serves as an active site,catalyzes the condensation process and promotes the product desorption.Studies on structure-property correlations demonstrate that Ga as a structural promoter induces a moderate expansion of the laminate lattice,which results in a significant increase in the concentration of weak basic sites in re-Ca4Al0.90Ga0.10-LDHs,accounting for its high catalytic activity.This work illuminates that geometric structure of basic active sites can be tuned via introducing catalyst additive,which leads to a largely improved performance of hydrotalcite solid basic catalysts towards aldol condensation reaction.
基金the University of Guilan Research Council for the partial support of this work
文摘A basic ionic liquid, namely 1,1'-(butane-1,4-diyl)bis(1,4-diazabicyclo [2.2.2]octan-1-ium) hydrox-ide, was prepared and characterized using Fourier-transform infrared spectroscopy, XH nuclear magnetic resonance spectroscopy, and pH measurements. The ionic liquid was used for efficient promotion of the synthesis of pyrano[2,3-d]pyrimidinone and pyrido[2,3-d]pyrimidine derivatives at room temperature under grinding conditions. A simple procedure, short reaction time, high yields, non-column chromatographic separation, commercial availability of the starting materials, and recyclability of the catalyst are attractive features of this process.
基金The National Natural Science Foundation of China (No. 59973028), The Team Project of the Natural Science Foundation of Guangdong (No.[( )(20003038)]), and The Talent Training Program Foundation of the Higher Education Departmen
文摘A new method for the fabrication of carbon aerogels is reported in this paper. Resorcinol and furfural were gelated in isopropanol with basic catalysts and then dried directly under isopropanol supercritical condition, followed by carbonization under nitrogen atmosphere. The bulk densities of carbon aerogels obtained are in the range of 0.21g/cm3~0.27g/cm3 and the sizes of the interconnected carbon nano-particles are in the range of 20nm^30nm. All of the aerogel samples exhibit high BET surface areas in the range of 730m2/g^900m2/g. The bulk density, micro-pore volume, meso-pore volume and meso-pore diameter can be controlled by gelation conditions such as R/I ratio and R/C ratio.
基金Supported by the National Natural Science Foundation of China(21366004)Guangxi Natural Science Foundation(2016GXNSFFA380015)the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2016Z003)
文摘The Co3O4 and Zr-,Ce-,and La-Co3O4 catalysts were prepared,characterized,and applied to produce CH4 from CO2 catalytic hydrogenation in low temperature as 140–220℃.The results indicated that the addition of Zr,Ce,or La to the Co3O4 decreased the crystallite sizes of Co and the outer-shell electron density of Co^3+,and increased the specific surface area,which would provide more active sites for the CO2 methanation.Especially,the addition of Zr also changed the reducing state of Co3O4 via an obvious change in the interaction between Co3O4 and ZrO2.Furthermore,Zr doped into the Co3O4 increased the basic intensity of the weak and medium basic sites,as well as the amount of Lewis acid sites,and Bronsted acid sites were also found on the Zr-Co3O4 surface.The introduction of Zr,Ce,or La favored the production of CH4,and the Zr-Co3O4catalyst exhibited the highest CO2 conversion(58.2%)and CH4 selectivity(100%)at 200℃,and 0.5 MPa with a gaseous hourly space velocity of 18,000 ml·g^-1(cat)·h^-1,and the catalytic activity of CO2methanation for the Zr-,Ce-,and La-Co3O4 exhibited more stable than Co3O4 in a 20-h reaction.
基金supported by the Natural Science Basic Research Plan in Shaanxi Province of China (No.2010JM2003)the Fundamental Research Funds for the Central Universities (No. GK200902006)
文摘Red mud was investigated in triglyceride transesterification with a view to determine its viability as a basic catalyst for use in biodiesel synthesis. The effect of calcination temperature on the structure and activity of red mud catalysts was investigated. It was found that highly active catalyst was obtained by simply drying red mud at 200℃. Utilization of red mud as a catalyst for biodiesel production not only provides a cost-effective and environmentally friendly way of recycling this solid red mud waste, significantly reducing its environmental effects, but also reduces the price of biodiesel to make biodiesel competitive with petroleum diesel.
基金This work received a scholarship from the Thailand Research Fund(TRF)through the Royal Golden Jubilee Ph.D.(RGJ)program(Grant No.PHD/0150/2561).
文摘Renewable biofuels have gained increasing attention as a potential alternative fuel to decrease CO_(2) emission from combustion of fossil fuels.The aims of the work were to modify Thai dolomite by adding magnesium carbonate(MgCO_(3))at various contents(0-30 wt%),and used as catalyst in pyrolytic catalysis cracking(PCC)process to produce light biofuels including gasoline and kerosene.All catalysts were calcined at 600℃ for 4 h prior to the characterization and experiments.The physicochemical properties were done by various techniques such as X-ray diffractometer(XRD),N2 adsorption-desorption,thermogravimetric analyzer and differential thermal analyzer(TGA-DTA),Field-emission scanning electron microscope(FE-SEM),and energy dispersive X-ray spectroscopy(EDX).The experiments of PCC process were carried out at different reaction temperatures of 450-550℃.The results from XRD and SEM-EDX confirmed that the Mg was successfully added in Thai dolomite.The Mg content in the catalysts increased with increasing MgCO_(3) loadings.The calcination temperature of 600℃ cannot completely convert CaCO3 to CaO form.The pyrolytic oil and distilled oil yields and quality were affected by both Mg content and reaction temperature.In addition,pyrolytic oil was completely distillated according to ASTM D86 to separate into gasoline,kerosene,and diesel.The light biofuel production was enhanced with increasing Mg content in the reaction temperatures of 500 and 550℃.The appropriate condition was suggested at reaction temperature of 500℃ with 20 wt%Mg/dolomite catalyst as it showed the highest production yield of about 84 vol%and light biofuel yield of about 65 vol%.