The crystallization behavior and kinetics of CaO-MgO-Al2O3 SiO2(CMAS) glass with the Fe2O3 content ranging from zero to 5%were investigated by differential scanning calorimetry(DSC).The structure and phase analyse...The crystallization behavior and kinetics of CaO-MgO-Al2O3 SiO2(CMAS) glass with the Fe2O3 content ranging from zero to 5%were investigated by differential scanning calorimetry(DSC).The structure and phase analyses were made by Fourier transform infrared spectroscopy(FT-IR) and X-ray diffraction(XRD).The experiment results show that the endothermic peak temperature about 760℃ is associated with transition and the exothermic peak temperature about 1000℃ is associated with crystallization.The crystallization peak temperature decreases with increasing the Fe203 content.The crystallization mechanism is changed from two-dimensional crystallization to one-dimensional growth,and the intensity of diopside peaks becomes stronger gradually.There is a saltation for the crystallization temperature with the addition of 0.5%Fe2O3 due to the decomposition of Fe2O3.Si-O-Si,O-Si-O and T-O-T(T=Si,Fe,Al) linkages are observed in Fe2O3-CaO-MgO-Al2O3-SiO2 glass.展开更多
The incorporation of ZnO into Fe2O3-K2O system increases its activity, enhances its moisture stability and mechanical strength. The origin of the enhancement in activity and moisture stability is discussed in the lig...The incorporation of ZnO into Fe2O3-K2O system increases its activity, enhances its moisture stability and mechanical strength. The origin of the enhancement in activity and moisture stability is discussed in the light of experimental results obtained by BET, XRD, XPS. It was found that the addition of ZnO to Fe2O3-K2O system strengthens the interaction between Fe2O3 and K2O, reduces the formation temperature of KFe11O17 at least by 50 oC, and promotes the transformation of Fe3+ to Fe2+ further.展开更多
separation is an attractive alternative to filtration or centrifugation for separating solid catalysts from a liquid phase, Here, core-shell Fe3O4@UiO-66-NH2 nanohybrids with well-defined structures were constructed b...separation is an attractive alternative to filtration or centrifugation for separating solid catalysts from a liquid phase, Here, core-shell Fe3O4@UiO-66-NH2 nanohybrids with well-defined structures were constructed by dispersing magnets in a dimethylformamide (DMF) solution con- taining two metal-organic framework (MOF) precursors, namely ZrCI4 and 2-aminobenzenetricar- boxylic acid. This method is simpler and more efficient than previously reported step-by-step method in which magnets were consecutively dispersed in DMF solutions each containing one MOF precursor, and the obtained Fe304@UiO-66-NH2 with three assembly cycles has a higher degree of crystallinity and porosiW. The core-shell Fe3O4@UiO-66-NH2 is highly active and selective in Knoevenagel condensations because of the bifunctionality of UiO-66-NH2 and better mass transfer in the nano-sized shells. It also has good recycling stability, and can be recovered magnetically and reused at least four times without significant loss of catalytic activity and framework integrity. The effects of substitution on the reactivity of benzaldehyde and of substrate size were also investigated.展开更多
The development of efficient systems for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene(NMST)to 2-nitro-4-methylsulfonyl benzoic acid(NMSBA)with atmospheric air or molecular oxygen in alkaline medium prese...The development of efficient systems for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene(NMST)to 2-nitro-4-methylsulfonyl benzoic acid(NMSBA)with atmospheric air or molecular oxygen in alkaline medium presents a significant challenge for the chemical industry.Here,we report the synthesis of FeOOH/Fe_(3)O_(4)/metal-organic framework(MOF)polygonal mesopores microflower templated from a MIL-88B(Fe)at room temperature,which exposes polygonal mesopores with atomistic edge steps and lattice defects.The obtained FeOOH/Fe_(3)O_(4)/MOF catalyst was adsorbed onto glass beads and then introduced into the microchannel reactor.In the alkaline environment,oxygen was used as oxidant to catalyze the oxidation of NMST to NMSBA,showing impressive performance.This sustainable system utilizes oxygen as a clean oxidant in an inexpensive and environmentally friendly NaOH/methanol mixture.The position and type of substituent critically affect the products.Additionally,this sustainable protocol enabled gram-scale preparation of carboxylic acid and benzyl alcohol derivatives with high chemoselectivities.Finally,the reactions can be conducted in a pressure reactor,which can conserve oxygen and prevent solvent loss.Moreover,compared with the traditional batch reactor,the self-built microchannel reactor can accelerate the reaction rate,shorten the reaction time,and enhance the selectivity of catalytic oxidation reactions.This approach contributes to environmental protection and holds potential for industrial applications.展开更多
In this work, a series of coal-based active carbon (CAC) catalysts loaded by A1203 were prepared by sol-gel method and used for the simulta- neous catalytic hydrolysis of carbonyl sulfide (COS) and carbon disulfi...In this work, a series of coal-based active carbon (CAC) catalysts loaded by A1203 were prepared by sol-gel method and used for the simulta- neous catalytic hydrolysis of carbonyl sulfide (COS) and carbon disulfide (CS2) at relatively low temperatures of 30-70 ℃. The influences of calcinations temperatures and operation conditions such as: reaction temperature, 02 concentration, gas hourly space velocity (GHSV) and relative humidity (RH) were also discussed respectively. The results showed that catalysts with 5.0 wt% A1203 calcined at 300 ℃ had supe- rior activity for the simultaneous catalytic hydrolysis of COS and CS2. When the reaction temperature was above 50 ℃, catalytic hydrolysis activity of COS could be enhanced but that of CS2 was inhibited. Too high RH could make the catalytic hydrolysis activities of COS and CS2 decrease. A small amount of 02 introduction could enhance the simultaneous catalytic hydrolysis activities of COS and CS2.展开更多
基金Projects(51264023,51364020,U1202271)supported by the National Natural Science Foundation of ChinaProject(IRT1250)supported by the Program for Innovative Research Team in University of Ministry of Education of ChinaProject(2014HA003)supported by the Science and Technology Leading Talent of Yunnan Province,China
文摘The crystallization behavior and kinetics of CaO-MgO-Al2O3 SiO2(CMAS) glass with the Fe2O3 content ranging from zero to 5%were investigated by differential scanning calorimetry(DSC).The structure and phase analyses were made by Fourier transform infrared spectroscopy(FT-IR) and X-ray diffraction(XRD).The experiment results show that the endothermic peak temperature about 760℃ is associated with transition and the exothermic peak temperature about 1000℃ is associated with crystallization.The crystallization peak temperature decreases with increasing the Fe203 content.The crystallization mechanism is changed from two-dimensional crystallization to one-dimensional growth,and the intensity of diopside peaks becomes stronger gradually.There is a saltation for the crystallization temperature with the addition of 0.5%Fe2O3 due to the decomposition of Fe2O3.Si-O-Si,O-Si-O and T-O-T(T=Si,Fe,Al) linkages are observed in Fe2O3-CaO-MgO-Al2O3-SiO2 glass.
文摘The incorporation of ZnO into Fe2O3-K2O system increases its activity, enhances its moisture stability and mechanical strength. The origin of the enhancement in activity and moisture stability is discussed in the light of experimental results obtained by BET, XRD, XPS. It was found that the addition of ZnO to Fe2O3-K2O system strengthens the interaction between Fe2O3 and K2O, reduces the formation temperature of KFe11O17 at least by 50 oC, and promotes the transformation of Fe3+ to Fe2+ further.
基金supported by the National Natural Science Foundation of China (21203017)Open Fund of State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences (N-11-3)+1 种基金Program for Liaoning Excellent Talents in University (LNET)the Funda-mental Research Funds for the Central Universities (DC201502020304)~~
文摘separation is an attractive alternative to filtration or centrifugation for separating solid catalysts from a liquid phase, Here, core-shell Fe3O4@UiO-66-NH2 nanohybrids with well-defined structures were constructed by dispersing magnets in a dimethylformamide (DMF) solution con- taining two metal-organic framework (MOF) precursors, namely ZrCI4 and 2-aminobenzenetricar- boxylic acid. This method is simpler and more efficient than previously reported step-by-step method in which magnets were consecutively dispersed in DMF solutions each containing one MOF precursor, and the obtained Fe304@UiO-66-NH2 with three assembly cycles has a higher degree of crystallinity and porosiW. The core-shell Fe3O4@UiO-66-NH2 is highly active and selective in Knoevenagel condensations because of the bifunctionality of UiO-66-NH2 and better mass transfer in the nano-sized shells. It also has good recycling stability, and can be recovered magnetically and reused at least four times without significant loss of catalytic activity and framework integrity. The effects of substitution on the reactivity of benzaldehyde and of substrate size were also investigated.
基金supported by the National Natural Science Foundation of China(22078251)Hubei Province Key Research and Development Program(2023DJC167)the research project of Hubei Provincial Department of Education(D20191504).
文摘The development of efficient systems for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene(NMST)to 2-nitro-4-methylsulfonyl benzoic acid(NMSBA)with atmospheric air or molecular oxygen in alkaline medium presents a significant challenge for the chemical industry.Here,we report the synthesis of FeOOH/Fe_(3)O_(4)/metal-organic framework(MOF)polygonal mesopores microflower templated from a MIL-88B(Fe)at room temperature,which exposes polygonal mesopores with atomistic edge steps and lattice defects.The obtained FeOOH/Fe_(3)O_(4)/MOF catalyst was adsorbed onto glass beads and then introduced into the microchannel reactor.In the alkaline environment,oxygen was used as oxidant to catalyze the oxidation of NMST to NMSBA,showing impressive performance.This sustainable system utilizes oxygen as a clean oxidant in an inexpensive and environmentally friendly NaOH/methanol mixture.The position and type of substituent critically affect the products.Additionally,this sustainable protocol enabled gram-scale preparation of carboxylic acid and benzyl alcohol derivatives with high chemoselectivities.Finally,the reactions can be conducted in a pressure reactor,which can conserve oxygen and prevent solvent loss.Moreover,compared with the traditional batch reactor,the self-built microchannel reactor can accelerate the reaction rate,shorten the reaction time,and enhance the selectivity of catalytic oxidation reactions.This approach contributes to environmental protection and holds potential for industrial applications.
基金The Opening Project of Shanghai Key Laboratory of Special Artificial Microstructure Materials and Technology(ammt2011A-4)The Innovation Fund Project for Graduate Student of Shanghai(JWCXSL1102)
基金supported by the Ministry of Environmental Protection,Public Welfare Project(Contract No 201109034)the National Natural Science Foundation(U1137603)
文摘In this work, a series of coal-based active carbon (CAC) catalysts loaded by A1203 were prepared by sol-gel method and used for the simulta- neous catalytic hydrolysis of carbonyl sulfide (COS) and carbon disulfide (CS2) at relatively low temperatures of 30-70 ℃. The influences of calcinations temperatures and operation conditions such as: reaction temperature, 02 concentration, gas hourly space velocity (GHSV) and relative humidity (RH) were also discussed respectively. The results showed that catalysts with 5.0 wt% A1203 calcined at 300 ℃ had supe- rior activity for the simultaneous catalytic hydrolysis of COS and CS2. When the reaction temperature was above 50 ℃, catalytic hydrolysis activity of COS could be enhanced but that of CS2 was inhibited. Too high RH could make the catalytic hydrolysis activities of COS and CS2 decrease. A small amount of 02 introduction could enhance the simultaneous catalytic hydrolysis activities of COS and CS2.