采用直接水热合成和后合成两种方法制备Al-ITQ-13分子筛,用于催化甲醇转化制备烃类化合物。采用XRD、27Al M AS NM R、NH3-TPD、Py-FTIR和SEM等技术对所合成样品进行了表征。结果表明,两种方法制备的Al-ITQ-13结晶度都较高,且晶体形貌...采用直接水热合成和后合成两种方法制备Al-ITQ-13分子筛,用于催化甲醇转化制备烃类化合物。采用XRD、27Al M AS NM R、NH3-TPD、Py-FTIR和SEM等技术对所合成样品进行了表征。结果表明,两种方法制备的Al-ITQ-13结晶度都较高,且晶体形貌为薄片。与ZSM-5相比,Al-ITQ-13在甲醇转化反应中显示出较高的丙烯选择性、较高的丙烯/乙烯产物比以及较好的催化稳定性。同时,由于后合成所得到的Si Al(B)-ITQ-13强酸量减少,其催化性能优于直接合成的Si Ge Al-ITQ-13。展开更多
The nanoparticles of the hydrophobic drug of danazol with narrow size distribution are facilely prepared by controlled high-gravity anti-solvent precipitation (HGAP) process. Intensified micromixing and uniform nucl...The nanoparticles of the hydrophobic drug of danazol with narrow size distribution are facilely prepared by controlled high-gravity anti-solvent precipitation (HGAP) process. Intensified micromixing and uniform nucleation environment are created by the high-gravity equipment (rotating packed bed) in carrying out the anti-solvent precipitation process to produce nanoparticles. The average particle size decreases from 55 μm of the raw danazol to 190 nm of the nanoparticles. The Brunauer-Emmett-Teller (BET) surface area sharply increases from 0.66 m^2·g^-1 to 15.08 m^2·g^-l. Accordingly, the dissolution rate is greatly improved. The molecular state, chemical composition, and crystal form of the danazol nanoparticles remains unchanged after processing according to Fourier transform infrared (FTIR) and X-ray diffraction (XRD), The high recovery ratio and continuous production capacity are highly appreciated in industry. Therefore, the HGAP method might offer a general and facile platform for mass production of hydrophobic pharmaceutical danazol particles in nanometer range.展开更多
Production of 6-aminopenicillanic acid (6-APA) by hydrolysis using penicillin acylase (PA) was studied as a model of an enzymatic emulsion liquid membrane (ELM) process. The loss of PA activity was examined for variou...Production of 6-aminopenicillanic acid (6-APA) by hydrolysis using penicillin acylase (PA) was studied as a model of an enzymatic emulsion liquid membrane (ELM) process. The loss of PA activity was examined for various membrane compositions (organic solvent, surfactant, carrier). The effects of some experimental variables on the stability of emulsion were investigated. It was found that the choice of organic solvent greatly affected the stability of the emulsion. Increasing the concentration of the carrier in the membrane phase increases the transfer rate of substrate and products but also has a destabilizing effect on the emulsion. The recovery of 6-APA obtained by a di-carrier system (N263-N1923) was much higher than those when either of the di-carriers was used separately. The whole process was controlled both by the enzymatic reaction rate and by the transfer rate of the substrate and the products, however, the ratio of them could be changed by varying the composition of the system. For an optimum condition, it was obtained that the recovery ratio of 6-APA was over 80% and the conversion of benzyl penicillin (PG) was up to 90% in the external phase after 30 minutes. Meanwhile, the breakage percentage of the emulsion was less than 2%.展开更多
It is already well known that availability of petroleum oil, as a world energy source, is running low. Much work has been done by experts to produce renewable energy, especially using vegetable oil as a raw material. ...It is already well known that availability of petroleum oil, as a world energy source, is running low. Much work has been done by experts to produce renewable energy, especially using vegetable oil as a raw material. Accordingly, this paper presents preparation and activity test of Cu catalyst using coconut shell activated carbon (AC) as a support, for conversion of n-pentanol and n-butanol to their alkenes as the first step of conversion of ethanol to biogasoline. This conversion is interesting due to any agriculture product containing sugar or starch can be converted to ethanol. Activated carbon was used as a catalyst support because this material is inert; hence, it would not yield unexpected side product, and pollution of environment with the used catalyst can be prevented because the used catalytic metal can easily be recovered. Results of the work showed that coconut shell carbon contained some metals, which disturbed in preparation catalyst by cation exchange process. Washing the carbon with ammonium acetate or HCI solution could reduce the metals content more compared to using water, with optimum concentration for ammonium acetate solution was 1.25 M. Application of Cu/AC in converting n-pentanol and n-butanol, based on qualitative analysis to the products using GLC, GC-MS, and FTIR, when n-pentanol and nitrogen gas were flowed into a reactor filled with Cu/AC catalyst, it could be converted to n-pentene with 200 ℃ as the optimal temperature. While when n-butanol and nitrogen gas were flowed into a reactor filled with more Cu/AC catalyst, the product was supposed to contain its aldehyde and butyl vinyl ether.展开更多
This study reports preparation of glass composition (54.50 wt.%) SiO2, (10.80 wt.%) B2O3, (14.20 wt.%) Na2O, (1.20 wt.%) K2O, (6.00 wt.%) CaO, (4.00 wt.%) Fe2O3 and (9.30 wt.%) TiO2 by melt quenching met...This study reports preparation of glass composition (54.50 wt.%) SiO2, (10.80 wt.%) B2O3, (14.20 wt.%) Na2O, (1.20 wt.%) K2O, (6.00 wt.%) CaO, (4.00 wt.%) Fe2O3 and (9.30 wt.%) TiO2 by melt quenching method using direct microwave heating and conventional resistive heating. Study of dielectric loss factor of the glass as function of temperature illustrated increasing loss factor above 370 ℃, 550 ℃, 650 ℃ and 900 ℃, indicating enhanced microwave absorption by the glass at above these temperatures. Chemical analysis results of both the glasses depicted more volatilization loss of volatile ingredients in conventional heating. The study of chemical durability was performed from leachate analysis describing less leaching of Na2O, K2O and other constituents from glass melted in microwave furnace. Glass transition temperatures (Tg) were found to be 576.3 ℃ and 569.5 ℃ for glass melted in conventional and microwave heating route, respectively. Laboratory experiment of glass melting utilizing microwave energy as an alternate heating source demonstrated 70%-75% electrical power saving.展开更多
With oil-soluble molybdenum compound and sublimed sulfur serving as raw materials, two dispersed Mo-based catalysts were prepared, characterized and then applied to the hydrogenation conversion of phenanthrene. The te...With oil-soluble molybdenum compound and sublimed sulfur serving as raw materials, two dispersed Mo-based catalysts were prepared, characterized and then applied to the hydrogenation conversion of phenanthrene. The test results showed that under the conditions specified by this study, the catalyst prepared in a higher sulfiding atmosphere was more catalytically active due to its higher content of MoS2 and stronger intrinsic catalytic activity of MoS2 unit, which demonstrated that the sulfiding atmosphere for the preparation of catalysts not only could influence the yield of MoS2 but also the structure of MoS2.The analysis on the selectivity of octahydrophenanthrene isomers revealed that the catalyst prepared in a lower sulfiding atmosphere had a relatively higher catalytic selectivity to the hydrogenation of outer aromatic ring and the structure of catalysts could be modified under the specific reaction conditions. Moreover, the selectivity between the isomers of as-octahydrophenanthrene at different reaction time and temperature was analyzed and, based on the results, a hydrogenation mechanism over dispersed Mo-based catalysts was suggested, with monatomic hydrogen transfer and catalytic surface desorption of the half-addition intermediates functioning as the key points. In addition, it is concluded that the catalyst prepared in a lower sulfiding atmosphere was more capable of adsorption than the other one.展开更多
FeCrAI (Ce) stainless steel was functionalized by a conversion treatment in order to allow alumina by diffusion coatings with strong interfacial bonding. The very porous conversion coating produced in a pack alumini...FeCrAI (Ce) stainless steel was functionalized by a conversion treatment in order to allow alumina by diffusion coatings with strong interfacial bonding. The very porous conversion coating produced in a pack aluminization technique had excellent adhesion and was conductive enough to permit conditions favorable for the precipitation of alumina oxyhydroxide during aluminum diffusion coatings. In this work, the bed was prepared as a mixture of A1, NH4C1 and A1203. In the high-activity bed were heat-treated at 1,173 K in an atmosphere made up of team with subsequent air-cooling. The effect of the bed content on the coating was examined. With the high-activity, the desired Fe2Al5 was formed as the outermost coating layer. The coating presented chemical composition gradients suitable for strong adhesion. The improvement of the thermal oxidation behaviour was studied at 1,373 K. Two different aqueous environments, which are (1) NaC1 and (2) H2SO4, are employed for using the technique of potentiodynamic polarization curve. The obtained experimental electrochemical parameters (Ecorr, Jcorr etc,) were used to compare the corrosion resistance of the tested steel state complemented by MEB (electronic scanning microscopy) in combination with dispersive analysis X in energy (EDS) or X ray diffraction indicated that the elements concentration maximum was located in the vicinity of the interface especially in the FeCrAI (Ce) coated by spherical A1203 powder. These results an discussed in terms of an addition effect on the development of the microstructure of oxide films.展开更多
With concerns of diminishing fossil fuel reserves and environmental deterioration, great efforts have been made to explore novel approaches of efficiently utilizing bio-renewable feedstocks to produce chemicals and fu...With concerns of diminishing fossil fuel reserves and environmental deterioration, great efforts have been made to explore novel approaches of efficiently utilizing bio-renewable feedstocks to produce chemicals and fuels. 5-Hydroxymethylfurfural(HMF),generated from dehydration of six-carbon ketose, is regarded as a primary and versatile renewable building block to realize the goal of production of these high valued products from renewable biomass resources transformation. In this review, we summarize the recent advances via green routes in the heterogeneous reaction system for the catalytic production of HMF from glucose conversion, and emphasize reaction pathways of these reaction approaches based on the fundamental mechanistic chemistry as well as highlight the challenges(such as separation and purification of products, reusing and regeneration of catalyst, recycling solvent) in this field.展开更多
The power conversion efficiency of organometallic perovskite-based solar cells has skyrocketed in recent years. Intensive efforts have been made to prepare high-quality perovskite films tailored to various device conf...The power conversion efficiency of organometallic perovskite-based solar cells has skyrocketed in recent years. Intensive efforts have been made to prepare high-quality perovskite films tailored to various device configurations. Planar heterojunction devices have achieved record efficiencies; however, the preparation of perovskite films for planar junction devices requires the use of expensive vacuum facilities and/or the fine control of experimental conditions. Here, we demonstrate a facile preparation of perovskite films using solid-state chemistry. Solid-state precursor thin films of CHBNH3I and PbI2 are brought into contact with each other and allowed to react via thermally accelerated diffusion. The resulting perovskite film displays good optical absorption and a smooth morphology. Solar cells based on these films show an average efficiency of 8.7% and a maximum efficiency of 10%. The solid-state synthesis of organometallic perovskite can also be carried out on flexible plastic substrates. Using this method on a PET/ITO substrate produces devices with an efficiency of 3.2%. Unlike existing synthetic methods for organometallic perovskite films, the solid-state reaction method does not require the use of orthogonal solvents or careful adjustment of reaction conditions, and thus shows good potential for mass production in the future.展开更多
基金supported by Doctoral Scientific Research Foundation of Shanxi Datong University (2015-B-02)
文摘采用直接水热合成和后合成两种方法制备Al-ITQ-13分子筛,用于催化甲醇转化制备烃类化合物。采用XRD、27Al M AS NM R、NH3-TPD、Py-FTIR和SEM等技术对所合成样品进行了表征。结果表明,两种方法制备的Al-ITQ-13结晶度都较高,且晶体形貌为薄片。与ZSM-5相比,Al-ITQ-13在甲醇转化反应中显示出较高的丙烯选择性、较高的丙烯/乙烯产物比以及较好的催化稳定性。同时,由于后合成所得到的Si Al(B)-ITQ-13强酸量减少,其催化性能优于直接合成的Si Ge Al-ITQ-13。
基金Supported by the National High Technology Research and Development Program of China (2006AA030202)the Talent Training Program of Beijing (2007B022)
文摘The nanoparticles of the hydrophobic drug of danazol with narrow size distribution are facilely prepared by controlled high-gravity anti-solvent precipitation (HGAP) process. Intensified micromixing and uniform nucleation environment are created by the high-gravity equipment (rotating packed bed) in carrying out the anti-solvent precipitation process to produce nanoparticles. The average particle size decreases from 55 μm of the raw danazol to 190 nm of the nanoparticles. The Brunauer-Emmett-Teller (BET) surface area sharply increases from 0.66 m^2·g^-1 to 15.08 m^2·g^-l. Accordingly, the dissolution rate is greatly improved. The molecular state, chemical composition, and crystal form of the danazol nanoparticles remains unchanged after processing according to Fourier transform infrared (FTIR) and X-ray diffraction (XRD), The high recovery ratio and continuous production capacity are highly appreciated in industry. Therefore, the HGAP method might offer a general and facile platform for mass production of hydrophobic pharmaceutical danazol particles in nanometer range.
基金the National Natural Science Foundation of China (No. 29136130).
文摘Production of 6-aminopenicillanic acid (6-APA) by hydrolysis using penicillin acylase (PA) was studied as a model of an enzymatic emulsion liquid membrane (ELM) process. The loss of PA activity was examined for various membrane compositions (organic solvent, surfactant, carrier). The effects of some experimental variables on the stability of emulsion were investigated. It was found that the choice of organic solvent greatly affected the stability of the emulsion. Increasing the concentration of the carrier in the membrane phase increases the transfer rate of substrate and products but also has a destabilizing effect on the emulsion. The recovery of 6-APA obtained by a di-carrier system (N263-N1923) was much higher than those when either of the di-carriers was used separately. The whole process was controlled both by the enzymatic reaction rate and by the transfer rate of the substrate and the products, however, the ratio of them could be changed by varying the composition of the system. For an optimum condition, it was obtained that the recovery ratio of 6-APA was over 80% and the conversion of benzyl penicillin (PG) was up to 90% in the external phase after 30 minutes. Meanwhile, the breakage percentage of the emulsion was less than 2%.
文摘It is already well known that availability of petroleum oil, as a world energy source, is running low. Much work has been done by experts to produce renewable energy, especially using vegetable oil as a raw material. Accordingly, this paper presents preparation and activity test of Cu catalyst using coconut shell activated carbon (AC) as a support, for conversion of n-pentanol and n-butanol to their alkenes as the first step of conversion of ethanol to biogasoline. This conversion is interesting due to any agriculture product containing sugar or starch can be converted to ethanol. Activated carbon was used as a catalyst support because this material is inert; hence, it would not yield unexpected side product, and pollution of environment with the used catalyst can be prevented because the used catalytic metal can easily be recovered. Results of the work showed that coconut shell carbon contained some metals, which disturbed in preparation catalyst by cation exchange process. Washing the carbon with ammonium acetate or HCI solution could reduce the metals content more compared to using water, with optimum concentration for ammonium acetate solution was 1.25 M. Application of Cu/AC in converting n-pentanol and n-butanol, based on qualitative analysis to the products using GLC, GC-MS, and FTIR, when n-pentanol and nitrogen gas were flowed into a reactor filled with Cu/AC catalyst, it could be converted to n-pentene with 200 ℃ as the optimal temperature. While when n-butanol and nitrogen gas were flowed into a reactor filled with more Cu/AC catalyst, the product was supposed to contain its aldehyde and butyl vinyl ether.
文摘This study reports preparation of glass composition (54.50 wt.%) SiO2, (10.80 wt.%) B2O3, (14.20 wt.%) Na2O, (1.20 wt.%) K2O, (6.00 wt.%) CaO, (4.00 wt.%) Fe2O3 and (9.30 wt.%) TiO2 by melt quenching method using direct microwave heating and conventional resistive heating. Study of dielectric loss factor of the glass as function of temperature illustrated increasing loss factor above 370 ℃, 550 ℃, 650 ℃ and 900 ℃, indicating enhanced microwave absorption by the glass at above these temperatures. Chemical analysis results of both the glasses depicted more volatilization loss of volatile ingredients in conventional heating. The study of chemical durability was performed from leachate analysis describing less leaching of Na2O, K2O and other constituents from glass melted in microwave furnace. Glass transition temperatures (Tg) were found to be 576.3 ℃ and 569.5 ℃ for glass melted in conventional and microwave heating route, respectively. Laboratory experiment of glass melting utilizing microwave energy as an alternate heating source demonstrated 70%-75% electrical power saving.
基金the financial support from the National Basic Research Program of China (Grant 2012CB224801)
文摘With oil-soluble molybdenum compound and sublimed sulfur serving as raw materials, two dispersed Mo-based catalysts were prepared, characterized and then applied to the hydrogenation conversion of phenanthrene. The test results showed that under the conditions specified by this study, the catalyst prepared in a higher sulfiding atmosphere was more catalytically active due to its higher content of MoS2 and stronger intrinsic catalytic activity of MoS2 unit, which demonstrated that the sulfiding atmosphere for the preparation of catalysts not only could influence the yield of MoS2 but also the structure of MoS2.The analysis on the selectivity of octahydrophenanthrene isomers revealed that the catalyst prepared in a lower sulfiding atmosphere had a relatively higher catalytic selectivity to the hydrogenation of outer aromatic ring and the structure of catalysts could be modified under the specific reaction conditions. Moreover, the selectivity between the isomers of as-octahydrophenanthrene at different reaction time and temperature was analyzed and, based on the results, a hydrogenation mechanism over dispersed Mo-based catalysts was suggested, with monatomic hydrogen transfer and catalytic surface desorption of the half-addition intermediates functioning as the key points. In addition, it is concluded that the catalyst prepared in a lower sulfiding atmosphere was more capable of adsorption than the other one.
文摘FeCrAI (Ce) stainless steel was functionalized by a conversion treatment in order to allow alumina by diffusion coatings with strong interfacial bonding. The very porous conversion coating produced in a pack aluminization technique had excellent adhesion and was conductive enough to permit conditions favorable for the precipitation of alumina oxyhydroxide during aluminum diffusion coatings. In this work, the bed was prepared as a mixture of A1, NH4C1 and A1203. In the high-activity bed were heat-treated at 1,173 K in an atmosphere made up of team with subsequent air-cooling. The effect of the bed content on the coating was examined. With the high-activity, the desired Fe2Al5 was formed as the outermost coating layer. The coating presented chemical composition gradients suitable for strong adhesion. The improvement of the thermal oxidation behaviour was studied at 1,373 K. Two different aqueous environments, which are (1) NaC1 and (2) H2SO4, are employed for using the technique of potentiodynamic polarization curve. The obtained experimental electrochemical parameters (Ecorr, Jcorr etc,) were used to compare the corrosion resistance of the tested steel state complemented by MEB (electronic scanning microscopy) in combination with dispersive analysis X in energy (EDS) or X ray diffraction indicated that the elements concentration maximum was located in the vicinity of the interface especially in the FeCrAI (Ce) coated by spherical A1203 powder. These results an discussed in terms of an addition effect on the development of the microstructure of oxide films.
基金supported by the National Natural Science Foundation of China(91545103,21273071,21403065)the Commission of Science and Technology of Shanghai Municipality(10dz2220500)
文摘With concerns of diminishing fossil fuel reserves and environmental deterioration, great efforts have been made to explore novel approaches of efficiently utilizing bio-renewable feedstocks to produce chemicals and fuels. 5-Hydroxymethylfurfural(HMF),generated from dehydration of six-carbon ketose, is regarded as a primary and versatile renewable building block to realize the goal of production of these high valued products from renewable biomass resources transformation. In this review, we summarize the recent advances via green routes in the heterogeneous reaction system for the catalytic production of HMF from glucose conversion, and emphasize reaction pathways of these reaction approaches based on the fundamental mechanistic chemistry as well as highlight the challenges(such as separation and purification of products, reusing and regeneration of catalyst, recycling solvent) in this field.
文摘The power conversion efficiency of organometallic perovskite-based solar cells has skyrocketed in recent years. Intensive efforts have been made to prepare high-quality perovskite films tailored to various device configurations. Planar heterojunction devices have achieved record efficiencies; however, the preparation of perovskite films for planar junction devices requires the use of expensive vacuum facilities and/or the fine control of experimental conditions. Here, we demonstrate a facile preparation of perovskite films using solid-state chemistry. Solid-state precursor thin films of CHBNH3I and PbI2 are brought into contact with each other and allowed to react via thermally accelerated diffusion. The resulting perovskite film displays good optical absorption and a smooth morphology. Solar cells based on these films show an average efficiency of 8.7% and a maximum efficiency of 10%. The solid-state synthesis of organometallic perovskite can also be carried out on flexible plastic substrates. Using this method on a PET/ITO substrate produces devices with an efficiency of 3.2%. Unlike existing synthetic methods for organometallic perovskite films, the solid-state reaction method does not require the use of orthogonal solvents or careful adjustment of reaction conditions, and thus shows good potential for mass production in the future.