The objective of this work is to study the reactive crystallization in an airlift-loop reactor （ALR） using the precipitation of Ni（OH）2 as a model reaction. The growth of Ni（OH）2 particles in an ALR and a stirre...The objective of this work is to study the reactive crystallization in an airlift-loop reactor （ALR） using the precipitation of Ni（OH）2 as a model reaction. The growth of Ni（OH）2 particles in an ALR and a stirred tank was quantified by scanning electronic microscope （SEM）, X-ray diffraction （XRD）, laser particle analyzer, tap densitometer and optical microscope, and the growth process of Ni（OH）2 particles is analyzed. It is found that the Ni（OH）2 particles prepared in an ALR have a better sphericity than those in a stirred tank and the growth of Ni（OH）2 particle tap density mainly depends on the size of crystallites： the bigger the size of crystallites, the bigger the tap density is. Based on these, the growth process of Ni（OH）2 particles in ALR is elaborated. Crystallites precipitated from solution aggregate to form large particles with much void. These constituting crystallites continue to grow up, that takes up the void inside particles and makes the tap densitv increase.展开更多
A dichlorosilane gas and a trichlorosilane gas in ambient hydrogen were evaluated to show their different gas flow motions in a slim vertical cold wall chemical vapor deposition reactor for the Minimal Fab system. Thi...A dichlorosilane gas and a trichlorosilane gas in ambient hydrogen were evaluated to show their different gas flow motions in a slim vertical cold wall chemical vapor deposition reactor for the Minimal Fab system. This evaluation was performed for improving and controlling the film qualities and the productivities, using two quartz crystal microbalances (QCM) installed at the </span><span style="font-family:Verdana;">inlet and exhaust of the chamber by taking into account that the QCM frequency corresponds to the real time changes in the gas properties.</span><span style="font-family:Verdana;"> Typically, the time period approaching from the inlet to the exhaust was shorter for the trichlorosilane gas than that for the dichlorosilane gas. The trichlorosilane gas was shown to move like plug flow, while the dichlorosilane gas seemed to be well mixed in the entire chamber.展开更多
The selective aerobic oxidation of benzyl alcohol to benzaldehyde has attracted considerable attention because benzaldehyde is a high value-added product. The rate of this typical gas–liquid reaction is significantly...The selective aerobic oxidation of benzyl alcohol to benzaldehyde has attracted considerable attention because benzaldehyde is a high value-added product. The rate of this typical gas–liquid reaction is significantly affected by mass transfer. In this study, CoTPP-mediated(CoTPP: cobalt(II) mesotetraphenylporphyrin) selective benzyl alcohol oxidation with oxygen was conducted in a membrane microchannel(MMC) reactor and a bubble column(BC) reactor, respectively. We observed that 83% benzyl alcohol was converted within 6.5 min in the MMC reactor, but only less than 10% benzyl alcohol was converted in the BC reactor. Hydrodynamic characteristics and gas–liquid mass transfer performances were compared for the MMC and BC reactors. The MMC reactor was assumed to be a plug flow reactor,and the dimensionless variance was 0.29. Compared to the BC reactor, the gas–liquid mass transfer was intensified significantly in MMC reactor. It could be ascribed to the high gas holdup(2.9 times higher than that of BC reactor), liquid film mass transfer coefficient(8.2 times higher than that of BC reactor), and mass transfer coefficient per unit interfacial area(3.8 times higher than that of BC reactor). Moreover,the Hatta number for the MMC reactor reached up to 0.61, which was about 15 times higher than that of the BC reactor. The computational fluid dynamics calculations for mass fractions in both liquid and gas phases were consistent with the experimental data.展开更多
1 INTRODUCTIONTrickle bed reactors are widely used in the process industry,particularly in petroleumhydroprocessing operations,and have been extensively studied by chemical engineers.In atrickle bed reactor,the gas an...1 INTRODUCTIONTrickle bed reactors are widely used in the process industry,particularly in petroleumhydroprocessing operations,and have been extensively studied by chemical engineers.In atrickle bed reactor,the gas and liquid flow cocurrently down through the packed bedand undergo chemical reactions.However,there exist multiple hydrodynamic stateswhich correspond to either uniform or,in most cases,nonuniform radial distributionof the gas and liquid flows in the packed section.Moreover,the hydrodynamic state展开更多
The research on gas-liquid multiphase reactions using micro reactors is becoming increasingly widespread, given their excellent mass transfer performance. Establishing an accurate and reliable method to measure the ga...The research on gas-liquid multiphase reactions using micro reactors is becoming increasingly widespread, given their excellent mass transfer performance. Establishing an accurate and reliable method to measure the gas-liquid mass transfer performance of micro reactors is crucial for evaluating and optimizing the design of micro reactor structure. In this paper, the physical absorption method of aqueous solution-CO_(2) and the chemical absorption method of sodium carbonate solution-CO_(2) were proposed. By analyzing the chemical reaction equilibrium during the absorption process, the relationship between the mass transfer of CO_(2) and the solubility of hydroxide ions in the solution was established, and the total gas-liquid mass transfer coefficient was immediately obtained by measuring the p H value. The corresponding testing platform and process have been established based on the characteristics of the proposed method to ensure fast and accurate measurement. In addition, the chemical absorption method takes into account temperature factors that were not previously considered. The volumetric mass transfer coefficient measured by these two methods is in the same range as those measured by other methods using the same microchannel structure in previous literature. The methods have the advantages of low equipment cost, faster measurement speed, and simpler procedures, which can facilitate its wide application to the evaluation of the mass transfer performance and hence can guide the structure optimization of microchannel reactors.展开更多
Evaporating bubble column reactor (EBCR) is a kind of aerated reactor in which the reaction heat is removed by the evaporation of volatile reaction mixture. In this paper, a mathematical model that accounts for the ga...Evaporating bubble column reactor (EBCR) is a kind of aerated reactor in which the reaction heat is removed by the evaporation of volatile reaction mixture. In this paper, a mathematical model that accounts for the gas-liquid exothermic reaction and axial dispersions of both gas and liquid phase is employed to study the performance of EBCR for the process of p-xylene(PX) oxidation. The computational results show that there are remarkable concentration and temperature gradients in EBCR for high ratio of height to diameter (H/DT). The temperature is lower at the bottom of column and higher at the top, due to rapid evaporation induced by the feed gas near the bottom. The concentration profiles in the gas phase are more nonuniform than those (except PX) in the liquid phase, which causes more solvent burning consumption at high H/DT ratio. For p-xylene oxidation, theo ptimal H/DT is around 5.展开更多
Unsteady-state operation has been widely applied in chemical engineering, such as optimizing a process, increasing yield and saving energy, etc. But the knowledge of the flow characteristics in bubble column reactors(...Unsteady-state operation has been widely applied in chemical engineering, such as optimizing a process, increasing yield and saving energy, etc. But the knowledge of the flow characteristics in bubble column reactors(BCRs) under unsteady state control is far from enough. In order to study the flow structures in this operation, the volume of fluid (VOF) model and the standard k-ε model to simulate the evolution of gas-liquid flow in BCRs under the start-up state are combined. For both the symmetry and asymmetry flow, the layout of the gas-inlets, the gas-in velocity, the liquid viscosity and the aspect ratio of the BCR all have effects on the liquid velocity distribution. The simulation results could provide some information for the design and scale-up of the BCRs.展开更多
The temporal and spatial growth behaviour of protein crystals, subject to different cooling strategies in protein crystallisation was investigated. Although the impact of temperature and cooling rate on crystal growth...The temporal and spatial growth behaviour of protein crystals, subject to different cooling strategies in protein crystallisation was investigated. Although the impact of temperature and cooling rate on crystal growth of small molecules was well documented, much less has been reported on their impact on the crystallisation of proteins. In this paper, an experimental set-up is configured to carry out such a study which involves an automatic temperature controlled hot-stage crystalliser fitted with a real-time imaging system. Linbro parallel crystallisation experiments(24-well plate) were also conducted to find the suitable initial conditions to be used in the hot-stage crystallisation experiments, including the initial concentration of HEW lysozyme solutions, precipitate concentration and pH value. It was observed that fast cooling rates at the early stage led to precipitates while slow cooling rates produced crystal nuclei, and very slow cooling rates, much smaller than for small molecules are critical to the growth of the nuclei and the crystals to a desired shape. The interesting results provide valuable insight as well as experimental proof of the feasibility and effectiveness of cooling as a means for achieving controlled protein crystallisation, compared with the evaporation approach which was widely used to grow single large crystals for X-ray diffraction study. Since cooling rate control can be easily achieved and has good repeatability, it suggests that large-scale production of protein crystals can be effectively achieved by manipulating cooling rates.展开更多
The hysteresis of gas-liquid mass transfer rate and the corresponding radial liquiddistribution in a trickle bed reactor are measured to provide evidence for the correlation between thesetwo behaviors.Experimental res...The hysteresis of gas-liquid mass transfer rate and the corresponding radial liquiddistribution in a trickle bed reactor are measured to provide evidence for the correlation between thesetwo behaviors.Experimental results indicate that the hysteresis of gas-liquid mass transfer originatesfrom the nonuniformity of the hydrodynamic state of gas-liquid flow and the radial maldistributionof local k<sub>gia</sub> corresponds very well to the radial maldistribution of liquid flow in the bed.The localliquid flow rate is also found to be nonuniform in the azimuthal direction.In view of maldistributedliquid flow even in the pulsing flow regime,the conventional plug flow model seems oversimplifiedfor describing the behavior of a trickle bed.展开更多
A new method is proposed here aiming at designing a shielding wall with the efficiency significantly higher than that of traditional designs. This new design arises from the idea of using channeling in multilayered sh...A new method is proposed here aiming at designing a shielding wall with the efficiency significantly higher than that of traditional designs. This new design arises from the idea of using channeling in multilayered shielding wall structure, each layer composed of bent crystallites distributed in a way that each layer covers a small section of 2π angular range of which wall is exposed. Part of the incident charged particles will get channeled in bent crystallites in each layer. Bending of channeled particles in bent crystallites will change their directions in the wall increasing their path lengths in the wall which would enhance its shielding efficiency for charged particle radiations. Proposed design is useful for radiation shielding in fission power plants, future fusion reactors and air travel.展开更多
Recently,the continuous tube-in-tube reactor based on the Teflon AF membrane is emerging as a powerful toolkit for accelerating gas-liquid mass transfer and reaction rate.Because of its large gas-liquid interfacial ar...Recently,the continuous tube-in-tube reactor based on the Teflon AF membrane is emerging as a powerful toolkit for accelerating gas-liquid mass transfer and reaction rate.Because of its large gas-liquid interfacial area and short mass transfer distance,the reactor can allow a fast gas-liquid mass transfer without direct contact between gas and liquid phases,offering an efficient and safe platform for implementing gas-liquid reaction and rapid determination of gas-liquid parameters.In this review,a detailed description and construction method of this reactor are pro-vided.Then,the recent advancements of the tube-in-tube reactor in fundamental studies and practical applica-tions in gas-involved chemical reactions and biosynthetic processes are discussed.Finally,a perspective on future potential applications of such flow reactors is provided.展开更多
基金Supported by the National Key Research and Development Program(2016YFB0301701)the National Natural Science Foundation of China(21406236,91434126)+1 种基金the Major National Scientific Instrument Development Project(21427814)Jiangsu National Synergetic Innovation Center for Advanced Materials
文摘The objective of this work is to study the reactive crystallization in an airlift-loop reactor （ALR） using the precipitation of Ni（OH）2 as a model reaction. The growth of Ni（OH）2 particles in an ALR and a stirred tank was quantified by scanning electronic microscope （SEM）, X-ray diffraction （XRD）, laser particle analyzer, tap densitometer and optical microscope, and the growth process of Ni（OH）2 particles is analyzed. It is found that the Ni（OH）2 particles prepared in an ALR have a better sphericity than those in a stirred tank and the growth of Ni（OH）2 particle tap density mainly depends on the size of crystallites： the bigger the size of crystallites, the bigger the tap density is. Based on these, the growth process of Ni（OH）2 particles in ALR is elaborated. Crystallites precipitated from solution aggregate to form large particles with much void. These constituting crystallites continue to grow up, that takes up the void inside particles and makes the tap densitv increase.
文摘A dichlorosilane gas and a trichlorosilane gas in ambient hydrogen were evaluated to show their different gas flow motions in a slim vertical cold wall chemical vapor deposition reactor for the Minimal Fab system. This evaluation was performed for improving and controlling the film qualities and the productivities, using two quartz crystal microbalances (QCM) installed at the </span><span style="font-family:Verdana;">inlet and exhaust of the chamber by taking into account that the QCM frequency corresponds to the real time changes in the gas properties.</span><span style="font-family:Verdana;"> Typically, the time period approaching from the inlet to the exhaust was shorter for the trichlorosilane gas than that for the dichlorosilane gas. The trichlorosilane gas was shown to move like plug flow, while the dichlorosilane gas seemed to be well mixed in the entire chamber.
基金financially supported by the National Key Research and Development Program of China (2020YFA0210900)the National Natural Science Foundation of China (21938001 and 21878344)+1 种基金Guangdong Provincial Key Research and Development Programme (2019B110206002)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01C102)。
文摘The selective aerobic oxidation of benzyl alcohol to benzaldehyde has attracted considerable attention because benzaldehyde is a high value-added product. The rate of this typical gas–liquid reaction is significantly affected by mass transfer. In this study, CoTPP-mediated(CoTPP: cobalt(II) mesotetraphenylporphyrin) selective benzyl alcohol oxidation with oxygen was conducted in a membrane microchannel(MMC) reactor and a bubble column(BC) reactor, respectively. We observed that 83% benzyl alcohol was converted within 6.5 min in the MMC reactor, but only less than 10% benzyl alcohol was converted in the BC reactor. Hydrodynamic characteristics and gas–liquid mass transfer performances were compared for the MMC and BC reactors. The MMC reactor was assumed to be a plug flow reactor,and the dimensionless variance was 0.29. Compared to the BC reactor, the gas–liquid mass transfer was intensified significantly in MMC reactor. It could be ascribed to the high gas holdup(2.9 times higher than that of BC reactor), liquid film mass transfer coefficient(8.2 times higher than that of BC reactor), and mass transfer coefficient per unit interfacial area(3.8 times higher than that of BC reactor). Moreover,the Hatta number for the MMC reactor reached up to 0.61, which was about 15 times higher than that of the BC reactor. The computational fluid dynamics calculations for mass fractions in both liquid and gas phases were consistent with the experimental data.
文摘1 INTRODUCTIONTrickle bed reactors are widely used in the process industry,particularly in petroleumhydroprocessing operations,and have been extensively studied by chemical engineers.In atrickle bed reactor,the gas and liquid flow cocurrently down through the packed bedand undergo chemical reactions.However,there exist multiple hydrodynamic stateswhich correspond to either uniform or,in most cases,nonuniform radial distributionof the gas and liquid flows in the packed section.Moreover,the hydrodynamic state
文摘The research on gas-liquid multiphase reactions using micro reactors is becoming increasingly widespread, given their excellent mass transfer performance. Establishing an accurate and reliable method to measure the gas-liquid mass transfer performance of micro reactors is crucial for evaluating and optimizing the design of micro reactor structure. In this paper, the physical absorption method of aqueous solution-CO_(2) and the chemical absorption method of sodium carbonate solution-CO_(2) were proposed. By analyzing the chemical reaction equilibrium during the absorption process, the relationship between the mass transfer of CO_(2) and the solubility of hydroxide ions in the solution was established, and the total gas-liquid mass transfer coefficient was immediately obtained by measuring the p H value. The corresponding testing platform and process have been established based on the characteristics of the proposed method to ensure fast and accurate measurement. In addition, the chemical absorption method takes into account temperature factors that were not previously considered. The volumetric mass transfer coefficient measured by these two methods is in the same range as those measured by other methods using the same microchannel structure in previous literature. The methods have the advantages of low equipment cost, faster measurement speed, and simpler procedures, which can facilitate its wide application to the evaluation of the mass transfer performance and hence can guide the structure optimization of microchannel reactors.
基金Supported by the National Natural Science Foundation of China (No. 20076039) and SINOPEC.
文摘Evaporating bubble column reactor (EBCR) is a kind of aerated reactor in which the reaction heat is removed by the evaporation of volatile reaction mixture. In this paper, a mathematical model that accounts for the gas-liquid exothermic reaction and axial dispersions of both gas and liquid phase is employed to study the performance of EBCR for the process of p-xylene(PX) oxidation. The computational results show that there are remarkable concentration and temperature gradients in EBCR for high ratio of height to diameter (H/DT). The temperature is lower at the bottom of column and higher at the top, due to rapid evaporation induced by the feed gas near the bottom. The concentration profiles in the gas phase are more nonuniform than those (except PX) in the liquid phase, which causes more solvent burning consumption at high H/DT ratio. For p-xylene oxidation, theo ptimal H/DT is around 5.
文摘Unsteady-state operation has been widely applied in chemical engineering, such as optimizing a process, increasing yield and saving energy, etc. But the knowledge of the flow characteristics in bubble column reactors(BCRs) under unsteady state control is far from enough. In order to study the flow structures in this operation, the volume of fluid (VOF) model and the standard k-ε model to simulate the evolution of gas-liquid flow in BCRs under the start-up state are combined. For both the symmetry and asymmetry flow, the layout of the gas-inlets, the gas-in velocity, the liquid viscosity and the aspect ratio of the BCR all have effects on the liquid velocity distribution. The simulation results could provide some information for the design and scale-up of the BCRs.
基金Supported by the China One Thousand Talent Scheme,the National Natural Science Foundation of China under its Major Research Scheme of Meso-scale Mechanism and Control in Multi-phase Reaction Processes(91434126)the Natural Science Foundation of Guangdong Province(2014A030313228)+1 种基金benefited from early work funded by UK Engineering and Physical Science Research Council(EP/H008012/1EP/H008853/1)
文摘The temporal and spatial growth behaviour of protein crystals, subject to different cooling strategies in protein crystallisation was investigated. Although the impact of temperature and cooling rate on crystal growth of small molecules was well documented, much less has been reported on their impact on the crystallisation of proteins. In this paper, an experimental set-up is configured to carry out such a study which involves an automatic temperature controlled hot-stage crystalliser fitted with a real-time imaging system. Linbro parallel crystallisation experiments(24-well plate) were also conducted to find the suitable initial conditions to be used in the hot-stage crystallisation experiments, including the initial concentration of HEW lysozyme solutions, precipitate concentration and pH value. It was observed that fast cooling rates at the early stage led to precipitates while slow cooling rates produced crystal nuclei, and very slow cooling rates, much smaller than for small molecules are critical to the growth of the nuclei and the crystals to a desired shape. The interesting results provide valuable insight as well as experimental proof of the feasibility and effectiveness of cooling as a means for achieving controlled protein crystallisation, compared with the evaporation approach which was widely used to grow single large crystals for X-ray diffraction study. Since cooling rate control can be easily achieved and has good repeatability, it suggests that large-scale production of protein crystals can be effectively achieved by manipulating cooling rates.
基金Supported by the National Natural Science Foundation of China and SINOPEC
文摘The hysteresis of gas-liquid mass transfer rate and the corresponding radial liquiddistribution in a trickle bed reactor are measured to provide evidence for the correlation between thesetwo behaviors.Experimental results indicate that the hysteresis of gas-liquid mass transfer originatesfrom the nonuniformity of the hydrodynamic state of gas-liquid flow and the radial maldistributionof local k<sub>gia</sub> corresponds very well to the radial maldistribution of liquid flow in the bed.The localliquid flow rate is also found to be nonuniform in the azimuthal direction.In view of maldistributedliquid flow even in the pulsing flow regime,the conventional plug flow model seems oversimplifiedfor describing the behavior of a trickle bed.
文摘A new method is proposed here aiming at designing a shielding wall with the efficiency significantly higher than that of traditional designs. This new design arises from the idea of using channeling in multilayered shielding wall structure, each layer composed of bent crystallites distributed in a way that each layer covers a small section of 2π angular range of which wall is exposed. Part of the incident charged particles will get channeled in bent crystallites in each layer. Bending of channeled particles in bent crystallites will change their directions in the wall increasing their path lengths in the wall which would enhance its shielding efficiency for charged particle radiations. Proposed design is useful for radiation shielding in fission power plants, future fusion reactors and air travel.
基金We gratefully acknowledge the supports of National Key Research and Development Program of China(2019YFA0905100)Tsinghua-Foshan Innovation Special Fund(2021THFS0214)the National Natural Science Foundation of China(21978146,22022809)on this work.
文摘Recently,the continuous tube-in-tube reactor based on the Teflon AF membrane is emerging as a powerful toolkit for accelerating gas-liquid mass transfer and reaction rate.Because of its large gas-liquid interfacial area and short mass transfer distance,the reactor can allow a fast gas-liquid mass transfer without direct contact between gas and liquid phases,offering an efficient and safe platform for implementing gas-liquid reaction and rapid determination of gas-liquid parameters.In this review,a detailed description and construction method of this reactor are pro-vided.Then,the recent advancements of the tube-in-tube reactor in fundamental studies and practical applica-tions in gas-involved chemical reactions and biosynthetic processes are discussed.Finally,a perspective on future potential applications of such flow reactors is provided.
