Hierarchical ZSM-11 microspheres with intercrystalline mesoporous properties and rod-like crystals intergrowth morphology have been synthesized using a spot of tetrabutylammonium as a single template.XRD,FTIR,SEM,TEM ...Hierarchical ZSM-11 microspheres with intercrystalline mesoporous properties and rod-like crystals intergrowth morphology have been synthesized using a spot of tetrabutylammonium as a single template.XRD,FTIR,SEM,TEM and N2 adsorption analysis revealed that each individual particle was composed of nanosized rod crystals inserting each other and the intercrystalline voids existing among rods gave a significant mesopore size distribution.Steam treatment result demonstrated the excellent hydrothermal stability of samples.Various crystallization modes including constant temperature crystallization (one-stage crystallization) and two-stage temperature-varying crystallization with different 1st stage durations were investigated.The results suggested that the crystallization modes were mainly responsible for the adjustable particle size and textural properties of samples while the small amount of tetrabutylammonium bromide was mainly used to direct the formation of both ZSM-11 framework and its intergrowth morphology.Furthermore,the performance of optimal ZSM-11 as an active component for the catalytic pyrolysis of heavy oil was also investigated.Compared with the commercial pyrolysis catalyst,the hierarchical ZSM-11 catalyst exhibited a high selectivity to desired products(LPG+gasoline+diesel),as well as a much lower dry gas and coke yield,plus a high selectivity and yield of light olefins(C=3 C=4)and very poor selectivity to benzene.Therefore,fully open micropore-mesopore connectivity would make such hierarchically porous ZSM-11 zeolites very attractive for applications in clean petrochemical catalysis field.展开更多
Using the JQ-Ⅱ high pressure hydrogenation micro-reactor unit, the reactivity of Athabasca bitumen derived heavy gas oil was studied over commercial and homemade hydrotreating catalysts. The effects of catalyst prepa...Using the JQ-Ⅱ high pressure hydrogenation micro-reactor unit, the reactivity of Athabasca bitumen derived heavy gas oil was studied over commercial and homemade hydrotreating catalysts. The effects of catalyst preparation variables and the influences of operation conditions, such as pressure, temperature, hydrogen/oil ratio and space velocity were also examined. It was shown that the optimal concentrations of the active components were 5% of NiO, 20% of MoO3 and 3.5% of phosphorus (by mass), and the suitable operation conditions were determined experimentally.展开更多
A bidisperse model for transient diffusion and adsorption processes in porous materials is presented in this paper.The mathematical model is solved by numerical methods based on finite elements combined with the linea...A bidisperse model for transient diffusion and adsorption processes in porous materials is presented in this paper.The mathematical model is solved by numerical methods based on finite elements combined with the linear driving force approximation.A criterion based on the model to identify the diffusion controlling mechanism(macropore diffusion,micropore diffusion,or both)is proposed.The effects of different adsorption isotherms(linear,Freundlich,or Langmuir)on the concentration profiles and on curves of fractional uptake versus time are investigated.In addition,the influences of model parameters concerning the pore networks on the fractional uptake are studied as well.展开更多
Large-scale use of detergents to remove oil-fouling in industry continuously generates tremendous amounts of wastewater and thus leads to both economic and environmental problems.To develop recyclable oil-fouling remo...Large-scale use of detergents to remove oil-fouling in industry continuously generates tremendous amounts of wastewater and thus leads to both economic and environmental problems.To develop recyclable oil-fouling removal strategy is an appealing solution but a challenging task.Herein,a kind of dynamic imine-based surfactant has been constructed by 2-formylbenzenesulfonic acid sodium salt(FBSS)and linear amines(CnNH_(2),n=6,7,8,10,and 12).Owing to high interfacial activity and strong assembly ability,dynamic FBSS/C8NH_(2)system can remove oil-fouling on multiple substrates for at least 10 cycles,largely reducing the toxicity to ecosystem.At basic pH,the hierarchical assemblies(from vesicle to network and hollow sphere)are formed and boost surfactant molecule enrichment around oil-fouling,leading to highly efficient emulsification.When pH is changed to acidic condition,the surfactant molecules dissociate due to the breaking of imine bonds,and accordingly the emulsion is destroyed and the released oil droplets float to the top layer.After removing the oil-fouling and adjusting the solution back to basic pH,the surfactant assemblies are reconstructed and used for the next oil-fouling cleaning cycle.This study provides a recyclable,efficient and eco-friendly oil-fouling removal approach,satisfying the need of sustainable development.展开更多
Understanding the coking behaviors has been considered to be really essential for developing better vacuum residue processing technologies.A battery of thermal cracking tests of typical vacuum residue at 410℃ with va...Understanding the coking behaviors has been considered to be really essential for developing better vacuum residue processing technologies.A battery of thermal cracking tests of typical vacuum residue at 410℃ with various reaction time were performed to evaluate the coke formation process.The total yields of ideal components including naphtha,atmospheric gas oil(AGO)and vacuum gas oil(VGO)of thermal cracking reactions increased from 10.89%to 40.81%,and the conversion ratios increased from8.05%to 43.33%with increasing the reaction time from 10 to 70 min.The asphaltene content increased from 12.14%to a maximum of 22.39%and then decreased,and this maximum of asphaltene content occurred at the end of the coking induction period.The asphaltenes during the coking induction period,at the end and after coking induction period of those tested thermal cracking reactions were characterized to disclose the structure changing rules for coke formation process,and the coke formation pathways were discussed to reveal the coke formation process at molecular level.展开更多
The filtration performance of the moving bed granular filter with axial flow (MBGF-AF) is investigated through a large cold experiment. The effect of different operation parameters on the filtration performance (colle...The filtration performance of the moving bed granular filter with axial flow (MBGF-AF) is investigated through a large cold experiment. The effect of different operation parameters on the filtration performance (collection efficiency, pressure drop) of the axial-flow moving bed filter is investigated in combination with the dust deposition effect and the mechanism of trapping dust by the capturing particles. The results show that the collection efficiency of MBGF-AF is enhanced by decreasing the superficial gas velocity, increasing the inlet dust concentration properly, or decreasing the moving velocity of the capturing particles. A model covering the above operation parameters is established to calculate the collection efficiency of the moving bed granular filter. It is used in a wide range of operating parameters for the MBGFs.展开更多
Group C particles are often regarded as non-fluidizable but have proven to effectively fluidize with nanoparticle addition,which results in small bubbles and a high gas holdup in the dense phase during the experiments...Group C particles are often regarded as non-fluidizable but have proven to effectively fluidize with nanoparticle addition,which results in small bubbles and a high gas holdup in the dense phase during the experiments.Group C^(+)particles provide an increased surface area for gas-solid contact and improve the reaction performance,especially for gas-phase catalytic reactions.On the basis of a previous study of the ozone decomposition reaction using Group C^(+)particles,a two-phase model was used to evaluate the reactor contact efficiency,and was used to compare the partial oxidation performance of the n-butane to maleic anhydride reaction in fluidized-bed catalytic reactors of Group C^(+)and Group A particles.The reactor with Group C^(+)particles achieved a higher n-butane conversion and MAN yield compared with that using Group A particles,based on the identical catalyst quantity or on the same gas residence time.Therefore,the reactor with Group C^(+)particles can achieve the same reaction conversion and yield with fewer catalysts or a smaller reactor size,or both.Therefore,the fluidized bed catalytic reactor of Group C^(+)particles is expected to be of major significance in industrial processes,especially for gas-phase catalytic reactions.展开更多
基金supported by the National Program on Key Basic Research Project(973 Program)(Grant No.2012CB215000)the financial support from Fundamental Research Funds for the Central Universities
文摘Hierarchical ZSM-11 microspheres with intercrystalline mesoporous properties and rod-like crystals intergrowth morphology have been synthesized using a spot of tetrabutylammonium as a single template.XRD,FTIR,SEM,TEM and N2 adsorption analysis revealed that each individual particle was composed of nanosized rod crystals inserting each other and the intercrystalline voids existing among rods gave a significant mesopore size distribution.Steam treatment result demonstrated the excellent hydrothermal stability of samples.Various crystallization modes including constant temperature crystallization (one-stage crystallization) and two-stage temperature-varying crystallization with different 1st stage durations were investigated.The results suggested that the crystallization modes were mainly responsible for the adjustable particle size and textural properties of samples while the small amount of tetrabutylammonium bromide was mainly used to direct the formation of both ZSM-11 framework and its intergrowth morphology.Furthermore,the performance of optimal ZSM-11 as an active component for the catalytic pyrolysis of heavy oil was also investigated.Compared with the commercial pyrolysis catalyst,the hierarchical ZSM-11 catalyst exhibited a high selectivity to desired products(LPG+gasoline+diesel),as well as a much lower dry gas and coke yield,plus a high selectivity and yield of light olefins(C=3 C=4)and very poor selectivity to benzene.Therefore,fully open micropore-mesopore connectivity would make such hierarchically porous ZSM-11 zeolites very attractive for applications in clean petrochemical catalysis field.
文摘Using the JQ-Ⅱ high pressure hydrogenation micro-reactor unit, the reactivity of Athabasca bitumen derived heavy gas oil was studied over commercial and homemade hydrotreating catalysts. The effects of catalyst preparation variables and the influences of operation conditions, such as pressure, temperature, hydrogen/oil ratio and space velocity were also examined. It was shown that the optimal concentrations of the active components were 5% of NiO, 20% of MoO3 and 3.5% of phosphorus (by mass), and the suitable operation conditions were determined experimentally.
基金financial support by the National Natural Science Foundation of China(Grant No.91534120)China National Petroleum Company under the contract number DQZX-KY-17-019
文摘A bidisperse model for transient diffusion and adsorption processes in porous materials is presented in this paper.The mathematical model is solved by numerical methods based on finite elements combined with the linear driving force approximation.A criterion based on the model to identify the diffusion controlling mechanism(macropore diffusion,micropore diffusion,or both)is proposed.The effects of different adsorption isotherms(linear,Freundlich,or Langmuir)on the concentration profiles and on curves of fractional uptake versus time are investigated.In addition,the influences of model parameters concerning the pore networks on the fractional uptake are studied as well.
基金the National Natural Science Foundation of China(Nos.21988102,22072161,and 21773261)the Ministry of Science and Technology of the People’s Republic of China(No.2021YFA0716700).
文摘Large-scale use of detergents to remove oil-fouling in industry continuously generates tremendous amounts of wastewater and thus leads to both economic and environmental problems.To develop recyclable oil-fouling removal strategy is an appealing solution but a challenging task.Herein,a kind of dynamic imine-based surfactant has been constructed by 2-formylbenzenesulfonic acid sodium salt(FBSS)and linear amines(CnNH_(2),n=6,7,8,10,and 12).Owing to high interfacial activity and strong assembly ability,dynamic FBSS/C8NH_(2)system can remove oil-fouling on multiple substrates for at least 10 cycles,largely reducing the toxicity to ecosystem.At basic pH,the hierarchical assemblies(from vesicle to network and hollow sphere)are formed and boost surfactant molecule enrichment around oil-fouling,leading to highly efficient emulsification.When pH is changed to acidic condition,the surfactant molecules dissociate due to the breaking of imine bonds,and accordingly the emulsion is destroyed and the released oil droplets float to the top layer.After removing the oil-fouling and adjusting the solution back to basic pH,the surfactant assemblies are reconstructed and used for the next oil-fouling cleaning cycle.This study provides a recyclable,efficient and eco-friendly oil-fouling removal approach,satisfying the need of sustainable development.
文摘Understanding the coking behaviors has been considered to be really essential for developing better vacuum residue processing technologies.A battery of thermal cracking tests of typical vacuum residue at 410℃ with various reaction time were performed to evaluate the coke formation process.The total yields of ideal components including naphtha,atmospheric gas oil(AGO)and vacuum gas oil(VGO)of thermal cracking reactions increased from 10.89%to 40.81%,and the conversion ratios increased from8.05%to 43.33%with increasing the reaction time from 10 to 70 min.The asphaltene content increased from 12.14%to a maximum of 22.39%and then decreased,and this maximum of asphaltene content occurred at the end of the coking induction period.The asphaltenes during the coking induction period,at the end and after coking induction period of those tested thermal cracking reactions were characterized to disclose the structure changing rules for coke formation process,and the coke formation pathways were discussed to reveal the coke formation process at molecular level.
基金supported by National Natural Science Foundation of China(U1862202).
文摘The filtration performance of the moving bed granular filter with axial flow (MBGF-AF) is investigated through a large cold experiment. The effect of different operation parameters on the filtration performance (collection efficiency, pressure drop) of the axial-flow moving bed filter is investigated in combination with the dust deposition effect and the mechanism of trapping dust by the capturing particles. The results show that the collection efficiency of MBGF-AF is enhanced by decreasing the superficial gas velocity, increasing the inlet dust concentration properly, or decreasing the moving velocity of the capturing particles. A model covering the above operation parameters is established to calculate the collection efficiency of the moving bed granular filter. It is used in a wide range of operating parameters for the MBGFs.
文摘Group C particles are often regarded as non-fluidizable but have proven to effectively fluidize with nanoparticle addition,which results in small bubbles and a high gas holdup in the dense phase during the experiments.Group C^(+)particles provide an increased surface area for gas-solid contact and improve the reaction performance,especially for gas-phase catalytic reactions.On the basis of a previous study of the ozone decomposition reaction using Group C^(+)particles,a two-phase model was used to evaluate the reactor contact efficiency,and was used to compare the partial oxidation performance of the n-butane to maleic anhydride reaction in fluidized-bed catalytic reactors of Group C^(+)and Group A particles.The reactor with Group C^(+)particles achieved a higher n-butane conversion and MAN yield compared with that using Group A particles,based on the identical catalyst quantity or on the same gas residence time.Therefore,the reactor with Group C^(+)particles can achieve the same reaction conversion and yield with fewer catalysts or a smaller reactor size,or both.Therefore,the fluidized bed catalytic reactor of Group C^(+)particles is expected to be of major significance in industrial processes,especially for gas-phase catalytic reactions.