Metal-organic polyhedra(MOPs)possess a microporous framework and impose hierarchical constraints on their surface ligands,leading to the long-ignored,logarithmic ligand exchange dynamics.Herein,polymer networks with M...Metal-organic polyhedra(MOPs)possess a microporous framework and impose hierarchical constraints on their surface ligands,leading to the long-ignored,logarithmic ligand exchange dynamics.Herein,polymer networks with MOP as nanoscale cross-linkers(MOP-CNs)can integrate unique ligand exchange dynamics and microporosity,affording vitrimer-like gas separation membranes with promising mechanical performance and(re)processability.All the ligands on the MOP surfaces are confined and correlated via a 3D coordination framework and their neighboring spaces,giving rise to a high energy barrier for ligand exchange.Therefore,MOP-CNs demonstrate high mechanical strengths at room temperature due to their negligible ligand dynamics.The thermo-activated ligand exchange process with integrated network topology enables facile(re)processing and high solvo-resistance at high temperatures.This facilitates Arrhenius type temperature dependence of flowability and stress relaxation,giving rise to the simultaneous achievement of promising mechanical strengths and(re)processability.Finally,the cage topologies of MOPs endow the materials with a bonus microporous feature and spur their applications as gas separation membranes.展开更多
Mixed matrix hollow fiber membranes(MMHFMs)filled with metal-organic frameworks(MOFs)have great potential for energy-efficient gas separation processes,but the major hurdle is polymer/MOFs interfacial defects and ...Mixed matrix hollow fiber membranes(MMHFMs)filled with metal-organic frameworks(MOFs)have great potential for energy-efficient gas separation processes,but the major hurdle is polymer/MOFs interfacial defects and membrane plasticization.Herein,lab-synthesized MIL-53 was post-functionalized by aminosilane grafting and subsequently incorporated into Ultem-1000 polymer matrix to fabricate high performance MMHFMs.SEM,DLS,XRD and TGA were performed to characterize silane-modified MIL-53(S-MIL-53)and prepared MMHFMs.Moreover,the effect of MOFs loading was systematically investigated first;then gas separation performance of MMHFMs for pure and mixed gas was evaluated under different pressures.MMHFMs containing post-functionalized S-MIL-53 achieved remarkable gas permeation properties which was better than model predictions.Compared to pure HFMs,CO2permeance of MMHFM loaded with 15%S-MIL-53 increased by 157%accompanying with 40%increase for CO2/N2selectivity,which outperformed the MMHFM filled with naked MIL-53.The pure and mixed gas permeation measurements with elevated feed pressure indicated that incorporation of S-MIL-53 also increased the resistance against CO2plasticization.This work reveals that post-modified MOFs embedded in MMHFMs facilitate the improvement of gas separation performance and suppression of membrane plasticization.展开更多
Six aromatic polyesters were prepared for gas separation membranes, and their permeation properties for hydrogen, oxygen, nitrogen, carbon dioxide, and methane were measured at 30 degrees C and 1 atmosphere by low pre...Six aromatic polyesters were prepared for gas separation membranes, and their permeation properties for hydrogen, oxygen, nitrogen, carbon dioxide, and methane were measured at 30 degrees C and 1 atmosphere by low pressure manometric method. The correlation between the gas transport behavior and molecular structure of aromatic polyester membrane is discussed. These data are interpreted qualitatively in terms of the calculated packing density, gas-polymer interaction, concentration of aryl bromine on backbone, and effect of silane group on main chain of polymer.展开更多
Poly(ethylene-oxide)(PEO)-based membranes have attracted much attention recently for CO2 separation because CO2 is highly soluble into PEO and shows high selectivity over other gases such as CH4 and N2.Unfortunately,t...Poly(ethylene-oxide)(PEO)-based membranes have attracted much attention recently for CO2 separation because CO2 is highly soluble into PEO and shows high selectivity over other gases such as CH4 and N2.Unfortunately,those membranes are not strong enough mechanically and highly crystalline,which hinders their broader applications for separation membranes.In this review discussions are made,as much in detail as possible,on the strategies to improve gas separation performance of PEO-based membranes.Some of techniques such as synthesis of graft copolymers that contain PEO,cross-linking of polymers and blending with long chains polymers contributed significantly to improvement of membrane.Incorporation of ionic liquids/nanoparticles has also been found effective.However,surface modification of nanoparticles has been done chemically or physically to enhance their compatibility with polymer matrix.As a result of all such efforts,an excellent performance,i.e.,CO2 permeability up to 200 Barrer,CO2/N2 selectivity up to 200 and CO2/CH4 selectivity up to 70,could be achieved.Another method is to introduce functional groups into PEO-based polymers which boosted CO2 permeability up to 200 Barrer with CO2/CH4 selectivity between 40 and 50.The CO2 permeability of PEO-based membranes increases,without much change in selectivity,when the length of ethylene oxide is increased.展开更多
Gas separation is a key issue in various industrial fields. Hydrogen has the potential for application in clean fuel technologies. Therefore, the separation and purification of hydrogen is an important research subjec...Gas separation is a key issue in various industrial fields. Hydrogen has the potential for application in clean fuel technologies. Therefore, the separation and purification of hydrogen is an important research subject. CO2 capture and storage have important roles in "green chemistry". As an effective clean technology, gas separation using inorganic membranes has attracted much attention in the last several decades. Membrane processes have many applications in the field of gas separation. Cement is one type of inorganic material, with the advantages of a lower cost and a longer lifespan. An experimental setup has been created and improved to measure twenty different cement membranes. The purpose of this work was to investigate the influence of gas molecule properties on the material transport and to explore the influence of operating conditions and membrane composition on separation efficiency. The influences of the above parameters are determined, the best conditions and membrane type are found, it is shown that cementitious material has the ability to separate gas mixtures, and the gas transport mechanism is studied.展开更多
Some novel polyimides containing bisthiazole rings were prepared by reacting 2,2'-diamino-4, 4'-bisthiazole (DART) with different aromatic dianhydride. The polyimides obtained had inherent viscosities of 0.37-...Some novel polyimides containing bisthiazole rings were prepared by reacting 2,2'-diamino-4, 4'-bisthiazole (DART) with different aromatic dianhydride. The polyimides obtained had inherent viscosities of 0.37-0.82 dl/g. Thermogravimetric analysis of the polyimides showed good thermal stability, the temperature at 5% weight loss being from 450 degrees to 560 degrees C. The permeability of two polymer membranes to H-2, O-2 and N-2 was determined, respectively. Three kinds of polyimide films were converted into electrical conductor by pyrolysis at high temperature in nitrogen atmosphere. The maximum room temperature conductivity as high as 3.9x10(2) S/cm for PI him pyrolyzed at 1200 degrees C for 10 min was obtained, and it was very stable in air.展开更多
Membrane technology holds great potential in gas separation applications,especially carbon dioxide capture from industrial processes.To achieve this potential,the outputs from global research endeavours into membrane ...Membrane technology holds great potential in gas separation applications,especially carbon dioxide capture from industrial processes.To achieve this potential,the outputs from global research endeavours into membrane technologies must be trialled in industrial processes,which requires membrane-based pilot plants.These pilot plants are critical to the commercialization of membrane technology,be it as gas separation membranes or membrane gas-solvent contactors,as failure at the pilot plant level may delay the development of the technology for decades.Here,the author reports on his experience of operating membrane-based pilot plants for gas separation and contactor configurations as part of three industrial carbon capture initiatives:the Mulgrave project,H3 project and Vales Point project.Specifically,the challenges of developing and operating membrane pilot plants are presented,as well as the key learnings on how to successfully manage membrane pilot plants to achieve desired performance outcomes.The purpose is to assist membrane technologists in the carbon capture field to achieve successful outcomes for their technology innovations.展开更多
基金The work is supported by the National Natural Science Foundation of China(grant nos.51873067 and 21961142018)the Natural Science Foundation of Guangdong Province(grant no.2021A1515012024).
文摘Metal-organic polyhedra(MOPs)possess a microporous framework and impose hierarchical constraints on their surface ligands,leading to the long-ignored,logarithmic ligand exchange dynamics.Herein,polymer networks with MOP as nanoscale cross-linkers(MOP-CNs)can integrate unique ligand exchange dynamics and microporosity,affording vitrimer-like gas separation membranes with promising mechanical performance and(re)processability.All the ligands on the MOP surfaces are confined and correlated via a 3D coordination framework and their neighboring spaces,giving rise to a high energy barrier for ligand exchange.Therefore,MOP-CNs demonstrate high mechanical strengths at room temperature due to their negligible ligand dynamics.The thermo-activated ligand exchange process with integrated network topology enables facile(re)processing and high solvo-resistance at high temperatures.This facilitates Arrhenius type temperature dependence of flowability and stress relaxation,giving rise to the simultaneous achievement of promising mechanical strengths and(re)processability.Finally,the cage topologies of MOPs endow the materials with a bonus microporous feature and spur their applications as gas separation membranes.
基金the financial support from the National Natural Science Foundation of China(No.21436009)
文摘Mixed matrix hollow fiber membranes(MMHFMs)filled with metal-organic frameworks(MOFs)have great potential for energy-efficient gas separation processes,but the major hurdle is polymer/MOFs interfacial defects and membrane plasticization.Herein,lab-synthesized MIL-53 was post-functionalized by aminosilane grafting and subsequently incorporated into Ultem-1000 polymer matrix to fabricate high performance MMHFMs.SEM,DLS,XRD and TGA were performed to characterize silane-modified MIL-53(S-MIL-53)and prepared MMHFMs.Moreover,the effect of MOFs loading was systematically investigated first;then gas separation performance of MMHFMs for pure and mixed gas was evaluated under different pressures.MMHFMs containing post-functionalized S-MIL-53 achieved remarkable gas permeation properties which was better than model predictions.Compared to pure HFMs,CO2permeance of MMHFM loaded with 15%S-MIL-53 increased by 157%accompanying with 40%increase for CO2/N2selectivity,which outperformed the MMHFM filled with naked MIL-53.The pure and mixed gas permeation measurements with elevated feed pressure indicated that incorporation of S-MIL-53 also increased the resistance against CO2plasticization.This work reveals that post-modified MOFs embedded in MMHFMs facilitate the improvement of gas separation performance and suppression of membrane plasticization.
文摘Six aromatic polyesters were prepared for gas separation membranes, and their permeation properties for hydrogen, oxygen, nitrogen, carbon dioxide, and methane were measured at 30 degrees C and 1 atmosphere by low pressure manometric method. The correlation between the gas transport behavior and molecular structure of aromatic polyester membrane is discussed. These data are interpreted qualitatively in terms of the calculated packing density, gas-polymer interaction, concentration of aryl bromine on backbone, and effect of silane group on main chain of polymer.
文摘Poly(ethylene-oxide)(PEO)-based membranes have attracted much attention recently for CO2 separation because CO2 is highly soluble into PEO and shows high selectivity over other gases such as CH4 and N2.Unfortunately,those membranes are not strong enough mechanically and highly crystalline,which hinders their broader applications for separation membranes.In this review discussions are made,as much in detail as possible,on the strategies to improve gas separation performance of PEO-based membranes.Some of techniques such as synthesis of graft copolymers that contain PEO,cross-linking of polymers and blending with long chains polymers contributed significantly to improvement of membrane.Incorporation of ionic liquids/nanoparticles has also been found effective.However,surface modification of nanoparticles has been done chemically or physically to enhance their compatibility with polymer matrix.As a result of all such efforts,an excellent performance,i.e.,CO2 permeability up to 200 Barrer,CO2/N2 selectivity up to 200 and CO2/CH4 selectivity up to 70,could be achieved.Another method is to introduce functional groups into PEO-based polymers which boosted CO2 permeability up to 200 Barrer with CO2/CH4 selectivity between 40 and 50.The CO2 permeability of PEO-based membranes increases,without much change in selectivity,when the length of ethylene oxide is increased.
基金supported by Federal Ministry of Food,Agriculture and Consumer Protection,Agency for Renewable Resources in Germany(No.22010502)
文摘Gas separation is a key issue in various industrial fields. Hydrogen has the potential for application in clean fuel technologies. Therefore, the separation and purification of hydrogen is an important research subject. CO2 capture and storage have important roles in "green chemistry". As an effective clean technology, gas separation using inorganic membranes has attracted much attention in the last several decades. Membrane processes have many applications in the field of gas separation. Cement is one type of inorganic material, with the advantages of a lower cost and a longer lifespan. An experimental setup has been created and improved to measure twenty different cement membranes. The purpose of this work was to investigate the influence of gas molecule properties on the material transport and to explore the influence of operating conditions and membrane composition on separation efficiency. The influences of the above parameters are determined, the best conditions and membrane type are found, it is shown that cementitious material has the ability to separate gas mixtures, and the gas transport mechanism is studied.
基金This project was supported by the National Natural Science Foundation of China
文摘Some novel polyimides containing bisthiazole rings were prepared by reacting 2,2'-diamino-4, 4'-bisthiazole (DART) with different aromatic dianhydride. The polyimides obtained had inherent viscosities of 0.37-0.82 dl/g. Thermogravimetric analysis of the polyimides showed good thermal stability, the temperature at 5% weight loss being from 450 degrees to 560 degrees C. The permeability of two polymer membranes to H-2, O-2 and N-2 was determined, respectively. Three kinds of polyimide films were converted into electrical conductor by pyrolysis at high temperature in nitrogen atmosphere. The maximum room temperature conductivity as high as 3.9x10(2) S/cm for PI him pyrolyzed at 1200 degrees C for 10 min was obtained, and it was very stable in air.
基金The author thanks the C02CRC Ltd.,especially Dr.Abdul Qader and Mr.Barry HooperProcess Group(now Suez Oil&Gas Systems),especially Dr.Trina Dreher+7 种基金Pilot Plant Management&Services Pty Ltd.,especially Mr.Kurt LuttinCommonwealth Scientific and Industrial Research Organisation(CSIRO),especially Mr.Dan Maher and Mr.Phillip GreenFurnace EngineeringHRL Technology Pty Ltd.Engie(formerly GDF Suez)Delta Electricitythe Victorian Government's Energy Technology Innovation Strategy(ETIS)and Victoria Fellowshipas well as Coal Innovation New South Wales.
文摘Membrane technology holds great potential in gas separation applications,especially carbon dioxide capture from industrial processes.To achieve this potential,the outputs from global research endeavours into membrane technologies must be trialled in industrial processes,which requires membrane-based pilot plants.These pilot plants are critical to the commercialization of membrane technology,be it as gas separation membranes or membrane gas-solvent contactors,as failure at the pilot plant level may delay the development of the technology for decades.Here,the author reports on his experience of operating membrane-based pilot plants for gas separation and contactor configurations as part of three industrial carbon capture initiatives:the Mulgrave project,H3 project and Vales Point project.Specifically,the challenges of developing and operating membrane pilot plants are presented,as well as the key learnings on how to successfully manage membrane pilot plants to achieve desired performance outcomes.The purpose is to assist membrane technologists in the carbon capture field to achieve successful outcomes for their technology innovations.