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1.发明授权Crosslinked organic-inorganic hybrid membranes and their use in gas separation 有权交联的有机 - 无机杂化膜及其在气体分离中的应用公开(公告)号：US08030399B2
公开(公告)日：2011-10-04
申请号：US12847067
申请日：2010-07-30
IPC分类号： C08B37/00
CPC分类号： C08L1/20 , B01D53/228 , B01D67/0079 , B01D71/00 , B01D71/16 , B01D71/52 , B01D71/70 , B01D2257/102 , B01D2257/504 , C08B7/00 , C08G65/33306 , C08G65/33351 , C08G65/336 , C08G2650/58 , C08L71/02 , Y02C10/10 , Y02P20/152
摘要： The present invention is for crosslinked membranes and in particular for crosslinked poly(ethylene oxide)-cellulose acetate-silsesquioxane (PEO-CA-Si) organic-inorganic hybrid membranes and their use in gas separation. These crosslinked PEO-CA-Si membranes were prepared by in-situ sol-gel co-condensation of crosslinkable PEO-organotrialkoxysilane and CA-organotrialkoxysilane polymers in the presence of acetic acid catalyst during the formation of membranes. The crosslinkable PEO- and CA-organotrialkoxysilane polymers were synthesized via the reaction between the hydroxyl groups on PEO (or on CA) and the isocyanate on organotrialkoxysilane to form urethane linkages under mild conditions. The crosslinked PEO-CA-Si membranes exhibited both increased selectivity of CO2/N2 and CO2 permeability as compared to a CA membrane, suggesting that these membranes are very promising for gas separations such as CO2/N2 separation.
摘要翻译： 本发明涉及交联膜，特别是交联聚（环氧乙烷） - 醋酸纤维素 - 倍半硅氧烷（PEO-CA-Si）有机 - 无机混合膜及其在气体分离中的应用。 这些交联的PEO-CA-Si膜通过在形成膜期间在乙酸催化剂存在下通过可交联的PEO-有机三烷氧基硅烷和CA-有机三烷氧基硅烷聚合物的原位溶胶 - 凝胶共缩合制备。 通过PEO（或CA）上的羟基与有机三烷氧基硅烷上的异氰酸酯之间的反应合成可交联PEO-和CA-有机三烷氧基硅烷聚合物，以在温和条件下形成氨基甲酸酯键。 与CA膜相比，交联的PEO-CA-Si膜显示出增加的CO 2 / N 2选择性和CO 2渗透性，这表明这些膜对于气体分离如CO 2 / N 2分离是非常有希望的。
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2.发明申请CROSSLINKED ORGANIC-INORGANIC HYBRID MEMBRANES AND THEIR USE IN GAS SEPARATION 有权交联有机无机混合膜及其在气体分离中的应用公开(公告)号：US20100288122A1
公开(公告)日：2010-11-18
申请号：US12847067
申请日：2010-07-30
IPC分类号： B01D53/22
CPC分类号： C08L1/20 , B01D53/228 , B01D67/0079 , B01D71/00 , B01D71/16 , B01D71/52 , B01D71/70 , B01D2257/102 , B01D2257/504 , C08B7/00 , C08G65/33306 , C08G65/33351 , C08G65/336 , C08G2650/58 , C08L71/02 , Y02C10/10 , Y02P20/152
摘要： The present invention is for crosslinked membranes and in particular for crosslinked poly(ethylene oxide)-cellulose acetate-silsesquioxane (PEO-CA-Si) organic-inorganic hybrid membranes and their use in gas separation. These crosslinked PEO-CA-Si membranes were prepared by in-situ sol-gel co-condensation of crosslinkable PEO-organotrialkoxysilane and CA-organotrialkoxysilane polymers in the presence of acetic acid catalyst during the formation of membranes. The crosslinkable PEO- and CA-organotrialkoxysilane polymers were synthesized via the reaction between the hydroxyl groups on PEO (or on CA) and the isocyanate on organotrialkoxysilane to form urethane linkages under mild conditions. The crosslinked PEO-CA-Si membranes exhibited both increased selectivity of CO2/N2 and CO2 permeability as compared to a CA membrane, suggesting that these membranes are very promising for gas separations such as CO2/N2 separation.
摘要翻译： 本发明涉及交联膜，特别是交联聚（环氧乙烷） - 醋酸纤维素 - 倍半硅氧烷（PEO-CA-Si）有机 - 无机混合膜及其在气体分离中的应用。 这些交联的PEO-CA-Si膜通过在形成膜期间在乙酸催化剂存在下通过可交联的PEO-有机三烷氧基硅烷和CA-有机三烷氧基硅烷聚合物的原位溶胶 - 凝胶共缩合制备。 通过PEO（或CA）上的羟基与有机三烷氧基硅烷上的异氰酸酯之间的反应合成可交联PEO-和CA-有机三烷氧基硅烷聚合物，以在温和条件下形成氨基甲酸酯键。 与CA膜相比，交联的PEO-CA-Si膜显示出增加的CO 2 / N 2选择性和CO 2渗透性，这表明这些膜对于气体分离如CO 2 / N 2分离是非常有希望的。
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公开(公告)号：US20100018926A1
公开(公告)日：2010-01-28
申请号：US12145559
申请日：2008-06-25
CPC分类号： B01D71/028 , B01D67/0079 , B01D69/148 , B01D2323/21 , B01D2323/36 , B01D2325/16
摘要： The present invention discloses mixed matrix membranes (MMMs) comprising ion-exchanged molecular sieves such as UZM-5 zeolite ion-exchanged with Li+ cation (Li-UZM-5) and a continuous polymer matrix and methods for making and using these membranes. These MMMs, comprising ion-exchanged molecular sieves, in the form of symmetric dense films, asymmetric flat sheets, asymmetric hollow fibers, or thin-film composites, have exhibited simultaneously increased selectivity and permeability (or permeance) over polymer-only membranes and the mixed matrix membranes made from molecular sieves that have not been ion exchanged for gas separations. These MMMs are suitable for a variety of liquid, gas, and vapor separations such as desalination of water by reverse osmosis, deep desulfurization of gasoline and diesel fuels, ethanol/water separations, pervaporation dehydration of aqueous/organic mixtures, CO2/CH4, CO2/N2, H2/CH4, O2/N2, olefin/paraffin, iso/normal paraffins separations, and other light gas mixture separations.
摘要翻译： 本发明公开了包含离子交换分子筛（例如与Li +阳离子（Li-UZM-5）离子交换的UZM-5沸石）和连续聚合物基质的混合基质膜（MMM）以及制造和使用这些膜的方法。 这些包含离子交换分子筛，以对称致密膜，不对称平板，不对称中空纤维或薄膜复合材料形式的MMM已经显示出与聚合物膜相比增加的选择性和渗透性（或渗透性），并且 由分子筛制成的未经离子交换进行气体分离的混合基质膜。 这些MMM适用于各种液体，气体和蒸汽分离，如通过反渗透脱水，汽油和柴油燃料的深度脱硫，乙醇/水分离，水/有机混合物的渗透蒸发脱水，CO 2 / CH 4，CO 2 / N2，H2 / CH4，O2 / N2，烯烃/石蜡，异/正链烷烃分离和其他轻质气体混合物分离。
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公开(公告)号：US20090149565A1
公开(公告)日：2009-06-11
申请号：US11954013
申请日：2007-12-11
IPC分类号： C08F16/06 , C08F283/04 , C08G18/00 , C08G63/91 , C08F283/00 , C08J3/28
CPC分类号： C08F20/52 , B01D67/0079 , B01D69/148 , B01D71/028 , B01D2323/21 , C08L75/04
摘要： The present invention discloses method for making defect-free high performance mixed matrix membranes (MMMs) containing a continuous polymer matrix and dispersed molecular sieves such as AlPO-14 or UZM-5. These MMMs can be used for separations. The novel method for making defect-free high performance MMMs comprises: post treating the MMM at a temperature ≧150° C. This new method results in a MMM with either no macrovoids or voids of less than 5 angstroms at the interface of the continuous polymer matrix and the molecular sieves. The MMMs are in the form of symmetric dense film, thin-film composite (TFC), asymmetric flat sheet or asymmetric hollow fiber. These MMMs have good flexibility and high mechanical strength, and exhibit high carbon dioxide/methane (CO2/CH4) selectivity and high CO2 permeance for CO2/CH4 separation. The MMMs are suitable for a variety of liquid, gas, and vapor separations.
摘要翻译： 本发明公开了制备含有连续聚合物基质和分散分子筛如AlPO-14或UZM-5的无缺陷高性能混合基质膜（MMM）的方法。 这些MMM可用于分离。 用于制造无缺陷的高性能MMM的新方法包括：在> = 150℃的温度下对MMM进行后处理。该新方法导致MMM在连续的界面处没有大孔或小于5埃的空隙 聚合物基质和分子筛。 MMM是对称致密膜，薄膜复合材料（TFC），不对称平板或不对称中空纤维的形式。 这些MMM具有良好的柔韧性和高的机械强度，并且对于CO 2 / CH 4分离显示出高二氧化碳/甲烷（CO 2 / CH 4）选择性和高CO 2渗透性。 MMM适用于各种液体，气体和蒸气分离。
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5.发明申请UV CROSS-LINKED POLYMER FUNCTIONALIZED MOLECULAR SIEVE/POLYMER MIXED MATRIX MEMBRANES 审中-公开紫外线交联聚合物官能化分子筛/聚合物混合基质膜公开(公告)号：US20080295691A1
公开(公告)日：2008-12-04
申请号：US11756988
申请日：2007-06-01
IPC分类号： B01D46/24
CPC分类号： B01D69/141 , B01D53/228 , B01D67/0006 , B01D69/125 , B01D2323/345 , B01D2325/02
摘要： The present invention discloses methods of separating gases using high performance UV cross-linked polymer functionalized molecular sieve/polymer mixed matrix membranes (MMMs) with either no macrovoids or voids of less than several angstroms at the interface of the polymer matrix and the molecular sieves. These UV cross-linked MMMs were prepared by incorporating polyethersulfone (PES) functionalized molecular sieves such as AIPO-14 and UZM-25 small pore microporous molecular sieves into a continuous UV cross-linkable polyimide polymer matrix followed by UV cross-linking. The UV cross-linked MMMs in the form of symmetric dense film, asymmetric flat sheet membrane, or asymmetric hollow fiber membranes have good flexibility, high mechanical strength, and exhibit significantly enhanced selectivity and permeability over polymer membranes made from corresponding continuous polyimide polymer matrices for carbon dioxide/methane and hydrogen/methane separations. The MMMs of the present invention are suitable for a variety of liquid, gas, and vapor separations.
摘要翻译： 本发明公开了使用高分子量UV交联聚合物官能化分子筛/聚合物混合基质膜（MMM）分离气体的方法，在聚合物基质和分子筛的界面处没有大孔或小于几埃的空隙。 这些UV交联MMM通过将聚醚砜（PES）官能化分子筛如AIPO-14和UZM-25小孔微孔分子筛掺入连续的可UV交联的聚酰亚胺聚合物基质中，然后进行UV交联来制备。 对称致密膜，不对称平板膜或不对称中空纤维膜形式的UV交联MMMs具有良好的柔韧性，高机械强度，并且在由相应的连续聚酰亚胺聚合物基质制成的聚合物膜上表现出显着增强的选择性和渗透性 二氧化碳/甲烷和氢气/甲烷分离。 本发明的MMM适用于各种液体，气体和蒸气分离。
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6.发明授权Mixed matrix membranes incorporating surface-functionalized molecular sieve nanoparticles 失效掺入表面官能化分子筛纳米颗粒的混合基质膜公开(公告)号：US08394453B2
公开(公告)日：2013-03-12
申请号：US12904673
申请日：2010-10-14
申请人： Chunqing Liu , Stephen T. Wilson , Beth McCulloch
发明人： Chunqing Liu , Stephen T. Wilson , Beth McCulloch
IPC分类号： B05D5/00
CPC分类号： B01D67/0079 , B01D69/148 , B01D71/028 , Y02C10/10
摘要： Mixed matrix membranes that are capable of separation and purification of gas mixtures are disclosed. These membranes comprise polymers that include dispersed therein nanomolecular sieve particles. In a preferred embodiment, the nanomolecular sieve particles contain attached functional groups to prevent their agglomeration.
摘要翻译： 公开了能够分离和纯化气体混合物的混合基质膜。 这些膜包括分散在纳米分子筛颗粒中的聚合物。 在优选的实施方案中，纳米分子筛颗粒含有附着的官能团以防止其结合。
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7.发明授权Crosslinked organic-inorganic hybrid membranes and their use in gas separation 有权交联的有机 - 无机杂化膜及其在气体分离中的应用公开(公告)号：US07790803B2
公开(公告)日：2010-09-07
申请号：US12131392
申请日：2008-06-02
IPC分类号： C07B37/00
CPC分类号： C08L1/20 , B01D53/228 , B01D67/0079 , B01D71/00 , B01D71/16 , B01D71/52 , B01D71/70 , B01D2257/102 , B01D2257/504 , C08B7/00 , C08G65/33306 , C08G65/33351 , C08G65/336 , C08G2650/58 , C08L71/02 , Y02C10/10 , Y02P20/152
摘要： The present invention is for crosslinked membranes and in particular for crosslinked poly(ethylene oxide)-cellulose acetate-silsesquioxane (PEO-CA-Si) organic-inorganic hybrid membranes and their use in gas separation. These crosslinked PEO-CA-Si membranes were prepared by in-situ sol-gel co-condensation of crosslinkable PEO-organotrialkoxysilane and CA-organotrialkoxysilane polymers in the presence of acetic acid catalyst during the formation of membranes. The crosslinkable PEO- and CA-organotrialkoxysilane polymers were synthesized via the reaction between the hydroxyl groups on PEO (or on CA) and the isocyanate on organotrialkoxysilane to form urethane linkages under mild conditions. The crosslinked PEO-CA-Si membranes exhibited both increased selectivity of CO2/N2 and CO2 permeability as compared to a CA membrane, suggesting that these membranes are very promising for gas separations such as CO2/N2 separation.
摘要翻译： 本发明涉及交联膜，特别是交联聚（环氧乙烷） - 醋酸纤维素 - 倍半硅氧烷（PEO-CA-Si）有机 - 无机混合膜及其在气体分离中的应用。 这些交联的PEO-CA-Si膜通过在形成膜期间在乙酸催化剂存在下通过可交联的PEO-有机三烷氧基硅烷和CA-有机三烷氧基硅烷聚合物的原位溶胶 - 凝胶共缩合制备。 通过PEO（或CA）上的羟基与有机三烷氧基硅烷上的异氰酸酯之间的反应合成可交联PEO-和CA-有机三烷氧基硅烷聚合物，以在温和条件下形成氨基甲酸酯键。 与CA膜相比，交联的PEO-CA-Si膜显示出增加的CO 2 / N 2选择性和CO 2渗透性，这表明这些膜对于气体分离如CO 2 / N 2分离是非常有希望的。
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公开(公告)号：US07637983B1
公开(公告)日：2009-12-29
申请号：US11427834
申请日：2006-06-30
IPC分类号： B01D53/22
CPC分类号： B01D53/228 , B01D53/02 , B01D67/0079 , B01D69/148 , B01D71/00 , B01D71/56 , B01D71/64 , B01D2253/204 , B01J20/22 , B01J20/226 , B01J20/26 , B01J20/28026 , B01J20/28033 , B01J20/2808 , B01J2220/44
摘要： Metal-organic framework (MOF)-polymer mixed matrix membranes (MOF-MMMs) have been prepared by dispersing high surface area MOFs (e.g. IRMOF-1) into a polymer matrix (e.g. Matrimid 5218). The MOFs allow the polymer to infiltrate the pores of the MOFs, which improves the interfacial and mechanical properties of the polymer and in turn affects permeability. Pure gas permeation tests show the incorporation of 20 wt-% of IRMOF-1 in Matrimid 5218 polyimide matrix results in 280% improvement in CO2 permeability without a loss of CO2/CH4 selectivity compared to those of the pure Matrimid 5218 membrane. This type of MOF-MMMs has significantly improved gas separation performance with dramatically high CO2 permeability (>35 barrer) and higher than 29 CO2/CH4 selectivity at 50° C. under 100 psig pressure, which are attractive candidates for practical gas separation applications such as CO2 removal from natural gas.
摘要翻译： 已经通过将高表面积MOF（例如IRMOF-1）分散到聚合物基质（例如Matrimid 5218）中制备了金属 - 有机骨架（MOF） - 聚合物混合基质膜（MOF-MMM）。 MOFs允许聚合物渗透MOFs的孔隙，这改善了聚合物的界面和机械性能，进而影响渗透性。 纯气体渗透测试显示，与Matrimid 5218聚酰亚胺基质相比，掺入20wt％的IRMOF-1导致CO 2渗透率提高280％，而与纯Matrimid 5218膜相比，CO 2 / CH 4选择性降低。 这种类型的MOF-MMM具有显着改善的气体分离性能，在100psig压力下，在50℃下具有显着高的CO 2渗透性（> 35巴勒）和高于29 CO 2 / CH 4选择性，这是实际气体分离应用的有吸引力的候选物 作为从天然气中去除二氧化碳。
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公开(公告)号：US20090155464A1
公开(公告)日：2009-06-18
申请号：US11954447
申请日：2007-12-12
申请人： Chunqing Liu , Stephen T. Wilson , David A. Lesch
发明人： Chunqing Liu , Stephen T. Wilson , David A. Lesch
IPC分类号： B05D5/00
CPC分类号： B01D69/148 , B01D67/0079 , B01D69/10 , B01D71/028 , B01D2325/022
摘要： The present invention discloses an approach for making mixed matrix membranes (MMMs) and methods for using these membranes. These MMMs contain a continuous polymer matrix and dispersed microporous molecular sieve particles. In particular, the present invention is directed to make asymmetric thin-film composite MMMs by coating a thin layer of molecular sieve/polymer mixed matrix solution on top of a porous support substrate followed by controlling the formation of a thin dense selective mixed matrix layer equal or larger in thickness than any of said molecular sieve particles. The MMMs of the present invention are suitable for a variety of liquid, gas, and vapor separations. The MMMs of the present invention have at least 20% increase in selectivity for these separations compared to the polymer membranes prepared from their corresponding continuous polymer matrices.
摘要翻译： 本发明公开了一种制备混合基质膜（MMM）的方法和使用这些膜的方法。 这些MMM含有连续的聚合物基质和分散的微孔分子筛颗粒。 特别地，本发明涉及通过在多孔载体基材的顶部涂覆分子筛/聚合物混合基质溶液的薄层，然后控制薄的致密选择性混合基质层的形成而形成不对称的薄膜复合MMM 或大于任何所述分子筛颗粒的厚度。 本发明的MMM适用于各种液体，气体和蒸气分离。 与从其相应的连续聚合物基质制备的聚合物膜相比，本发明的MMM对这些分离的选择性增加至少20％。
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10.发明申请公开(公告)号：US20090126566A1
公开(公告)日：2009-05-21
申请号：US11940549
申请日：2007-11-15
IPC分类号： B01D53/22
CPC分类号： B01D69/147 , B01D53/228 , B01D67/0046 , B01D69/141 , B01D71/028 , B01D2325/022
摘要： The invention discloses the use of polymer functionalized molecular sieve/polymer mixed matrix membranes (MMMs) with either no macrovoids or voids of less than several Angstroms at the interface of the polymer matrix and the molecular sieves by incorporating polyethersulfone (PES) or cellulose triacetate (CTA) functionalized molecular sieves into a continuous polyimide or cellulose acetate (CA) polymer matrix. The MMMs, particularly PES functionalized AlPO-14/polyimide MMMs and CTA functionalized AlPO-14/CA MMMs, in the form of symmetric dense film, asymmetric flat sheet membrane, or asymmetric hollow fiber have good flexibility and high mechanical strength, and exhibit significantly enhanced selectivity and/or permeability over the polymer membranes made from the corresponding continuous polymer matrices for carbon dioxide/methane (CO2/CH4), hydrogen/methane (H2/CH4), propylene/propane separations and a variety of liquid, gas, and vapor separations.
摘要翻译： 本发明公开了聚合物官能化分子筛/聚合物混合基质膜（MMM）在聚合物基体和分子筛的界面处没有大孔或小于几埃的空隙，通过引入聚醚砜（PES）或三乙酸纤维素 CTA）官能化分子筛成连续聚酰亚胺或乙酸纤维素（CA）聚合物基质。 对称致密膜，不对称平片膜或不对称中空纤维形式的MMMs，特别是PES官能化AlPO-14 /聚酰亚胺MMM和CTA官能化AlPO-14 / CA MMMs具有良好的柔韧性和高机械强度，并显示出显着的 由相应的二氧化碳/甲烷（CO 2 / CH 4），氢/甲烷（H 2 / CH 4），丙烯/丙烷分离和各种液体，气体和/或气体的连续聚合物基质制成的聚合物膜的选择性和/ 蒸气分离。
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