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Evaluation and Modification of 3-Component, Poly(Ionic Liquid)-Ionic Liquid-Zeolite Mixed-Matrix Membranes for CO2/CH4 Separations.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Evaluation and Modification of 3-Component, Poly(Ionic Liquid)-Ionic Liquid-Zeolite Mixed-Matrix Membranes for CO2/CH4 Separations./
Author:	Dunn, Collin Andrew.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2021,
Description:	211 p.
Notes:	Source: Dissertations Abstracts International, Volume: 82-11, Section: B.
Contained By:	Dissertations Abstracts International82-11B.
Subject:	Chemical engineering. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28415118
ISBN:	9798738628856

Evaluation and Modification of 3-Component, Poly(Ionic Liquid)-Ionic Liquid-Zeolite Mixed-Matrix Membranes for CO2/CH4 Separations.
Dunn, Collin Andrew.

Evaluation and Modification of 3-Component, Poly(Ionic Liquid)-Ionic Liquid-Zeolite Mixed-Matrix Membranes for CO2/CH4 Separations. - Ann Arbor : ProQuest Dissertations & Theses, 2021 - 211 p.

Source: Dissertations Abstracts International, Volume: 82-11, Section: B.

Thesis (Ph.D.)--University of Colorado at Boulder, 2021.

This item is not available from ProQuest Dissertations & Theses.

Polymer-based membranes can be employed to separate CO2 from CH4, which makes them useful for applications involving natural gas, but polymers suffer from an inherent trade-off between their CO2/CH4 selectivity and their CO2 permeability. Non-polymeric materials used as advanced sorbents do not have this issue, but they are difficult and expensive to form into membranes at commercial scale. It is possible to take advantage of their separation properties without making a neat membrane from them by dispersing them as small particles within a more easily processed polymer matrix to create a mixed-matrix membrane (MMM). However, MMMs are typically prone to interfacial issues between the components. The introduction of MMMs composed of polymerized ionic liquids (PILs), free ionic liquids (ILs), and zeolites led to some MMMs with the best combination of selectivity and permeability in literature. In this thesis, this three-component PIL-IL-zeolite MMM platform was tested under more realistic pipeline conditions and extensively modified by altering the PIL cross-linker loading, the type of zeolite used, the PIL cross-linking compound, and by replacing the starting IL monomer with a curable IL oligomer of controlled length.By evaluating the gas separation properties of this class of materials for the first time under binary CO2/CH4 feeds, high pressures, and elevated temperatures, insight into the effects of CO2 plasticization and competitive sorption were obtained. A new potential mode of defect formation was observed in MMMs incorporating the zeolite SSZ-13, and it was discovered that high temperatures have a strong, negative effect on CO2/CH4 selectivity in these MMMs. The need for more resilient systems was made apparent.Attempts were made to mitigate these selectivity losses by first increasing the amount of divinylbenzene (DVB) cross-linker ( a traditional commercial hydrocarbon cross-linker) in the PIL-IL-zeolite MMM films or replacing zeolite SSZ-13 with 4A. While these were simple modifications, they were ineffective in reducing the impact of CO2 pressure and heat on the gas separation performance. A more in-depth investigation based on introducing new cross-linking compounds (both commercially available and synthesized from literature) revealed that slight improvements in selectivity could be achieved by using cross-linkers with better inherent CO2 solubility such as those bearing ether groups or an ionic imidazolium group, and by using more highly functionalized cross-linkers. The replacement of the standard small-molecule IL monomer (which is polymerized to form the PIL matrix) for a curable IL oligomer of controlled length was found to afford casting solutions that soaked into support membranes less easily, opening the door to more traditional membrane processing for these materials. It was discovered that degree of polymerization of the curable IL oligomer greatly influences the gas separation properties of MMMs formed with them, and that they could be made to have similar ideal gas separation performances to MMMs prepared using IL-monomer-based analogues.In this thesis work, a more in-depth knowledge of MMM CO2/CH4 separation performance under adverse conditions was obtained. The effects of modifying PIL cross-linker loading and type, zeolite type, operating temperature and pressure, binary feed composition, and the PIL basis were explored and quantified. Issues in this class of membrane materials that must be addressed before commercialization were identified, and further experimental work is suggested.

ISBN: 9798738628856Subjects--Topical Terms:

560457
Chemical engineering.
Subjects--Index Terms:

CO2

Evaluation and Modification of 3-Component, Poly(Ionic Liquid)-Ionic Liquid-Zeolite Mixed-Matrix Membranes for CO2/CH4 Separations.
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506 $a This item must not be sold to any third party vendors.
520 $a Polymer-based membranes can be employed to separate CO2 from CH4, which makes them useful for applications involving natural gas, but polymers suffer from an inherent trade-off between their CO2/CH4 selectivity and their CO2 permeability. Non-polymeric materials used as advanced sorbents do not have this issue, but they are difficult and expensive to form into membranes at commercial scale. It is possible to take advantage of their separation properties without making a neat membrane from them by dispersing them as small particles within a more easily processed polymer matrix to create a mixed-matrix membrane (MMM). However, MMMs are typically prone to interfacial issues between the components. The introduction of MMMs composed of polymerized ionic liquids (PILs), free ionic liquids (ILs), and zeolites led to some MMMs with the best combination of selectivity and permeability in literature. In this thesis, this three-component PIL-IL-zeolite MMM platform was tested under more realistic pipeline conditions and extensively modified by altering the PIL cross-linker loading, the type of zeolite used, the PIL cross-linking compound, and by replacing the starting IL monomer with a curable IL oligomer of controlled length.By evaluating the gas separation properties of this class of materials for the first time under binary CO2/CH4 feeds, high pressures, and elevated temperatures, insight into the effects of CO2 plasticization and competitive sorption were obtained. A new potential mode of defect formation was observed in MMMs incorporating the zeolite SSZ-13, and it was discovered that high temperatures have a strong, negative effect on CO2/CH4 selectivity in these MMMs. The need for more resilient systems was made apparent.Attempts were made to mitigate these selectivity losses by first increasing the amount of divinylbenzene (DVB) cross-linker ( a traditional commercial hydrocarbon cross-linker) in the PIL-IL-zeolite MMM films or replacing zeolite SSZ-13 with 4A. While these were simple modifications, they were ineffective in reducing the impact of CO2 pressure and heat on the gas separation performance. A more in-depth investigation based on introducing new cross-linking compounds (both commercially available and synthesized from literature) revealed that slight improvements in selectivity could be achieved by using cross-linkers with better inherent CO2 solubility such as those bearing ether groups or an ionic imidazolium group, and by using more highly functionalized cross-linkers. The replacement of the standard small-molecule IL monomer (which is polymerized to form the PIL matrix) for a curable IL oligomer of controlled length was found to afford casting solutions that soaked into support membranes less easily, opening the door to more traditional membrane processing for these materials. It was discovered that degree of polymerization of the curable IL oligomer greatly influences the gas separation properties of MMMs formed with them, and that they could be made to have similar ideal gas separation performances to MMMs prepared using IL-monomer-based analogues.In this thesis work, a more in-depth knowledge of MMM CO2/CH4 separation performance under adverse conditions was obtained. The effects of modifying PIL cross-linker loading and type, zeolite type, operating temperature and pressure, binary feed composition, and the PIL basis were explored and quantified. Issues in this class of membrane materials that must be addressed before commercialization were identified, and further experimental work is suggested.
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