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  1. Article: Thermodynamic Evidence for Type II Porous Liquids.

    Borne, Isaiah / Saigal, Kartik / Jones, Christopher W / Lively, Ryan P

    Industrial & engineering chemistry research

    2023  Volume 62, Issue 29, Page(s) 11689–11696

    Abstract: Porous liquids are an emerging class of microporous materials where intrinsic, stable porosity is imbued in a liquid material. Many porous liquids are prepared by dispersing porous solids in bulky solvents; these can be contrasted by the method of ... ...

    Abstract Porous liquids are an emerging class of microporous materials where intrinsic, stable porosity is imbued in a liquid material. Many porous liquids are prepared by dispersing porous solids in bulky solvents; these can be contrasted by the method of dissolving microporous molecules. We highlight the latter "Type II" porous liquids-which are stable thermodynamic solutions with demonstrable colligative properties. This feature significantly impacts the ultimate utility of the liquid for various end-use applications. We also describe a facile method for determining if a Type II porous liquid candidate is "porous" based on assessing the partial molar volume of the porous host molecule dissolved in the solvent by measuring the densities of candidate solutions. Conventional CO
    Language English
    Publishing date 2023-07-11
    Publishing country United States
    Document type Journal Article
    ZDB-ID 1484436-9
    ISSN 1520-5045 ; 0888-5885
    ISSN (online) 1520-5045
    ISSN 0888-5885
    DOI 10.1021/acs.iecr.3c01201
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: Design of Gas Separation Processes Using Type II Porous Liquids as Physical Solvents

    Borne, Isaiah / Simon, Natalie / Jones, Christopher W. / Lively, Ryan P.

    Industrial & engineering chemistry process design and development. 2022 Aug. 04, v. 61, no. 32

    2022  

    Abstract: Solvent-based absorption systems are frequently used for industrial-scale CO₂ capture from point sources. Physical and chemical solvents are well understood; however, there are drawbacks such as low gas capacity, high regeneration energy, and large ... ...

    Abstract Solvent-based absorption systems are frequently used for industrial-scale CO₂ capture from point sources. Physical and chemical solvents are well understood; however, there are drawbacks such as low gas capacity, high regeneration energy, and large operating units. Porous liquids (liquids with intrinsic microporosity) present an opportunity to improve the effectiveness of solvent-based separation processes, especially physisorption-based systems. Type II porous liquids are developed by dissolving a discrete, microporous material in a sterically hindered solvent that cannot penetrate the pores of the porous material. These liquids exhibit dual-mode sorption (i.e., Henry + Langmuir) and show excellent potential for gas separations. In this work, a first-order high-pressure CO₂/CH₄ separation process is modeled using a porous liquid comprised of a discrete porous material dissolved in a sterically hindered solvent. Gas–liquid phase equilibria of the porous liquids are modeled using gas-cage equilibrium data. A McCabe–Thiele approach is employed to estimate the amount of solvent and size of the absorption tower needed compared to an industrial solvent, revealing that porous liquids can decrease the capital needed to adequately separate a gaseous mixture. The energy requirements for a variety of regeneration scenarios are calculated, highlighting that porous liquids can lower the energy burden necessary for gas separation processes. The porous liquid shows the potential to significantly reduce the solvent consumption and size of operating units for this gas separation, with the potential to lower the overall cost and energy required to capture CO₂.
    Keywords absorption ; capital ; carbon dioxide ; energy ; liquids ; porous media ; process design ; solvents
    Language English
    Dates of publication 2022-0804
    Size p. 11908-11921.
    Publishing place American Chemical Society
    Document type Article
    ZDB-ID 1484436-9
    ISSN 1520-5045 ; 0888-5885
    ISSN (online) 1520-5045
    ISSN 0888-5885
    DOI 10.1021/acs.iecr.2c01943
    Database NAL-Catalogue (AGRICOLA)

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  3. Article ; Online: Accelerating Solvent Selection for Type II Porous Liquids.

    Chang, Chao-Wen / Borne, Isaiah / Lawler, Robin M / Yu, Zhenzi / Jang, Seung Soon / Lively, Ryan P / Sholl, David S

    Journal of the American Chemical Society

    2022  Volume 144, Issue 9, Page(s) 4071–4079

    Abstract: Type II porous liquids, comprising intrinsically porous molecules dissolved in a liquid solvent, potentially combine the adsorption properties of porous adsorbents with the handling advantages of liquids. Previously, discovery of appropriate solvents to ... ...

    Abstract Type II porous liquids, comprising intrinsically porous molecules dissolved in a liquid solvent, potentially combine the adsorption properties of porous adsorbents with the handling advantages of liquids. Previously, discovery of appropriate solvents to make porous liquids had been limited to direct experimental tests. We demonstrate an efficient screening approach for this task that uses COSMO-RS calculations, predictions of solvent p
    MeSH term(s) Porosity ; Solubility ; Solvents
    Chemical Substances Solvents
    Language English
    Publishing date 2022-02-16
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c13049
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article: Accelerating Solvent Selection for Type II Porous Liquids

    Chang, Chao-Wen / Borne, Isaiah / Lawler, Robin M. / Yu, Zhenzi / Jang, Seung Soon / Lively, Ryan P. / Sholl, David S.

    Journal of the American Chemical Society. 2022 Feb. 16, v. 144, no. 9

    2022  

    Abstract: Type II porous liquids, comprising intrinsically porous molecules dissolved in a liquid solvent, potentially combine the adsorption properties of porous adsorbents with the handling advantages of liquids. Previously, discovery of appropriate solvents to ... ...

    Abstract Type II porous liquids, comprising intrinsically porous molecules dissolved in a liquid solvent, potentially combine the adsorption properties of porous adsorbents with the handling advantages of liquids. Previously, discovery of appropriate solvents to make porous liquids had been limited to direct experimental tests. We demonstrate an efficient screening approach for this task that uses COSMO-RS calculations, predictions of solvent pKₐ values from a machine-learning model, and several other features and apply this approach to select solvents from a library of more than 11,000 compounds. This method is shown to give qualitative agreement with experimental observations for two molecular cages, CC13 and TG-TFB-CHEDA, identifying solvents with higher solubility for these molecules than had previously been known. Ultimately, the algorithm streamlines the downselection of suitable solvents for porous organic cages to enable more rapid discovery of Type II porous liquids.
    Keywords adsorbents ; adsorption ; algorithms ; artificial intelligence ; liquids ; models ; solubility ; solvents
    Language English
    Dates of publication 2022-0216
    Size p. 4071-4079.
    Publishing place American Chemical Society
    Document type Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c13049
    Database NAL-Catalogue (AGRICOLA)

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  5. Article ; Online: Polymeric Fiber Sorbents Embedded with Porous Organic Cages.

    Borne, Isaiah / He, Donglin / DeWitt, Stephen J A / Liu, Ming / Cooper, Andrew I / Jones, Christopher W / Lively, Ryan P

    ACS applied materials & interfaces

    2021  Volume 13, Issue 39, Page(s) 47118–47126

    Abstract: The synthesis and functionalization of porous organic cages (POCs) for separation have attracted growing interest over the past decade. However, the potential of solid-phase POCs for practical, large-scale separations will require incorporation into ... ...

    Abstract The synthesis and functionalization of porous organic cages (POCs) for separation have attracted growing interest over the past decade. However, the potential of solid-phase POCs for practical, large-scale separations will require incorporation into appropriate gas-solid or liquid-solid contactors. Contactors with more effective mass transfer properties and lower pressure drops than pelletized systems are preferred. Here, we prepared and characterized fiber sorbents with POCs throughout a cellulose acetate (CA) polymer matrix, which were then deployed in model separations. The POC CC3 was shown to be stable after exposure to spinning solvents, as confirmed by NMR, powder X-ray diffraction, and gas sorption experiments. CC3-CA fibers were spun using the dry-jet wet-quench spinning method. Spun fibers retained the adsorptive properties of CC3 powders, as confirmed by CO
    Language English
    Publishing date 2021-09-27
    Publishing country United States
    Document type Journal Article
    ISSN 1944-8252
    ISSN (online) 1944-8252
    DOI 10.1021/acsami.1c12002
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article: Polymeric Fiber Sorbents Embedded with Porous Organic Cages

    Borne, Isaiah / He, Donglin / DeWitt, Stephen J. A. / Liu, Ming / Cooper, Andrew I. / Jones, Christopher W. / Lively, Ryan P.

    ACS applied materials & interfaces. 2021 Sept. 27, v. 13, no. 39

    2021  

    Abstract: The synthesis and functionalization of porous organic cages (POCs) for separation have attracted growing interest over the past decade. However, the potential of solid-phase POCs for practical, large-scale separations will require incorporation into ... ...

    Abstract The synthesis and functionalization of porous organic cages (POCs) for separation have attracted growing interest over the past decade. However, the potential of solid-phase POCs for practical, large-scale separations will require incorporation into appropriate gas–solid or liquid–solid contactors. Contactors with more effective mass transfer properties and lower pressure drops than pelletized systems are preferred. Here, we prepared and characterized fiber sorbents with POCs throughout a cellulose acetate (CA) polymer matrix, which were then deployed in model separations. The POC CC3 was shown to be stable after exposure to spinning solvents, as confirmed by NMR, powder X-ray diffraction, and gas sorption experiments. CC3-CA fibers were spun using the dry-jet wet-quench spinning method. Spun fibers retained the adsorptive properties of CC3 powders, as confirmed by CO₂ and N₂ physisorption and TGA, reaching upward of 60 wt % adsorbent loading, whereas the pelletized CC3 counterparts suffered significant losses in textural properties. The separation capabilities of the CC3-CA fibers are tested with both simulated postcombustion flue gas and with Xe/Kr mixtures. Fixed bed breakthrough experiments performed on fibers samples show that CC3 embedded in polymeric fibers can effectively perform these proof-of-concept gas separations. The development of fiber sorbents embedded with POCs provides an alternative to traditional pelletization for the incorporation of these materials into adsorptive separation systems.
    Keywords X-ray diffraction ; adsorbents ; carbon dioxide ; cellulose acetate ; flue gas ; mass transfer ; pelleting ; pellets ; polymers ; sorption
    Language English
    Dates of publication 2021-0927
    Size p. 47118-47126.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1944-8252
    DOI 10.1021/acsami.1c12002
    Database NAL-Catalogue (AGRICOLA)

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