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    CO2/CH4 Pure- and Mixed-Gas Dilation and Sorption in Thin (∼500 nm) and Ultrathin (∼50 nm) Polymers of Intrinsic Microporosity

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    Name:
    Macromolecules. IP.CTA-PIM1-PTMPS-thinfilm_manuscript_revised (1).pdf
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    Description:
    Accepted manuscript
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    Type
    Article
    Authors
    Ogieglo, Wojciech cc
    Genduso, Giuseppe cc
    Rubner, Jens
    Hofmann-Préveraud de Vaumas, Jacques
    Wessling, Matthias
    Pinnau, Ingo cc
    KAUST Department
    Advanced Membranes and Porous Materials Research Center
    Physical Science and Engineering (PSE) Division
    Chemical Engineering Program
    KAUST Grant Number
    BAS/1/1323-01-01
    Date
    2020-09-23
    Online Publication Date
    2020-09-23
    Print Publication Date
    2020-10-27
    Embargo End Date
    2021-09-23
    Submitted Date
    2020-05-17
    Permanent link to this record
    http://hdl.handle.net/10754/665324
    
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    Abstract
    In this work, we present (i) the dilation and refractive index variation associated with changes in film density and (ii) gas uptake of pure CO2 and CH4, as well as their equimolar mixture in thin films of two polymers of intrinsic microporosity (PIMs), that is, PIM-1 and poly(trimethylsilyl)propyne (PTMSP). A conventional low-free-volume glassy polymer, cellulose triacetate, was also investigated as the reference material. All experiments were performed with ∼50 and ∼500 nm-thick films up to partial pressures of 25 bar using in situ interference-enhanced spectroscopic ellipsometry. In all cases, film thickness reduction promoted the collapse of the frozen-in free volume. Particularly for thin PIM-1 and PTMSP films, the CO2 and CH4 pure-gas uptakes were generally lower than in bulk samples. In the most extreme case of the ultrathin ∼50 nm PTMSP film, we could detect a strikingly similar qualitative behavior to the penetrant partial molar volume and dilation in rubbery polymers. Remarkably, in PIM-1, the collapse of the frozen-in free volume seemed to be opposed by its ultra-micropores (<7 Å), which was not the case in PTMSP with larger micropores (>10 Å). In mixed-gas experiments, the refractive index response of all investigated films closely followed the trend observed during CO2 pure-gas sorption. In both thickness ranges and throughout the entire pressure range, the samples dilated less in the multicomponent environment than under the corresponding ideal pure-gas conditions. We found this phenomenon consistent with the pure- and mixed-gas uptake behavior of PIM-1 and PTMSP bulk films reported in the literature.
    Citation
    Ogieglo, W., Genduso, G., Rubner, J., Hofmann-Préveraud de Vaumas, J., Wessling, M., & Pinnau, I. (2020). CO2/CH4 Pure- and Mixed-Gas Dilation and Sorption in Thin (∼500 nm) and Ultrathin (∼50 nm) Polymers of Intrinsic Microporosity. Macromolecules. doi:10.1021/acs.macromol.0c01163
    Sponsors
    This work was supported by funding (BAS/1/1323-01-01) from King Abdullah University of Science and Technology (KAUST).
    Publisher
    American Chemical Society (ACS)
    Journal
    Macromolecules
    DOI
    10.1021/acs.macromol.0c01163
    Additional Links
    https://pubs.acs.org/doi/10.1021/acs.macromol.0c01163
    ae974a485f413a2113503eed53cd6c53
    10.1021/acs.macromol.0c01163
    Scopus Count
    Collections
    Articles; Advanced Membranes and Porous Materials Research Center; Physical Science and Engineering (PSE) Division; Chemical Engineering Program

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