Improving Gas Selectivity in Membranes Using Polymer-Grafted Silica Nanoparticles

Jeong, Seung Pyo; Kumar, Rajeev; Genix, Anne-Caroline; Popov, Ivan; Li, Congyi; Mahurin, Shannon M.; Hu, Xunxiang; Bras, Wim; Popovs, Ilja; Sokolov, Alexei P.; Bocharova, Vera

doi:10.1021/acsanm.1c00803

Title: Improving Gas Selectivity in Membranes Using Polymer-Grafted Silica Nanoparticles

Journal Article · Thu Jun 10 00:00:00 EDT 2021 · ACS Applied Nano Materials

DOI:https://doi.org/10.1021/acsanm.1c00803· OSTI ID:1833971

Jeong, Seung Pyo ^[1];

^[1]; Genix, Anne-Caroline ^[2];

^[1]; Li, Congyi ^[1]; Mahurin, Shannon M. ^[1];

^[1];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. de Montpellier (France). Lab. Charles Coulomb

Herein, we demonstrate that tuning of structural parameters and material chemistry enables control of the permeability and selectivity of gases (CO₂, He, and CH₄) in membranes based on poly(butyl methacrylate)-grafted nanoparticles (PGNs). Our data show that the presence of nanoparticles and the overall dense packing of grafted chains noticeable in PGNs with low grafting density have an adverse effect on the diffusivity of gases. This effect is compensated by an improvement in the solubility of CO₂ gas promoted by the silica nanoparticle surface, yielding a substantial improvement in the permeability of CO₂ versus CH₄. Furthermore, in membranes with high grafting density, changes in the structural arrangements and alterations in the membrane porosity, evident from small-angle X-ray scattering and positron annihilation lifetime spectroscopy, positively influence the permeability of He and CO₂ gases. In contrast, CH₄ permeability in the same membranes is significantly suppressed, suggesting the formation of a unique, highly selective environment for gas separation. As a result, an improvement of up to 50% in selectivity for gas pairs containing large CH₄ molecules is observed. Our studies provide fundamental insights into the role that structural parameters play in gas transport through polymer membranes, laying a foundation for the rational design of membranes with improved permeability and selectivity.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1833971

Journal Information:: ACS Applied Nano Materials, Vol. 4, Issue 6; ISSN 2574-0970

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Improving Gas Selectivity in Membranes Using Polymer-Grafted Silica Nanoparticles

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