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Physical Aging Investigations of a Spirobisindane-Locked Polymer of Intrinsic Microporosity AITranslate

Min Liu; Xinxin Lu; Mitchell D. Nothling; Cara M. Doherty; Lianhai Zu; Judy N. Hart; Paul A. Webley; Jianyong Jin; Qiang Fu; Greg G. Qiao;
The University of Melbourne; University of New South Wales Sydney; The University of Melbourne;Commonwealth Scientific and Industrial Research Organization (CSIRO); The University of Melbourne; University of New South Wales Sydney; The University of Melbourne; The University of Auckland; University of Technology Sydney; The University of Melbourne
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Publisher: ACS
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Abstract AITranslate

Polymers of intrinsic microporosity (PIMs) have exceptional gas separation performance for a broad range of applications. However, PIMs are highly susceptible to physical aging, which drastically reduces their long-term performance over time. In this work, we leverage complementary experimental and density functional theory (DFT) studies to decipher the inter-/intrachain changes that occur during aging of the prototypical PIM-1 and its rigidified analogue PIM-C1. By elucidating this hereto unexplored aging behavior, we reveal that the dramatic decrease in gas permeability of PIM materials during aging stems from a loss of fractional free volume (FFV) due to PIM chain relaxations induced by π–π interactions, hydrogen bonding, or van der Waals’ forces. While the PIM-1 based membranes displayed enhanced gas pair selectivities after aging, the PIM-C1 based membranes showed an opposite trend with unexpected reductions for CO2/N2 and CO2/CH4. This is due to the reductions in CO2/N2 and CO2/CH4 solubility (S) selectivities and, unlike PIM-1, the spirobisindane locked PIM-C1 (i.e., maintenance of micropore sizes) has a stable diffusivity (D) selectivities that cannot offset such reductions. These fundamental insights into the intrinsic relaxation of different PIM polymer chains during physical aging can guide the future design of high-performance PIM materials with enhanced anti-aging properties.

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DOI：https://doi.org/10.1021/acsmaterialslett.0c00184

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Citation Information:

Polymers of intrinsic microporosity (PIMs) have exceptional gas separation performance for a broad range of applications. However, PIMs are highly susceptible to physical aging, which drastically reduces their long-term performance over time. In this work, we leverage complementary experimental and density functional theory (DFT) studies to decipher the inter-/intrachain changes that occur during aging of the prototypical PIM-1 and its rigidified analogue PIM-C1. By elucidating this hereto unexplored aging behavior, we reveal that the dramatic decrease in gas permeability of PIM materials during aging stems from a loss of fractional free volume (FFV) due to PIM chain relaxations induced by π–π interactions, hydrogen bonding, or van der Waals’ forces. While the PIM-1 based membranes displayed enhanced gas pair selectivities after aging, the PIM-C1 based membranes showed an opposite trend with unexpected reductions for CO2/N2 and CO2/CH4. This is due to the reductions in CO2/N2 and CO2/CH4 solubility (S) selectivities and, unlike PIM-1, the spirobisindane locked PIM-C1 (i.e., maintenance of micropore sizes) has a stable diffusivity (D) selectivities that cannot offset such reductions. These fundamental insights into the intrinsic relaxation of different PIM polymer chains during physical aging can guide the future design of high-performance PIM materials with enhanced anti-aging properties.

quote

GB/T 7714-2015 [1] Min Liu, Xinxin Lu, Mitchell D. Nothling, et al. ACS Materials Letters, 2020(2). DOI:10.1021/acsmaterialslett.0c00184.
MLA [1] Min Liu, et al., ACS Materials Letters, no. 2, 2020, https://doi.org/10.1021/acsmaterialslett.0c00184.
APA [1] Min Liu, Xinxin Lu, Mitchell D. Nothling, Cara M. Doherty, Lianhai Zu, Judy N. Hart, Paul A. Webley, Jianyong Jin, Qiang Fu, & Greg G. Qiao. (2020). ACS Materials Letters(2). https://doi.org/10.1021/acsmaterialslett.0c00184
IEEE [1] Min Liu, Xinxin Lu, Mitchell D. Nothling, Cara M. Doherty, Lianhai Zu, Judy N. Hart, Paul A. Webley, Jianyong Jin, Qiang Fu, and Greg G. Qiao, ACS Materials Letters, no. 2, 2020, doi: 10.1021/acsmaterialslett.0c00184.