Physical Aging, Plasticization and Their Effects on Gas Permeation in “Rigid” Polymers of Intrinsic Microporosity
Long-term physical aging and plasticization, two mobility-based phenomena that are counterintuitive in the context of “rigid” polymers of intrinsic microporosity (PIMs), were evaluated using pure- and mixed-gas permeation data for representative ladder and semiladder PIMs. PIMs between 1 and 4 years...
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| Published in | Macromolecules Vol. 48; no. 18; pp. 6553 - 6561 |
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| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
22.09.2015
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Long-term physical aging and plasticization, two mobility-based phenomena that are counterintuitive in the context of “rigid” polymers of intrinsic microporosity (PIMs), were evaluated using pure- and mixed-gas permeation data for representative ladder and semiladder PIMs. PIMs between 1 and 4 years old retained from 10- to 1000-fold higher H2 and O2 permeabilities than commercial membrane materials with similar or higher selectivities. A triptycene-based ladder polymer (TPIM-1) exhibited very large selectivity gains outweighing permeability losses after 780 days, resulting in unprecedented performance for O2/N2 (P(O2) = 61 Barrer, α(O2/N2) = 8.6) and H2/N2 (P(H2) = 1105 Barrer, α(H2/N2) = 156) separations. Interestingly, TPIM-1 aged more and faster than its more flexible counterpart, PIM-1, which exhibited P(O2) = 317 Barrer and α(O2/N2) = 5.0 at 1380 days. Additionally, the more “rigid” TPIM-1 plasticized more significantly than PIM-1 (i.e., TPIM-1 endured ∼93% increases in mixed-gas CH4 permeability over pure-gas values compared to ∼60% for PIM-1). A flexible 9,10-bridgehead (i.e., TPIM-2) mitigated the enhancements induced by physical aging but reduced plasticization. Importantly, intra-chain rigidity alone, without consideration of chain architecture and ultra-microporosity, is insufficient for designing aging- and plasticization-resistant gas separation membranes with high permeability and high selectivity |
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| AbstractList | Long-term physical aging and plasticization, two mobility-based phenomena that are counterintuitive in the context of “rigid” polymers of intrinsic microporosity (PIMs), were evaluated using pure- and mixed-gas permeation data for representative ladder and semiladder PIMs. PIMs between 1 and 4 years old retained from 10- to 1000-fold higher H2 and O2 permeabilities than commercial membrane materials with similar or higher selectivities. A triptycene-based ladder polymer (TPIM-1) exhibited very large selectivity gains outweighing permeability losses after 780 days, resulting in unprecedented performance for O2/N2 (P(O2) = 61 Barrer, α(O2/N2) = 8.6) and H2/N2 (P(H2) = 1105 Barrer, α(H2/N2) = 156) separations. Interestingly, TPIM-1 aged more and faster than its more flexible counterpart, PIM-1, which exhibited P(O2) = 317 Barrer and α(O2/N2) = 5.0 at 1380 days. Additionally, the more “rigid” TPIM-1 plasticized more significantly than PIM-1 (i.e., TPIM-1 endured ∼93% increases in mixed-gas CH4 permeability over pure-gas values compared to ∼60% for PIM-1). A flexible 9,10-bridgehead (i.e., TPIM-2) mitigated the enhancements induced by physical aging but reduced plasticization. Importantly, intra-chain rigidity alone, without consideration of chain architecture and ultra-microporosity, is insufficient for designing aging- and plasticization-resistant gas separation membranes with high permeability and high selectivity Long-term physical aging and plasticization, two mobility-based phenomena that are counterintuitive in the context of “rigid” polymers of intrinsic microporosity (PIMs), were evaluated using pure- and mixed-gas permeation data for representative ladder and semiladder PIMs. PIMs between 1 and 4 years old retained from 10- to 1000-fold higher H₂ and O₂ permeabilities than commercial membrane materials with similar or higher selectivities. A triptycene-based ladder polymer (TPIM-1) exhibited very large selectivity gains outweighing permeability losses after 780 days, resulting in unprecedented performance for O₂/N₂ (P(O₂) = 61 Barrer, α(O₂/N₂) = 8.6) and H₂/N₂ (P(H₂) = 1105 Barrer, α(H₂/N₂) = 156) separations. Interestingly, TPIM-1 aged more and faster than its more flexible counterpart, PIM-1, which exhibited P(O₂) = 317 Barrer and α(O₂/N₂) = 5.0 at 1380 days. Additionally, the more “rigid” TPIM-1 plasticized more significantly than PIM-1 (i.e., TPIM-1 endured ∼93% increases in mixed-gas CH₄ permeability over pure-gas values compared to ∼60% for PIM-1). A flexible 9,10-bridgehead (i.e., TPIM-2) mitigated the enhancements induced by physical aging but reduced plasticization. Importantly, intra-chain rigidity alone, without consideration of chain architecture and ultra-microporosity, is insufficient for designing aging- and plasticization-resistant gas separation membranes with high permeability and high selectivity |
| Author | Swaidan, Raja Pinnau, Ingo Ghanem, Bader Litwiller, Eric |
| AuthorAffiliation | Advanced Membranes and Porous Materials Center (AMPMC), Physical Sciences and Engineering Division King Abdullah University of Science and Technology (KAUST) |
| AuthorAffiliation_xml | – name: Advanced Membranes and Porous Materials Center (AMPMC), Physical Sciences and Engineering Division – name: King Abdullah University of Science and Technology (KAUST) |
| Author_xml | – sequence: 1 givenname: Raja surname: Swaidan fullname: Swaidan, Raja – sequence: 2 givenname: Bader surname: Ghanem fullname: Ghanem, Bader – sequence: 3 givenname: Eric surname: Litwiller fullname: Litwiller, Eric – sequence: 4 givenname: Ingo surname: Pinnau fullname: Pinnau, Ingo email: ingo.pinnau@kaust.edu.sa |
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| Snippet | Long-term physical aging and plasticization, two mobility-based phenomena that are counterintuitive in the context of “rigid” polymers of intrinsic... |
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| SubjectTerms | hydrogen methane oxygen permeability polymers |
| Title | Physical Aging, Plasticization and Their Effects on Gas Permeation in “Rigid” Polymers of Intrinsic Microporosity |
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