Ethylene/ethane permeation, diffusion and gas sorption properties of carbon molecular sieve membranes derived from the prototype ladder polymer of intrinsic microporosity (PIM-1)
Fine-tuning the microporosity of PIM-1 by heat treatment was applied to develop a suitable carbon molecular sieve membrane for ethylene/ethane separation. Pristine PIM-1 films were heated from 400 to 800°C under inert N2 atmosphere (<2ppm O2). At 400°C, PIM-1 self-cross-linked and developed polar...
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| Published in | Journal of membrane science Vol. 504; pp. 133 - 140 |
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| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier B.V
15.04.2016
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Fine-tuning the microporosity of PIM-1 by heat treatment was applied to develop a suitable carbon molecular sieve membrane for ethylene/ethane separation. Pristine PIM-1 films were heated from 400 to 800°C under inert N2 atmosphere (<2ppm O2). At 400°C, PIM-1 self-cross-linked and developed polar carbonyl and hydroxyl groups due to partial dioxane splitting in the polymer backbone. Significant degradation occurred at 600°C due to carbonization of PIM-1 and resulted in 30% increase in cumulative surface area compared to its cross-linked predecessor. In addition, PIM-1-based CMS developed smaller ultramicropores with increasing pyrolysis temperature, which enhanced their molecular sieving capability by restricted diffusion of ethylene and ethane through the matrix due to microstructural carbon densification. Consequently, the pure-gas ethylene permeability (measured at 35°C and 2bar) decreased from 1600Barrer for the pristine PIM-1 to 1.3Barrer for the amorphous carbon generated at 800°C, whereas the ethylene/ethane pure-gas selectivity increased significantly from 1.8 to 13.
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•First report of ladder PIM-1-derived CMS membranes for ethylene/ethane separation.•PIM-1-derived CMS (pyrolized at 800°C) shows high pure-gas selectivity (αC2H4/C2H6~13).•Ethylene/ethane permselectivity of the CMS membrane is dominated by diffusivity selectivity.•Intrinsic polymer precursor microporosity appears to have influence on CMS gas permeability. |
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| AbstractList | Fine-tuning the microporosity of PIM-1 by heat treatment was applied to develop a suitable carbon molecular sieve membrane for ethylene/ethane separation. Pristine PIM-1 films were heated from 400 to 800 degree C under inert N sub(2) atmosphere (<2 ppm O sub(2)). At 400 degree C, PIM-1 self-cross-linked and developed polar carbonyl and hydroxyl groups due to partial dioxane splitting in the polymer backbone. Significant degradation occurred at 600 degree C due to carbonization of PIM-1 and resulted in 30% increase in cumulative surface area compared to its cross-linked predecessor. In addition, PIM-1-based CMS developed smaller ultramicropores with increasing pyrolysis temperature, which enhanced their molecular sieving capability by restricted diffusion of ethylene and ethane through the matrix due to microstructural carbon densification. Consequently, the pure-gas ethylene permeability (measured at 35 degree C and 2 bar) decreased from 1600 Barrer for the pristine PIM-1 to 1.3 Barrer for the amorphous carbon generated at 800 degree C, whereas the ethylene/ethane pure-gas selectivity increased significantly from 1.8 to 13. Fine-tuning the microporosity of PIM-1 by heat treatment was applied to develop a suitable carbon molecular sieve membrane for ethylene/ethane separation. Pristine PIM-1 films were heated from 400 to 800°C under inert N2 atmosphere (<2ppm O2). At 400°C, PIM-1 self-cross-linked and developed polar carbonyl and hydroxyl groups due to partial dioxane splitting in the polymer backbone. Significant degradation occurred at 600°C due to carbonization of PIM-1 and resulted in 30% increase in cumulative surface area compared to its cross-linked predecessor. In addition, PIM-1-based CMS developed smaller ultramicropores with increasing pyrolysis temperature, which enhanced their molecular sieving capability by restricted diffusion of ethylene and ethane through the matrix due to microstructural carbon densification. Consequently, the pure-gas ethylene permeability (measured at 35°C and 2bar) decreased from 1600Barrer for the pristine PIM-1 to 1.3Barrer for the amorphous carbon generated at 800°C, whereas the ethylene/ethane pure-gas selectivity increased significantly from 1.8 to 13. [Display omitted] •First report of ladder PIM-1-derived CMS membranes for ethylene/ethane separation.•PIM-1-derived CMS (pyrolized at 800°C) shows high pure-gas selectivity (αC2H4/C2H6~13).•Ethylene/ethane permselectivity of the CMS membrane is dominated by diffusivity selectivity.•Intrinsic polymer precursor microporosity appears to have influence on CMS gas permeability. Fine-tuning the microporosity of PIM-1 by heat treatment was applied to develop a suitable carbon molecular sieve membrane for ethylene/ethane separation. Pristine PIM-1 films were heated from 400 to 800°C under inert N2 atmosphere (<2ppm O2). At 400°C, PIM-1 self-cross-linked and developed polar carbonyl and hydroxyl groups due to partial dioxane splitting in the polymer backbone. Significant degradation occurred at 600°C due to carbonization of PIM-1 and resulted in 30% increase in cumulative surface area compared to its cross-linked predecessor. In addition, PIM-1-based CMS developed smaller ultramicropores with increasing pyrolysis temperature, which enhanced their molecular sieving capability by restricted diffusion of ethylene and ethane through the matrix due to microstructural carbon densification. Consequently, the pure-gas ethylene permeability (measured at 35°C and 2bar) decreased from 1600Barrer for the pristine PIM-1 to 1.3Barrer for the amorphous carbon generated at 800°C, whereas the ethylene/ethane pure-gas selectivity increased significantly from 1.8 to 13. |
| Author | Pinnau, Ingo Litwiller, Eric Salinas, Octavio Ma, Xiaohua |
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| SubjectTerms | artificial membranes Carbon Carbon molecular sieve carbonization crosslinking Diffusion dioxane Ethane Ethylene Ethylene/ethane separation heat treatment Hydroxyl groups Intrinsically microporous polymer Membranes Microporosity moieties Molecular sieves oxygen permeability PIM-1 polymers prototypes pyrolysis sieving sorption surface area temperature |
| Title | Ethylene/ethane permeation, diffusion and gas sorption properties of carbon molecular sieve membranes derived from the prototype ladder polymer of intrinsic microporosity (PIM-1) |
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