Natural gas purification and olefin/paraffin separation using thermal cross-linkable co-polyimide/ZIF-8 mixed matrix membranes

Using three 6FDA-based polyimides (6FDA-Durene, 6FDA-Durene/DABA (9/1), 6FDA-Durene/DABA (7/3)) and nano-size zeolitic imidazolate framework-8 (ZIF-8), we have fabricated mixed matrix membranes (MMMs) with uniform morphology comprising ZIF-8as high as 40wt% loading by directly mixing as-synthesized...

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Published inJournal of membrane science Vol. 444; pp. 173 - 183
Main Authors Askari, Mohammad, Chung, Tai-Shung
Format Journal Article
LanguageEnglish
Published Amsterdam Elsevier B.V 01.10.2013
Elsevier
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Abstract Using three 6FDA-based polyimides (6FDA-Durene, 6FDA-Durene/DABA (9/1), 6FDA-Durene/DABA (7/3)) and nano-size zeolitic imidazolate framework-8 (ZIF-8), we have fabricated mixed matrix membranes (MMMs) with uniform morphology comprising ZIF-8as high as 40wt% loading by directly mixing as-synthesized ZIF-8 suspension into the polymer solution. Permeability of all gases (CO2, CH4, C3H6, and C3H8) increases rapidly with an increase in ZIF-8 loading. However, the addition of ZIF-8 nano-particles into the polymer matrix increases the ideal CO2/CH4 selectivity of only 6.87%, while the ideal C3H6/C3H8 selectivity improves 134% from 11.68 to 27.38 for the MMM made of 6FDA-Durene/DABA (9/1) and 40wt% ZIF-8. Experimental data show that the plasticization resistance and gas pair selectivity of MMMs are strongly dependent on the amount of cross-linkable moiety and annealing temperature. MMMs made of 6FDA-Durene do not show considerable improvements on resistance against CO2-induced plasticization after annealing at 200–400°C, while MMMs synthesized from cross-linkable co-polyimides (6FDA-Durene/DABA (9/1) and 6FDA-Durene/DABA (7/3)) show significant enhancements in CO2/CH4 and C3H6/C3H8 selectivity as well as plasticization suppression characteristics up to a CO2 pressure of 30atm after annealing at 400°C due to the cross-linking reaction of the carboxyl acid (COOH) in the DABA moiety. The MMM made of 6FDA-Durene/DABA (9/1) and 40wt% ZIF-8 possess a notable ideal C3H6/C3H8 selectivity of 27.38 and a remarkable C3H6 permeability of 47.3 Barrer. After thermally annealed at 400°C, the MMM made of 6FDA-Durene/DABA (9/1) and 20wt% ZIF-8 shows a CO2/CH4 selectivity of 19.61 and an impressive CO2 permeability 728 Barrer in mixed gas tests. The newly developed MMMs may have great potential for industrial nature gas purification and C3H6/C3H8 separation. [Display omitted] •Cross-linkable co-polyimide/ZIF-8 mixed matrix membranes (MMMs) are fabricated.•Effects of diamine ratio on polymer structure and gas separation performance are studied.•Effect of heat treatment temperature on MMM performance is investigated.•Increasing ZIF-8 loading leads to increase MMM permeability for all gasses.•Cross-linkable co-polyimides thermally treated at 400°C have shown selectivity enhancement.
AbstractList Using three 6FDA-based polyimides (6FDA-Durene, 6FDA-Durene/DABA (9/1), 6FDA-Durene/DABA (7/3)) and nano-size zeolitic imidazolate framework-8 (ZIF-8), we have fabricated mixed matrix membranes (MMMs) with uniform morphology comprising ZIF-8 as high as 40 wt% loading by directly mixing as-synthesized ZIF-8 suspension into the polymer solution. Permeability of all gases (CO2, CH4, C3H6, and C3H8) increases rapidly with an increase in ZIF-8 loading. However, the addition of ZIF-8 nano-particles into the polymer matrix increases the ideal CO2/CH4 selectivity of only 6.87%, while the ideal C3H6/C3H8 selectivity improves 134% from 11.68 to 27.38 for the MMM made of 6FDA-Durene/DABA (9/1) and 40 wt% ZIF-8. Experimental data show that the plasticization resistance and gas pair selectivity of MMMs are strongly dependent on the amount of cross-linkable moiety and annealing temperature. MMMs made of 6FDA-Durene do not show considerable improvements on resistance against CO2-induced plasticization after annealing at 200a400 degree C, while MMMs synthesized from cross-linkable co-polyimides (6FDA-Durene/DABA (9/1) and 6FDA-Durene/DABA (7/3)) show significant enhancements in CO2/CH4 and C3H6/C3H8 selectivity as well as plasticization suppression characteristics up to a CO2 pressure of 30 atm after annealing at 400 degree C due to the cross-linking reaction of the carboxyl acid (COOH) in the DABA moiety. The MMM made of 6FDA-Durene/DABA (9/1) and 40 wt% ZIF-8 possess a notable ideal C3H6/C3H8 selectivity of 27.38 and a remarkable C3H6 permeability of 47.3 Barrer. After thermally annealed at 400 degree C, the MMM made of 6FDA-Durene/DABA (9/1) and 20 wt% ZIF-8 shows a CO2/CH4 selectivity of 19.61 and an impressive CO2 permeability 728 Barrer in mixed gas tests. The newly developed MMMs may have great potential for industrial nature gas purification and C3H6/C3H8 separation.
Using three 6FDA-based polyimides (6FDA-Durene, 6FDA-Durene/DABA (9/1), 6FDA-Durene/DABA (7/3)) and nano-size zeolitic imidazolate framework-8 (ZIF-8), we have fabricated mixed matrix membranes (MMMs) with uniform morphology comprising ZIF-8as high as 40wt% loading by directly mixing as-synthesized ZIF-8 suspension into the polymer solution. Permeability of all gases (CO₂, CH₄, C₃H₆, and C₃H₈) increases rapidly with an increase in ZIF-8 loading. However, the addition of ZIF-8 nano-particles into the polymer matrix increases the ideal CO₂/CH₄ selectivity of only 6.87%, while the ideal C₃H₆/C₃H₈ selectivity improves 134% from 11.68 to 27.38 for the MMM made of 6FDA-Durene/DABA (9/1) and 40wt% ZIF-8. Experimental data show that the plasticization resistance and gas pair selectivity of MMMs are strongly dependent on the amount of cross-linkable moiety and annealing temperature. MMMs made of 6FDA-Durene do not show considerable improvements on resistance against CO₂-induced plasticization after annealing at 200–400°C, while MMMs synthesized from cross-linkable co-polyimides (6FDA-Durene/DABA (9/1) and 6FDA-Durene/DABA (7/3)) show significant enhancements in CO₂/CH₄ and C₃H₆/C₃H₈ selectivity as well as plasticization suppression characteristics up to a CO₂ pressure of 30atm after annealing at 400°C due to the cross-linking reaction of the carboxyl acid (COOH) in the DABA moiety. The MMM made of 6FDA-Durene/DABA (9/1) and 40wt% ZIF-8 possess a notable ideal C₃H₆/C₃H₈ selectivity of 27.38 and a remarkable C₃H₆ permeability of 47.3 Barrer. After thermally annealed at 400°C, the MMM made of 6FDA-Durene/DABA (9/1) and 20wt% ZIF-8 shows a CO₂/CH₄ selectivity of 19.61 and an impressive CO₂ permeability 728 Barrer in mixed gas tests. The newly developed MMMs may have great potential for industrial nature gas purification and C₃H₆/C₃H₈ separation.
Using three 6FDA-based polyimides (6FDA-Durene, 6FDA-Durene/DABA (9/1), 6FDA-Durene/DABA (7/3)) and nano-size zeolitic imidazolate framework-8 (ZIF-8), we have fabricated mixed matrix membranes (MMMs) with uniform morphology comprising ZIF-8as high as 40wt% loading by directly mixing as-synthesized ZIF-8 suspension into the polymer solution. Permeability of all gases (CO2, CH4, C3H6, and C3H8) increases rapidly with an increase in ZIF-8 loading. However, the addition of ZIF-8 nano-particles into the polymer matrix increases the ideal CO2/CH4 selectivity of only 6.87%, while the ideal C3H6/C3H8 selectivity improves 134% from 11.68 to 27.38 for the MMM made of 6FDA-Durene/DABA (9/1) and 40wt% ZIF-8. Experimental data show that the plasticization resistance and gas pair selectivity of MMMs are strongly dependent on the amount of cross-linkable moiety and annealing temperature. MMMs made of 6FDA-Durene do not show considerable improvements on resistance against CO2-induced plasticization after annealing at 200–400°C, while MMMs synthesized from cross-linkable co-polyimides (6FDA-Durene/DABA (9/1) and 6FDA-Durene/DABA (7/3)) show significant enhancements in CO2/CH4 and C3H6/C3H8 selectivity as well as plasticization suppression characteristics up to a CO2 pressure of 30atm after annealing at 400°C due to the cross-linking reaction of the carboxyl acid (COOH) in the DABA moiety. The MMM made of 6FDA-Durene/DABA (9/1) and 40wt% ZIF-8 possess a notable ideal C3H6/C3H8 selectivity of 27.38 and a remarkable C3H6 permeability of 47.3 Barrer. After thermally annealed at 400°C, the MMM made of 6FDA-Durene/DABA (9/1) and 20wt% ZIF-8 shows a CO2/CH4 selectivity of 19.61 and an impressive CO2 permeability 728 Barrer in mixed gas tests. The newly developed MMMs may have great potential for industrial nature gas purification and C3H6/C3H8 separation. [Display omitted] •Cross-linkable co-polyimide/ZIF-8 mixed matrix membranes (MMMs) are fabricated.•Effects of diamine ratio on polymer structure and gas separation performance are studied.•Effect of heat treatment temperature on MMM performance is investigated.•Increasing ZIF-8 loading leads to increase MMM permeability for all gasses.•Cross-linkable co-polyimides thermally treated at 400°C have shown selectivity enhancement.
Author Askari, Mohammad
Chung, Tai-Shung
Author_xml – sequence: 1
  givenname: Mohammad
  surname: Askari
  fullname: Askari, Mohammad
– sequence: 2
  givenname: Tai-Shung
  surname: Chung
  fullname: Chung, Tai-Shung
  email: chencts@nus.edu.sg
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Keywords Mixed matrix membrane
Olefin/paraffin separation
Thermal cross-linking
Natural gas purification
Metal organic framework
Polyimide
Separation
Paraffin
Olefin
Gas purification
Membrane
Ethylenic compound
Natural gas
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Snippet Using three 6FDA-based polyimides (6FDA-Durene, 6FDA-Durene/DABA (9/1), 6FDA-Durene/DABA (7/3)) and nano-size zeolitic imidazolate framework-8 (ZIF-8), we have...
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SubjectTerms Annealing
artificial membranes
Carbon dioxide
Chemistry
Colloidal state and disperse state
Crosslinking
Exact sciences and technology
gases
General and physical chemistry
Membranes
methane
Mixed matrix membrane
mixing
nanoparticles
Nanostructure
natural gas
Natural gas purification
olefin
Olefin/paraffin separation
Permeability
polymers
Purification
Selectivity
temperature
Thermal cross-linking
Title Natural gas purification and olefin/paraffin separation using thermal cross-linkable co-polyimide/ZIF-8 mixed matrix membranes
URI https://dx.doi.org/10.1016/j.memsci.2013.05.016
https://www.proquest.com/docview/1513451570
https://www.proquest.com/docview/1671622574
https://www.proquest.com/docview/1803097243
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