Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide

Ainur Yerzhankyzy; Yingge Wang; Feng Xu; Xiaofan Hu; Bader Ghanem; Xiaohua Ma; Marcel Balcik; Nimer Wehbe; Yu Han; Ingo Pinnau

doi:10.1016/j.memsci.2023.121764

Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide

Ainur Yerzhankyzy, Yingge Wang, Feng Xu, Xiaofan Hu, Bader Ghanem, Xiaohua Ma, Marcel Balcik, Nimer Wehbe, Yu Han, Ingo Pinnau

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

The changes in physical, chemical, and gas permeation properties of a heat-treated hydroxyl-functionalized Tröger's base-derived intrinsically microporous polyimide, 6FDA-HTB, were systematically studied. Polyimide samples were heated-treated for 30 minutes at a fixed temperature to form (i) polybenzoxazole (PBO) by thermal rearrangement (TR) from ∼420 to ∼440 °C, (ii) polymer-carbon transition (PCT) from ∼460 to ∼500 °C, and (iii) early-stage carbon (ESC) membranes from >500 to 600 °C. As frequently observed in previous studies, TR-derived PBO membranes showed an increase in gas permeability with a concomitant decrease in gas-pair selectivity. The intermediate PCT region represents a transition state from a pure PBO to a partially carbonized polymer with superior properties by showing a simultaneous boost in gas permeability and gas-pair selectivity. The ESC membranes formed between 550 to 600 °C possessed further enhanced selectivity but reduced permeability due to tightening of the amorphous CMS structure. The mixed-gas separation properties of selected aged samples, pristine 6FDA-HTB, PBO (6FDA-HTB-420), intermediate PCT (6FDA-HTB-480), and early stage CMS analogs (6FDA-HTB-550 and 600), were investigated using a 1:1 CO2/CH4 feed up to 30 bar. In this series, early-stage CMS membranes displayed the best mixed-gas CO2/CH4 separation properties with performance significantly surpassing the 2018 polymer mixed-gas upper bound.

Original language	English (US)
Pages (from-to)	121764
Journal	Journal of Membrane Science
DOIs	https://doi.org/10.1016/j.memsci.2023.121764
State	Published - May 29 2023

Bibliographical note

KAUST Repository Item: Exported on 2023-06-01
Acknowledged KAUST grant number(s): BAS/1/1323-01-01, BAS/1/1372-01-01
Acknowledgements: This research was supported by funding (BAS/1/1323-01-01) and (BAS/1/1372-01-01) from King Abdullah University of Science and Technology.

ASJC Scopus subject areas

Biochemistry
Filtration and Separation
General Materials Science
Physical and Theoretical Chemistry

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https://repository.kaust.edu.sa/bitstream/10754/692277/1/1-s2.0-S0376738823004209-main_removed.pdf

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Yerzhankyzy, A., Wang, Y., Xu, F., Hu, X., Ghanem, B., Ma, X., Balcik, M., Wehbe, N., Han, Y., & Pinnau, I. (2023). Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide. Journal of Membrane Science, 121764. https://doi.org/10.1016/j.memsci.2023.121764

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title = "Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tr{\"o}ger's base polyimide",

abstract = "The changes in physical, chemical, and gas permeation properties of a heat-treated hydroxyl-functionalized Tr{\"o}ger's base-derived intrinsically microporous polyimide, 6FDA-HTB, were systematically studied. Polyimide samples were heated-treated for 30 minutes at a fixed temperature to form (i) polybenzoxazole (PBO) by thermal rearrangement (TR) from ∼420 to ∼440 °C, (ii) polymer-carbon transition (PCT) from ∼460 to ∼500 °C, and (iii) early-stage carbon (ESC) membranes from >500 to 600 °C. As frequently observed in previous studies, TR-derived PBO membranes showed an increase in gas permeability with a concomitant decrease in gas-pair selectivity. The intermediate PCT region represents a transition state from a pure PBO to a partially carbonized polymer with superior properties by showing a simultaneous boost in gas permeability and gas-pair selectivity. The ESC membranes formed between 550 to 600 °C possessed further enhanced selectivity but reduced permeability due to tightening of the amorphous CMS structure. The mixed-gas separation properties of selected aged samples, pristine 6FDA-HTB, PBO (6FDA-HTB-420), intermediate PCT (6FDA-HTB-480), and early stage CMS analogs (6FDA-HTB-550 and 600), were investigated using a 1:1 CO2/CH4 feed up to 30 bar. In this series, early-stage CMS membranes displayed the best mixed-gas CO2/CH4 separation properties with performance significantly surpassing the 2018 polymer mixed-gas upper bound.",

author = "Ainur Yerzhankyzy and Yingge Wang and Feng Xu and Xiaofan Hu and Bader Ghanem and Xiaohua Ma and Marcel Balcik and Nimer Wehbe and Yu Han and Ingo Pinnau",

note = "KAUST Repository Item: Exported on 2023-06-01 Acknowledged KAUST grant number(s): BAS/1/1323-01-01, BAS/1/1372-01-01 Acknowledgements: This research was supported by funding (BAS/1/1323-01-01) and (BAS/1/1372-01-01) from King Abdullah University of Science and Technology.",

year = "2023",

month = may,

day = "29",

doi = "10.1016/j.memsci.2023.121764",

language = "English (US)",

pages = "121764",

journal = "Journal of Membrane Science",

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Yerzhankyzy, A, Wang, Y, Xu, F, Hu, X, Ghanem, B, Ma, X, Balcik, M , Wehbe, N, Han, Y & Pinnau, I 2023, 'Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide', Journal of Membrane Science, pp. 121764. https://doi.org/10.1016/j.memsci.2023.121764

Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide. / Yerzhankyzy, Ainur; Wang, Yingge; Xu, Feng et al.
In: Journal of Membrane Science, 29.05.2023, p. 121764.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide

AU - Yerzhankyzy, Ainur

AU - Wang, Yingge

AU - Xu, Feng

AU - Hu, Xiaofan

AU - Ghanem, Bader

AU - Ma, Xiaohua

AU - Balcik, Marcel

AU - Wehbe, Nimer

AU - Han, Yu

AU - Pinnau, Ingo

N1 - KAUST Repository Item: Exported on 2023-06-01 Acknowledged KAUST grant number(s): BAS/1/1323-01-01, BAS/1/1372-01-01 Acknowledgements: This research was supported by funding (BAS/1/1323-01-01) and (BAS/1/1372-01-01) from King Abdullah University of Science and Technology.

PY - 2023/5/29

Y1 - 2023/5/29

N2 - The changes in physical, chemical, and gas permeation properties of a heat-treated hydroxyl-functionalized Tröger's base-derived intrinsically microporous polyimide, 6FDA-HTB, were systematically studied. Polyimide samples were heated-treated for 30 minutes at a fixed temperature to form (i) polybenzoxazole (PBO) by thermal rearrangement (TR) from ∼420 to ∼440 °C, (ii) polymer-carbon transition (PCT) from ∼460 to ∼500 °C, and (iii) early-stage carbon (ESC) membranes from >500 to 600 °C. As frequently observed in previous studies, TR-derived PBO membranes showed an increase in gas permeability with a concomitant decrease in gas-pair selectivity. The intermediate PCT region represents a transition state from a pure PBO to a partially carbonized polymer with superior properties by showing a simultaneous boost in gas permeability and gas-pair selectivity. The ESC membranes formed between 550 to 600 °C possessed further enhanced selectivity but reduced permeability due to tightening of the amorphous CMS structure. The mixed-gas separation properties of selected aged samples, pristine 6FDA-HTB, PBO (6FDA-HTB-420), intermediate PCT (6FDA-HTB-480), and early stage CMS analogs (6FDA-HTB-550 and 600), were investigated using a 1:1 CO2/CH4 feed up to 30 bar. In this series, early-stage CMS membranes displayed the best mixed-gas CO2/CH4 separation properties with performance significantly surpassing the 2018 polymer mixed-gas upper bound.

AB - The changes in physical, chemical, and gas permeation properties of a heat-treated hydroxyl-functionalized Tröger's base-derived intrinsically microporous polyimide, 6FDA-HTB, were systematically studied. Polyimide samples were heated-treated for 30 minutes at a fixed temperature to form (i) polybenzoxazole (PBO) by thermal rearrangement (TR) from ∼420 to ∼440 °C, (ii) polymer-carbon transition (PCT) from ∼460 to ∼500 °C, and (iii) early-stage carbon (ESC) membranes from >500 to 600 °C. As frequently observed in previous studies, TR-derived PBO membranes showed an increase in gas permeability with a concomitant decrease in gas-pair selectivity. The intermediate PCT region represents a transition state from a pure PBO to a partially carbonized polymer with superior properties by showing a simultaneous boost in gas permeability and gas-pair selectivity. The ESC membranes formed between 550 to 600 °C possessed further enhanced selectivity but reduced permeability due to tightening of the amorphous CMS structure. The mixed-gas separation properties of selected aged samples, pristine 6FDA-HTB, PBO (6FDA-HTB-420), intermediate PCT (6FDA-HTB-480), and early stage CMS analogs (6FDA-HTB-550 and 600), were investigated using a 1:1 CO2/CH4 feed up to 30 bar. In this series, early-stage CMS membranes displayed the best mixed-gas CO2/CH4 separation properties with performance significantly surpassing the 2018 polymer mixed-gas upper bound.

UR - http://hdl.handle.net/10754/692277

UR - https://linkinghub.elsevier.com/retrieve/pii/S0376738823004209

U2 - 10.1016/j.memsci.2023.121764

DO - 10.1016/j.memsci.2023.121764

M3 - Article

SN - 0376-7388

SP - 121764

JO - Journal of Membrane Science

JF - Journal of Membrane Science

ER -

Yerzhankyzy A, Wang Y, Xu F, Hu X, Ghanem B, Ma X et al. Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide. Journal of Membrane Science. 2023 May 29;121764. doi: 10.1016/j.memsci.2023.121764

Structural evolution and gas separation properties of thermally rearranged polybenzoxazole (TR-PBO), polymer-carbon transition (PCT) and early-stage carbon (ESC) membranes derived from a 6FDA-hydroxyl-functionalized Tröger's base polyimide

Abstract

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