Molecular origins of fast and selective gas transport in pentiptycene-containing polyimide membranes and their physical aging behavior

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	Molecular origins of fast and selective gas transport in pentiptycene-containing polyimide membranes and their physical aging behavior
	Luo, Shuangjiang 1; Wiegand, Jennifer R.1; Gao, Peiyuan 2; Doherty, Cara M.3; Hill, Anita J.3; Guo, Ruilan 1
刊名	JOURNAL OF MEMBRANE SCIENCE
	2016-11-15
卷号	518 页码:100-109
关键词	Pentiptycene Polyimides Gas separation membrane Bimodal microporosity Physical aging
英文摘要	This paper reports comprehensive characterization and detailed analyses of microporous structure and fundamental gas transport properties for a series of new pentiptycene-containing polyimide gas separation membranes prepared from custom-synthesized pentiptycene-based diamines and 4,4'-hexafluoroisopropylidene bisphthalic dianhydride (6FDA) to identify the molecular origins for fast and selective gas transport. Both experimental characterizations of inter-chain spacing and microporosity and molecular modeling analysis of chain conformations and rigidity suggested that rigid H-shape pentiptycene units effectively disrupted chain packing, resulting in large fractional free volume and consequent high gas permeabilities in these membranes. Atomic-level detection of free volume architecture by positron annihilation lifetime spectroscopy (PALS) analysis revealed a bimodal microcavity size distribution with cavity sizes of d(4 similar to)7-8 angstrom and d(3)similar to 3-4 angstrom in this series of membranes. The microcavity size and size distribution were found to be sensitively affected by the substituent groups in the pentiptycene monomer structure based on the mechanism of "partial filling" of internal molecular cavities defined by the shape of pentiptycene units. Analysis of fundamental gas transport properties in terms of diffusivity (D) and solubility (S) coefficients demonstrated that size sieving mechanism (diffusivity contribution) dominates the gas transport in these polymers and bimodal microcavity size distribution with ultrafine microporosity is responsible for the excellent H2-related gas separation performance. Superior resistance against physical aging was observed for these high-free-volume polymers, which is ascribed to the stable, configuration-induced microcavity structure constructed by the rigid pentiptycene units. (C) 2016 Elsevier B.V. All rights reserved.
收录类别	SCI
语种	英语
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/35396]
专题	化学研究所_其它
作者单位	1.Univ Notre Dame, Dept Chem & Biomol Engn, Notre Dame, IN 46556 USA 2.Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China 3.CSIRO Mfg, Private Bag 10, Clayton, Vic 3169, Australia
推荐引用方式 GB/T 7714	Luo, Shuangjiang,Wiegand, Jennifer R.,Gao, Peiyuan,et al. Molecular origins of fast and selective gas transport in pentiptycene-containing polyimide membranes and their physical aging behavior[J]. JOURNAL OF MEMBRANE SCIENCE,2016,518:100-109.
APA	Luo, Shuangjiang,Wiegand, Jennifer R.,Gao, Peiyuan,Doherty, Cara M.,Hill, Anita J.,&Guo, Ruilan.(2016).Molecular origins of fast and selective gas transport in pentiptycene-containing polyimide membranes and their physical aging behavior.JOURNAL OF MEMBRANE SCIENCE,518,100-109.
MLA	Luo, Shuangjiang,et al."Molecular origins of fast and selective gas transport in pentiptycene-containing polyimide membranes and their physical aging behavior".JOURNAL OF MEMBRANE SCIENCE 518(2016):100-109.