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题名: Molecular origins of fast and selective gas transport in pentiptycene-containing polyimide membranes and their physical aging behavior
作者: Luo, Shuangjiang1; Wiegand, Jennifer R.1; Gao, Peiyuan2; Doherty, Cara M.3; Hill, Anita J.3; Guo, Ruilan1
关键词: Pentiptycene ; Polyimides ; Gas separation membrane ; Bimodal microporosity ; Physical aging
刊名: JOURNAL OF MEMBRANE SCIENCE
发表日期: 2016-11-15
卷: 518, 页:100-109
收录类别: SCI
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.
语种: 英语
内容类型: 期刊论文
URI标识: http://ir.iccas.ac.cn/handle/121111/35396
Appears in Collections:其它_期刊论文

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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
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