Unraveling the Interfacial Structure−Performance Correlation of Flexible Metal−Organic Framework Membranes on Polymeric Substrates

Hou, Jingwei and Sutrisna, Putu Doddy and Wang, Tiesheng and Gao, Song and Li, Qi and Zhou, Chao and Sun, Shijing and Yang, Hao-Cheng and Wei, Fengxia and Ruggiero, M.T. and Zeitler, Z.A. and Cheetham, A.K. and Liang, Kang and Chen, Vicki (2019) Unraveling the Interfacial Structure−Performance Correlation of Flexible Metal−Organic Framework Membranes on Polymeric Substrates. ACS Applied Materials and Interfaces, 11 (5). pp. 5570-5577. ISSN 1944-8252

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Abstract

Pure metal−organic framework (MOF) layers deposited on porous supports are important candidates for molecular sieving membranes, but their performance usually deviates from theoretical estimations. Here, we combine stepwise scanning electron microscopy imaging, time-resolved synchrotron X-ray scattering, terahertz infrared spectroscopy, and density functional theory calculation to investigate the ZIF-8 membrane formation on two types (polydopamine and TiO2) of functionalized porous supports. Though molecular sieving of ZIF-8 membranes for smaller gases (He, H2, and CO2) can be achieved with both types of functionalized supports, we unravel that the strong interaction between MOF and polydopamine can disrupt the formation of “perfect” MOF crystals at the interface, leading to a “contracted” MOF structure with partially uncoordinated imidazolate ligands. This further affects the low-frequency dynamical parameters of the framework and inhibits the effective seeded growth. Eventually, it leads to an unexpected loss of selectivity for the bulkier gases (N2 and CH4) for ZIF-8 on polydopamine-functionalized supports. This work links the dynamical aspects of MOFs with their gas transport behavior and highlights the importance of regulating the interfacial weak forces to preserve the ideal molecular sieving efficiency of MOF membranes, which also provides guidance for defect engineering of MOF film fabrication for sensing and electronic devices beyond membranes.

Item Type:	Article
Uncontrolled Keywords:	ZIF-8 membrane, molecular sieving, interfacial crystal structure, defects, metal−organic frameworks, crystallization
Subjects:	T Technology > TP Chemical technology
Divisions:	Faculty of Engineering > Department of Chemical Engineering
Depositing User:	Putu Doddy S, 61107 - 200042
Date Deposited:	09 Mar 2020 04:09
Last Modified:	21 Mar 2022 08:02
URI:	http://repository.ubaya.ac.id/id/eprint/37579

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