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

Hou, Jingwei; Sutrisna, Putu D.; Wang, Tiesheng; Gao, Song; Li, Qi; Zhou, Chao; Sun, Shijing; Yang, Hao-Cheng; Wei, Fengxia; Ruggiero, Michael T.; Zeitler, J. Axel; Cheetham, Anthony K.; Liang, Kang; Chen, Vicki

doi:10.1021/acsami.8b20570

Title: Unraveling the Interfacial Structure–Performance Correlation of Flexible Metal–Organic Framework Membranes on Polymeric Substrates

Journal Article · Thu Jan 10 00:00:00 EST 2019 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.8b20570· OSTI ID:1499805

; Sutrisna, Putu D.;

; Gao, Song; Li, Qi;

; Sun, Shijing ^[1]; Yang, Hao-Cheng ^[2]; Wei, Fengxia;

^[3];

;

; Chen, Vicki ^[4]

Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge 02139, Massachusetts, United States
School of Chemical Engineering and Technology, Sun Yat-Sen University, Zhuhai 519082, China
Department of Chemistry, University of Vermont, Burlington 05405, United States
School of Chemical Engineering, University of Queensland, St Lucia 4072, Australia

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 a

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: Australian Research Council (ARC); China Scholarship Council (CSC); Engineering and Physical Sciences Research Council (EPSRC); UNSW Scientia Fellowship

OSTI ID:: 1499805

Journal Information:: ACS Applied Materials and Interfaces, Vol. 11, Issue 5; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 23 works

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