High Gas Permeability in Aged Superglassy Membranes with Nanosized UiO‐66−NH2/cPIM‐1 Network Fillers

Superglassy membranes synthesised by polymers of intrinsic microporosity (PIMs) suffer from physical aging and show poor gas permeance over time, especially thin membranes, due to the fast rearrangement of nonequilibrium polymer chains. Herein, we constructed a novel PIM‐1 thin film nanocomposite me...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2024-01, Vol.63 (1), p.e202316356-n/a
Main Authors: Qiu, Boya, Yu, Ming, Luque‐Alled, Jose Miguel, Ding, Shengzhe, Foster, Andrew B., Budd, Peter M., Fan, Xiaolei, Gorgojo, Patricia
Format: Article
Language:English
Subjects:
Aging
Carbon dioxide
Chains (polymeric)
Chemical synthesis
Dimensional stability
Fillers
Functional groups
Gas Separation
Hydrogen bonding
Membrane permeability
Membranes
Metal–Organic Frameworks
Microporosity
Nanocomposites
Nucleation
Permeability
Polymer of Intrinsic Microporosity
Polymers
Quantum dots
Reluctance
Thin Film Nanocomposite Membranes
Thin films
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Summary:Superglassy membranes synthesised by polymers of intrinsic microporosity (PIMs) suffer from physical aging and show poor gas permeance over time, especially thin membranes, due to the fast rearrangement of nonequilibrium polymer chains. Herein, we constructed a novel PIM‐1 thin film nanocomposite membrane (TFN) using nanosized UiO‐66−NH2 (≈10 nm)/carboxylated PIM‐1 (cPIM‐1) as the composite filler. Unlike conventional fillers, which interact with the polymer only via the surface, the UiO‐66−NH2/cPIM‐1 forms a stable three‐dimensional (3D) network intertwining with the polymer chains, being very effective to impede chain relaxation, and thus physical aging. Nanosizing of UiO‐66−NH2 was achieved by regulating the nucleation kinetics using carbon quantum dots (CQD) during the synthesis. This led to increased surface area, and hence more functional groups to bond with cPIM‐1 (via hydrogen bonding between −NH2 and −COOH groups), which also improved interfacial compatibility between the 3D network and polymer chains avoiding defect formation. As a result, the novel TFN showed significantly improved performance in gas separation along with reduced aging (i.e. ≈6 % loss in CO2 permeability over 63 days); the aged membranes had a CO2 permeance of 2504 GPU and ideal selectivity values of 37.2 and 23.8 for CO2/N2 and CO2/CH4, respectively. A novel network filler, composed of nanosized UiO‐66−NH2 (≈10 nm) and carboxylated PIM‐1 (cPIM‐1) was prepared and was introduced into PIM‐1 thin film nanocomposite membranes (TFN). Unlike conventional fillers, which interact with the polymer only via the surface, the UiO‐66−NH2/cPIM‐1 forms a stable three‐dimensional (3D) network intertwining with the polymer chains, being very effective to impede chain relaxation and physical aging.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202316356