Nested non-covalent interactions expand the functions of supramolecular polymer networks
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Published version
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Author(s) • • • • • • • •
Lundberg, David J
Brown, Christopher M
Bobylev, Eduard O
Oldenhuis, Nathan J
Alfaraj, Yasmeen S
Zhao, Julia
Kevlishvili, Ilia
Kulik, Heather J
Johnson, Jeremiah A
Date Issued
May 10, 2024
Journal
Nature Communications
Publisher
Springer Science and Business Media LLC
Citation
Lundberg, D.J., Brown, C.M., Bobylev, E.O. et al. Nested non-covalent interactions expand the functions of supramolecular polymer networks. Nat Commun 15, 3951 (2024).
Version
Final published version
Abstract
Supramolecular polymer networks contain non-covalent cross-links that enable access to broadly tunable mechanical properties and stimuli-responsive behaviors; the incorporation of multiple unique non-covalent cross-links within such materials further expands their mechanical responses and functionality. To date, however, the design of such materials has been accomplished through discrete combinations of distinct interaction types in series, limiting materials design logic. Here we introduce the concept of leveraging “nested” supramolecular crosslinks, wherein two distinct types of non-covalent interactions exist in parallel, to control bulk material functions. To demonstrate this concept, we use polymer-linked Pd2L4 metal–organic cage (polyMOC) gels that form hollow metal–organic cage junctions through metal–ligand coordination and can exhibit well-defined host-guest binding within their cavity. In these “nested” supramolecular network junctions, the thermodynamics of host-guest interactions within the junctions affect the metal–ligand interactions that form those junctions, ultimately translating to substantial guest-dependent changes in bulk material properties that could not be achieved in traditional supramolecular networks with multiple interactions in series.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Chemistry
Koch Institute for Integrative Cancer Research at MIT
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DOI of Published Version
https://doi.org/10.1038/s41467-024-47666-x