Mechanoresponsive Metal‐Organic Cage‐Crosslinked Polymer Hydrogels

Author:

Küng Robin1ORCID,Germann Anne1ORCID,Krüsmann Marcel2,Niggemann Louisa P.34,Meisner Jan5ORCID,Karg Matthias2ORCID,Göstl Robert3ORCID,Schmidt Bernd M.1ORCID

Affiliation:

1. Institute for Organic Chemistry and Macromolecular Chemistry Heinrich Heine University Düsseldorf Universitätsstr. 1 40225 Düsseldorf Germany

2. Institute for Physical Chemistry I: Colloids and Nanooptics Heinrich Heine University Düsseldorf Universitätsstr. 1 40225 Düsseldorf Germany

3. DWI – Leibniz Institute for Interactive Materials Forckenbeckstr. 50 52056 Aachen Germany

4. Institute of Technical and Macromolecular Chemistry RWTH Aachen University Worringerweg 1 52074 Aachen Germany

5. Institute for Physical Chemistry Heinrich Heine University Düsseldorf Universitätsstr. 1 40225 Düsseldorf Germany

Abstract

AbstractWe report the formation of metal‐organic cage‐crosslinked polymer hydrogels. To enable crosslinking of the cages and subsequent network formation, we used homodifunctionalized poly(ethylene glycol) (PEG) chains terminally substituted with bipyridines as ligands for the Pd6L4 corners. The encapsulation of guest molecules into supramolecular self‐assembled metal‐organic cage‐crosslinked hydrogels, as well as ultrasound‐induced disassembly of the cages with release of their cargo, is presented in addition to their characterization by nuclear magnetic resonance (NMR) techniques, rheology, and comprehensive small‐angle X‐ray scattering (SAXS) experiments. The constrained geometries simulating external force (CoGEF) method and barriers using a force‐modified potential energy surface (FMPES) suggest that the cage‐opening mechanism starts with the dissociation of one pyridine ligand at around 0.5 nN. We show the efficient sonochemical activation of the hydrogels HG36, increasing the non‐covalent guest‐loading of completely unmodified drugs available for release by a factor of ten in comparison to non‐crosslinked, star‐shaped assemblies in solution.

Funder

Deutsche Forschungsgemeinschaft

Volkswagen Foundation

Jürgen Manchot Stiftung

Publisher

Wiley

Subject

General Chemistry,Catalysis,Organic Chemistry

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