Hydrogelation via Supramolecular Copolymerization of Structural Water within Adaptive Metal-Organic Fibers

Titelangaben

Stühler, Merlin S. ; Makki, Hesam ; Hilal, Tarek ; Chakraboty, Debsena ; Dimde, Mathias ; Ludwig, Kai ; Haag, Rainer ; Rosenfeldt, Sabine ; Silbermagl, Dorothee ; Schäfer, Andreas ; Plajer, Alex:
Hydrogelation via Supramolecular Copolymerization of Structural Water within Adaptive Metal-Organic Fibers.
In: Advanced Materials. Bd. 38 (2026) Heft 31 . - e19933.
ISSN 1521-4095
DOI der Verlagsversion: https://doi.org/10.1002/adma.202519933

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Abstract

Water is conventionally viewed as a disruptive solvent for supramolecular materials, destabilizing directional noncovalent interactions. Here, we report a metal–organic material in which water instead acts as a structural co-monomer driving the formation of supramolecular fibers. A zinc(II) bisphenoxyimine (“Salphen”) complex featuring convergent hydrogen-bond acceptor sites assembles in bulk water into long, hollow nanofibers stabilized by confined structural water molecules. Single-particle analysis and density functional theory reveal tubular architectures in which intercalated water bridges the metal centers and defines a hydrophilic inner channel. The fibers form hydrogels with thermomechanical response, chemically triggerable disassembly and enable selective chiral recognition of amino acids via water-mediated molecular–to–supramolecular information transfer. In organic solvents, the water content can be used for control over supramolecular self-assembly and hence gelation and liquefaction. Our findings establish structural water as a design element for creating adaptive, chiral, and dynamically reconfigurable metal–organic materials, offering a new paradigm to unlock this sustainable building block in supramolecular materials design.