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Ion Valency as a Molecular Switch for Salt-Resistant Underwater Adhesion
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DOI：10.1002/adma.202508666.png)
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Abstract
En 中文
Achieving underwater adhesion remains challenging due to the disruption of interfacial interactions by hydration layers and the ionic environment. This study shows how high adhesion in a saline environment can be achieved in adhesive peptide systems relying on π–π and cation-π interactions using multivalent ions. Monovalent ions (K+) disrupt native peptide-peptide interactions, drastically reducing adhesion strength. Conversely, multivalent ions (Mg2+ and Y3+) enable robust interfacial adhesion by forming stable π-cation-π networks, effectively compensating for disrupted native pairings. The adhesion enhancement by Y3+ is particularly pronounced, highlighting its unique capability for multidentate bridging. Molecular dynamics simulations and quantum mechanical analyses confirm that Y3+ ions stabilize extended interfacial interactions, enabling stronger stress dissipation during tensile deformation. Additionally, NMR spectroscopy supports these observations by demonstrating significant cation-dependent perturbations of aromatic (Phe) and cationic (Lys) peptide residues. A thermodynamic model further elucidates the competitive binding dynamics underpinning adhesion modulation and capturing all experimental trends. This work provides detailed molecular insights into ion valency effects on cation-π mediated underwater adhesion, guiding the development of bio-inspired materials with tailored ionic responsiveness suitable for biomedical and technological applications in saline environments.
Keywords:
adhesion
bottlebrush polymer
cation-π interaction
molecular switch
molecular dynamics simulation
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