Enhancing ion transport in polymer hydrogels is essential for the development of hydrogel‐based electrochemical devices. Herein, this study investigates the molecular mechanisms by which embedded SiO 2 nanoparticles enhance the ionic conductivity of poly(acrylic acid) (PAA) hydrogels. Upon hydration, the deprotonated PAA chains expand the intermolecular space through electrostatic repulsion. Concurrently, the strong surface energy of SiO 2 drives the formation of solvent‐enriched interfacial water channels. These interfacial structures facilitate ion transport via two synergistic effects: 1) Zn 2+ ions near the nanoparticle interface experience reduced structural constraints from the polymer network, and 2) the hydration shells of interfacial Zn 2+ ions are partially disturbed and asymmetric, weakening the ion‐water binding. These nanoscale alterations reduce both steric hindrance and solvation energy barriers, resulting in enhanced Zn 2+ mobility within the hydrogel domains. This work provides a mechanistic framework for understanding nanoparticle–hydrogel interactions and offers insights into the design of composite hydrogel electrolytes with enhanced ion‐transport performance.
Kim et al. (Thu,) studied this question.
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