Moisture-Responsive Ion-Coupling Networks in Molecularly Engineered MoS₂ Channels for Enhanced Ion Transport

Classical nanofluidic ion transport predominantly relies on fixed surface charges for selectivity. However, such static-charge systems are fundamentally limited by an "immobilization effect"; the deep energy wells required for ion recruitment inevitably hinder subsequent release, stifling continuous transport kinetics. Herein, we report a paradigm-shifting dynamic ion-coupling mechanism mediated by surface-anchored counter-ions that establish transient, moisture-responsive coordination with mobile species. By decorating angstrom-scale 2D molybdenum disulfide (MoS₂) channels with single-site Pb²⁺, we create a molecularly engineered interface that facilitates rapid ion hopping. This strategy flattens the migration energy landscape and decouples ion entry from release, circumventing the inherent trade-off in traditional fixed-charge membranes. Our biomimetic approach achieves an extraordinary 30-fold enhancement in ionic current compared to pristine channels. Leveraging these dynamic interactions, we demonstrate a humidity-driven energy generator delivering a record-high power density of 532.8 µW cm^{- 2} at ∼75% RH, significantly surpassing state-of-the-art technologies. These findings establish dynamic ion coupling as a powerful blueprint for advancing molecular iontronics, self-powered sensing, and next-generation energy conversion.