Abstract
Biological ion channels exhibit strong gating effects due to their zero-current closed states. However, the gating capabilities of artificial nanochannels have typically fallen short of biological channels, primarily owing to the larger nanopores that fail to completely block ion transport in the off-states. Here, we demonstrate solid-state hydrogen-bonded organic frameworks-based membranes to achieve high-performance ambient humidity-controlled proton gating, accomplished by switching the proton transport pathway instead of relying on conventional ion blockage/activation effects. Density functional theory calculations reveal that the reversible formation and disruption of humidity-induced water bridges within the frameworks facilitates the switching of proton transport mode from the adsorption site hopping to the Grotthuss mechanism. This transition, coupled with the introduction of bacterial cellulose to enhance desorption/adsorption of water clusters, enables us to achieve a superior proton gating ratio of up to 5740, surpassing state-of-the-art solid-state gating devices. Moreover, the developed membrane operates entirely on solid-state principles, rendering it highly versatile for a myriad of applications from environmental detection to human health monitoring. This study offers perspectives for the design of efficient proton gating systems.