Accelerating Ion Desolvationvia Bioinspired Ion ChannelDesign in Nonconcentrated Aqueous Electrolytes

In aqueous-based electrochemical energy storage devices, uncontrolled hydrolysis of water at the electrochemical interfaces limits the application of such aqueous batteries or supercapacitors in business. The “water-in-salt” design is a valid strategy to broaden the electrochemical stability window in aqueous electrolytes, but drawbacks such as high manufacturing cost, high electrolyte viscosity, etc., also hinder its development. Here, inspired by biological ion channels in cell membranes, we propose an effective approach to engineer the electrode surface, inducing the desolvation of hydrated ions at the electrochemical interface and inhibiting water decomposition in nonconcentrated electrolytes. The biological engineering strategy enables the induction of controlled desolvation and accelerates the transportation of hydrated ions, e.g., potassium. The subnanometer design (0.8 nm) forces the hydrated potassium ions to shed their solvation shell with a hydration number of only 0.3, while the electrostatic interactions between the pore groups and the potassium ions facilitate their transport. The Zn||Zn cells demonstrate a stable cycling lifespan of over 1000 h at 1 mA cm^–2/10 mAh cm^–2. This work sheds new light on regulating the electrochemical interfaces in low-concentration aqueous electrolytes for designing aqueous-based energy storage devices.