Limiting Interfacial Free Water and Proton Concentration by Hydrogel Electrolytes for Stable MoO₃ Anode in a Proton Battery

Aqueous rechargeable proton batteries are attractive due to the small ionic radius, light mass, and ultrafast diffusion kinetics of proton as charge carriers. However, the commonly used acidic electrolyte is usually very corrosive to the electrode material, which seriously affects the cycle life of the battery. Here, it is proposed that decreasing water activity and limiting proton concentration can effectively prevent side reactions of the MoO3 anode such as corrosion and hydrogen precipitation by using a lean-water hydrogel electrolyte. The as-prepared polyacrylamide (PAAM)-poly2-acrylamide-2-methylpropanesulfonic acid (PAMPS)/MnSO4 (PPM) hydrogel electrolyte not only has abundant hydrophilic groups that can form hydrogen bonds with free water and inhibit solvent-electrode interaction, but also has fixed anions that can maintain a certain interaction with protons. The assembled MoO3||MnO2 full battery can stably cycle over 500 times for approximate to 350 h with an unprecedented capacity retention of 100% even at a low current density of 0.5 A g(-1). This work gives a hint that limiting free water as well as proton concentration is important for the design of electrolytes or interfaces in aqueous proton batteries.