Interfacial chemistry in multivalent aqueous batteries: fundamentals, challenges, and advances

As one of the most promising electrochemical energy storage systems, aqueous batteries are attracting great interest due to their advantages of high safety, high sustainability, and low costs when compared with commercial lithium-ion batteries, showing great promise for grid-scale energy storage. This invited tutorial review aims to provide universal design principles to address the critical challenges at the electrode-electrolyte interfaces faced by various multivalent aqueous battery systems. Specifically, deposition regulation, ion flux homogenization, and solvation chemistry modulation are proposed as the key principles to tune the inter-component interactions in aqueous batteries, with corresponding interfacial design strategies and their underlying working mechanisms illustrated. In the end, we present a critical analysis on the remaining obstacles necessitated to overcome for the use of aqueous batteries under different practical conditions and provide future prospects towards further advancement of sustainable aqueous energy storage systems with high energy and long durability.