Interfacial chemistry regulation using functional frameworks for stable metal batteries

Rechargeable metal batteries (RMBs) stand out as an attractive energy storage technique owing to their high theoretical energy density. However, their unstable electrode-electrolyte interface, resulting from parasitic reactions between electrolytes and active metal anodes (Li/Na/Zn), leads to safety concerns and performance decay in RMBs. Constructing functional frameworks on metal anodes has been demonstrated for achieving stable interfacial chemistry. The frameworks can regulate cation desolvation and substrate metallic affinity to provide sufficient ion flux and abundant nucleation sites, thus realizing uniform metal deposition and dendrite suppression. This review focuses on material engineering in functional frameworks to improve reversible interfacial reactions. Furthermore, porous crystalline frameworks (PCFs), including metal-organic frameworks (MOFs), covalent organic frameworks (COFs), and zeolites, are considered to tailor the solvation sheath and accelerate cation desolvation. Three-dimensional inorganic frameworks (IOFs), such as metal-based and carbon-based materials, are introduced to enhance ionic diffusion and metal nucleation for enhanced metal plating. Additionally, an outlook on the design strategies and challenges in the development of framework materials is provided for the future development of practical RMBs. Recent advances on functional framework materials, including PCFs and IOFs, are summarized to regulate interfacial chemistry in metal batteries, which facilitate cation desolvation and metal nucleation for improved electrochemical performance.