Covalent Organic Frameworks-Derived Functional Interphase for Improving Zn Chemistry in Aqueous Zinc-Ion Batteries

Abstract

As promising candidates adapted for large-scale energy storage, aqueous zinc-ion batteries (AZIBs) offer inherent safety and cost advantages yet face commercialization barriers from Zn anode degradation, attributed to dendrite growth, hydrogen evolution, and surface passivation. Covalent organic frameworks (COFs), with their nanostructured porosity and programmable functionalities, demonstrate exceptional Zn stabilization capability through stabilized interfaces and enhanced ion transport, improving anodic cycling durability and Coulombic efficiency. This review systematically summarizes COFs engineering strategies for improving the reversibility of Zn plating/stripping chemistry, focusing on three synergistic approaches: 1) surface modification via coatings; 2) physical modulation through structural adjustment; 3) chemical functionalization by targeted active sites. Current challenges regarding interfacial kinetics optimization and long-term stability are critically assessed. Perspectives on molecular-level design principles and scalable integration methods outline pathways for developing COF-enhanced AZIBs with commercial viability. The analysis establishes fundamental structure-property relationships and provides actionable guidelines for next-generation COF-integrated energy storage systems.