Zigzag Hopping Site Embedded Covalent Organic Frameworks Coating for Zn Anode

Abstract Precise design and tuning of Zn hopping/transfer sites with deeper understanding of the dendrite‐formation mechanism is vital in artificial anode protective coating for aqueous Zn‐ion batteries (AZIBs). Here, we probe into the role of anode‐coating interfaces by designing a series of anhydride‐based covalent organic frameworks (i.e., PI‐DP‐COF and PI‐DT‐COF) with specifically designed zigzag hopping sites and zincophilic anhydride groups that can serve as desired platforms to investigate the related Zn 2+ hopping/transfer behaviours as well as the interfacial interaction. Combining theoretical calculations with experiments, the ABC stacking models of these COFs endow the structures with specific zigzag sites along the 1D channel that can accelerate Zn 2+ transfer kinetics, lower surface‐energy, homogenize ion‐distribution or electric‐filed. Attributed to these superiorities, thus‐obtained optimal PI‐DT‐COF cells offer excellent cycling lifespan in both symmetric‐cell (2000 cycles at 60 mA cm −2 ) and full‐cell (1600 cycles at 2 A g −1 ), outperforming almost all the reported porous crystalline materials.