Highly stable Zn anodes enabled by molecular channel of zincophilic supermolecules with abundant lone-pair electrons

Rechargeable aqueous zinc-ion batteries offer significant potential for applications in flexible electronics and stationary energy storage grids. However, their development is impeded by interfacial instability, leading to deleterious side reactions and dendritic zinc growth. Here, we introduce a novel solution by employing zincophilic cucurbit[7]uril supermolecules, which are rich in lone-pair electrons. These supramolecules feature distinct molecular channels that can adeptly accommodate Zn ions during the electrochemical process, thus mitigating Zn ion migration and dendrite formation. Moreover, the supramolecular layer offers a wealth of Lewis basic sites (tertiary-N and carbonyl-O) with lone-pair electrons, acting as electron-donating nucleation sites for Zn2+ ions, promoting localized nucleation while concurrently repelling water molecules, effectively reducing undesired side reactions such as hydrogen evolution and enhancing the stability and efficiency of the system. As a result, symmetric cells and Zn//V2O5 full cells all deliver prolonged cycle life and outstanding coulombic efficiency. These findings highlight the potential of zincophilic supramolecules with lone-pair electrons as promising additives for highly stable Zn metal anodes in advanced energy storage devices.