Engineering Robust Hydrophilic-Hydrophobic Interface via π-electron Delocalization for Ultralong-Lived Zinc-Ion...

Aqueous zinc ion batteries (AZIBs) are hindered by the severe interfacial issues of Zn anode such as side reactions and dendrite growth. The in-situ construction of robust interface to tackle above issues remains a grand challenge and lacks rational design principles, especially under high current density. Herein, a π-electron delocalization strategy is proposed to in-situ construct the self-assembled hydrophilic-hydrophobic interface layer (HHIL) for ultralong-lived AZIBs, where interface design principles are built based on the electronic structure and spatial configuration of additives. Encouragingly, HHIL derived by π-π interactions and ion-dipole interactions is robust during long-term cycling and facilitates the generation of an inorganic-rich interface chemistry. The flexible HHIL and rigid inorganic-rich interface afford the rapid interface kinetics, and effectively suppresses side reactions and dendrite growth. Notably, Zn//Zn cells deliver the cycling life over 900 h at 20 mA cm^-2 and 10 mAh cm^-2, and Zn//NVO full cells stably perform over 25 000 cycles at 10 A g^-1. Furthermore, the practical pouch cell is also demonstrated.