Phosphorylation Regulation Promotes Bidirectional Dynamic Adaptive Interface for Achieving Stable Zn–I ₂ Batteries

Abstract

Abstract Unstable electrode–electrolyte interfaces resulting from severe cathodic polyiodide shuttling, anodic parasitic corrosion reactions, and dendrite growth significantly impede the performance of zinc–iodine (Zn–I 2 ) batteries. Here, phosphorylation regulation is proposed to create dynamically adaptive water‐lean interfaces for long‐term Zn–I 2 batteries. Phosphorylation reinforces the adaptive interface construction through the increased adsorption capability on the Zn anode and introduces a dynamic pH‐balancing capability while simultaneously offering extra sites for the real‐time capture of polyiodide intermediates at the cathode. Consequently, extended durability (4400 h at 5 mA cm −2 and 1 mAh cm −2 ), boosted coulombic efficiency (99.8% for 7500 cycles), and ultralong cycling for 8000 cycles at a high loading of 10 mg cm −2 were maintained. These findings provide crucial insights into the optimization of adaptive interfaces through phosphorylation regulation for high‐performance Zn–I 2 batteries.