Formulating Self‐Repairing Solid Electrolyte Interface via Dynamic Electric Double Layer for Practical Zinc Ion Batteries

Abstract

Zinc ion batteries (ZIBs) encounter interface issues stemming from the water-rich electrical double layer (EDL) and unstable solid-electrolyte interphase (SEI). Herein, we propose the dynamic EDL and self-repairing hybrid SEI for practical ZIBs via incorporating the horizontally-oriented dual-site additive. The rearrangement of distribution and molecular configuration of additive constructs the robust dynamic EDL under different interface charges. And, a self-repairing organic-inorganic hybrid SEI is constructed via the electrochemical decomposition of additive. The dynamic EDL and self-repairing SEI accelerate interfacial kinetics, regulate deposition and suppress side reactions in the both stripping and plating during long-term cycles, which affords high reversibility for 500 h at 42.7 % depth of discharge or 50 mA ⋅ cm^-1. Remarkably, Zn//NVO full cells deliver the impressive cycling stability for 10000 cycles with 100 % capacity retention at 3 A ⋅ g^-1 and for over 3000 cycles even at lean electrolyte (7.5 μL ⋅ mAh^-1) and high loading (15.26 mg ⋅ cm^-2). Moreover, effectiveness of this strategy is further demonstrated in the low-temperature full cell (-30 °C).