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).