High‐Capacity and Long‐Life Zinc Electrodeposition Enabled by a Self‐Healable and Desolvation Shield for Aqueous Zinc‐Ion Batteries

Artificial interfaces can alleviate the side reactions and the formation of the metallic (e.g., Li, Na, and Zn) dendrites. However, the traditional ones always breakdown during the repeated plating/stripping and fail to regulate the electrodeposition behaviors of the electrodes. Herein, a self‐healable ion regulator (SIR) is designed as a desolvation shield to protect the Zn electrodes and guide the Zn electrodeposition. Benefiting from the intermolecular hydrogen bonds, SIR shows a superb capability to in situ repair the plating/stripping‐induced cracks. Besides, the results of theoretical calculations and electrochemical characterizations show that the coating reduces water molecules in the solvated sheath of hydrated Zn2+ and restrains the random Zn2+ diffusion on the Zn surface. Even with a coating layer of only 360 nm, the SIR‐modified Zn electrode exhibits excellent long‐term stability for >3500 h at 2 mAh cm−2 and >950 h at an ultrahigh areal capacity of 20 mAh cm−2. A self‐healable and desolvation shield is designed as an artificial coating for aqueous Zn electrodes. This interface regulates the solvation sheath of hydrated Zn2+, restrains the random Zn2+ diffusion, and in‐situ repairs the plating/stripping‐induced cracks. By means of the coating, a long‐term cycling stability for >3500 h is achieved.