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

Abstract

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 selfhealable 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 Zn 2 + and restrains the random Zn 2 + 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 À 2 and > 950 h at an ultrahigh areal capacity of 20 mAh cm À 2 .

Challenges and Strategies in the Development of Zinc‐Ion Batteries

“…[65] Dendrites are formed due to the nonuniform distribution of charge on the Zn electrode surface, which can originate from irregular surface imperfections that act as nucleation sites for growth. [66][67][68][69][70][71] Yang et al also proposed that some Zn atoms with a low 2D diffusion energy barrier could preferentially gather together to form a small crystallite. [25] Furthermore, the nonuniform electric field distribution and the high zinc ion distribution in the electrolyte near the electrode would further worsen inhomogeneous electrodeposition.…”

“…[ 65 ] Dendrites are formed due to the nonuniform distribution of charge on the Zn electrode surface, which can originate from irregular surface imperfections that act as nucleation sites for growth. [ 66–71 ] Yang et al. also proposed that some Zn atoms with a low 2D diffusion energy barrier could preferentially gather together to form a small crystallite.…”

Dendrite‐free Zn deposition initiated by nanoscale inorganic–organic coating‐modified 3D host for stable Zn‐ion battery

“…8,11 Whereafter, such inhomogeneous nucleation may induce the irregular electric field distribution, which produces a large amount of Zn dendrites and "dead" Zn. [12][13][14] Over the past years, several strategies, including the employment of artificial coating layers and electrolyte additives, have been explored to promote smooth Zn deposition. [15][16][17][18] Nevertheless, the rational formulation of electrolytes, like "water-in salt" and "deep eutectic solvent," not only increases the cost, but also reduces the ion conductivity.…”

A High‐Capacity Gradient Zn Powder Anode for Flexible Zn‐Ion Batteries

“…[1][2][3][4][5] However, the further application of flexible ZIBs is still restricted by the poor mechanical stability of Zn anodes during long-term deformation and the Zn dendrite growth in the cycling processes, which ultimately results in short-circuits, irreversible capacity loss, and poor cycling efficiency. [6][7][8][9][10] Currently, Zn foil-based anodes have been widely studied for ZIBs, and various surface modification strategies have been adopted for the improvement of Zn foils. [11][12][13][14][15][16] However, the flexibility of Zn foil is limited, and during continuous deformation, the protective coating materials could be easily detached from the planar Zn foil, which results in uneven current density and dendrite growth.…”