Aqueous zinc (Zn)-ion batteries are considered very promising in grid-scale energy storage systems. However, the dendrite, corrosion, and H2 evolution issues of Zn anode have restricted their further applications. Herein, to solve these issues, a hydrophilic layer, consisting of a covalent organic polymer (COP) and carboxylmethyl cellulose (CMC), is designed to in situ construct a multifunctional quasi-gel (COP-CMC/QG) interface between Zn metal and the electrolyte. The COP-CMC/QG interface can significantly improve the rechargeability of the Zn anode through enhancing Zn2+ transport kinetics, guiding uniform nucleation, and suppressing Zn corrosion and H2 evolution. As a result, the COP-CMC-Zn anode exhibits a reduced overpotential (12 mV at 0.25 mA cm–2), prolonged cycle life (over 4000 h at 0.25 mA cm–2 and 2000 h at 5 mA cm–2 in symmetrical cells), and elevated full-cell (Zn/MnO2) performance. This work provides an efficient approach to achieve long-life Zn metal anodes and paves the way toward high-performance Zn-based and other metal-ion batteries.

A disordered phase in Li-deposit nanostructure is greatly attractive, but plagued by the uncontrollable and unstable growth, and the nanoscale characterization in the structure. Here, fully characterized in cryogenic transmission electron microscopy (cryo-TEM), more robust amorphous-Li (ALi) clusters are revealed and effectively regulated on heteroatom-activating electronegative sites and an advanced solid electrolyte interphase (SEI) layer. Heteroatom-activating electronegative sites capably enhance the electrostatic interaction of Li + and heteroatom-doping graphene-like film (HDGs), meaning lower Li diffusion barrier and larger binding energy that is confirmed by small nucleation overpotentials of 13.9 and 10 mV at 0.1 mA cm −2 in the fluoroethylene carbonate-adding ester-based (FEC-ester) and LiNO 3 -adding ether-based (LiNO 3 -ether) electrolytes. Orderly multilayer SEI structure comprised of inorganic-rich components enables fast ion transports and durable capabilities to construct highly reversible and long-term plating/stripping cycling. ALi cluster anodes exhibit non-crystalline morphologies and perform ultrastable dendrite-free cycling over 2800 times. Stable ALi clusters are also grown in LiFePO 4 (LFP) (LFP-ALi-HDGs-N||LiFePO 4 [LFP]) full cells with advantageous capacities up to 165.5 and 164.3 mAh g −1 in these optimized electrolytes at 0.1 C; the remarkable capacity retentions maintain to 93% and 91% after 150 cycles at 0.2 C. Structure viability, electrochemical reversibility, and excellent performance in ALi clusters are effectively regulated.

No abstract