A brightener-inspired polymer interphase enables highly reversible aqueous Zn anodes via suppressing side-reactions and manipulating the nucleation process.

The surface chemistry of solid electrolyte interphase is one of the critical factors that govern the cycling life of rechargeable batteries. However, this chemistry is less explored for zinc anodes, owing to their relatively high redox potential and limited choices in electrolyte. Here, we report the observation of a zinc fluoride-rich organic/inorganic hybrid solid electrolyte interphase on zinc anode, based on an acetamide-Zn(TFSI)2 eutectic electrolyte. A combination of experimental and modeling investigations reveals that the presence of anion-complexing zinc species with markedly lowered decomposition energies contributes to the in situ formation of an interphase. The as-protected anode enables reversible (~100% Coulombic efficiency) and dendrite-free zinc plating/stripping even at high areal capacities (>2.5 mAh cm‒2), endowed by the fast ion migration coupled with high mechanical strength of the protective interphase. With this interphasial design the assembled zinc batteries exhibit excellent cycling stability with negligible capacity loss at both low and high rates.

In-situ constructing multifunctional solid electrolyte interphase (SEI) for Zn anode is promising to address the dendrite growth and side reactions (corrosion and hydrogen evolution) in aqueous Zn-ion batteries. However, there...

Low ionic conductivity at room temperature and limited electrochemical window of poly(ethylene oxide) (PEO) are the bottlenecks restricting its further application in high‐energy density lithium metal battery. Herein, a differentiated salt designed multilayered PEO‐based solid polymer electrolyte (DSM‐SPE) is exploited to achieve excellent electrochemical performance toward both the high‐voltage LiCoO2 cathode and the lithium metal anode. The LiCoO2/Li metal battery with DSM‐SPE displays a capacity retention of 83.3% after 100 cycles at 60 °C with challenging voltage range of 2.5 to 4.3 V, which is the best cycling performance for high‐voltage (≥4.3 V) LiCoO2/Li metal battery with PEO‐based electrolytes up to now. Moreover, the Li/Li symmetrical cells present stable and low polarization plating/stripping behavior (less than 80 mV over 600 h) at current density of 0.25 mA cm−2 (0.25 mAh cm−2). Even under a high‐area capacity of 2 mAh cm−2, the profiles still maintain stable. The pouch cell with DSM‐SPE exhibits no volume expansion, voltage decline, ignition or explosion after being impaled and cut at a fully charged state, proving the excellent safety characteristic of the DSM‐SPE‐based lithium metal battery.