Durable and Adjustable Interfacial Engineering of Polymeric Electrolytes for Both Stable Ni-Rich Cathodes and High-Energy Metal Anodes.

Chen, Yong; Cui, Yingyue; Wang, Simeng; Xiao, Ying; Niu, Jin; Huang, Jiajia; Wang, Feng; Chen, Shimou · Adv Mater · 2023

basic_science · Level V

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Abstract

Achieving stable cycling of high-voltage solid-state lithium metal batteries is crucial for next-generation rechargeable batteries with high energy density and high safety. However, the complicated interface problems in both cathode/anode electrodes preclude their practical applications hitherto. Herein, to simultaneously solve such interfacial limitations and obtain sufficient Li<sup>+</sup> conductivity in the electrolyte, an ultrathin and adjustable interface is developed at the cathode side through a convenient surface in situ polymerization (SIP), achieving a durable high-voltage tolerance and Li-dendrite inhibition. The integrated interfacial engineering fabricates a homogeneous solid electrolyte with optimized interfacial interactions that contributes to tame the interfacial compatibility between LiNi<sub>x</sub> Co<sub>y</sub> Mn<sub>z</sub> O<sub>2</sub> and polymeric electrolyte accompanied by anticorrosion of aluminum current collector. Further, the SIP enables a uniform adjustment of solid electrolyte composition by dissolving additives such as Na<sup>+</sup> and K<sup>+</sup> salts, which presents prominent cyclability in symmetric Li cells (>300 cycles at 5 mA cm<sup>-2</sup> ). The assembled LiNi<sub>0.8</sub> Co<sub>0.1</sub> Mn<sub>0.1</sub> O<sub>2</sub> (4.3 V)||Li batteries show excellent cycle life with high Coulombic efficiencies (>99%). This SIP strategy is also investigated and verified in sodium metal batteries. It opens a new frontier for solid electrolytes toward high-voltage and high-energy metal battery technologies.