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

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+ 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 LiNixCoyMnzO2 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+ and K+ salts, which presents prominent cyclability in symmetric Li cells (>300 cycles at 5 mA cm−2). The assembled LiNi0.8Co0.1Mn0.1O2 (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.

Polymer-based electrolytes for high-voltage solid-state lithium batteries

“…This figure is quoted with permission from Chen et al [87] Copyright 2023 Wiley. and room temperature ionic conductivity [85,86] . Surface in-situ polymerization (SIP) with optimized interface interactions can enhance interface compatibility between various cathodes and PEs, offering the potential for enduring high-voltage tolerance.…”

Interface Engineering for 3D Printed Energy Storage Materials and Devices

“…By means of both experimental and computational tools, interface engineering has been found to undoubtedly enhance the interface properties, optimize the overall structures, and ultimately achieve superior electrochemical energy storage. [71][72][73] Nanocompositing is one of the most promising experimental solutions that offer good opportunities in electrochemistry for both conventionally manufactured energy storage devices and 3D printed ones. [65,[74][75][76] The combinations of carbon and non-carbon lowdimensional materials, such as 1D and 2D materials, are regarded as efficient routes for nanocomposite electrodes, wherein a series of unprecedented electrochemical properties are manifested with enhanced interface properties.…”

Constructing host–guest recognition electrolytes promotes the Li+ kinetics in solid-state batteries

“…In addition, the instability of SPEs under high voltage has seriously hindered their practical applications. 6–8 There is increasing demand to develop novel materials, improve architectures, optimize conventional SPEs and understand Li + transport mechanisms in order to meet the requirements for energy storage in the future.…”