Progress and Perspective of Ceramic/Polymer Composite Solid Electrolytes for Lithium Batteries

Abstract

Solid composite electrolytes (SCEs) that combine the advantages of solid polymer electrolytes (SPEs) and inorganic ceramic electrolytes (ICEs) present acceptable ionic conductivity, high mechanical strength, and favorable interfacial contact with electrodes, which greatly improve the electrochemical performance of all‐solid‐state batteries compared to single SPEs and ICEs. However, there are many challenges to overcome before the practical application of SCEs, including the low ionic conductivity less than 10−3 S cm−1 at ambient temperature, poor interfacial stability, and high interfacial resistance, which greatly restrict the room temperature performance. Herein, the advances of SCEs applied in all‐solid‐state lithium batteries are presented, including the Li ion migration mechanism of SCEs, the strategies to enhance the ionic conductivity of SCEs by various morphologies of ICEs, and construction methods of the low resistance and stable interfaces of SCEs with both cathode and anode. Finally, some typical applications of SCEs in lithium batteries are summarized and future development directions are prospected. This work presents how it is quite significant to further enhance the ionic conductivity of SCEs by developing the novel SPEs with the special morphology of ICEs for advanced all‐solid‐state lithium batteries.

Recent Progress in Designing Stable Composite Lithium Anodes with Improved Wettability

“…They also show good thermal stability, high mechanical rigidity, and nonflammability. [110][111][112] Common SSEs include polymer electrolytes, [113][114][115] polymer-inorganic composite electrolytes, [116][117][118] and inorganic electrolytes. [119][120][121] Amongst these, inorganic electrolytes have received great attention due to their high ionic conductivity and extremely high Young's modulus, which can enhance the safety of Li-metal batteries.…”

Ultra-high throughput manufacturing method for composite solid-state electrolytes

“…The polymer helps obtain a large and stable coating window so that web speeds and thus film thicknesses can be varied over a wide range. At the same time, use of a polymer is an accepted approach to solving adhesion and mechanical stability issues in solid-state battery technology ( Yao et al, 2019 ; Li et al, 2020 ). The application of heat during calendaring results in dense films with excellent adhesion between the ceramic and polymer as the current collector.…”

“…The work of Li et al. provides a good overview of composite systems that range from 1wt% to 70wt% content of inorganic lithium-ion conducting materials ( Li et al, 2020 ). The optimal choice depends strongly on size and shape of the fillers and the resulting morphology.…”

Manufacturing Strategies for Solid Electrolyte in Batteries

“…The CSEs consisting of polymer and inorganic portions are developed to achieve satisfactory comprehensive properties and exceptional synergistic effects compared to the single-component electrolyte. Due to the presence of polymer, the manufacturing strategies of the CSEs are similar to that of SPEs, which have been reported in the previous reviews (Commarieu et al, 2018;Liu et al, 2018;Tan et al, 2018;Li et al, 2020). One of the most popular technologies to prepare CSEs is electrospinning, which produces interlaced and highly porous nanofibers with a large surface-to-volume ratio and improved mechanical strength due to the entanglement and reinforcing effects (Cavaliere et al, 2011;Wootthikanokkhan et al, 2015;Carli et al, 2019).…”