Construction of a High-Performance Composite Solid Electrolyte Through In-Situ Polymerization within a Self-Supported Porous Garnet Framework
An‐Giang Nguyen, Min‐Ho Lee, Jaekook Kim, Chan‐Jin Park
Abstract
Abstract Composite solid electrolytes (CSEs) have emerged as promising candidates for safe and high-energy–density solid-state lithium metal batteries (SSLMBs). However, concurrently achieving exceptional ionic conductivity and interface compatibility between the electrolyte and electrode presents a significant challenge in the development of high-performance CSEs for SSLMBs. To overcome these challenges, we present a method involving the in-situ polymerization of a monomer within a self-supported porous Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZT) to produce the CSE. The synergy of the continuous conductive LLZT network, well-organized polymer, and their interface can enhance the ionic conductivity of the CSE at room temperature. Furthermore, the in-situ polymerization process can also construct the integration and compatibility of the solid electrolyte–solid electrode interface. The synthesized CSE exhibited a high ionic conductivity of 1.117 mS cm −1 , a significant lithium transference number of 0.627, and exhibited electrochemical stability up to 5.06 V vs. Li/Li + at 30 °C. Moreover, the Li|CSE|LiNi 0.8 Co 0.1 Mn 0.1 O 2 cell delivered a discharge capacity of 105.1 mAh g −1 after 400 cycles at 0.5 C and 30 °C, corresponding to a capacity retention of 61%. This methodology could be extended to a variety of ceramic, polymer electrolytes, or battery systems, thereby offering a viable strategy to improve the electrochemical properties of CSEs for high-energy–density SSLMBs.