Construction of a High-Performance Composite Solid Electrolyte Through In-Situ Polymerization within a Self-Supported Porous Garnet Framework

• Published in: Nano-micro letters 2024-12, Vol.16 (1), p.83-15, Article 83
• Main Authors: Nguyen, An-Giang, Lee, Min-Ho, Kim, Jaekook, Park, Chan-Jin
• Format: Article
• Language: English
• Subjects: Compatibility; Composite solid electrolyte; Density; Electrochemical analysis; Electrodes; Electrolytes; Electrolytic cells; Engineering; Interface reactions; Ion currents; LiF-and B-rich interphase layers; Lithium batteries; Molten salt electrolytes; Nanoscale Science and Technology; Nanotechnology; Nanotechnology and Microengineering; Polymerization; Polymers; Room temperature; Scalable tape-casting method; Self-supported porous Li6.4La3Zr1.4Ta0.6O12; Solid electrolytes; Solid state; Solid-state batteries; Tape casting
• ISSN: 2311-6706; 2150-5551; 2150-5551
• DOI: 10.1007/s40820-023-01294-0

Highlights A scalable tape-casting method produces self-supported porous Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 . Combining the in-situ polymerization approach, a composite solid electrolyte with superior electrochemical properties is fabricated. Solid-state Li|CSE|LiNi 0.8 Co 0.1 Mn 0.1 O 2 cells show remarkable cyclability and rate capability. LiF-and B-rich interphase layers mitigate interfacial reactions, enhancing solid-state battery performance. 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.