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Vol. 16 (2024)

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

https://doi.org/10.1007/s40820-023-01294-0
An‑Giang Nguyen
Department of Materials Science and Engineering, Chonnam National University, 77 Yongbong‑ro, Buk‑gu, Gwangju 61186, South Korea
Min‑Ho Lee
Department of Materials Science and Engineering, Chonnam National University, 77 Yongbong‑ro, Buk‑gu, Gwangju 61186, South Korea
Jaekook Kim
Department of Materials Science and Engineering, Chonnam National University, 77 Yongbong‑ro, Buk‑gu, Gwangju 61186, South Korea
Chan‑Jin Park
Department of Materials Science and Engineering, Chonnam National University, 77 Yongbong‑ro, Buk‑gu, Gwangju 61186, South Korea

Corresponding Author: Chan‑Jin Park

parkcj@jnu.ac.kr

Nano-Micro Letters, Vol. 16 (2024), Article Number: 83

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 Li6.4La3Zr1.4Ta0.6O12 (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|LiNi0.8Co0.1Mn0.1O2 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.


Highlights:
1 A scalable tape-casting method produces self-supported porous Li6.4La3Zr1.4Ta0.6O12.
2 Combining the in-situ polymerization approach, a composite solid electrolyte with superior electrochemical properties is fabricated.
3 Solid-state Li|CSE|LiNi0.8Co0.1Mn0.1O2 cells show remarkable cyclability and rate capability.
4 LiF-and B-rich interphase layers mitigate interfacial reactions, enhancing solid-state battery performance.

Keywords

Scalable tape-casting method Self-supported porous Li6.4La3Zr1.4Ta0.6O12 Composite solid electrolyte LiF-and B-rich interphase layers
Nguyen, An‑Giang, Min‑Ho Lee, Jaekook Kim, and Chan‑Jin Park. 2024. “Construction of a High-Performance Composite Solid Electrolyte Through In-Situ Polymerization Within a Self-Supported Porous Garnet Framework”. Nano-Micro Letters 16 (January):83. https://doi.org/10.1007/s40820-023-01294-0.
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