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Vol. 16 (2024)

12.6 μm-Thick Asymmetric Composite Electrolyte with Superior Interfacial Stability for Solid-State Lithium-Metal Batteries

https://doi.org/10.1007/s40820-024-01389-2
Zheng Zhang
Beijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
Jingren Gou
Beijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
Kaixuan Cui
Beijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
Xin Zhang
Beijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
Yujian Yao
Beijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
Suqing Wang
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510000, People’s Republic of China
Haihui Wang
Beijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, People’s Republic of China

Corresponding Author: Haihui Wang

cehhwang@tsinghua.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 181

Abstract

Solid-state lithium metal batteries (SSLMBs) show great promise in terms of high-energy–density and high-safety performance. However, there is an urgent need to address the compatibility of electrolytes with high-voltage cathodes/Li anodes, and to minimize the electrolyte thickness to achieve high-energy–density of SSLMBs. Herein, we develop an ultrathin (12.6 µm) asymmetric composite solid-state electrolyte with ultralight areal density (1.69 mg cm−2) for SSLMBs. The electrolyte combining a garnet (LLZO) layer and a metal organic framework (MOF) layer, which are fabricated on both sides of the polyethylene (PE) separator separately by tape casting. The PE separator endows the electrolyte with flexibility and excellent mechanical properties. The LLZO layer on the cathode side ensures high chemical stability at high voltage. The MOF layer on the anode side achieves a stable electric field and uniform Li flux, thus promoting uniform Li+ deposition. Thanks to the well-designed structure, the Li symmetric battery exhibits an ultralong cycle life (5000 h), and high-voltage SSLMBs achieve stable cycle performance. The assembled pouch cells provided a gravimetric/volume energy density of 344.0 Wh kg−1/773.1 Wh L−1. This simple operation allows for large-scale preparation, and the design concept of ultrathin asymmetric structure also reveals the future development direction of SSLMBs.


Highlights:
1 Ultra-thin asymmetric composite solid-state electrolytes with ultralight areal density were designed for solid-state lithium metal batteries, achieving interfacial stability to Li metal and high-voltage cathode.
2 The improved mechanical properties of the electrolyte contribute to the inhibition of Li dendrite growth was demonstrated by both experimental and theoretical simulations.
3 The assembled pouch cell exhibited a high gravimetric/volume energy density of 344.0 Wh kg−1/773.1 Wh L−1.

Keywords

Solid-state lithium metal batteries Composite solid-state electrolyte Ultrathin asymmetric structure Pouch cells
Zhang, Zheng, Jingren Gou, Kaixuan Cui, Xin Zhang, Yujian Yao, Suqing Wang, and Haihui Wang. 2024. “12.6 μm-Thick Asymmetric Composite Electrolyte With Superior Interfacial Stability for Solid-State Lithium-Metal Batteries”. Nano-Micro Letters 16 (April):181. https://doi.org/10.1007/s40820-024-01389-2.
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