Ultralong Cycling and Interfacial Regulation of Bilayer Heterogeneous Composite Solid-State Electrolytes in Lithium Metal Batteries

• Published in: ACS applied materials & interfaces 2024-07, Vol.16 (26), p.33578-33589
• Main Authors: Wei, Lai, Xu, Xin, Xi, Kang, Lei, Yue, Cheng, Xiang, Shi, Xiaobei, Wu, Haihua, Gao, Yunfang
• Format: Article
• Language: English
• Subjects: Energy, Environmental, and Catalysis Applications
• ISSN: 1944-8244; 1944-8252; 1944-8252
• DOI: 10.1021/acsami.4c06026

Under the background of “carbon neutral”, lithium-ion batteries (LIB) have been widely used in portable electronic devices and large-scale energy storage systems, but the current commercial electrolyte is mainly liquid organic compounds, which have serious safety risks. In this paper, a bilayer heterogeneous composite solid-state electrolyte (PLPE) was constructed with the 3D LiX zeolite nanofiber (LiX-NF) layer and in-situ interfacial layer, which greatly extends the life span of lithium metal batteries (LMB). LiX-NF not only offers a continuous fast path for Li+, but also zeolite’s Lewis acid–base interaction can immobilize large anions, which significantly improves the electrochemical performance of the electrolyte. In addition, the in-situ interfacial layer at the electrode–electrolyte interface can effectively facilitate the uniform deposition of Li+ and inhibit the growth of lithium dendrites. As a result, the Li/Li battery assembled with PLPE can be stably cycled for more than 2500 h at 0.1 mA cm–2. Meanwhile, the initial discharge capacity of the LiFePO4/PLPE/Li battery can be 162.43 mAh g–1 at 0.5 C, and the capacity retention rate is 82.74% after 500 cycles. These results emphasize that this bilayer heterogeneous composite solid-state electrolyte has distinct properties and shows excellent potential for application in LMB.