Hao Xu,Shuai Liu,Zhiang Li,Fan Ding,Jie Liu,Weimin Wang,Kaikai Song,Ting Liu,Lina Hu
Solid polymer electrolytes (SPEs) have been considered the most promising separators for all-solid-state lithium metal batteries (ASSLMBs) due to their ease of processing and low cost. However, the practical applications of SPEs in ASSLMBs are limited by their low ionic conductivities and mechanical strength. Herein, we developed a three-dimensional (3D) interconnected MXene (Ti 3 C 2 T x ) network and Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) particles synergistically reinforced polyethylene oxide (PEO)-based SPE, where the association of Li + with ether-oxygen in PEO could be significantly weakened through the Lewis acid-base interactions between the electron-absorbing group (Ti–F, −O–) of Ti 3 C 2 T x and Li + . Besides, the TFSI − in lithium salts could be immobilized by hydrogen bonds from the Ti–OH of Ti 3 C 2 T x . The 3D interconnected Ti 3 C 2 T x network not only alleviated the agglomeration of inorganic fillers (LLZTO), but also improved the mechanical strength of composite solid electrolyte (CSE). Consequently, the assembled Li||CSE||Li symmetric battery showed excellent cycling stability at 35 ℃ (stable cycling over 3000 h at 0.1 mA cm −2 , 0.1 mAh cm −2 ) and −2 ℃ (stable cycling over 2500 h at 0.05 mA cm −2 , 0.05 mAh cm −2 ). Impressively, the LiFePO 4 ||CSE||Li battery showed a high discharge capacity of 145.3 mAh/g at 0.3 C after 300 cycles at 35 ℃. This rational structural design provided a new strategy for the preparation of high-performance solid-state electrolytes for lithium metal batteries.
Amin Chen,Na Li,Chenxu Sun,Yanmin Qin,Luyao Qi,Huipei Zhang,Haifeng Bao
Both inorganic solid electrolytes and organic polymer solid electrolytes face limitations in practical applications due to their shortcomings. Inorganic solid electrolytes suffer from high interface impedance and poor mechanical properties, while polymer solid electrolytes struggle with low Li-ion conductivity, thermal stability and electrochemical stability. To overcome the drawbacks of single phase solid electrolytes while utilizing their respective advantages, composite solid electrolytes have emerged as a popular research direction in recent years. Typical composite solid electrolytes feature inorganic filler particles dispersed in a polymer matrix. In this work, we introduce a novel non-flammable composite solid electrolyte with inorganic matrix and inorganic fillers. The composite solid electrolyte was prepared by integrating a 3D Si-Zr-O-C inorganic fiber film with Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) particles that have high ionic conductivity via a vacuum impregnation process, which is all-inorganic solid state electrolyte. This unique design of established network structure provides fast Li-ion transport channels, enabling high ionic conductivity (2.3 × 10 −4 S cm −1 at room temperature). Furthermore, the Si-Zr-O-C/LLZTO (SLTO) composite electrolyte also exhibits superior flexibility, thermal stability, and electrochemical stability. The SLTO composite solid electrolyte presents a promising electrolyte candidate for next generation lithium ion batteries.
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