Jiechen Song,Yuxing Xu,Yuncheng Zhou,Rui He,Ai-Jia Wei,Qiangqiang Tan
Solid-state lithium metal batteries with poly(ethylene glycol) acrylates (PEGAs) solid electrolytes are considered as one of the promising candidates for next generation power sources. Constructing composite solid electrolytes (CSEs) by adding Li1.3Al0.3Ti1.7(PO4)3 (LATP) particles into PEGAs matrix is a fantastic way to improve the overall electrochemical properties. However, the inorganic LATP particles tend to agglomerate together in the organic PEGAs matrix. Designing LATP into 3D porous oxide electrolyte framework can address the agglomeration issue effectively, but the preparation of the LATP framework is always complicated to operate and difficult to reproduce on a large scale. In this work, a scalable CSE with PEGAs matrix and LATP framework is directly prepared on cathode by integrating with polyvinylidene difluoride (PVDF) and organic solvent, which is friendly to operate and matches the production of the mainstream LIBs. The designed CSE generates a fantastic conductivity of 0.22 mS cm-1 and Li+ transference number (tLi+ = 0.60) at room temperature. The Li/Li symmetric cell with the designed CSE can cycle steadily for 1645 h at 0.1 mA cm-2 and room temperature. Li/LiFePO4 full cells are assembled to assess battery performance, which delivers excellent stable discharge capacity (146.7 mAh g-1 at 0.5 C) and cycling stability with a capacity retention of 96.9% at 0.5 C after 300 cycles at room temperature. The work addresses the issue of hard reproduction of 3D porous oxide electrolyte framework and provides a CSE with 3D porous LATP framework having a high development potential and its feasible scale-up preparation method.
Zhengpeng Song,Haotong Li,Fei Zheng,Husitu Lin,Jing Liu,Wei Liu,Guohua Sun,Xia Tao
Ceramic Li1.3Al0.3Ti1.7(PO4)3 (LATP) with high ionic conductivity and stability in ambient atmosphere is considered to be potent as a solid-state electrolyte of solid-state lithium metal batteries (SSLMBs), but its huge interfacial impedance with electrodes and the unwanted Ti4+-mediated reduction reaction caused by the lithium (Li) metal anode greatly limit its application in LMBs. Herein, a composite polymer electrolyte (CPET) was integrated by in situ gelation of dual-permeable 1, 3-dioxolane (DOL) in the tandem framework composed of the commercial cellulose membrane TF4030 and a porous three-dimensional (3D) skeleton-structured LATP. The in situ gelled DOL anchored in the tandem framework ensured nice interfacial contact between the as-prepared CPET and electrodes. The introduction of the porous 3D LATP endowed CPET the increased lithium-ion migration number (tLi+) of 0.70, a wide electrochemical stability window (ESW) of 4.86 V, and a high ionic conductivity of 1.16 × 10–4 S cm–1 at room temperature (RT). Meanwhile, the side reaction of the LATP/Li metal was adequately restrained by inserting TF4030 between the porous LATP and Li anode. Profiting from the superb interfacial stability and the enhanced ionic transport capacity of CPET, Li/Li batteries based on the optimal CPET (CPET2) cycled over 2000 h at 20∼30 °C smoothly. Moreover, solid-state LiFePO4 (LFP)/Li with CPET2 exhibited excellent electrochemical performance with a capacity retention ratio of 72.2% after 400 cycles at 0.5C. This work offers an integrated strategy to guide the fabrication of a highly conductive solid electrolyte and a stable interface design for high-performance SSLMBs.
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