Enabling a scalable composite solid electrolyte via cathode-supported scale-up processing†
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Qiangqiang
Tan
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Abstract
Solid-state lithium metal batteries with poly(ethylene glycol) acrylate (PEGA) solid electrolytes are considered 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 the PEGA matrix is a fantastic way to improve their overall electrochemical properties. However, the inorganic LATP particles tend to agglomerate in the organic PEGA matrix. Designing LATP into a 3D porous oxide electrolyte framework can address the agglomeration issue effectively, but the preparation of the LATP framework is complicated and difficult to reproduce on a large scale. In this work, a scalable CSE with a PEGA matrix and LATP framework is directly prepared on a cathode by integrating with polyvinylidene difluoride (PVDF) and an organic solvent, which is friendly to operate and matches the production of 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. A Li/Li symmetric cell fabricated using the designed CSE can cycle steadily for 1645 h at 0.1 mA cm−2 and room temperature. Li/LiFePO4 full cells were assembled to assess battery performance, which delivers excellent stable discharge capacity (146.7 mA h g−1 at 0.5C) and cycling stability with a capacity retention of 96.9% at 0.5C after 300 cycles at room temperature. The work addresses the issue of difficult reproduction of a 3D porous oxide electrolyte framework and provides a CSE with a 3D porous LATP framework possessing a high development potential and its feasible scale-up preparation method.
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