Multi-strategy synergistic in-situ constructed gel electrolyte-binder system for high-performance lithium-ion batteries with Si-based anode

Silicon-based material have been considered as the most competitive candidate for next-generation anode in lithium-ion batteries (LIBs) due to its high specific energy density, natural abundance and attractive operating voltage. However, silicon-based anodes generally undergo significant volume changes and structural collapse during cycling, resulting in limited battery lifespan. Herein, a multi-strategy optimized in-situ gel electrolyte-binder system (GEBS) is rationally constructed, and electrochemical performances of the LIBs with Silicon-Graphite (Si-Gr) anodes are systematically evaluated by half-cell and full-cells. The in-situ generated polymer skeleton and improved interfacial compatibility of the GEBS effectively preserve the electrode structural integrity. Compared with the commercial liquid electrolyte , the volume change of the anode cycled with GEBS is suppressed from 208 % to 126 %. Benefiting from these merits, the full-cell with LiFePO 4 cathode displays stable cycling stability with the capacity retention of 96.8 % after 260 cycles. Besides, the reversible capacity of the LiNi 0.6 Co 0.2 Mn 0.2 O 2 ║Si-Gr full-cell is as high as 121.7 mAh g −1 after 200 cycles (capacity retention of 85.1 %), and the GEBS also exhibits obvious dominance at 55°C. This contribution effectively integrates multiple optimization strategies for Si-based anode and provides a feasible solution to address the challenge of its practical application in LIBs.