Stable operation of highly loaded pure Si-Fe anode under ambient pressure via carboxy silane-directed robust solid electrolyte interphase

Incorporation of higher content Si anode material beyond 5 wt% to Li-ion batteries (LIBs) is challenging, owing to large volume change, swelling, and solid electrolyte interphase (SEI) instability issues. Herein, a strategy of diacetoxydimethylsilane (DAMS) additive-directed SEI stabilization is proposed for a stable operation of Si-0.33FeSi2 (named as Si-Fe) anode without graphite, which provides siloxane inorganics and organics enrichment that compensate insufficient passivation of fluoroethylene carbonate (FEC) additive and reduce a dependence on FEC. Unprecedented stable cycling performance of highly loaded (3.5 mA h cm−2) pure Si-Fe anode is achieved with 2 wt% DAMS combined with 9 wt% FEC additives under ambient pressure, yielding high capacity 1270 mA h g−1 at 0.5 C and significantly improved capacity retention of 81% after 100 cycles, whereas short circuit and rapid capacity fade occur with FEC only additive. DAMS-directed robust SEI layer dramatically suppresses swelling and particles crossover through separator, and therefore prevents short circuit, demonstrating a possible operation of pure Si or Si-dominant anodes in the next-generation high-energy-density and safe LIBs.