Stabilizing Silicon Anode Chemistry for Long Cycle and Calendar Life Electrodes

Sunday, 13 October 2019: 12:20
Room 219 (The Hilton Atlanta)
B. Han (Argonne National Laboratory), C. Liao, F. Dogan (Argonne National Lab), S. E. Trask, S. Lapidus, J. T. Vaughey, and B. Key (Argonne National Laboratory)
Replacing traditional graphite anode by Si anode can greatly improve the energy density of lithium-ion batteries. However, the large volume expansion and the formation of highly reactive lithium silicides during charging cause the continuous lithium and electrolyte consumption as well as the fast decay of Si anodes. In this work, by formulating new electrolytes and additives, we demonstrate lifetime stabilization of the anode chemistry during the initial lithiation process. Using solid-state nuclear magnetic resonance spectroscopy, we show that stabilization suppresses the detrimental chemical reactions between the lithium silicides and common electrolyte solvents as well as binders. Formulated electrolytes were tested in commercially relevant electrodes, which show higher capacity, superior cyclability, and higher coulombic efficiencies in both half-cell and full-cell configurations when compared with standard electrolytes. We show an improvement in capacity retention from ~25% after 270 cycles to ~60% and a consistent 0.2%+ improvement in coulombic efficiencies in full cells when compared to state of the art baselines with silicon anodes. Post-electrochemistry characterizations demonstrate the mechanistic details silicon anion stabilization. This study opens a new and simple way to stabilize silicon anodes to enable widespread application of Si anodes for lithium-ion batteries.