Magnetic Force Dilatometry of Silicon-NMC622 Lithium-Ion Coin Cells: The Effects of Binder, Capacity Ratio, and Electrolyte Selection

Abstract

Operando cell expansion measurements on Si-NMC622 coin cells using a magnetic dilatometer were performed to understand the effects of electrode binder content, electrode formulation, negative-to-positive electrode capacity ratio (N/P ratio), and electrolyte selection on reversible and irreversible cell expansions. Our experiments reveal a complex relationship between cell properties, imparted by the selected cell parameters, and cell expansion. Reversible cell expansions scaled with cell discharge capacity and electrode mechanical properties, while irreversible cell expansions were sensitive to capacity fade, silicon utilization, and electrolyte decomposition mechanisms. Additionally, volumetric cell energy densities were calculated using the measured capacities and irreversible expansions over the life of the cells. We show that judicious selection of cell parameters can improve volumetric energy density after 200 charge/discharge cycles by approximately two-fold. Our work provides valuable insight, at an early stage of cell development, towards minimizing the effects of cell expansion on battery cell, pack, and module designs.