Critical Role of Pressure for Chemo-Mechanical-Induced Stability of Sodium Metal Battery Anodes

In this work we demonstrate that cell pressure controls the morphology and stability of electroplated sodium metal deposits on carbon black nucleation layers in ether-based electrolytes. At pressures below 500 kPa we observe the presence of three-dimensional Na nuclei accompanied by low Coulombic efficiencies (CEs less than 98%). Conversely, at pressures between 500 and 1272 kPa we observe smooth, planar Na deposits, high CEs up to 99.9%, and stable electrochemical cycling. Through a series of tests conducted at elevated current densities and with or without rest stages, our findings elucidate the balance of important competing time scales for creep and morphology evolution under pressure and the rate of charge transfer that determines Na morphology and stability. This highlights how chemo-mechanical effects at pressure ranges relevant for battery packaging in coin and pouch cells are key factors in the design and operation of Na metal batteries.