All-solid-state sodium batteries promised low-cost grid energy storage but suffered from catastrophic short circuits caused by hidden metal dendrites; multi-physics phase-field modeling uncovers how mechanical grain boundaries channel dendrite penetration.
Sodium is vastly more abundant and cheaper than lithium, making all-solid-state sodium batteries the premier candidate to store renewable solar and wind energy on regional electrical grids.
Engineers assumed that rigid ceramic solid electrolytes would mechanically block metallic dendrites, yet experimental sodium cells consistently suffered sudden internal short circuits at modest charging currents.
This computational physics study develops an electrochemical-mechanical phase-field model simulating sodium electrodeposition along ceramic grain boundaries. The simulations prove that non-uniform interfacial stresses and electron leakage into grain boundary cracks drive intergranular dendrite propagation.
These phase-field insights provide battery engineers with quantitative design guidelines to engineer microstructurally uniform ceramic electrolytes, preventing dendrite growth and enabling long-lived grid-scale sodium energy storage.
Phase-Field Simulation of Dendrite Evolution in All-Solid-State Sodium Batteries during Cycling
Dendrite growth during cycling remains a critical challenge for all-solid-state batteries (SSBs), limiting the full realization of their inherent safety and high energy density. In particular, the mechanisms of continuous dendrite penetration during charge-discharge cycling remain poorly understood and are difficult to characterize experimentally. This study applies a phase-field model, informed by density functional theory calculations, to rationalize and visualize the dendrite penetration behaviors during cycling in sodium (Na) SSBs with pure Na or Na-Sb alloy anodes and polycrystalline NaSbS electrolyte. We show that dendrite stripping is intrinsically asymmetric with respect to plating due to grain boundary geometry, leading to the formation of isolated Na metal that persists between cycles. This residual Na metal becomes kinetically stabilized at grain-boundary junctions and is readily reactivated during subsequent plating, thereby accelerating and amplifying dendrite penetration. We further investigate the effects of applied voltage, solid-electrolyte microstructure, and anode chemistry on this phenomenon. These findings establish isolated Na metal as a key contributor for continued dendrite propagation in Na SSBs and provide design principles for stabilizing anode/electrolyte interfaces in Na SSBs.
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