Publication date: 10th April 2024
Solid-state batteries based on a ceramic electrolyte and lithium metal anode promise to transform battery safety and energy density, but both charging and discharging rates are limited to below what is required. On discharge, voids form in the lithium metal at the Li/solid electrolyte interface due to limited Li metal creep at practical stack pressures and under practical current densities. These voids accumulate on cycling, leading to detachment of the Li anode and consequently high local currents during charge, triggering the growth of dendrites (filaments of Li metal that penetrate the ceramic electrolyte) resulting in short-circuit and cell failure. Furthermore, even without any prior voiding, charging currents are limited to levels too low for practical applications by dendrite formation. Important efforts are being made to understand dendrites in ceramic electrolytes and to mitigate them.
We describe the formation and progression of lithium dendrites, informed by observing dendritic cracks operando using X-ray computed tomography (XCT). Dendrites are found to follow a two-stage process of initiation then propagation, with distinct mechanisms for each. Initiation occurs in sub-surface pores where pressure builds to exceed the local fracture strength at the grain boundaries, by the mechanism of slow lithium extrusion. Propagation involves dry cracks, with Li driving the crack forward from the rear by a wedge-opening mechanism, rather than lithium at the crack tip, as had often been assumed previously. Informed by the description of dendrite cracks, we control the microstructure of an Argyrodite (Li6PS5Cl) solid electrolyte and examine the impact of different microstructures on the dendrites. These studies consider how microstructure influences critical current densities for dendrite growth.
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