Accordion Strain Accommodation Mechanism within the Epitaxially Constrained Electrode AITranslate

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DOI：https://doi.org/10.1021/acsenergylett.8b00829

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The tremendous benefits of all-solid-state Li-ion batteries will only be reaped if the cycle-induced strain mismatch across the electrode/electrolyte interfaces can be managed at the atomic scale to ensure that structural coherency is maintained over the lifetime of the battery. We have discovered a unique strain accommodation mechanism within an epitaxially constrained high-performance bronze TiO2 (TiO2-B) electrode that relieves coherency stresses that arise upon Li insertion. In situ transmission electron microscopy observation reveals the formation of anatase shear bands within the TiO2-B crystal that play the same role that interface dislocations do to relieve growth stresses. While first-principles calculations indicate that anatase is the favored crystal structure of TiO2 in the lithiated state, its continued propagation is suppressed by the epitaxial constraints of the substrate. This discovery reveals an accordion-like mechanism relying on an otherwise undesirable structural transformation that can be exploited to manage the cyclic strain mismatch across the electrode/electrolyte interfaces that plague all solid-state batteries.