Understanding and Controlling Structural Defects and Disordering in LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> Cathodes for Direct Recycling.
basic_science · Level V
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- Record sourced from PubMed, PMID 39433302.
- Also identified by DOI 10.1021/acsnano.4c10164.
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Abstract
Despite significant progress in recycling spent lithium-ion batteries (LIBs), nondestructive, direct recycling methods still face untenable discrepancies in multiple cathode chemistries, which primarily originate from a variety of structure stabilities during the recycling process. Through systematic investigation of the microstructure evolution during the relithiation treatment, we observed the inevitably induced defects and Li/Mn disordering in the LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> cathode, contributing to the sluggish Li<sup>+</sup> transport and irreversible capacity loss. Employing a defect engineering approach to achieve twin boundaries and preferred grain orientation, we show the regenerated cathodes demonstrate a substantial enhancement of Li<sup>+</sup> diffusion and cycling stability, retaining 97.4% capacity after 100 cycles and 87.96% after 200 cycles at C/3. This work not only elaborates on a systematic investigation of defect inducement and structural restoration mechanism but also provides an effective approach to directly recycle high-voltage spinel-type cathodes, contributing to the sustainability of next-generation LIBs.