Practical insights into high-temperature storage of lithium-rich layered oxide cathodes

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ID: 328893
2026
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Abstract
Abstract Lithium-rich layered oxides (LRLOs) deliver exceptional gravimetric energy density (>1000 Wh kg−1 at 4.8 V) via anion redox reactions, but inherently suffer from low volumetric energy density (VED) due to Li-rich phase and inherent porous granular architecture. In practical industrial applications, the operating voltage window is strictly limited to ∼4.5 V to ensure long-term durability and safety, which further exacerbates the VED deficiency. To bridge this gap, industrial wide distribution composite strategies involving blending large polycrystalline matrices with small polycrystalline (PP) or single-crystalline (PS) interstitial fillers can improve electrode packing density. Although PP offers superior rate capability and cost-effectiveness, it suffers from severe high-temperature (HT) storage instability. In this study, we reveal a cathode-dominated failure driven by accelerated ligand-to-metal charge transfer (LMCT) that activates lattice oxygen, prompting their transformation into highly reactive O-O dimers. In the PP route, abundant intergranular boundaries act as nucleation sites, triggering a destructive feedback loop of secondary cracking, gas release, and detrimental phase transitions. Based on these mechanistic insights, we propose a targeted first-cycle formation voltage regulation strategy to thermodynamically suppress excessive initial oxygen activation. Validated in 60 Ah-level cells, this approach effectively mitigates intergranular degradation and significantly extends the HT storage lifespan of PP cathodes, thus supporting the practical application of high-VED LRLOs.
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Authors Kang Zhang, Chunpu Li, Yuan Tian, Changxu Wu, Yizhen Huang, Li Li, Yilong Chen, Lianpeng Li, Wen Jiao, Na Liu, Qingsong Wang, Maolin Yang, Chongheng Shen, Yu Qiao, Shi‐Gang Sun
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Journal national science review
Year 2026
DOI
10.1093/nsr/nwag596
URL
https://academic.oup.com/nsr/advance-article-pdf/doi/10.1093/nsr/nwag596/71088940/nwag596.pdf
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