Eliminating interfacial O-involving degradation in Li-rich Mn-based cathodes for all-solid-state lithium batteries.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 36427308.
- Also identified by DOI 10.1126/sciadv.add5189 and PMC identifier 9699669.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
In the pursuit of energy-dense all-solid-state lithium batteries (ASSBs), Li-rich Mn-based oxide (LRMO) cathodes provide an exciting path forward with unexpectedly high capacity, low cost, and excellent processibility. However, the cause for LRMO|solid electrolyte interfacial degradation remains a mystery, hindering the application of LRMO-based ASSBs. Here, we first reveal that the surface oxygen instability of LRMO is the driving force for interfacial degradation, which severely blocks the interfacial Li-ion transport and triggers fast battery failure. By replacing the charge compensation of surface oxygen with sulfite, the overoxidation and interfacial degradation can be effectively prevented, therefore achieving a high specific capacity (~248 mAh g<sup>-1</sup>, 1.1 mAh cm<sup>-2</sup>; ~225 mAh g<sup>-1</sup>, 2.9 mAh cm<sup>-2</sup>) and excellent long-term cycling stability of >300 cycles with 81.2% capacity retention at room temperature. These findings emphasize the importance of irreversible anion reactions in interfacial failure and provide fresh insights into constructing stable interfaces in LRMO-based ASSBs.