Journal
SCIENCE ADVANCES
Volume 8, Issue 47, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.add5189
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Funding
- National Key Research and Development Program [2021YFB2500300]
- National Natural Science Foundation of China [22108151, 22075029, 21805161, 21808124, 21825501, U1801257]
- China Postdoctoral Science Foundation [BX2021135, 2021TQ0164, 2021 M701827]
- Beijing Municipal Natural Science Foundation [Z20J00043]
- Shuimu Tsinghua Scholar Program of Tsinghua University
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The surface oxygen instability of Li-rich Mn-based oxide (LRMO) cathodes is identified as the cause for interfacial degradation in all-solid-state lithium batteries (ASSBs). By replacing surface oxygen with sulfite, overoxidation and interfacial degradation can be effectively prevented, leading to high capacity and cycling stability.
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 (similar to 248 mAh g(-1), 1.1 mAh cm(-2); similar to 225 mAh g(-1), 2.9 mAh cm(-2)) 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.
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