Targeted masking enables stable cycling of LiNi0.6Co0.2Mn0.2O2 at 4.6V

Hu, Qiao; He, Yufang; Ren, Dongsheng; Song, Youzhi; Wu, Yanzhou; Liang, Hongmei; Gao, Jinhui; Xu, Gang; Cai, Jiyu; Li, Tianyi; Xu, Hong; Wang, Li; Chen, Zonghai; He, Xiangming

doi:10.1016/j.nanoen.2022.107123

Targeted masking enables stable cycling of LiNi_0.6Co_0.2Mn_0.2O₂ at 4.6V

Journal Article · Fri Mar 11 00:00:00 EST 2022 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2022.107123· OSTI ID:1880828

Hu, Qiao ^[1]; He, Yufang ^[1]; Ren, Dongsheng ^[1]; Song, Youzhi ^[1]; Wu, Yanzhou ^[1]; Liang, Hongmei ^[1]; Gao, Jinhui ^[2]; Xu, Gang ^[3]; Cai, Jiyu ^[4]; Li, Tianyi ^[5]; Xu, Hong ^[1]; Wang, Li ^[1]; Chen, Zonghai ^[4]; He, Xiangming ^[1]

Tsinghua Univ., Beijing (China)
Tsinghua Univ., Beijing (China); Tianjin Lishen Battery Joint-Stock Co., Ltd. (China)
Tianjin Lishen Battery Joint-Stock Co., Ltd. (China)
Argonne National Lab. (ANL), Lemont, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Layered LiNi_xCo_yMn_1–x-yO₂ (NCM, or NCMxy(1-x-y)) is a dominant family of cathode materials for lithium-ion batteries (LIBs) due to its high energy density. Among all NCM cathode materials, NCM622 possess the optimal energy density at high potential (≥ 4.6 V vs. Li/Li⁺). However, the practical application of NCM622 at high voltage (≥ 4.6 V) is limited by its parasitic reactions and associated safety concerns. Completely physical isolation has been considered as the main approach to mitigate the parasitic reaction. It has also been previously demonstrated that the interface reaction has active site selectivity, and that the reactivity of the active sites can effectively suppressed by blocking the chemically active sites. Herein, a targeted masking by LiFePO₄ @C nanoplates is reported to unlock the stable performance of NCM622 up to 4.6 V vs. Li/Li⁺. The (targeted masked-NCM622)|graphite pouch cell shows 86.5% capacity retention after 1000 cycles and its maximum temperature during thermal runaway is dramatically reduced from 570 °C to 415 °C. Systematic in/ex situ characterizations, first-principles calculations and half/pouch targeted LiFePO₄@C covers the surface of NCM partcell evaluation prove that PO₄^3- is preferentially adsorbed on transition metal sites, stabilizing both the transition metal ions and oxygen ions on the surface against the ethylene carbonate-containing traditional electrolyte even under high voltage (≥ 4.6 V vs. Li/Li⁺). Furthermore, this work opens up new venue for rational design of high-performance cathode materials through a low-cost and scalable decoration process, and reveal a new understanding of interfacial activity of materials.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Ministry of Science and Technology of the People’s Republic of China (MOST); National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1880828

Journal Information:: Nano Energy, Journal Name: Nano Energy Vol. 96; ISSN 2211-2855

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

25 ENERGY STORAGE
NCM622
high voltage
parasitic reaction
surface decoration
thermal runaway

Targeted masking enables stable cycling of LiNi0.6Co0.2Mn0.2O2 at 4.6V

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Targeted masking enables stable cycling of LiNi_0.6Co_0.2Mn_0.2O₂ at 4.6V