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

Abstract

Layered LiNixCoyMn1–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 PO43- is preferentially adsorbed on transition metal sites, stabilizing both the transition metal ions and oxygen ions on the surface againstmore » 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.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [2];  [3];  [4];  [5];  [1];  [1];  [4];  [1]
  1. Tsinghua Univ., Beijing (China)
  2. Tsinghua Univ., Beijing (China); Tianjin Lishen Battery Joint-Stock Co., Ltd. (China)
  3. Tianjin Lishen Battery Joint-Stock Co., Ltd. (China)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Natural Science Foundation of China (NSFC); Ministry of Science and Technology of the People’s Republic of China (MOST)
OSTI Identifier:
1880828
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 96; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; high voltage; surface decoration; thermal runaway; NCM622; parasitic reaction

Citation Formats

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, and He, Xiangming. Targeted masking enables stable cycling of LiNi0.6Co0.2Mn0.2O2 at 4.6V. United States: N. p., 2022. Web. doi:10.1016/j.nanoen.2022.107123.
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. Targeted masking enables stable cycling of LiNi0.6Co0.2Mn0.2O2 at 4.6V. United States. https://doi.org/10.1016/j.nanoen.2022.107123
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, and He, Xiangming. Fri . "Targeted masking enables stable cycling of LiNi0.6Co0.2Mn0.2O2 at 4.6V". United States. https://doi.org/10.1016/j.nanoen.2022.107123. https://www.osti.gov/servlets/purl/1880828.
@article{osti_1880828,
title = {Targeted masking enables stable cycling of LiNi0.6Co0.2Mn0.2O2 at 4.6V},
author = {Hu, Qiao and He, Yufang and Ren, Dongsheng and Song, Youzhi and Wu, Yanzhou and Liang, Hongmei and Gao, Jinhui and Xu, Gang and Cai, Jiyu and Li, Tianyi and Xu, Hong and Wang, Li and Chen, Zonghai and He, Xiangming},
abstractNote = {Layered LiNixCoyMn1–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 PO43- 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.},
doi = {10.1016/j.nanoen.2022.107123},
journal = {Nano Energy},
number = ,
volume = 96,
place = {United States},
year = {Fri Mar 11 00:00:00 EST 2022},
month = {Fri Mar 11 00:00:00 EST 2022}
}

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