Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide
Abstract
Lithium-rich nickel-manganese-cobalt (LirNMC) layered material is a promising cathode for lithium-ion batteries thanks to its large energy density enabled by coexisting cation and anion redox activities. It however suffers from a voltage decay upon cycling, urging for an in-depth understanding of the particle-level structure and chemical complexity. In this work, we investigate the Li1.2Ni0.13Mn0.54Co0.13O2 particles morphologically, compositionally, and chemically in three-dimensions. While the composition is generally uniform throughout the particle, the charging induces a strong depth dependency in transition metal valence. Such a valence stratification phenomenon is attributed to the nature of oxygen redox which is very likely mostly associated with Mn. The depth-dependent chemistry could be modulated by the particles’ core-multi-shell morphology, suggesting a structural-chemical interplay. These findings highlight the possibility of introducing a chemical gradient to address the oxygen-loss-induced voltage fade in LirNMC layered materials.
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES); National Key Research and Development Program of China; National Science Foundation (NSF)
- OSTI Identifier:
- 1735389
- Alternate Identifier(s):
- OSTI ID: 1737442; OSTI ID: 1779170
- Report Number(s):
- BNL-220716-2020-JAAM
Journal ID: ISSN 2041-1723; 6342; PII: 20198
- Grant/Contract Number:
- SC0012704; AC02-76SF00515; 2016YFA0400900; ECCS-1542152
- Resource Type:
- Published Article
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Name: Nature Communications Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; batteries; lithium-rich layered; spectro-imaging
Citation Formats
Zhang, Jin, Wang, Qinchao, Li, Shaofeng, Jiang, Zhisen, Tan, Sha, Wang, Xuelong, Zhang, Kai, Yuan, Qingxi, Lee, Sang-Jun, Titus, Charles J., Irwin, Kent D., Nordlund, Dennis, Lee, Jun-Sik, Pianetta, Piero, Yu, Xiqian, Xiao, Xianghui, Yang, Xiao-Qing, Hu, Enyuan, and Liu, Yijin. Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide. United Kingdom: N. p., 2020.
Web. doi:10.1038/s41467-020-20198-w.
Zhang, Jin, Wang, Qinchao, Li, Shaofeng, Jiang, Zhisen, Tan, Sha, Wang, Xuelong, Zhang, Kai, Yuan, Qingxi, Lee, Sang-Jun, Titus, Charles J., Irwin, Kent D., Nordlund, Dennis, Lee, Jun-Sik, Pianetta, Piero, Yu, Xiqian, Xiao, Xianghui, Yang, Xiao-Qing, Hu, Enyuan, & Liu, Yijin. Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide. United Kingdom. https://doi.org/10.1038/s41467-020-20198-w
Zhang, Jin, Wang, Qinchao, Li, Shaofeng, Jiang, Zhisen, Tan, Sha, Wang, Xuelong, Zhang, Kai, Yuan, Qingxi, Lee, Sang-Jun, Titus, Charles J., Irwin, Kent D., Nordlund, Dennis, Lee, Jun-Sik, Pianetta, Piero, Yu, Xiqian, Xiao, Xianghui, Yang, Xiao-Qing, Hu, Enyuan, and Liu, Yijin. Fri .
"Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide". United Kingdom. https://doi.org/10.1038/s41467-020-20198-w.
@article{osti_1735389,
title = {Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide},
author = {Zhang, Jin and Wang, Qinchao and Li, Shaofeng and Jiang, Zhisen and Tan, Sha and Wang, Xuelong and Zhang, Kai and Yuan, Qingxi and Lee, Sang-Jun and Titus, Charles J. and Irwin, Kent D. and Nordlund, Dennis and Lee, Jun-Sik and Pianetta, Piero and Yu, Xiqian and Xiao, Xianghui and Yang, Xiao-Qing and Hu, Enyuan and Liu, Yijin},
abstractNote = {Lithium-rich nickel-manganese-cobalt (LirNMC) layered material is a promising cathode for lithium-ion batteries thanks to its large energy density enabled by coexisting cation and anion redox activities. It however suffers from a voltage decay upon cycling, urging for an in-depth understanding of the particle-level structure and chemical complexity. In this work, we investigate the Li1.2Ni0.13Mn0.54Co0.13O2 particles morphologically, compositionally, and chemically in three-dimensions. While the composition is generally uniform throughout the particle, the charging induces a strong depth dependency in transition metal valence. Such a valence stratification phenomenon is attributed to the nature of oxygen redox which is very likely mostly associated with Mn. The depth-dependent chemistry could be modulated by the particles’ core-multi-shell morphology, suggesting a structural-chemical interplay. These findings highlight the possibility of introducing a chemical gradient to address the oxygen-loss-induced voltage fade in LirNMC layered materials.},
doi = {10.1038/s41467-020-20198-w},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United Kingdom},
year = {2020},
month = {12}
}
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