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Title: High-Voltage Charging-Induced Strain, Heterogeneity, and Micro-Cracks in Secondary Particles of a Nickel-Rich Layered Cathode Material

Abstract

Nickel-rich layered materials LiNi 1-x-yMn xCo yO 2 are promising candidates for high-energy-density lithium-ion battery cathodes. Unfortunately, they suffer from capacity fading upon cycling, especially with high-voltage charging. It is critical to have a mechanistic understanding of such fade. Synchrotron-based techniques (including scattering, spectroscopy, and microcopy) and finite element analysis are utilized to understand the LiNi 0.6Mn 0.2Co 0.2O 2 material from structural, chemical, morphological, and mechanical points of view. The lattice structural changes are shown to be relatively reversible during cycling, even when 4.9 V charging is applied. However, local disorder and strain are induced by high-voltage charging. Nano-resolution 3D transmission X-ray microscopy data analyzed by machine learning methodology reveal that high-voltage charging induced significant oxidation state inhomogeneities in the cycled particles. Regions at the surface have a rock salt–type structure with lower oxidation state and build up the impedance, while regions with higher oxidization state are scattered in the bulk and are likely deactivated during cycling. In addition, the development of micro-cracks is highly dependent on the pristine state morphology and cycling conditions. Hollow particles seem to be more robust against stress-induced cracks than the solid ones, suggesting that morphology engineering can be effective in mitigating the crackmore » problem in these materials.« less

Authors:
 [1];  [2];  [3];  [4];  [3];  [2];  [2];  [5];  [6];  [7];  [3];  [8];  [9];  [7];  [10];  [10]; ORCiD logo [2];  [2];  [3]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Light Source; Nanjing Univ. of Aeronautics and Astronautics (China). School of Computer Science and Technology
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Light Source
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Light Source; Chinese Academy of Sciences (CAS), Beijing (China). Beijing Synchrotron Radiation Facility. Inst. of High Energy Physics
  5. Nanjing Univ. of Aeronautics and Astronautics (China). School of Computer Science and Technology
  6. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  7. Purdue Univ., West Lafayette, IN (United States). School of Mechanical Engineering
  8. Stanford Univ., CA (United States). Dept. of Computer Science
  9. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
  10. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Purdue Univ., West Lafayette, IN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1498873
Alternate Identifier(s):
OSTI ID: 1498588
Report Number(s):
BNL-211348-2019-JAAM
Journal ID: ISSN 1616-301X
Grant/Contract Number:  
SC0012704; AC02-76SF00515; DMR-1832613; DMR-1832707; DE‐SC0012704; DE‐AC02‐76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 18; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; data mining; finite element analysis; lithium ion batteries; nickel-rich layered; synchrotron characterization

Citation Formats

Mao, Yuwei, Wang, Xuelong, Xia, Sihao, Zhang, Kai, Wei, Chenxi, Bak, Seongmin, Shadike, Zulipiya, Liu, Xuejun, Yang, Yang, Xu, Rong, Pianetta, Piero, Ermon, Stefano, Stavitski, Eli, Zhao, Kejie, Xu, Zhengrui, Lin, Feng, Yang, Xiao-Qing, Hu, Enyuan, and Liu, Yijin. High-Voltage Charging-Induced Strain, Heterogeneity, and Micro-Cracks in Secondary Particles of a Nickel-Rich Layered Cathode Material. United States: N. p., 2019. Web. doi:10.1002/adfm.201900247.
Mao, Yuwei, Wang, Xuelong, Xia, Sihao, Zhang, Kai, Wei, Chenxi, Bak, Seongmin, Shadike, Zulipiya, Liu, Xuejun, Yang, Yang, Xu, Rong, Pianetta, Piero, Ermon, Stefano, Stavitski, Eli, Zhao, Kejie, Xu, Zhengrui, Lin, Feng, Yang, Xiao-Qing, Hu, Enyuan, & Liu, Yijin. High-Voltage Charging-Induced Strain, Heterogeneity, and Micro-Cracks in Secondary Particles of a Nickel-Rich Layered Cathode Material. United States. doi:10.1002/adfm.201900247.
Mao, Yuwei, Wang, Xuelong, Xia, Sihao, Zhang, Kai, Wei, Chenxi, Bak, Seongmin, Shadike, Zulipiya, Liu, Xuejun, Yang, Yang, Xu, Rong, Pianetta, Piero, Ermon, Stefano, Stavitski, Eli, Zhao, Kejie, Xu, Zhengrui, Lin, Feng, Yang, Xiao-Qing, Hu, Enyuan, and Liu, Yijin. Thu . "High-Voltage Charging-Induced Strain, Heterogeneity, and Micro-Cracks in Secondary Particles of a Nickel-Rich Layered Cathode Material". United States. doi:10.1002/adfm.201900247. https://www.osti.gov/servlets/purl/1498873.
@article{osti_1498873,
title = {High-Voltage Charging-Induced Strain, Heterogeneity, and Micro-Cracks in Secondary Particles of a Nickel-Rich Layered Cathode Material},
author = {Mao, Yuwei and Wang, Xuelong and Xia, Sihao and Zhang, Kai and Wei, Chenxi and Bak, Seongmin and Shadike, Zulipiya and Liu, Xuejun and Yang, Yang and Xu, Rong and Pianetta, Piero and Ermon, Stefano and Stavitski, Eli and Zhao, Kejie and Xu, Zhengrui and Lin, Feng and Yang, Xiao-Qing and Hu, Enyuan and Liu, Yijin},
abstractNote = {Nickel-rich layered materials LiNi1-x-yMnxCoyO2 are promising candidates for high-energy-density lithium-ion battery cathodes. Unfortunately, they suffer from capacity fading upon cycling, especially with high-voltage charging. It is critical to have a mechanistic understanding of such fade. Synchrotron-based techniques (including scattering, spectroscopy, and microcopy) and finite element analysis are utilized to understand the LiNi0.6Mn0.2Co0.2O2 material from structural, chemical, morphological, and mechanical points of view. The lattice structural changes are shown to be relatively reversible during cycling, even when 4.9 V charging is applied. However, local disorder and strain are induced by high-voltage charging. Nano-resolution 3D transmission X-ray microscopy data analyzed by machine learning methodology reveal that high-voltage charging induced significant oxidation state inhomogeneities in the cycled particles. Regions at the surface have a rock salt–type structure with lower oxidation state and build up the impedance, while regions with higher oxidization state are scattered in the bulk and are likely deactivated during cycling. In addition, the development of micro-cracks is highly dependent on the pristine state morphology and cycling conditions. Hollow particles seem to be more robust against stress-induced cracks than the solid ones, suggesting that morphology engineering can be effective in mitigating the crack problem in these materials.},
doi = {10.1002/adfm.201900247},
journal = {Advanced Functional Materials},
issn = {1616-301X},
number = 18,
volume = 29,
place = {United States},
year = {2019},
month = {3}
}

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