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Title: A Comprehensive Analysis of the Interphasial and Structural Evolution over Long–Term Cycling of Ultrahigh–Nickel Cathodes in Lithium–Ion Batteries

Abstract

Abstract Ultrahigh‐Ni layered oxides hold great promise as high‐energy‐density cathodes at an affordable cost for lithium‐ion batteries, yet their practical application is greatly hampered by the poor cyclability. Herein, by employing LiNi 0.94 Co 0.06 O 2 as a model cathode in a full‐cell configuration, the interphasial and structural evolution processes of ultrahigh‐Ni layered oxides are systematically investigated over the course of their service life (1500 cycles). By applying advanced analytic techniques (e.g., Li‐isotope labeling, region‐of‐interest method), the dynamic chemical evolution on the cathode surface is revealed with spatial resolution, and the correlation between lattice distortion and cathode surface reactivity is established. Benefiting from in situ X‐ray diffraction (XRD) analysis, the ultrahigh‐Ni layered oxide is demonstrated to undergo dual‐phase reaction mechanisms with huge lattice variation, which leads to a decrease in crystallinity and secondary particle pulverization. Furthermore, the critical impact of cathode surface reaction on the graphite anode–electrolyte interphase (AEI) is revealed at nanometer scale, and a universal chemical/physical evolution process of the AEI is illustrated, for the first time. Finally, the practical viability of ultrahigh‐Ni layered oxides is demonstrated through Al‐doping strategy. This work presents a comprehensive understanding of the structural and interphasial degradation of ultrahigh‐Ni layered oxide cathodesmore » for developing high‐energy‐density lithium‐ion batteries.« less

Authors:
 [1]; ORCiD logo [1]
  1. Univ. of Texas, Austin, TX (United States)
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); Welch Foundation; USDOE
OSTI Identifier:
2217333
Alternate Identifier(s):
OSTI ID: 1572119
Grant/Contract Number:  
EE0007762; F-1254; DE‐EE0007762
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 45; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electrode-electrolyte interphase; interphasial evolution; lithium-ion batteries; structural degradation; ultrahigh-Ni layered oxides

Citation Formats

Li, Jianyu, and Manthiram, Arumugam. A Comprehensive Analysis of the Interphasial and Structural Evolution over Long–Term Cycling of Ultrahigh–Nickel Cathodes in Lithium–Ion Batteries. United States: N. p., 2019. Web. doi:10.1002/aenm.201902731.
Li, Jianyu, & Manthiram, Arumugam. A Comprehensive Analysis of the Interphasial and Structural Evolution over Long–Term Cycling of Ultrahigh–Nickel Cathodes in Lithium–Ion Batteries. United States. https://doi.org/10.1002/aenm.201902731
Li, Jianyu, and Manthiram, Arumugam. Mon . "A Comprehensive Analysis of the Interphasial and Structural Evolution over Long–Term Cycling of Ultrahigh–Nickel Cathodes in Lithium–Ion Batteries". United States. https://doi.org/10.1002/aenm.201902731. https://www.osti.gov/servlets/purl/2217333.
@article{osti_2217333,
title = {A Comprehensive Analysis of the Interphasial and Structural Evolution over Long–Term Cycling of Ultrahigh–Nickel Cathodes in Lithium–Ion Batteries},
author = {Li, Jianyu and Manthiram, Arumugam},
abstractNote = {Abstract Ultrahigh‐Ni layered oxides hold great promise as high‐energy‐density cathodes at an affordable cost for lithium‐ion batteries, yet their practical application is greatly hampered by the poor cyclability. Herein, by employing LiNi 0.94 Co 0.06 O 2 as a model cathode in a full‐cell configuration, the interphasial and structural evolution processes of ultrahigh‐Ni layered oxides are systematically investigated over the course of their service life (1500 cycles). By applying advanced analytic techniques (e.g., Li‐isotope labeling, region‐of‐interest method), the dynamic chemical evolution on the cathode surface is revealed with spatial resolution, and the correlation between lattice distortion and cathode surface reactivity is established. Benefiting from in situ X‐ray diffraction (XRD) analysis, the ultrahigh‐Ni layered oxide is demonstrated to undergo dual‐phase reaction mechanisms with huge lattice variation, which leads to a decrease in crystallinity and secondary particle pulverization. Furthermore, the critical impact of cathode surface reaction on the graphite anode–electrolyte interphase (AEI) is revealed at nanometer scale, and a universal chemical/physical evolution process of the AEI is illustrated, for the first time. Finally, the practical viability of ultrahigh‐Ni layered oxides is demonstrated through Al‐doping strategy. This work presents a comprehensive understanding of the structural and interphasial degradation of ultrahigh‐Ni layered oxide cathodes for developing high‐energy‐density lithium‐ion batteries.},
doi = {10.1002/aenm.201902731},
journal = {Advanced Energy Materials},
number = 45,
volume = 9,
place = {United States},
year = {Mon Oct 28 00:00:00 EDT 2019},
month = {Mon Oct 28 00:00:00 EDT 2019}
}

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