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Title: A Cobalt– and Manganese–Free High–Nickel Layered Oxide Cathode for Long–Life, Safer Lithium–Ion Batteries

Abstract

High-nickel LiNi1–x–yMnxCoyO2 and LiNi1–x–yCoxAlyO2 cathodes are receiving growing attention due to the burgeoning demands on high-energy-density lithium-ion batteries. The presence of both cobalt and manganese in them, however, triggers multiple issues, including high cost, high toxicity, rapid surface deterioration, and severe transition-metal dissolution. Herein, a Co- and Mn-free ultrahigh-nickel LiNi0.93Al0.05Ti0.01Mg0.01O2 (NATM) cathode that exhibits 82% capacity retention over 800 deep cycles in full cells, outperforming two representative high-Ni cathodes LiNi0.94Co0.06O2 (NC, 52%) and LiNi0.90Mn0.05Co0.05O2 (NMC, 60%) is presented. It is demonstrated that a titanium-enriched surface along with aluminum and magnesium as the stabilizing ions in NATM not only ameliorates unwanted side reactions with the electrolyte and structural disintegrity, but also mitigates transition-metal dissolution and active lithium loss on the graphite anode. As a result, the graphite anode paired with NATM displays an ultrathin (≈8 nm), monolayer anode-electrolyte interphase architecture after extensive cycling. Furthermore, NATM displays considerably enhanced thermal stability with an elevated exothermic temperature (213 °C for NATM vs 180 and 190 °C for NC and NMC, respectively) and remarkably reduced heat release. This work sheds light on rational compositional design to adopt ultrahigh-Ni cathodes in lithium-based batteries with low cost, long service life, and improved thermal stability.

Authors:
 [1];  [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); National Science Foundation (NSF)
OSTI Identifier:
2217347
Grant/Contract Number:  
EE0007762; 1827608
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 11; Journal Issue: 41; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; batteries; cathodes; cobalt- and manganese-free cathodes; electrolyte-electrode interphases; high-nickel layered oxides; lithium-ion batteries; thermal stability

Citation Formats

Cui, Zehao, Xie, Qiang, and Manthiram, Arumugam. A Cobalt– and Manganese–Free High–Nickel Layered Oxide Cathode for Long–Life, Safer Lithium–Ion Batteries. United States: N. p., 2021. Web. doi:10.1002/aenm.202102421.
Cui, Zehao, Xie, Qiang, & Manthiram, Arumugam. A Cobalt– and Manganese–Free High–Nickel Layered Oxide Cathode for Long–Life, Safer Lithium–Ion Batteries. United States. https://doi.org/10.1002/aenm.202102421
Cui, Zehao, Xie, Qiang, and Manthiram, Arumugam. Mon . "A Cobalt– and Manganese–Free High–Nickel Layered Oxide Cathode for Long–Life, Safer Lithium–Ion Batteries". United States. https://doi.org/10.1002/aenm.202102421. https://www.osti.gov/servlets/purl/2217347.
@article{osti_2217347,
title = {A Cobalt– and Manganese–Free High–Nickel Layered Oxide Cathode for Long–Life, Safer Lithium–Ion Batteries},
author = {Cui, Zehao and Xie, Qiang and Manthiram, Arumugam},
abstractNote = {High-nickel LiNi1–x–yMnxCoyO2 and LiNi1–x–yCoxAlyO2 cathodes are receiving growing attention due to the burgeoning demands on high-energy-density lithium-ion batteries. The presence of both cobalt and manganese in them, however, triggers multiple issues, including high cost, high toxicity, rapid surface deterioration, and severe transition-metal dissolution. Herein, a Co- and Mn-free ultrahigh-nickel LiNi0.93Al0.05Ti0.01Mg0.01O2 (NATM) cathode that exhibits 82% capacity retention over 800 deep cycles in full cells, outperforming two representative high-Ni cathodes LiNi0.94Co0.06O2 (NC, 52%) and LiNi0.90Mn0.05Co0.05O2 (NMC, 60%) is presented. It is demonstrated that a titanium-enriched surface along with aluminum and magnesium as the stabilizing ions in NATM not only ameliorates unwanted side reactions with the electrolyte and structural disintegrity, but also mitigates transition-metal dissolution and active lithium loss on the graphite anode. As a result, the graphite anode paired with NATM displays an ultrathin (≈8 nm), monolayer anode-electrolyte interphase architecture after extensive cycling. Furthermore, NATM displays considerably enhanced thermal stability with an elevated exothermic temperature (213 °C for NATM vs 180 and 190 °C for NC and NMC, respectively) and remarkably reduced heat release. This work sheds light on rational compositional design to adopt ultrahigh-Ni cathodes in lithium-based batteries with low cost, long service life, and improved thermal stability.},
doi = {10.1002/aenm.202102421},
journal = {Advanced Energy Materials},
number = 41,
volume = 11,
place = {United States},
year = {Mon Oct 04 00:00:00 EDT 2021},
month = {Mon Oct 04 00:00:00 EDT 2021}
}

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