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Title: Stabilizing the Interphase in Cobalt–Free, Ultrahigh–Nickel Cathodes for Lithium–Ion Batteries

Abstract

Abstract High‐nickel layered oxide cathodes, such as LiNi 1‐ x y Mn x Co y O 2 (NMC) and LiNi 1‐ x y Co x Al y O 2 (NCA), are at the forefront for implementation in high‐energy‐density lithium‐ion batteries. The presence of cobalt in both cathode chemistries, however, largely deters their application due to fiscal and humanitarian issues affiliated with cobalt sourcing. Increasing the Ni content drives down the Co content, but introduces additional structural and electrochemical problems attributed to high‐Ni cathodes. Herein a dually modified cobalt‐free ultrahigh‐nickel cathode 0.02B‐LiNi 0.99 Mg 0.01 O 2 (NBM) is presented with 1 mol% Mg and 2 mol% B that exhibits a high initial 1C discharge capacity of 210 mA h g −1 with a 20% capacity retention improvement over 500 cycles when benchmarked against LiNiO 2 (LNO) in pouch full cell configurations with graphite anode. Postmortem analyses reveal the enhanced performance stems from reduced active lithium inventory loss and localized surface reactivity in the NBM cathode. The stabilized cathode‐electrolyte interphase subsequently reduces transition‐metal dissolution and ensuing chemical crossover to the graphite anode, which prevents further catalyzed parasitic reactions that harmfully passivate the anode surface. Altogether, this study aims to highlight the importance of electrode characterization and analysis from anmore » interphasial viewpoint and to push the ongoing research to stabilize cobalt‐free ultrahigh‐Ni cathodes for industrial feasibility.« less

Authors:
 [1];  [1]; ORCiD logo [1]
  1. Univ. of Texas at Austin, TX (United States)
Publication Date:
Research Org.:
Univ. of Texas at 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:
1972451
Alternate Identifier(s):
OSTI ID: 1983548
Grant/Contract Number:  
EE0008445; F-1254; DE‐EE0008445
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 33; Journal Issue: 14; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium-ion batteries; cobalt-free cathodes; ultrahigh-nickel cathodes; electrode-electrolyte interphases

Citation Formats

Yi, Michael, Dolocan, Andrei, and Manthiram, Arumugam. Stabilizing the Interphase in Cobalt–Free, Ultrahigh–Nickel Cathodes for Lithium–Ion Batteries. United States: N. p., 2023. Web. doi:10.1002/adfm.202213164.
Yi, Michael, Dolocan, Andrei, & Manthiram, Arumugam. Stabilizing the Interphase in Cobalt–Free, Ultrahigh–Nickel Cathodes for Lithium–Ion Batteries. United States. https://doi.org/10.1002/adfm.202213164
Yi, Michael, Dolocan, Andrei, and Manthiram, Arumugam. Sun . "Stabilizing the Interphase in Cobalt–Free, Ultrahigh–Nickel Cathodes for Lithium–Ion Batteries". United States. https://doi.org/10.1002/adfm.202213164. https://www.osti.gov/servlets/purl/1972451.
@article{osti_1972451,
title = {Stabilizing the Interphase in Cobalt–Free, Ultrahigh–Nickel Cathodes for Lithium–Ion Batteries},
author = {Yi, Michael and Dolocan, Andrei and Manthiram, Arumugam},
abstractNote = {Abstract High‐nickel layered oxide cathodes, such as LiNi 1‐ x ‐ y Mn x Co y O 2 (NMC) and LiNi 1‐ x ‐ y Co x Al y O 2 (NCA), are at the forefront for implementation in high‐energy‐density lithium‐ion batteries. The presence of cobalt in both cathode chemistries, however, largely deters their application due to fiscal and humanitarian issues affiliated with cobalt sourcing. Increasing the Ni content drives down the Co content, but introduces additional structural and electrochemical problems attributed to high‐Ni cathodes. Herein a dually modified cobalt‐free ultrahigh‐nickel cathode 0.02B‐LiNi 0.99 Mg 0.01 O 2 (NBM) is presented with 1 mol% Mg and 2 mol% B that exhibits a high initial 1C discharge capacity of 210 mA h g −1 with a 20% capacity retention improvement over 500 cycles when benchmarked against LiNiO 2 (LNO) in pouch full cell configurations with graphite anode. Postmortem analyses reveal the enhanced performance stems from reduced active lithium inventory loss and localized surface reactivity in the NBM cathode. The stabilized cathode‐electrolyte interphase subsequently reduces transition‐metal dissolution and ensuing chemical crossover to the graphite anode, which prevents further catalyzed parasitic reactions that harmfully passivate the anode surface. Altogether, this study aims to highlight the importance of electrode characterization and analysis from an interphasial viewpoint and to push the ongoing research to stabilize cobalt‐free ultrahigh‐Ni cathodes for industrial feasibility.},
doi = {10.1002/adfm.202213164},
journal = {Advanced Functional Materials},
number = 14,
volume = 33,
place = {United States},
year = {Sun Jan 15 00:00:00 EST 2023},
month = {Sun Jan 15 00:00:00 EST 2023}
}

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