Long-Term Cyclability of NCM-811 at High Voltages in Lithium-Ion Batteries: an In-Depth Diagnostic Study
Abstract
High-nickel layered oxides, such as LiNi0.8Co0.1Mn0.1O2 (NCM-811), offer higher energy density than their low-nickel counterparts at a given voltage and are gaining major traction in automotive lithium-ion batteries for electric vehicles. Besides high-Ni content, higher charging voltages above 4.3 V vs Li+/Li boost the energy and represent another focus in battery development. Here, we investigate the long-term cyclability of NCM-811 in graphite pouch cells over 1000 deep cycles between 2.5–4.2, 2.5–4.4, and 2.5–4.5 V through a suite of sensitive characterization techniques. The NCM-811 full cells show severely deteriorated cyclability with higher charging voltages, from 78% at 4.2 V to 52 and 32% at 4.4 and 4.5 V, respectively. At 4.2 V, minor parasitic electrolyte oxidation as well as cathode Li/Ni mixing and cracking are revealed after cycling, while transition-metal dissolution and surface reconstruction into rock-salt NiO are virtually undetectable. At 4.4 and 4.5 V, transition-metal dissolution and crossover to the anode become much more pronounced and a primary contributor to the capacity fade, while significant surface NiO formation causes substantial voltage polarization, which is less noticeable at 4.2 V. Meanwhile, more severe electrolyte oxidation, Li/Ni mixing, and particle pulverization exacerbate the voltage and capacity fade. Finally, these results outline distinctmore »
- Authors:
-
[1];
[2];
[1]
- Univ. of Texas, Austin, TX (United States)
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- 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); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
- OSTI Identifier:
- 2217338
- Grant/Contract Number:
- EE0007762
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 32; Journal Issue: 18; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; anode materials; carbon; electrochemical cells; electrodes; X-ray photoelectron spectroscopy
Citation Formats
Li, Wangda, Liu, Xiaoming, Xie, Qiang, You, Ya, Chi, Miaofang, and Manthiram, Arumugam. Long-Term Cyclability of NCM-811 at High Voltages in Lithium-Ion Batteries: an In-Depth Diagnostic Study. United States: N. p., 2020.
Web. doi:10.1021/acs.chemmater.0c02398.
Li, Wangda, Liu, Xiaoming, Xie, Qiang, You, Ya, Chi, Miaofang, & Manthiram, Arumugam. Long-Term Cyclability of NCM-811 at High Voltages in Lithium-Ion Batteries: an In-Depth Diagnostic Study. United States. https://doi.org/10.1021/acs.chemmater.0c02398
Li, Wangda, Liu, Xiaoming, Xie, Qiang, You, Ya, Chi, Miaofang, and Manthiram, Arumugam. Thu .
"Long-Term Cyclability of NCM-811 at High Voltages in Lithium-Ion Batteries: an In-Depth Diagnostic Study". United States. https://doi.org/10.1021/acs.chemmater.0c02398. https://www.osti.gov/servlets/purl/2217338.
@article{osti_2217338,
title = {Long-Term Cyclability of NCM-811 at High Voltages in Lithium-Ion Batteries: an In-Depth Diagnostic Study},
author = {Li, Wangda and Liu, Xiaoming and Xie, Qiang and You, Ya and Chi, Miaofang and Manthiram, Arumugam},
abstractNote = {High-nickel layered oxides, such as LiNi0.8Co0.1Mn0.1O2 (NCM-811), offer higher energy density than their low-nickel counterparts at a given voltage and are gaining major traction in automotive lithium-ion batteries for electric vehicles. Besides high-Ni content, higher charging voltages above 4.3 V vs Li+/Li boost the energy and represent another focus in battery development. Here, we investigate the long-term cyclability of NCM-811 in graphite pouch cells over 1000 deep cycles between 2.5–4.2, 2.5–4.4, and 2.5–4.5 V through a suite of sensitive characterization techniques. The NCM-811 full cells show severely deteriorated cyclability with higher charging voltages, from 78% at 4.2 V to 52 and 32% at 4.4 and 4.5 V, respectively. At 4.2 V, minor parasitic electrolyte oxidation as well as cathode Li/Ni mixing and cracking are revealed after cycling, while transition-metal dissolution and surface reconstruction into rock-salt NiO are virtually undetectable. At 4.4 and 4.5 V, transition-metal dissolution and crossover to the anode become much more pronounced and a primary contributor to the capacity fade, while significant surface NiO formation causes substantial voltage polarization, which is less noticeable at 4.2 V. Meanwhile, more severe electrolyte oxidation, Li/Ni mixing, and particle pulverization exacerbate the voltage and capacity fade. Finally, these results outline distinct challenges for stable high-Ni layered oxide cathodes in high-voltage Li-ion batteries.},
doi = {10.1021/acs.chemmater.0c02398},
journal = {Chemistry of Materials},
number = 18,
volume = 32,
place = {United States},
year = {Thu Aug 27 00:00:00 EDT 2020},
month = {Thu Aug 27 00:00:00 EDT 2020}
}
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