Insight into the Atomic Structure of High-Voltage Spinel LiNi0.5Mn1.5O4 Cathode Material in the First Cycle
Abstract
Application of high-voltage spinel LiNi0.5Mn1.5O4 cathode material is the closest and the most realistic approach to meeting the midterm goal of lithium-ion batteries for electric vehicles (EVs) and plug-in hybrid electric vehicles (HEVs). However, this application has been hampered by long-standing issues, such as capacity degradation and poor first-cycle Coulombic efficiency of LiNi0.5Mn1.5O4 cathode material. Although it is well-known that the structure of LiNi0.5Mn1.5O4 into which Li ions are reversibly intercalated plays a critical role in the above issues, performance degradation related to structural changes, particularly in the first cycle, are not fully understood. Here, we report detailed investigations of local atomic-level and average structure of LiNi0.5Mn1.5O4 during first cycle (3.5–4.9 V) at room temperature. We observed two types of local atomic-level migration of transition metals (TM) ions in the cathode of a well-prepared LiNi0.5Mn1.5O4//Li half-cell during first charge via an aberration-corrected scanning transmission electron microscopy (STEM). Surface regions (~2 nm) of the cycled LiNi0.5Mn1.5O4 particles show migration of TM ions into tetrahedral Li sites to form a Mn3O4-like structure. However, subsurface regions of the cycled particles exhibit migration of TM ions into empty octahedral sites to form a rocksalt-like structure. The migration of these TM ions are closely relatedmore »
- Authors:
-
- Chinese Academy of Sciences, Beijing (China)
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- CIC Energigune, Alava (Spain)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1169558
- Report Number(s):
- BNL-107260-2014-JA
Journal ID: ISSN 0897-4756; R&D Project: MA453MAEA; VT1201000
- Grant/Contract Number:
- DE-SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 27; Journal Issue: 1; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; NSLS
Citation Formats
Huang, Xuejie, Yu, Xiqian, Lin, Mingxiang, Ben, Liubin, Sun, Yang, Wang, Hao, Yang, Zhenzhong, Gu, Lin, Yang, Xiao -Qing, Zhao, Haofei, Yu, Richeng, and Armand, Michel. Insight into the Atomic Structure of High-Voltage Spinel LiNi0.5Mn1.5O4 Cathode Material in the First Cycle. United States: N. p., 2014.
Web. doi:10.1021/cm503972a.
Huang, Xuejie, Yu, Xiqian, Lin, Mingxiang, Ben, Liubin, Sun, Yang, Wang, Hao, Yang, Zhenzhong, Gu, Lin, Yang, Xiao -Qing, Zhao, Haofei, Yu, Richeng, & Armand, Michel. Insight into the Atomic Structure of High-Voltage Spinel LiNi0.5Mn1.5O4 Cathode Material in the First Cycle. United States. https://doi.org/10.1021/cm503972a
Huang, Xuejie, Yu, Xiqian, Lin, Mingxiang, Ben, Liubin, Sun, Yang, Wang, Hao, Yang, Zhenzhong, Gu, Lin, Yang, Xiao -Qing, Zhao, Haofei, Yu, Richeng, and Armand, Michel. Mon .
"Insight into the Atomic Structure of High-Voltage Spinel LiNi0.5Mn1.5O4 Cathode Material in the First Cycle". United States. https://doi.org/10.1021/cm503972a. https://www.osti.gov/servlets/purl/1169558.
@article{osti_1169558,
title = {Insight into the Atomic Structure of High-Voltage Spinel LiNi0.5Mn1.5O4 Cathode Material in the First Cycle},
author = {Huang, Xuejie and Yu, Xiqian and Lin, Mingxiang and Ben, Liubin and Sun, Yang and Wang, Hao and Yang, Zhenzhong and Gu, Lin and Yang, Xiao -Qing and Zhao, Haofei and Yu, Richeng and Armand, Michel},
abstractNote = {Application of high-voltage spinel LiNi0.5Mn1.5O4 cathode material is the closest and the most realistic approach to meeting the midterm goal of lithium-ion batteries for electric vehicles (EVs) and plug-in hybrid electric vehicles (HEVs). However, this application has been hampered by long-standing issues, such as capacity degradation and poor first-cycle Coulombic efficiency of LiNi0.5Mn1.5O4 cathode material. Although it is well-known that the structure of LiNi0.5Mn1.5O4 into which Li ions are reversibly intercalated plays a critical role in the above issues, performance degradation related to structural changes, particularly in the first cycle, are not fully understood. Here, we report detailed investigations of local atomic-level and average structure of LiNi0.5Mn1.5O4 during first cycle (3.5–4.9 V) at room temperature. We observed two types of local atomic-level migration of transition metals (TM) ions in the cathode of a well-prepared LiNi0.5Mn1.5O4//Li half-cell during first charge via an aberration-corrected scanning transmission electron microscopy (STEM). Surface regions (~2 nm) of the cycled LiNi0.5Mn1.5O4 particles show migration of TM ions into tetrahedral Li sites to form a Mn3O4-like structure. However, subsurface regions of the cycled particles exhibit migration of TM ions into empty octahedral sites to form a rocksalt-like structure. The migration of these TM ions are closely related to dissolution of Ni/Mn ions and building-up of charge transfer impedance, which contribute significantly to the capacity degradation and the poor first-cycle Coulombic efficiency of spinel LiNi0.5Mn1.5O4 cathode material. Accordingly, we provide suggestions of effective stabilization of LiNi0.5Mn1.5O4 structure to obtain better electrochemical performance.},
doi = {10.1021/cm503972a},
journal = {Chemistry of Materials},
number = 1,
volume = 27,
place = {United States},
year = {Mon Dec 22 00:00:00 EST 2014},
month = {Mon Dec 22 00:00:00 EST 2014}
}
Web of Science
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