Li‐Rich Li[Li 1/6 Fe 1/6 Ni 1/6 Mn 1/2 ]O 2 (LFNMO) Cathodes: Atomic Scale Insight on the Mechanisms of Cycling Decay and of the Improvement due to Cobalt Phosphate Surface Modification
Abstract
Abstract Lithium‐rich Li[Li 1/6 Fe 1/6 Ni 1/6 Mn 1/2 ]O 2 (0.4Li 2 MnO 3 ‐0.6LiFe 1/3 Ni 1/3 Mn 1/3 O 2 , LFNMO) is a new member of the x Li 2 MnO 3 ·(1 − x )LiMO 2 family of high capacity–high voltage lithium‐ion battery (LIB) cathodes. Unfortunately, it suffers from the severe degradation during cycling both in terms of reversible capacity and operating voltage. Here, the corresponding degradation occurring in LFNMO at an atomic scale has been documented for the first time, using high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM), as well as tracing the elemental crossover to the Li metal anode using X‐ray photoelectron spectroscopy (XPS). It is also demonstrated that a cobalt phosphate surface treatment significantly boosts LFNMO cycling stability and rate capability. Due to cycling, the unmodified LFNMO undergoes extensive elemental dissolution (especially Mn) and O loss, forming Kirkendall‐type voids. The associated structural degradation is from the as‐synthesized R‐ 3 m layered structure to a disordered rock‐salt phase. Prior to cycling, the cobalt phosphate coating is epitaxial, sharing the crystallography of the parent material. During cycling, a 2–3 nm thick disordered Co‐rich rock‐salt structure is formed as the outer shell, whilemore »
- Authors:
-
[1];
- The Center of New Energy Materials and Technology Southwest Petroleum University Chengdu Sichuan 610500 China
- Chemical &, Biomolecular Engineering Clarkson University Potsdam NY 13699 USA
- Physical and Computational Sciences Directorate Pacific Northwest National Laboratory 902 Battelle Boulevard Richland WA 99352 USA
- Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China
- Energy and Environment Directorate Pacific Northwest National Laboratory 902 Battelle Boulevard Richland WA 99354 USA
- Research Institute (RI) NingDe Amperex Technology Limited Ningde Fujian 352100 China
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1469230
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Small
- Additional Journal Information:
- Journal Name: Small Journal Volume: 14 Journal Issue: 40; Journal ID: ISSN 1613-6810
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Li, Xing, Zhang, Kangjia, Mitlin, David, Paek, Eunsu, Wang, Mingshan, Jiang, Fei, Huang, Yun, Yang, Zhenzhong, Gong, Yue, Gu, Lin, Zhao, Wengao, Du, Yingge, and Zheng, Jianming. Li‐Rich Li[Li 1/6 Fe 1/6 Ni 1/6 Mn 1/2 ]O 2 (LFNMO) Cathodes: Atomic Scale Insight on the Mechanisms of Cycling Decay and of the Improvement due to Cobalt Phosphate Surface Modification. Germany: N. p., 2018.
Web. doi:10.1002/smll.201802570.
Li, Xing, Zhang, Kangjia, Mitlin, David, Paek, Eunsu, Wang, Mingshan, Jiang, Fei, Huang, Yun, Yang, Zhenzhong, Gong, Yue, Gu, Lin, Zhao, Wengao, Du, Yingge, & Zheng, Jianming. Li‐Rich Li[Li 1/6 Fe 1/6 Ni 1/6 Mn 1/2 ]O 2 (LFNMO) Cathodes: Atomic Scale Insight on the Mechanisms of Cycling Decay and of the Improvement due to Cobalt Phosphate Surface Modification. Germany. https://doi.org/10.1002/smll.201802570
Li, Xing, Zhang, Kangjia, Mitlin, David, Paek, Eunsu, Wang, Mingshan, Jiang, Fei, Huang, Yun, Yang, Zhenzhong, Gong, Yue, Gu, Lin, Zhao, Wengao, Du, Yingge, and Zheng, Jianming. Sun .
"Li‐Rich Li[Li 1/6 Fe 1/6 Ni 1/6 Mn 1/2 ]O 2 (LFNMO) Cathodes: Atomic Scale Insight on the Mechanisms of Cycling Decay and of the Improvement due to Cobalt Phosphate Surface Modification". Germany. https://doi.org/10.1002/smll.201802570.
@article{osti_1469230,
title = {Li‐Rich Li[Li 1/6 Fe 1/6 Ni 1/6 Mn 1/2 ]O 2 (LFNMO) Cathodes: Atomic Scale Insight on the Mechanisms of Cycling Decay and of the Improvement due to Cobalt Phosphate Surface Modification},
author = {Li, Xing and Zhang, Kangjia and Mitlin, David and Paek, Eunsu and Wang, Mingshan and Jiang, Fei and Huang, Yun and Yang, Zhenzhong and Gong, Yue and Gu, Lin and Zhao, Wengao and Du, Yingge and Zheng, Jianming},
abstractNote = {Abstract Lithium‐rich Li[Li 1/6 Fe 1/6 Ni 1/6 Mn 1/2 ]O 2 (0.4Li 2 MnO 3 ‐0.6LiFe 1/3 Ni 1/3 Mn 1/3 O 2 , LFNMO) is a new member of the x Li 2 MnO 3 ·(1 − x )LiMO 2 family of high capacity–high voltage lithium‐ion battery (LIB) cathodes. Unfortunately, it suffers from the severe degradation during cycling both in terms of reversible capacity and operating voltage. Here, the corresponding degradation occurring in LFNMO at an atomic scale has been documented for the first time, using high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM), as well as tracing the elemental crossover to the Li metal anode using X‐ray photoelectron spectroscopy (XPS). It is also demonstrated that a cobalt phosphate surface treatment significantly boosts LFNMO cycling stability and rate capability. Due to cycling, the unmodified LFNMO undergoes extensive elemental dissolution (especially Mn) and O loss, forming Kirkendall‐type voids. The associated structural degradation is from the as‐synthesized R‐ 3 m layered structure to a disordered rock‐salt phase. Prior to cycling, the cobalt phosphate coating is epitaxial, sharing the crystallography of the parent material. During cycling, a 2–3 nm thick disordered Co‐rich rock‐salt structure is formed as the outer shell, while the bulk material retains R‐ 3 m crystallography. These combined cathode–anode findings significantly advance the microstructural design principles for next‐generation Li‐rich cathode materials and coatings.},
doi = {10.1002/smll.201802570},
journal = {Small},
number = 40,
volume = 14,
place = {Germany},
year = {Sun Sep 09 00:00:00 EDT 2018},
month = {Sun Sep 09 00:00:00 EDT 2018}
}
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- Energy & Environmental Science, Vol. 7, Issue 4
Fundamental Insight into Zr Modification of Li- and Mn-Rich Cathodes: Combined Transmission Electron Microscopy and Electrochemical Impedance Spectroscopy Study
journal, March 2018
- Li, Xing; Zhang, Kangjia; Mitlin, David
- Chemistry of Materials, Vol. 30, Issue 8
Ionic Liquid Redox Catholyte for High Energy Efficiency, Low-Cost Energy Storage
journal, April 2015
- Xue, Leigang; Tucker, Telpriore G.; Angell, C. Austen
- Advanced Energy Materials, Vol. 5, Issue 12
ALD TiO2 coated silicon nanowires for lithium ion battery anodes with enhanced cycling stability and coulombic efficiency
journal, January 2013
- Memarzadeh Lotfabad, Elmira; Kalisvaart, Peter; Cui, Kai
- Physical Chemistry Chemical Physics, Vol. 15, Issue 32
Effect of synthesis temperature on the structural defects of integrated spinel-layered Li 1.2 Mn 0.75 Ni 0.25 O 2+δ : a strategy to develop high-capacity cathode materials for Li-ion batteries
journal, January 2017
- Vu, Ngoc Hung; Arunkumar, Paulraj; Im, Jong Chan
- Journal of Materials Chemistry A, Vol. 5, Issue 30
Studies of Li and Mn-Rich Li x [MnNiCo]O 2 Electrodes: Electrochemical Performance, Structure, and the Effect of the Aluminum Fluoride Coating
journal, January 2013
- Amalraj, Francis; Talianker, Michael; Markovsky, Boris
- Journal of The Electrochemical Society, Vol. 160, Issue 11
Corrosion/Fragmentation of Layered Composite Cathode and Related Capacity/Voltage Fading during Cycling Process
journal, July 2013
- Zheng, Jianming; Gu, Meng; Xiao, Jie
- Nano Letters, Vol. 13, Issue 8
Simultaneous surface modification method for 0.4Li2MnO3-0.6LiNi1/3Co1/3Mn1/3O2 cathode material for lithium ion batteries: Acid treatment and LiCoPO4 coating
journal, June 2017
- Lee, Min-Joon; Lho, Eunsol; Oh, Pilgun
- Nano Research, Vol. 10, Issue 12
Bifurcation of the Kirkendall marker plane and the role of Ni and other impurities on the growth of Kirkendall voids in the Cu–Sn system
journal, June 2017
- Baheti, Varun A.; Kashyap, Sanjay; Kumar, Praveen
- Acta Materialia, Vol. 131
Self-supporting activated carbon/carbon nanotube/reduced graphene oxide flexible electrode for high performance supercapacitor
journal, April 2018
- Li, Xing; Tang, Yao; Song, Junhua
- Carbon, Vol. 129
A New Type of Protective Surface Layer for High-Capacity Ni-Based Cathode Materials: Nanoscaled Surface Pillaring Layer
journal, February 2013
- Cho, Yonghyun; Oh, Pilgun; Cho, Jaephil
- Nano Letters, Vol. 13, Issue 3
Understanding the Degradation Mechanisms of LiNi 0.5 Co 0.2 Mn 0.3 O 2 Cathode Material in Lithium Ion Batteries
journal, August 2013
- Jung, Sung-Kyun; Gwon, Hyeokjo; Hong, Jihyun
- Advanced Energy Materials, Vol. 4, Issue 1
Exploration of a Metastable Normal Spinel Phase Diagram for the Quaternary Li–Ni–Mn–Co–O System
journal, February 2016
- Kan, Wang Hay; Huq, Ashfia; Manthiram, Arumugam
- Chemistry of Materials, Vol. 28, Issue 6
Structural and Electrochemical Study of Al 2 O 3 and TiO 2 Coated Li 1.2 Ni 0.13 Mn 0.54 Co 0.13 O 2 Cathode Material Using ALD
journal, June 2013
- Zhang, Xiaofeng; Belharouak, Ilias; Li, Li
- Advanced Energy Materials, Vol. 3, Issue 10
Balancing stability and specific energy in Li-rich cathodes for lithium ion batteries: a case study of a novel Li–Mn–Ni–Co oxide
journal, January 2015
- Li, Qi; Li, Guangshe; Fu, Chaochao
- Journal of Materials Chemistry A, Vol. 3, Issue 19
Functional surface modifications of a high capacity layered Li[Li0.2Mn0.54Ni0.13Co0.13]O2 cathode
journal, January 2010
- Liu, Jun; Manthiram, Arumugam
- Journal of Materials Chemistry, Vol. 20, Issue 19
A Novel Surface Treatment Method and New Insight into Discharge Voltage Deterioration for High-Performance 0.4Li 2 MnO 3- 0.6LiNi 1/3 Co 1/3 Mn 1/3 O 2 Cathode Materials
journal, June 2014
- Oh, Pilgun; Ko, Minseong; Myeong, Seungjun
- Advanced Energy Materials, Vol. 4, Issue 16
Synthesis and characterization of Li(Li0.23Mn0.47Fe0.2Ni0.1)O2 cathode material for Li-ion batteries
journal, December 2013
- Li, Jiangang; Wang, Li; Wang, Lei
- Journal of Power Sources, Vol. 244
Predominant growth orientation of Li 1.2 (Mn 0.4 Co 0.4 )O 2 cathode materials produced by the NaOH compound molten salt method and their enhanced electrochemical performance
journal, January 2014
- Liu, Xialin; Wu, Jingjing; Huang, Xiaolan
- Journal of Materials Chemistry A, Vol. 2, Issue 36
Surface Chemistry Mechanism of Ultra-Low Interfacial Resistance in the Solid-State Electrolyte Li 7 La 3 Zr 2 O 12
journal, September 2017
- Sharafi, Asma; Kazyak, Eric; Davis, Andrew L.
- Chemistry of Materials, Vol. 29, Issue 18
Insight into the atomic structure of Li 2 MnO 3 in Li-rich Mn-based cathode materials and the impact of its atomic arrangement on electrochemical performance
journal, January 2017
- Song, Yuanzhe; Zhao, Xuebing; Wang, Chao
- Journal of Materials Chemistry A, Vol. 5, Issue 22
Mn source effects on electrochemical properties of Fe -and Ni-substituted Li2MnO3 positive electrode material
journal, April 2015
- Tabuchi, Mitsuharu; Kitta, Mitsunori; Kageyama, Hiroyuki
- Journal of Power Sources, Vol. 279
Nickel-Rich and Lithium-Rich Layered Oxide Cathodes: Progress and Perspectives
journal, October 2015
- Manthiram, Arumugam; Knight, James C.; Myung, Seung-Taek
- Advanced Energy Materials, Vol. 6, Issue 1
Dependence of Electrochemical Behavior on Concentration and Annealing Temperature of Li[sub x]CoPO[sub 4] Phase-Grown LiNi[sub 0.8]Co[sub 0.16]Al[sub 0.04]O[sub 2] Cathode Materials
journal, January 2008
- Eom, Junho; Sun Ryu, Kwang; Cho, Jaephil
- Journal of The Electrochemical Society, Vol. 155, Issue 3
From Surface ZrO 2 Coating to Bulk Zr Doping by High Temperature Annealing of Nickel-Rich Lithiated Oxides and Their Enhanced Electrochemical Performance in Lithium Ion Batteries
journal, September 2017
- Schipper, Florian; Bouzaglo, Hana; Dixit, Mudit
- Advanced Energy Materials, Vol. 8, Issue 4