High-performance heterostructured cathodes for lithium-ion batteries with a Ni-rich layered oxide core and a Li-rich layered oxide shell
Abstract
The Ni-rich layered oxides with a Ni content of >0.5 are drawing much attention recently to increase the energy density of lithium-ion batteries. However, the Ni-rich layered oxides suffer from aggressive reaction of the cathode surface with the organic electrolyte at the higher operating voltages, resulting in consequent impedance rise and capacity fade. To overcome this difficulty, we present here a heterostructure composed of a Ni-rich LiNi0.7Co0.15Mn0.15O2 core and a Li-rich Li1.2-xNi0.2Mn0.6O2 shell, incorporating the advantageous features of the structural stability of the core and chemical stability of the shell. With a unique chemical treatment for the activation of the Li2MnO3 phase of the shell, a high capacity is realized with the Li-rich shell material. Aberration-corrected scanning transmission electron microscopy (STEM) provides direct evidence for the formation of surface Li-rich shell layer. Finally, the heterostructure exhibits a high capacity retention of 98% and a discharge- voltage retention of 97% during 100 cycles with a discharge capacity of 190 mA h g-1 (at 2.0–4.5 V under C/3 rate, 1C = 200 mA g-1).
- Authors:
-
- The Univ. of Texas, Austin, TX (United States)
- Ulsan National Institute of Science and Technology (UNIST), Ulsan (South Korea)
- Publication Date:
- Research Org.:
- Univ. of Texas, Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1363894
- Grant/Contract Number:
- EE0006447
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Science
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 11; Journal ID: ISSN 2198-3844
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; chemical activation; heterostructure; lithium-rich layered oxide; nickel-rich layered oxide; surface stabilization
Citation Formats
Oh, Pilgun, Oh, Seung -Min, Li, Wangda, Myeong, Seunjun, Cho, Jaephil, and Manthiram, Arumugam. High-performance heterostructured cathodes for lithium-ion batteries with a Ni-rich layered oxide core and a Li-rich layered oxide shell. United States: N. p., 2016.
Web. doi:10.1002/advs.201600184.
Oh, Pilgun, Oh, Seung -Min, Li, Wangda, Myeong, Seunjun, Cho, Jaephil, & Manthiram, Arumugam. High-performance heterostructured cathodes for lithium-ion batteries with a Ni-rich layered oxide core and a Li-rich layered oxide shell. United States. https://doi.org/10.1002/advs.201600184
Oh, Pilgun, Oh, Seung -Min, Li, Wangda, Myeong, Seunjun, Cho, Jaephil, and Manthiram, Arumugam. Mon .
"High-performance heterostructured cathodes for lithium-ion batteries with a Ni-rich layered oxide core and a Li-rich layered oxide shell". United States. https://doi.org/10.1002/advs.201600184. https://www.osti.gov/servlets/purl/1363894.
@article{osti_1363894,
title = {High-performance heterostructured cathodes for lithium-ion batteries with a Ni-rich layered oxide core and a Li-rich layered oxide shell},
author = {Oh, Pilgun and Oh, Seung -Min and Li, Wangda and Myeong, Seunjun and Cho, Jaephil and Manthiram, Arumugam},
abstractNote = {The Ni-rich layered oxides with a Ni content of >0.5 are drawing much attention recently to increase the energy density of lithium-ion batteries. However, the Ni-rich layered oxides suffer from aggressive reaction of the cathode surface with the organic electrolyte at the higher operating voltages, resulting in consequent impedance rise and capacity fade. To overcome this difficulty, we present here a heterostructure composed of a Ni-rich LiNi0.7Co0.15Mn0.15O2 core and a Li-rich Li1.2-xNi0.2Mn0.6O2 shell, incorporating the advantageous features of the structural stability of the core and chemical stability of the shell. With a unique chemical treatment for the activation of the Li2MnO3 phase of the shell, a high capacity is realized with the Li-rich shell material. Aberration-corrected scanning transmission electron microscopy (STEM) provides direct evidence for the formation of surface Li-rich shell layer. Finally, the heterostructure exhibits a high capacity retention of 98% and a discharge- voltage retention of 97% during 100 cycles with a discharge capacity of 190 mA h g-1 (at 2.0–4.5 V under C/3 rate, 1C = 200 mA g-1).},
doi = {10.1002/advs.201600184},
journal = {Advanced Science},
number = 11,
volume = 3,
place = {United States},
year = {Mon May 30 00:00:00 EDT 2016},
month = {Mon May 30 00:00:00 EDT 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 69 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Reversible anionic redox chemistry in high-capacity layered-oxide electrodes
journal, July 2013
- Sathiya, M.; Rousse, G.; Ramesha, K.
- Nature Materials, Vol. 12, Issue 9
A New Coating Method for Alleviating Surface Degradation of LiNi 0.6 Co 0.2 Mn 0.2 O 2 Cathode Material: Nanoscale Surface Treatment of Primary Particles
journal, February 2015
- Kim, Hyejung; Kim, Min Gyu; Jeong, Hu Young
- Nano Letters, Vol. 15, Issue 3
Superior Long-Term Energy Retention and Volumetric Energy Density for Li-Rich Cathode Materials
journal, September 2014
- Oh, Pilgun; Myeong, Seungjun; Cho, Woongrae
- Nano Letters, Vol. 14, Issue 10
Effect of Residual Lithium Compounds on Layer Ni-Rich Li[Ni 0.7 Mn 0.3 ]O 2
journal, January 2014
- Cho, Dae-Hyun; Jo, Chang-Heum; Cho, Woosuk
- Journal of The Electrochemical Society, Vol. 161, Issue 6
The Role of AlF3 Coatings in Improving Electrochemical Cycling of Li-Enriched Nickel-Manganese Oxide Electrodes for Li-Ion Batteries
journal, February 2012
- Sun, Yang-Kook; Lee, Min-Joon; Yoon, Chong S.
- Advanced Materials, Vol. 24, Issue 9
Mitigating Voltage Fade in Cathode Materials by Improving the Atomic Level Uniformity of Elemental Distribution
journal, April 2014
- Zheng, Jianming; Gu, Meng; Genc, Arda
- Nano Letters, Vol. 14, Issue 5
Structural evolution and the capacity fade mechanism upon long-term cycling in Li-rich cathode material
journal, January 2012
- Song, Bohang; Liu, Zongwen; Lai, Man On
- Physical Chemistry Chemical Physics, Vol. 14, Issue 37
Origin of voltage decay in high-capacity layered oxide electrodes
journal, December 2014
- Sathiya, M.; Abakumov, A. M.; Foix, D.
- Nature Materials, Vol. 14, Issue 2
Detailed Studies of a High-Capacity Electrode Material for Rechargeable Batteries, Li 2 MnO 3 −LiCo 1/3 Ni 1/3 Mn 1/3 O 2
journal, March 2011
- Yabuuchi, Naoaki; Yoshii, Kazuhiro; Myung, Seung-Taek
- Journal of the American Chemical Society, Vol. 133, Issue 12
The effect of Al2O3-coating coverage on the electrochemical properties in LiCoO2 thin films
journal, October 2009
- Oh, Yuhong; Ahn, Donggi; Nam, Seunghoon
- Journal of Solid State Electrochemistry, Vol. 14, Issue 7
Voltage Fade of Layered Oxides: Its Measurement and Impact on Energy Density
journal, January 2013
- Bettge, Martin; Li, Yan; Gallagher, Kevin
- Journal of The Electrochemical Society, Vol. 160, Issue 11
Direct In situ Observation of Li 2 O Evolution on Li-Rich High-Capacity Cathode Material, Li[Ni x Li (1–2 x )/3 Mn (2– x )/3 ]O 2 (0 ≤ x ≤0.5)
journal, January 2014
- Hy, Sunny; Felix, Felix; Rick, John
- Journal of the American Chemical Society, Vol. 136, Issue 3
Direct Atomic-Resolution Observation of Two Phases in the Li 1.2 Mn 0.567 Ni 0.166 Co 0.067 O 2 Cathode Material for Lithium-Ion Batteries
journal, April 2013
- Yu, Haijun; Ishikawa, Ryo; So, Yeong-Gi
- Angewandte Chemie International Edition, Vol. 52, Issue 23
Synthesis and Characterization of the Lithium-Rich Core–Shell Cathodes with Low Irreversible Capacity and Mitigated Voltage Fade
journal, April 2015
- Li, Jing; Camardese, John; Shunmugasundaram, Ramesh
- Chemistry of Materials, Vol. 27, Issue 9
First Evidence of Manganese–Nickel Segregation and Densification upon Cycling in Li-Rich Layered Oxides for Lithium Batteries
journal, July 2013
- Boulineau, Adrien; Simonin, Loïc; Colin, Jean-François
- Nano Letters, Vol. 13, Issue 8
Nickel-Rich Layered Lithium Transition-Metal Oxide for High-Energy Lithium-Ion Batteries
journal, March 2015
- Liu, Wen; Oh, Pilgun; Liu, Xien
- Angewandte Chemie International Edition, Vol. 54, Issue 15
Conflicting Roles of Nickel in Controlling Cathode Performance in Lithium Ion Batteries
journal, September 2012
- Gu, Meng; Belharouak, Ilias; Genc, Arda
- Nano Letters, Vol. 12, Issue 10
A New High Power LiNi 0.81 Co 0.1 Al 0.09 O 2 Cathode Material for Lithium-Ion Batteries
journal, April 2014
- Jo, Minki; Noh, Mijung; Oh, Pilgun
- Advanced Energy Materials, Vol. 4, Issue 13
High-Energy Cathode Materials (Li 2 MnO 3 –LiMO 2 ) for Lithium-Ion Batteries
journal, March 2013
- Yu, Haijun; Zhou, Haoshen
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 8
High Performance LiMn 2 O 4 Cathode Materials Grown with Epitaxial Layered Nanostructure for Li-Ion Batteries
journal, January 2014
- Lee, Min-Joon; Lee, Sanghan; Oh, Pilgun
- Nano Letters, Vol. 14, Issue 2
Roles of Surface Chemistry on Safety and Electrochemistry in Lithium Ion Batteries
journal, April 2012
- Lee, Kyu Tae; Jeong, Sookyung; Cho, Jaephil
- Accounts of Chemical Research, Vol. 46, Issue 5
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
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
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
High-energy cathode material for long-life and safe lithium batteries
journal, March 2009
- Sun, Yang-Kook; Myung, Seung-Taek; Park, Byung-Chun
- Nature Materials, Vol. 8, Issue 4
Atomic Structure of a Lithium-Rich Layered Oxide Material for Lithium-Ion Batteries: Evidence of a Solid Solution
journal, August 2011
- Jarvis, Karalee A.; Deng, Zengqiang; Allard, Lawrence F.
- Chemistry of Materials, Vol. 23, Issue 16
Atomic Structure of Li 2 MnO 3 after Partial Delithiation and Re-Lithiation
journal, June 2013
- Wang, Rui; He, Xiaoqing; He, Lunhua
- Advanced Energy Materials, Vol. 3, Issue 10
High-energy ‘composite’ layered manganese-rich cathode materials via controlling Li2MnO3 phase activation for lithium-ion batteries
journal, January 2012
- Yu, Haijun; Kim, Hyunjeong; Wang, Yarong
- Physical Chemistry Chemical Physics, Vol. 14, Issue 18
Stabilization of xLi2MnO3 ⋅ ( 1 − x ) LiMO2 Electrode Surfaces ( M = Mn , Ni , Co ) with Mildly Acidic, Fluorinated Solutions
journal, January 2008
- Kang, S.-H.; Thackeray, M. M.
- Journal of The Electrochemical Society, Vol. 155, Issue 4, p. A269-A275
Factors that affect Li mobility in layered lithium transition metal oxides
journal, September 2006
- Kang, Kisuk; Ceder, Gerbrand
- Physical Review B, Vol. 74, Issue 9
The role of nanoscale-range vanadium treatment in LiNi 0.8 Co 0.15 Al 0.05 O 2 cathode materials for Li-ion batteries at elevated temperatures
journal, January 2015
- Lee, Min-Joon; Noh, Mijung; Park, Mi-Hee
- Journal of Materials Chemistry A, Vol. 3, Issue 25
Direct Atomic-Resolution Observation of Two Phases in the Li 1.2 Mn 0.567 Ni 0.166 Co 0.067 O 2 Cathode Material for Lithium-Ion Batteries
journal, April 2013
- Yu, Haijun; Ishikawa, Ryo; So, Yeong-Gi
- Angewandte Chemie, Vol. 125, Issue 23
Roles of Surface Chemistry on Safety and Electrochemistry in Lithium Ion Batteries
journal, April 2012
- Lee, Kyu Tae; Jeong, Sookyung; Cho, Jaephil
- Accounts of Chemical Research, Vol. 46, Issue 5
Detailed Studies of a High-Capacity Electrode Material for Rechargeable Batteries, Li 2 MnO 3 −LiCo 1/3 Ni 1/3 Mn 1/3 O 2
journal, March 2011
- Yabuuchi, Naoaki; Yoshii, Kazuhiro; Myung, Seung-Taek
- Journal of the American Chemical Society, Vol. 133, Issue 12
High-Energy Cathode Materials (Li 2 MnO 3 –LiMO 2 ) for Lithium-Ion Batteries
journal, March 2013
- Yu, Haijun; Zhou, Haoshen
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 8
High Performance LiMn 2 O 4 Cathode Materials Grown with Epitaxial Layered Nanostructure for Li-Ion Batteries
journal, January 2014
- Lee, Min-Joon; Lee, Sanghan; Oh, Pilgun
- Nano Letters, Vol. 14, Issue 2
Mitigating Voltage Fade in Cathode Materials by Improving the Atomic Level Uniformity of Elemental Distribution
journal, April 2014
- Zheng, Jianming; Gu, Meng; Genc, Arda
- Nano Letters, Vol. 14, Issue 5
Superior Long-Term Energy Retention and Volumetric Energy Density for Li-Rich Cathode Materials
journal, September 2014
- Oh, Pilgun; Myeong, Seungjun; Cho, Woongrae
- Nano Letters, Vol. 14, Issue 10
High-energy cathode material for long-life and safe lithium batteries
journal, March 2009
- Sun, Yang-Kook; Myung, Seung-Taek; Park, Byung-Chun
- Nature Materials, Vol. 8, Issue 4
Reversible anionic redox chemistry in high-capacity layered-oxide electrodes
journal, July 2013
- Sathiya, M.; Rousse, G.; Ramesha, K.
- Nature Materials, Vol. 12, Issue 9
Origin of voltage decay in high-capacity layered oxide electrodes
journal, December 2014
- Sathiya, M.; Abakumov, A. M.; Foix, D.
- Nature Materials, Vol. 14, Issue 2
High-energy ‘composite’ layered manganese-rich cathode materials via controlling Li2MnO3 phase activation for lithium-ion batteries
journal, January 2012
- Yu, Haijun; Kim, Hyunjeong; Wang, Yarong
- Physical Chemistry Chemical Physics, Vol. 14, Issue 18
Works referencing / citing this record:
Surface Engineering Strategies of Layered LiCoO 2 Cathode Material to Realize High-Energy and High-Voltage Li-Ion Cells
journal, October 2016
- Kalluri, Sujith; Yoon, Moonsu; Jo, Minki
- Advanced Energy Materials, Vol. 7, Issue 1
Improving rate performance of cathode material Li1.2Mn0.54Co0.13Ni0.13O2 via niobium doping
journal, February 2018
- Zhao, Li; Wu, Qing; Wu, Jinzhu
- Journal of Solid State Electrochemistry, Vol. 22, Issue 7
Advanced cathode materials and efficient electrolytes for rechargeable batteries: practical challenges and future perspectives
journal, January 2019
- Khan, Safyan Akram; Ali, Shahid; Saeed, Khalid
- Journal of Materials Chemistry A, Vol. 7, Issue 17
Multishelled Ni x Co 3- x O 4 Hollow Microspheres Derived from Bimetal-Organic Frameworks as Anode Materials for High-Performance Lithium-Ion Batteries
journal, February 2017
- Wu, Lan-Lan; Wang, Zhuo; Long, Yan
- Small, Vol. 13, Issue 17
Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries
journal, April 2017
- Li, Wangda; Dolocan, Andrei; Oh, Pilgun
- Nature Communications, Vol. 8, Issue 1
Enhanced high-voltage cycling stability of Ni-rich cathode materials via the self-assembly of Mn-rich shells
journal, January 2019
- Dong, Xinyu; Yao, Junyi; Zhu, Wenchang
- Journal of Materials Chemistry A, Vol. 7, Issue 35
Synchronous Tailoring Surface Structure and Chemical Composition of Li-Rich-Layered Oxide for High-Energy Lithium-Ion Batteries
journal, August 2018
- Wu, Bing; Yang, Xiukang; Jiang, Xia
- Advanced Functional Materials, Vol. 28, Issue 37
Tuning Anionic Redox Activity and Reversibility for a High‐Capacity Li‐Rich Mn‐Based Oxide Cathode via an Integrated Strategy
journal, March 2019
- Li, Qingyuan; Zhou, Dong; Zhang, Lijuan
- Advanced Functional Materials, Vol. 29, Issue 10
Recent Developments on and Prospects for Electrode Materials with Hierarchical Structures for Lithium-Ion Batteries
journal, November 2017
- Zhou, Limin; Zhang, Kai; Hu, Zhe
- Advanced Energy Materials, Vol. 8, Issue 6
Artificial interphase engineering of electrode materials to improve the overall performance of lithium-ion batteries
journal, August 2017
- Zhu, Zhiqiang; Chen, Xiaodong
- Nano Research, Vol. 10, Issue 12
High-voltage positive electrode materials for lithium-ion batteries
journal, January 2017
- Li, Wangda; Song, Bohang; Manthiram, Arumugam
- Chemical Society Reviews, Vol. 46, Issue 10
Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies
journal, December 2019
- Liang, Longwei; Zhang, Wenheng; Zhao, Fei
- Advanced Materials Interfaces, Vol. 7, Issue 3
Li-Rich Layered Oxides and Their Practical Challenges: Recent Progress and Perspectives
journal, March 2019
- Hu, Sijiang; Pillai, Anoop. S.; Liang, Gemeng
- Electrochemical Energy Reviews, Vol. 2, Issue 2
Ultrathin Al2O3 Coating on LiNi0.8Co0.1Mn0.1O2 Cathode Material for Enhanced Cycleability at Extended Voltage Ranges
journal, February 2019
- Zhu, Wenchang; Huang, Xue; Liu, Tingting
- Coatings, Vol. 9, Issue 2
Extending the Service Life of High-Ni Layered Oxides by Tuning the Electrode-Electrolyte Interphase
journal, September 2018
- Li, Jianyu; Li, Wangda; You, Ya
- Advanced Energy Materials, Vol. 8, Issue 29
Degradation Mechanisms and Mitigation Strategies of Nickel-Rich NMC-Based Lithium-Ion Batteries
journal, October 2019
- Li, Tianyu; Yuan, Xiao-Zi; Zhang, Lei
- Electrochemical Energy Reviews, Vol. 3, Issue 1
A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries
journal, October 2019
- Li, Jianyu; Manthiram, Arumugam
- Advanced Energy Materials, Vol. 9, Issue 45
Advanced Lithium-Ion Batteries for Practical Applications: Technology, Development, and Future Perspectives
journal, July 2018
- Choi, Sinho; Wang, Guoxiu
- Advanced Materials Technologies, Vol. 3, Issue 9
Comparison of electrochemical performance of LiNi 1−x Co x O 2 cathode materials synthesized from coated (1− x )Ni(OH) 2 @ x Co(OH) 2 and doped Ni 1−x Co x (OH) 2 precursors
journal, January 2019
- Tang, Lei; Li, Gang; Xiao, Peng
- RSC Advances, Vol. 9, Issue 16