Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes

Han, Binghong; Paulauskas, Tadas; Key, Baris; Peebles, Cameron; Park, Joong Sun; Klie, Robert F.; Vaughey, John T.; Dogan, Fulya

doi:10.1021/acsami.7b00595

Title: Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes

Journal Article · Fri Apr 07 00:00:00 EDT 2017 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b00595· OSTI ID:1374597

Han, Binghong ^[1]; Paulauskas, Tadas ^[2]; Key, Baris ^[1]; Peebles, Cameron ^[1]; Park, Joong Sun ^[1]; Klie, Robert F. ^[2];

^[1];

^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Illinois, Chicago, IL (United States)

Here, surface coating of cathode materials with Al₂O₃ has been shown to be a promising method for cathode stabilization and improved cycling performance at high operating voltages. However, a detailed understanding on how coating process and cathode composition changes the chemical composition, morphology and distribution of coating within cathode interface and bulk lattice, is still missing. In this study, we use a wet-chemical method to synthesize a series of Al₂O₃-coated LiNi_0.5Co_0.2Mn_0.3O₂ and LiCoO₂ cathodes treated under various annealing temperatures and a combination of structural characterization techniques to understand the composition, homogeneity and morphology of coating layer and the bulk cathode. Nuclear magnetic resonance and electron microscopy results reveal that the nature of the interface is highly depended on the annealing temperature and cathode composition. For Al₂O₃-coated LiNi_0.5Co_0.2Mn_0.3O₂, higher annealing temperature leads to more homogeneous and more closely attached coating on cathode materials, corresponding to better electrochemical performance. Lower Al₂O₃ coating content is found to be helpful to further improve the initial capacity and cyclability, which can greatly outperform the pristine cathode material. For Al₂O₃-coated LiCoO₂, the incorporation of Al into the cathode lattice is observed after annealing at high temperatures, implying the transformation from “surface coatings” to “dopants”, which is not observed for LiNi_0.5Co_0.2Mn_0.3O₂. As a result, Al₂O₃-coated LiCoO₂ annealed at higher temperature shows similar initial capacity but lower retention compared to that annealed at a lower temperature, due to the intercalation of surface alumina into the bulk layered structure forming a solid solution.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1374597

Journal Information:: ACS Applied Materials and Interfaces, Vol. 9, Issue 17; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 104 works

Citation information provided by
Web of Science

References (36)

Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
Recent advances in the US Department of Energy’s energy storage technology research and development programs for hybrid electric and electric vehicles Weinstock, Irwin B. Journal of Power Sources, Vol. 110, Issue 2 https://doi.org/10.1016/S0378-7753(02)00211-2	journal	August 2002
Performance of layered Li(Ni1/3Co1/3Mn1/3)O2 as cathode for Li-ion batteries Shaju, K. M.; Subba Rao, G. V.; Chowdari, B. V. R. Electrochimica Acta, Vol. 48, Issue 2 https://doi.org/10.1016/S0013-4686(02)00593-5	journal	November 2002
Understanding the Degradation Mechanisms of LiNi _0.5 Co _0.2 Mn _0.3 O ₂ Cathode Material in Lithium Ion Batteries Jung, Sung-Kyun; Gwon, Hyeokjo; Hong, Jihyun Advanced Energy Materials, Vol. 4, Issue 1 https://doi.org/10.1002/aenm.201300787	journal	August 2013
Synthesis, Characterization, and Electrochemical Behavior of Improved Li[Ni[sub x]Co[sub 1−2x]Mn[sub x]]O[sub 2] (0.1≤x≤0.5) Jouanneau, S.; Eberman, K. W.; Krause, L. J. Journal of The Electrochemical Society, Vol. 150, Issue 12 https://doi.org/10.1149/1.1622956	journal	January 2003
Layered Li[Ni[sub x]Co[sub 1−2x]Mn[sub x]]O[sub 2] Cathode Materials for Lithium-Ion Batteries Lu, Zhonghua; MacNeil, D. D.; Dahn, J. R. Electrochemical and Solid-State Letters, Vol. 4, Issue 12 https://doi.org/10.1149/1.1413182	journal	January 2001
Novel lithium insertion material of LiCo1/3Ni1/3Mn1/3O2 for advanced lithium-ion batteries Yabuuchi, Naoaki; Ohzuku, Tsutomu Journal of Power Sources, Vol. 119-121 https://doi.org/10.1016/S0378-7753(03)00173-3	journal	June 2003
Layered Lithium Insertion Material of LiCo _1/3 Ni _1/3 Mn _1/3 O ₂ for Lithium-Ion Batteries Ohzuku, Tsutomu; Makimura, Yoshinari Chemistry Letters, Vol. 30, Issue 7 https://doi.org/10.1246/cl.2001.642	journal	July 2001
Synthesis and characterization of LiNi1−x−yCoxMnyO2 as the cathode materials of secondary lithium batteries Liu, Zhaolin; Yu, Aishui; Lee, Jim Y. Journal of Power Sources, Vol. 81-82 https://doi.org/10.1016/S0378-7753(99)00221-9	journal	September 1999
Influence of the synthesis route on the electrochemical properties of LiNi0.425Mn0.425Co0.15O2 Tran, N.; Croguennec, L.; Jordy, C. Solid State Ionics, Vol. 176, Issue 17-18 https://doi.org/10.1016/j.ssi.2005.04.039	journal	May 2005
Structural and electrochemical behavior of LiMn0.4Ni0.4Co0.2O2 Ma, Miaomiao; Chernova, Natasha A.; Toby, Brian H. Journal of Power Sources, Vol. 165, Issue 2 https://doi.org/10.1016/j.jpowsour.2006.10.022	journal	March 2007
Electrochemical Evaluation and Structural Characterization of Commercial LiCoO[sub 2] Surfaces Modified with MgO for Lithium-Ion Batteries Wang, Zhaoxiang; Wu, Chuan; Liu, Lijun Journal of The Electrochemical Society, Vol. 149, Issue 4 https://doi.org/10.1149/1.1456919	journal	January 2002
A simple mechano-thermal coating process for improved lithium battery cathode materials Fey, George Ting-Kuo; Yang, Hao-Zhong; Prem Kumar, T. Journal of Power Sources, Vol. 132, Issue 1-2 https://doi.org/10.1016/j.jpowsour.2004.01.033	journal	May 2004
Electrochemical Performance and Surface Properties of Bare and TiO ₂ -Coated Cathode Materials in Lithium-Ion Batteries Zhang, Zhongru; Gong, Zhengliang; Yang, Yong The Journal of Physical Chemistry B, Vol. 108, Issue 45 https://doi.org/10.1021/jp046980h	journal	November 2004
Improvement of Degradation at Elevated Temperature and at High State-of-Charge Storage by ZrO[sub 2] Coating on LiCoO[sub 2] Miyashiro, Hajime; Yamanaka, Atsushi; Tabuchi, Mitsuharu Journal of The Electrochemical Society, Vol. 153, Issue 2 https://doi.org/10.1149/1.2149306	journal	January 2006
Effects of ZnO coating on electrochemical performance and thermal stability of LiCoO2 as cathode material for lithium-ion batteries Chang, Wonyoung; Choi, Jung-Woo; Im, Jong-Choo Journal of Power Sources, Vol. 195, Issue 1 https://doi.org/10.1016/j.jpowsour.2009.06.104	journal	January 2010
Novel LiCoO₂ Cathode Material with Al₂O₃ Coating for a Li Ion Cell Cho, Jaephil; Kim, Yong Jeong; Park, Byungwoo Chemistry of Materials, Vol. 12, Issue 12, p. 3788-3791 https://doi.org/10.1021/cm000511k	journal	December 2000
Al2O3-coated LiCoO2 as cathode material for lithium ion batteries Liu, L. Solid State Ionics, Vol. 152-153 https://doi.org/10.1016/S0167-2738(02)00333-8	journal	December 2002
High Capacity Surface-Modified LiCoO[sub 2] Cathodes for Lithium-Ion Batteries Kannan, A. M.; Rabenberg, L.; Manthiram, A. Electrochemical and Solid-State Letters, Vol. 6, Issue 1 https://doi.org/10.1149/1.1526782	journal	January 2003
Electrochemical and solid-state NMR studies on LiCoO2 coated with Al2O3 derived from carboxylate-alumoxane Fey, George T. K.; Kao, H. M.; Muralidharan, P. Journal of Power Sources, Vol. 163, Issue 1 https://doi.org/10.1016/j.jpowsour.2006.01.076	journal	December 2006
Effects of Al<sub>2</sub>O<sub>3</sub> Coating on the Structural and Electrochemical Performance of LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub> Cathode Material Cao, Kun Jian; Wang, Li; Li, Lin Ci Applied Mechanics and Materials, Vol. 320 https://doi.org/10.4028/www.scientific.net/AMM.320.235	journal	May 2013
Surface-modified concentration-gradient Ni-rich layered oxide cathodes for high-energy lithium-ion batteries Liao, Jin-Yun; Manthiram, Arumugam Journal of Power Sources, Vol. 282 https://doi.org/10.1016/j.jpowsour.2015.02.078	journal	May 2015
Role of Alumina Coating on Li−Ni−Co−Mn−O Particles as Positive Electrode Material for Lithium-Ion Batteries Myung, Seung-Taek; Izumi, Kentarou; Komaba, Shinichi Chemistry of Materials, Vol. 17, Issue 14, p. 3695-3704 https://doi.org/10.1021/cm050566s	journal	July 2005
Ultrathin Al2O3 Coatings for Improved Cycling Performance and Thermal Stability of LiNi0.5Co0.2Mn0.3O2 Cathode Material Shi, Yang; Zhang, Minghao; Qian, Danna Electrochimica Acta, Vol. 203 https://doi.org/10.1016/j.electacta.2016.03.185	journal	June 2016
Atomic Layer Deposition: An Overview George, Steven M. Chemical Reviews, Vol. 110, Issue 1, p. 111-131 https://doi.org/10.1021/cr900056b	journal	January 2010
Electrochemical effects of ALD surface modification on combustion synthesized LiNi1/3Mn1/3Co1/3O2 as a layered-cathode material Riley, Leah A.; Van Atta, Sky; Cavanagh, Andrew S. Journal of Power Sources, Vol. 196, Issue 6 https://doi.org/10.1016/j.jpowsour.2010.11.124	journal	March 2011
Enhancing the High-Voltage Cycling Performance of LiNi _0.5 Mn _0.3 Co _0.2 O ₂ by Retarding Its Interfacial Reaction with an Electrolyte by Atomic-Layer-Deposited Al ₂ O ₃ Su, Yantao; Cui, Suihan; Zhuo, Zengqing ACS Applied Materials & Interfaces, Vol. 7, Issue 45 https://doi.org/10.1021/acsami.5b05500	journal	November 2015
Low-Cost Al ₂ O ₃ Coating Layer As a Preformed SEI on Natural Graphite Powder To Improve Coulombic Efficiency and High-Rate Cycling Stability of Lithium-Ion Batteries Feng, Tianyu; Xu, Youlong; Zhang, Zhengwei ACS Applied Materials & Interfaces, Vol. 8, Issue 10 https://doi.org/10.1021/acsami.6b00231	journal	March 2016
Ultrathin Coatings on Nano-LiCoO₂ for Li-Ion Vehicular Applications Scott, Isaac D.; Jung, Yoon Seok; Cavanagh, Andrew S. Nano Letters, Vol. 11, Issue 2, p. 414-418 https://doi.org/10.1021/nl1030198	journal	February 2011
Ultrathin Direct Atomic Layer Deposition on Composite Electrodes for Highly Durable and Safe Li-Ion Batteries Jung, Yoon Seok; Cavanagh, Andrew S.; Riley, Leah A. Advanced Materials, Vol. 22, Issue 19 https://doi.org/10.1002/adma.200903951	journal	April 2010
Direct Observation of Lattice Aluminum Environments in Li Ion Cathodes LiNi _{1– y – z} Co _y Al _z O ₂ and Al-Doped LiNi _x Mn _y Co _z O ₂ via ²⁷ Al MAS NMR Spectroscopy Dogan, Fulya; Vaughey, John T.; Iddir, Hakim ACS Applied Materials & Interfaces, Vol. 8, Issue 26 https://doi.org/10.1021/acsami.6b04516	journal	June 2016
Characterization of interphases appearing on LiNi0.5Mn0.5O2 using 7Li MAS NMR Dupré, Nicolas; Martin, Jean-Frédéric; Guyomard, Dominique Journal of Power Sources, Vol. 189, Issue 1 https://doi.org/10.1016/j.jpowsour.2008.10.017	journal	April 2009
Detection of surface layers using 7Li MAS NMR Dupré, Nicolas; Martin, Jean-Frédéric; Guyomard, Dominique Journal of Materials Chemistry, Vol. 18, Issue 36 https://doi.org/10.1039/b807778a	journal	January 2008
Cobalt(III) Effect on ²⁷ Al NMR Chemical Shifts in LiAl _x Co ₁ _- _x O ₂ Gaudin, E.; Taulelle, F.; Stoyanova, R. The Journal of Physical Chemistry B, Vol. 105, Issue 34 https://doi.org/10.1021/jp0105948	journal	August 2001
How Do Li Atoms Pass through the Al ₂ O ₃ Coating Layer during Lithiation in Li-ion Batteries? Jung, Sung Chul; Han, Young-Kyu The Journal of Physical Chemistry Letters, Vol. 4, Issue 16 https://doi.org/10.1021/jz401231e	journal	July 2013
Phase Separation Tendencies of Aluminum-Doped Transition-Metal Oxides (LiAl[sub 1−x]M[sub x]O[sub 2]) in the α-NaFeO[sub 2] Crystal Structure Buta, S. Journal of The Electrochemical Society, Vol. 146, Issue 12 https://doi.org/10.1149/1.1392639	journal	January 1999

Cited By (12)

Editors' Choice—Coating-Dependent Electrode-Electrolyte Interface for Ni-Rich Positive Electrodes in Li-Ion Batteries Karayaylali, Pinar; Tatara, Ryoichi; Zhang, Yirui Journal of The Electrochemical Society, Vol. 166, Issue 6 https://doi.org/10.1149/2.0461906jes	journal	January 2019
Development of Electrolytes for Single Crystal NMC532/Artificial Graphite Cells with Long Lifetime Li, Jing; Li, Hongyang; Stone, Will Journal of The Electrochemical Society, Vol. 165, Issue 3 https://doi.org/10.1149/2.0971803jes	journal	January 2018
Horizons for Li-Ion Batteries Relevant to Electro-Mobility: High-Specific-Energy Cathodes and Chemically Active Separators Susai, Francis Amalraj; Sclar, Hadar; Shilina, Yuliya Advanced Materials, Vol. 30, Issue 41 https://doi.org/10.1002/adma.201801348	journal	July 2018
Effect of Low-Temperature Al2O3 ALD Coating on Ni-Rich Layered Oxide Composite Cathode on the Long-Term Cycling Performance of Lithium-Ion Batteries Neudeck, Sven; Mazilkin, Andrey; Reitz, Christian Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-41767-0	journal	March 2019
Ni–Al–Cr superalloy as high temperature cathode current collector for advanced thin film Li batteries Filippin, Alejandro N.; Lin, Tzu-Ying; Rawlence, Michael RSC Advances, Vol. 8, Issue 36 https://doi.org/10.1039/c8ra02461h	journal	January 2018
A Critical Review: The Impact of the Battery Electrode Material Substrate on the Composition and Properties of Atomic Layer Deposition (ALD) Coatings Tiurin, Ortal; Ein‐Eli, Yair Advanced Materials Interfaces, Vol. 6, Issue 24 https://doi.org/10.1002/admi.201901455	journal	October 2019
Oxygen Release Degradation in Li‐Ion Battery Cathode Materials: Mechanisms and Mitigating Approaches Sharifi‐Asl, Soroosh; Lu, Jun; Amine, Khalil Advanced Energy Materials, Vol. 9, Issue 22 https://doi.org/10.1002/aenm.201900551	journal	April 2019
Controllable Cathode–Electrolyte Interface of Li[Ni _0.8 Co _0.1 Mn _0.1 ]O ₂ for Lithium Ion Batteries: A Review Maleki Kheimeh Sari, Hirbod; Li, Xifei Advanced Energy Materials, Vol. 9, Issue 39 https://doi.org/10.1002/aenm.201901597	journal	August 2019
Influence of Coating Protocols on Alumina-Coated Cathode Material: Atomic Layer Deposition versus Wet-Chemical Coating Han, Binghong; Key, Baris; Lipton, Andrew S. Journal of The Electrochemical Society, Vol. 166, Issue 15 https://doi.org/10.1149/2.0681915jes	journal	January 2019
Tailoring Alumina Based Interphases on Lithium Ion Cathodes Han, Binghong; Dunlop, Alison R.; Trask, Stephen E. Journal of The Electrochemical Society, Vol. 165, Issue 14 https://doi.org/10.1149/2.0211814jes	journal	January 2018
Ni-Al-Cr superalloy as high temperature cathode current collector for advanced thin film Li batteries N., Filippin, Alejandro; Tzu-Ying, Lin,; Michael, Rawlence, ETH Zurich https://doi.org/10.3929/ethz-b-000271469	text	January 2018
Room temperature, liquid-phase Al 2 O 3 surface coating approach for Ni-rich layered oxide cathode material Neudeck, S.; Strauss, F.; Garcia, G. Karlsruhe https://doi.org/10.5445/ir/1000092529	text	January 2019

Similar Records

From Coating to Dopant: How the Transition Metal Composition Affects Alumina Coatings on Ni-Rich Cathodes

Journal Article · Wed Nov 01 00:00:00 EDT 2017 · ACS Applied Materials and Interfaces · OSTI ID:1374597

Han, Binghong; Key, Baris; Lapidus, Saul H.; +4 more

Tailoring Alumina Based Interphases on Lithium Ion Cathodes

Journal Article · Fri Oct 19 00:00:00 EDT 2018 · Journal of the Electrochemical Society · OSTI ID:1374597

Han, Binghong; Dunlop, Alison R.; Trask, Stephen E.; +3 more

Interfacial engineering for stabilizing polymer electrolytes with 4V cathodes in lithium metal batteries at elevated temperature

Journal Article · Thu Mar 05 00:00:00 EST 2020 · Nano Energy · OSTI ID:1374597

Li, Zeyuan; Li, Aijun; Zhang, Hanrui; +16 more

Related Subjects

36 MATERIALS SCIENCE
25 ENERGY STORAGE
27Al MAS NMR
Al2O3 coating
coating vs doping
LCO
NMC
TEM

Title: Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes

Citation Formats

References (36)

Cited By (12)

Similar Records

Related Subjects