Mesoscale Chemomechanical Interplay of the LiNi0.8Co0.15Al0.05O2 Cathode in Solid-State Polymer Batteries
Abstract
Complex chemomechanical interplay exists over a wide range of length scales within the hierarchically structured lithium-ion battery. At the mesoscale, the interdependent structural complexity and chemical heterogeneity collectively govern the local chemistry and, as a result, critically influence the cell level performance. Here in this paper we investigate the morphology and state of charge (SOC) inhomogeneity within secondary NCA particles that were cycled in solid polymer batteries. We observe substantial inhomogeneity in the nickel oxidation state (a proxy for SOC) and loss of structural integrity within secondary particles after only 20 cycles due to significant intergranular cracking. The formation of mesoscale cracks causes loss of ionic and electrical contact within cathode particles, triggering increases in local impedance and rearrangement of transport pathways for charge carriers. This can eventually lead to deactivation of subparticle level domains in solid-state lithium-ion batteries. Our findings highlight the importance of proper mesoscale strain and defect management in polymer lithium-ion batteries.
- Authors:
-
- Robert Bosch LLC, Sunnyvale, CA (United States). Research and Technology Center; Karlsruhe Inst. of Technology (KIT) (Germany). Dept. of Mechanical Engineering
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Robert Bosch LLC, Sunnyvale, CA (United States). Research and Technology Center
- Seeo Inc., Hayward, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center of Electron Microscopy, Molecular Foundry
- Karlsruhe Inst. of Technology (KIT) (Germany). Dept. of Mechanical Engineering; Aalen Univ., Aalen (Germany). Materials Research Inst.
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Technologies Area; Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1503545
- Alternate Identifier(s):
- OSTI ID: 1637289
- Grant/Contract Number:
- AC02-76SF00515; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 31; Journal Issue: 2; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE
Citation Formats
Besli, Münir M., Xia, Sihao, Kuppan, Saravanan, Huang, Yiqing, Metzger, Michael, Shukla, Alpesh Khushalchand, Schneider, Gerhard, Hellstrom, Sondra, Christensen, Jake, Doeff, Marca M., and Liu, Yijin. Mesoscale Chemomechanical Interplay of the LiNi0.8Co0.15Al0.05O2 Cathode in Solid-State Polymer Batteries. United States: N. p., 2018.
Web. doi:10.1021/acs.chemmater.8b04418.
Besli, Münir M., Xia, Sihao, Kuppan, Saravanan, Huang, Yiqing, Metzger, Michael, Shukla, Alpesh Khushalchand, Schneider, Gerhard, Hellstrom, Sondra, Christensen, Jake, Doeff, Marca M., & Liu, Yijin. Mesoscale Chemomechanical Interplay of the LiNi0.8Co0.15Al0.05O2 Cathode in Solid-State Polymer Batteries. United States. https://doi.org/10.1021/acs.chemmater.8b04418
Besli, Münir M., Xia, Sihao, Kuppan, Saravanan, Huang, Yiqing, Metzger, Michael, Shukla, Alpesh Khushalchand, Schneider, Gerhard, Hellstrom, Sondra, Christensen, Jake, Doeff, Marca M., and Liu, Yijin. Wed .
"Mesoscale Chemomechanical Interplay of the LiNi0.8Co0.15Al0.05O2 Cathode in Solid-State Polymer Batteries". United States. https://doi.org/10.1021/acs.chemmater.8b04418. https://www.osti.gov/servlets/purl/1503545.
@article{osti_1503545,
title = {Mesoscale Chemomechanical Interplay of the LiNi0.8Co0.15Al0.05O2 Cathode in Solid-State Polymer Batteries},
author = {Besli, Münir M. and Xia, Sihao and Kuppan, Saravanan and Huang, Yiqing and Metzger, Michael and Shukla, Alpesh Khushalchand and Schneider, Gerhard and Hellstrom, Sondra and Christensen, Jake and Doeff, Marca M. and Liu, Yijin},
abstractNote = {Complex chemomechanical interplay exists over a wide range of length scales within the hierarchically structured lithium-ion battery. At the mesoscale, the interdependent structural complexity and chemical heterogeneity collectively govern the local chemistry and, as a result, critically influence the cell level performance. Here in this paper we investigate the morphology and state of charge (SOC) inhomogeneity within secondary NCA particles that were cycled in solid polymer batteries. We observe substantial inhomogeneity in the nickel oxidation state (a proxy for SOC) and loss of structural integrity within secondary particles after only 20 cycles due to significant intergranular cracking. The formation of mesoscale cracks causes loss of ionic and electrical contact within cathode particles, triggering increases in local impedance and rearrangement of transport pathways for charge carriers. This can eventually lead to deactivation of subparticle level domains in solid-state lithium-ion batteries. Our findings highlight the importance of proper mesoscale strain and defect management in polymer lithium-ion batteries.},
doi = {10.1021/acs.chemmater.8b04418},
journal = {Chemistry of Materials},
number = 2,
volume = 31,
place = {United States},
year = {Wed Dec 19 00:00:00 EST 2018},
month = {Wed Dec 19 00:00:00 EST 2018}
}
Web of Science
Works referenced in this record:
Aging Mechanisms of Electrode Materials in Lithium-Ion Batteries for Electric Vehicles
journal, January 2015
- Lin, Cheng; Tang, Aihua; Mu, Hao
- Journal of Chemistry, Vol. 2015
Electrical Energy Storage for the Grid: A Battery of Choices
journal, November 2011
- Dunn, B.; Kamath, H.; Tarascon, J. -M.
- Science, Vol. 334, Issue 6058
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
Atomic Layer Deposition of the Solid Electrolyte Garnet Li 7 La 3 Zr 2 O 12
journal, April 2017
- Kazyak, Eric; Chen, Kuan-Hung; Wood, Kevin N.
- Chemistry of Materials, Vol. 29, Issue 8
Are All-Solid-State Lithium-Ion Batteries Really Safe?–Verification by Differential Scanning Calorimetry with an All-Inclusive Microcell
journal, January 2017
- Inoue, Takao; Mukai, Kazuhiko
- ACS Applied Materials & Interfaces, Vol. 9, Issue 2
Recent progress in solid oxide and lithium ion conducting electrolytes research
journal, April 2006
- Thangadurai, V.; Weppner, W.
- Ionics, Vol. 12, Issue 1
Issues and challenges facing rechargeable lithium batteries
journal, November 2001
- Tarascon, J.-M.; Armand, M.
- Nature, Vol. 414, Issue 6861, p. 359-367
A perspective on nickel-rich layered oxide cathodes for lithium-ion batteries
journal, January 2017
- Manthiram, Arumugam; Song, Bohang; Li, Wangda
- Energy Storage Materials, Vol. 6
Deformation and stress in electrode materials for Li-ion batteries
journal, June 2014
- Mukhopadhyay, Amartya; Sheldon, Brian W.
- Progress in Materials Science, Vol. 63
Microstructural Observation of LiNi 0.8 Co 0.15 Al 0.05 O 2 after Charge and Discharge by Scanning Transmission Electron Microscopy
journal, January 2012
- Makimura, Yoshinari; Zheng, Shijian; Ikuhara, Yuichi
- Journal of The Electrochemical Society, Vol. 159, Issue 7
Intrinsic Origins of Crack Generation in Ni-rich LiNi0.8Co0.1Mn0.1O2 Layered Oxide Cathode Material
journal, January 2017
- Lim, Jin-Myoung; Hwang, Taesoon; Kim, Duho
- Scientific Reports, Vol. 7, Issue 1
Impact of Microcrack Generation and Surface Degradation on a Nickel-Rich Layered Li[Ni 0.9 Co 0.05 Mn 0.05 ]O 2 Cathode for Lithium-Ion Batteries
journal, September 2017
- Sun, Ho-Hyun; Manthiram, Arumugam
- Chemistry of Materials, Vol. 29, Issue 19
Degradation analysis of a Ni-based layered positive-electrode active material cycled at elevated temperatures studied by scanning transmission electron microscopy and electron energy-loss spectroscopy
journal, September 2011
- Kojima, Y.; Muto, S.; Tatsumi, K.
- Journal of Power Sources, Vol. 196, Issue 18
Capacity fading of LiAlyNi1−x−yCoxO2 cathode for lithium-ion batteries during accelerated calendar and cycle life tests (effect of depth of discharge in charge–discharge cycling on the suppression of the micro-crack generation of LiAlyNi1−x−yCoxO2 particle)
journal, August 2014
- Watanabe, Shoichiro; Kinoshita, Masahiro; Hosokawa, Takashi
- Journal of Power Sources, Vol. 260
Electrolyte-Induced Surface Transformation and Transition-Metal Dissolution of Fully Delithiated LiNi 0.8 Co 0.15 Al 0.05 O 2
journal, June 2017
- Faenza, Nicholas V.; Lebens-Higgins, Zachary W.; Mukherjee, Pinaki
- Langmuir, Vol. 33, Issue 37
Charge Heterogeneity and Surface Chemistry in Polycrystalline Cathode Materials
journal, March 2018
- Tian, Chixia; Xu, Yahong; Nordlund, Dennis
- Joule, Vol. 2, Issue 3
Probing electrical degradation of cathode materials for lithium-ion batteries with nanoscale resolution
journal, July 2018
- Park, Seong Yong; Baek, Woon Joong; Lee, Seung Yeon
- Nano Energy, Vol. 49
STEM characterization for lithium-ion battery cathode materials
journal, February 2012
- Huang, Rong; Ikuhara, Yuichi
- Current Opinion in Solid State and Materials Science, Vol. 16, Issue 1
Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials
journal, April 2018
- Mu, Linqin; Lin, Ruoqian; Xu, Rong
- Nano Letters, Vol. 18, Issue 5
Modeling Diffusion-Induced Stress in Li-Ion Cells with Porous Electrodes
journal, January 2010
- Christensen, Jake
- Journal of The Electrochemical Society, Vol. 157, Issue 3, p. A366-A380
Stress generation and fracture in lithium insertion materials
journal, March 2006
- Christensen, John; Newman, John
- Journal of Solid State Electrochemistry, Vol. 10, Issue 5
Evolution of stress within a spherical insertion electrode particle under potentiostatic and galvanostatic operation
journal, May 2009
- Cheng, Yang-Tse; Verbrugge, Mark W.
- Journal of Power Sources, Vol. 190, Issue 2, p. 453-460
“Electrochemical Shock” of Intercalation Electrodes: A Fracture Mechanics Analysis
journal, January 2010
- Woodford, William H.; Chiang, Yet-Ming; Carter, W. Craig
- Journal of The Electrochemical Society, Vol. 157, Issue 10
Failure mechanism analysis of LiNi 0.88 Co 0.09 Mn 0.03 O 2 cathodes in Li-ion full cells
journal, August 2017
- Woo, Sang-Gil; Kim, Jae-Hun; Kim, Hyang-Rim
- Journal of Electroanalytical Chemistry, Vol. 799
Intragranular cracking as a critical barrier for high-voltage usage of layer-structured cathode for lithium-ion batteries
journal, January 2017
- Yan, Pengfei; Zheng, Jianming; Gu, Meng
- Nature Communications, Vol. 8, Issue 1
Suppressed oxygen extraction and degradation of LiNi x Mn y Co z O2 cathodes at high charge cut-off voltages
journal, September 2017
- Zheng, Jianming; Yan, Pengfei; Zhang, Jiandong
- Nano Research, Vol. 10, Issue 12
Post mortem analysis of fatigue mechanisms in LiNi0.8Co0.15Al0.05O2 – LiNi0.5Co0.2Mn0.3O2 – LiMn2O4/graphite lithium ion batteries
journal, September 2016
- Lang, Michael; Darma, Mariyam Susana Dewi; Kleiner, Karin
- Journal of Power Sources, Vol. 326
Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries
journal, November 2018
- Xia, Sihao; Mu, Linqin; Xu, Zhengrui
- Nano Energy, Vol. 53
High-Energy Ni-Rich Li[Ni x Co y Mn 1 –x–y ]O 2 Cathodes via Compositional Partitioning for Next-Generation Electric Vehicles
journal, November 2017
- Yoon, Chong S.; Park, Kang-Joon; Kim, Un-Hyuck
- Chemistry of Materials, Vol. 29, Issue 24
Capacity fading behavior of Ni-rich layered cathode materials in Li-ion full cells
journal, December 2016
- Kim, Hyang-Rim; Woo, Sang-Gil; Kim, Jae-Hun
- Journal of Electroanalytical Chemistry, Vol. 782
Structural Origin of Overcharge-Induced Thermal Instability of Ni-Containing Layered-Cathodes for High-Energy-Density Lithium Batteries
journal, September 2011
- Wu, Lijun; Nam, Kyung-Wan; Wang, Xiaojian
- Chemistry of Materials, Vol. 23, Issue 17
Correlating Structural Changes and Gas Evolution during the Thermal Decomposition of Charged Li x Ni 0.8 Co 0.15 Al 0.05 O 2 Cathode Materials
journal, January 2013
- Bak, Seong-Min; Nam, Kyung-Wan; Chang, Wonyoung
- Chemistry of Materials, Vol. 25, Issue 3
Mechanism of anodic cleavage of benzyl ethers
journal, May 1980
- Boyd, Jean W.; Schmalzl, Paul W.; Miller, Larry L.
- Journal of the American Chemical Society, Vol. 102, Issue 11
Revisiting the Corrosion of the Aluminum Current Collector in Lithium-Ion Batteries
journal, February 2017
- Ma, Tianyuan; Xu, Gui-Liang; Li, Yan
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 5
In Situ X-Ray Absorption Studies of a High-Rate LiNi[sub 0.85]Co[sub 0.15]O[sub 2] Cathode Material
journal, January 2000
- Balasubramanian, M.; Sun, X.; Yang, X. Q.
- Journal of The Electrochemical Society, Vol. 147, Issue 8
A study of room-temperature LixMn1.5Ni0.5O4 solid solutions
journal, January 2015
- Saravanan, Kuppan; Jarry, Angelique; Kostecki, Robert
- Scientific Reports, Vol. 5, Issue 1
Profiling the nanoscale gradient in stoichiometric layered cathode particles for lithium-ion batteries
journal, January 2014
- Lin, Feng; Nordlund, Dennis; Markus, Isaac M.
- Energy & Environmental Science, Vol. 7, Issue 9
Investigation of Changes in the Surface Structure of Li x Ni 0.8 Co 0.15 Al 0.05 O 2 Cathode Materials Induced by the Initial Charge
journal, December 2013
- Hwang, Sooyeon; Chang, Wonyoung; Kim, Seung Min
- Chemistry of Materials, Vol. 26, Issue 2
Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries
journal, March 2014
- Lin, Feng; Markus, Isaac M.; Nordlund, Dennis
- Nature Communications, Vol. 5, Issue 1
High performance PEO-based polymer electrolytes and their application in rechargeable lithium polymer batteries
journal, August 2007
- Sumathipala, H. H.; Hassoun, J.; Panero, S.
- Ionics, Vol. 13, Issue 5
Mesoscale Battery Science: The Behavior of Electrode Particles Caught on a Multispectral X-ray Camera
journal, June 2018
- Wei, Chenxi; Xia, Sihao; Huang, Hai
- Accounts of Chemical Research, Vol. 51, Issue 10
TXM-Wizard : a program for advanced data collection and evaluation in full-field transmission X-ray microscopy
journal, January 2012
- Liu, Yijin; Meirer, Florian; Williams, Phillip A.
- Journal of Synchrotron Radiation, Vol. 19, Issue 2
Three-dimensional imaging of chemical phase transformations at the nanoscale with full-field transmission X-ray microscopy
journal, July 2011
- Meirer, Florian; Cabana, Jordi; Liu, Yijin
- Journal of Synchrotron Radiation, Vol. 18, Issue 5
Nanoscale elemental sensitivity study of Nd 2 Fe 14 B using absorption correlation tomography : Nanoscale Elemental Sensitivity Study of N
journal, August 2013
- Kao, Thomas L.; Shi, Crystal Y.; Wang, Junyue
- Microscopy Research and Technique, Vol. 76, Issue 11
Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy
journal, February 2017
- Kuppan, Saravanan; Xu, Yahong; Liu, Yijin
- Nature Communications, Vol. 8, Issue 1
Single-particle measurements of electrochemical kinetics in NMC and NCA cathodes for Li-ion batteries
journal, January 2018
- Tsai, Ping-Chun; Wen, Bohua; Wolfman, Mark
- Energy & Environmental Science, Vol. 11, Issue 4
Formation of an Anti-Core–Shell Structure in Layered Oxide Cathodes for Li-Ion Batteries
journal, October 2017
- Zhang, Hanlei; Omenya, Fredrick; Whittingham, M. Stanley
- ACS Energy Letters, Vol. 2, Issue 11
Investigation of the Charge Compensation Mechanism on the Electrochemically Li-Ion Deintercalated Li 1 - x Co 1/3 Ni 1/3 Mn 1/3 O 2 Electrode System by Combination of Soft and Hard X-ray Absorption Spectroscopy
journal, December 2005
- Yoon, Won-Sub; Balasubramanian, Mahalingam; Chung, Kyung Yoon
- Journal of the American Chemical Society, Vol. 127, Issue 49
Structural and Electrochemical Investigation of Li(Ni[sub 0.4]Co[sub 0.15]Al[sub 0.05]Mn[sub 0.4])O[sub 2] Cathode Material
journal, January 2010
- Rumble, C.; Conry, T. E.; Doeff, Marca
- Journal of The Electrochemical Society, Vol. 157, Issue 12
A review of Ni-based layered oxides for rechargeable Li-ion batteries
journal, January 2017
- Xu, Jing; Lin, Feng; Doeff, Marca M.
- Journal of Materials Chemistry A, Vol. 5, Issue 3
Single-Crystalline Particles: An Effective Way to Ameliorate the Intragranular Cracking, Thermal Stability, and Capacity Fading of the LiNi 0.6 Co 0.2 Mn 0.2 O 2 Electrodes
journal, January 2018
- Liu, Guilong; Li, Minglu; Wu, Naiteng
- Journal of The Electrochemical Society, Vol. 165, Issue 13
Modification of Ni-Rich FCG NMC and NCA Cathodes by Atomic Layer Deposition: Preventing Surface Phase Transitions for High-Voltage Lithium-Ion Batteries
journal, May 2016
- Mohanty, Debasish; Dahlberg, Kevin; King, David M.
- Scientific Reports, Vol. 6, Issue 1
Effect of Molecular Weight and Salt Concentration on Conductivity of Block Copolymer Electrolytes
journal, July 2009
- Panday, Ashoutosh; Mullin, Scott; Gomez, Enrique D.
- Macromolecules, Vol. 42, Issue 13
Simultaneous Electronic and Ionic Conduction in a Block Copolymer: Application in Lithium Battery Electrodes
journal, September 2011
- Javier, Anna E.; Patel, Shrayesh N.; Hallinan, Daniel T.
- Angewandte Chemie International Edition, Vol. 50, Issue 42
Discharge Characteristics of Lithium Battery Electrodes with a Semiconducting Polymer Studied by Continuum Modeling and Experiment
journal, January 2014
- Wu, Shao-Ling; Javier, Anna E.; Devaux, Didier
- Journal of The Electrochemical Society, Vol. 161, Issue 12
Phase retrieval using polychromatic illumination for transmission X-ray microscopy
journal, January 2011
- Liu, Yijin; Andrews, Joy C.; Wang, Junyue
- Optics Express, Vol. 19, Issue 2
Works referencing / citing this record:
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
Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials
journal, January 2020
- Xu, Zhengrui; Jiang, Zhisen; Kuai, Chunguang
- Nature Communications, Vol. 11, Issue 1
Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries
journal, January 2020
- Teichert, Philipp; Eshetu, Gebrekidan Gebresilassie; Jahnke, Hannes
- Batteries, Vol. 6, Issue 1
Enhanced High‐Temperature Electrochemical Performance of Layered Nickel‐Rich Cathodes for Lithium‐Ion Batteries after LiF Surface Modification
journal, October 2019
- Huang, Jinlong; Du, Ke; Peng, Zhongdong
- ChemElectroChem, Vol. 6, Issue 21
Long-term chemothermal stability of delithiated NCA in polymer solid-state batteries
journal, January 2019
- Besli, Münir M.; Usubelli, Camille; Metzger, Michael
- Journal of Materials Chemistry A, Vol. 7, Issue 47
Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries
text, January 2020
- Teichert, Philipp; Eshetu, Gebrekidan Gebresilassie; Jahnke, Hannes
- RWTH Aachen University
Long-Term Chemothermal Stability of Delithiated NCA in Polymer Solid-State Batteries
text, January 2019
- Besli, Münir M.; Usubelli, Camille; Metzger, Michael
- Karlsruhe