Influence of Calendering on the Electrochemical Performance of LiNi0.9Mn0.05Al0.05O2 Cathodes in Lithium-Ion Cells

Sim, Richard; Lee, Steven; Li, Wangda; Manthiram, Arumugam

doi:10.1021/acsami.1c12543

Title: Influence of Calendering on the Electrochemical Performance of LiNi_0.9Mn_0.05Al_0.05O₂ Cathodes in Lithium-Ion Cells

Journal Article · 30 August 2021 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.1c12543 · OSTI ID:1972444

Sim, Richard ^[1]; Lee, Steven ^[2];

^[2];

^[2]

Univ. of Texas at Austin, TX (United States); University of Texas at Austin
Univ. of Texas at Austin, TX (United States)

Electrode calendering is a necessary process used in industry to improve the volumetric capacity of lithium-ion batteries. However, calendering high-nickel cathodes leads to electrode particle pulverization, raising concerns of a reduced cycle life due to parasitic side reactions. We present here an investigation of the impact of calendering on the morphology and electrochemical performance of the cobalt-free layered oxide cathode LiNi_0.9Mn_0.05Al_0.05O₂ (NMA-90). We find that secondary particle pulverization and fusion simultaneously occur at sufficiently high pressures. The initial surface area of the cathode is shown to increase with the degree of calendering, despite the higher likelihood of secondary particle fusion. Long-term cycling of full coin cells assembled with the NMA-90 cathode and the graphite anode indicates that cells with higher degrees of cathode calendering exhibit lower capacity fade compared to uncalendered cathodes. Hybrid pulse-power tests demonstrate that the usable capacity range of cells with calendered cathodes far exceeds those with uncalendered cells after long-term cycling. The improved capacity retention and pulse-power performance are attributed to the enhanced mechanical properties of the electrode after calendering that prevents loss of the primary particle contact during long-term cycling. As a result, we find that calendering high-nickel NMA-90 to industrially relevant densities does not have a detrimental effect on capacity fade, marking an important step toward commercial adoption.

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Research Organization:: Univ. of Texas at Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: EE0008445

OSTI ID:: 1972444

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 36 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (44)

High‐Nickel NMA: A Cobalt‐Free Alternative to NMC and NCA Cathodes for Lithium‐Ion Batteries Li, Wangda; Lee, Steven; Manthiram, Arumugam Advanced Materials, Vol. 32, Issue 33 https://doi.org/10.1002/adma.202002718	journal	July 2020
X-Ray Tomography of Porous, Transition Metal Oxide Based Lithium Ion Battery Electrodes Ebner, Martin; Geldmacher, Felix; Marone, Federica Advanced Energy Materials, Vol. 3, Issue 7 https://doi.org/10.1002/aenm.201200932	journal	March 2013
Tortuosity Anisotropy in Lithium-Ion Battery Electrodes Ebner, Martin; Chung, Ding-Wen; García, R. Edwin Advanced Energy Materials, Vol. 4, Issue 5 https://doi.org/10.1002/aenm.201301278	journal	October 2013
Numerical simulation of porous networks in relation to battery electrodes and separators Patel, Kamalnayan Kantilal; Paulsen, Jens M.; Desilvestro, Johann Journal of Power Sources, Vol. 122, Issue 2 https://doi.org/10.1016/S0378-7753(03)00399-9	journal	July 2003
A comparison of high voltage outgassing of LiCoO2, LiNiO2, and Li2MnO3 layered Li-ion cathode materials Papp, Joseph K.; Li, Ning; Kaufman, Lori A. Electrochimica Acta, Vol. 368 https://doi.org/10.1016/j.electacta.2020.137505	journal	February 2021
Lithium-Ion Battery Supply Chain Considerations: Analysis of Potential Bottlenecks in Critical Metals Olivetti, Elsa A.; Ceder, Gerbrand; Gaustad, Gabrielle G. Joule, Vol. 1, Issue 2 https://doi.org/10.1016/j.joule.2017.08.019	journal	October 2017
Understanding Full-Cell Evolution and Non-chemical Electrode Crosstalk of Li-Ion Batteries Knehr, Kevin W.; Hodson, Thomas; Bommier, Clement Joule, Vol. 2, Issue 6 https://doi.org/10.1016/j.joule.2018.03.016	journal	June 2018
Zn-Sn Interdigitated Eutectic Alloy Anodes with High Volumetric Capacity for Lithium-Ion Batteries Heligman, Brian Theodore; Kreder, Karl Joseph; Manthiram, Arumugam Joule, Vol. 3, Issue 4 https://doi.org/10.1016/j.joule.2019.01.005	journal	April 2019
Microstructural Evolution of Battery Electrodes During Calendering Lu, Xuekun; Daemi, Sohrab R.; Bertei, Antonio Joule, Vol. 4, Issue 12 https://doi.org/10.1016/j.joule.2020.10.010	journal	December 2020
Measurement of three-dimensional microstructure in a LiCoO2 positive electrode Wilson, James R.; Cronin, J. Scott; Barnett, Scott A. Journal of Power Sources, Vol. 196, Issue 7 https://doi.org/10.1016/j.jpowsour.2010.04.066	journal	April 2011
Calendering effects on the physical and electrochemical properties of Li[Ni1/3Mn1/3Co1/3]O2 cathode Zheng, Honghe; Tan, Li; Liu, Gao Journal of Power Sources, Vol. 208 https://doi.org/10.1016/j.jpowsour.2012.02.001	journal	June 2012
Understanding the calendering processability of Li(Ni0.33Mn0.33Co0.33)O2-based cathodes Primo, Emiliano N.; Chouchane, Mehdi; Touzin, Matthieu Journal of Power Sources, Vol. 488 https://doi.org/10.1016/j.jpowsour.2020.229361	journal	March 2021
Capacity Fading of Ni-Rich Li[Ni _x Co _y Mn _{1– x – y} ]O ₂ (0.6 ≤ x ≤ 0.95) Cathodes for High-Energy-Density Lithium-Ion Batteries: Bulk or Surface Degradation? Ryu, Hoon-Hee; Park, Kang-Joon; Yoon, Chong S. Chemistry of Materials, Vol. 30, Issue 3 https://doi.org/10.1021/acs.chemmater.7b05269	journal	January 2018
An Unavoidable Challenge for Ni-Rich Positive Electrode Materials for Lithium-Ion Batteries Li, Hongyang; Liu, Aaron; Zhang, Ning Chemistry of Materials, Vol. 31, Issue 18 https://doi.org/10.1021/acs.chemmater.9b02372	journal	August 2019
Anisotropic Lattice Strain and Mechanical Degradation of High- and Low-Nickel NCM Cathode Materials for Li-Ion Batteries Kondrakov, Aleksandr O.; Schmidt, Alexander; Xu, Jin The Journal of Physical Chemistry C, Vol. 121, Issue 6 https://doi.org/10.1021/acs.jpcc.6b12885	journal	February 2017
Operando Monitoring of Early Ni-mediated Surface Reconstruction in Layered Lithiated Ni–Co–Mn Oxides Streich, Daniel; Erk, Christoph; Guéguen, Aurelie The Journal of Physical Chemistry C, Vol. 121, Issue 25 https://doi.org/10.1021/acs.jpcc.7b02303	journal	June 2017
Quantification of Surface Oxygen Depletion and Solid Carbonate Evolution on the First Cycle of LiNi _0.6 Mn _0.2 Co _0.2 O ₂ Electrodes Renfrew, Sara E.; McCloskey, Bryan D. ACS Applied Energy Materials, Vol. 2, Issue 5 https://doi.org/10.1021/acsaem.9b00459	journal	April 2019
Synthesis of LiNiO ₂ at Moderate Oxygen Pressure and Long-Term Cyclability in Lithium-Ion Full Cells Mesnier, Alex; Manthiram, Arumugam ACS Applied Materials & Interfaces, Vol. 12, Issue 47 https://doi.org/10.1021/acsami.0c16648	journal	November 2020
Role of Manganese Deposition on Graphite in the Capacity Fading of Lithium Ion Batteries Vissers, Daniel R.; Chen, Zonghai; Shao, Yuyan ACS Applied Materials & Interfaces, Vol. 8, Issue 22 https://doi.org/10.1021/acsami.6b02061	journal	May 2016
Soft Chemistry Synthesis and Characterization of Layered Li_1-_xNi_1-_yCo_yO_2-_δ (0 ≤ x ≤ 1 and 0 ≤ y ≤ 1) Chebiam, R. V.; Prado, F.; Manthiram, A. Chemistry of Materials, Vol. 13, Issue 9, p. 2951-2957 https://doi.org/10.1021/cm0102537	journal	September 2001
Electrochemical methods, fundamentals and applications Aikens, D. A. Journal of Chemical Education, Vol. 60, Issue 1 https://doi.org/10.1021/ed060pA25.1	journal	January 1983
Collapse of LiNi _{1– x – y} Co _x Mn _y O ₂ Lattice at Deep Charge Irrespective of Nickel Content in Lithium-Ion Batteries Li, Wangda; Asl, Hooman Yaghoobnejad; Xie, Qiang Journal of the American Chemical Society, Vol. 141, Issue 13 https://doi.org/10.1021/jacs.8b13798	journal	March 2019
Manganese in Graphite Anode and Capacity Fade in Li Ion Batteries Shkrob, Ilya A.; Kropf, A. Jeremy; Marin, Timothy W. The Journal of Physical Chemistry C, Vol. 118, Issue 42 https://doi.org/10.1021/jp507833u	journal	October 2014
Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries Li, Wangda; Dolocan, Andrei; Oh, Pilgun Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14589	journal	April 2017
A reflection on lithium-ion battery cathode chemistry Manthiram, Arumugam Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15355-0	journal	March 2020
Performance and cost of materials for lithium-based rechargeable automotive batteries Schmuch, Richard; Wagner, Ralf; Hörpel, Gerhard Nature Energy, Vol. 3, Issue 4 https://doi.org/10.1038/s41560-018-0107-2	journal	April 2018
Post-lithium-ion battery cell production and its compatibility with lithium-ion cell production infrastructure Duffner, Fabian; Kronemeyer, Niklas; Tübke, Jens Nature Energy, Vol. 6, Issue 2 https://doi.org/10.1038/s41560-020-00748-8	journal	January 2021
High-voltage positive electrode materials for lithium-ion batteries Li, Wangda; Song, Bohang; Manthiram, Arumugam Chemical Society Reviews, Vol. 46, Issue 10 https://doi.org/10.1039/c6cs00875e	journal	January 2017
Intrinsic origin of intra-granular cracking in Ni-rich layered oxide cathode materials Min, Kyoungmin; Cho, Eunseog Physical Chemistry Chemical Physics, Vol. 20, Issue 14 https://doi.org/10.1039/c7cp06615e	journal	January 2018
4D visualisation of in situ nano-compression of Li-ion cathode materials to mimic early stage calendering Daemi, S. R.; Lu, X.; Sykes, D. Materials Horizons, Vol. 6, Issue 3 https://doi.org/10.1039/c8mh01533c	journal	January 2019
Towards more environmentally and socially responsible batteries Sharma, Shyam S.; Manthiram, Arumugam Energy & Environmental Science, Vol. 13, Issue 11 https://doi.org/10.1039/d0ee02511a	journal	January 2020
Lithium Diffusion in Layered Li[sub x]CoO[sub 2] Van der Ven, A. Electrochemical and Solid-State Letters, Vol. 3, Issue 7 https://doi.org/10.1149/1.1391130	journal	January 1999
Particle Compression and Conductivity in Li-Ion Anodes with Graphite Additives Wang, C. -W.; Yi, Y. -B.; Sastry, A. M. Journal of The Electrochemical Society, Vol. 151, Issue 9 https://doi.org/10.1149/1.1783909	journal	January 2004
Modeling 3D Microstructure and Ion Transport in Porous Li-Ion Battery Electrodes Stephenson, David E.; Walker, Bryce C.; Skelton, Cole B. Journal of The Electrochemical Society, Vol. 158, Issue 7 https://doi.org/10.1149/1.3579996	journal	January 2011
Novel Method for Monitoring the Electrochemical Capacitance by In Situ Impedance Spectroscopy as Indicator for Particle Cracking of Nickel-Rich NCMs: Part I. Theory and Validation Oswald, Stefan; Pritzl, Daniel; Wetjen, Morten Journal of The Electrochemical Society, Vol. 167, Issue 10 https://doi.org/10.1149/1945-7111/ab9187	journal	June 2020
Oxygen Release and Its Effect on the Cycling Stability of LiNi _x Mn _y Co _z O ₂ (NMC) Cathode Materials for Li-Ion Batteries Jung, Roland; Metzger, Michael; Maglia, Filippo Journal of The Electrochemical Society, Vol. 164, Issue 7 https://doi.org/10.1149/2.0021707jes	journal	January 2017
An Analysis Protocol for Three-Electrode Li-Ion Battery Impedance Spectra: Part I. Analysis of a High-Voltage Positive Electrode Landesfeind, Johannes; Pritzl, Daniel; Gasteiger, Hubert A. Journal of The Electrochemical Society, Vol. 164, Issue 7 https://doi.org/10.1149/2.0131709jes	journal	January 2017
Review—Recent Advances and Remaining Challenges for Lithium Ion Battery Cathodes: I. Nickel-Rich, LiNi Schipper, Florian; Erickson, Evan M.; Erk, Christoph Journal of The Electrochemical Society, Vol. 164, Issue 1 https://doi.org/10.1149/2.0351701jes	journal	December 2016
Identifying Contact Resistances in High-Voltage Cathodes by Impedance Spectroscopy Pritzl, Daniel; Bumberger, Andreas E.; Wetjen, Morten Journal of The Electrochemical Society, Vol. 166, Issue 4 https://doi.org/10.1149/2.0451904jes	journal	January 2019
The Role of Oxygen Release from Li- and Mn-Rich Layered Oxides during the First Cycles Investigated by On-Line Electrochemical Mass Spectrometry Strehle, Benjamin; Kleiner, Karin; Jung, Roland Journal of The Electrochemical Society, Vol. 164, Issue 2 https://doi.org/10.1149/2.1001702jes	journal	December 2016
Tortuosity Determination of Battery Electrodes and Separators by Impedance Spectroscopy Landesfeind, Johannes; Hattendorff, Johannes; Ehrl, Andreas Journal of The Electrochemical Society, Vol. 163, Issue 7 https://doi.org/10.1149/2.1141607jes	journal	January 2016
Simulation-Supported Analysis of Calendering Impacts on the Performance of Lithium-Ion-Batteries Lenze, Georg; Röder, Fridolin; Bockholt, Henrike Journal of The Electrochemical Society, Vol. 164, Issue 6 https://doi.org/10.1149/2.1141706jes	journal	January 2017
Analyses of the Calendaring Process for Performance Optimization of Li-Ion Battery Cathode Oladimeji, Charles F.; Moss, Pedro L.; Weatherspoon, Mark H. Advances in Chemistry, Vol. 2016 https://doi.org/10.1155/2016/7395060	journal	August 2016
U.S. Department of Energy Vehicle Technologies Program: Battery Test Manual For Plug-In Hybrid Electric Vehicles Christophersen, Jon P. https://doi.org/10.2172/1169249	report	September 2014

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Title: Influence of Calendering on the Electrochemical Performance of LiNi0.9Mn0.05Al0.05O2 Cathodes in Lithium-Ion Cells

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Title: Influence of Calendering on the Electrochemical Performance of LiNi_0.9Mn_0.05Al_0.05O₂ Cathodes in Lithium-Ion Cells