Predicting Morphological Evolution during Coprecipitation of MnCO3 Battery Cathode Precursors Using Multiscale Simulations Aided by Targeted Synthesis

Garcia, Juan C.; Barai, Pallab; Chen, Jiajun; Gutierrez, Arturo; Wen, Jianguo; Arslan, Ilke; Wang, Xiaoping; Fister, Timothy T.; Iddir, Hakim; Srinivasan, Venkat

doi:10.1021/acs.chemmater.0c01929

Predicting Morphological Evolution during Coprecipitation of MnCO₃ Battery Cathode Precursors Using Multiscale Simulations Aided by Targeted Synthesis

Journal Article · Fri Oct 23 00:00:00 EDT 2020 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.0c01929· OSTI ID:1826064

^[1]; ^[1]; Chen, Jiajun ^[1]; ^[1]; ^[1]; Arslan, Ilke ^[1]; Wang, Xiaoping ^[1]; ^[1]; ^[1]; ^[1]

Argonne National Laboratory. (ANL), Lemont, IL (United States)

The performance of lithium-ion batteries is intimately linked to both the structure and the morphology of the cathode material, which in turn is critically linked to the synthesis conditions. However, few studies focus on understanding synthesis, especially during the coprecipitation of metal oxide precursors, a process that largely determines the final morphology of the material. In this paper, we go beyond the typical equilibrium particle shape analysis conducted in the literature and incorporate kinetic aspects of morphology evolution. We perform these studies using controlled synthesis on a well-defined metal salt system (MnCO₃) combined with multiscale simulations and high-resolution microscopy. Results show that with increasing metal concentration, the particles transition from rhombohedral to cubic to spherical shapes. Computational analysis using density functional theory (DFT) reveals that rhombohedral shaped particles evolve under equilibrium conditions. Phase field techniques indicate that at higher metal concentrations, fast growth kinetics of the precipitates result in the transition to cubic and, subsequently, spherical shapes, accompanied by a decrease in particle size. This study, while limited to the one metal salt system, provides an approach to shed light on the synthesis process of mixed transition metal salts, gradient materials, and other cathode materials of interest to the battery community.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1826064

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 21 Vol. 32; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (57)

Agglomerate breakage and adhesion upon impact with complex‐shaped particles Tamadondar, Mohammad R.; Martín, Lilian; Rasmuson, Anders AIChE Journal, Vol. 65, Issue 6 https://doi.org/10.1002/aic.16581	journal	March 2019
Review: Nucleation in solutions revisited Kashchiev, D.; van Rosmalen, G. M. Crystal Research and Technology, Vol. 38, Issue 78 https://doi.org/10.1002/crat.200310070	journal	July 2003
Crystal shapes and phase equilibria: A common mathematical basis Cahn, J. W.; Carter, W. C. Metallurgical and Materials Transactions A, Vol. 27, Issue 6 https://doi.org/10.1007/BF02649804	journal	June 1996
Building Safe Lithium-Ion Batteries for Electric Vehicles: A Review Duan, Jian; Tang, Xuan; Dai, Haifeng Electrochemical Energy Reviews, Vol. 3, Issue 1 https://doi.org/10.1007/s41918-019-00060-4	journal	December 2019
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Particle nucleation and growth models Leubner, Ingo H. Current Opinion in Colloid & Interface Science, Vol. 5, Issue 1-2 https://doi.org/10.1016/S1359-0294(00)00048-0	journal	March 2000
Phase-field modeling of twin-related faceted dendrite growth of silicon Chen, G. Y.; Lin, H. K.; Lan, C. W. Acta Materialia, Vol. 115 https://doi.org/10.1016/j.actamat.2016.06.008	journal	August 2016
2D Phase field modeling of sintering of silver nanoparticles Chockalingam, K.; Kouznetsova, V. G.; van der Sluis, O. Computer Methods in Applied Mechanics and Engineering, Vol. 312 https://doi.org/10.1016/j.cma.2016.07.002	journal	December 2016
In-situ analysis of nucleation and growth of transition metal oxalate battery precursor particles via time evolution of solution composition and particle size distribution Dong, Hongxu; Wang, Anny; Smart, Guillermo Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 558 https://doi.org/10.1016/j.colsurfa.2018.08.047	journal	December 2018
A Review of Lithium-Ion Battery for Electric Vehicle Applications and Beyond Chen, Weidong; Liang, Jun; Yang, Zhaohua Energy Procedia, Vol. 158 https://doi.org/10.1016/j.egypro.2019.01.783	journal	February 2019
Co–precipitation synthesis of Ni0.6Co0.2Mn0.2(OH)2 precursor and characterization of LiNi0.6Co0.2Mn0.2O2 cathode material for secondary lithium batteries Liang, Longwei; Du, Ke; Peng, Zhongdong Electrochimica Acta, Vol. 130 https://doi.org/10.1016/j.electacta.2014.02.100	journal	June 2014
An improved carbonate co-precipitation method for the preparation of spherical Li[Ni1/3Co1/3Mn1/3]O2 cathode material Zhang, S.; Deng, C.; Yang, S. Y. Journal of Alloys and Compounds, Vol. 484, Issue 1-2 https://doi.org/10.1016/j.jallcom.2009.04.149	journal	September 2009
Physical and electrochemical properties of spherical Li1+x(Ni1/3Co1/3Mn1/3)1−xO2 cathode materials Park, S. -H.; Kang, S. -H.; Belharouak, I. Journal of Power Sources, Vol. 177, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.10.062	journal	February 2008
Synthesis of high capacity cathodes for lithium-ion batteries by morphology-tailored hydroxide co-precipitation Wang, Dapeng; Belharouak, Ilias; Ortega, Luis H. Journal of Power Sources, Vol. 274 https://doi.org/10.1016/j.jpowsour.2014.10.016	journal	January 2015
Li-ion battery materials: present and future Nitta, Naoki; Wu, Feixiang; Lee, Jung Tae Materials Today, Vol. 18, Issue 5 https://doi.org/10.1016/j.mattod.2014.10.040	journal	June 2015
Tuning solution chemistry for morphology control of lithium-ion battery precursor particles Robinson, J. Pierce; Koenig, Gary M. Powder Technology, Vol. 284 https://doi.org/10.1016/j.powtec.2015.06.070	journal	November 2015
Role of coprecipitation and calcination of precursors on phase homogeneity and electrochemical properties of battery active materials Dong, Hongxu; Wang, Anny; Koenig, Gary M. Powder Technology, Vol. 335 https://doi.org/10.1016/j.powtec.2018.05.020	journal	July 2018
A Review of Classical and Nonclassical Nucleation Theories Karthika, S.; Radhakrishnan, T. K.; Kalaichelvi, P. Crystal Growth & Design, Vol. 16, Issue 11 https://doi.org/10.1021/acs.cgd.6b00794	journal	October 2016
Solubility and Growth Kinetics of Ammonium Bicarbonate in Aqueous Solution Sutter, Daniel; Mazzotti, Marco Crystal Growth & Design, Vol. 17, Issue 6 https://doi.org/10.1021/acs.cgd.6b01751	journal	May 2017
Particle Breakage: Limiting Conditions for Crystal–Crystallizer Collisions Tyrrell, Rory; De Souza, Brian; Frawley, Patrick J. Crystal Growth & Design, Vol. 18, Issue 2 https://doi.org/10.1021/acs.cgd.7b00125	journal	January 2018
Synthesis of Li-Rich NMC: A Comprehensive Study Pimenta, Vanessa; Sathiya, Mariyappan; Batuk, Dmitry Chemistry of Materials, Vol. 29, Issue 23 https://doi.org/10.1021/acs.chemmater.7b03230	journal	November 2017
Multiscale Computational Model for Particle Size Evolution during Coprecipitation of Li-Ion Battery Cathode Precursors Barai, Pallab; Feng, Zhange; Kondo, Hiroki The Journal of Physical Chemistry B, Vol. 123, Issue 15 https://doi.org/10.1021/acs.jpcb.8b12004	journal	March 2019
Understanding Particle-Size-Dependent Electrochemical Properties of Li ₂ MnO ₃ -Based Positive Electrode Materials for Rechargeable Lithium Batteries Yabuuchi, Naoaki; Kubota, Kei; Aoki, Yoshinori The Journal of Physical Chemistry C, Vol. 120, Issue 2 https://doi.org/10.1021/acs.jpcc.5b10517	journal	January 2016
Surface Structure, Morphology, and Stability of Li(Ni _1/3 Mn _1/3 Co _1/3 )O ₂ Cathode Material Garcia, Juan C.; Bareño, Javier; Yan, Jianhua The Journal of Physical Chemistry C, Vol. 121, Issue 15 https://doi.org/10.1021/acs.jpcc.7b00896	journal	April 2017
Pb ²⁺ –Calcite Interactions under Far-from-Equilibrium Conditions: Formation of Micropyramids and Pseudomorphic Growth of Cerussite Yuan, Ke; De Andrade, Vincent; Feng, Zhange The Journal of Physical Chemistry C, Vol. 122, Issue 4 https://doi.org/10.1021/acs.jpcc.7b11682	journal	January 2018
Modeling Nucleation, Growth, and Ostwald Ripening in Crystallization Processes: A Comparison between Population Balance and Kinetic Rate Equation Vetter, Thomas; Iggland, Martin; Ochsenbein, David R. Crystal Growth & Design, Vol. 13, Issue 11 https://doi.org/10.1021/cg4010714	journal	October 2013
Synthesis of Nanostructured Li[Ni _1/3 Co _1/3 Mn _1/3 ]O ₂ via a Modified Carbonate Process Park, S. -H.; Shin, H. -S.; Myung, S. -T. Chemistry of Materials, Vol. 17, Issue 1 https://doi.org/10.1021/cm048433e	journal	January 2005
Composition-Tailored Synthesis of Gradient Transition Metal Precursor Particles for Lithium-Ion Battery Cathode Materials Koenig, Gary M.; Belharouak, Ilias; Deng, Haixai Chemistry of Materials, Vol. 23, Issue 7 https://doi.org/10.1021/cm200058c	journal	April 2011
First-Principles Analysis of Phase Stability in Layered–Layered Composite Cathodes for Lithium-Ion Batteries Iddir, Hakim; Benedek, Roy Chemistry of Materials, Vol. 26, Issue 7 https://doi.org/10.1021/cm403256a	journal	March 2014
Analysis of the Growth Mechanism of Coprecipitated Spherical and Dense Nickel, Manganese, and Cobalt-Containing Hydroxides in the Presence of Aqueous Ammonia van Bommel, Andrew; Dahn, J. R. Chemistry of Materials, Vol. 21, Issue 8 https://doi.org/10.1021/cm803144d	journal	April 2009
Coprecipitation Synthesis of Ni _x Mn _1−x (OH) ₂ Mixed Hydroxides Zhou, Fu; Zhao, Xuemei; van Bommel, Andrew Chemistry of Materials, Vol. 22, Issue 3 https://doi.org/10.1021/cm9018309	journal	November 2009
Metal Flux and Dynamic Speciation at (Bio)interfaces. Part I: Critical Evaluation and Compilation of Physicochemical Parameters for Complexes with Simple Ligands and Fulvic/Humic Substances Buffle, Jacques; Zhang, Zeshi; Startchev, Konstantin Environmental Science & Technology, Vol. 41, Issue 22 https://doi.org/10.1021/es070702p	journal	November 2007
Breakage Rate of Colloidal Aggregates in Shear Flow through Stokesian Dynamics Harshe, Yogesh M.; Lattuada, Marco Langmuir, Vol. 28, Issue 1 https://doi.org/10.1021/la2038476	journal	December 2011
Flow-Induced Aggregation and Breakup of Particle Clusters Controlled by Surface Nanoroughness Moussa, Amgad S.; Lattuada, Marco; Conchúir, Breanndán Ó. Langmuir, Vol. 29, Issue 47 https://doi.org/10.1021/la403240k	journal	November 2013
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
Single-crystal based studies for correlating the properties and high-voltage performance of Li[Ni _x Mn _y Co _1−x−y ]O ₂ cathodes Zhu, Jian; Chen, Guoying Journal of Materials Chemistry A, Vol. 7, Issue 10 https://doi.org/10.1039/C8TA10329A	journal	January 2019
A review on synthesis and engineering of crystal precursors produced via coprecipitation for multicomponent lithium-ion battery cathode materials Dong, Hongxu; Koenig, Gary M. CrystEngComm, Vol. 22, Issue 9 https://doi.org/10.1039/C9CE00679F	journal	January 2020
Growth mechanism of Ni0.3Mn0.7CO3 precursor for high capacity Li-ion battery cathodes Wang, Dapeng; Belharouak, Ilias; Koenig, Gary M. Journal of Materials Chemistry, Vol. 21, Issue 25 https://doi.org/10.1039/c1jm11077b	journal	January 2011
Porous LiMn2O4 cubes architectured with single-crystalline nanoparticles and exhibiting excellent cyclic stability and rate capability as the cathode of a lithium ion battery Lin, H. B.; Hu, J. N.; Rong, H. B. Journal of Materials Chemistry A, Vol. 2, Issue 24 https://doi.org/10.1039/c4ta01474j	journal	January 2014
Phase-field modeling of solute precipitation and dissolution Xu, Zhijie; Meakin, Paul The Journal of Chemical Physics, Vol. 129, Issue 1 https://doi.org/10.1063/1.2948949	journal	July 2008
Phase-field modeling of two-dimensional solute precipitation/dissolution: Solid fingers and diffusion-limited precipitation Xu, Zhijie; Meakin, Paul The Journal of Chemical Physics, Vol. 134, Issue 4 https://doi.org/10.1063/1.3537973	journal	January 2011
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Phase-field method for computationally efficient modeling of solidification with arbitrary interface kinetics Karma, Alain; Rappel, Wouter-Jan Physical Review E, Vol. 53, Issue 4 https://doi.org/10.1103/PhysRevE.53.R3017	journal	April 1996
Quantitative phase-field modeling of dendritic growth in two and three dimensions Karma, Alain; Rappel, Wouter-Jan Physical Review E, Vol. 57, Issue 4 https://doi.org/10.1103/PhysRevE.57.4323	journal	April 1998
Unveiling the Formation Mechanism of Pseudo-Single-Crystal Aragonite Platelets in Nacre Li, Xiaodong; Huang, Zaiwang Physical Review Letters, Vol. 102, Issue 7 https://doi.org/10.1103/PhysRevLett.102.075502	journal	February 2009
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Crystallization by particle attachment in synthetic, biogenic, and geologic environments De Yoreo, J. J.; Gilbert, P. U. P. A.; Sommerdijk, N. A. J. M. Science, Vol. 349, Issue 6247 https://doi.org/10.1126/science.aaa6760	journal	July 2015
Phase-Field Models for Microstructure Evolution Chen, Long-Qing Annual Review of Materials Research, Vol. 32, Issue 1 https://doi.org/10.1146/annurev.matsci.32.112001.132041	journal	August 2002
Optimized Synthetic Conditions of LiNi _0.5 Co _0.2 Mn _0.3 O ₂ Cathode Materials for High Rate Lithium Batteries via Co-Precipitation Method Noh, Mijung; Cho, Jaephil Journal of The Electrochemical Society, Vol. 160, Issue 1 https://doi.org/10.1149/2.004302jes	journal	November 2012
The Development and Future of Lithium Ion Batteries Blomgren, George E. Journal of The Electrochemical Society, Vol. 164, Issue 1 https://doi.org/10.1149/2.0251701jes	journal	December 2016
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
Review—Recent Advances and Remaining Challenges for Lithium Ion Battery Cathodes: II. Lithium-Rich, xLi Erickson, Evan M.; Schipper, Florian; Penki, Tirupathi Rao Journal of The Electrochemical Society, Vol. 164, Issue 1 https://doi.org/10.1149/2.0461701jes	journal	January 2017
In Situ Monitoring of the Growth of Nickel, Manganese, and Cobalt Hydroxide Precursors during Co-Precipitation Synthesis of Li-Ion Cathode Materials Feng, Zhange; Barai, Pallab; Gim, Jihyeon Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0511813jes	journal	January 2018
Computational modeling of calcite cementation in saline limestone aquifers: a phase-field study Prajapati, Nishant; Selzer, Michael; Nestler, Britta Geothermal Energy, Vol. 5, Issue 1 https://doi.org/10.1186/s40517-017-0072-1	journal	August 2017
Concepts of modeling surface energy anisotropy in phase-field approaches Tschukin, Oleg; Silberzahn, Alexander; Selzer, Michael Geothermal Energy, Vol. 5, Issue 1 https://doi.org/10.1186/s40517-017-0077-9	journal	October 2017
Modeling fracture cementation processes in calcite limestone: a phase-field study Prajapati, Nishant; Selzer, Michael; Nestler, Britta Geothermal Energy, Vol. 6, Issue 1 https://doi.org/10.1186/s40517-018-0093-4	journal	June 2018

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