Generating multi-scale Li-ion battery cathode particles with radial grain architectures using stereological generative adversarial networks

Fuchs, Lukas; Furat, Orkun; Finegan, Donal P.; Allen, Jeffery; Usseglio-Viretta, Francois L. E.; Ozdogru, Bertan; Weddle, Peter J.; Smith, Kandler; Schmidt, Volker

doi:10.1038/s43246-024-00728-5

Title: Generating multi-scale Li-ion battery cathode particles with radial grain architectures using stereological generative adversarial networks

Journal Article · 07 January 2025 · Communications Materials

DOI: https://doi.org/10.1038/s43246-024-00728-5 · OSTI ID:2497350

;

; Allen, Jeffery;

; Ozdogru, Bertan; Weddle, Peter J.;

; Schmidt, Volker

Abstract Understanding structure-property relationships of Li-ion battery cathodes is crucial for optimizing rate-performance and cycle-life resilience. However, correlating the morphology of cathode particles, such as in LiNi0.8Mn0.1Co0.1O2 (NMC811), and their inner grain architecture with electrode performance is challenging, particularly, due to the significant length-scale difference between grain and particle sizes. Experimentally, it is not feasible to image such a high number of particles with full granular detail. A second challenge is that sufficiently high-resolution 3D imaging techniques remain expensive and are sparsely available at research institutions. Here, we present a stereological generative adversarial network-based model fitting approach to tackle this, that generates representative 3D information from 2D data, enabling characterization of materials in 3D using cost-effective 2D data. Once calibrated, this multi-scale model can rapidly generate virtual cathode particles that are statistically similar to experimental data, and thus is suitable for virtual characterization and materials testing through numerical simulations. A large dataset of simulated particles with inner grain architecture has been made publicly available.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

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

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 2497350

Report Number(s):: NREL/JA--5700-91478; 4; PII: 728

Journal Information:: Communications Materials, Journal Name: Communications Materials Journal Issue: 1 Vol. 6; ISSN 2662-4443

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (66)

Stochastic Geometry and its Applications Chiu, Sung Nok; Stoyan, Dietrich; Kendall, Wilfrid S. Wiley Series in Probability and Statistics https://doi.org/10.1002/9781118658222	book	August 2013
High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material Mao, Yuwei; Wang, Xuelong; Xia, Sihao Advanced Functional Materials, Vol. 29, Issue 18 https://doi.org/10.1002/adfm.201900247	journal	March 2019
Radially Oriented Single‐Crystal Primary Nanosheets Enable Ultrahigh Rate and Cycling Properties of LiNi _0.8 Co _0.1 Mn _0.1 O ₂ Cathode Material for Lithium‐Ion Batteries Xu, Xing; Huo, Hua; Jian, Jiyuan Advanced Energy Materials, Vol. 9, Issue 15 https://doi.org/10.1002/aenm.201803963	journal	February 2019
A Comprehensive Understanding of the Aging Effects of Extreme Fast Charging on High Ni NMC Cathode Tanim, Tanvir R.; Yang, Zhenzhen; Finegan, Donal P. Advanced Energy Materials, Vol. 12, Issue 22 https://doi.org/10.1002/aenm.202103712	journal	April 2022
Enabling Extreme Fast‐Charging: Challenges at the Cathode and Mitigation Strategies Tanim, Tanvir R.; Weddle, Peter J.; Yang, Zhenzhen Advanced Energy Materials, Vol. 12, Issue 46 https://doi.org/10.1002/aenm.202202795	journal	November 2022
Li-ion batteries: basics, progress, and challenges Deng, Da Energy Science & Engineering, Vol. 3, Issue 5 https://doi.org/10.1002/ese3.95	journal	September 2015
Spherical Harmonics and Approximations on the Unit Sphere: An Introduction Atkinson, Kendall; Han, Weimin https://doi.org/10.1007/978-3-642-25983-8	book	January 2012
A stochastic multiscale algorithm for modeling complex granular materials Tahmasebi, Pejman; Sahimi, Muhammad Granular Matter, Vol. 20, Issue 3 https://doi.org/10.1007/s10035-018-0816-z	journal	June 2018
Disintegration of Meatball Electrodes for LiNi x Mn y Co z O2 Cathode Materials Xu, R.; de Vasconcelos, L. S.; Shi, J. Experimental Mechanics, Vol. 58, Issue 4 https://doi.org/10.1007/s11340-017-0292-0	journal	May 2017
Anisotropic power diagrams for polycrystal modelling: Efficient generation of curved grains via optimal transport Buze, M.; Feydy, J.; Roper, S. M. Computational Materials Science, Vol. 245 https://doi.org/10.1016/j.commatsci.2024.113317	journal	October 2024
Three-dimensional particle-resolved models of Li-ion batteries to assist the evaluation of empirical parameters in one-dimensional models Goldin, Graham M.; Colclasure, Andrew M.; Wiedemann, Andreas H. Electrochimica Acta, Vol. 64 https://doi.org/10.1016/j.electacta.2011.12.119	journal	March 2012
A Computational Model of the Mechanical Behavior within Reconstructed LixCoO2 Li-ion Battery Cathode Particles Malavé, Veruska; Berger, J. R.; Zhu, Huayang Electrochimica Acta, Vol. 130 https://doi.org/10.1016/j.electacta.2014.03.113	journal	June 2014
Electro-chemo-mechanical finite-element model of single-crystal and polycrystalline NMC cathode particles embedded in an argyrodite solid electrolyte Taghikhani, Kasra; Weddle, Peter J.; Hoffman, Robert M. Electrochimica Acta, Vol. 460 https://doi.org/10.1016/j.electacta.2023.142585	journal	August 2023
On the fragmentation of active material secondary particles in lithium ion battery cathodes induced by charge cycling Sun, Guanhua; Sui, Tan; Song, Bohang Extreme Mechanics Letters, Vol. 9 https://doi.org/10.1016/j.eml.2016.03.018	journal	December 2016
Extended cycle life implications of fast charging for lithium-ion battery cathode Tanim, Tanvir R.; Yang, Zhenzhen; Colclasure, Andrew M. Energy Storage Materials, Vol. 41 https://doi.org/10.1016/j.ensm.2021.07.001	journal	October 2021
Effective and practical parameters of electrochemical Li-ion battery models for degradation diagnosis Kim, Jungsoo; Chun, Huiyong; Kim, Minho Journal of Energy Storage, Vol. 42 https://doi.org/10.1016/j.est.2021.103077	journal	October 2021
The diffusion induced stress and cracking behaviour of primary particle for Li-ion battery electrode Zhu, Xuanchen; Chen, Ying; Chen, Haofeng International Journal of Mechanical Sciences, Vol. 178 https://doi.org/10.1016/j.ijmecsci.2020.105608	journal	July 2020
Quantifying the influence of microstructure on effective conductivity and permeability: Virtual materials testing Neumann, Matthias; Stenzel, Ole; Willot, François International Journal of Solids and Structures, Vol. 184 https://doi.org/10.1016/j.ijsolstr.2019.03.028	journal	February 2020
Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling Xu, Rong; Yang, Yang; Yin, Fei Journal of the Mechanics and Physics of Solids, Vol. 129 https://doi.org/10.1016/j.jmps.2019.05.003	journal	August 2019
Chemo-mechanical modeling of inter- and intra-granular fracture in heterogeneous cathode with polycrystalline particles for lithium-ion battery Singh, Avtar; Pal, Siladitya Journal of the Mechanics and Physics of Solids, Vol. 163 https://doi.org/10.1016/j.jmps.2022.104839	journal	June 2022
Chemo-mechanical modeling of stress evolution in all-solid-state lithium-ion batteries using synchrotron transmission X-ray microscopy tomography Fathiannasab, Hamed; Zhu, Likun; Chen, Zhongwei Journal of Power Sources, Vol. 483 https://doi.org/10.1016/j.jpowsour.2020.229028	journal	January 2021
Quantifying the influence of charge rate and cathode-particle architectures on degradation of Li-ion cells through 3D continuum-level damage models Allen, Jeffery M.; Weddle, Peter J.; Verma, Ankit Journal of Power Sources, Vol. 512 https://doi.org/10.1016/j.jpowsour.2021.230415	journal	November 2021
Cracking predictions of lithium-ion battery electrodes by X-ray computed tomography and modelling Boyce, Adam M.; Martínez-Pañeda, Emilio; Wade, Aaron Journal of Power Sources, Vol. 526 https://doi.org/10.1016/j.jpowsour.2022.231119	journal	April 2022
Coupled electrochemical–mechanical model for fracture analysis in active materials of lithium ion batteries Pistorio, Francesca; Clerici, Davide; Mocera, Francesco Journal of Power Sources, Vol. 580 https://doi.org/10.1016/j.jpowsour.2023.233378	journal	October 2023
Cohesive phase-field chemo-mechanical simulations of inter- and trans- granular fractures in polycrystalline NMC cathodes via image-based 3D reconstruction Chen, Wan-Xin; Allen, Jeffery M.; Rezaei, Shahed Journal of Power Sources, Vol. 596 https://doi.org/10.1016/j.jpowsour.2024.234054	journal	March 2024
Structural characterization of particle systems using spherical harmonics Feinauer, Julian; Spettl, Aaron; Manke, Ingo Materials Characterization, Vol. 106 https://doi.org/10.1016/j.matchar.2015.05.023	journal	August 2015
Investigation of the relationship between morphology and permeability for open-cell foams using virtual materials testing Westhoff, Daniel; Skibinski, Jakub; Šedivý, Ondřej Materials & Design, Vol. 147 https://doi.org/10.1016/j.matdes.2018.03.022	journal	June 2018
Reconstruction, optimization, and design of heterogeneous materials and media: Basic principles, computational algorithms, and applications Sahimi, Muhammad; Tahmasebi, Pejman Physics Reports, Vol. 939 https://doi.org/10.1016/j.physrep.2021.09.003	journal	December 2021
3D quantitative shape analysis on form, roundness, and compactness with μCT Zhao, Budi; Wang, Jianfeng Powder Technology, Vol. 291 https://doi.org/10.1016/j.powtec.2015.12.029	journal	April 2016
A chemo-mechanical grain boundary model and its application to understand the damage of Li-ion battery materials Bai, Yang; Zhao, Kejie; Liu, Yao Scripta Materialia, Vol. 183 https://doi.org/10.1016/j.scriptamat.2020.03.027	journal	July 2020
Electron Backscatter Diffraction for Investigating Lithium-Ion Electrode Particle Architectures Quinn, Alexander; Moutinho, Helio; Usseglio-Viretta, Francois Cell Reports Physical Science, Vol. 1, Issue 8 https://doi.org/10.1016/j.xcrp.2020.100137	journal	August 2020
Lectures on the Poisson Process Last, Günter; Penrose, Mathew https://doi.org/10.1017/9781316104477	book	January 2017
Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials Mu, Linqin; Lin, Ruoqian; Xu, Rong Nano Letters, Vol. 18, Issue 5 https://doi.org/10.1021/acs.nanolett.8b01036	journal	April 2018
How Fast Can a Li-Ion Battery Be Charged? Determination of Limiting Fast Charging Conditions F. Rodrigues, Marco T.; Son, Seoung-Bum; Colclasure, Andrew M. ACS Applied Energy Materials, Vol. 4, Issue 2 https://doi.org/10.1021/acsaem.0c03114	journal	January 2021
Fast-Charging Aging Considerations: Incorporation and Alignment of Cell Design and Material Degradation Pathways Chinnam, Parameswara R.; Colclasure, Andrew M.; Chen, Bor-Rong ACS Applied Energy Materials, Vol. 4, Issue 9 https://doi.org/10.1021/acsaem.1c01398	journal	September 2021
Ultrahigh Rate Performance of a Robust Lithium Nickel Manganese Cobalt Oxide Cathode with Preferentially Orientated Li-Diffusing Channels Ren, Dong; Padgett, Elliot; Yang, Yao ACS Applied Materials & Interfaces, Vol. 11, Issue 44 https://doi.org/10.1021/acsami.9b05602	journal	October 2019
Voltage-Based Strategies for Preventing Battery Degradation under Diverse Fast-Charging Conditions Konz, Zachary M.; Weddle, Peter J.; Gasper, Paul ACS Energy Letters, Vol. 8, Issue 10 https://doi.org/10.1021/acsenergylett.3c01591	journal	September 2023
Artificial generation of representative single Li-ion electrode particle architectures from microscopy data Furat, Orkun; Petrich, Lukas; Finegan, Donal P. npj Computational Materials, Vol. 7, Issue 1 https://doi.org/10.1038/s41524-021-00567-9	journal	July 2021
Heuristic solution for achieving long-term cycle stability for Ni-rich layered cathodes at full depth of discharge Kim, Un-Hyuck; Park, Geon-Tae; Son, Byoung-Ki Nature Energy, Vol. 5, Issue 11 https://doi.org/10.1038/s41560-020-00693-6	journal	September 2020
Generating three-dimensional structures from a two-dimensional slice with generative adversarial network-based dimensionality expansion Kench, Steve; Cooper, Samuel J. Nature Machine Intelligence, Vol. 3, Issue 4 https://doi.org/10.1038/s42256-021-00322-1	journal	April 2021
Generalized balanced power diagrams for 3D representations of polycrystals Alpers, Andreas; Brieden, Andreas; Gritzmann, Peter Philosophical Magazine, Vol. 95, Issue 9, p. 1016-1028 https://doi.org/10.1080/14786435.2015.1015469	journal	February 2015
Using convolutional neural networks for stereological characterization of 3D hetero-aggregates based on synthetic STEM data Fuchs, Lukas; Kirstein, Tom; Mahr, Christoph Machine Learning: Science and Technology, Vol. 5, Issue 2 https://doi.org/10.1088/2632-2153/ad38fd	journal	April 2024
Principal component analysis: a review and recent developments Jolliffe, Ian T.; Cadima, Jorge Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 374, Issue 2065 https://doi.org/10.1098/rsta.2015.0202	journal	April 2016
Recent Progress on Generative Adversarial Networks (GANs): A Survey Pan, Zhaoqing; Yu, Weijie; Yi, Xiaokai IEEE Access, Vol. 7 https://doi.org/10.1109/ACCESS.2019.2905015	journal	January 2019
Deconvolutional networks Zeiler, Matthew D.; Krishnan, Dilip; Taylor, Graham W. 2010 IEEE Computer Society Conference on Computer Vision and Pattern Recognition https://doi.org/10.1109/CVPR.2010.5539957	conference	June 2010
Deep Back-Projection Networks for Super-Resolution Haris, Muhammad; Shakhnarovich, Greg; Ukita, Norimichi 2018 IEEE/CVF Conference on Computer Vision and Pattern Recognition https://doi.org/10.1109/CVPR.2018.00179	conference	June 2018
Least Squares Generative Adversarial Networks Mao, Xudong; Li, Qing; Xie, Haoran 2017 IEEE International Conference on Computer Vision (ICCV) https://doi.org/10.1109/ICCV.2017.304	conference	October 2017
Pix2Vox: Context-Aware 3D Reconstruction From Single and Multi-View Images Xie, Haozhe; Yao, Hongxun; Sun, Xiaoshuai 2019 IEEE/CVF International Conference on Computer Vision (ICCV) https://doi.org/10.1109/ICCV.2019.00278	conference	October 2019
A Generalized Normalized Gradient Descent Algorithm Mandic, D. P. IEEE Signal Processing Letters, Vol. 11, Issue 2 https://doi.org/10.1109/LSP.2003.821649	journal	February 2004
A Threshold Selection Method from Gray-Level Histograms Otsu, Nobuyuki IEEE Transactions on Systems, Man, and Cybernetics, Vol. 9, Issue 1 https://doi.org/10.1109/TSMC.1979.4310076	journal	January 1979
Laser-preparation of geometrically optimised samples for X-ray nano-CT: LASER-PREPARATION OF GEOMETRICALLY OPTIMISED SAMPLES FOR X-RAY NANO-CT Bailey, J. J.; Heenan, T. M. M.; Finegan, D. P. Journal of Microscopy, Vol. 267, Issue 3 https://doi.org/10.1111/jmi.12577	journal	May 2017
Insights Into Lithium-Ion Battery Degradation and Safety Mechanisms From Mesoscale Simulations Using Experimentally Reconstructed Mesostructures Roberts, Scott A.; Mendoza, Hector; Brunini, Victor E. Journal of Electrochemical Energy Conversion and Storage, Vol. 13, Issue 3 https://doi.org/10.1115/1.4034410	journal	August 2016
Dynamic Noncooperative Game Theory, 2nd Edition Başar, Tamer; Olsder, Geert Jan https://doi.org/10.1137/1.9781611971132	book	January 1998
Centroidal Voronoi Tessellations: Applications and Algorithms Du, Qiang; Faber, Vance; Gunzburger, Max SIAM Review, Vol. 41, Issue 4 https://doi.org/10.1137/S0036144599352836	journal	January 1999
Avoiding Overfitting: A Survey on Regularization Methods for Convolutional Neural Networks Santos, Claudio Filipi Gonçalves Dos; Papa, João Paulo ACM Computing Surveys, Vol. 54, Issue 10s https://doi.org/10.1145/3510413	journal	January 2022
Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell Doyle, Marc Journal of The Electrochemical Society, Vol. 140, Issue 6 https://doi.org/10.1149/1.2221597	journal	January 1993
Model-Instructed Design of Novel Charging Protocols for the Extreme Fast Charging of Lithium-Ion Batteries Without Lithium Plating Mai, Weijie; Colclasure, Andrew M.; Smith, Kandler Journal of The Electrochemical Society, Vol. 167, Issue 8 https://doi.org/10.1149/1945-7111/ab8c84	journal	May 2020
Quantitative Relationships Between Pore Tortuosity, Pore Topology, and Solid Particle Morphology Using a Novel Discrete Particle Size Algorithm Usseglio-Viretta, Francois L. E.; Finegan, Donal P.; Colclasure, Andrew Journal of The Electrochemical Society, Vol. 167, Issue 10 https://doi.org/10.1149/1945-7111/ab913b	journal	June 2020
Modeling Coupled Chemo-Mechanical Behavior of Randomly Oriented NMC811 Polycrystalline Li-Ion Battery Cathodes Taghikhani, Kasra; Weddle, Peter J.; Berger, J. R. Journal of The Electrochemical Society, Vol. 168, Issue 8 https://doi.org/10.1149/1945-7111/ac1811	journal	August 2021
Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating Colclasure, Andrew M.; Dunlop, Alison R.; Trask, Stephen E. Journal of The Electrochemical Society, Vol. 166, Issue 8 https://doi.org/10.1149/2.0451908jes	journal	January 2019
Review of deep learning: concepts, CNN architectures, challenges, applications, future directions Alzubaidi, Laith; Zhang, Jinglan; Humaidi, Amjad J. Journal of Big Data, Vol. 8, Issue 1 https://doi.org/10.1186/s40537-021-00444-8	journal	March 2021
Measuring and testing dependence by correlation of distances Székely, Gábor J.; Rizzo, Maria L.; Bakirov, Nail K. The Annals of Statistics, Vol. 35, Issue 6 https://doi.org/10.1214/009053607000000505	journal	December 2007
Isotropic Gaussian random fields on the sphere: Regularity, fast simulation and stochastic partial differential equations Lang, Annika; Schwab, Christoph The Annals of Applied Probability, Vol. 25, Issue 6 https://doi.org/10.1214/14-AAP1067	journal	December 2015
Random Laguerre tessellations Lautensack, Claudia; Zuyev, Sergei Advances in Applied Probability, Vol. 40, Issue 3 https://doi.org/10.1239/aap/1222868179	journal	September 2008
Efficient Fitting of 3D Tessellations to Curved Polycrystalline Grain Boundaries Petrich, Lukas; Furat, Orkun; Wang, Mingyan Frontiers in Materials, Vol. 8 https://doi.org/10.3389/fmats.2021.760602	journal	December 2021
A Review of Watershed Implementations for Segmentation of Volumetric Images Kornilov, Anton; Safonov, Ilia; Yakimchuk, Ivan Journal of Imaging, Vol. 8, Issue 5 https://doi.org/10.3390/jimaging8050127	journal	April 2022

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