Digital twin quantifies spatial-heterogeneity-driven failure in fast-charging lithium-ion battery anodes

Abstract

Fast charging of lithium-ion batteries is critically constrained by the anode degradation processes—including Li plating, solid electrolyte interphase (SEI) formation, and stress accumulation—yet the impact of microstructural heterogeneity on these coupled degradation modes remains elusive. Here, we present a 3D digital twin framework to quantitatively reveal that phase-level heterogeneity is a decisive driver of reaction asymmetry, side-reaction imbalance, and stress localization. Using an experimentally informed electrode validated against measured charge profiles, we varied binder distribution, porosity, and electrode thickness to resolve their global and localized effects. Binder heterogeneity exerts only marginal impact on overall capacity in 50 μm electrodes; however, under steep gradients, its effect becomes markedly amplified—intensifying electrolyte concentration variations, disturbing Li-ion flux, promoting uneven Li plating and SEI formation, and inducing stress hotspots. Higher porosity moderates these imbalances by improving ionic transport. In contrast, mild gradients preserve more homogeneous reaction kinetics across the electrode depth. These effects become more pronounced in thicker electrodes (83 μm), where mild gradients clearly surpass the steep one. This work identifies microstructural heterogeneity as a predictive descriptor of anode degradation under fast charging, demonstrating that regulation of heterogeneity over averaged structural metrics mitigates Li plating, SEI growth, and stress localization effects.

Keywords

digital twin / electrochemical–mechanical stress / Li plating / lithium-ion battery / microstructural heterogeneity / SEI layer

References

[1] Kim T, Song W, Son D-Y, Ono LK, Qi Y. Lithium-ion batteries: outlook on present, future, and hybridized technologies. J Mater Chem A. 2019; 7(7): 2942-2964.

[2] Liu Y, Zhu Y, Cui Y. Challenges and opportunities towards fast-charging battery materials. Nat Energy. 2019; 4(7): 540-550.

[3] Wang C-Y, Liu T, Yang X-G, et al. Fast charging of energy-dense lithium-ion batteries. Nature. 2022; 611(7936): 485-490.

[4] Weng J, Jossen A, Stefanopoulou A, Li J, Feng X, Offer G. Fast-charging lithium-ion batteries require a systems engineering approach. Nat Energy. 2025; 10(11): 1-2.

[5] Agubra VA, Fergus JW. The formation and stability of the solid electrolyte interface on the graphite anode. J Power Sources. 2014; 268: 153-162.

[6] McShane EJ, Colclasure AM, Brown DE, Konz ZM, Smith K, McCloskey BD. Quantification of inactive lithium and solid–electrolyte interphase species on graphite electrodes after fast charging. ACS Energy Lett. 2020; 5(6): 2045-2051.

[7] Wu S, Zhang Y, Liang H, et al. In-situ electrochemical customization of solid electrolyte interphase for fast-charging and long-cycle-life graphite anodes. Energy Storage Mater. 2025; 75:104024.

[8] Cai W, Yan C, Yao YX, et al. The boundary of lithium plating in graphite electrode for safe lithium-ion batteries. Angew Chem Int Ed. 2021; 60(23): 13007-13012.

[9] Mei W, Jiang L, Liang C, Sun J, Wang Q. Understanding of Li-plating on graphite electrode: detection, quantification and mechanism revelation. Energy Storage Mater. 2021; 41: 209-221.

[10] Gu X, Zhang Q, Chen Q, et al. A lithium dendrite inhibitor in graphite anodes enabling fast-charging and low-temperature lithium-ion pouch cells. Adv Mater. 2025; 37(21):2501448.

[11] Zheng H, Zhang L, Liu G, Song X, Battaglia VS. Correlationship between electrode mechanics and long-term cycling performance for graphite anode in lithium ion cells. J Power Sources. 2012; 217: 530-537.

[12] Üçel İ, Gupta P, Gudmundson P. Experimental determination of the constitutive properties of a graphite anode layer in lithium-ion batteries using a bending test method. J Energy Storage. 2022; 46:103845.

[13] Ding S, Wang L, Dai H, He X. Prognosticating nonlinear degradation in lithium-ion batteries: operando pressure as an early indicator preceding other signals of capacity fade and safety risks. Energy Storage Mater. 2025; 75:103998.

[14] Adebanjo IT, Eko J, Agbeyegbe AG, et al. A comprehensive review of lithium-ion battery components degradation and operational considerations: a safety perspective. Energ Adv. 2025; 4(7): 820-877.

[15] Shu W, Zeng Z, Qin M, et al. Perspective on fast-charging lithium-ion batteries: mechanism, detection, and suppression of graphite anode lithium plating. Energy Storage Mater. 2025; 81:104479.

[16] Liang Z, Liu C, Bai X, et al. Composite electrolyte with self-inserted structure and all-trans F conformation provides fast Li⁺ transport for solid-state Li metal batteries. InfoMat. 2024; 6(11):e12613.

[17] Yang B, Wang Y, Zheng R, et al. Conformational engineering of solvent molecules for high-voltage and fast-charging lithium metal batteries. Angew Chem. 2025; 137(33):e202508486.

[18] Xu W, Mu Y, Yin Y, et al. Conjugated topologically confined composite electrolytes for robust high-voltage and high-temperature semi-solid-state lithium metal batteries. Energy Environ Sci. 2026; 19(1): 384-396.

[19] Mao S, Wang Y, Lu Y, et al. In situ evaluation and manipulation of lithium plating morphology enabling safe and long-life lithium-ion batteries. InfoMat. 2025; 7(1):e12612.

[20] Jang D, Suh S, Yoon H, et al. Enhancing rate capability of graphite anodes for lithium-ion batteries by pore-structuring. Appl Surf Sci Adv. 2021; 6(9):100168.

[21] Robertson DC, Flores L, Dunlop AR, et al. Effect of anode porosity and temperature on the performance and lithium plating during fast-charging of lithium-ion cells. Energ Technol. 2021; 9(1):2000666.

[22] Ahmadi S, Maddipatla D, Bazuin BJ, Atashbar MZ. A comprehensive experimental study on microstructure-graded graphite anodes for enhancing fast-charging capability of lithium-ion batteries. Adv Energy Sustain Res. 2024; 5(8):202300213.

[23] Lu X, Lagnoni M, Bertei A, et al. Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling. Nat Commun. 2023; 14(1):5127.

[24] Duan X, Li B, Li J, Gao X, Wang L, Xu J. Quantitative understanding of lithium deposition-stripping process on graphite anodes of lithium-ion batteries. Adv Energ Mater. 2023; 13(10):202203767.

[25] Jang S, Kang Y, Kim H, Park J, Lee KT. Digital twin reveals the impact of carbon binder domain distribution on performance of lithium-ion battery cathodes. Small Struct. 2025; 6(4):2400350.

[26] Lu L-L, Lu Y-Y, Zhu Z-X, et al. Extremely fast-charging lithium ion battery enabled by dual-gradient structure design. Sci Adv. 2022; 8(17):eabm6624.

[27] Liao Z, Li H, Wang H, Liu B. Mesoscale mechanical models for active materials in lithium-ion batteries using the multi-particle finite element method. Extreme Mech Lett. 2024; 69:102154.

[28] Usseglio-Viretta FL, Colclasure AM, Allen J, et al. Microstructure scale lithium-ion battery modeling: part III. When and where lithium plating occurs and its correlation with the electrode microstructure. J Electrochem Soc. 2025; 172(9):90502.

[29] Luo W, Jiao J-Y, Wang J, Duan Y-L, Shen Z-H. Understanding the microstructure effects of graphite electrode in lithium-ion batteries through multi-physics simulation. Appl Phys Lett. 2025; 126(12):257063.

[30] Li X, Chen Y, Lu Y, et al. Spatial-dependent coupling of electrochemistry, mass transport, and stress in silicon-graphite composite electrodes for lithium-ion batteries. Adv Funct Mater. 2025; 35(3):2413560.

[31] Niu X, Lu Y, Chen P, et al. Gradient-matched microstructural engineering for fast-charging, damage-tolerant thick electrodes of lithium-ion batteries. Adv Energ Mater. 2025; 15(29):202502245.

[32] He X, Zheng S, Sun K, et al. Operando electrode-scale stress characterization revealing the Li⁺ insertion mechanism of graphite anode. Energy Storage Mater. 2025; 82:104629.

[33] Kang Y, Jang S, Kim H, Park J, Lee KT. Digital twin-driven insights into electrochemical, mechanical and microstructural interactions of lithium-ion battery anode. Chem Eng J. 2025; 518:164524.

[34] Chen F, Chen T, Lu K, et al. Three-dimensional electrochemical-thermodynamic modeling reveals manufacturing defect mechanisms governing lithium plating in lithium-ion batteries. Chem Eng J. 2025; 521:166887.

[35] Tariq F, Yufit V, Kishimoto M, et al. Three-dimensional high resolution X-ray imaging and quantification of lithium ion battery mesocarbon microbead anodes. J Power Sources. 2014; 248: 1014-1020.

[36] Sarkar A, Shrotriya P, Nlebedim IC. Parametric analysis of anodic degradation mechanisms for fast charging lithium batteries with graphite anode. Comput Mater Sci. 2022; 202:110979.

[37] Gao X, Li S, Xue J, Hu D, Xu J. Toward a fundamental understanding of the heterogeneous multiphysics behaviors of silicon monoxide/graphite composite anodes. Carbon Energ. 2023; 6(1):e385.

[38] Kraft L, Habedank JB, Frank A, Rheinfeld A, Jossen A. Modeling and simulation of pore morphology modifications using laser-structured graphite anodes in lithium-ion batteries. J Electrochem Soc. 2020; 167(1):13506.

[39] Han S, Tang Y, Rahimian SK. A numerically efficient method of solving the full-order pseudo-2-dimensional (P2D) Li-ion cell model. J Power Sources. 2021; 490:229571.

[40] Kumaresan K, Sikha G, White RE. Thermal model for a Li-ion cell. J Electrochem Soc. 2007; 155(2): A164.

[41] Karthikeyan DK, Sikha G, White RE. Thermodynamic model development for lithium intercalation electrodes. J Power Sources. 2008; 185(2): 1398-1407.

[42] Aylward GH, Findlay T. SI Chemical Data. 3rd ed. John Wiley & Sons; 1994.

[43] Qi Y, Guo H, Hector LG, Timmons A. Threefold increase in the Young's modulus of graphite negative electrode during lithium intercalation. J Electrochem Soc. 2010; 157(5): A558.

[44] Park J, Kim D, Appiah WA, et al. Electrode design methodology for all-solid-state batteries: 3D structural analysis and performance prediction. Energy Storage Mater. 2019; 19: 124-129.

[45] Güneren A, Nada AA, Šišková AO, et al. Novel alginate-based binders for silicon–graphite anodes in lithium-ion batteries: effect of binder chemistry on the electrochemical performance. J Appl Electrochem. 2024; 54(6): 1409-1423.

[46] Chen C-H, Planella FB, O'Regan K, Gastol D, Widanage WD, Kendrick E. Development of experimental techniques for parameterization of multi-scale lithium-ion battery models. J Electrochem Soc. 2020; 167(8):080534.

[47] Zavalis TG, Behm M, Lindbergh G. Investigation of short-circuit scenarios in a lithium-ion battery cell. J Electrochem Soc. 2012; 159(6): A848-A859.

[48] Nyman A, Behm M, Lindbergh G. Electrochemical characterisation and modelling of the mass transport phenomena in LiPF6–EC–EMC electrolyte. Electrochim Acta. 2008; 53(22): 6356-6365.

[49] Mei W, Zhang L, Sun J, Wang Q. Experimental and numerical methods to investigate the overcharge caused lithium plating for lithium ion battery. Energy Storage Mater. 2020; 32: 91-104.

[50] Liu C, Liu L. Optimal design of Li-ion batteries through multi-physics modeling and multi-objective optimization. J Electrochem Soc. 2017; 164(11): E3254-E3264.

[51] Keil J, Jossen A. Electrochemical modeling of linear and nonlinear aging of lithium-ion cells. J Electrochem Soc. 2020; 167(11):110535.

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