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  • https://doi.org/10.1149/ma2025-0283604mtgabsCopy DOI Icon

Unveiling the Effects of Laser Structuring on Thick Electrodes Using an Electrochemical Model

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Abstract

Developing thick electrodes is a promising strategy to increase the energy density of lithium-ion batteries (LIBs), but severe polarization and ion transport limitations hinder their electrochemical performance [1–3]. Laser structuring has recently emerged as an attractive method to create ion-conducting pathways within the electrode, thereby alleviating transport restrictions and enhancing performance [4–6]. In this study, we systematically investigate the influence of laser structuring on the electrochemical behavior of thick electrodes by combining experiments with a physics-based electrochemical model. Pouch-type mono-cells (50 × 50 mm²) composed of NMC622 cathodes and graphite anodes were fabricated with unstructured and laser-structured electrodes at pitches of 100, 200, and 300 μm. The model was validated against discharge experiments, achieving voltage RMSE values of 61–79 mV across all cases, confirming its predictive reliability. [5,6].The results show that for thin electrodes (~50 μm), laser structuring provides negligible improvement, whereas for electrodes thicker than 100 μm, the benefits become significant. At 100 μm thickness, the liquid-phase ohmic overpotential was reduced by ~62 mV at 1C, and the total overpotential decreased by ~220 mV at 3C compared to unstructured electrodes [4,7]. During 1C charging, structured electrodes achieved nearly twice the usable capacity while maintaining the anode overpotential above 0 V, thereby fully suppressing lithium plating [7]. For thicker electrodes (e.g., 300 μm), unstructured cells suffered from concentration depletion and failed even at 0.1C, whereas structured electrodes alleviated polarization and sustained stable operation. Furthermore, when electrolytes with higher ionic conductivity and diffusivity were employed, overall transport limitations in thick electrodes were substantially alleviated, and the beneficial effects of laser structuring were reinforced under demanding conditions [8,9].These findings demonstrate that laser structuring effectively mitigates transport limitations in thick electrodes, improving charging efficiency, reducing polarization, and suppressing lithium plating. Importantly, the results clarify the thickness and porosity ranges in which structuring is most effective and highlight its synergy with advanced electrolytes. Overall, this work provides design guidelines for next-generation LIBs that balance energy density and rate capability through application-specific electrode structuring strategies References [1] M. Singh, J. Kaiser, H. Hahn, Thick Electrodes for High Energy Lithium Ion Batteries, J. Electrochem. Soc., 162 (2015) A1196–A1201.[2] H. Gao, Q. Wu, Y.X. Hu, J.P. Zheng, K. Amine, Z.H. Chen, Revealing the Rate-Limiting Li-Ion Diffusion Pathway in Ultrathick Electrodes for Li-Ion Batteries, J. Phys. Chem. Lett., 9 (2018) 5100–5104.[3] H.H. Zheng, J. Li, X.Y. Song, G. Liu, V.S. Battaglia, A comprehensive understanding of electrode thickness effects on the electrochemical performances of Li-ion battery cathodes, Electrochim. Acta, 71 (2012) 258–265.[4] J. Kriegler, L. Hille, S. Stock, et al., Enhanced performance and lifetime of lithium-ion batteries by laser structuring of graphite anodes, Appl. Energy, 303 (2021) 117611.[5] J. Park, S. Hyeon, S. Jeong, H.J. Kim, Performance enhancement of Li-ion battery by laser structuring of thick electrode with low porosity, J. Ind. Eng. Chem., 70 (2019) 178–185.[6] V. Goel, K.H. Chen, N.P. Dasgupta, K. Thornton, Optimization of laser-patterned electrode architectures for fast charging of Li-ion batteries using simulations parameterized by machine learning, Energy Storage Mater., 57 (2023) 44–58.[7] J.B. Habedank, J. Kriegler, M.F. Zaeh, Enhanced Fast Charging and Reduced Lithium-Plating by Laser-Structured Anodes for Lithium-Ion Batteries, J. Electrochem. Soc., 166 (2019) A3940–A3949.[8] K.M. Diederichsen, E.J. McShane, B.D. McCloskey, Promising Routes to a High Li+ Transference Number Electrolyte for Lithium Ion Batteries, ACS Energy Lett., 2 (2017) 2563–2575.[9] P. Zhou, X.K. Zhang, Y. Xiang, K. Liu, Strategies to enhance Li+ transference number in liquid electrolyte for better lithium batteries, Nano Res., 16 (2023) 8055–8071.

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