Micro-Scale Modeling of Li-Ion Batteries: Parameterization and Validation

Less, Gregory B.; Seo, Je Hoon; Han, Sangwoo; Sastry, Ann Marie; Zausch, Jochen; Latz, Arnulf; Schmidt, Sebastian; Wieser, Christian; Kehrwald, Dirk; Fell, Stephan

doi:10.1149/2.096205jes

Cited by 133 publications

(136 citation statements)

References 53 publications

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“…30,42,43 As shown schematically in Figure 2a, the simulation environment consists of a porous, three-dimensional electrode microstructure, a 13 μm thick homogenized separator, and a one-voxel thick counter electrode made of pure, non-porous lithium. The pores are filled with electrolyte.…”

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confidence: 99%

Quantifying Inhomogeneity of Lithium Ion Battery Electrodes and Its Influence on Electrochemical Performance

Müller

Eller

Ebner

et al. 2018

J. Electrochem. Soc.

116

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This paper presents an approach to quantify microstructural inhomegeneity in lithium ion battery electrodes over multiple length scales and examines the impact of this microstructural inhomogeneity on electrochemical performance. Commerical graphite anodes are investigated because graphite remains the anode material of choice due to its low cost, mechanical robustness, and suitable electrochemical properties. At the same time, the graphite anode often plays a role in cell degradation and failure, as lithium plating can occur on the graphite anode during charge, when unfavorable microstructure in the graphite electrode leads to a large overpotential. Here, three-dimensional representations of four different commercial anodes obtained with X-ray tomographic microscopy are statistically analyzed to quantify the microstructural inhomogeneity that is commonly present in lithium ion battery electrodes. Electrochemical simulations on the digitalized microstructures are performed to isolate and understand the influence of different types of microstructural inhomogeneity on battery performance. By understanding how distributions in particle size and shape or slurry and electrode processing cause microstructural inhomogeneity and impact performance, it is possible to determine the extent to which homogeneity should be prioritized for specific applications and how homogeneity could be achieved through smart material selection and processing.

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mentioning

confidence: 99%

Quantifying Inhomogeneity of Lithium Ion Battery Electrodes and Its Influence on Electrochemical Performance

Müller

Eller

Ebner

et al. 2018

J. Electrochem. Soc.

116

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“…[18][19][20] Wiedemann et al 19 clearly demonstrated how the complex shape of reconstructed particles changed the electrochemical behavior over more simplistic spherical representations. The effect of aniostropic diffusion of lithium through the particle has also been studied.…”

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confidence: 99%

A Framework for Three-Dimensional Mesoscale Modeling of Anisotropic Swelling and Mechanical Deformation in Lithium-Ion Electrodes

Roberts

Brunini

Long

et al. 2014

J. Electrochem. Soc.

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Lithium-ion battery electrodes rely on a percolated network of solid particles and binder that must maintain a high electronic conductivity in order to function. Coupled mechanical and electrochemical simulations may be able to elucidate the mechanisms for capacity fade. We present a framework for coupled simulations of electrode mechanics that includes swelling, deformation, and stress generation driven by lithium intercalation. These simulations are performed at the mesoscale, which requires 3D reconstruction of the electrode microstructure from experimental imaging or particle size distributions. We present a novel approach for utilizing these complex reconstructions within a finite element code. A mechanical model that involves anisotropic swelling in response to lithium intercalation drives the deformation. Stresses arise from small-scale particle features and lithium concentration gradients. However, we demonstrate, for the first time, that the largest stresses arise from particle-to-particle contacts, making it important to accurately represent the electrode microstructure on the multi-particle scale. Including anisotropy in the swelling mechanics adds considerably more complexity to the stresses and can significantly enhance peak particle stresses. Shear forces arise at contacts due to the misorientation of the lattice structure. These simulations will be used to study mechanical degradation of the electrode structure through charge/discharge cycles. Capacity fade in lithium-ion batteries (LIB) is potentially influenced by a large number of mechanisms, 1 one of which is mechanical degradation of the electrode microstructure. Both electrodes experience mechanical deformation, and in this paper, we focus on the cathode of the lithium-cobalt-oxide (LiCoO 2 , or LCO) system.2 Cathodes are made up of a three-dimensional (3D), percolating, bicontinuous network consisting of solid, electroactive particles, a polymer binder, and electrolyte. The bicontinuous nature of this network is critical, as Li + ions must be able to transport from the anode, through the separator, to any particle in the cathode via the electrolyte. At the same time, electrons must be able to transport through the solid particle network to the current collector. Any particle that becomes physically isolated from, or poorly connected to, its network or from the electrolyte does not contribute to the electrochemical reactions, resulting in capacity loss.One way in which particles may become disconnected from their network is by the swelling, shrinking, and fracture mechanisms that may occur through many charge-discharge cycles.3-6 As lithium intercalates into the electrode particles, the crystal lattice spacing may change either isotropically or anisotropically. For LiCoO 2 cathodes in particular, the crystal lattice shrinks anisotropically upon lithium intercalation 7,8 As was measured by Reimers and Dahn, 7 and later in more detail by Amatucci et al., 8 the lattice shrinkage upon lithiation can be quite significant and is anisotropic in n...

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“…In the second example, we investigate crack initiation and propagation under potentiostatic charging of LiMn 2 O 4 cathodic electrode particle. A two dimensional realistic particle geometry is depicted from SEM micrograph presented in [6] and analysed under plain-strain conditions. The particle size is around ≈ 10µm.…”

Section: Results and Conclusionmentioning

confidence: 99%

Coupled chemomechanics and phase field modeling of failure in electrode materials of Li‐ion batteries

Dal¹,

Miehé²

2013

Proc Appl Math and Mech

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We propose a canonical finite strain theory for diffusion-mechanics coupling for the intercalation induced stress generation in Li-ion electrode particles. The intrinsic coupling arises from both mechanical pressure gradient-induced diffusion of Li-ion particles and diffusion induced swelling/shrinkage leading to mechanical stresses. In addition, we extend the finite strain theory for diffusion-mechanics coupling to chemomechanical fracture of electrode particles by introducing a nonlocal crack phase field which replaces a sharp crack topology with a smooth diffuse interpolation between the intact and broken states of the material. We employ a semi-implicit Galerkin-type finite element method for the solution of resulting set of differential equations. In addition to the mechanical, chemical and crack phase field, we introduce the pressure as an independent field variable in order to reduce the smoothness requirements on the interpolation functions. We illustrate characteristic features of the proposed model by means of representative initial-boundary value problems.

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Micro-Scale Modeling of Li-Ion Batteries: Parameterization and Validation

Cited by 133 publications

References 53 publications

Quantifying Inhomogeneity of Lithium Ion Battery Electrodes and Its Influence on Electrochemical Performance

Quantifying Inhomogeneity of Lithium Ion Battery Electrodes and Its Influence on Electrochemical Performance

A Framework for Three-Dimensional Mesoscale Modeling of Anisotropic Swelling and Mechanical Deformation in Lithium-Ion Electrodes

Coupled chemomechanics and phase field modeling of failure in electrode materials of Li‐ion batteries

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