Diffusion–deformation theory for amorphous silicon anodes: The role of plastic deformation on electrochemical performance

Leo, Claudio V. Di; Rejovitzky, Elisha; Anand, Lallit

doi:10.1016/j.ijsolstr.2015.04.028

Cited by 122 publications

(84 citation statements)

References 29 publications

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“…1d and 1e, respectively. Although the diffusion of Li in Si could be influenced by stresses in the particle [24,34,35], the coupling was not considered in this study as the shape changes of particles may be weakly dependent on this coupling. As a result,the diffusion of Li in Si was assumed to be driven by the gradient of concentration alone and was modeled with a constant Li diffusivity = 10 −16 2 /s [36,37].…”

Section: Methodsmentioning

confidence: 99%

Inelastic shape changes of silicon particles and stress evolution at binder/particle interface in a composite electrode during lithiation/delithiation cycling

Wang

Nadimpalli

Shenoy

2016

Extreme Mechanics Letters

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Inelastic shape changes of Si particles and stress evolution at binder/particle interface was modeled using coupled diffusion-stress framework available in finite element software. A simple model that contains two spherical Si particles with and without the polymer binder film was used to represent the composite electrode. The particles were lithiated and delithiated at two different rates: onerepresenting a slow charging case which results in a uniform Li concentration throughout the Si particles and the other representing a fast charging condition which results in non-uniform lithium concentration within the spherical Si particles. The inelastic shape changes and associated contact forces predicted by the model are qualitatively consistent with experimental data. Further, the effect of binder mechanical properties and the binder fraction on the stress evolution in Si particles and at the binder/particle interface was calculated. The proposed model, although simple, can guide a battery design engineer to choose a proper binder, charge/discharge strategy, and binder fraction for a durable electrode design.

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Section: Methodsmentioning

confidence: 99%

Inelastic shape changes of silicon particles and stress evolution at binder/particle interface in a composite electrode during lithiation/delithiation cycling

Wang

Nadimpalli

Shenoy

2016

Extreme Mechanics Letters

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“…The notion of algorithmic functionals further motivates a staggered scheme in line with [48,50,55] to solve the update of the fracture phase field and the coupled deformation-diffusion problem as two successive updates to avoid a computationally more expensive monolithic scheme. In this work, rather than using the concentration field as the primary unknown of the diffusion process [21,79,80], we derive a variational framework in Section 2 that makes use of a global chemical potential field, similar to works such as [81][82][83]. Furthermore, instead of using Cahn-Hilliard type diffusion [75,[84][85][86] to account for the arising two-phase lithiation, we use our recently proposed reaction controlled diffusion model [87] to describe the initial lithiation of c-Si and a-Si.…”

Section: Glass 2µm 1µmmentioning

confidence: 99%

A variational framework to model diffusion induced large plastic deformation and phase field fracture during initial two-phase lithiation of silicon electrodes

Zhang

Krischok

Linder

2016

Computer Methods in Applied Mechanics and Engineering

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Silicon (Si) is considered as a promising next-generation anode material for lithium-ion batteries. However, the large volume change during (de)lithiation processes causes fracture of Si electrodes, thereby limiting Si's practical application in lithium-ion batteries. In this work, we formulate a variational-based fully chemo-mechanical coupled computational framework to study diffusion induced large plastic deformation and phase field fracture in Si electrodes. Into this framework we incorporate a recently developed reaction-controlled diffusion model to predict two-phase lithiation for amorphous Si (a-Si) and crystalline Si (c-Si) as well as diffusion induced anisotropic deformation for c-Si. The variational formulation suggests to consider the deformation field, chemical potential, and the damage field as primary unknowns. The concentration field is considered as a local variable and is recovered from the chemical potential on the element level. We carry out several numerical simulations to show the performance of our computational model and point out the significance of accurately accounting for the presence of the reaction front when modeling diffusion induced fracture problems for both a-Si and c-Si electrodes. In addition, we investigate how the fracture energy release rate, diffusion coefficient, electrode geometry, and geometrical constraints affect the fracture behavior of Si electrodes.

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“…For high-capacity electrodes, lithiation-induced strains are often accommodated by inelastic deformation. Continuum models that account for large elastoplastic deformation of the electrode have appeared more recently [42,[76][77][78][79][80][81]. The simplest formula, regardless the deformation kinematics and constitutive behaviors of the electrodes, may be following [49]:…”

Section: Diffusion-induced Stressesmentioning

confidence: 99%

Electrochemomechanics of Electrodes in Li-Ion Batteries: A Review

Zhao

2016

Journal of Electrochemical Energy Conversion and Storage

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A Li-ion battery is a system that dynamically couples electrochemistry and mechanics. The electrochemical processes of Li insertion and extraction in the electrodes lead to a wealth of phenomena of mechanics, such as large deformation, plasticity, cavitation, fracture, and fatigue. Likewise, mechanics influences the thermodynamics and kinetics of interfacial reactions, ionic transport, and phase transformation of the electrodes. The emergence of high-capacity batteries particularly enriches the field of electrochemomechanics. This paper reviews recent observations on the intimate coupling between stresses and electrochemical processes, including diffusion-induced stresses, stressregulated surface charge transfer, interfacial reactions, inhomogeneous growth of lithiated phases, instability of solid-state reaction front (SSRF), as well as lithiationmodulated plasticity and fracture in the electrodes. Most of the coupling effects are at the early stage of study and are to be better understood. We focus on the elaboration of these phenomena using schematic illustration. A deep understanding of the interactions between mechanics and electrochemistry and bridging these interdisciplinary fields can be truly rewarding in the development of resilient high-capacity batteries.

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Diffusion–deformation theory for amorphous silicon anodes: The role of plastic deformation on electrochemical performance

Cited by 122 publications

References 29 publications

Inelastic shape changes of silicon particles and stress evolution at binder/particle interface in a composite electrode during lithiation/delithiation cycling

Inelastic shape changes of silicon particles and stress evolution at binder/particle interface in a composite electrode during lithiation/delithiation cycling

A variational framework to model diffusion induced large plastic deformation and phase field fracture during initial two-phase lithiation of silicon electrodes

Electrochemomechanics of Electrodes in Li-Ion Batteries: A Review

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