Diffusion‐Induced Stress within Core–Shell Structures and Implications for Robust Electrode Design and Materials Selection

Qi, Yue; Baker, Daniel R.; Cheng, Yang‐Tse

doi:10.1002/9783527690633.ch6

Cited by 11 publications

(12 citation statements)

References 117 publications

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“…[31,[62][63][64] Several groups developed mechanistic models to describe the mechanical response of the SEI on battery cycling. [14,[64][65][66][67][68][69][70][71][72][73][74][75][76][77][78][79] However, these models focus on SEI mechanics and incorporate at most simple SEI growth models. [14,[65][66][67][68]75,79] In this paper, we develop a detailed electrochemo-mechanical model to describe SEI mechanics and growth on a deforming electrode particle.…”

Section: Introductionmentioning

confidence: 99%

Chemo‐Mechanical Model of SEI Growth on Silicon Electrode Particles**

Kolzenberg

Latz

Horstmann

2021

Batteries & Supercaps

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Silicon anodes promise high energy densities of next-generation lithium-ion batteries, but suffer from shorter cycle life. The accelerated capacity fade stems from the repeated fracture and healing of the solid-electrolyte interphase (SEI) on the silicon surface. This interplay of chemical and mechanical effects in SEI on silicon electrodes causes a complex aging behavior. However, so far, no model mechanistically captures the interrelation between mechanical SEI deterioration and accelerated SEI growth. In this article, we present a thermodynamically consistent continuum model of an electrode particle surrounded by an SEI layer. The silicon particle model consistently couples chemical reactions, physical transport, and elastic deformation. The SEI model comprises elastic and plastic deformation, fracture, and growth. Capacity fade measurements on graphite anodes and in-situ mechanical SEI measurements on lithium thin films provide parametrization for our model. For the first time, we model the influence of cycling rate on the long-term mechanical SEI deterioration and regrowth. Our model predicts the experimentally observed transition in time dependence from square-root-of-time growth during battery storage to linear-in-time growth during continued cycling. Thereby our model unravels the mechanistic dependence of battery aging on operating conditions and supports the efforts to prolong the battery life of next-generation lithium-ion batteries.

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Section: Introductionmentioning

confidence: 99%

Chemo‐Mechanical Model of SEI Growth on Silicon Electrode Particles**

Kolzenberg

Latz

Horstmann

2021

Batteries & Supercaps

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“…There have been only a few attempts to study multicomponent diffusion in the systems of an arbitrary geometry. Verbrugge et al [20] simulated Fickian diffusion ( s = 1 ) and stress formation in a spherical core-shell system, as in lithium-ion batteries. Experimentally, the interdiffusion and migration of associated voids, as manifested in bimetallic core-shell nanoparticles, were studied by Chee et al [21].…”

Section: Introductionmentioning

confidence: 99%

Interdiffusion in many dimensions: mathematical models, numerical simulations and experiment

Sapa

Bożek

Tkacz–Śmiech

et al. 2020

Mathematics and Mechanics of Solids

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Over the last two decades, there have been tremendous advances in the computation of diffusion and today many key properties of materials can be accurately predicted by modelling and simulations. In this paper, we present, for the first time, comprehensive studies of interdiffusion in three dimensions, a model, simulations and experiment. The model follows from the local mass conservation with Vegard’s rule and is combined with Darken’s bi-velocity method. The approach is expressed using the nonlinear parabolic–elliptic system of strongly coupled differential equations with initial and nonlinear coupled boundary conditions. Implicit finite difference methods, preserving Vegard’s rule, are generated by some linearization and splitting ideas, in one- and two-dimensional cases. The theorems on the existence and uniqueness of solutions of the implicit difference schemes and the consistency of the difference methods are studied. The numerical results are compared with experimental data for a ternary Fe-Co-Ni system. A good agreement of both sets is revealed, which confirms the strength of the method.

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“…With classical Monte Carlo (MC) and DFT-based methods, Soto and Balbuena 190 found that the oligomers attach/adhere firmly to the Li 13 Si 4 (010) surface with calculated adsorption energies in a range of 3-4 eV and if the coverage oligomer on the surface reaches approximately 1 oligomer per nm 2 , the surface-oligomer interaction will dominate the stabilization of the interface system. Verbrugge et al 191 constructed a core-shell model and derived the lithiation-induced-stress model to evaluate the stress in the SEI layer due to the volume change of the electrode. Taking the input from DFT-computed chemical and mechanical properties, they showed that the SEI layer can sustain the deformation of a conventional graphite electrode but not a silicon electrode.…”

Section: Correlation Of Sei Properties With Battery Performance Starmentioning

confidence: 99%

“…Design of the coating geometry: considering the evolving properties Verbrugge et al 191 pointed out that artificial coatings need to be designed along with the structure of Si and Li electrodes, as the naturally formed SEI components cannot accommodate the large electrode deformation. ALD and MLD provide coating materials with various mechanical properties, such as being more elastic and/or having larger elongation till fracture.…”

Section: In Vitro Design Of the Seimentioning

confidence: 99%

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

et al. 2018

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A passivation layer called the solid electrolyte interphase (SEI) is formed on electrode surfaces from decomposition products of electrolytes. The SEI allows Li + transport and blocks electrons in order to prevent further electrolyte decomposition and ensure continued electrochemical reactions. The formation and growth mechanism of the nanometer thick SEI films are yet to be completely understood owing to their complex structure and lack of reliable in situ experimental techniques. Significant advances in computational methods have made it possible to predictively model the fundamentals of SEI. This review aims to give an overview of state-of-the-art modeling progress in the investigation of SEI films on the anodes, ranging from electronic structure calculations to mesoscale modeling, covering the thermodynamics and kinetics of electrolyte reduction reactions, SEI formation, modification through electrolyte design, correlation of SEI properties with battery performance, and the artificial SEI design. Multiscale simulations have been summarized and compared with each other as well as with experiments. Computational details of the fundamental properties of SEI, such as electron tunneling, Li-ion transport, chemical/mechanical stability of the bulk SEI and electrode/(SEI/) electrolyte interfaces have been discussed. This review shows the potential of computational approaches in the deconvolution of SEI properties and design of artificial SEI. We believe that computational modeling can be integrated with experiments to complement each other and lead to a better understanding of the complex SEI for the development of a highly efficient battery in the future.

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Diffusion‐Induced Stress within Core–Shell Structures and Implications for Robust Electrode Design and Materials Selection

Cited by 11 publications

References 117 publications

Chemo‐Mechanical Model of SEI Growth on Silicon Electrode Particles**

Chemo‐Mechanical Model of SEI Growth on Silicon Electrode Particles**

Interdiffusion in many dimensions: mathematical models, numerical simulations and experiment

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

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