Multiscale Modeling and Design of Electrochemical Systems

Braatz, Richard D.; Seebauer, Edmund G.; Alkire, Richard C.

doi:10.1002/9783527625307.ch4

Cited by 16 publications

(17 citation statements)

References 156 publications

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“…Dependent on the particular simulation, the robustness of the multiscale model can be sensitive on coupling strategy, such as iteration time step and data filter type. 34 The whole code including macroscopic and atomistic model is implemented in MATLAB. Partial differential equations are solved by the finite volume method and adaptive ODE solvers.…”

Section: Mathematical Modelingmentioning

confidence: 99%

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Multi-Scale Simulation of Heterogeneous Surface Film Growth Mechanisms in Lithium-Ion Batteries

Röder

Braatz

Krewer

2017

J. Electrochem. Soc.

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A quantitative description of the formation process of the solid electrolyte interface (SEI) on graphite electrodes requires the description of heterogeneous surface film growth mechanisms and continuum models. This article presents such an approach, which uses multi-scale modeling techniques to investigate multi-scale effects of the surface film growth. The model dynamically couples a macroscopic battery model with a kinetic Monte Carlo algorithm. The latter allows the study of atomistic surface reactions and heterogeneous surface film growth. The capability of this model is illustrated on an example using the common ethylene carbonatebased electrolyte in contact with a graphite electrode that features different particle radii. In this model, the atomistic configuration of the surface film structure impacts reactivity of the surface and thus the macroscopic reaction balances. The macroscopic properties impact surface current densities and overpotentials and thus surface film growth. The potential slope and charge consumption in graphite electrodes during the formation process qualitatively agrees with reported experimental results. A long lifetime for lithium-ion batteries is key to reducing battery cost and increasing acceptance for new applications. The most important but still not well understood aging phenomenon is the growth of a solid film at graphite negative electrodes.1-3 Graphite is the common negative electrode and operates at conditions outside the electrochemical stability window of the electrolyte.2,4 Its decomposition takes place at the surface of the electrode particles and leads to the formation of a surface film, i.e. solid electrolyte interface (SEI). The SEI is mainly built during the first cycles prior to use and is considered to be part of the manufacturing process. 5 The aim of the formation process is to create an interface that is a good lithium-ion conductor but insulating for electrons and prohibits direct contact between electrode and electrolyte in order to provide good performance and long lifetime.4 Different compositions of the film have been proposed by different research groups. 6,7 Since the composition and structure and so the film characteristic is determined during the first cycles, 7 a detailed understanding of this growth mechanism is needed to improve cycling performance.The SEI is formed by a complex mechanism. 5 An atomistic reaction mechanism involves lithium salt and solvent as reactants as well as a variety of different organic and inorganic intermediates and solid products. 7,8 The observation of the formation process is challenging, because of the film's thickness of only several nanometers. Additionally, macroscopic properties such as particle size or operating conditions, e.g. C-rate and environmental temperature, have an important impact on the formation process.3,4 Although SEI film formation has been studied for decades using experimental and simulation-based methods, the exact mechanism of chemical and electrochemical reactions and the growth of the solid fi...

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Section: Mathematical Modelingmentioning

confidence: 99%

“…Therefore, data filters are applied to smooth the output of the atomistic model in Step 3. 34 The smoothed output is used in Step 5 to predict the parameters of the following multi-scale iteration and is provided as continuous time dependent function to the macroscopic model.…”

Section: Mathematical Modelingmentioning

confidence: 99%

Multi-Scale Simulation of Heterogeneous Surface Film Growth Mechanisms in Lithium-Ion Batteries

Röder

Braatz

Krewer

2017

J. Electrochem. Soc.

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“…Reactions generate a flux F of new particles depositing onto the surface, which constitutes the simulation domain (1). Those particles can then move around the domain according to the laws of random walks (2). Particles can collide and form a nucleus (3), which is assumed to be a stable aggregate of two adjacent particles.…”

Section: The Exact-lattice-first-passage-time (Elfpt) Methodsmentioning

confidence: 99%

“…Combined with the coin flip for the x-location (x 0 + L or x 0 − L), we then have the coordinates of the exit location. This problem can be written formally in terms of the evolution of the probability density function P i (t) already given by the diffusion master equation (2). The initial conditions are given by…”

Section: Exit Locationmentioning

confidence: 99%

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An exact and efficient first passage time algorithm for reaction–diffusion processes on a 2D-lattice

Bezzola¹,

Bales²,

Alkire³

et al. 2014

Journal of Computational Physics

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We present an exact and efficient algorithm for reaction-diffusion-nucleation processes on a 2D-lattice. The algorithm makes use of first passage time (FPT) to replace the computationally intensive simulation of diffusion hops in KMC by larger jumps when particles are far away from step-edges or other particles. Our approach computes exact probability distributions of jump times and target locations in a closed-form formula, based on the eigenvectors and eigenvalues of the corresponding 1D transition matrix, maintaining atomic-scale resolution of resulting shapes of deposit islands. We have applied our method to three different test cases of electrodeposition: pure diffusional aggregation for large ranges of diffusivity rates and for simulation domain sizes of up to 4096 × 4096 sites, the effect of diffusivity on island shapes and sizes in combination with a KMC edge diffusion, and the calculation of an exclusion zone in front of a step-edge, confirming statistical equivalence to standard KMC simulations. The algorithm achieves significant speedup compared to standard KMC for cases where particles diffuse over long distances before nucleating with other particles or being captured by larger islands.

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Electrodeposition of Copper

Dini

Snyder

2010

Modern Electroplating

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Polyethylene oxides, glycols, and amines U.S.5,024,736 6/18/91 Clauss et al. Disubstituted ethane sulfonic compounds U.S.4,990,224 2/5/91 Mahmoud Urea, sodium lauryl sulfate, and tosyl or mesyl sulfonic acid U.S.4,975,159 12/4/90 Dahms Alkoxylated lactam amides U.S.4,954,226 9/4/90 Mahmoud Urea and glycerin U.S.4,948,474 8/14/90 Miljkovic Alkylarylene U.S.4,897,165 1/30/90 Bernards et al. Copper/sulfuric acid ratios U.S.4,781,801 11/1/88 Frisby Polyether surfactants þ sulfurized benzene þ grain refiner U.S.4,673,467 6/16/87 Nee Polyethers þ mercaptoimidazole þ sulfurized benzene U.S.4,555,315 11/26/85 Barbieri et al. Polyethers þ organic divalent sulfur compound þ tertiary alkyl amine with polyepichlorohydrin U.S.4,551,212 11/5/85 Rao et al. Phenazine dyestuffs U.S.4,540,473 11/22/83 Bindra et al. S-containing anions other than SO 4 U.S.4,521,282 7/11/84 Tremmel Sulfamic acid U.S.4,490,220 12/25/84 Houman Nitrogen-carbon-sulfur compound U.S.4,430,173 2/7/84 Boudot et al. Sodium salt of W-sulfo-n-propyl N,N-diethyldithiocarbamate, PEG, and crystal violet U.S.4,376,685 6/24/81 Watson Alkylated polyalkyleneimine U.S.4,347,108 8/31/82 Willis Nitrogen-and sulfur-containing compounds U.S.4,336,114 6/22/82 Mayer et al. Phthalocyanine, tertiary alkyl amine with polyepichloro hydrin, polyethyleneimine U.S.4,334,966 12/2/81 Beach et al. Polyether, mercaptoimidazole, sulfurized benzene U.S.4,310,392 1/12/82 Kohl Phenolphthalein U.S.4,272,335 2/19/80 Combs Substituted phthalocyanine radical U.S.4,242,181 12/30/80 Malak Regular coffee U.S.4,134,803 1/16/79 Eckles et al. Disulfides, sulfonic acids, and aliphatic aldehyde U.S.4,110,176 8/29/78 Creutz et al.

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Multiscale Modeling and Design of Electrochemical Systems

Cited by 16 publications

References 156 publications

Multi-Scale Simulation of Heterogeneous Surface Film Growth Mechanisms in Lithium-Ion Batteries

Multi-Scale Simulation of Heterogeneous Surface Film Growth Mechanisms in Lithium-Ion Batteries

An exact and efficient first passage time algorithm for reaction–diffusion processes on a 2D-lattice

Electrodeposition of Copper

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