Modeling the Electrical Conductive Paths within All‐Solid‐State Battery Electrodes

Giménez, Clara Sangrós; Helmers, Laura; Schilde, Carsten; Diener, Alexander C.; Kwade, Arno

doi:10.1002/ceat.201900501

Cited by 29 publications

(21 citation statements)

References 42 publications

(48 reference statements)

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“…The electrical network conductivity is strongly dependent on the conductive paths from the current collector to the separator. 39 Therefore, it is of interest to evaluate conductivity with respect to these paths. Here, the focus is set on two structural network properties: (I) the number of transit edges χ TP and (II) the transit path length λ TP .…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Conductive Networks and Their Impact on Uncertainty, Degradation, and Failure of Lithium-Ion Battery Electrodes

Schmidt

Röder

2021

ACS Appl. Energy Mater.

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Manufacturing high-quality lithium-ion batteries requires a detailed understanding of the complex correlations between the electrode microstructure and the kinetic processes. Sophisticated microstructure design is of interest to enable optimal ionic and electrical transport to minimize uncertainties and capacity fade. One important feature of the microstructure is the carbon black-binder matrix (CBM) forming a network-like structure. The CBM is often solely evaluated by its electrical bulk conductivity of the electrode. In this work, a hybrid model approach is established and applied to gain mechanistic understanding of the influence of different electrical network structures on uncertainty, degradation, and failure of battery cells. Artificial network structures are generated based on degree distributions, that is, normal distributions or power-law distributions. Degradation is modeled by edge removal, representing the mechanical decomposition of the CBM during battery utilization. Simulation results show that the electrical bulk conductivity is not sufficient to rate the quality of the electrical network, and also other properties such as the connectivity and the number of transit paths need to be taken into account. It can be seen that normally distributed connectivity in general yields low uncertainties and is robust against edge removal. In contrast, power-law distributions, that is, scale-free-like networks, possess few critical edges that yield significant uncertainty. The presented model approach allows us to study network structures in-depth and to identify beneficial structural network properties.

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Section: ■ Results and Discussionmentioning

confidence: 99%

“…The electrical network conductivity is strongly dependent on the conductive paths from the current collector to the separator . Therefore, it is of interest to evaluate conductivity with respect to these paths.…”

Section: Resultsmentioning

confidence: 99%

Conductive Networks and Their Impact on Uncertainty, Degradation, and Failure of Lithium-Ion Battery Electrodes

Schmidt

Röder

2021

ACS Appl. Energy Mater.

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“…Alternative approaches, leading to qualitatively similar results were presented previously. 28,29 In the first case, 25 a Hertz−Mindlin type contact law was applied to calculate contact forces between particles, and an empirically derived expression for the resistance between two spheres, normalized to a resistance of a cylinder was used. In the second case, 29 a similar approximation of a sphere to a cylinder was used and a similar assumption of parallel connectivity paths was used as in Figure 3.…”

Section: Methodsmentioning

confidence: 99%

Li-Ion Permeability of Holey Graphene in Solid State Batteries: A Particle Dynamics Study

Barrios

Rains

Lin³

et al. 2022

ACS Appl. Mater. Interfaces

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Lithium (Li)-ion permeability of holey graphene (hG) for use as an electrically conducting scaffold in solid-state battery electrodes is explored through the means of a particle dynamics simulation model. While carbon materials do not typically exhibit Li-ion conductivity, the unique structural motif of hG, which consists of two-dimensional nanosheets with arrays of through-thickness holes, may present an opportunity for Li-ion conductors (i.e., solid electrolyte (SE) particles) to make contacts through the holes. In our model, the SE is presented as a system of hard elastic spheres conductive to Li-ions. The SE spheres are in contact with each other through compression between two plane current collectors. One hG layer is inserted between the current collectors and parallel to them. Randomly distributed circular holes in the hG allow for contact between the SE particles on both sides of the hG layer. By solving the Li-ion conducting network formed between the electrodes through the contact points of all the particles, the overall conductivity of the system was calculated as a function of SE particle size and the size and number of the hG holes (i.e., hG porosity). A critical ratio of around 4 between the SE particle size and the pore size was found. Below this critical value, the hG layer becomes practically transparent for Li-ions. This study helps to guide the design of highly efficient solid-state electrode composition and architectures using hG as a unique electrically conducting scaffold.

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“…3b). Further investigations have also shown that the amount and the particle size of electrolytes, active materials and electron conductors are key for effective contact [34][35][36]. For example, Kimura et al [37] perform operando 3D observations of electrolyte/electrode microstructures using a combination of computed-tomography and X-ray absorption near edge structure spectroscopy and found that higher active material loadings can lead to aggregation and Li-ion and electron transfer pathway reduction.…”

Section: Electrolyte and Electrode Microstructuresmentioning

confidence: 99%

Electrolyte/Electrode Interfaces in All-Solid-State Lithium Batteries: A Review

Pang

Pan

Yang

et al. 2021

Electrochem. Energ. Rev.

173

104

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All-solid-state lithium batteries are promising next-generation energy storage devices that have gained increasing attention in the past decades due to their huge potential towards higher energy density and safety. As a key component, solid electrolytes have also attracted significant attention and have experienced major breakthroughs, especially in terms of Li-ion conductivity. However, the poor electrode compatibility of solid electrolytes can lead to the degradation of electrolyte/electrode interfaces, which is the major cause for failure in all-solid-state lithium batteries. To address this, this review will summarize the indepth understanding of physical and chemical interactions between electrolytes and electrodes with a focus on the contact, charge transfer and Li dendrite formation occurring at electrolyte/electrode interfaces. Based on mechanistic analyses, this review will also briefly present corresponding strategies to enhance electrolyte/electrode interfaces through compositional modifications and structural designs. Overall, the comprehensive insights into electrolyte/electrode interfaces provided by this review can guide the future investigation of all-solid-state lithium batteries.

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Modeling the Electrical Conductive Paths within All‐Solid‐State Battery Electrodes

Cited by 29 publications

References 42 publications

Conductive Networks and Their Impact on Uncertainty, Degradation, and Failure of Lithium-Ion Battery Electrodes

Conductive Networks and Their Impact on Uncertainty, Degradation, and Failure of Lithium-Ion Battery Electrodes

Li-Ion Permeability of Holey Graphene in Solid State Batteries: A Particle Dynamics Study

Electrolyte/Electrode Interfaces in All-Solid-State Lithium Batteries: A Review

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