Topological and network analysis of lithium ion battery components: the importance of pore space connectivity for cell operation

Lagadec, Marie Francine; Zahn, Raphael; Müller, Simon; Wood, Vanessa

doi:10.1039/c8ee00875b

Cited by 65 publications

(63 citation statements)

References 47 publications

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“…The tortuosity factor was estimated by Equation (1) through the calculation of the macroscopic effective diffusion (D eff ) through Fick's first law. [40][41][42] The Neumann boundary condition was implemented at the interface between the solid electrolyte and the other components (Sn, Li x Sn, and cracks), namely, no flux penetration from the solid electrolyte to the other components was considered. The reconstructed electrode was subjected to an ion pool with fixed concentration, then the ions start to diffuse into the electrode through the solid electrolyte toward the steady states.…”

Section: Methodsmentioning

confidence: 99%

“…The tortuosity factor was estimated by Equation through the calculation of the macroscopic effective diffusion ( D eff ) through Fick's first law . The Neumann boundary condition was implemented at the interface between the solid electrolyte and the other components (Sn, Li x Sn, and cracks), namely, no flux penetration from the solid electrolyte to the other components was considered.…”

Section: Methodsmentioning

confidence: 99%

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Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Billaud

Jerjen

et al. 2019

Advanced Energy Materials

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materials generates volume changes. [2,3] In conventional lithium-ion batteries (LiBs) employing liquid electrolytes, volume expansion dissipates in the electrode matrix (carbon/binder) and depends only on the intrinsic properties of the active material. [4,5] The mechanical fracture of the active material particles and mechanical disintegration of the electrode might be even more severe for all-solid-state batteries (SSBs) as the battery needs to maintain its mechanical integrity for proper cycling.Research in the field of SSBs is motivated by their promised high power and energy density on the cell level compared to conventional LiBs. [6] In particular, inorganic glassy and ceramic solid electrolyte (SE), for example, the thio-LiSICON family [6][7][8] and garnet-type (Li 5 La 3 M 2 O 12 ) conductors, [9] with high room-temperature ionic conductivity up to 10 mS cm −1 , moved the performance of SSBs close to and beyond that of the state-of-the-art LiB. [6] Among all superionic conductors, amorphous Li 2 S-P 2 S 5 (LPS) stands out due to its low Young's modulus (E = 18.5 GPa) [10] and its ability to be well densified by cold pressing. [11] Theoretically, the elasticity of LPS is beneficial for accommodating the stress caused by the volume change of the active material during cycling. However, All-solid-state batteries (SSBs) are considered as attractive options for next-generation energy storage owing to the favorable properties (unit transference number and thermal stabilities) of solid electrolytes. However, there are also serious concerns about mechanical deformation of solid electrolytes leading to the degradation of the battery performance. Therefore, understanding the mechanism underlying the electromechanical properties in SSBs is essentially important. Here, 3D and time-resolved measurements of an all-solid-state cell using synchrotron radiation X-ray tomographic microscopy are shown. The gradient of the electrochemical reaction and the morphological evolution in the composite layer can be clearly observed. Volume expansion/compression of the active material (Sn) is strongly oriented along the thickness of the electrode. While this results in significant deformation (cracking) in the solid electrolyte region, organized cracking patterns depending on the particle size and their arrangements is also found. This study based on operando visualization therefore opens the door toward rational design of particles and electrode morphology for all-solid-state batteries. BatteriesThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Billaud

Jerjen

et al. 2019

Advanced Energy Materials

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“…This is consistent with wet-stretched PE separators being highly isotropic, 20 and implies that PE separators tolerate multidirectional loading. In contrast, the node angle distributions in the non-compressed PP structure are skewed for nodes of order 3 due to the anisotropic structure of PP 22,38 (Sections 9-10 in the SM). The inset illustrates how the presence of nanofibers for example in the transverse direction leads to angles for nodes of orders 3 and 4 that are smaller and larger than 120 • (i.e., near 90 • and 180 • ).…”

Section: Optimizing Separator Structure To Minimize Local Compressivementioning

confidence: 96%

“…The connectivity density gives insight into how connected a structure is and has previously been used to described the pore space of LIB separators. 22 For both PE and PP under compressive strains up to 20%, the connectivity density of the pore space increases by ∼23 and ∼65%, respectively compared to the dry, non-compressed state (Figure 5h). This is because the polymer bulges into the pores adding more complexity to the pore space.…”

Section: Changes To Microstructure In Response To Compressive Strainmentioning

confidence: 97%

Designing Polyolefin Separators to Minimize the Impact of Local Compressive Stresses on Lithium Ion Battery Performance

Lagadec

Zahn

Wood

2018

J. Electrochem. Soc.

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In this paper, we study how polyolefin separators respond to compressive stress, which can occur during battery operation as active particles lithiate, expand, and push into and deform the separator. We use real microstructures of polyethylene and polypropylene separators acquired with focused ion beam scanning electron microscopic (FIB-SEM) tomography and simulate how these structures deform under compressive strain. After validating our mechanical simulations, we characterize how the microstructural properties of the separators change as a function of compressive strain and simulate the influence these changes in microstructure have on the lithium ion transport through the separator. We find that a given compressive strain negatively impacts the microstructure of polyethylene separator more than that of a polypropylene separator. To understand the origins of the different response to compressive strains in polyethylene and polypropylene separators, we use a network-based analysis to assess the type of mechanical deformations occurring in the separator membrane and show that it is the combination of material properties and structure that are responsible for the greater stability of polypropylene. This work highlights how the structure of a separator plays an important role in its mechanical robustness and prevention of cell degradation.

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“…The tortuosity factor was estimated by equation (1) through the calculation of the macroscopic effective diffusion (D eff ) through Fick's first law. [39,40,41] The Neumann boundary condition was implemented at the interface between the solid electrolyte and the other components (Sn, Li x Sn and cracks); namely no flux penetration from the solid electrolyte to the other components was considered. The reconstructed electrode was subjected to an ion pool with fixed concentration, then the ions start to diffuse into the electrode through the solid electrolyte towards the steady states.…”

Section: Tortuosity Factor Estimationmentioning

confidence: 99%

Operando Visualization of Morphological Dynamics in All-Solid-State Batteries

Wu¹,

Billaud²,

Jerjen³

et al. 2019

Preprint

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All-solid-state batteries are considered as attractive options for next-generation energy storage owing to the favourable properties (unit transference number and thermal stabilities) of solid electrolytes. However, there are also serious concerns about mechanical deformation of solid electrolytes leading to the degradation of the battery performance. Therefore, understanding the mechanism underlying the electro-mechanical properties in SSBs are essentially important.Here, we show three-dimensional and time-resolved measurements of an all-solid-state cell using synchrotron radiation x-ray tomographic microscopy. We could clearly observe the gradient of the electrochemical reaction and the morphological evolution in the composite layer. Volume expansion/compression of the active material (Sn) was strongly oriented along the thickness of the electrode. While this results in significant deformation (cracking) in the solid electrolyte region, we also find organized cracking patterns depending on the particle size and their arrangements. This study based on operando visualization therefore opens the door towards rational design of particles and electrode morphology for all-solid-state batteries.

show abstract

Topological and network analysis of lithium ion battery components: the importance of pore space connectivity for cell operation

Abstract: Pore space connectivity is a useful metric for describing microstructure of lithium ion battery components.

Cited by 65 publications

References 47 publications

Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Operando Visualization of Morphological Dynamics in All‐Solid‐State Batteries

Designing Polyolefin Separators to Minimize the Impact of Local Compressive Stresses on Lithium Ion Battery Performance

Operando Visualization of Morphological Dynamics in All-Solid-State Batteries

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