Morphological evolution of a single crystal silicon battery electrode during lithiation and delithiation: An operando phase-contrast imaging study

Ronneburg, Arne; Osenberg, Markus; Dong, Kang; Hilger, André; Härk, Eneli; Silvi, Luca; Manke, Ingo; Ballauff, Matthias; Risse, Sebastian

doi:10.1016/j.ensm.2020.06.007

Cited by 5 publications

(2 citation statements)

References 57 publications

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“…Operando methods for the characterization of (dis-)charge processes in batteries have been already demonstrated to gain completely new insights into the crucial transformation, distribution, and degradation processes in various systems, i.e., Li-ion, [30] Li/S, [31][32][33][34][35][36] and Li-ion with silicon as anode. [37] However, most studies are performed with the coin cell format due to its simpler feasibility, especially in terms of material quantity and processing. Furthermore, only one characterization method is used in most cases, limiting the perspective on specific battery processes.…”

Section: Operando Approachmentioning

confidence: 99%

Operando Radiography and Multimodal Analysis of Lithium–Sulfur Pouch Cells—Electrolyte Dependent Morphology Evolution at the Cathode

Müller

Manke

Hilger

et al. 2022

Advanced Energy Materials

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compared to conventional lithium-ion batteries. [3] However, their widespread commercialization is hampered by the problem of capacity degradation during cycling, even in the state-ofthe-art ether-based electrolyte: Lithium bis(trifluoromethanesulfonyl)imide) (LiTFSI) in 1,2-dimethoxyethane/1,3dioxolane (DME/DOL) with LiNO 3 additive. These degradation processes have various origins and are caused, for example, by the so-called polysulfide shuttle effect. [4][5][6] The diffusion of soluble polysulfides from the cathode side to the anode lowers the coulombic efficiency and may lead to irreversible chemical reactions. This gradual consumption of active material and electrolyte and the corrosion of the metallic lithium anode lead to battery degradation. Another major challenge of Li/S batteries on their way to commercialization is the electrically insulating properties of the two end products of the cathode after charging (elemental sulfur) and discharging (lithium sulfide, Li 2 S). To still achieve the highest possible energy density, carbon is used as the cathode host. Carbon is exceptionally lightweight and offers many different synthesis routes being able to selectively adjust material properties such as porosity, surface functionalization, wettability, and conductivity. [7][8][9][10][11] Many improvements in Li/S battery performance have been achieved in recent years through materials science In recent years, the technology readiness level of next-generation lithium-sulfur (Li/S) batteries has shifted from coin cell to pouch cell dimensions. Promising optimizations of the electrodes, electrolytes, active materials, and additives lead to improved performance and cycling stability. However, new challenges arise with the pouch cell design and engineering (including electrode stacking and electrolyte filling), which influence the mechanistic processes of the cell. This study presents an unprecedented multimodal operando investigation of Li/S batteries on a pouch cell level and provides an inside view of material transformations during battery cycling, using X-ray radiography, electrochemical impedance spectroscopy, and spatially resolved temperature monitoring. With the comparison of two different electrolytes, new experimental details about sulfur and lithium sulfide deposition and dissolution processes are revealed and related to electrolyte and temperature distribution. Operando impedance measurements on monolayer pouch cells yield a clear correlation of electrochemical and macroscopic radiographic observations. Understanding the monolayer cells' behavior represents an optimal foundation for further studies on multilayer pouch cell prototypes and demonstrators with the developed operando setup. Herein the proof of principle for correlated measurement methods on pouch cell level is shown, and the experimental proof of concept for sulfur crystal suppression in sparingly solvating electrolyte is visualized.

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Section: Operando Approachmentioning

confidence: 99%

Operando Radiography and Multimodal Analysis of Lithium–Sulfur Pouch Cells—Electrolyte Dependent Morphology Evolution at the Cathode

Müller

Manke

Hilger

et al. 2022

Advanced Energy Materials

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“…1 Unfortunately, some of these materials show a strong irreversible behavior, mainly due to lithiation induced large volumetric changes, causing poor cycle life of the batteries where they are used. 2 There have been numerous attempts to intricately understand the process of charging and discharging and improve the performance of the batteries. [3][4][5] The functioning of LIB electrodes involves the interaction of several phenomena, such as, chemical diffusion, phase transformation, mechanical deformations and stresses, fracture and electric charge movement.…”

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confidence: 99%

Numerical Voltammetry of Phase Separating Materials Using Phase Field Modeling

Hussain,

Swaminathan,

Phanikumar

2024

J. Electrochem. Soc.

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Higher capacity materials, such as Si and Sn are known to have phase separating behavior during the (de)lithiation. While initial models for lithiation in graphite electrode were based on single phase diffusion, with the introduction of Si and Sn, disposition of the models has shifted to the two-phase diffusion. It is important to understand the interaction of various phenomenon in materials which show phase change during (dis)charging cycles. In this work, we present a phase field model to simulate two-phase lithiation. This model is used to study the electrochemical response of the system by conducting numerical voltammetry. The main goal of this effort is to highlight the difference in electrochemical response occurring during single-phase diffusion and two-phase diffusion and explain the ensuing physics. Furthermore, effect of elasticity which governs the phase-change process and also alters corresponding voltammograms is also studied in detail. The voltammograms show clear shift in current peaks’ size and position for the changing diffusion behavior. Also as elasticity affects the two-phase diffusion, change in nucleation timing and diffusion rate are visible in voltammograms. Additionally, it is also observed how elasticity can cease the phase separation behavior and voltammogram for two-phase diffusion can become identical to single-phase diffusion.

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High-areal capacity Si architecture as an on-chip anode for lithium-ion batteries

Abdelouhab,

Abrenica,

Heitz

et al. 2024

Energy Storage Materials

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Morphological evolution of a single crystal silicon battery electrode during lithiation and delithiation: An operando phase-contrast imaging study

Cited by 5 publications

References 57 publications

Operando Radiography and Multimodal Analysis of Lithium–Sulfur Pouch Cells—Electrolyte Dependent Morphology Evolution at the Cathode

Operando Radiography and Multimodal Analysis of Lithium–Sulfur Pouch Cells—Electrolyte Dependent Morphology Evolution at the Cathode

Numerical Voltammetry of Phase Separating Materials Using Phase Field Modeling

High-areal capacity Si architecture as an on-chip anode for lithium-ion batteries

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