Low‐Temperature Charging and Aging Mechanisms of Si/C Composite Anodes in Li‐Ion Batteries: An Operando Neutron Scattering Study

Richter, Karsten; Waldmann, Thomas; Paul, Neelima; Jobst, Nicola; Scurtu, Rares-George; Hofmann, M.; Gilles, Ralph; Wohlfahrt‐Mehrens, Margret

doi:10.1002/cssc.201903139

Cited by 44 publications

(68 citation statements)

References 51 publications

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“…Furthermore, it is shown that the relative lithiation/delithiation is influenced by the applied current and the competition between different transport processes. Richter et al [44] . recently studied low temperature charging and aging mechanisms of Si/Gr blended anodes using operando neutron scattering.…”

Section: Introductionmentioning

confidence: 99%

Understanding Component‐Specific Contributions and Internal Dynamics in Silicon/Graphite Blended Electrodes for High‐Energy Lithium‐Ion Batteries

Heubner

Liebmann

Lohrberg

et al. 2021

Batteries & Supercaps

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Blended electrode materials containing high‐capacity silicon (Si) and robust graphite (Gr) materials are considered advanced alternatives to pure graphite electrodes used in Li‐ion batteries. Understanding the component‐specific lithiation and delithiation behavior and electrochemical interactions between the blended materials is of crucial importance for targeted optimization of composition and microstructural design, yet hardly addressed to date. Herein, a model‐like Si/Gr blended electrode and special electrochemical cell are introduced to directly capture the component specific behaviors for the first time. This includes studies of the formation cycles, the reaction distribution between Si and Gr, the component‐specific contributions to the capacity at different charge and discharge rates, and the internal dynamics during pulse loads and subsequent relaxation. The deconvolution of the components’ behavior during operation provides fundamental insights that contribute to a profound understanding and targeted optimization of Si/Gr blended electrodes. Furthermore, the application of the presented experimental approach can serve scientists to identify and study other advanced materials combinations as blended electrodes for rechargeable batteries.

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Section: Introductionmentioning

confidence: 99%

Understanding Component‐Specific Contributions and Internal Dynamics in Silicon/Graphite Blended Electrodes for High‐Energy Lithium‐Ion Batteries

Heubner

Liebmann

Lohrberg

et al. 2021

Batteries & Supercaps

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“…3f) and is consistent with the behavior of deposited Li during rest after charging. 5,[7][8][9][10][11][12]14,15,31 The main difference is that deposited Li metal often shows a dendritic micro structure, whereas the Li metal is compact in our experiment.…”

Section: Resultsmentioning

confidence: 66%

“…This is in accordance with results on re-intercalation of Li deposition by others. 12,[14][15][16][17] In cells with higher internal pressure, e.g. cylindrical cells, it is likely that Li depositions re-intercalate faster due to better contact with the electrode.…”

Section: Discussionmentioning

confidence: 99%

“…9,12 We observed by neutron diffraction that Li deposited on a Si/C electrode re-intercalates into graphite and is then re-distributed to the Si compound. 15 Wandt et al 16 investigated Li deposition with operando electron paramagnetic resonance and observed the re-intercalation of Li as well. However, there is still a lack of knowledge on the mechanistic details.…”

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confidence: 99%

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Mechanistic Details of the Spontaneous Intercalation of Li Metal into Graphite Electrodes

Hogrefe

Hein

Waldmann

et al. 2020

J. Electrochem. Soc.

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The mechanism of the spontaneous intercalation of Li metal into graphite electrodes is highly relevant for aging mechanisms and pre-lithiation of Li-ion cells. In the present work, we introduce a method to investigate this mechanism via measuring the opencircuit-potential (OCP). Experiments without electrolyte, with organic solutions without and with LiPF 6 reveal details on the reaction mechanism at 29 °C. The electrodes are investigated by Raman spectroscopy and glow-discharge optical emission spectroscopy (GD-OES) depth profiling to reveal the spatial distribution of the lithiated phases. The analytical information is enriched by simulations with the Battery and Electrochemistry Simulation Tool (BEST). The combination of tools gives interesting insights into the behavior of negative electrodes regarding re-intercalation of deposited Li into graphite and its kinetics, development of inhomogeneities during aging, as well as pre-lithiation and post-mortem analysis methodology.

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“…In literature, the mechanism of lithium metal deposition is mostly investigated for graphite anodes, [ 102,105,172–175,177,184,185 ] although it is also studied in Si/C composite anodes. [ 186 ] The phenomenon of lithium metal deposition on anodes is highly critical since it can reduce safety by dendrite growth [ 187 ] and exothermic reactions. [ 175,188 ] On graphite anodes, lithium metal deposition is favored during charging at low temperatures, [ 38,102,103,185 ] high charging C‐rates, [ 103,185 ] and high SOCs, [ 103 ] as well as their combination.…”

Section: Anodementioning

confidence: 99%

Fast Charging of Lithium‐Ion Batteries: A Review of Materials Aspects

Weiß

Rueß

Kasnatscheew

et al. 2021

Advanced Energy Materials

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603

348

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Fast charging is considered to be a key requirement for widespread economic success of electric vehicles. Current lithium‐ion batteries (LIBs) offer high energy density enabling sufficient driving range, but take considerably longer to recharge than traditional vehicles. Multiple properties of the applied anode, cathode, and electrolyte materials influence the fast‐charging ability of a battery cell. In this review, the physicochemical basics of different material combinations are considered in detail, identifying the transport of lithium inside the electrodes as the crucial rate‐limiting steps for fast‐charging. Lithium diffusion within the active materials inherently slows down the charging process and causes high overpotentials. In addition, concentration polarization by slow lithium‐ion transport within the electrolyte phase in the porous electrodes also limits the charging rate. Both kinetic effects are responsible for lithium plating observed on graphite anodes. Conclusions drawn from potential and concentration profiles within LIB cells are complemented by extensive literature surveys on anode, cathode, and electrolyte materials—including solid‐state batteries. The advantages and disadvantages of typical LIB materials are analyzed, resulting in suggestions for optimum properties on the material and electrode level for fast‐charging applications. Finally, limitations on the cell level are discussed briefly as well.

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Low‐Temperature Charging and Aging Mechanisms of Si/C Composite Anodes in Li‐Ion Batteries: An Operando Neutron Scattering Study

Cited by 44 publications

References 51 publications

Understanding Component‐Specific Contributions and Internal Dynamics in Silicon/Graphite Blended Electrodes for High‐Energy Lithium‐Ion Batteries

Understanding Component‐Specific Contributions and Internal Dynamics in Silicon/Graphite Blended Electrodes for High‐Energy Lithium‐Ion Batteries

Mechanistic Details of the Spontaneous Intercalation of Li Metal into Graphite Electrodes

Fast Charging of Lithium‐Ion Batteries: A Review of Materials Aspects

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