Aging in 18650-type Li-ion cells examined with neutron diffraction, electrochemical analysis and physico-chemical modeling

Paul, Neelima; Keil, Jonas; Kindermann, Frank M.; Schebesta, Sebastian; Dolotko, Oleksandr; Mühlbauer, Martin; Kraft, Ludwig; Erhard, Simon V.; Jossen, Andreas; Gilles, Ralph

doi:10.1016/j.est.2018.03.016

Cited by 29 publications

(21 citation statements)

References 61 publications

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“…The loss of cyclable Lih as also been observed for other cells withoutS i compound in the anode. [39][40][41][42][43][44] Therefore, ap art of the capacity loss in the cells was likely to originate from the growth of a solid electrolyte interphase (SEI) layer on the graphite particles in addition to the aging effect of the Si compound;h owever,a large part of the film growth and the low coulombic efficiency can most likely be attributed to the formation of Li silicates.…”

Section: Relaxationmechanism After Charging In Fresh Cellsmentioning

confidence: 99%

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

et al. 2019

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The addition of Si compounds to graphite anodes has become an attractive way of increasing the practical specific energies in Li‐ion cells. Previous studies involving Si/C anodes lacked direct insight into the processes occurring in full cells during low‐temperature operation. In this study, a powerful combination of operando neutron diffraction, electrochemical tests, and post‐mortem analysis is used for the investigation of Li‐ion cells. 18650‐type cylindrical cells in two different aging states are investigated by operando neutron diffraction. The experiments reveal deep insights and important trends in low‐temperature charging mechanisms involving intercalation, alloying, Li metal deposition, and relaxation processes as a function of charging C‐rates and temperatures. Additionally, the main aging mechanism caused by long‐term cycling and interesting synergistic effects of Si and graphite are elucidated.

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Section: Relaxationmechanism After Charging In Fresh Cellsmentioning

confidence: 99%

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

et al. 2019

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“…Additionally, neutrons, having significantly higher penetration depth than X‐rays, can also be used to study LiBs. [ 39–47 ] Recent developments in neutron diffraction imaging techniques, such as neutron diffraction computed tomography (ND‐CT) and direct/real space neutron diffraction imaging, [ 48–51 ] have shown that neutron diffraction can be considered as a powerful characterization tool for ex situ measurements.…”

Section: Introductionmentioning

confidence: 99%

Cycling Rate‐Induced Spatially‐Resolved Heterogeneities in Commercial Cylindrical Li‐Ion Batteries

et al. 2021

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Synchrotron high‐energy X‐ray diffraction computed tomography has been employed to investigate, for the first time, commercial cylindrical Li‐ion batteries electrochemically cycled over the two cycling rates of C/2 and C/20. This technique yields maps of the crystalline components and chemical species as a cross‐section of the cell with high spatiotemporal resolution (550 × 550 images with 20 × 20 × 3 µm3 voxel size in ca. 1 h). The recently developed Direct Least‐Squares Reconstruction algorithm is used to overcome the well‐known parallax problem and led to accurate lattice parameter maps for the device cathode. Chemical heterogeneities are revealed at both electrodes and are attributed to uneven Li and current distributions in the cells. It is shown that this technique has the potential to become an invaluable diagnostic tool for real‐world commercial batteries and for their characterization under operating conditions, leading to unique insights into “real” battery degradation mechanisms as they occur.

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“…However, none of these techniques directly monitor lithium ions. Although neutron diffraction is a promising non-destructive probe, it fails to observe local regions in the cell [16,17]. The present Compton scattering based approach thus offers advantages over other methods in probing the structure of commercial large-scale cells non-destructively.…”

Section: Introductionmentioning

confidence: 97%

High-Energy X-Ray Compton Scattering Imaging of 18650-Type Lithium-Ion Battery Cell

et al. 2019

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High-energy synchrotron X-ray Compton scattering imaging was applied to a commercial 18650-type cell, which is a cylindrical lithium-ion battery in wide current use. By measuring the Compton scattering X-ray energy spectrum non-destructively, the lithiation state in both fresh and aged cells was obtained from two different regions of the cell, one near the outer casing and the other near the center of the cell. Our technique has the advantage that it can reveal the lithiation state with a micron-scale spatial resolution even in large cells. The present method enables us to monitor the operation of large-scale cells and can thus accelerate the development of advanced lithium-ion batteries.

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Aging in 18650-type Li-ion cells examined with neutron diffraction, electrochemical analysis and physico-chemical modeling

Cited by 29 publications

References 61 publications

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

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

Cycling Rate‐Induced Spatially‐Resolved Heterogeneities in Commercial Cylindrical Li‐Ion Batteries

High-Energy X-Ray Compton Scattering Imaging of 18650-Type Lithium-Ion Battery Cell

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