EPR Imaging of Metallic Lithium and its Application to Dendrite Localisation in Battery Separators

Niemöller, Arvid; Jakes, Peter; Eichel, Rüdiger‐A.; Granwehr, Josef

doi:10.1038/s41598-018-32112-y

Cited by 48 publications

(58 citation statements)

References 43 publications

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“…MRI is a powerful tool for studying chemical, biological, and solid-state phenomena (5)(6)(7)(8). Recently, in situ MRI of model electrochemical devices shed light on underlying physical and mechanistic processes (9)(10)(11)(12)(13)(14)(15)(16). These techniques however could not be used to study commercial cells due to the conductive casings and small distances between electrodes, which hamper radiofrequency (RF) penetration.…”

mentioning

confidence: 99%

Distortion-free inside-out imaging for rapid diagnostics of rechargeable Li-ion cells

Romanenko

Jerschow

2019

Proc. Natl. Acad. Sci. U.S.A.

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Safety risks associated with modern high energy-dense rechargeable cells highlight the need for advanced battery screening technologies. A common rechargeable cell exposed to a uniform magnetic field creates a characteristic field perturbation due to the inherent magnetism of electrochemical materials. The perturbation pattern depends on the design, state of charge, accumulated mechanical defects, and manufacturing flaws of the device. The quantification of the induced magnetic field with MRI provides a basis for noninvasive battery diagnostics. MRI distortions and rapid signal decay are the main challenges associated with strongly magnetic components present in most commercial cells. These can be avoided by using Single-Point Ramped Imaging with T1 enhancement (SPRITE). The method is immune to image artifacts arising from strong background gradients and eddy currents. Due to its superior image quality, SPRITE is highly sensitive to defects and the state of charge distribution in commercial Li-ion cells.

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mentioning

confidence: 99%

Distortion-free inside-out imaging for rapid diagnostics of rechargeable Li-ion cells

Romanenko

Jerschow

2019

Proc. Natl. Acad. Sci. U.S.A.

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“…Previous EPR investigations showed that the lineshape, linewidth and integrated intensity were highly dependent on the morphology of metallic lithium 6,7,9 . The EPR spectrum lineshape of a metallic conductor is indeed controlled by the limited penetration depth δ mw of the microwave field in the metal, known as the skin effect 10 :…”

Section: Resultsmentioning

confidence: 97%

“…In continuation of the latter an extensive study by operando EPR spectroscopy was performed for Li plating on graphite 8 . Niemöller et al also studied, ex situ, the potential and limitations of ex situ EPR imaging (EPRI) on metallic Li 9 .…”

mentioning

confidence: 99%

Monitoring metallic sub-micrometric lithium structures in Li-ion batteries by in situ electron paramagnetic resonance correlated spectroscopy and imaging

et al. 2021

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Monitoring the formation of dendrites or filaments of lithium is of paramount importance for Li-based battery technologies, hence the intense activities in designing in situ techniques to visualize their growth. Herein we report the benefit of correlating in situ electron paramagnetic resonance (EPR) spectroscopy and EPR imaging to analyze the morphology and location of metallic lithium in a symmetric Li/LiPF6/Li electrochemical cell during polarization. We exploit the variations in shape, resonance field and amplitude of the EPR spectra to follow, operando, the nucleation of sub-micrometric Li particles (narrow and symmetrical signal) that conjointly occurs with the fragmentation of bulk Li on the opposite electrode (asymmetrical signal). Moreover, in situ EPR correlated spectroscopy and imaging (spectral-spatial EPR imaging) allows the identification (spectral) and localization (spatial) of the sub-micrometric Li particles created by plating (deposition) or stripping (altered bulk Li surface). We finally demonstrate the possibility to visualize, via in situ EPR imaging, dendrites formed through the separator in the whole cell. Such a technique could be of great help in mastering the Li-electrolyte interface issues that plague the development of solid-state batteries.

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“…Neimöller et al used CEPR to study dendrite growth on separator. [212] They explained how the EPR line shape serves to distinguish different kinds of Li morphologies. EPR of conductive samples are influenced by the skin effect, which leads to a depth dependent attenuation and sample thickness dependent phase shift of the EPR signal [211,213] .…”

Section: Electron Paramagnetic Resonancementioning

confidence: 99%

“…Reproduced from Neimöller et al Scientific Reports, 8, 14331 (2018). [212] . (CC BY, https://creativecommons.org/licenses/by/4.0)…”

Section: Electron Paramagnetic Resonancementioning

confidence: 99%

Lithium Plating Detection Methods in Lithium-Ion Batteries

2020

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Lithium-ion batteries provide a low-cost, long cycle-life and high energy density solution to the expediting energy requirement of the automotive industry. There is a growing need of fast charging batteries for commercial application. However, large charging currents may cause Lithium plating which describes the deposition of metallic Lithium at the anode surface. It takes place at conditions of high currents and/or low temperatures because of kinetic limitations. The main reason behind plating is the slow solid-state diffusion of Lithium ions inside the active material. If the anode surface potential falls below 0 V versus Li/Li+, the formation of metallic Lithium is thermodynamically feasible. To avoid or reduce the amount Lithium plating, it is essential to detect its onset during a charging event. Determination of accurate Lithium plating curve is crucial in estimating the boundary conditions for battery operation without compromising life and safety. There are various data analysis methods involved in deriving the Lithium plating curve: anode potential using a three-electrode cell, variation of relaxation voltage after charging (dV/dt), variation of accumulated charge with voltage (dQ/dV) and coulombic efficiency of charge/discharge with %SOC (state of charge) are more commonly employed techniques. In addition to these methods, estimation of its occurrence is typically underpinned by electrochemical models where the negative (anode) electrode potential is expressed by a set of partial differential equations based on the electrochemical and physical properties of the battery components such as the electrodes and electrolyte. The present paper reviews the common test methods and analysis that are currently utilized in Lithium plating determination. Knowledge gaps are identified, and recommendations are made for the future development in the determination and verification of Lithium plating curve in terms of modelling and analysis.

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EPR Imaging of Metallic Lithium and its Application to Dendrite Localisation in Battery Separators

Cited by 48 publications

References 43 publications

Distortion-free inside-out imaging for rapid diagnostics of rechargeable Li-ion cells

Distortion-free inside-out imaging for rapid diagnostics of rechargeable Li-ion cells

Monitoring metallic sub-micrometric lithium structures in Li-ion batteries by in situ electron paramagnetic resonance correlated spectroscopy and imaging

Lithium Plating Detection Methods in Lithium-Ion Batteries

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