Three-dimensional characterization of electrodeposited lithium microstructures using synchrotron X-ray phase contrast imaging

Eastwood, David S.; Bayley, Paul M.; Chang, Hee Jung; Taiwo, Oluwadamilola O.; Vila‐Comamala, Joan; Brett, Dan J. L.; Rau, Christoph; Withers, Philip J.; Shearing, Paul R.; Grey, Clare P.; Lee, Peter

doi:10.1039/c4cc03187c

Cited by 137 publications

(103 citation statements)

References 23 publications

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“…Dendrites can be thought of as fractal (16), and hence this macroscopic shape is expected to be representative of the dendrite shape on the microscopic scale. The chosen structure resembles sections of lithium microstructures seen in SEM (15) and X-ray phasecontrast imaging (17).…”

Section: Resultsmentioning

confidence: 99%

Real-time 3D imaging of microstructure growth in battery cells using indirect MRI

Ilott

Mohammadi

Chang

et al. 2016

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

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127

102

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Lithium metal is a promising anode material for Li-ion batteries due to its high theoretical specific capacity and low potential. The growth of dendrites is a major barrier to the development of high capacity, rechargeable Li batteries with lithium metal anodes, and hence, significant efforts have been undertaken to develop new electrolytes and separator materials that can prevent this process or promote smooth deposits at the anode. Central to these goals, and to the task of understanding the conditions that initiate and propagate dendrite growth, is the development of analytical and nondestructive techniques that can be applied in situ to functioning batteries. MRI has recently been demonstrated to provide noninvasive imaging methodology that can detect and localize microstructure buildup. However, until now, monitoring dendrite growth by MRI has been limited to observing the relatively insensitive metal nucleus directly, thus restricting the temporal and spatial resolution and requiring special hardware and acquisition modes. Here, we present an alternative approach to detect a broad class of metallic dendrite growth via the dendrites' indirect effects on the surrounding electrolyte, allowing for the application of fast 3D 1 H MRI experiments with high resolution. We use these experiments to reconstruct 3D images of growing Li dendrites from MRI, revealing details about the growth rate and fractal behavior. Radiofrequency and static magnetic field calculations are used alongside the images to quantify the amount of the growing structures.Li-ion batteries | in situ MRI | dendrite growth L ithium metal is a promising anode material for secondary lithium batteries because it has the highest theoretical specific capacity of possible anode materials (3,860 mAh/g), and the most negative voltage. The metal's use is currently limited due to irregular microstructure buildup on the electrode during charging (1). These mossy, needle-like, or dendritic structures severely compromise battery performance and can eventually penetrate the separator and cause overheating and short circuiting, thus presenting serious safety concerns. Preventing dendrite growth has proven to be extremely challenging, due in part to the current poor understanding of the conditions under which the dendrites' growth is initiated and the factors that contribute to their continued growth (2, 3). The development of new analytical techniques that are sensitive to dendrite growth and amenable to studying electrochemical cells in situ is crucial to future efforts of improving battery designs and performance (4, 5).In situ NMR spectroscopy and MRI are powerful noninvasive methods that can provide time-resolved and quantitative information about the changes within the electrolyte and the electrodes. NMR measurements are sensitive to dendrite growth and are also able to resolve different lithium microstructure morphologies through chemical shift measurements (6-9). MRI approaches provide additional spatial information, allowing specific structural changes ...

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Section: Resultsmentioning

confidence: 99%

Real-time 3D imaging of microstructure growth in battery cells using indirect MRI

Ilott

Mohammadi

Chang

et al. 2016

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

Self Cite

127

102

View full text Add to dashboard Cite

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“…Harry et al 4 first used synchrotron-based X-ray CT to image metallic Li microstructures in Li-polymer cells, demonstrating the role of subsurface dendritic structures within a Li metal electrode in the failure of lithium batteries. With bespoke Li/Li symmetrical cells, Eastwood et al 23 used synchrotron X-ray phase contrast imaging to characterise different forms of Li microstructures. In this previous study, Eastwood et al were able to distinguish between mossy metallic Li microstructures from high surface area lithium salt deposits by their contrasting X-ray attenuation.…”

Section: Introductionmentioning

confidence: 99%

Investigating the evolving microstructure of lithium metal electrodes in 3D using X-ray computed tomography

Taiwo

Finegan

Paz‐Garcia

et al. 2017

Phys. Chem. Chem. Phys.

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The growth of electrodeposited lithium microstructures on metallic lithium electrodes has prevented their use in rechargeable lithium batteries due to early performance degradation and safety implications. Understanding the evolution of lithium microstructures during battery operation is crucial for the development of an effective and safe rechargeable lithium-metal battery. This study employs both synchrotron and laboratory X-ray computed tomography to investigate the morphological evolution of the surface of metallic lithium electrodes during a single cell discharge and over numerous cycles, respectively. The formation of surface pits and the growth of mossy lithium deposits through the separator layer are characterised in threedimensions. This has provided insight into the microstructural evolution of lithium--metal electrodes during rechargeable battery operation, and further understanding of the importance of separator architecture in mitigating lithium dendrite growth.

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“…The field of view (FoV) Morphological characterization of Li/Li-1 cell and electrochemical characterization of Li/Li-2 cell A cross-sectional X-ray tomographic slice of the uncycled Li/Li-1 cell is shown in Figure 2c, in which the two Li electrodes and the separator are clearly discernable due to the partially light and partially dark boundaries between them arising from in-line phase contrast. 42,53 The interface between the Li electrode and the separator of Li/Li-1 cell is flat and gapless. The Li/Li-2 cell was galvanostatically "cycled" until an internal short circuit occurred.…”

mentioning

confidence: 99%

Study of the Mechanisms of Internal Short Circuit in a Li/Li Cell by Synchrotron X-ray Phase Contrast Tomography

et al. 2016

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Knowledge about degradation and failure of Li-ion batteries (LIBs) is of paramount importance especially because failure can be accompanied by severe hazards. To contribute to the understanding of such phenomena synchrotron in-line phase contrast Xray tomography was employed to investigate internal cell deformation and degradation caused by an internal short circuit (ISC). The tomographic images taken from an uncycled Li/Li cell and a short-circuited Li/Li cell reveal how lithium microstructures (LmS) develop during electrochemical stripping and plating during discharge and charge and how the three-layer separator used is damaged by growing LmSs and delaminates and melts as a consequence of an ISC. Previously unknown insights into the internal cell degradation and deformation mechanisms caused by an ISC are obtained and provide hints of how the properties of the separator could be modified in order to improve the reliability and safety of current and next-generation LIBs.

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Three-dimensional characterization of electrodeposited lithium microstructures using synchrotron X-ray phase contrast imaging

Cited by 137 publications

References 23 publications

Real-time 3D imaging of microstructure growth in battery cells using indirect MRI

Real-time 3D imaging of microstructure growth in battery cells using indirect MRI

Investigating the evolving microstructure of lithium metal electrodes in 3D using X-ray computed tomography

Study of the Mechanisms of Internal Short Circuit in a Li/Li Cell by Synchrotron X-ray Phase Contrast Tomography

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