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7Li MRI of Li batteries reveals location of microstructural lithium

Abstract

There is an ever-increasing need for advanced batteries for portable electronics, to power electric vehicles and to facilitate the distribution and storage of energy derived from renewable energy sources1,2. The increasing demands on batteries and other electrochemical devices have spurred research into the development of new electrode materials that could lead to better performance and lower cost (increased capacity, stability and cycle life, and safety)1,2,3. These developments have, in turn, given rise to a vigorous search for the development of robust and reliable diagnostic tools to monitor and analyse battery performance, where possible, in situ4,5,6,7,8,9. Yet, a proven, convenient and non-invasive technology, with an ability to image in three dimensions the chemical changes that occur inside a full battery as it cycles, has yet to emerge. Here we demonstrate techniques based on magnetic resonance imaging, which enable a completely non-invasive visualization and characterization of the changes that occur on battery electrodes and in the electrolyte. The current application focuses on lithium-metal batteries and the observation of electrode microstructure build-up as a result of charging. The methods developed here will be highly valuable in the quest for enhanced battery performance and in the evaluation of other electrochemical devices.

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Figure 1: Schematic representations of a bag-cell battery and one-dimensional 7Li NMR spectra in the pristine and charged states.
Figure 2: 7Li magnetic resonance and SEM images of Li microstructure formation in Li bag cells.
Figure 3: Three-dimensional MRI images of the Li-metal bag cells.
Figure 4: 7Li chemical-shift images of the Li-metal bag cell.

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Acknowledgements

We would like to thank R. Bhattacharrya, B. Key and L. Zhou for their help in the initial stages to this project. Research was carried out as part of the NECCES, an Energy Frontier Research Center funded by the US Department of Energy, Office of Basic Energy Sciences, under award DE-SC0001294. We thank the US National Science Foundation (and grant CMI 0957586) for summer salary for A.J.

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Contributions

S.C., N.M.T. and H.J.C. carried out experiments, N.M.T. and H.J.C. prepared samples, S.C. and A.J. carried out data processing, S.C., L-S.D. and H.J.C. prepared figures and S.C., N.M.T., C.P.G. and A.J. wrote the manuscript. All authors analysed and discussed the results.

Corresponding authors

Correspondence to Clare P. Grey or Alexej Jerschow.

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The authors declare no competing financial interests.

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Chandrashekar, S., Trease, N., Chang, H. et al. 7Li MRI of Li batteries reveals location of microstructural lithium. Nature Mater 11, 311–315 (2012). https://doi.org/10.1038/nmat3246

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