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Magnetically aligned graphite electrodes for high-rate performance Li-ion batteries

A Corrigendum to this article was published on 10 April 2017

Abstract

As lithium-ion batteries become ubiquitous, the energy storage market is striving for better performance, longer lifetime and better safety of the devices. This race for performance is often focused on the search for new materials, whereas less effort has been dedicated to the electrode engineering. Enhancing the power density by increasing the amount of active material remains impractical since it impinges the transport of ions across the electrode during the charging and discharging processes. Here, we show that the electrochemical performance of a battery containing a thick (about 200 μm), highly loaded (about 10 mg cm−2) graphite electrode can be remarkably enhanced by fabricating anodes with an out-of-plane aligned architecture using a low external magnetic field. The lower tortuosity resulting from such a simple and scalable magnetic alignment approach leads to a specific charge up to three times higher than that of non-architectured electrodes at a rate of 1C.

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Figure 1: Functionalization of the graphite flakes and electrode fabrication.
Figure 2: Effect of the magnetic field on the orientation of graphite flakes.
Figure 3: 3D architectures of aligned and reference graphite electrodes.
Figure 4: Electrochemical performance of aligned and reference electrodes.
Figure 5: Capacity retention in highly loaded electrodes.

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Acknowledgements

A.R.S. and F.B. acknowledge the financial support of the ETH Zürich and the Swiss National Science Foundation (grant 200020_146509). We are indebted to A. G. Bittermann and the Center for Optical and Electron microscopy of ETH Zürich (ScopeM) for the FIB-tomography measurement. Acknowledgements are also due to P. Novàk and N. Kränzlin for the XRD measurements, E. Maire for his contributions to the image analysis, D. Marinha for insightful discussions on ionic conductivity, and D. Billaud for sharing his knowledge on insertion compounds and ideas.

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Contributions

Experiments were designed by J.B., F.B., T.M., C.V., A.R.S. and conducted by J.B., F.B. and T.M. T.M. and J.B. developed the slurry composition. T.M. and F.B. developed the set-up and casting method. T.M. cast the electrodes for each test. J.B. prepared the cells for the electrochemical characterization and performed all the measurements and data processing. F.B. carried out the image analysis and FIB-tomography processing. J.B., F.B. and T.M. drafted the manuscript and figures. All authors discussed the results, their implications and revised the manuscript at all stages.

Corresponding authors

Correspondence to Claire Villevieille or André R. Studart.

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The authors declare no competing financial interests.

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Supplementary Information

Supplementary Figures 1–10, Supplementary Table 1, Supplementary Notes, Supplementary Methods, Supplementary References. (PDF 6191 kb)

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Billaud, J., Bouville, F., Magrini, T. et al. Magnetically aligned graphite electrodes for high-rate performance Li-ion batteries. Nat Energy 1, 16097 (2016). https://doi.org/10.1038/nenergy.2016.97

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