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

Nature Energy volume 1, Article number: 16097 (2016) Cite this article

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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.

Lithium-ion batteries are the most advanced devices for portable energy storage and are making their way into the electric vehicle market1,2,3. Many studies focus on discovering new materials to compete with the ones already in use in commercial devices4,5,6. A step change approach consists of enhancing the battery performance by improving only the design of the electrodes without changing the underlying materials chemistry.

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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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Author notes

  1. Juliette Billaud and Florian Bouville: These authors contributed equally to this work.

Authors and Affiliations

  1. Paul Scherrer Institut, Electrochemical Laboratory, CH-5232 Villigen PSI, Switzerland

    Juliette Billaud & Claire Villevieille

  2. Department of Materials, Complex Materials, ETH Zürich, CH-8093 Zürich, Switzerland

    Florian Bouville, Tommaso Magrini & André R. Studart

Authors
  1. Juliette Billaud
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  4. Claire Villevieille
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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.

Supplementary information

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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