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Calendar aging of silicon-containing batteries

Abstract

High-energy batteries for automotive applications require cells to endure well over a decade of constant use, making their long-term stability paramount. This is particularly challenging for emerging cell chemistries containing silicon, for which extended testing information is scarce. While much of the research on silicon anodes has focused on mitigating the consequences of volume changes during cycling, comparatively little is known about the time-dependent degradation of silicon-containing batteries. Here we discuss a series of studies on the reactivity of silicon that, collectively, paint a picture of how the chemistry of silicon exacerbates the calendar aging of lithium-ion cells. Assessing and mitigating this shortcoming should be the focus of future research to fully realize the benefits of this battery technology.

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Fig. 1: Performance gap in the calendar life of Si cells.
Fig. 2: Mechanisms of long-term performance fade in Si-containing cells due to Si and SEI reactivity.
Fig. 3: Visualizing SEI reactivity in Si-containing and Si-free cells.
Fig. 4: Promising strategies to address calendar aging of Si electrodes.

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Acknowledgements

This research was supported by the US Department of Energy (DOE)’s Vehicle Technologies Office under the Silicon Consortium Project. This work was conducted in part by the Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the DOE under contract no. DE-AC36-08GO28308. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (‘Argonne’). Argonne, a US DOE Office of Science laboratory, is operated under contract no. DE-AC02-06CH11357. This manuscript has been authored by UT-Battelle, LLC, under contract no. DE-AC05-00OR22725 with the US DOE. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the US DOE’s National Nuclear Security Administration under contract DE-NA0003525. Lawrence Berkeley National Laboratory is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US DOE under contract no. DE-AC02-05CH11231. The views expressed in the article do not necessarily represent the views of the DOE or the US Government. The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for US Government purposes.

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Correspondence to Christopher S. Johnson.

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Peer review information Nature Energy thanks Jun-Tao Li and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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McBrayer, J.D., Rodrigues, MT.F., Schulze, M.C. et al. Calendar aging of silicon-containing batteries. Nat Energy 6, 866–872 (2021). https://doi.org/10.1038/s41560-021-00883-w

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