Elucidating the evolution of silicon anodes in lithium based batteries
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MRS Advances © 2020 Materials Research Society DOI: 10.1557/adv.2020.312
Elucidating the evolution of silicon anodes in lithium based batteries Wenzao Li,1,┼ Mallory N. Vila,1,┼ Esther S. Takeuchi,1,2,3 Kenneth J. Takeuchi,1,2 Amy C. Marschilok1,2,3,* 1
Department of Chemistry, Stony Brook University, Stony Brook, NY 11794
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Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794
3
Energy and Photon Sciences Directorate, Brookhaven National Laboratory, Upton NY 11973
┼
equal contributions by W. Li and M. Vila.
*Corresponding author: [email protected]
Silicon has attracted particular attention as a potential high capacity material for lithium based batteries. However, the application of Si-based electrodes remains challenging, in major part due to its significant irreversible energy loss during cycling. Here isothermal microcalorimetry (IMC) is demonstrated to be a precise and operando characterization method for tracking a battery’s thermal behaviour and deconvoluting the contributions from electrochemical polarization, entropy change, and parasitic reactions. Cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and x-ray powder diffraction (XRD) further elucidate the Si reactivity in conjunction with the IMC.
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INTRODUCTION Lithium ion batteries (LIBs) have shown significant success under application for consumer electronics. Nevertheless, non-negligible heat generation can reduces the useful energy density, poses a potential safety hazard and shortens battery life-time.1, 2 To avoid possible risks, advanced characterization methods should be utilized to gain a comprehensive understanding of a battery’s thermal behaviour to help mitigate unnecessary heat propagation and the associated parasitic reactions. Calorimetry through cell and component level studies has been shown to be a powerful approach to assess safety of lithium ion battery systems.3, 4 Isothermal microcalorimetry (IMC) has also been employed as a tool to characterize the evolution of 7 multiple battery systems, including Li/graphite,5 Li/Fe3O4,6, 8 9 10 Li/LiNi0.8Mn0.1Co0.1O2(NMC811), graphite/LiCoO2, and Li/Li2Ru0.75Sn0.25O3. The heat flow (instantaneous power) monitored by the IMC can be further analysed by a 3component model where the total heat flow is composed of polarization, entropic heat, and parasitic reaction heat.11 Determining the magnitude of the heat flow specifically attributable to parasitic reactions can help diagnose battery failure and provide insight on the mechanisms that contribute to limited cyclability.12 Among various electrode materials for LIBs, silicon has attracted particular attention, as it can achieve an ultrahigh theoretical electrochemical capacity (3579 mAh/g), when reaching a lithium-rich state (Li1
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