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A Commercial Conducting Polymer as Both Binder and Conductive Additive for Silicon Nanoparticle-Based Lithium-Ion Battery Negative Electrodes

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Centre for Research on Adaptive Nanostructures and Nanodevices (CRANN) & Advanced Materials Bio-Engineering Research Centre (AMBER), Trinity College Dublin, Dublin 2, Ireland
School of Physics, Trinity College Dublin, Dublin 2, Ireland
§ School of Chemistry, Trinity College Dublin, Dublin 2, Ireland
Efficient Energy Transfer Deptmartment, Bell Labs Research, Nokia, Blanchardstown Business & Technology Park, Snugborough Road, Dublin 15, Ireland
Cite this: ACS Nano 2016, 10, 3, 3702–3713
Publication Date (Web):March 3, 2016
Copyright © 2016 American Chemical Society

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    This work describes silicon nanoparticle-based lithium-ion battery negative electrodes where multiple nonactive electrode additives (usually carbon black and an inert polymer binder) are replaced with a single conductive binder, in this case, the conducting polymer PEDOT:PSS. While enabling the production of well-mixed slurry-cast electrodes with high silicon content (up to 95 wt %), this combination eliminates the well-known occurrence of capacity losses due to physical separation of the silicon and traditional inorganic conductive additives during repeated lithiation/delithiation processes. Using an in situ secondary doping treatment of the PEDOT:PSS with small quantities of formic acid, electrodes containing 80 wt % SiNPs can be prepared with electrical conductivity as high as 4.2 S/cm. Even at the relatively high areal loading of 1 mg/cm2, this system demonstrated a first cycle lithiation capacity of 3685 mA·h/g (based on the SiNP mass) and a first cycle efficiency of ∼78%. After 100 repeated cycles at 1 A/g this electrode was still able to store an impressive 1950 mA·h/g normalized to Si mass (∼75% capacity retention), corresponding to 1542 mA·h/g when the capacity is normalized by the total electrode mass. At the maximum electrode thickness studied (∼1.5 mg/cm2), a high areal capacity of 3 mA·h/cm2 was achieved. Importantly, these electrodes are based on commercially available components and are produced by the standard slurry coating methods required for large-scale electrode production. Hence, the results presented here are highly relevant for the realization of commercial LiB negative electrodes that surpass the performance of current graphite-based negative electrode systems.

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