Silicon has attracted ever-increasing attention as a high-capacity anode material in Li-ion batteries owing to its extremely high theoretical capacity. However, practical application of silicon anodes is seriously hindered by its fast capacity fading as a result of huge volume changes during the charge/discharge process. Here, an interpenetrated gel polymer binder for high-performance silicon anodes is created through in-situ crosslinking of water-soluble poly(acrylic acid) (PAA) and polyvinyl alcohol (PVA) precursors. This gel polymer binder with deformable polymer network and strong adhesion on silicon particles can effectively accommodate the large volume change of silicon anodes upon lithiation/delithiation, leading to an excellent cycling stability and high Coulombic efficiency even at high current densities. Moreover, high areal capacity of ∼4.3 mAh/cm2 is achieved based on the silicon anode using the gel PAA–PVA polymer binder with a high mass loading. In view of simplicity in using the water soluble gel polymer binder, it is believed that this novel binder has a great potential to be used for high capacity silicon anodes in next generation Li-ion batteries, as well as for other electrode materials with large volume change during cycling.

Interpenetrated Gel Polymer Binder for High Performance Silicon Anodes in Lithium-Ion Batteries

Author(s): Liu, G; Zheng, H; Song, X; Battaglia, VS | Abstract: This paper investigates lithium-ion electrode laminates as polymer composites to explain their performance variation due to changes in formulation. There are three essential components in a positive electrode laminate: active material (AM) particles, acetylene black (AB) particles, and the polymer binder. The high filler content and discrete particle sizes make the electrode laminate a very unique polymer composite. This work introduces a physical model in which AB and AM particles compete for polymer binder, which forms fixed layers of polymer on their surfaces. This competition leads to the observed variations in electrode morphology and performance for different electrode formulations. The electronic conductivities of the cathode laminates were measured and compared to an effective conductivity calculation based on the physical model to probe the interaction among the three components to reveal the critical factors controlling electrode conductivity and electrochemical performance. The data and effective conductivity calculation results agree very well with each other. This developed physical model provides a theoretical guideline for optimization of electrode composition for most polymer binder-based Li-ion battery electrodes. © 2012 The Electrochemical Society.

http://ma.ecsdl.org/content/MA2012-01/9/529.full.pdf

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