Silicon is capable of delivering a high theoretical specific capacity of 3579 mAh g â1 which is about 10 times higher than that of the state-of-the-art graphite based negative electrodes for lithium-ion batteries. However, the poor cycle life of silicon electrodes, caused by the large volumetric strain during cycling, limits the commercialization of silicon electrodes. As one of the essential components, the polymeric binder is critical to the performance and durability of lithium-ion batteries as it keeps the integrity of electrodes, maintains conductive path and must be stable in the electrolyte. In this work, we demonstrate that electrodes consisting of silicon nanoparticles mixed with commercially available Nafion and ion-exchanged Nafion can maintain a high specific capacity over 2000 mAh g â1 cycled between 1.0 V and 0.01 V. For comparison, the capacity of electrodes made of the same silicon nanoparticles mixed with a traditional binder, polyvinylidene fluoride (PVDF), fades rapidly. In addition, stable cycling at 1C rate for more than 500 cycles is achieved by limiting the lithiation capacity to 1200 mAh g There is an intense effort worldwide to develop new electrode materials for lithium-ion batteries (LIBs) to satisfy future high power and energy density applications. Silicon can provide theoretical capacity up to 3579 mAh g â1 (based on Li 15 Si 4 ), which is about ten times higher than that of graphite electrode. 1 Resulting from large volume changes as lithium goes into and out of silicon, cracking and pulverization of Si electrodes can cause the loss of electrical contact and new solid electrolyte interphase (SEI) formation on exposed surface, leading to rapid capacity fade. Novel binders and nanostructured silicon are two general approaches to improve the durability and performance of silicon electrodes.For commercial LIBs, electrodes are composed of three essential components, which are active material, conductive additive and binder. The fundamental role of binder is to keep the electrode mechanically intact and adhered well to the current collector. Other ideal characteristics of binders include electrochemical stability over wide potential range, high melting point, low swelling rate in nonaqueous electrolyte, high lithium ionic conductivity, high electrical conductivity, capability to sustain volume change of active material particles, and good manufacturability.2-4 Today, polyvinylidene fluoride (PVDF, monomer -CH 2 -CF 2 -) and styrene butadiene rubber (SBR) are commonly used as binders for graphite anodes, and PVDF and polytetrafluoroethylene (PTFE, monomer -CF 2 -CF 2 -) can be used as binders for cathodes.
2PVDF is known to perform poorly for high energy density electrode materials, such as silicon, because it fails to accommodate the large volume change during lithiation and delithiation. 5,6 Presently, there is much interest in developing effective binders for siliconbased electrodes. Crosslinked elastomeric polymer (PVDF + tetrafluoroethylene + propylene) was shown to maintain good cap...