Towards Scalable Binderless Electrodes: Carbon Coated Silicon Nanofiber Paper via Mg Reduction of Electrospun SiO2 Nanofibers

The need for more energy dense and scalable Li-ion battery electrodes has become increasingly pressing with the ushering in of more powerful portable electronics and electric vehicles (EVs) requiring substantially longer range capabilities. Herein, we report on the first synthesis of nano-silicon paper electrodes synthesized via magnesiothermic reduction of electrospun SiO2 nanofiber paper produced by an in situ acid catalyzed polymerization of tetraethyl orthosilicate (TEOS) in-flight. Free-standing carbon-coated Si nanofiber binderless electrodes produce a capacity of 802 mAh g(-1) after 659 cycles with a Coulombic efficiency of 99.9%, which outperforms conventionally used slurry-prepared graphite anodes by over two times on an active material basis. Silicon nanofiber paper anodes offer a completely binder-free and Cu current collector-free approach to electrode fabrication with a silicon weight percent in excess of 80%. The absence of conductive powder additives, metallic current collectors, and polymer binders in addition to the high weight percent silicon all contribute to significantly increasing capacity at the cell level.