Synthesis and Extreme Rate Capability of Si–Al–C–N Functionalized Carbon Nanotube Spray-on Coatings as Li-Ion Battery Electrode

Silicon-based precursor derived glass-ceramics or PDCs have proven to be an attractive alternative anode material for Li ion batteries. Main challenges associated with PDC anodes are their low electrical conductivity, first cycle loss, and meager C-rate performance. Here, we show that thermal conversion of single source aluminum-modified polysilazane on the surfaces of carbon nanotubes (CNTs) results in a robust Si-Al-C-N/CNT shell/core composite that offers extreme C-rate capability as battery electrode. Addition of Al to the molecular network of Si-C-N improved electrical conductivity of Si-C-N by 4 orders of magnitude, while interfacing with CNTs showed 7-fold enhancement. Further, we present a convenient spray-coating technique for PDC composite electrode preparation that eliminates polymeric binder and conductive agent there-by reducing processing steps and eradicating foreign material in the electrode. The Si-Al-C-N/CNT electrode showed stable charge capacity of 577 mAh g(-1) at 100 mA g(-1) and a remarkable 400 mAh g(-1) at 10,000 mA g(-1), which is the highest reported value for a silazane derived glass-ceramic or nanocomposite electrode. Under symmetric cycling conditions, a high charge capacity of ∼350 mA g(-1) at 1600 mA g(-1) was continuously observed for over 1000 cycles.