Cycling performance of SiO_x-Si-C composite anode with different blend ratios of PAA-CMC as binder for lithium sulfur batteries

Silicon (Si) -based materials have been identified as a potential alternative anode owing to their superior theoretical capacity compared to conventional graphitic carbon. Nevertheless, the huge volume change (approximately 300%) that occurs while cycling still hampers this system from 100% practical applications. Silicon-monoxide (SiO_x)-based anode materials, on the other hand, are being explored extensively due to their unique properties such as high theoretical capacity, formation of Li₂O and LiSiO₄ during initial lithiation process that act as a natural volume buffer matrix to accommodate volume changes and formation of a stable solid electrolyte interphase layer, which improves the cyclability and capacity retention. Although poly (vinylidene fluoride) (PVdF) is widely used as a binder, the weak van der Waals forces between PVdF and silicon-based particles fail to bind particles effectively, when substantial volume change occurs. Herein, we prepare a series of SiO_x-Si-C electrodes with different binders poly (acrylic acid) (PAA), carboxyl methyl cellulose (CMC) and their blends as binder. The prepared polymeric blends are subjected to thermal, morphological, mechanical and physico-chemical analyses. The Li/ SiO_x-Si-C cell assembled with 100% PAA as binder delivered a discharge capacity of 1908 mAh g⁻¹ on its first cycle and 724 mAh g⁻¹ on its 100th cycle with a fade in capacity of 11.8 mAh g⁻¹ per cycle. Upon the incorporation of CMC in the PAA blend the cycling performance was found to be poor. Among the various investigated compositions, the electrode with sole poly (acrylic acid) as a binder offers the highest discharge capacity and this is attributed to the high concentration of the functional (carboxylic) group which forms strong hydrogen bonds with - OH groups on the SiO_x or carbon surface. The interfacial properties of the polymeric binders are thoroughly investigated by spectroscopies and electrochemical tests. Graphical abstract: (Figure presented.)