Engineering Polymer-Assisted Self-Assembly Process for High-Capacity and Cycle-Stable Si-on-Graphite Anode of Li-Ion Batteries

Abstract

A facile and ready for scale-up process based on polymer-assisted solution self-assembly is developed for manufacturing high-capacity and cycle-stable silicon-on-graphite (Si@G) lithium-ion battery anode materials. The process involves first coating a polyelectrolyte poly(diallyldimethylammonium chloride, anchored by a cross-linked polyvinyl alcohol-glutaraldehyde matrix, onto micron-sized graphite particles using spray-drying. Process optimization succeeds in imparting the graphite particles with a permanent high positive zeta potential (>40 mV), which enables attracting Si nanoparticles (NPs) (zeta potential= -28.5 mV) uniformly and firmly onto the graphite surfaces in water. Collected by filtration, the resulting Si@G composite particles are finally subjected to a high-temperature (1000 oC) treatment in Ar to turn the polymer coating into a carbon layer, which engulfs the Si NPs. A Si@G composite powder containing nearly 7 wt.% Si and produced in a batch size of approximately 20 gram is demonstrated to have a high specific capacity of 605 mAh g-1, a remarkable cycle stability showing only 11% capacity loss after 300 cycles and notably high coulombic efficiencies comparable to those of a graphite electrode upon cycling. The designed polymer coating realizes charge-carrying graphite particle without damaging its surface structure and eventually leads to a surface carbon layer that prevents Si NP detachment, improves powder conductivity, and mitigates solid-electrolyte-interphase formation.