Disruption in the restacking of the graphene present in the electrodes could hamper the reduction in the conductivity and also the surface area, which may be a good reason why graphene has not yet performed as predicted. In this research, we employed the scalable electrophoretic deposition (EPD) procedure to make instantly a binder-free Li-ion battery cathode, consisting of LiNi0.8Mn0.1Co0.1O2 (NMC811), sulfonated reduced graphene oxide (SRGO) sheets, and carbon black (CB) particles. The EPD process caused a squeezing force, which not only wrapped the SRGO sheets around the NMC811 nanoparticles, but also inserted the CB particles into the composite in an electrostatically stabilized combination. As evidenced by the electrochemical measurements, the binder-free NMC/SRGO/CB electrode manifested better cycling performance at the current density of 0.2 C, where this electrode delivered discharge capacities of 170.3 and 143.7 mAh g−1, respectively, at the 1st and 200th cycle compared to discharge capacities of 162.3 and 122.6 mAh g−1 acquired for the NMC/SRGO electrode. The excellent cycle stability and rate capability of the optimized binder-free NMC/SRGO/CB cathode can be attributed to withstanding the volume expansion of the active particles during cycling due to wrapping graphene sheets, inhibition of the restacking of graphene sheets by sulfonated groups and CB spacers, electrostatic interaction between sulfonated groups and lithium ions, and efficient electrolyte infiltration by ion and electron conductive channels in the binder-free cathode structure.
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