Chemically Active Reduced Graphene Oxide with Tunable C/O Ratios

Organic dispersions of graphene oxide can be thermally reduced in polar organic solvents under reflux conditions to afford electrically conductive, chemically active reduced graphene oxide (CARGO) with tunable C/O ratios, dependent on the boiling point of the solvent. The reductions are achieved after only 1 h of reflux, and the corresponding C/O ratios do not change upon further thermal treatment. Hydroxyl and carboxyl groups can be removed when the reflux is carried out above 155 °C, while epoxides are removable only when the temperature is higher than 200 °C. The increasing hydrophobic nature of CARGO, as its C/O ratio increases, improves the dispersibility of the nanosheets in a polystyrene matrix, in contrast to the aggregates formed with CARGO having lower C/O ratios. The excellent processability of the obtained CARGO dispersions is demonstrated via free-standing CARGO papers that exhibit tunable electrical conductivity/chemical activity and can be used as lithium-ion battery anodes with enhanced Coulombic efficiency.