Tuning the hierarchical pore structure of graphene oxide through dual thermal activation for high-performance supercapacitor

Herein, we introduce a simple method to prepare hierarchical graphene with a tunable pore structure by activating graphene oxide (GO) with a two-step thermal annealing process. First, GO was treated at 600 °C by rapid thermal annealing in air, followed by subsequent thermal annealing in N₂. The prepared graphene powder comprised abundant slit nanopores and micropores, showing a large specific surface area of 653.2 m²/g with a microporous surface area of 367.2 m²/g under optimized conditions. The pore structure was easily tunable by controlling the oxidation degree of GO and by the second annealing process. When the graphene powder was used as the supercapacitor electrode, a specific capacitance of 372.1 F/g was achieved at 0.5 A/g in 1 M H₂SO₄ electrolyte, which is a significantly enhanced value compared to that obtained using activated carbon and commercial reduced GO. The performance of the supercapacitor was highly stable, showing 103.8% retention of specific capacitance after 10,000 cycles at 10 A/g. The influence of pore structure on the supercapacitor performance was systematically investigated by varying the ratio of micro- and external surface areas of graphene.