Heteroatoms-doped hierarchically porous graphene as electrode material for supercapacitors with ultra-high capacitance

In this work, a dual-templating pyrolysis strategy is successfully developed to synthesize a highly crumpled graphene (N-TRPG-800). The achievement of the graphene is based on the carbonization of the d(+)-glucosamine hydrochloride and the spatial confinement effect of the graphitic carbon nitride (g-C3N4) in the presence of zinc nanoparticles (Zn NPs). During the pyrolysis process, the d(+)-glucosamine hydrochloride first polymerizes into the layers of g-C3N4, which is derived from melamine. Afterwards, a further increase in pyrolysis temperature leads to the decomposition of g-C3N4 and the generation of reducing NH3 gas, which eventually resulting in the formation of 2D ultrathin structure and high heteroatoms doping degree. Simultaneously, the volatilization of the Zn NPs also plays a key role in the pore formation and the hierarchical structure generation. As a result, the as-synthesized graphene sheets simultaneously possesses hierarchical porous structure, high heteroatoms-doped degree, and large specific surface area (506 m2 g−1). Electrochemical measurements show that the N-TRPG-800 exhibits an ultrahigh supercapacitance of 471 F g−1 at 0.2 A g−1 in a three-electrode mode, approaching the theoretical capacitance of 550 F g−1 of graphene, which is superior to that of the state-of-the-art heteroatom-doped porous carbons in literature.