High surface area microporous carbon nanocubes from controlled processing of graphene oxide nanoribbons

Abstract

A new, facile, and template-free method to prepare high surface area microporous carbon nanocubes (CNCs) from a mixture of graphene oxide nanoribbons (NRs), graphene oxide, and carbon dots is reported. The nanoribbons, approximately 30 nm wide and with lengths ranging from a few tens of nanometres up to several micrometres, were obtained from the oxidation of Black Pearls 2000 carbon black in nitric acid solution. The non-purified nanoribbons further contained additional fragments of graphene oxide, and of graphene oxide quantum dots. Slow pyrolysis of the nanoribbon mixture with slow heating rates, e.g., 3 °C/min, yielded carbon nanocubes approximately 250 nm in size with surface areas greater than 900 m2/g. Heating rates of 50 °C/min led to carbons with ∼800 m2/g surface area but bulk morphology. Precipitating the nanoribbons in potassium hydroxide solution, followed by carbonization, yielded microporous nanoparticle aggregates that were 20 nm in size with surface areas greater than 2000 m2/g. The particles exhibited complex, quasi-spherical morphology. Pyrolysis of other products obtained from oxidation in HNO3 of different grades of carbon black, specifically graphene oxide nanoparticles and quantum dots, yielded high surface area microporous carbons but with bulk morphology regardless of the processing conditions. Despite the lower surface area and pore volume of the CNCs in comparison to the nanospheres, the former contained ultramicropores that were highly accessible to CO2 as a molecular probe and had excellent selectivity of CO2 over N2. Hence, CNC materials have promising properties for applications where particle surface-to-volume ratios, high internal surface areas, and abundant super and ultramicropores are desired.