Vacuum or flowing argon: What is the best synthesis atmosphere for nanodiamond-derived carbon onions for supercapacitor electrodes?

Abstract

We present a comprehensive study on the influence of the synthesis atmosphere on the structure and properties of nanodiamond-derived carbon onions. Carbon onions were synthesized at 1300 and 1700 °C in high vacuum or argon flow, using rapid dynamic heating and cooling. High vacuum annealing yielded carbon onions with nearly perfect spherical shape. An increase in surface area was caused by a decrease in particle density when transitioning from sp3 to sp2 hybridization and negligible amounts of disordered carbon were produced. In contrast, carbon onions from annealing nanodiamonds in flowing argon are highly interconnected by few-layer graphene nanoribbons. The presence of the latter improves the electrical conductivity, which is reflected by an enhanced power handling ability of supercapacitor electrodes operated in an organic electrolyte (1 M tetraethylammonium tetrafluoroborate in acetonitrile). Carbon onions synthesized in argon flow at 1700 °C show a specific capacitance of 20 F/g at 20 A/g current density and 2.7 V cell voltage which is an improvement of more than 40% compared to vacuum annealing. The same effect was measured for a synthesis temperature of 1300 °C, with a 140% higher capacitance at 20 A/g for argon flow compared to vacuum annealing.