Nitrogen-Doped Carbon Nanotube Spherical Particles for Supercapacitor Applications: Emulsion-Assisted Compact Packing and Capacitance Enhancement.

The combination of the control of CNT assembly density and the control of intrinsic carbon properties by doping can synergistically improve the supercapacitor performance of CNT-based electrodes. We prepared a dense-packed CNT spherical assembly via emulsion-assisted evaporation and subsequently conducted nitrogen (N) doping to make CNT-based supercapacitors. The assembly of CNT spherical particles is applied as the supercapacitor electrode. We control the N doping content and obtain a specific capacity of 215 F/g at a current density of 0.2 A/g, which is 3.1 times higher than that of the untreated sample. The enhancement stems from high pseudocapacitance and high electrical conductivity that result from the N doping of the CNT assembly. In a comparison of the specific capacitance of N-CNT spherical particles with that of the CNT films prepared by conventional solution-coating, we found that N-CNT samples display a capacitance that is 1.8 times higher, thus confirming the morphological advantage provided by the CNT packing and the hierarchical porous structure in the CNT particle assembly. Our approach allows a facile and high throughput production of high performance electrodes based on CNTs that are commercially available. Moreover, our approach can be extended to produce spherical particles consisting of other nanostructured carbon materials and their composites.