Electrochemical capacitors (best known as supercapacitors) are high‐performance energy storage devices featuring higher capacity than conventional capacitors and higher power densities than batteries, and are among the key enabling technologies of the clean energy future. This review focuses on performance enhancement of carbon‐based supercapacitors by doping other elements (heteroatoms) into the nanostructured carbon electrodes. The nanocarbon materials currently exist in all dimensionalities (from 0D quantum dots to 3D bulk materials) and show good stability and other properties in diverse electrode architectures. However, relatively low energy density and high manufacturing cost impede widespread commercial applications of nanocarbon‐based supercapacitors. Heteroatom doping into the carbon matrix is one of the most promising and versatile ways to enhance the device performance, yet the mechanisms of the doping effects still remain poorly understood. Here the effects of heteroatom doping by boron, nitrogen, sulfur, phosphorus, fluorine, chlorine, silicon, and functionalizing with oxygen on the elemental composition, structure, property, and performance relationships of nanocarbon electrodes are critically examined. The limitations of doping approaches are further discussed and guidelines for reporting the performance of heteroatom doped nanocarbon electrode‐based electrochemical capacitors are proposed. The current challenges and promising future directions for clean energy applications are discussed as well.

We report catalyst-free direct synthesis of vertical graphene nanosheets (VGNs) on SiO2/Si and quartz substrates using microwave electron cyclotron resonance - plasma enhanced chemical vapor deposition. The evolution of VGNs is studied systematically at different growth stages. Raman analysis as a function of growth time reveals that two different disorder-induced competing mechanisms contributing to the defect band intensity. The VGNs grown on SiO2/Si substrates predominantly consists of both vacancy-like and hopping defects. On the other hand, the VGNs grown on quartz substrates contain mainly boundary-like defects. XPS studies also corroborate Raman analysis in terms of defect density and vacancy-like defects for the VGNs grown on SiO2/Si substrates. Moreover, the grown VGNs exhibit a high optical transmittance from 95 to 78 % at 550 nm and the sheet resistance varies from 30 to 2.17 kohms/square depending on growth time.Comment: 19 pages, 8 figures, 1 table; Accepted in Journal of Raman Spectroscopy (2014

Defects in planar and vertically oriented nanographitic structures (NGSs) synthesized by plasma enhanced chemical vapor deposition (PECVD) have been investigated using Raman and X-ray photoelectron spectroscopy. While Raman spectra reveal the dominance of vacancy and boundary type defects respectively in vertical and planar NGSs, XPS provides additional information on vacancy related defect peaks in the C 1s spectrum, which originate from non-conjugated carbon atoms in the hexagonal lattice. Although an excellent correlation prevails between these two techniques, our results show that estimation of surface defects by XPS is more accurate than Raman analysis. Nuances of these techniques are discussed in the context of assessing defects in nanographitic structures.