Akshay S. Raut

Graphenated carbon nanotubes for enhanced electrochemical double layer capacitor performance

This letter reports on nucleation and growth of graphene foliates protruding from the sidewalls of aligned carbon nanotubes (CNTs) and their impact on the electrochemical double-layer capacitance. Arrays of CNTs were grown for different time intervals, resulting in an increasing density of graphene foliates with deposition time. The samples were characterized using electrochemical impedance spectroscopy, scanning electron microscopy, and transmission electron microscopy. Both low and high frequency capacitance increased with increasing foliate density. A microstructural classification is proposed to explain the role of graphene edges, three-dimensional organization, and other features of hybrid carbon systems on their electrochemical properties.

Perspectives on the Growth of High Edge Density Carbon Nanostructures: Transitions from Vertically Oriented Graphene Nanosheets to Graphenated Carbon Nanotubes

Insights into the growth of high edge density carbon nanostructures were achieved by a systematic parametric study of plasma-enhanced chemical vapor deposition (PECVD). Such structures are important for electrode performance in a variety of applications such as supercapacitors, neural stimulation, and electrocatalysis. A morphological trend was observed as a function of temperature whereby graphenated carbon nanotubes (g-CNTs) emerged as an intermediate structure between carbon nanotubes (CNTs) at lower temperatures and vertically oriented carbon nanosheets (CNS), composed of few-layered graphene, at higher temperatures. This is the first time that three distinct morphologies and dimensionalities of carbon nanostructures (i.e., 1D CNTs, 2D CNSs, and 3D g-CNTs) have been synthesized in the same reaction chamber by varying only a single parameter (temperature). A design of experiments (DOE) approach was utilized to understand the range of growth permitted in a microwave PECVD reactor, with a focus on identifying graphenated carbon nanotube growth within the process space. Factors studied in the experimental design included temperature, gas ratio, catalyst thickness, pretreatment time, and deposition time. This procedure facilitates predicting and modeling high edge density carbon nanostructure characteristics under a complete range of growth conditions that yields various morphologies of nanoscale carbon. Aside from the morphological trends influenced by temperature, a relationship between deposition temperature and specific capacitance emerged from the DOE study. Transmission electron microscopy was also used to understand the morphology and microstructure of the various high edge density structures. From these results, a new graphene foliate formation mechanism is proposed for synthesis of g-CNTs in a single deposition process.