Formation, Characterization, and Dynamics of Onion-Like Carbon Structures for Electrical Energy Storage from Nanodiamonds Using Reactive Force Fields
Abstract
We simulate the experimentally observed graphitization of nanodiamonds into multi-shell onion-like carbon nanostructures, also called carbon onions, at different temperatures, using reactive force fields. The simulations include long-range Coulomb and van der Waals interactions. Our results suggest that long-range interactions play a crucial role in the phase-stability and the graphitization process. Graphitization is both enthalpically and entropically driven and can hence be controlled with temperature. The outer layers of the nanodiamond have a lower kinetic barrier toward graphitization irrespective of the size of the nanodiamond and graphitize within a few-hundred picoseconds, with a large volume increase. The inner core of the nanodiamonds displays a large size-dependent kinetic barrier, and graphitizes much more slowly with abrupt jumps in the internal energy. It eventually graphitizes by releasing pressure and expands once the outer shells have graphitized. The degree of transformation at a particular temperature is thereby determined by a delicate balance between the thermal energy, long-range interactions, and the entropic/enthalpic free energy gained by graphitization. Upon full graphitization, a multi-shell carbon nanostructure appears, with a shell-shell spacing of about ~3.4 Å for all sizes. The shells are highly defective with predominantly five- and seven-membered rings to curve space. Larger nanodiamonds with a diameter of 4 nm can graphitize into spiral structures with a large (~29-atom carbon ring) pore opening on the outermost shell. Such a large one-way channel is most attractive for a controlled insertion of molecules/ions such as Li ions, water, or ionic liquids, for increased electrochemical capacitor or battery electrode applications.
Recommended Citation
P. Ganesh et al., "Formation, Characterization, and Dynamics of Onion-Like Carbon Structures for Electrical Energy Storage from Nanodiamonds Using Reactive Force Fields," Journal of Applied Physics, vol. 110, no. 7, American Institute of Physics (AIP) Publishing LLC, Jan 2011.
The definitive version is available at https://doi.org/10.1063/1.3641984
Department(s)
Chemistry
International Standard Serial Number (ISSN)
0021-8979
Document Type
Article - Journal
Document Version
Citation
File Type
text
Language(s)
English
Rights
© 2011 American Institute of Physics (AIP) Publishing LLC, All rights reserved.
Publication Date
01 Jan 2011
