FY2010 - Oak Ridge National Laboratory

Director’s R&D Fund—
Ultrascale Computing and Data Science
occur at the interface. This is a very interesting topic that has only been studied experimentally in the
past few years but to which very little theoretical work has been devoted. We have made significant
progress in this area, hinging on our team’s expertise in chemistry in nano-confined systems. We have
provided the first systematic study of carbon nanostructure functionalization through single atom
doping for all the relevant atomic species such as B, N, O, F, Si, P, S, Se. We also collaborated with
various international groups to corroborate our findings with their experimental results, leading to a
number of high-impact publications in international journals (see full listing of publications). In
addition, we have continued to work on the materials aspects of the supercapacitor science, focusing
on the promising graphitic nanoribbons materials, for which we collaborated with the group of Millie
Dressehaus at MIT in a publication in Science (Jia et al. 2009) and another in Phys. Rev. Lett. (Cruz-
Silva 2010a), on the intriguing metal-oxide nanotubes, solid electrolytic-carbon interactions, and finally,
semiconducting polymers with carbon nanotubes and graphene.
This has been a timely project in the area of energy storage materials and has already begun to show
tremendous international recognition (see journal references and invited talks listed as follows).
Energy storage is clearly an important topic that is strategically aligned with the DOE mission for a
secure and sustainable energy future. In the past 2 years, we have witnessed a large effort put forth to
develop the Energy Frontier Research Centers, the Energy Innovation Hubs, and the focus from the
Office of Advanced Scientific Computing Research (OASCR) to push the computational capabilities for
energy science forward towards exascale. The subject LDRD effort has contributed towards
providing an ORNL foundation along these lines.
Notable from this work are the strong collaborations formed with Georgia Tech (G. Yushin), Drexell
University (Y. Gogotsi), and Rice University (P. Ajayan) and its synergistic, but complementary,
connections to the ORNL Fluid Interface Reactions, Structures, and Transport (FIRST) Energy Frontier
Research Center. In the teams’ work, the focus was on structural details of realistic pores (e.g., well
beyond slit-pore or cylindrical pore models) and to begin to examine a hybrid energy storage process
known as pseudo-capacitance. The objective is notably distinct from the FIRST center’s scope,
where effort is on understanding, predicting, and controlling interfacial transport and reaction at
idealized planar and nano-textured surfaces. Finally, it should be highly noted that this was a vibrant and
creative team partnership that exemplifies the power of an excellent team effort.
Program Development
The research and development of this project will have immediate impact into the prime mission of
DOE. It fits exceptionally well with the anticipated calls by DOE Office of Basic Energy Sciences
for Energy Innovation Hubs (one of which will be solely devoted to electrochemical storage) and from
DOE Energy Efficiency and Renewable Energy (EERE). Because of the achievements made in this
project, we have been invited to take part in ORNL workshops set up to delineate the path to prepare
proposals for these calls. We have also participated in the DOE Workshop on Computational
Materials Science and Chemistry for Innovation that has led to the publication of a report
(http://www.ornl.gov/sci/cmsinn/index.shtml). In addition, the fundamental aspects of charge storage,
motion, solvation, and desolvation have large ramifications to biology because ion channels are quite
important in nearly all types of life forms. As such we expect considerable interest from the National
Institute of Health (NIH) and the Environmental Protection Agency (EPA). Efficient energy storage
is also of importance to the Global Nuclear Energy Partnership (GNEP). In addition, the potential
use of supercapacitors for portable power systems cross-cuts the continued and high-priority interest of the
Department of Defense.
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