Oxygen adsorption on graphite and nanotubes.pdf英文资料.pdfVIP

JOURNAL OF CHEMICAL PHYSICS VOLUME 118, NUMBER 3 15 JANUARY 2003 Oxygen adsorption on graphite and nanotubes P. Giannozzi,a) R. Car, and G. Scoles Chemistry Department and Princeton Materials Institute, Princeton University, Princeton, New Jersey 08544 Received 29 August 2002; accepted 18 November 2002 We study the binding of molecular oxygen to a graphene sheet and to a 8,0 single walled carbon nanotube, by means of spin-unrestricted density-functional calculations. We find that triplet oxygen retains its spin-polarized state when interacting with graphene or the nanotube. This leads to the formation of a weak bond with essentially no charge transfer between the molecule and the sheet or tube, as one would expect for a physisorptive bond. This result is independent on the approximation used for the exchange-correlation functional. The binding strength, however, depends strongly on the functional, reflecting the inability of current approximation functionals to deal correctly with dispersion forces. Gradient-corrected functionals yield very weak binding at distances around 4 Å, whereas local density functional results yield substantially stronger binding for both graphene and the nanotube at distances of less than 3 Å. The picture of oxygen physisorption is not substantially altered by the presence of topological defects such as 5–7 Stone–Wales pairs. © 2003 American Institute of Physics. DOI: 10.1063/1.1536636 There is currently a strong interest on the phenomenol- nanotube with a binding energy E 0.25 eV at a distance d ogy of gas adsorption by carbon nanotubes. Recent experi- 2.7 Å from the nanotube. A weak