Theory of genus reduction in alkali-induced graphitization of nanoporous carbon

2007; American Physical Society; Volume: 76; Issue: 11 Linguagem: Inglês

10.1103/physrevb.76.115436

ISSN

1550-235X

Autores

Elena R. Margine, Aleksey N. Kolmogorov, Dragan Stojkovic, Jorge O. Sofo, Vincent H. Crespi,

Tópico(s)

Catalytic Processes in Materials Science

Resumo

Exposure to elemental Cs generates graphitic domains within nanoporous carbon at only $50\phantom{\rule{0.2em}{0ex}}\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}$, well below the typical graphitization temperatures of $>1000\phantom{\rule{0.2em}{0ex}}\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}$. We present a model of nanoporous carbon, the wormhole, which can express the fundamental topological elements of graphitization: a negative-curvature analog to ${\mathrm{C}}_{60}$ fullerene. The pathway to wormhole annihilation comprises an initial Stone-Wales transformation and a subsequent unzipping of the defect. This complex $\ensuremath{\sim}100$-atom collective defect disintegrates with the formation of only two dangling bonds. Our ab initio calculations show that while the activation barrier against reduction in topological genus is indeed lowered by interaction with alkali, an additional chemical constituent must be involved to account for this remarkable local graphitization of nanoporous carbons at near-room temperature.

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