Nanoscale Zirconia as a Nonmetallic Catalyst for Graphitization of Carbon and Growth of Single- and Multiwall Carbon Nanotubes

作者:Steiner Stephen A III*; Baumann Theodore F; Bayer Bernhard C; Blume Raoul; Worsley Marcus A; MoberlyChan Warren J; Shaw Elisabeth L; Schloegl Robert; Hart A John; Hofmann Stephan; Wardle Brian L
来源:Journal of the American Chemical Society, 2009, 131(34): 12144-12154.
DOI:10.1021/ja902913r

摘要

We report that nanoparticulate zirconia (ZrO(2)) catalyzes both growth of single-wall and multiwall carbon nanotubes (CNTs) by thermal chemical vapor deposition (CVD) and graphitization of solid amorphous carbon. We observe that silica-, silicon nitride-, and alumina-supported zirconia on silicon nucleates single- and multiwall carbon nanotubes upon exposure to hydrocarbons at moderate temperatures (750 degrees C). High-pressure, time-resolved X-ray photoelectron spectroscopy (XPS) of these substrates during carbon nanotube nucleation and growth shows that the zirconia catalyst neither reduces to a metal nor forms a carbide. Point-localized energy-dispersive X-ray spectroscopy (EDAX) using scanning transmission electron microscopy (STEM) confirms catalyst nanoparticles attached to CNTs are zirconia. We also observe that carbon aerogels prepared through pyrolysis of a Zr(IV)-containing resorcinol-formaldehyde polymer aerogel precursor at 800 degrees C contain fullerenic cage structures absent in undoped carbon aerogels. Zirconia nanoparticles embedded in these carbon aerogels are further observed to act as nucleation sites for multiwall carbon nanotube growth upon exposure to hydrocarbons at CVD growth temperatures. Our study unambiguously demonstrates that a nonmetallic catalyst can catalyze CNT growth by thermal CVD while remaining in an oxidized state and provides new insight into the interactions between nanoparticulate metal oxides and carbon at elevated temperatures.

  • 出版日期2009-9-2