- Title
- Quantum chemical simulation of carbon nanotube nucleation on Al₂O₃ catalysts via CH₄ chemical vapor deposition
- Creator
- Page, Alister J.; Saha, Supriya; Li, Hai-Bei; Irle, Stephan; Morokuma, Keiji
- Relation
- ARC.DP140102894 http://purl.org/au-research/grants/arc/DP140102894
- Relation
- Journal of the American Chemical Society Vol. 137, Issue 29, p. 9281-9288
- Publisher Link
- http://dx.doi.org/10.1021/jacs.5b02952
- Publisher
- American Chemical Society
- Resource Type
- journal article
- Date
- 2015
- Description
- We present quantum chemical simulations demonstrating how single-walled carbon nanotubes (SWCNTs) form, or "nucleate", on the surface of Al₂O₃ nanoparticles during chemical vapor deposition (CVD) using CH₄. SWCNT nucleation proceeds via the formation of extended polyyne chains that only interact with the catalyst surface at one or both ends. Consequently, SWCNT nucleation is not a surface-mediated process. We demonstrate that this unusual nucleation sequence is due to two factors. First, the π interaction between graphitic carbon and Al₂O₃ is extremely weak, such that graphitic carbon is expected to desorb at typical CVD temperatures. Second, hydrogen present at the catalyst surface actively passivates dangling carbon bonds, preventing a surface-mediated nucleation mechanism. The simulations reveal hydrogen's reactive chemical pathways during SWCNT nucleation and that the manner in which SWCNTs form on Al₂O₃ is fundamentally different from that observed using "traditional" transition metal catalysts. (Chemical Equation Presented).
- Subject
- quantum chemical simulations; single-walled carbon nanotubes; chemical vapor deposition
- Identifier
- http://hdl.handle.net/1959.13/1317386
- Identifier
- uon:23406
- Identifier
- ISSN:0002-7863
- Rights
- This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright ©2015 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/jacs.5b02952
- Language
- eng
- Full Text
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