Experimental Gibbs Free Energy Considerations in the Nucleation and Growth of Single-Walled Carbon Nanotubes

Larry M. Wagg; G. Louis Hornyak; Leonid Grigorian; Anne C. Dillon; Kim M. Jones; Jeffrey Blackburn; Philip A. Parilla; Michael J. Heben

doi:10.1021/jp050445f

Experimental Gibbs Free Energy Considerations in the Nucleation and Growth of Single-Walled Carbon Nanotubes

Larry M. Wagg, G. Louis Hornyak, Leonid Grigorian, Anne C. Dillon, Kim M. Jones, Jeffrey Blackburn, Philip A. Parilla, Michael J. Heben

Materials Science

Research output: Contribution to journal › Article › peer-review

20 Scopus Citations

Abstract

Gas feed composition and reaction temperature were varied to identify the thermodynamic threshold conditions for the nucleation and growth of SWNT from methane on supported Fe/Mo catalyst. These reaction conditions closely approximate the pseudoequilibrium conditions that lead to the nucleation and growth of SWNT. These measurements also serve to determine an upper limit of the Gibbs free energy of formation for SWNT. The Gibbs free energy of formation relative to graphite is in good agreement with literature values predicted from simulations for SWNT nuclei containing approximately 80 atoms, while considerably larger than that predicted for bulk (5,5) SWNT. Our estimate over the range 700 to 1000 °C of 16.1 to 13.9 kJ mol ^-1 falls between the results of these simulations and literature values for diamond.

Original language	American English
Pages (from-to)	10435-10440
Number of pages	6
Journal	Journal of Physical Chemistry B
Volume	109
Issue number	20
DOIs	https://doi.org/10.1021/jp050445f https://doi.org/10.1021/jp050445f
State	Published - 2005

NREL Publication Number

NREL/JA-590-38427

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title = "Experimental Gibbs Free Energy Considerations in the Nucleation and Growth of Single-Walled Carbon Nanotubes",

abstract = "Gas feed composition and reaction temperature were varied to identify the thermodynamic threshold conditions for the nucleation and growth of SWNT from methane on supported Fe/Mo catalyst. These reaction conditions closely approximate the pseudoequilibrium conditions that lead to the nucleation and growth of SWNT. These measurements also serve to determine an upper limit of the Gibbs free energy of formation for SWNT. The Gibbs free energy of formation relative to graphite is in good agreement with literature values predicted from simulations for SWNT nuclei containing approximately 80 atoms, while considerably larger than that predicted for bulk (5,5) SWNT. Our estimate over the range 700 to 1000 °C of 16.1 to 13.9 kJ mol -1 falls between the results of these simulations and literature values for diamond.",

author = "Wagg, {Larry M.} and Hornyak, {G. Louis} and Leonid Grigorian and Dillon, {Anne C.} and Jones, {Kim M.} and Jeffrey Blackburn and Parilla, {Philip A.} and Heben, {Michael J.}",

year = "2005",

doi = "10.1021/jp050445f",

language = "American English",

volume = "109",

pages = "10435--10440",

journal = "Journal of Physical Chemistry B",

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T1 - Experimental Gibbs Free Energy Considerations in the Nucleation and Growth of Single-Walled Carbon Nanotubes

AU - Wagg, Larry M.

AU - Hornyak, G. Louis

AU - Grigorian, Leonid

AU - Dillon, Anne C.

AU - Jones, Kim M.

AU - Blackburn, Jeffrey

AU - Parilla, Philip A.

AU - Heben, Michael J.

PY - 2005

Y1 - 2005

N2 - Gas feed composition and reaction temperature were varied to identify the thermodynamic threshold conditions for the nucleation and growth of SWNT from methane on supported Fe/Mo catalyst. These reaction conditions closely approximate the pseudoequilibrium conditions that lead to the nucleation and growth of SWNT. These measurements also serve to determine an upper limit of the Gibbs free energy of formation for SWNT. The Gibbs free energy of formation relative to graphite is in good agreement with literature values predicted from simulations for SWNT nuclei containing approximately 80 atoms, while considerably larger than that predicted for bulk (5,5) SWNT. Our estimate over the range 700 to 1000 °C of 16.1 to 13.9 kJ mol -1 falls between the results of these simulations and literature values for diamond.

AB - Gas feed composition and reaction temperature were varied to identify the thermodynamic threshold conditions for the nucleation and growth of SWNT from methane on supported Fe/Mo catalyst. These reaction conditions closely approximate the pseudoequilibrium conditions that lead to the nucleation and growth of SWNT. These measurements also serve to determine an upper limit of the Gibbs free energy of formation for SWNT. The Gibbs free energy of formation relative to graphite is in good agreement with literature values predicted from simulations for SWNT nuclei containing approximately 80 atoms, while considerably larger than that predicted for bulk (5,5) SWNT. Our estimate over the range 700 to 1000 °C of 16.1 to 13.9 kJ mol -1 falls between the results of these simulations and literature values for diamond.

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DO - 10.1021/jp050445f

M3 - Article

AN - SCOPUS:20344404473

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EP - 10440

JO - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

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ER -

Experimental Gibbs Free Energy Considerations in the Nucleation and Growth of Single-Walled Carbon Nanotubes

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