Origin of the Linear Relationship between CH/NH/O—SWNT Reaction Energies and Sidewall Curvature: Armchair Nanotubes.

The origin of the linear relationship between the reaction energy of the CH/NH/O exo and endo additions to armchair (n, n) single-walled carbon nanotubes (SWNTs) and the inverse tube diameter (1/d) measuring sidewall curvature was elucidated using density functional theory and density functional tig...

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Publicado en:Journal of the American Chemical Society Vol. 128; no. 47; pp. 15117 - 15127
Autores principales: Guishan Zheng, Zhi Wang, Irie, Stephan, Morokuma, Keiji
Formato: Artículo
Publicado: American Chemical Society 11/29/2006
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 11/29/2006
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        10.1021/ja061306u
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        atl: Origin of the Linear Relationship between CH/NH/O—SWNT Reaction Energies and Sidewall Curvature: Armchair Nanotubes.
      aug:
        au:
          Guishan Zheng
          Zhi Wang
          Irie, Stephan
          Morokuma, Keiji
        affil:
          Cherry L. Emerson Center for Scientific Computation
          Department of Chemistry, Emory University, Atlanta, Georgia 30322
          Department of Chemistry, University of Illinois, Urbana-Champaign, Urbana, IL 61801
          Fukui Institute for Fundamental Chemistry, Kyoto University, Kyoto 606-8103, Japan
      su:
        Nanotubes
        Chemical reactions
        Chemical processes
        Density functionals
        Functional analysis
        Potential energy surfaces
      sug:
        subj:
          Nanotubes
          Chemical reactions
          Chemical processes
          Density functionals
          Functional analysis
          Potential energy surfaces
      ab: The origin of the linear relationship between the reaction energy of the CH/NH/O exo and endo additions to armchair (n, n) single-walled carbon nanotubes (SWNTs) and the inverse tube diameter (1/d) measuring sidewall curvature was elucidated using density functional theory and density functional tight binding methods for finite-size SWNT models with n = 3, 4…13. A nearly perfect linear relationship between ΔE and 1/d all through exohedral (positive curvature) and endohedral (negative curvature) additions is due to cancellation between the quadratic contributions of the SWNT deformation energy and the interaction energy (INT) between the deformed SWNT and CH/NH/O adducts. Energy decomposition analysis shows that the quadratic contributions in electrostatic, exchange, and orbital terms mostly cancel each other, making INT weakly quadratic, and that the linear 1/d dependence of INT, and therefore of ΔE, is a reflection of the 1/d dependence of the back-donative orbital interaction of b symmetry from the occupied CH/NH/O pπ orbital to the vacant C=C π* LUMO of the SWNT. We also discuss the origin of the two isomers (open and three-membered ring) of the exohedral addition product and explain the behavior of their associated minima on the C-C potential energy surfaces with changing d.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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