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On the Role of Hydrogen Bonding in Gas-Phase SN2 Reactions at Silicon.
Fugel, Malte; Dittmer, Anneke; Kleemiss, Florian; Grabowsky, Simon.
Afiliación
  • Fugel M; Fachbereich 2-Biologie/ Chemie, Universität Bremen, Leobener Str. 3, 28359 Bremen, Germany.
  • Dittmer A; Fachbereich 2-Biologie/ Chemie, Universität Bremen, Leobener Str. 3, 28359 Bremen, Germany.
  • Kleemiss F; Fachbereich 2-Biologie/ Chemie, Universität Bremen, Leobener Str. 3, 28359 Bremen, Germany.
  • Grabowsky S; Departement für Chemie, Biochemie und Pharmazie, Universität Bern, Freiestrasse 3, 3012 Bern, Switzerland.
J Phys Chem A ; 125(19): 4070-4078, 2021 May 20.
Article en En | MEDLINE | ID: mdl-33974418
The shape of the potential energy surface (PES) of gas-phase SN2 reactions at silicon is determined by the type of nucleophile, the leaving group, and substituents which remain bonded to silicon. In this study, we present PES scans along the reaction coordinate of six symmetrical SN2 reactions: X- + SiR3X → XSiR3 + X-, where X = Cl or F and R = H, Me, or OMe. While the fluorine systems and the ClSiH3Cl system only give single-well PESs, ClSiMe3Cl and ClSi(OMe)3Cl give triple- and double-well PESs with stable pre- and post-reaction complexes. A complementary bonding analysis (energy decomposition analysis, quantum theory of atoms in molecules, and natural bond orbitals) reveals that the leaving group (X-) is stabilized by hydrogen bonding in the XSiMe3X and XSi(OMe)3X systems. It is shown that this so far neglected stabilizing contribution, along with σ-hole bonding, is responsible for the shapes of the PESs of ClSiMe3Cl and ClSi(OMe)3Cl in the gas phase.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem A Asunto de la revista: QUIMICA Año: 2021 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem A Asunto de la revista: QUIMICA Año: 2021 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Estados Unidos