A quantum molecular dynamics simulation study of the initial hydrolysis step in sol-gel process

Mohamed Elanany, Parasuraman Selvam, Toshiyuki Yokosuka, Seiichi Takami, Momoji Kubo, Akira Imamura, Akira Miyamoto

研究成果: Article査読

116 被引用数 (Scopus)

抄録

The dynamic behavior of the hydrolysis reaction of Si(OCH3)4 under neutral, basic, and acidic conditions was investigated, for the first time, at the atomic level with short time intervals using a novel tight-binding quantum chemical molecular dynamics program "Colors". The initial parameters required for the computation were determined completely on the basis of the first principles density functional calculations using Amsterdam density functional program. The simulation results of this study clearly indicate that a flank-side attack mechanism is favored, in all the three cases, for the hydrolysis process, and pentacoordinate silicon intermediates are easy pathways for the displacement of -OCH3 by -OH on silicon. Moreover, the presence of the acid or the base as catalyst promotes the hydrolysis by rapid formation of Si-OH bond in comparison to the hydrolysis under neutral condition. Furthermore, in the case of the latter condition, it was observed that the proton oscillates between -OH and -OCH3 before it migrates to the latter group.

本文言語English
ページ(範囲)1518-1524
ページ数7
ジャーナルJournal of Physical Chemistry B
107
7
DOI
出版ステータスPublished - 2003 2月 20

ASJC Scopus subject areas

  • 物理化学および理論化学
  • 表面、皮膜および薄膜
  • 材料化学

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