A quantum chemical mechanism for the water-initiated decomposition of silica

Janet E. Del Bene, Keith A Runge, Rodney J. Bartlett

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

An ab initio quantum chemical investigation of the interaction of water with amorphous silica is carried out using model systems that contain the Si-O-Si bridging unit. Interaction of the silicon-oxygen bond with a water dimer is found to be most favorable, in contrast to the Michalske-Freiman model, which assumes that the interaction occurs with a single water molecule. Formation of a five-coordinated silicon atom is an essential intermediate in the bond fracture process, which involves proton transfer from the water dimer to the bridging oxygen, proton transfer within the water dimer, and the formation of a new Si-O bond. The activation barrier to rupture the Si-O bond in the Si-O-Si unit in the presence of water dimer is ∼30 kcal/mol.

Original languageEnglish (US)
Pages (from-to)102-108
Number of pages7
JournalComputational Materials Science
Volume27
Issue number1-2
DOIs
StatePublished - Mar 2003
Externally publishedYes

Fingerprint

Silica
Silicon Dioxide
Dimer
silicon dioxide
Decomposition
Water
decomposition
Decompose
Dimers
dimers
water
Proton transfer
Silicon
Oxygen
Interaction
Unit
protons
Rupture
interactions
silicon

Keywords

  • Ab initio quantum chemistry
  • Hydrolytic weakening
  • Quantum mechanics
  • Silica
  • Water
  • Water dimer

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

A quantum chemical mechanism for the water-initiated decomposition of silica. / Del Bene, Janet E.; Runge, Keith A; Bartlett, Rodney J.

In: Computational Materials Science, Vol. 27, No. 1-2, 03.2003, p. 102-108.

Research output: Contribution to journalArticle

Del Bene, Janet E. ; Runge, Keith A ; Bartlett, Rodney J. / A quantum chemical mechanism for the water-initiated decomposition of silica. In: Computational Materials Science. 2003 ; Vol. 27, No. 1-2. pp. 102-108.
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