Multinuclear NMR Study of Aluminosilicate Sol-Gel Synthesis Reasons for the Homogeneous Gelation Using the Prehydrolysis Method

Abstract

Aluminosilicate gels have been utilized in numerous optical, dielectric, and catalytic applications. These applications require a high degree of molecular homogeneity, but reproducible means of achieving this remain unobtainable for many compositions. In this work, reaction occurring in one of the most successful sol/gel processes are examined by means of both liquid and solid 13C, 29 si, 17), and Al NMR. The synthesis process studied was the method, optimized by Krol, of prehydrolyzing tetraethylorthosilicate, TEOS, in ethanol, and subsequently adding aluminum sec-butoxide, and then further water. After prehydrolysis and addition of aluminum sec-butoxide, an aluminosilicate precursor is formed in which the aluminum is tetrahedrally coordinated to four silicate ligands. After adding further water, gelation is accompanied by the expansion of the tetrahedral aluminum to octahedral coordination; this apparently. occurs by nucleophilic attack of silanol groups on the aluminum in the aluminosilicate precursor. At sufficiently low water to silicon molar ratios, where transparent gels and longer gel times result, this coordination expansion is preceded by condensation of the silicate ligands to form Si-O-Si.

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Document Details

Document Type
Technical Report
Publication Date
Jun 12, 1993
Accession Number
ADA266877

Entities

People

  • A. V. Mccormick
  • G. A. Pozarnsky

Organizations

  • University of Minnesota

Tags

DTIC Thesaurus Topics

  • Aluminum
  • Chemical Compounds
  • Chemical Engineering
  • Chemical Shifts
  • Chemical Synthesis
  • Chemistry
  • Condensation
  • Condensation Reactions
  • Engineering
  • Gelation
  • Homogeneity
  • Materials
  • Materials Science
  • Military Research
  • Polymerization
  • Precursors
  • Silicates

Readers

  • Organic Chemistry
  • Reinforced Composite Materials
  • Surface Engineering/Surface Coating Technology.