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Sol-Gel Kinetics: 29Si NMR and a Statistical Reaction Model*

Published online by Cambridge University Press:  25 February 2011

Roger A. Assitik
Affiliation:
Sandia National Laboratories Albuquerque, NM 87185, USA
Bruce D. Kay
Affiliation:
Sandia National Laboratories Albuquerque, NM 87185, USA
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Abstract

The early time behavior of an acid catalyzed Si(OCH3),4 (TMOS) sol-gel was studied by high resolution 29Si nuclear magnetic resonance (NMR). Both the water producing and the alcohol producing condensation reactions were found to contribute significantly to the overall condensation rate. A general theoretical kinetic formalism which specifically treats the temporal evolution of the various chemical function groups about a specific silicon atom was developed. The experimentally observed functional group distribution was in agreement with the distribution predicted by a simplified statistical reaction model. The mathematical framework for the study of chemical speciation at the next-to-nearest functional group level was developed. This framework was used to assign several fine structure resonances, and to show that the formation of various dimeric species is also largely statistical in nature.

Type
Research Article
Copyright
Copyright © Materials Research Society 1988

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Footnotes

*

This work performed at Sandia National Laboratories supported by the U. S. Department of Energy under contract number DE-AC04–76DP00789.

References

REFERENCES

Better Ceramics Through Chemistry, edited by Brinker, C. J., Clark, D. E., and Ulrich, D. R. (Mater. Res. Sec. Proc. 32, Albuquerque, NM 1984).Google Scholar
2. Better Ceramics Through Chemistry II. edited by Brinker, C. J., Clark, D. E., and Ulrich, D. R. (Mater. Res. Soc. Proc. 73, Palo Alto, CA 1986).Google Scholar
3. Brinker, C. J., Keefer, K. D., Schaefer, D. W., Assink, R. A., Kay, B. D., and Ashley, C. S., J. Non-Crystalline Solids 63, 45 (1984).CrossRefGoogle Scholar
4. Assink, R. A. and Kay, B. D., Ref. 1, p. 301.Google Scholar
5. Kay, B. D. and Assink, R. A., Ref. 2, p. 157.Google Scholar
6. Assink, R. A. and Kay, B. D., J. Non-Crystalline Solids (in press).Google Scholar
7. Kay, B. D. and Assink, R. A., J. Non-Crystalline Solids (accepted for publication).Google Scholar
8. Artaki, I., Sinha, S. and Jonas, J., Materials Letters 2, 448 (1984).Google Scholar
9. Artaki, I., Bradley, M., Zerda, T. W. and Jonas, J., J. Phys. Chem. 81, 4399 (1985).Google Scholar
10. Artaki, I., Sinha, S., Irwin, A. D. and Jonas, J., J. Non-Crystalline Solids 22, 391 (1985).Google Scholar
11. Pohl, E. R. and Osterholtz, F. D. in: Molecular Characterization of Composite Interfaces. Eds. Ishida, H. and Kumar, G., (Plenum, NY, 1985), p. 157170.Google Scholar
12. Lin, C. C. and Basil, J. D., Ref. 2, p. 585.Google Scholar
13. Balfe, C. A. and Martinez, S. L., Ref. 2, p. 27.Google Scholar
14. Kelts, L. W., Effinger, N. J. and Melpolder, S. M., J. Non-Crystalline Solids 81, 353 (1986).Google Scholar
15. Pouxviel, J. C., Boilot, J. C., Beloeil, J. C. and Lallemand, J. Y., J. Non-Crystalline Solids 89, 345 (1987).CrossRefGoogle Scholar
16. Turner, C. W. and Franklin, K. J., J. Non-Crystalline Solids 91, 402 (1987).Google Scholar
17. Myers-Acosta, B. L. (private communication).Google Scholar