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Journal of Materials Science

, Volume 29, Issue 15, pp 3926–3940 | Cite as

In situ solid-state NMR studies of Ca3SiO5: hydration at room temperature and at elevated temperatures using 29Si enrichment

  • A. R. Brough
  • C. M. Dobson
  • I. G. Richardson
  • G. W. Groves
Papers

Abstract

29Si isotopic enrichment was used for acquisition of multiple 29Si magic-angle spinning (MAS) and cross-polarization magic-angle spinning (CPMAS) nuclear magnetic resonance (NMR) spectra, in situ in an NMR probe, from a single sample of hydrating Ca3SiO5 (C3S). Data with excellent signal-to-noise ratios were obtained at 20, 50 and 75 °C, with minimal use of spectrometer time, and without the need for the quenching of multiple samples. Spectral line widths and polymer-chain lengths derived from the spectra had no detectable differences from experiments in which the quenching was carried out with propan-2-ol. Furthermore, the effects of the MAS technique on the hydration reaction appeared to be minimal. At 20 °C, the bulk hydrate initially produced was dimeric; at later stages of the reaction, polymerization occurred. Arrhenius energies of 35 and 100 kJ mol−1, respectively, were calculated for these two reactions. The cross-polarization (CP) spectra acquired throughout the hydration showed that at 20 °C, 2% of the hydrated monomeric Q o (H) species persisted from after the induction period through to the late stages of the hydration reaction; this indicates that this species is unlikely to result from surface hydroxylation of C3S; an upfield shift of this species occurred with increasing hydration, indicating a possible change of environment for the silicate species. The amount of Q o (H) produced was found to increase at higher temperatures. Potential mechanisms for polymerization were assessed and a model in which dimeric-silicate units are linked together by insertion of monomers (dimer → pentamer → octomer) was found to give the best fit to the observed data; these results support a dreierketten model for the structure of the hydrate.

Keywords

Nuclear Magnetic Resonance Induction Period Surface Hydroxylation Isotopic Enrichment Nuclear Magnetic Resonance Study 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.

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Copyright information

© Chapman & Hall 1994

Authors and Affiliations

  • A. R. Brough
    • 1
  • C. M. Dobson
    • 1
  • I. G. Richardson
    • 2
  • G. W. Groves
    • 2
  1. 1.Inorganic Chemistry LaboratoryUniversity of OxfordOxfordUK
  2. 2.Department of MaterialsUniversity of OxfordOxfordUK

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