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Effect of synthesis conditions on the microstructure of TEOS derived silica hydrogels synthesized by the alcohol-free sol–gel route

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Abstract

Silica matrices synthesized from a pre-hydrolysis step in ethanol followed by alcohol removal at low pressure distillation, and condensation in water, are suitable for encapsulation of biomolecules and microorganisms and building bioactive materials with optimized optical properties. Here we analyze the microstructure of these hydrogels from the dependence of I(q) data acquired from SAXS experiments over a wide range of silica concentration and pH employed in the condensation step. From the resulting data it is shown that there is a clear correlation between the microscopic parameters—cluster fractal dimension (D), elementary particle radius (a) and cluster gyration radius (R)—with the attenuation of visible light when the condensation step proceeds at pH < 6. At higher pHs, there is a steep dependence of the cluster density (~R D−3) with the condensation pH, and non-monotonous changes of attenuance are less than 20%, revealing the complexity of the system. These results, which were obtained for a wide pH and silica concentration range, reinforce the idea that the behavior of gels determined in a restricted interval of synthesis variables cannot be extrapolated, and comparison of gelation times is not enough for predicting their properties.

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Notes

  1. As discussed later, in the Sect. 3, the interpretation of experimental results as indicating “fractality” is a matter of discussion (see Vinogradova et al. [39]).

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Acknowledgements

This work has been supported by the Brazilian Synchrotron Light Laboratory (LNLS, Brazil, proposal D11A-SAXS-6039), the scientific collaboration agreement CAPES-SECyT (Brazil-Argentina, 011/02), the University of Buenos Aires (UBACyT X-003), and by National Research Council of Argentina (CONICET PIP 11220080102533). SAB, RC, MJ and MP are Research Scientists of CONICET (Argentina).

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Authors and Affiliations

  1. INQUIMAE-DQIAQF, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria, Pab. II, C1428EHA, Buenos Aires, Argentina

    Mercedes Perullini, Matías Jobbágy, Sara A. Bilmes & Roberto Candal

  2. ECyT, Universidad Nacional de San Martín, Campus Miguelete, San Martín, Buenos Aires, Argentina

    Roberto Candal

  3. Institute of Physics Gleb Wataghin, State University of Campinas, Campinas, SP, Brazil

    Iris L. Torriani

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  1. Mercedes Perullini
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  2. Matías Jobbágy
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  3. Sara A. Bilmes
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  4. Iris L. Torriani
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  5. Roberto Candal
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Correspondence to Mercedes Perullini or Roberto Candal.

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Perullini, M., Jobbágy, M., Bilmes, S.A. et al. Effect of synthesis conditions on the microstructure of TEOS derived silica hydrogels synthesized by the alcohol-free sol–gel route. J Sol-Gel Sci Technol 59, 174–180 (2011). https://doi.org/10.1007/s10971-011-2478-8

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