Molecular aspects on the amino acid-mediated sol–gel process of tetramethoxysilane in water

The aqueous sol–gel process of (TMOS) in conjunction with several natural amino acids (AAs) is employed for synthesis of amino acid/silica hybrid materials. These hybrid materials contain the amino acid physically bonded within the matrix. The sol–gel process occurs readily in unbuffered aqueous ami...

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Veröffentlicht in:Journal of sol-gel science and technology 2019-05, Vol.90 (2), p.250-262
Hauptverfasser: Kaßner, Lysann, Kronawitt, Julia, Klimm, Daniela, Seifert, Andreas, Spange, Stefan
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Sprache:eng
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Zusammenfassung:The aqueous sol–gel process of (TMOS) in conjunction with several natural amino acids (AAs) is employed for synthesis of amino acid/silica hybrid materials. These hybrid materials contain the amino acid physically bonded within the matrix. The sol–gel process occurs readily in unbuffered aqueous amino acid solution. The pH value during the processing is only determined by the dissolved amino acid. It ranges between pH 3–11 as function of the isoelectrical point (IEP) of the AAs. Systematic study of the influence of molecular structure of the AAs L-alanine, ε -aminocaproic acid, L-arginine, L-asparagine, L-aspartic acid, L-glutamic acid, L-glutamine, glycine, L-histidine, L-hydroxyproline, L-leucine, L-lysine, L-methionine, L-phenylalanine, L-proline, L-serine, L-threonine, L-tryptophan, and L-valine on the gelation time and dissolution behavior of TMOS in water is discussed. The IEP of the AA determines both dissolution and gelation of TMOS in water. Glycine was used as a model compound to investigate how concentration affects dissolution and gelation time of TMOS as well as porosity of resulting silica. As a result, the hydrolysis rate of TMOS in water and therewith dissolution is decelerated and gelation process is accelerated by increasing glycine concentration. Glycine-mediated sol–gel processes of TMOS were additionally examined by 1 H NMR spectroscopy, dynamic light scattering, and ATR-FTIR spectroscopy as a function of reaction time to support the visual observed results. Furthermore, various glycine derivatives such as N -acetylglycine, N- benzoylglycine, glycine ethylester, glycine ethylester·HCl , N -methylglycine, N,N -dimethylglycine, N,N -dimethylglycine methylester, and N -phenylglycine are used for studying the influence of amino acid structure functionalities on dissolution and gelation time of TMOS. The amino acid-mediated sol–gel process of tetramethoxysilane in aqueous solution is presented using 27 various AAs (derivatives). Hydrolysis of TMOS and condensation reactions to AA/silica hybrid materials are influenced in different ways by structure and concentration of the amino acid. The impact of molecular structure is examined with regard to reaction rate to produce monolithic amino acid/silica hybrid materials of type A. Highlights Sol–gel process for the manufacture of amino acid/silica type A hybrid materials is presented. Simple sol–gel process of TMOS influenced by amino acids is developed. Impact of molecular structure of amino aci
ISSN:0928-0707
1573-4846
DOI:10.1007/s10971-019-04930-7