Synthesis and Characterization of Functionalized Silica-Based Nanohybrid Materials for Oxyanions Adsorption

Abstract

This study investigates the structural evolution of a series of nanohybrid powders and coatings synthesized by direct co-condensation of amino-functionalized alkyltrialkoxysilanes and tetraalkoxysilanes with an aromatic carboxylic acid (trimesic acid, TMA) as a structure directing agent. Fourier transform infrared spectroscopy (FTIR) and (13)C CP-MAS NMR results have suggested the formation of secondary (-CO-NH-) amide linkages upon interaction of TMA with the amino functionalized silane thus creating a "scaffold" around which the silica network is formed and also assisting in more homogeneous distribution of nitrogen sites within the nanohybrid structure. Functionalized silica powders were investigated for their potential to remove toxic oxyanions from mildly acidic or basic solutions. The uptake of Mo(VI), Se(VI), and Cr(VI) oxyanions was investigated as a function of the nanohybrid composition, oxyanion concentration, and solution pH using laser diffraction particle sizing, gas adsorption, and various spectroscopic techniques. The adsorption data obtained for Mo and Se could be adequately described by Langmuir adsorption isotherms, while the Freundlich isotherm is employed to fit the adsorption data for Cr. An easily accessible processing window (of pH, aging time, etc.) has been identified allowing production of continuous and uniform thin nanohybrid coatings on silicon and glass substrates. These coatings were tested as chemical barriers against Mo leaching from specially prepared Mo-doped glass. Leaching studies were conducted over 200 days in water at 90 degrees C and the Mo leaching from coated and uncoated samples compared.