Ionic liquid-silica precursors via solvent-free sol-gel process and their application in epoxy-amine network: a theoretical/experimental study

0474629 - ÚMCH 2018 RIV US eng J - Článek v odborném periodiku
Perchacz, Magdalena - Donato, R. K. - Seixas, L. - Zhigunov, Alexander - Konefal, Rafal - Serkis-Rodzen, Magdalena - Beneš, Hynek
Ionic liquid-silica precursors via solvent-free sol-gel process and their application in epoxy-amine network: a theoretical/experimental study.
ACS Applied Materials and Interfaces. Roč. 9, č. 19 (2017), s. 16474-16487. ISSN 1944-8244. E-ISSN 1944-8252
Grant CEP: GA ČR(CZ) GA17-08273S; GA MŠMT(CZ) LO1507
Institucionální podpora: RVO:61389013
Klíčová slova: 3D POSS structures * epoxy-silica hybrid material * IL-silica precursor
Obor OECD: Polymer science
Impakt faktor: 8.097, rok: 2017

This work describes the solvent-free sol–gel synthesis of epoxy-functionalized silica-based precursors in the presence of 1-butyl-3-methylimidazolium-based ionic liquids (ILs) containing different anions: chloride (Cl–) and methanesulfonate (MeSO3–). The IL-driven sol–gel mechanisms were investigated in detail using experimental characterizations (29Si NMR and ATR FTIR spectroscopy) and a theoretical computational method based on density functional theory (DFT). We observed complex IL influence on both hydrolysis and condensation steps, involving especially H-bonding and Coulomb coupling stabilization of the process intermediates. The obtained IL–silica precursors and their further xerogels were widely characterized (rheology measurements, MALDI TOF, 29Si NMR, ATR FTIR, and DFT simulation), which allowed observation of their precise silica structures and established their most energetically favorable conformations. The detected silica structures were dependent on the IL type and varied from highly condensed 3D cage-like to branched ladder-like and cyclic ones. The application of prepared IL–silica precursors as reinforcing additives into the epoxy–amine network led to an improvement in the organic/inorganic interphase interactions through chemical and physical bonding. Uniform and well-dispersed silica aggregates, in the size of approximately 30 nm, were formed when <= 6.8 wt % of each IL–silica precursor was applied into the epoxy–amine network. The use of imidazolium-based ILs contributed to a significant improvement in thermomechanical properties of hybrids and reduced their UV absorption ability compared to that of the reference matrix. All hybrids exhibited an increase in energy to break (up to approximately 53%), elongation at break (up to approximately 43%), shear storage modulus in the rubbery region (up to 4 times), and thermo-oxidative stability.
Trvalý link: http://hdl.handle.net/11104/0271925