Self-Assembly of Bridged Silsesquioxanes: Modulating Structural Evolution via Cooperative Covalent and Non-covalent Interactions

Gaëlle Creff (1, 2) , Benoît P. Pichon (3) , Christophe Blanc (1) , David Maurin (1) , Jean-Louis Sauvajol (1) , Carole Carcel (3) , Joël Moreau (3) , Pascale Roy (2) , John R. Bartlett (4) , Michel Wong Chi Man (3) , Jean-Louis Bantignies (1)

1 L2C - Laboratoire Charles Coulomb
2 SSOLEIL - Synchrotron SOLEIL
3 ICGM ICMMM - Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier
4 USC - Faculty of Science, Health, Education and Engineering

The self-assembly of a bis-urea phenylene-bridged silsesquioxane precursor during sol-gel synthesis has been investigated by in situ infrared spectroscopy, optical microscopy and light scattering. In particular, the evolution of the system as a function of processing time was correlated with covalent interactions associated with increasing polycondensation and non-covalent interactions such as hydrogen bonding. A comprehensive mechanism based on the hydrolysis of the phenylene-bridged organosilane precursor prior to the crystallization of the corresponding bridged silsesquioxane via H bonding and subsequent irreversible polycondensation is proposed.

Mots clés: Bridged silsesquioxanes; hydrogen bonding; hydrolysis-condensation; self-assembly; sol-gel

Domaines: Matériaux

Gaëlle Creff, Benoît P. Pichon, Christophe Blanc, David Maurin, Jean-Louis Sauvajol, et al.. Self-Assembly of Bridged Silsesquioxanes: Modulating Structural Evolution via Cooperative Covalent and Non-covalent Interactions. Langmuir, 2013, 29, pp.5581. ⟨10.1021/la400293k⟩. ⟨hal-00819327⟩