Le Dizès Castell Romane, Mirzahossein Elham, Grzelka Marion, Jabbari-Farouji Sara, Bonn Daniel, Shahidzadeh Noushine
Institute of Physics, University of Amsterdam, Amsterdam 1098XH, The Netherlands.
Laboratoire Léon Brillouin, Université Paris-Saclay, CEA-Saclay, 91191 Gif-sur-Yvette Cedex, France.
J Phys Chem Lett. 2024 Jan 18;15(2):628-635. doi: 10.1021/acs.jpclett.3c02634. Epub 2024 Jan 11.
The sol-gel transition involves the transformation of a colloidal suspension into a system-spanning, interconnected gel. This process is widely used to reinforce mechanically weakened porous artifacts, such as sculptures but the impact of the restricted geometry (porous network) on the gelation dynamics of the solution remains unclear. Here, using fluorescent viscosity-sensitive molecular rotors, confocal microscopy, and model pores, we visualize the local viscosity changes at the microscale that accompany the sol-gel transition of a methyltriethoxysilane solution into a gel network. We show that, with evaporation of the solvent, a viscosity gradient develops near the free surface, triggering the sol-gel transition inside small pores near the surface. In homogeneous porous media, this leads to skin formation, which reduces the evaporation rate. In heterogeneous porous media, a gradient in gel density develops toward the heart of the porous material, where the gel formation mainly occurs as capillary bridges within smaller pores.
溶胶-凝胶转变涉及胶体悬浮液转变为贯穿整个体系的相互连接的凝胶。这个过程被广泛用于增强机械强度较弱的多孔文物,如雕塑,但受限的几何结构(多孔网络)对溶液凝胶化动力学的影响仍不清楚。在这里,我们使用荧光粘度敏感分子转子、共聚焦显微镜和模型孔隙,可视化了甲基三乙氧基硅烷溶液转变为凝胶网络的溶胶-凝胶转变过程中伴随的微观尺度局部粘度变化。我们表明,随着溶剂的蒸发,在自由表面附近会形成粘度梯度,从而触发表面附近小孔内的溶胶-凝胶转变。在均匀多孔介质中,这会导致形成皮层,从而降低蒸发速率。在非均匀多孔介质中,凝胶密度会朝着多孔材料的中心形成梯度,凝胶形成主要发生在较小孔隙内的毛细管桥处。