A transition from hierarchical pore structures (macro- and meso-pores) to uniform mesopores in monolithic polymethylsilsesquioxane (PMSQ, CH(3)SiO(1.5)) gels has been investigated using a sol-gel system containing surfactant Pluronic F127. The precursor methyltrimethoxysilane (MTMS) undergoes an acid/base two-step reaction, in which hydrolysis and polycondensation proceed in acidic and basic aqueous media, respectively, as a one-pot reaction. Porous morphology is controlled by changing the concentration of F127. Sufficient concentrations of F127 inhibit the occurrence of micrometer-scale phase separation (spinodal decomposition) of hydrophobic PMSQ condensates and lead to well-defined mesoporous transparent aerogels with high specific pore volume as a result of the colloidal network formation in a large amount of solvent. Phase separation regulates well-defined macropores in the micrometer range on decreasing concentrations of F127. In the PMSQ-rich gelling domain formed by phase separation, the PMSQ colloidal network formation forms mesopores, leading to monolithic PMSQ gels with hierarchical macro- and meso-pore structures. Mesopores in these gels do not collapse on evaporative drying owing to the flexible networks and repulsive interactions of methyl groups in PMSQ.
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