Facile one-pot approach to the synthesis of spherical mesoporous silica nanoflowers with hierarchical pore structure

Hierarchically structured spherical mesoporous nanoflowers (HSMNF) with well-defined morphology and uniform size were synthesized by a hydrothermal method, in which a mixture of cyclohexane and water was used as the solvent, with cetylpyridinium bromide (CPB) as the template, tetraethyl ortho-silicate as the source of inorganic silica, and urea as the hydrolysis additive. The flower size ranged from 200 nm to 500 nm, and the thickness of a "petal" was about 10 nm. We investigated the effects of solvent composition (V-cyclohexane/V-water), hydrothermal temperature, and molar ratio of Si to CPB on morphology and structure. The presence of cyclohexane was found to be crucial for the nanoflowers to form, and a solvent with high cyclohexane content was beneficial for the formation of smaller and more uniform nanoflowers, whereas low cyclohexane content resulted in the collapse of the nanoflower structure. The optimal ratio of cyclohexane to water was 1:1 by volume. The hydrothermal temperature and molar ratio of Si to CPB strongly affected nanoflower size and structure, as well as petal thickness. The optimal hydrothermal temperature was 120 degrees C, and the optimal molar ratio of Si to CPB was 4.37. The sample synthesized under optimal conditions exhibited well-defined morphology and uniform flower size. Its BET surface area reached 502 m(2)/g. The nanoflowers were under 200 nm in diameter, and their average mesopore size was ca. 4 nm, as measured by N-2 adsorption-desorption. Using synthesized nanoflowers as the support, we prepared a supported PdAu bimetallic catalyst for the hydrogenation of phenol. This catalyst exhibited high activity (with a conversion rate of up to 90%) and high selectivity for cyclohexanone (up to 92%). This nanoflower's morphology, high surface area, and large pore size may make it a valuable and promising material for applications in the catalysis, adsorption and controlled release of drugs fields. (C) 2014 Elsevier B.V. All rights reserved.