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Abstract: Ordered 2-D hexagonal mesoporous TiO2–SiO2 nanocomposites consisted of anatase TiO2 nanocrystals and amorphous SiO2 nanoparticles, with large mesochannels and high specific surface areas, have been extensively and detailedly evaluated using various cationic dyes (methylene blue, safranin O, crystal violet, brilliant green, basic fuchsin and rhodamine-6G), anionic dyes (acid fuchsin, orange II, reactive brilliant red X3B and acid red 1) and microcystin-LR. We use mesoporous 80TiO2–20SiO2-900 for the degradation of cationic dyes and MC-LR, due to the dominant adsorption of Si and synergistic role of coupled adsorption and photocatalytic oxidation. For anionic dyes, due to the adsorption results predominantly from Ti, our strategy realizes the enhanced photocatalytic oxidation by strong surface acids and larger available specific surface area. Based on this, we prepared 90TiO2–10SiO2-700 to degrade them. The results show that our samples exhibit excellent degradation activities to all the contaminants, which are much higher than that of P25 photocatalyst. The dyes are not only decolorized promptly but degraded readily as well. It is strongly indicated that our mesoporous nanocomposites are considerably stable and reusable. These results demonstrate that our mesoporous TiO2–SiO2 nanocomposites present extensive and promising application in the fast and highly efficient degradation of various organic pollutants. [Copyright &y& Elsevier]

• Mesoporous anatase titania with 3D large secondary mesopores was prepared. • The preparation approach is mild, simple and facilely reproducible. • The photocatalyst with 3D large secondary pores displays quite excellent activities. • The activities are far higher than that of P25 photocatalyst and the parent sample. • The photocatalyst with 3D large secondary mesopores is rather stable and reusable. A mesoporous titania (SN2) with three-dimensional (3D) large secondary mesopores (6.2 nm) highly connecting the mesochannels was prepared employing the method of first synthesizing an ordered 2D hexagonal mesoporous titania-silica nanocomposite (SN1) via "synchronous-assembly" of inorganic precursors with surfactant molecules, then "extracting silica". Our tactic adopts a large amount of silica, a high crystallization temperature and mild silica extraction. The 3D interconnectivities of the resultant mesochannels are quite high, but the mesostructures are retained intact. Titania is fully anatase crystalline with uniform nanocrystals size (11.2 nm) and a high specific surface area (∼ 174 m2 g−1). This strategy is gentle, simple and easily reproducible. SN2 presents extremely-high photocatalytic degradation activities to anionic azo dyes like acid red 1 and reactive brilliant red X3B, which reach 55.9 and 51.1 times that of commercial P25 photocatalyst, even up to 87.0 and 84.7 times that of SN1, respectively; and far higher than that of the contrast sample (CS) possessing 3D small secondary mesopores (2.7 nm). Additionally, SN2 also displays a very high activity to microcystin-LR, which is much higher than that of P25 and CS, respectively. Our results clearly indicate that the large secondary mesopores play a key role in the great increases of activities. Moreover, our photocatalyst is considerably stable and reusable. Such results have hitherto not been seen in the literature. Furthermore, this method would pave the way for the rational design and preparation of ordered mesoporous other metal-oxides with large secondary mesopores and unexpected performances. [ABSTRACT FROM AUTHOR]