Construction of large-aperture mesoporous silica spheres supported polyoxometalate heterogeneous catalysts and their high-efficiency for the ultra-deep desulfurization.

• The large-aperture mesoporous silica spheres was achieved. • The catalyst PMo 10 V 2 /APTES-HMSNS was synthesized by chemical bonding. • The catalytic activity of nanocomposite was tested on the ODS for fuel. • The catalyst can be easily separated and reused at least 8 times. • The possible desulfurization mechanism was proposed by the quenching experiments and GC–MS analyses. A kind of large-aperture mesoporous silica spheres (HMSNS) has been innovatively synthesized via "Stöber- Phenolic resin" assistance, mainly attributed to the similarity on reaction conditions between the Stöber method and phenolic resin polymerization, as well inspired by the idea of obtaining large-aperture carbon spheres by simple etching and removing templates. To develop the high efficiency heterogeneous catalyst for oxidative desulfurization of fuel, the P-Mo-V type polyoxometalate as active sites, which was considered to own great influence on catalytic performance, was dispersedly immobilized onto HMSNS under the chemical bonding, named PMo 10 V 2 /APTES-HMSNS. The PMo 10 V 2 /APTES-HMSNS possessed the ultra-deep ODS performance under the optimal reaction conditions. It is worth mentioning that the 20-Mo 10 V 2 /APTES-HMSNS could catalyze the degradation for the four sulfur-containing components simultaneously, as high as 86.84 %, 99.99 %, 97.84 % and 91.35 % for benzothiophene (BT), dibenzothiophene (DBT), 4-methyl-dibenzothiophene (4-MDBT) and 4,6-dimethyl-dibenzothiophene (4,6-DMDBT). In addition, 20-PMo 10 V 2 /APTES-HMSNS displayed an outstanding reusability at least 8 times and the plausible ODS mechanism has been proposed. [ABSTRACT FROM AUTHOR]