Synthesis and physicochemical properties of Zr-MCM-41 mesoporous molecular sieves and Pt/H3PW12O40/Zr-MCM-41 catalysts

摘要

For the first time, modifications of the surface and framework of Si-MCM-41 by depositing a heteropolyacid on the surface and by introducing foreign Zr4+ ions into the framework are investigated. The Zr-modified Si-MCM-41 mesoporous materials (hereafter referred as WSZn, n = Si/Zr = 25, 15, 8, 4) were synthesized through a surfactant-templated preparation approach, using low-cost fumed silica as the Si precursor. After impregnation with 25wt% of H3PW12O40, the surface Bronsted acidity of the Pt/H3PW12O40/WSZn catalysts was greatly enhanced by 2-10 times relative to the bare WSZn support. Two kinds of supported heteropolyacids were formed: (i) bulk-like heteropolyacid crystals with unchanged Keggin structures, and (ii) highly dispersed heteropolyacid with distorted Keggin units. The formation of various kinds of heteropolyacid structures is closely related to the interaction between the heteropolyanions and the hydroxyl groups in the host support. (C) 2007 Elsevier Inc. All rights reserved.