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Preparation of Fe-substituted Mesoporous Silicas with Highly Isolated Iron Species in Buffer Solution

XIN Hong-Chuan,TANG Jian-Ting,FAN Feng-Tao,YANG Qi-Hua,LI Can(State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China)  
The iron-substituted mesoporous silicas were synthesized under mild acidic conditions(pH=4.4,HOAc-NaOAc buffer solution) using tetramethoxysilane(TMOS),tetraethoxysilane(TEOS) or sodium silicate solution as silica source in the presence of block copolymer pluronic P123 as the mesoporous template.TMOS and sodium silicate led to iron-containing silicas with ordered two-dimensional hexagonal mesoporous structure,and vesicle mesostructure was obtained using TEOS as silica precursor.UV-Vis and UV resonance Raman spectra show that highly isolated iron species can be predominantly obtained on mesoporous iron-containing silicas synthesized using inexpensive sodium silicate and Fe(NO3)3 as precursors.The buffer solution provides a facile strategy for controlling the mesostructure of iron-containing silicas by simply varying the silica source.Mesoporous iron-substituted silicas are highly efficient in hydroxylation of phenol because of a high dispersion of active iron centers within silica matrices and a high accessibility of active iron species to reactants.
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