Mesoporous ferrosilicates with high content of isolated iron species synthesized in mild buffer solution and their catalytic application

Mesoporous ferrosilicates with high content of isolated iron species synthesized in mild buffer solution and their catalytic application
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温和缓冲溶液中高含量分离铁的介孔硅酸铁合成及其催化应用

DOI:
10.1016/j.micromeso.2007.11.022
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发表时间:
2008-08
影响因子:
5.2
通讯作者:
Yang, Qihua
Yang, Qihua
中科院分区:
材料科学2区
文献类型:
--
作者:
Jia, Guoqing;Xin, Hongchuan;Feng, Zhaochi;Liu, Jian;Li, Can;Fan, Fengtao;Yang, Qihua

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以嵌段共聚物Pluronic P123为模板剂,以乙酰丙酮铁与四乙氧基硅烷(TEOS)和水玻璃的混合物为原料,在温和的酸性条件下(pH 4.4,缓冲溶液)共缩聚合成了骨架铁含量高的介孔硅酸铁。XRD、n2吸附和TEM结果表明,材料具有有序的二维六方介孔结构,大孔均匀。介孔骨架中铁的掺入量较高,可归因于温和的酸性条件,以及在此条件下合成过程中硅源和铁源的水解速率更匹配。紫外-可见漫反射光谱、紫外共振拉曼光谱和EPR光谱的结果表明,介孔骨架中以四面体铁为主。介孔硅酸铁以h2o2为氧化剂,能有效催化苯酚在水中的羟基化反应。在苯酚羟基化反应中,框架铁比框架外氧化铁低聚物更有活性。
The mesoporous ferrosilicates with high content of framework iron species have been synthesized under mild acidic conditions (pH 4.4, buffer solution) by co-condensation of iron acetylacetonate and a mixture of tetraethoxysilane (TEOS) and sodium silicate using block copolymer Pluronic P123 as the template. The XRD, N2sorption and TEM results show that the materials have well-ordered, two-dimensional, hexagonal mesoporous structure with uniform large pore. The higher amount of iron species incorporated in the mesoporous framework could be attributed to the mild acidic conditions and a better match of the hydrolysis rates of silica source and iron source during the synthesis under such conditions. The results of UV–vis diffuse reflectance spectra, UV resonance Raman spectra and EPR spectra show that tetrahedral iron species incorporated in the mesoporous framework of the materials are predominant. The mesoporous ferrosilicates can efficiently catalyze the hydroxylation of phenol in water using H2O2as an oxidant. The framework iron species are found to be more active than the extra-framework iron oxide oligomer in the hydroxylation of phenol.
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DOI: 10.1021/jp061523h
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期刊: The journal of physical chemistry. B
影响因子: --
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DOI: 10.1016/j.cattod.2005.10.037
发表时间: 2006-02-15
期刊: CATALYSIS TODAY
影响因子: 5.3
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