TITANIUM-CONTAINING MESOPOROUS MOLECULAR-SIEVES FOR CATALYTIC-OXIDATION OF AROMATIC-COMPOUNDS
TITANIUM-CONTAINING MESOPOROUS MOLECULAR-SIEVES FOR CATALYTIC-OXIDATION OF AROMATIC-COMPOUNDS
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DOI：
10.1038/368321a0
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发表时间：
1994-03-24
期刊：
影响因子：
64.8
通讯作者：
PINNAVAIA, TJ
中科院分区：
文献类型：
--
作者：
TANEV, PT;CHIBWE, M;PINNAVAIA, TJ
钛硅分子筛是一种有效的分子筛催化剂，用于H_2O_2存在下烷烃的选择性氧化、苯酚的羟基化和烯烃的环氧化反应（参考文献1-3）。然而，可被氧化的有机化合物的范围受到主体骨架（4）的相对小的孔径（约0.6nm）的极大限制。大孔（介孔）二氧化硅基分子筛最近已经由Kresge等人制备。(5-7)和黑田等人。(8)前者使用的模板方法，其中的无机介孔结构的形成是由表面活性剂的自组织辅助，和后者涉及的层状二氧化硅前体的拓扑化学重排。在这里，我们描述了使用模板法合成介孔硅基分子筛部分取代钛-大孔类似物的钛硅分子筛。我们发现，这些材料对2，6-二叔丁基苯酚氧化为相应的醌和苯转化为苯酚显示出选择性催化活性。
TITANIUM silicalite is an effective molecular-sieve catalyst for the selective oxidation of alkanes, the hydroxylation of phenol and the epoxidation of alkenes in the presence of H2O2 (refs 1-3). The range of organic compounds that can be oxidized is greatly limited, however, by the relatively small pore size (about 0.6 nm) of the host framework(4). Large-pore (mesoporous) silica-based molecular sieves have been prepared recently by Kresge et al.(5-7) and Kuroda et al.(8); the former used a templating approach in which the formation of an inorganic mesoporous structure is assisted by self-organization of surfactants, and the latter involved topochemical rearrangement of a layered silica precursor. Here we describe the use of the templating approach to synthesize mesoporous silica-based molecular sieves partly substituted with titanium-large-pore analogues of titanium silicalite. We find that these materials show selective catalytic activity towards the oxidation of 2,6-di-tert-butyl phenol to the corresponding quinone and the conversion of benzene to phenol.