We report a novel, facile, physical mixing synthetic method that leads to titanium silicate and copper titanium silicate materials or highly effective solid acid catalysts for toluene oxidation reaction. The synthesis involves simple physical mixing of tetraethyl orthosilicate and various titanium alkoxide (and also copper(II) chloride), and then calcination of the products. The effects of the types of precursors on the catalytic activity of the resulting materials are investigated. Notably, titanium(IV) n-butoxide, whose hydrolysis rate is close to that of tetraethyl orthosilicate, yields a material that exhibits strong acidic properties and excellent catalytic activity for toluene oxidation with hydrogen peroxide (H₂O₂) as oxidant, giving 98% conversion of toluene and ca. 100% selectivity to benzaldehyde product. The work demonstrates not only simplicity in terms of synthesis of the materials but also unprecedented solid-acid catalytic activity for titanium silicate materials, the catalytic properties of which can be easily tailored by varying the types of precursors. It is also noteworthy that the materials give among the best catalytic performance (in terms of both conversion and product selectivity) under mild reaction conditions that has been reported for toluene oxidation with H₂O₂ as oxidant for heterogeneous catalysts.

我们报告了一种新颖，简便，物理混合的合成方法，可导致硅酸钛和硅酸铜钛材料或用于甲苯氧化反应的高效固体酸催化剂。合成过程包括原硅酸四乙酯和各种烷氧基钛（以及氯化铜（II））的简单物理混合，然后煅烧产物。研究了前体类型对所得材料催化活性的影响。值得注意的是，水解速率接近原硅酸四乙酯的正丁醇钛（IV）生成的材料具有强酸性，对过氧化氢（H ₂ O _2）的甲苯氧化具有出色的催化活性。）作为氧化剂，可实现98％的甲苯和ca转化率。对苯甲醛产品具有100％的选择性。这项工作不仅证明了合成材料的简单性，而且还证明了硅酸钛材料具有空前的固体酸催化活性，可以通过改变前体的类型来轻松调整其催化性能。还值得注意的是，据报道该材料在温和的反应条件下具有最佳的催化性能（就转化率和产物选择性而言），这已经报道了用H ₂ O ₂作为多相催化剂的氧化剂进行甲苯氧化。