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Direct hydrothermal synthesis of Mo-containing MFI zeolites using Mo-EDTA complex and their catalytic application in cyclohexene epoxidation
Chinese Journal of Catalysis ( IF 16.5 ) Pub Date : 2021-09-15 , DOI: 10.1016/s1872-2067(21)63826-3
Haoyang Zhang 1 , Lifen Xu 1 , Xinyu Chang 1 , Songsong Miao 1 , Yuting Sun 1 , Mingjun Jia 1
Affiliation  

A series of Mo-containing MFI zeolites with different Mo loadings (Mo-MFI-n, n represent the initial Si/Mo molar ratio) was hydrothermally synthesized by using tetrapropylammonium hydroxide as the template and Mo-EDTA complex as the Mo source. Various characterization results demonstrated that the use of the Mo-EDTA complex is beneficial for the incorporation of more Mo species into the MFI-type zeolites. The special complexing capability of EDTA2– plays a critical role in adjusting the release rate of the Mo species to combine with the Si tetrahedron species during the zeolite growth process, thus leading to a uniform distribution of Mo in the MFI framework. In addition, a small portion of extra-framework Mo clusters may be distributed inside the channels or near the pore window of the zeolites. The catalytic properties of these Mo-containing MFI zeolites were evaluated for the epoxidation of cyclohexene with H2O2 as the oxidant. The composition-optimized catalyst, Mo-MFI-50, efficiently converted cyclohexene to the corresponding epoxide with a relatively high conversion (93%) and epoxide selectivity (82%) at 75 °C after 9 h of reaction. Moreover, the resultant Mo-containing MFI catalyst exhibited excellent structural stability and recoverability and was easily recycled by simple filtration without the need for calcination treatment.



中文翻译:

Mo-EDTA配合物直接水热合成含Mo的MFI沸石及其在环己烯环氧化中的催化应用

以氢氧化四丙铵为模板剂,Mo-EDTA配合物为Mo源,水热合成了一系列具有不同Mo负载量(Mo-MFI- n,n表示初始Si/Mo摩尔比)的含Mo的MFI沸石。各种表征结果表明,使用 Mo-EDTA 复合物有利于将更多的 Mo 物质结合到 MFI 型沸石中。EDTA 2–的特殊络合能力在沸石生长过程中,在调节 Mo 物质与 Si 四面体物质结合的释放速率方面起着关键作用,从而导致 Mo 在 MFI 框架中的均匀分布。此外,一小部分框架外的 Mo 簇可能分布在通道内或沸石的孔窗附近。评估了这些含 Mo MFI 沸石对环己烯与 H 2 O 2环氧化的催化性能作为氧化剂。组成优化的催化剂 Mo-MFI-50 在 75°C 反应 9 小时后,以相对较高的转化率 (93%) 和环氧化物选择性 (82%) 有效地将环己烯转化为相应的环氧化物。此外,所得含Mo的MFI催化剂表现出优异的结构稳定性和可回收性,并且无需煅烧处理即可通过简单过滤轻松回收。

更新日期:2021-09-16
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