Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2023-06-23 , DOI: 10.1016/j.micromeso.2023.112704 Guoqing An , Hongyi Gao , Yibin Luo , Ying Ouyang , Ge Wang , Siqi Liu , Chang'an Wang , Zhiyuan Liu , Zhixiang Cheng , Xingtian Shu
Metal organic frameworks (MOFs)-induced synthetic strategy has been proven a convenient and efficient way for preparing anatase-free hierarchical TS-1 zeolite in our previous study. Here, to further enhance the catalytic performance on 1-hexene, the MOFs-induced hydrothermal synthesis route is optimized by adjusting the amount of tetrapropylammonium hydroxide (TPAOH) and performing different degrees of silanization treatment. A low TPAOH dosage can ensure the synthesized samples have abundant and dense active framework Ti at the expense of partial hierarchical structure. Further deep silanization treatment created mesoporous structure ranging between 20 and 30 nm without affecting the content or distribution of active titanium. The obtained anatase-free hierarchical TS-1 sample Sil-0.150 possesses excellent 1-hexene conversion of >38%. Based on detailed NH3-TPD and Py-IR tests, the presence of high-density Lewis acid sites (LAS) leads to a decreased epoxy product selectivity of 91.5%, and the optimized MOFs-induced synthesis strategy may open up new perspectives for the design and application of high-performance TS-1 catalysts in selective epoxidation reactions of various alkenes.
中文翻译:
MOFs 诱导制备无锐钛矿分级 TS-1 的 1-己烯环氧化策略优化:TPAOH 剂量调节、硅烷化和稳定酸性位点
金属有机骨架(MOF)诱导的合成策略已被证明是制备无锐钛矿分级TS-1沸石的便捷有效的方法在我们之前的研究中。为了进一步提高对1-己烯的催化性能,通过调整氢氧化四丙基铵(TPAOH)的用量并进行不同程度的硅烷化处理来优化MOFs诱导的水热合成路线。较低的TPAOH用量可以保证合成的样品具有丰富且致密的活性骨架Ti,但会牺牲部分分级结构。进一步的深度硅烷化处理形成了20至30 nm的介孔结构,而不影响活性钛的含量或分布。获得的无锐钛矿分级TS-1样品Sil-0.150具有>38%的优异1-己烯转化率。基于详细的NH 3-TPD和Py-IR测试,高密度路易斯酸位点(LAS)的存在导致环氧产物选择性下降91.5%,优化的MOFs诱导合成策略可能为环氧化合物的设计和应用开辟新的视角用于各种烯烃选择性环氧化反应的高性能 TS-1 催化剂。