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TS-1 Zeolite with Homogeneous Distribution of Ti Atoms in the Framework: Synthesis, Crystallization Mechanism and its Catalytic Performance
Journal of Catalysis ( IF 7.3 ) Pub Date : 2021-11-10 , DOI: 10.1016/j.jcat.2021.11.001
Zhen Chen 1 , Lianlin Zhang 1 , Yunkai Yu 1 , Dongxu Liu 1 , Nan Fang 1 , Yuxia Lin 1 , Deyi Xu 1 , Fang Li 1 , Yueming Liu 1 , Mingyuan He 1
Affiliation  

The distribution of titanium (Ti) active sites in the framework of TS-1 zeolite is one of the critical factors affecting its catalytic performance, since it can influence accessibility of the Ti active sites and the catalytic utilization of Ti atoms. Here, TS-1 zeolite with homogeneous distribution of titanium atoms in the framework (named BUS-TS-1) is successfully synthesized via bottom-up strategy at high basicity conditions, and BUS-TS-1 zeolite exhibits better catalytic performance for both olefin and alkane oxidation. The comprehensive explorations on the crystallization behavior of BUS-TS-1 zeolite show that, the gripper-like silicon species, as condensed matter in Q2 and Q3 states (detected by 29Si NMR), can be obtained by the condensation of tetraethyl orthosilicate (TEOS) at high alkalinity conditions. The gripper-like silicon species can condense with Ti-OH to form stable and isolated Si-O-Ti species, so that the phase transfer rates of Si and Ti species match during the entire crystallization process, resulting in the homogeneous distribution of Ti atoms. This work offers a useful strategy for the synthesis of high-performance catalysts by regulating the distribution of Ti active-site within TS-1 framework.



中文翻译:

骨架中Ti原子分布均匀的TS-1沸石:合成、结晶机理及其催化性能

钛(Ti)活性位点在TS-1沸石骨架中的分布是影响其催化性能的关键因素之一,因为它会影响Ti活性位点的可及性和Ti原子的催化利用率。在这里,在高碱度条件下,通过自下而上的策略成功合成了骨架中钛原子分布均匀的 TS-1 沸石(命名为 BUS-TS-1),并且 BUS-TS-1 沸石对两种烯烃均表现出更好的催化性能和烷烃氧化。对 BUS-TS-1 沸石结晶行为的综合探索表明,类似抓手的硅物种,作为 Q 2和 Q 3态的凝聚物(由29Si NMR),可以通过原硅酸四乙酯 (TEOS) 在高碱度条件下缩合获得。类似抓手的硅物种可以与 Ti-OH 凝聚形成稳定且孤立的 Si-O-Ti 物种,从而在整个结晶过程中使 Si 和 Ti 物种的相转移速率匹配,从而导致 Ti 原子的均匀分布. 这项工作通过调节 TS-1 框架内 Ti 活性位点的分布,为合成高性能催化剂提供了一种有用的策略。

更新日期:2021-11-10
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