Titanosilicate zeolites are an important class of heterogeneous catalysts that are widely used in several catalytic processes. The construction of hierarchical titanosilicate zeolites (e.g., TS-1 with an MFI structure) is of great interest as they can promote the mass transportation and molecular accessibility of reactant molecules. Herein, we presented a temperature-regulated method to construct anatase-free hierarchical TS-1 zeolite catalysts by utilizing a two-step hydrothermal crystallization strategy with tetrabutylammonium hydroxide (TBAOH) as the sole organic structure-directing agent. The two-step crystallization process, i.e., initial crystallization at lower temperature followed by secondary crystallization at higher temperature, afforded the incorporation of more active Ti species into TS-1 and the formation of hierarchical structures resulting from the layer-stacking growth. The prepared hierarchical TS-1 zeolite catalysts showed superior catalytic performance in the oxidative desulfurization of bulky organosulfur compound dibenzothiophene compared with their microporous counterpart, giving a higher turnover number (23.5 vs. 1.7). The temperature-based kinetic regulation approach offers an effective way to construct hierarchical titanosilicate zeolite catalysts with controllable active Ti atoms.

中文翻译：

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分层钛硅酸盐沸石的温度调节结构

钛硅酸盐沸石是一类重要的非均相催化剂，广泛用于多种催化工艺中。分层的钛硅酸盐沸石（例如具有MFI结构的TS-1）的构造引起人们极大的兴趣，因为它们可以促进反应物分子的质量传递和分子可及性。本文中，我们提出了一种温度调节方法，该方法利用四丁基氢氧化铵（TBAOH）作为唯一的有机结构导向剂，利用两步水热结晶策略来构建无锐钛矿型分层TS-1沸石催化剂。两步结晶过程，即在较低的温度下进行初始结晶，然后在较高的温度下进行二次结晶，则将更多的活性Ti物种掺入TS-1中，并且由于层堆叠生长而形成了分层结构。所制备的分级TS-1沸石催化剂在大体积有机硫化合物二苯并噻吩的氧化脱硫中比其微孔对应物表现出优异的催化性能，从而提供更高的周转率（23.5对1.7）。基于温度的动力学调节方法提供了一种有效的方法来构造具有可控制的活性Ti原子的分级钛硅酸盐沸石催化剂。