Bai Risheng, Navarro M Teresa, Song Yue, Zhang Tianjun, Zou Yongcun, Feng Zhaochi, Zhang Peng, Corma Avelino, Yu Jihong
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University Changchun 130012 China
Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas Avenida de los Naranjos s/n 46022 Valencia Spain
Chem Sci. 2020 Oct 23;11(45):12341-12349. doi: 10.1039/d0sc04603e.
Titanosilicate zeolites are catalysts of interest in the field of fine chemicals. However, the generation and accessibility of active sites in titanosilicate materials for catalyzing reactions with large molecules is still a challenge. Herein, we prepared titanosilicate zeolite precursors with open zeolitic structures, tunable pore sizes, and controllable Si/Ti ratios through a hydrothermal crystallization strategy by using quaternary ammonium templates. A series of quaternary ammonium ions are discovered as effective organic templates. The prepared amorphous titanosilicate zeolites with some zeolite framework structural order have extra-large micropores and abundant octahedrally coordinated isolated Ti species, which lead to a superior catalytic performance in the oxidative desulfurization of dibenzothiophene (DBT) and epoxidation of cyclohexene. It is anticipated that the amorphous prezeolitic titanosilicates will benefit the catalytic conversion of bulky molecules in a wide range of reaction processes.
钛硅沸石是精细化学品领域中备受关注的催化剂。然而，对于钛硅材料中用于催化大分子反应的活性位点的生成和可及性仍然是一个挑战。在此，我们通过使用季铵模板，采用水热结晶策略制备了具有开放沸石结构、可调孔径和可控硅钛比的钛硅沸石前驱体。发现一系列季铵离子是有效的有机模板。所制备的具有一定沸石骨架结构有序性的非晶态钛硅沸石具有超大微孔和丰富的八面体配位孤立钛物种，这使其在二苯并噻吩（DBT）的氧化脱硫和环己烯的环氧化反应中表现出优异的催化性能。预计非晶态沸石前驱体钛硅酸盐将有利于在广泛的反应过程中对大分子进行催化转化。
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