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Reversing Titanium Oligomer Formation towards High‐Efficiency and Green Synthesis of Titanium‐Containing Molecular Sieves
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2020-10-28 , DOI: 10.1002/anie.202011821
Dong Lin 1 , Quande Zhang 1 , Zhengxing Qin 1 , Qing Li 1 , Xiang Feng 1 , Zhaoning Song 1 , Zhenping Cai 2 , Yibin Liu 1 , Xiaobo Chen 1 , De Chen 2 , Svetlana Mintova 3 , Chaohe Yang 1
Affiliation  

Green and efficient synthesis of titanium‐containing molecular sieves is limited by the quantity of environmentally unfriendly additives and complicated synthesis procedures required. Oligomerization of Ti monomers into anatase TiO2 is the typical outcome of such procedures because of a mismatch between hydrolysis rates of Si and Ti precursors. We report a simple and generic additive‐free route for the synthesis of Ti‐containing molecular sieves (MFI, MEL, and BEA). This approach successfully reverses the formation of Ti oligomers to match hydrolysis rates of Ti and Si species with the assistance of hydroxyl free radicals generated in situ from ultraviolet irradiation. Moreover, fantastic catalytic performance for propene epoxidation with H2 and O2 was observed. Compared with the conventional hydrothermal method, this approach opens up new opportunities for high‐efficiency, environmentally benign, and facile production of pure titanium‐containing molecular sieves.

中文翻译:

将含钛低聚物转变为高效的绿色合成含钛分子筛

含钛分子筛的绿色和高效合成受到环境不友好的添加剂数量和所需复杂合成程序的限制。Ti单体向锐钛矿型TiO 2的低聚是这种方法的典型结果,因为Si和Ti前体的水解速率不匹配。我们报告了一种简单且通用的无添加剂路线,用于合成含钛分子筛(MFI,MEL和BEA)。该方法借助紫外线辐射原位产生的羟基自由基,成功地逆转了Ti低聚物的形成,以匹配Ti和Si物种的水解速率。此外,H 2和O 2对丙烯环氧化的出色催化性能被观测到。与传统的水热法相比,该方法为高效,对环境无害且易于生产纯钛分子筛开辟了新的机遇。
更新日期:2020-10-28
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