Zhu Xiaochun, Gao Yu, Chen Haorong, Jiang Mengwei, Wang Xinyu, Miao Caixia, Shen Yanfeng, Ji Yonggang, Qin Zhengxing, Wu Zhijie, Song Weiyu, Xu Chunming, Shen Baojian
State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering and Environment, China University of Petroleum (Beijing), Beijing 102249 (P. R. China), State Key Laboratory of Heavy Oil Processing, College of Science, China University of Petroleum (Beijing), Beijing, 102249, P. R. China.
Laboratory of Inorganic Materials Chemistry, Eindhoven University of Technology, PO Box 513, 5600 MB, Eindhoven (the, Netherlands.
Angew Chem Int Ed Engl. 2024 Dec 9;63(50):e202411446. doi: 10.1002/anie.202411446. Epub 2024 Oct 24.
Desilication in alkaline medium has been widely used in construction of hierarchical zeolites for industrially relevant catalytic processes. The built of hierarchy in zeolites, especially with low aluminum stability or high Si/Al ratio, often suffers from uncontrolled destruction of zeolitic framework, accompanied by a significant loss of microporous domains and intrinsic acidity after desilication. Here, we report a novel and simple methodology for preparation of hierarchical zeolites with highly complete framework and minimum sacrifice of microporosity and acidity. The pre-impregnated amines in zeolite micropores act as inner pore-directing agents (iPDAs), largely protecting the zeolitic framework and moderating the silicon extraction during the alkaline treatment. The resulting hierarchical zeolites exhibit high crystallinity, tunable hierarchy, stable framework, and well-preserved acidity, endowing them with significantly improved mass transport properties and enhanced activities in catalytic conversion of methanol or furfural.
在碱性介质中脱硅已广泛应用于工业相关催化过程的分级沸石的构建。沸石中分级结构的构建,特别是对于低铝稳定性或高硅铝比的沸石,常常会出现沸石骨架不受控制的破坏,脱硅后伴随着微孔域和固有酸性的显著损失。在此,我们报道了一种新颖且简单的方法来制备具有高度完整骨架且微孔率和酸度损失最小的分级沸石。沸石微孔中预浸渍的胺充当内孔导向剂(iPDAs),在很大程度上保护沸石骨架并调节碱性处理过程中的硅提取。所得的分级沸石表现出高结晶度、可调谐的分级结构、稳定的骨架和良好保留的酸度,使其在甲醇或糠醛的催化转化中具有显著改善的传质性能和增强的活性。