State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun, 130012, P.R. China.
Faculty of Chemistry and Chemical Engineering, Yunnan Normal University, Kunming, 650500, P.R. China.
Chemistry. 2018 Aug 27;24(48):12600-12606. doi: 10.1002/chem.201801185. Epub 2018 Jul 24.
Much effort has been invested in the designed synthesis of zeolites with nanosized and hierarchical structures in recent decades, on account of increasing demands in practical applications, especially catalysis. Herein, a new topotactic synthetic strategy is demonstrated to synthesize nanosized and hierarchical zeolites in a one-step procedure. By using silica spheres as the adjustable amorphous precursors and tetrapropylammonium hydroxide as a structure-directing agent, effortless control of both size and porosity can be achieved in this system with no extra templates. With a simple hydrothermal process, hierarchical zeolite spheres can be modified with acid cites (Al species incorporated in the framework). Benefitting from its mesoporosity, palladium nanoparticles are incorporated into the nanosized hierarchical zeolite, which makes the materials suitable for use in a cascade catalysis reaction of benzimidazole derivatives, including independent acid catalysis and hydrogenation sites. The nanocomposites show exceptional activity and stability in catalysis and recycling reaction. This strategy can be developed into other versatile and practicable scaffolds for advanced zeolite catalytic nanoreactor systems.
近几十年来,人们投入了大量精力设计合成具有纳米级和分级结构的沸石,这是因为实际应用,特别是催化领域的需求不断增加。在此,本文展示了一种新的、在一步法中合成纳米级和分级沸石的位构合成策略。通过使用硅球作为可调节的无定形前体和四丙基氢氧化铵作为结构导向剂,在该体系中无需额外模板即可轻松控制尺寸和孔隙率。采用简单的水热法,可在分级沸石球上修饰酸位(骨架中掺入的铝物种)。得益于其介孔性,钯纳米粒子被掺入纳米分级沸石中,这使得该材料适用于苯并咪唑衍生物的级联催化反应,包括独立的酸催化和加氢位点。该纳米复合材料在催化和回收反应中表现出优异的活性和稳定性。该策略可进一步发展为用于先进沸石催化纳米反应器系统的其他多功能和实用支架。