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Organosilane with gemini-type structure as the mesoporogen for synthesis of hierarchical porous ZSM-5 zeolite

机译:双子型结构的有机硅烷作为介孔原,用于合成分级多孔ZSM-5沸石

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摘要

A new kind of organosilane (1,6-bis (diethyl(3-trimethoxysilylpropyl)ammonium) hexane bromide) with a gemini-type structure was prepared and used as a mesoporogen for the synthesis of hierarchical porous ZSM-5 zeolite. There are two quaternary ammonium centers along with double hydrolysable -RSi(OMe)3 fragments in the organosilane, which results in a strong interaction between this mesoporogen and silica-alumina gel. The organosilane can be easily incorporated into ZSM-5 zeolite structure during the crystallization process, and it was finally removed by calcination leading to secondary pores in ZSM-5. The synthesized ZSM-5 has been systematically studied by XRD, nitrogen adsorption, SEM, TEM, TG and solid-state one-dimensional (1D) and two-dimensional (2D) NMR, which reveals information on its detailed structure. It has a hierarchical porosity system, which combines the intrinsic micropores coming from the crystalline structure and irregular mesopores created by the organosilane template. Moreover, the mesoposity including pore size and volume within ZSM-5 can be systematically tuned by changing the organosilane/TEOS ratios, which confirms this organosilane has high flexibility of using as template for the synthesis of hierarchical porous zeolite.
机译:制备了一种具有双子型结构的新型有机硅烷(1,6-双(二乙基(3-三甲氧基甲硅烷基丙基)铵)己烷溴化物),并将其用作介孔原,用于合成多孔ZSM-5分子筛。在有机硅烷中有两个季铵中心以及两个可水解的-RSi(OMe)3片段,这导致该介孔原与二氧化硅-氧化铝凝胶之间发生了强烈的相互作用。在结晶过程中,有机硅烷很容易掺入ZSM-5沸石结构中,最后通过煅烧将其除去,从而在ZSM-5中形成次级孔。通过XRD,氮吸附,SEM,TEM,TG和固态一维(1D)和二维(2D)NMR对合成的ZSM-5进行了系统的研究,揭示了其详细的结构信息。它具有分层的孔隙度系统,该系统结合了来自晶体结构的固有微孔和有机硅烷模板生成的不规则中孔。此外,通过改变有机硅烷/ TEOS的比例,可以系统地调节ZSM-5中包括孔径和体积在内的介孔性,这证实了该有机硅烷具有用作模板用于合成多孔沸石的高度灵活性。

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