Synthesis and characterisation of zeolites using saturated cyclic amines as structure-directing agents

H. Jongkind, K.P. Datema, S. Nabuurs, A. Seive, W.H.J. Stork
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引用次数: 26

Abstract

A synthesis route to obtain high-silica MOR using cyclic amines as structure-directing agents is described. As far as we know, the use of these structure-directing agents for the synthesis of high silica MOR is not described elsewhere.

The pore size of the synthesised products (zeolite MOR, FER and mixtures of zeolite MOR and FER), was related to the ring size of the organic structure-directing agent in the reaction mixture. Various saturated cyclic amines were used. Pure high-silica MOR of high crystallinity was obtained via direct synthesis using hexa- and heptamethyleneimine. In addition, high-silica FER was prepared among others with pyrrolidine. A mixture of MOR and FER was synthesised in the presence of piperidine. The materials were characterised and the catalytic performance of the high silica MOR was evaluated.

Catalysts prepared with direct synthesis of high-silica MOR as base material were active in the isomerisation of pentane and hexane. Presumably the direct-synthesis high-silica MOR samples were somewhat less active than conventional MOR (dealuminated by leaching to the same Si/Al ratio SAR), because of a lower accessibility of acid sites. The lower accessibility of the direct synthesis mordenite may be due to amorphous material. Other explanations are that extra-framework aluminum species were formed during calcination and preferential aluminium siting in these MOR crystals.

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以饱和环胺为结构导向剂的沸石合成与表征
介绍了一种以环胺为结构导向剂制备高硅MOR的合成路线。据我们所知,使用这些结构导向剂合成高硅MOR在其他地方没有描述。合成产物(沸石MOR、FER以及沸石MOR和FER的混合物)的孔径与反应混合物中有机结构导向剂的环大小有关。使用了各种饱和环胺。以六亚胺和七亚胺为原料,直接合成了高结晶度的纯高硅MOR。此外,还以吡咯烷为主要原料制备了高硅fe。在哌啶的存在下合成了MOR和FER的混合物。对材料进行了表征,评价了高硅MOR的催化性能。以直接合成高硅MOR为基料制备的催化剂在戊烷和己烷异构化反应中具有较强的活性。据推测,直接合成的高硅MOR样品的活性略低于传统的MOR(通过浸出获得相同的Si/Al比SAR),因为酸位的可及性较低。直接合成丝光沸石的可及性较低可能是由于非晶态物质的存在。另一种解释是,在煅烧过程中形成了框架外铝种,并且这些MOR晶体中的铝优先定位。
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Author index Subject index Contents Investigation of organosilanes as structure-directing agents in zeolite synthesis The influence of gel properties on the kinetics of crystallization and particulate properties of MFI-type zeolities. I. The influence of time and temperature of gel ageing on the particulate properties of silicalite-1 microcrystals
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