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Several Factors Affectingthe Novel Synthesis of Mesoporous Aluminosilicate MCM-41 through Non-hydrothermal Conditions

机译:非水热条件下介孔铝硅酸盐MCM-41新型合成的几个影响因素

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摘要

In order to elucidate the effect of synthesis conditions of Al-MCM-41 on the characteristics of the resultant samples, Al-MCM-41 samples were synthesized through non-hydrothermal reactions under diverse conditions. The following conditions were found to be favorable to prepare Al-MCM-41 with well ordered 2D-hexagonal structure from the reaction mixtures of lower Si/Al ratios: simultaneous addition of Si and Al sources into the solution containing both template of surfactant and anti-foaming agent, in neutral to acidic media (pH 3-7), at temperatures above Krafft point of the surfactant, and under vigorous stirring. These conditions may be associated with assembly of aluminosilicate sources with uniform composition (i.e., constant Si/Al ratio) around the template micelles, promoting hydrolysis and/or condensation of aluminosilicate and forming Al-MCM-41 with highly-ordered structures. Relatively weak acid sites are mainly consisted of Al-MCM-41 and similar distributions of acid strength are observed for the samples with different Si/Al species. Dealkylation reactions of 1,3,5-triisopropylbenzene, which are well known to proceed on Bronsted acid sites are catalyzed more effectively on Al-MCM-41 samples than on HY-zeolites. This means that at least, a part of Al was incorporated into the silica framework of MCM-41 structure as tetrahedrally coordinated species in Al-MCM-41 samples prepared in the present study.
机译:为了阐明Al-MCM-41的合成条件对所得样品特性的影响,在不同条件下通过非水热反应合成了Al-MCM-41样品。发现以下条件有利于从较低Si / Al比的反应混合物中制备具有良好有序2D六方结构的Al-MCM-41:将Si和Al源同时添加到含有表面活性剂和抗模板剂的溶液中-在中性至酸性介质中(pH 3-7),在高于表面活性剂Krafft点的温度下,并在剧烈搅拌下的发泡剂。这些条件可能与在模板胶束周围具有均匀组成(即恒定的Si / Al比)的硅铝酸盐源的组装有关,促进了硅铝酸盐的水解和/或缩合并形成具有高度有序结构的Al-MCM-41。相对较弱的酸位主要由Al-MCM-41组成,对于具有不同Si / Al物种的样品,观察到的酸强度分布相似。众所周知,在布朗斯台德酸位点进行的1,3,5-三异丙基苯的脱烷基反应在Al-MCM-41样品上比在HY沸石上更有效地催化。这意味着在本研究中制备的Al-MCM-41样品中,至少有一部分Al作为四面体配位物质掺入了MCM-41结构的二氧化硅骨架中。

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