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Green synthesis of low-silica CHA zeolite without organic structural directing agents, fluoride media and seeds
Microporous and Mesoporous Materials ( IF 5.2 ) Pub Date : 2020-09-18 , DOI: 10.1016/j.micromeso.2020.110618
Xiaojun Deng , Ping Zhou , Xiayan Yan , Renjin Xiong , Huaqin Kou , Wenhua Luo

To spare the use of OSDA and fluorides, for the sake of reducing cost and environmental conservation, a green and efficient synthesis recipe of low-silica CHA zeolites has been demonstrated, without using seeds or any other zeolites. The main factors that determine the formation of CHA zeolites have been investgated systemmatically, and several rules are obtained. (i) just considering simple memallic cations acting as the SDA, K+ is indispensable for the formation of CHA framework, with noting that K+ can also direct to MER topology. (ii) working as catalyst or minerization agent, OH and F function almost identically, but when the concentration of F has reached a really high level or even only Fwas used, CHA framework can not form because the intermediate fluoride complexes are inclined to produce small melecules of fluoride salts with morderate solubility over to enter the zeolite framework. (iii) at conditions of this work, the second stirring after the RT aging should be adopted since the contrastive tests have showed the benifits of the second stirring in making fewer or smaller impurity grains. (iv) when the concentration of K+is too high in reactive gels, with the other same conditions, MER over CHA framework is preferentially to form. (v) it is reasonable to consider the as-synthesized K-CHA materials can be used to research the novel “trapdoor” effect later. The authors considered the discussions and conclusions would offer some beneficial references to the green synthesis of zeolites and further understanding of the mechanism of hydrothermal treatment.



中文翻译:

不含有机结构导向剂,氟化物介质和种子的绿色合成低硅CHA沸石

为了节省OSDA和氟化物的使用,为了降低成本和环境保护,已经证明了一种绿色高效的低硅CHA沸石合成配方,而无需使用种子或任何其他沸石。已经系统地研究了确定CHA沸石形成的主要因素,并获得了一些规则。(i)仅考虑简单的阳离子阳离子作为SDA,K +对于CHA框架的形成是必不可少的,并注意到K +也可以直接导向MER拓扑。(ⅱ)工作作为催化剂或minerization剂,OH -和F -功能几乎相同,但是,当F的浓度-已经达到了非常高的水平,甚至仅F使用−时,CHA骨架无法形成,因为中间的氟化物络合物倾向于生成小分子的氟化物盐,并具有中等溶解度,从而进入沸石骨架。(iii)在这项工作的条件下,应采用RT老化后的第二次搅拌,因为对比试验表明第二次搅拌的好处是可以减少或减少杂质颗粒的数量。(iv)当K +的浓度如果在其他条件相同的情况下,反应性凝胶的分子量太高,则优先形成MER而不是CHA骨架。(v)有理由考虑将合成后的K-CHA材料用于以后研究新颖的“活板门”效应。作者认为,这些讨论和结论将为沸石的绿色合成以及对水热处理机理的进一步理解提供有益的参考。

更新日期:2020-10-02
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