Preparation of Al-rich hierarchical zeolites by conventional alkali treatment: Defects as mesopore directing agents

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
Xingyang Li, Dandan Zhang, Quanwei Zheng, Jiakui Chang, Xuan Liu, Renchun Yang, Meng Pan
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Abstract

In industry, it is highly desired to prepare Al-rich hierarchical zeolites by conventional alkali treatment without the use of costly chemical and special process. Here we provide an alternative strategy in which crystal defects are employed as mesopore directing agents. The effective elimination of the intracrystalline defects induces the generation of mesoporous structure in the alkali treatment process. Thus, the limitation originating from the framework Si/Al ratio of parent zeolite is circumvented. This strategy holds all merits of the conventional alkali treatment approach, which is industrially unfavorable. As an example, the Al-rich hierarchical ZSM-5 zeolites with very low Si/Al ratios were successfully prepared. The obtained Al-rich hierarchical zeolites were characterized by XRD, XRF, SEM, TEM, N2 adsorption-desorption, in-situ IR, MAS NMR and NH3-TPD. The results showed that Si/Al ratios of the prepared hierarchical ZSM-5 zeolites were around 10 and the increases of external surface area and mesoporous volume were up to 2.6 and 3.7 times respectively in comparison with parent zeolite. Moreover, the constructed mesopores were interconnected open channels. In the catalytic cracking of 1,3,5-triisopropylbenzene, the Al-rich hierarchical ZSM-5 zeolites exhibited an excellent performance because of the improved diffusion of reactant and product.
常规碱处理制备富铝分级沸石:作为介孔导向剂的缺陷
在工业上,人们迫切希望通过常规碱处理制备富铝分级沸石,而不使用昂贵的化学和特殊工艺。在这里,我们提供了一种替代策略,其中晶体缺陷被用作介孔导向剂。在碱处理过程中,有效消除晶内缺陷导致介孔结构的产生。这样就绕过了母体分子筛硅铝比的限制。该策略具有传统碱处理方法的所有优点,这在工业上是不利的。成功制备了硅铝比极低的富铝级联ZSM-5分子筛。采用XRD、XRF、SEM、TEM、N2吸附-脱附、原位IR、MAS NMR和NH3-TPD等手段对所制得的富铝层叠沸石进行了表征。结果表明,制备的分级ZSM-5分子筛的Si/Al比在10左右,外表面积和介孔体积分别比母体分子筛增大2.6倍和3.7倍。此外,所构建的中孔是相互连接的开放通道。在1,3,5-三异丙苯催化裂化过程中,富铝分级ZSM-5分子筛由于改善了反应物和生成物的扩散而表现出优异的性能。
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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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