High yield synthesis and catalytic performance of aluminogermanosilicate IWV zeolite with tunable Ge content

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
Chao Hu , Chuang Liu , Wenhua Fu , Zhiqing Yuan , Zhendong Wang , Weimin Yang
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Abstract

The chemical composition of IWV-type zeolite has extended from traditional aluminosilicate to germanosilicate. Due to the unique 12 × 12-ring channel system and the feasibility of structural transformation based on the lability of Ge-O bonds, the synthesis of Ge-containing IWV zeolite has aroused continuous interest. Despite all the progress, it's still challenging to prepare Ge-IWV zeolite with tunable Ge content and high product yield. In this contribution, we report the high yield (>85 %) synthesis of aluminogermanosilicate IWV zeolite using commercially available 1,1,3,5-tetramethylpiperidinium hydroxide (1,1,3,5-TMPOH) as organic structure-directing agent (OSDA). The effects of synthesis parameters, such as the Si/Ge molar ratio, Al content and dilution of the initial gel are investigated. Highly crystalline IWV zeolites can be obtained in the Si/Ge ratio range of 2.5–10. The physicochemical properties of IWV zeolites with various Ge contents are studied using multiple characterization techniques. Like in most germanosilicate zeolites, Ge atoms are preferentially incorporated into the double-four-ring (D4R) units. The IWV zeolites are endowed with nanoplate-like crystal morphology, high specific surface area and strong acidity, thus can be utilized as catalysts for the conversion of bulky molecules. In the catalytic cracking of 1,3,5-triisopropyl benzene (TiPB), IWV zeolites show high conversion and prolonged lifetime, superior to Beta zeolite. Moreover, the catalytic performance strongly depends on the Ge content and acidity of the IWV zeolites.

Abstract Image

锗含量可调铝-锗硅酸盐IWV沸石的高产率合成及其催化性能
iwv型沸石的化学成分已由传统的铝硅酸盐扩展到锗硅酸盐。由于其独特的12 × 12环通道体系和基于Ge-O键不稳定性进行结构转化的可行性,含ge IWV沸石的合成引起了人们的持续关注。尽管取得了这些进展,但制备锗含量可调、产品收率高的Ge- iwv沸石仍然具有挑战性。在这篇文章中,我们报道了用市售的1,1,3,5-四甲基氢氧化铵(1,1,3,5- tmpoh)作为有机结构导向剂(OSDA)高产率(> 85%)合成铝-德国硅酸盐IWV沸石。考察了Si/Ge摩尔比、Al含量和初始凝胶稀释度等合成参数的影响。在Si/Ge比为2.5 ~ 10的范围内,可以得到高结晶的IWV沸石。采用多种表征技术研究了不同锗含量的IWV沸石的理化性质。与大多数锗硅酸盐沸石一样,锗原子优先结合到双四环(D4R)单元中。IWV分子筛具有纳米片状晶体形态、高比表面积和强酸性,可作为大分子转化的催化剂。在1,3,5-三异丙基苯(TiPB)的催化裂化中,IWV分子筛表现出较高的转化率和较长的寿命,优于β分子筛。此外,催化性能强烈依赖于锗含量和IWV沸石的酸度。
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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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