Chao Hu , Chuang Liu , Wenhua Fu , Zhiqing Yuan , Zhendong Wang , Weimin Yang
{"title":"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","authors":"Chao Hu , Chuang Liu , Wenhua Fu , Zhiqing Yuan , Zhendong Wang , Weimin Yang","doi":"10.1016/j.micromeso.2025.113650","DOIUrl":null,"url":null,"abstract":"<div><div>The chemical composition of <strong>IWV</strong>-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 <strong>IWV</strong> zeolite has aroused continuous interest. Despite all the progress, it's still challenging to prepare Ge-<strong>IWV</strong> zeolite with tunable Ge content and high product yield. In this contribution, we report the high yield (>85 %) synthesis of aluminogermanosilicate <strong>IWV</strong> 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 <strong>IWV</strong> zeolites can be obtained in the Si/Ge ratio range of 2.5–10. The physicochemical properties of <strong>IWV</strong> 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 <strong>IWV</strong> 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), <strong>IWV</strong> 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 <strong>IWV</strong> zeolites.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"394 ","pages":"Article 113650"},"PeriodicalIF":4.8000,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"High yield synthesis and catalytic performance of aluminogermanosilicate IWV zeolite with tunable Ge content\",\"authors\":\"Chao Hu , Chuang Liu , Wenhua Fu , Zhiqing Yuan , Zhendong Wang , Weimin Yang\",\"doi\":\"10.1016/j.micromeso.2025.113650\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The chemical composition of <strong>IWV</strong>-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 <strong>IWV</strong> zeolite has aroused continuous interest. Despite all the progress, it's still challenging to prepare Ge-<strong>IWV</strong> zeolite with tunable Ge content and high product yield. In this contribution, we report the high yield (>85 %) synthesis of aluminogermanosilicate <strong>IWV</strong> 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 <strong>IWV</strong> zeolites can be obtained in the Si/Ge ratio range of 2.5–10. The physicochemical properties of <strong>IWV</strong> 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 <strong>IWV</strong> 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), <strong>IWV</strong> 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 <strong>IWV</strong> zeolites.</div></div>\",\"PeriodicalId\":392,\"journal\":{\"name\":\"Microporous and Mesoporous Materials\",\"volume\":\"394 \",\"pages\":\"Article 113650\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2025-04-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Microporous and Mesoporous Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1387181125001647\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Microporous and Mesoporous Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1387181125001647","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
High yield synthesis and catalytic performance of aluminogermanosilicate IWV zeolite with tunable Ge content
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.
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.