利用渐进式加热高效合成纳米Y型沸石:合成后改性及其丙烯低聚催化性能

IF 3.2 4区 材料科学 Q2 CHEMISTRY, APPLIED
Cecilia Manrique, Tatiana Botero, Roger Solano, Carlos Mendoza, Adriana Echavarría-Isaza
{"title":"利用渐进式加热高效合成纳米Y型沸石:合成后改性及其丙烯低聚催化性能","authors":"Cecilia Manrique,&nbsp;Tatiana Botero,&nbsp;Roger Solano,&nbsp;Carlos Mendoza,&nbsp;Adriana Echavarría-Isaza","doi":"10.1007/s10934-024-01703-8","DOIUrl":null,"url":null,"abstract":"<div><p>Producing nanosized zeolites Y has been restricted to a Si/Al ratio lower than 2.0, requiring prolonged crystallization periods. This study employed temperature ramps during nucleation and crystallization to synthesize nanosized zeolites Y with a Si/Al ratio of 2.4, ranging from 47 to 100 nm, in just one day. Sequential post-synthesis desilication and dealumination treatments were used to modify the pore structure and acidity of the zeolites, leading to hierarchical zeolite formation. These modifications enhanced the structural stability and porosity of the zeolites while preserving their high crystallinity. Desilicated zeolites, unlike dealuminated ones, possessed straighter and more uniform mesoporous within their crystals, with diameters smaller than 5 nm. Additionally, successive desilication produced a greater number of intracrystalline mesoporous. The solids obtained from both processes exhibited porosity within the zeolite structure connected to the external surface, potentially improving the mass transfer limitations of the original zeolite due to the lack of mesoporous. Catalysts were prepared using modified nanozeolites for evaluation in the propylene oligomerization reaction. Catalysts based on dealuminated and desilicated nanosized zeolite Y showed high conversions above 20%, especially for dealuminated zeolites with conversions of 50%. Additionally, the catalysts demonstrated selectivity towards hydrocarbons in the C5-C7 range, suggesting better diffusion and access of propylene molecules to the active sites, favoring the formation of medium-sized hydrocarbon fractions. Conversely, the formation of longer hydrocarbon chains (C12<sup>+</sup>) was not favored, possibly due to insufficient mesoporous for larger molecule diffusion and a distribution of acid sites that encourages the union of longer hydrocarbon chains.</p></div>","PeriodicalId":660,"journal":{"name":"Journal of Porous Materials","volume":"32 3","pages":"1039 - 1056"},"PeriodicalIF":3.2000,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10934-024-01703-8.pdf","citationCount":"0","resultStr":"{\"title\":\"Efficient synthesis of nanosized zeolite Y utilizing gradual heating: post-synthesis modification and their catalytic performance in propylene oligomerization\",\"authors\":\"Cecilia Manrique,&nbsp;Tatiana Botero,&nbsp;Roger Solano,&nbsp;Carlos Mendoza,&nbsp;Adriana Echavarría-Isaza\",\"doi\":\"10.1007/s10934-024-01703-8\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Producing nanosized zeolites Y has been restricted to a Si/Al ratio lower than 2.0, requiring prolonged crystallization periods. This study employed temperature ramps during nucleation and crystallization to synthesize nanosized zeolites Y with a Si/Al ratio of 2.4, ranging from 47 to 100 nm, in just one day. Sequential post-synthesis desilication and dealumination treatments were used to modify the pore structure and acidity of the zeolites, leading to hierarchical zeolite formation. These modifications enhanced the structural stability and porosity of the zeolites while preserving their high crystallinity. Desilicated zeolites, unlike dealuminated ones, possessed straighter and more uniform mesoporous within their crystals, with diameters smaller than 5 nm. Additionally, successive desilication produced a greater number of intracrystalline mesoporous. The solids obtained from both processes exhibited porosity within the zeolite structure connected to the external surface, potentially improving the mass transfer limitations of the original zeolite due to the lack of mesoporous. Catalysts were prepared using modified nanozeolites for evaluation in the propylene oligomerization reaction. Catalysts based on dealuminated and desilicated nanosized zeolite Y showed high conversions above 20%, especially for dealuminated zeolites with conversions of 50%. Additionally, the catalysts demonstrated selectivity towards hydrocarbons in the C5-C7 range, suggesting better diffusion and access of propylene molecules to the active sites, favoring the formation of medium-sized hydrocarbon fractions. Conversely, the formation of longer hydrocarbon chains (C12<sup>+</sup>) was not favored, possibly due to insufficient mesoporous for larger molecule diffusion and a distribution of acid sites that encourages the union of longer hydrocarbon chains.</p></div>\",\"PeriodicalId\":660,\"journal\":{\"name\":\"Journal of Porous Materials\",\"volume\":\"32 3\",\"pages\":\"1039 - 1056\"},\"PeriodicalIF\":3.2000,\"publicationDate\":\"2025-02-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://link.springer.com/content/pdf/10.1007/s10934-024-01703-8.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Porous Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10934-024-01703-8\",\"RegionNum\":4,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Porous Materials","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s10934-024-01703-8","RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0

摘要

生产纳米级沸石Y被限制在硅/铝比低于2.0,需要较长的结晶周期。本研究利用成核和结晶过程中的温度梯度,在一天内合成了Si/Al比为2.4的纳米级沸石Y,范围为47 ~ 100 nm。通过合成后的连续脱硅和脱铝处理,改变了沸石的孔隙结构和酸性,形成了分级沸石。这些修饰提高了沸石的结构稳定性和孔隙度,同时保持了沸石的高结晶度。脱硅沸石与脱铝沸石不同,其晶体内具有更直、更均匀的介孔,直径小于5纳米。此外,连续脱硅会产生更多的晶内介孔。通过这两种方法获得的固体在与外表面相连的沸石结构中表现出孔隙,这可能会改善由于缺乏介孔而导致的原始沸石传质限制。采用改性纳米沸石制备催化剂,对丙烯低聚反应进行了评价。以脱铝脱硅纳米沸石Y为原料制备的催化剂转化率高达20%以上,其中脱铝沸石的转化率达到50%以上。此外,催化剂对C5-C7范围内的烃类表现出选择性,表明丙烯分子更容易扩散和接近活性位点,有利于形成中等大小的烃类馏分。相反,较长的烃链(C12+)的形成并不有利,可能是由于没有足够的介孔来进行大分子的扩散,以及酸位的分布促进了较长的烃链的结合。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Efficient synthesis of nanosized zeolite Y utilizing gradual heating: post-synthesis modification and their catalytic performance in propylene oligomerization

Producing nanosized zeolites Y has been restricted to a Si/Al ratio lower than 2.0, requiring prolonged crystallization periods. This study employed temperature ramps during nucleation and crystallization to synthesize nanosized zeolites Y with a Si/Al ratio of 2.4, ranging from 47 to 100 nm, in just one day. Sequential post-synthesis desilication and dealumination treatments were used to modify the pore structure and acidity of the zeolites, leading to hierarchical zeolite formation. These modifications enhanced the structural stability and porosity of the zeolites while preserving their high crystallinity. Desilicated zeolites, unlike dealuminated ones, possessed straighter and more uniform mesoporous within their crystals, with diameters smaller than 5 nm. Additionally, successive desilication produced a greater number of intracrystalline mesoporous. The solids obtained from both processes exhibited porosity within the zeolite structure connected to the external surface, potentially improving the mass transfer limitations of the original zeolite due to the lack of mesoporous. Catalysts were prepared using modified nanozeolites for evaluation in the propylene oligomerization reaction. Catalysts based on dealuminated and desilicated nanosized zeolite Y showed high conversions above 20%, especially for dealuminated zeolites with conversions of 50%. Additionally, the catalysts demonstrated selectivity towards hydrocarbons in the C5-C7 range, suggesting better diffusion and access of propylene molecules to the active sites, favoring the formation of medium-sized hydrocarbon fractions. Conversely, the formation of longer hydrocarbon chains (C12+) was not favored, possibly due to insufficient mesoporous for larger molecule diffusion and a distribution of acid sites that encourages the union of longer hydrocarbon chains.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Journal of Porous Materials
Journal of Porous Materials 工程技术-材料科学:综合
CiteScore
4.80
自引率
7.70%
发文量
203
审稿时长
2.6 months
期刊介绍: The Journal of Porous Materials is an interdisciplinary and international periodical devoted to all types of porous materials. Its aim is the rapid publication of high quality, peer-reviewed papers focused on the synthesis, processing, characterization and property evaluation of all porous materials. The objective is to establish a unique journal that will serve as a principal means of communication for the growing interdisciplinary field of porous materials. Porous materials include microporous materials with 50 nm pores. Examples of microporous materials are natural and synthetic molecular sieves, cationic and anionic clays, pillared clays, tobermorites, pillared Zr and Ti phosphates, spherosilicates, carbons, porous polymers, xerogels, etc. Mesoporous materials include synthetic molecular sieves, xerogels, aerogels, glasses, glass ceramics, porous polymers, etc.; while macroporous materials include ceramics, glass ceramics, porous polymers, aerogels, cement, etc. The porous materials can be crystalline, semicrystalline or noncrystalline, or combinations thereof. They can also be either organic, inorganic, or their composites. The overall objective of the journal is the establishment of one main forum covering the basic and applied aspects of all porous materials.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信