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, Tatiana Botero, Roger Solano, Carlos Mendoza, 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, Tatiana Botero, Roger Solano, Carlos Mendoza, 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}
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.
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.