对大孔隙沸石 Beta 进行选择性脱铝以有效利用勃朗斯特德酸位点

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-10-16 DOI:10.1016/j.jcat.2024.115796
Pranit Samanta, Mohd. Ussama, Gourav Shrivastav, M. Ali Haider, K.K. Pant, Manjesh Kumar
{"title":"对大孔隙沸石 Beta 进行选择性脱铝以有效利用勃朗斯特德酸位点","authors":"Pranit Samanta,&nbsp;Mohd. Ussama,&nbsp;Gourav Shrivastav,&nbsp;M. Ali Haider,&nbsp;K.K. Pant,&nbsp;Manjesh Kumar","doi":"10.1016/j.jcat.2024.115796","DOIUrl":null,"url":null,"abstract":"<div><div>Tuning of Al sites through spatial and geometric distribution is a novel pursuit for deterministic catalytic performance. To design an efficient Zeolite Beta for phenol alkylation with optimal physicochemical attributes, we conducted a systematic study with a series of dicarboxylic acids to selectively extract the framework and/or non-framework Aluminium. Herein, the post-synthetic treatment resulted in dealuminated catalysts of silicon-to-aluminum ratio ∼15–53. Extensive Al and Si NMR studies glean the selective extraction of aluminum from the zeolitic framework along with recomposition in T sites. The potency study alludes to the convoluted role of pH, chelating ability, and/or site accessibility for complexation. The differentiated Al extraction results in the emergence of unique super-strong acid sites. The novelty of our approach was established using phenol alkylation with cyclohexanol wherein we observed the highest conversion and desired C<img>C alkylated product formation for the malonic acid-treated Zeolite Beta.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115796"},"PeriodicalIF":6.5000,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective dealumination of large pore Zeolite Beta for effective Brønsted acid site utilization\",\"authors\":\"Pranit Samanta,&nbsp;Mohd. Ussama,&nbsp;Gourav Shrivastav,&nbsp;M. Ali Haider,&nbsp;K.K. Pant,&nbsp;Manjesh Kumar\",\"doi\":\"10.1016/j.jcat.2024.115796\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Tuning of Al sites through spatial and geometric distribution is a novel pursuit for deterministic catalytic performance. To design an efficient Zeolite Beta for phenol alkylation with optimal physicochemical attributes, we conducted a systematic study with a series of dicarboxylic acids to selectively extract the framework and/or non-framework Aluminium. Herein, the post-synthetic treatment resulted in dealuminated catalysts of silicon-to-aluminum ratio ∼15–53. Extensive Al and Si NMR studies glean the selective extraction of aluminum from the zeolitic framework along with recomposition in T sites. The potency study alludes to the convoluted role of pH, chelating ability, and/or site accessibility for complexation. The differentiated Al extraction results in the emergence of unique super-strong acid sites. The novelty of our approach was established using phenol alkylation with cyclohexanol wherein we observed the highest conversion and desired C<img>C alkylated product formation for the malonic acid-treated Zeolite Beta.</div></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"440 \",\"pages\":\"Article 115796\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-10-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951724005098\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951724005098","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

通过空间和几何分布调节铝位点是实现确定性催化性能的一种新方法。为了设计出具有最佳物理化学属性的高效沸石 Beta 用于苯酚烷基化,我们使用一系列二羧酸进行了系统研究,以选择性地提取框架和/或非框架铝。在这里,后合成处理产生了硅铝比为 15-53 的脱铝催化剂。大量的铝和硅核磁共振研究表明,铝从沸石框架中被选择性地提取出来,并在 T 位点上重新合成。效力研究表明,pH 值、螯合能力和/或络合位点的可及性具有复杂的作用。不同的铝萃取导致了独特的超强酸性位点的出现。我们使用苯酚与环己醇进行烷基化,观察到丙二酸处理的沸石 Beta 转化率最高,并形成了所需的 CC 烷基化产物,这证明了我们的方法具有新颖性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

摘要图片

摘要图片

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
Selective dealumination of large pore Zeolite Beta for effective Brønsted acid site utilization
Tuning of Al sites through spatial and geometric distribution is a novel pursuit for deterministic catalytic performance. To design an efficient Zeolite Beta for phenol alkylation with optimal physicochemical attributes, we conducted a systematic study with a series of dicarboxylic acids to selectively extract the framework and/or non-framework Aluminium. Herein, the post-synthetic treatment resulted in dealuminated catalysts of silicon-to-aluminum ratio ∼15–53. Extensive Al and Si NMR studies glean the selective extraction of aluminum from the zeolitic framework along with recomposition in T sites. The potency study alludes to the convoluted role of pH, chelating ability, and/or site accessibility for complexation. The differentiated Al extraction results in the emergence of unique super-strong acid sites. The novelty of our approach was established using phenol alkylation with cyclohexanol wherein we observed the highest conversion and desired CC alkylated product formation for the malonic acid-treated Zeolite Beta.
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 Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
期刊最新文献
Detailing the redox ability of supported Pt-Sn and Pt-In catalysts for CO2-assisted PDH Minimizing CoxMn1-xO content in a Co2C catalyst for low CO2 selectivity in Fischer-Tropsch synthesis to olefins Enhancement of CuBr-based catalysts for aerobic alcohol oxidation enabled by rational design of bifunctional ligands featuring both a N-alkyl substituted ethylenediamine skeleton and a TEMPO moiety Selenium-modulated Pt/Al2O3 electronic structure induces deactivation during catalytic CO oxidation Enhanced metal-support interaction over Pd-Au/TiO2 catalysts for vinyl acetate synthesis
×
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
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 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 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1