Non‐Oxidative Dehydroaromatization of Linear Alkanes on Intermetallic Nanoparticles

IF 3.8 3区 化学 Q2 CHEMISTRY, PHYSICAL
ChemCatChem Pub Date : 2024-09-02 DOI:10.1002/cctc.202401263
Ranjan K. Behera, Andrew R. Lamkins, Minda Chen, Raghu V. Maligal-Ganesh, Jiaqi Yu, Wenyu Huang
{"title":"Non‐Oxidative Dehydroaromatization of Linear Alkanes on Intermetallic Nanoparticles","authors":"Ranjan K. Behera, Andrew R. Lamkins, Minda Chen, Raghu V. Maligal-Ganesh, Jiaqi Yu, Wenyu Huang","doi":"10.1002/cctc.202401263","DOIUrl":null,"url":null,"abstract":"There has been significant interest in developing new catalytic systems to convert linear chain alkanes into olefins and aromatics. In the case of higher alkanes (≥ C6), the production of aromatic compounds such as benzene‐toluene‐xylenes is highly desirable. However, as the length of the carbon chain increases, the dehydrogenation process becomes more complex, not only due to the challenges of C‐H activation but also the need for selectivity towards the desired products by the possibility of side reactions such as isomerization and cracking. Here, we present a detailed analysis of the dehydroaromatization of n‐hexane, n‐heptane, and n‐octane, using PtSn intermetallic nanoparticles supported on SBA‐15 as the catalyst. Through in‐situ spectroscopic and kinetic analysis, we have probed into the reaction kinetics, catalyst deactivation, and a mechanistic understanding of the dehydroaromatization process on the surface of the PtSn intermetallic nanoparticles. Introducing Sn has been shown to be crucial not only for enhancement of catalytic activity, but also for higher aromatics selectivity and stability on stream. Furthermore, the analysis of dehydroaromatization reaction rates of reactant and possible intermediates indicates that the dehydroaromatization of n‐hexane to benzene likely proceeds through initial dehydrogenation steps followed by ring closing.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"18 1","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemCatChem","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/cctc.202401263","RegionNum":3,"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

Abstract

There has been significant interest in developing new catalytic systems to convert linear chain alkanes into olefins and aromatics. In the case of higher alkanes (≥ C6), the production of aromatic compounds such as benzene‐toluene‐xylenes is highly desirable. However, as the length of the carbon chain increases, the dehydrogenation process becomes more complex, not only due to the challenges of C‐H activation but also the need for selectivity towards the desired products by the possibility of side reactions such as isomerization and cracking. Here, we present a detailed analysis of the dehydroaromatization of n‐hexane, n‐heptane, and n‐octane, using PtSn intermetallic nanoparticles supported on SBA‐15 as the catalyst. Through in‐situ spectroscopic and kinetic analysis, we have probed into the reaction kinetics, catalyst deactivation, and a mechanistic understanding of the dehydroaromatization process on the surface of the PtSn intermetallic nanoparticles. Introducing Sn has been shown to be crucial not only for enhancement of catalytic activity, but also for higher aromatics selectivity and stability on stream. Furthermore, the analysis of dehydroaromatization reaction rates of reactant and possible intermediates indicates that the dehydroaromatization of n‐hexane to benzene likely proceeds through initial dehydrogenation steps followed by ring closing.
线性烷烃在金属间纳米颗粒上的非氧化脱氢芳香化反应
人们对开发新的催化系统以将线性链烷烃转化为烯烃和芳香烃非常感兴趣。就高碳烷烃(≥ C6)而言,生产苯-甲苯-二甲苯等芳香族化合物是非常理想的。然而,随着碳链长度的增加,脱氢过程也变得更加复杂,这不仅是由于 C-H 活化所带来的挑战,还因为可能发生异构化和裂解等副反应而需要对所需产物具有选择性。在此,我们以支撑在 SBA-15 上的 PtSn 金属间纳米粒子为催化剂,详细分析了正己烷、正庚烷和正辛烷的脱氢芳构化过程。通过原位光谱和动力学分析,我们探究了反应动力学、催化剂失活以及 PtSn 金属间纳米颗粒表面脱氢芳构化过程的机理。研究表明,引入 Sn 不仅对提高催化活性至关重要,而且对提高芳烃选择性和流稳定性也至关重要。此外,对反应物和可能的中间产物的脱氢芳香化反应速率的分析表明,正己烷到苯的脱氢芳香化反应可能是通过最初的脱氢步骤进行的,然后是闭环。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
×
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:481959085
Book学术官方微信