由二二元磷钨酸酯和Hβ沸石组成的氧化还原-酸协同双功能催化剂合成乙酰丙酸正丁酯和琥珀酸

IF 4 3区 化学 Q2 CHEMISTRY, PHYSICAL
Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-04-21 DOI:10.1039/d5cy01399b
Anjali Patel , Margi Joshi
{"title":"由二二元磷钨酸酯和Hβ沸石组成的氧化还原-酸协同双功能催化剂合成乙酰丙酸正丁酯和琥珀酸","authors":"Anjali Patel ,&nbsp;Margi Joshi","doi":"10.1039/d5cy01399b","DOIUrl":null,"url":null,"abstract":"<div><div>In the present work, a bifunctional heterogeneous catalyst was designed by integrating the redox active centres of lacunary phosphotungstates with the tunable acidity and stability of the zeolite Hβ framework. The catalyst, dilacunary phosphotungstate anchored to zeolite Hβ, was synthesized and characterized using NH<sub>3</sub>-TPD, EDX, FTIR, BET, XRD, <sup>29</sup>Si NMR and HRTEM analyses. The proposed interaction between the redox-active PW<sub>10</sub> units and the surface silanol groups of zeolite Hβ enabled dual catalytic functionality. This efficiently catalyses both the esterification and the oxidation of levulinic acid under mild and green conditions for the selective synthesis of <em>n</em>-butyl levulinate (96% selectivity) and succinic acid (100% selectivity), respectively. Notably, this study represents the first successful effort to achieve complete selectivity toward succinic acid. Validation of the kinetic mechanism was performed, followed by recycling experiments. The alignment of this work with sustainable development goals highlights its broader societal relevance, positioning the catalyst as a promising platform for future green and energy-efficient transformations.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3236-3254"},"PeriodicalIF":4.0000,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Redox–acid cooperative bifunctional catalysts comprising dilacunary phosphotungstates and zeolite Hβ for the synthesis of n-butyl levulinate and succinic acid\",\"authors\":\"Anjali Patel ,&nbsp;Margi Joshi\",\"doi\":\"10.1039/d5cy01399b\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In the present work, a bifunctional heterogeneous catalyst was designed by integrating the redox active centres of lacunary phosphotungstates with the tunable acidity and stability of the zeolite Hβ framework. The catalyst, dilacunary phosphotungstate anchored to zeolite Hβ, was synthesized and characterized using NH<sub>3</sub>-TPD, EDX, FTIR, BET, XRD, <sup>29</sup>Si NMR and HRTEM analyses. The proposed interaction between the redox-active PW<sub>10</sub> units and the surface silanol groups of zeolite Hβ enabled dual catalytic functionality. This efficiently catalyses both the esterification and the oxidation of levulinic acid under mild and green conditions for the selective synthesis of <em>n</em>-butyl levulinate (96% selectivity) and succinic acid (100% selectivity), respectively. Notably, this study represents the first successful effort to achieve complete selectivity toward succinic acid. Validation of the kinetic mechanism was performed, followed by recycling experiments. The alignment of this work with sustainable development goals highlights its broader societal relevance, positioning the catalyst as a promising platform for future green and energy-efficient transformations.</div></div>\",\"PeriodicalId\":66,\"journal\":{\"name\":\"Catalysis Science & Technology\",\"volume\":\"16 9\",\"pages\":\"Pages 3236-3254\"},\"PeriodicalIF\":4.0000,\"publicationDate\":\"2026-05-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Science & Technology\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/org/science/article/pii/S2044475326001711\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2026/4/21 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Science & Technology","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S2044475326001711","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2026/4/21 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

在本工作中,设计了一种双功能的非均相催化剂,该催化剂将腔隙磷钨酸盐的氧化还原活性中心与沸石Hβ框架的可调酸度和稳定性相结合。合成了锚定在Hβ分子筛上的二二元磷钨酸盐催化剂,并通过NH3-TPD、EDX、FTIR、BET、XRD、29Si NMR和HRTEM等分析对催化剂进行了表征。提出的氧化还原活性PW10单元与沸石Hβ表面硅醇基之间的相互作用实现了双催化功能。在温和和绿色条件下有效催化乙酰丙酸的酯化反应和氧化反应,分别选择性合成乙酰丙酸正丁酯(96%选择性)和琥珀酸(100%选择性)。值得注意的是,这项研究首次成功地实现了对琥珀酸的完全选择性。进行了动力学机理验证,并进行了循环实验。这项工作与可持续发展目标的一致性突出了其更广泛的社会相关性,将催化剂定位为未来绿色和节能转型的有前途的平台。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Redox–acid cooperative bifunctional catalysts comprising dilacunary phosphotungstates and zeolite Hβ for the synthesis of n-butyl levulinate and succinic acid

Redox–acid cooperative bifunctional catalysts comprising dilacunary phosphotungstates and zeolite Hβ for the synthesis of n-butyl levulinate and succinic acid
In the present work, a bifunctional heterogeneous catalyst was designed by integrating the redox active centres of lacunary phosphotungstates with the tunable acidity and stability of the zeolite Hβ framework. The catalyst, dilacunary phosphotungstate anchored to zeolite Hβ, was synthesized and characterized using NH3-TPD, EDX, FTIR, BET, XRD, 29Si NMR and HRTEM analyses. The proposed interaction between the redox-active PW10 units and the surface silanol groups of zeolite Hβ enabled dual catalytic functionality. This efficiently catalyses both the esterification and the oxidation of levulinic acid under mild and green conditions for the selective synthesis of n-butyl levulinate (96% selectivity) and succinic acid (100% selectivity), respectively. Notably, this study represents the first successful effort to achieve complete selectivity toward succinic acid. Validation of the kinetic mechanism was performed, followed by recycling experiments. The alignment of this work with sustainable development goals highlights its broader societal relevance, positioning the catalyst as a promising platform for future green and energy-efficient transformations.
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
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
×
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
小红书