广泛底物适用- MWCNT负载的Co-Ni合金催化剂上木质素衍生愈创木酚高效转化为环己醇

IF 7.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yuhao Yan, , , Daxin Jiang, , , Xianliang Song, , , Rui Li*, , and , Yulong Wu*, 
{"title":"广泛底物适用- MWCNT负载的Co-Ni合金催化剂上木质素衍生愈创木酚高效转化为环己醇","authors":"Yuhao Yan,&nbsp;, ,&nbsp;Daxin Jiang,&nbsp;, ,&nbsp;Xianliang Song,&nbsp;, ,&nbsp;Rui Li*,&nbsp;, and ,&nbsp;Yulong Wu*,&nbsp;","doi":"10.1021/acssuschemeng.5c05346","DOIUrl":null,"url":null,"abstract":"<p >The green production of cyclohexanol can be achieved through the hydrogenation of lignin-derived guaiacol. This work demonstrates that a Co–Ni bimetallic catalyst supported on multiwalled carbon nanotubes (Co<sub>5</sub>Ni<sub>5</sub>/MWCNT) is a promising candidate for this application. Characterization results confirm that the synergistic effects between Co and Ni enhance the reducibility, H<sub>2</sub> adsorption, and binding capability of the catalysts. A response surface model for guaiacol hydrogenation over the Co<sub>5</sub>Ni<sub>5</sub>/MWCNT was established. Under optimized conditions of 190 °C, 1 MPa initial H<sub>2</sub> pressure, and 60 min, Co<sub>5</sub>Ni<sub>5</sub>/MWCNT achieved 100% guaiacol conversion and 95.6% cyclohexanol yield. This performance surpasses four commercial catalysts (NiAl, Pd/C, Ru/C, and Pt/C) and most recent literature reports. Furthermore, Co<sub>5</sub>Ni<sub>5</sub>/MWCNT exhibits exceptional substrate versatility, enabling the efficient conversion of nine lignin derivatives to cyclohexanol-type products under optimized conditions. And the reactivity hierarchy of functional groups during hydrogenation was summarized. Alkoxy group cleavage difficulty correlates with substitution position, from easy to difficult as ortho-position &lt; meta-position &lt; para-position. Functional group cleavage from easy to difficult as alkoxy groups &lt; hydroxyl groups &lt; alkyl groups. After six cycles, the residual activity of Co<sub>5</sub>Ni<sub>5</sub>/MWCNT remained comparable to that of a fresh monometallic catalyst.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 39","pages":"16390–16402"},"PeriodicalIF":7.3000,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Broadly Substrate-Applicable Efficient Conversion of Lignin-Derived Guaiacol to Cyclohexanol over Co–Ni Alloy Catalyst Supported on MWCNT\",\"authors\":\"Yuhao Yan,&nbsp;, ,&nbsp;Daxin Jiang,&nbsp;, ,&nbsp;Xianliang Song,&nbsp;, ,&nbsp;Rui Li*,&nbsp;, and ,&nbsp;Yulong Wu*,&nbsp;\",\"doi\":\"10.1021/acssuschemeng.5c05346\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The green production of cyclohexanol can be achieved through the hydrogenation of lignin-derived guaiacol. This work demonstrates that a Co–Ni bimetallic catalyst supported on multiwalled carbon nanotubes (Co<sub>5</sub>Ni<sub>5</sub>/MWCNT) is a promising candidate for this application. Characterization results confirm that the synergistic effects between Co and Ni enhance the reducibility, H<sub>2</sub> adsorption, and binding capability of the catalysts. A response surface model for guaiacol hydrogenation over the Co<sub>5</sub>Ni<sub>5</sub>/MWCNT was established. Under optimized conditions of 190 °C, 1 MPa initial H<sub>2</sub> pressure, and 60 min, Co<sub>5</sub>Ni<sub>5</sub>/MWCNT achieved 100% guaiacol conversion and 95.6% cyclohexanol yield. This performance surpasses four commercial catalysts (NiAl, Pd/C, Ru/C, and Pt/C) and most recent literature reports. Furthermore, Co<sub>5</sub>Ni<sub>5</sub>/MWCNT exhibits exceptional substrate versatility, enabling the efficient conversion of nine lignin derivatives to cyclohexanol-type products under optimized conditions. And the reactivity hierarchy of functional groups during hydrogenation was summarized. Alkoxy group cleavage difficulty correlates with substitution position, from easy to difficult as ortho-position &lt; meta-position &lt; para-position. Functional group cleavage from easy to difficult as alkoxy groups &lt; hydroxyl groups &lt; alkyl groups. After six cycles, the residual activity of Co<sub>5</sub>Ni<sub>5</sub>/MWCNT remained comparable to that of a fresh monometallic catalyst.</p>\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":\"13 39\",\"pages\":\"16390–16402\"},\"PeriodicalIF\":7.3000,\"publicationDate\":\"2025-08-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acssuschemeng.5c05346\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acssuschemeng.5c05346","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

摘要

木质素衍生愈创木酚的加氢可以实现环己醇的绿色生产。这项工作表明,在多壁碳纳米管(Co5Ni5/MWCNT)上负载的Co-Ni双金属催化剂是一种很有前途的应用候选人。表征结果证实,Co和Ni之间的协同作用增强了催化剂的还原性、H2吸附能力和结合能力。建立了愈创木酚在Co5Ni5/MWCNT上加氢的响应面模型。在190℃、1 MPa初始H2压力、60 min的优化条件下,Co5Ni5/MWCNT的愈创木酚转化率为100%,环己醇收率为95.6%。这种性能超过了四种商业催化剂(NiAl, Pd/C, Ru/C和Pt/C)和最近的文献报道。此外,Co5Ni5/MWCNT具有出色的底物通用性,能够在优化条件下将9种木质素衍生物有效地转化为环己醇型产品。总结了官能团在加氢过程中的反应性等级。烷氧基裂解难易程度与取代位有关,由易到难依次为邻位&间位&对位。官能团拆分由易到难依次为烷氧基、羟基、烷基。经过6次循环后,Co5Ni5/MWCNT的剩余活性仍然与新鲜的单金属催化剂相当。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Broadly Substrate-Applicable Efficient Conversion of Lignin-Derived Guaiacol to Cyclohexanol over Co–Ni Alloy Catalyst Supported on MWCNT

Broadly Substrate-Applicable Efficient Conversion of Lignin-Derived Guaiacol to Cyclohexanol over Co–Ni Alloy Catalyst Supported on MWCNT

The green production of cyclohexanol can be achieved through the hydrogenation of lignin-derived guaiacol. This work demonstrates that a Co–Ni bimetallic catalyst supported on multiwalled carbon nanotubes (Co5Ni5/MWCNT) is a promising candidate for this application. Characterization results confirm that the synergistic effects between Co and Ni enhance the reducibility, H2 adsorption, and binding capability of the catalysts. A response surface model for guaiacol hydrogenation over the Co5Ni5/MWCNT was established. Under optimized conditions of 190 °C, 1 MPa initial H2 pressure, and 60 min, Co5Ni5/MWCNT achieved 100% guaiacol conversion and 95.6% cyclohexanol yield. This performance surpasses four commercial catalysts (NiAl, Pd/C, Ru/C, and Pt/C) and most recent literature reports. Furthermore, Co5Ni5/MWCNT exhibits exceptional substrate versatility, enabling the efficient conversion of nine lignin derivatives to cyclohexanol-type products under optimized conditions. And the reactivity hierarchy of functional groups during hydrogenation was summarized. Alkoxy group cleavage difficulty correlates with substitution position, from easy to difficult as ortho-position < meta-position < para-position. Functional group cleavage from easy to difficult as alkoxy groups < hydroxyl groups < alkyl groups. After six cycles, the residual activity of Co5Ni5/MWCNT remained comparable to that of a fresh monometallic catalyst.

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
ACS Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
×
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