{"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, , , Daxin Jiang, , , Xianliang Song, , , Rui Li*, , and , Yulong Wu*, ","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 < 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 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, , , Daxin Jiang, , , Xianliang Song, , , Rui Li*, , and , Yulong Wu*, \",\"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 < 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 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}
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.
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.