Xu Yang, Zidong Huang, Wu Liu, Xu Li, Shuyi Su, Hongliang Peng, Yanxiong Fang, Jinxiang Dong, Qiming Sun
{"title":"Regioselective Upgrading of Furfural into 2-Methyl Furan over Cobalt Confined in Microporous Carbon Spheres","authors":"Xu Yang, Zidong Huang, Wu Liu, Xu Li, Shuyi Su, Hongliang Peng, Yanxiong Fang, Jinxiang Dong, Qiming Sun","doi":"10.1021/acscatal.4c07956","DOIUrl":null,"url":null,"abstract":"The selective hydrogenative upgrading of lignocellulose-derived furanic molecules into 2-methylfuran (2-MF) represents an appealing yet challenging goal, primarily due to the competing furan ring on metal surfaces, especially at low temperatures. This issue significantly limits the overall yield of 2-MF. Herein, we present an efficient regioselective strategy to maximize the 2-MF yield from furfural hydrodeoxygenation by encapsulating active cobalt species within microporous carbon spheres (Co@MCS). Both experimental results and theoretical calculations reveal that the micropores in MCS act as shape-selective fillers, guiding furfural’s access to the cobalt sites in a small, tilted configuration rather than a large, coplanar arrangement, thereby significantly suppressing the side reaction of ring hydrogenation. Remarkably, the high 2-MF productivity of 1.7 g<sub>2-MF</sub> g<sub>Cat.</sub><sup>–1</sup> h<sup>–1</sup> with nearly 100% selectivity is achieved over Co@MCS at 130 °C and 2 MPa of <i>p</i><sub>H<sub>2</sub></sub>, overcoming all previously reported results. This work provides valuable insights for designing catalysts with high selectivity for the conversion of lignin-derived platform chemicals. Furthermore, the concept of confined catalysis holds promise for broader application in other industrial catalytic processes.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"72 1","pages":""},"PeriodicalIF":11.3000,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c07956","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The selective hydrogenative upgrading of lignocellulose-derived furanic molecules into 2-methylfuran (2-MF) represents an appealing yet challenging goal, primarily due to the competing furan ring on metal surfaces, especially at low temperatures. This issue significantly limits the overall yield of 2-MF. Herein, we present an efficient regioselective strategy to maximize the 2-MF yield from furfural hydrodeoxygenation by encapsulating active cobalt species within microporous carbon spheres (Co@MCS). Both experimental results and theoretical calculations reveal that the micropores in MCS act as shape-selective fillers, guiding furfural’s access to the cobalt sites in a small, tilted configuration rather than a large, coplanar arrangement, thereby significantly suppressing the side reaction of ring hydrogenation. Remarkably, the high 2-MF productivity of 1.7 g2-MF gCat.–1 h–1 with nearly 100% selectivity is achieved over Co@MCS at 130 °C and 2 MPa of pH2, overcoming all previously reported results. This work provides valuable insights for designing catalysts with high selectivity for the conversion of lignin-derived platform chemicals. Furthermore, the concept of confined catalysis holds promise for broader application in other industrial catalytic processes.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.