Shuang Wang , Huihui Zhang , Chunyan Yu , Yue Liu , Yanju Lu , Lu Li
{"title":"用于研究木质素中 β-O-4 键合活性的均匀分散 Co-Corrin/C 催化剂","authors":"Shuang Wang , Huihui Zhang , Chunyan Yu , Yue Liu , Yanju Lu , Lu Li","doi":"10.1016/j.jaap.2024.106826","DOIUrl":null,"url":null,"abstract":"<div><div>In this study, Co-Corrin/C catalysts with corrin active skeleton were prepared by pyrolysis under anaerobic conditions using vitamin B12 (VB12) as a precursor and activated carbon with rich mesoporous structure as a carrier. The Co-Corrin/C catalyst was applied to the oxidative cleavage reaction of lignin, showing a 92.74 % breakage of β-O-4 bonds. Density functional theory (DFT) calculations indicate that the low energy gap difference of Co-Corrin/C promotes electron transfer between Co and O. Meanwhile, the pyrrole ring in the corrin structure will be adsorbed and bonded to oxygen, which promotes the generation of large amounts of oxygen free radicals. The C<sub>α</sub>-OH bond in the lignin aliphatic chain is oxidized to C<sub>α</sub>=O bond under the action of oxygen radicals, which reduces the dissociation energy of the β-O-4 bond and significantly improves the oxidation efficiency. Cycling experiments proved that Co-Corrin/C has good stability.</div></div>","PeriodicalId":345,"journal":{"name":"Journal of Analytical and Applied Pyrolysis","volume":"183 ","pages":"Article 106826"},"PeriodicalIF":5.8000,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Uniformly dispersed Co-Corrin/C catalysts for the study of β-O-4 bonding activity in lignin\",\"authors\":\"Shuang Wang , Huihui Zhang , Chunyan Yu , Yue Liu , Yanju Lu , Lu Li\",\"doi\":\"10.1016/j.jaap.2024.106826\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this study, Co-Corrin/C catalysts with corrin active skeleton were prepared by pyrolysis under anaerobic conditions using vitamin B12 (VB12) as a precursor and activated carbon with rich mesoporous structure as a carrier. The Co-Corrin/C catalyst was applied to the oxidative cleavage reaction of lignin, showing a 92.74 % breakage of β-O-4 bonds. Density functional theory (DFT) calculations indicate that the low energy gap difference of Co-Corrin/C promotes electron transfer between Co and O. Meanwhile, the pyrrole ring in the corrin structure will be adsorbed and bonded to oxygen, which promotes the generation of large amounts of oxygen free radicals. The C<sub>α</sub>-OH bond in the lignin aliphatic chain is oxidized to C<sub>α</sub>=O bond under the action of oxygen radicals, which reduces the dissociation energy of the β-O-4 bond and significantly improves the oxidation efficiency. Cycling experiments proved that Co-Corrin/C has good stability.</div></div>\",\"PeriodicalId\":345,\"journal\":{\"name\":\"Journal of Analytical and Applied Pyrolysis\",\"volume\":\"183 \",\"pages\":\"Article 106826\"},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Analytical and Applied Pyrolysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0165237024004819\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Analytical and Applied Pyrolysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0165237024004819","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
Uniformly dispersed Co-Corrin/C catalysts for the study of β-O-4 bonding activity in lignin
In this study, Co-Corrin/C catalysts with corrin active skeleton were prepared by pyrolysis under anaerobic conditions using vitamin B12 (VB12) as a precursor and activated carbon with rich mesoporous structure as a carrier. The Co-Corrin/C catalyst was applied to the oxidative cleavage reaction of lignin, showing a 92.74 % breakage of β-O-4 bonds. Density functional theory (DFT) calculations indicate that the low energy gap difference of Co-Corrin/C promotes electron transfer between Co and O. Meanwhile, the pyrrole ring in the corrin structure will be adsorbed and bonded to oxygen, which promotes the generation of large amounts of oxygen free radicals. The Cα-OH bond in the lignin aliphatic chain is oxidized to Cα=O bond under the action of oxygen radicals, which reduces the dissociation energy of the β-O-4 bond and significantly improves the oxidation efficiency. Cycling experiments proved that Co-Corrin/C has good stability.
期刊介绍:
The Journal of Analytical and Applied Pyrolysis (JAAP) is devoted to the publication of papers dealing with innovative applications of pyrolysis processes, the characterization of products related to pyrolysis reactions, and investigations of reaction mechanism. To be considered by JAAP, a manuscript should present significant progress in these topics. The novelty must be satisfactorily argued in the cover letter. A manuscript with a cover letter to the editor not addressing the novelty is likely to be rejected without review.