Fei Song , Kai Du , Huamei Yang , Qi Luo , Yuxuan Liu , Qian Qiang , Yangming Ding , Qingda An , Changzhi Li
{"title":"Depolymerization of lignin over heterogeneous Co-NC catalyst","authors":"Fei Song , Kai Du , Huamei Yang , Qi Luo , Yuxuan Liu , Qian Qiang , Yangming Ding , Qingda An , Changzhi Li","doi":"10.1016/j.jes.2024.05.025","DOIUrl":null,"url":null,"abstract":"<div><p>Green and atom-economic depolymerization of lignin remains a great challenge due to its complex non-repetitive structure and the inert property for chemo-digestion. A redox-neutral lignin depolymerization system without the use of extra oxidant and/or reductant over a Co-NC catalyst has been developed in this work, providing the first non-noble metal heterogeneous catalytic system for redox-neutral valorization of lignin. Mechanistic studies based on control reactions and deuterium labeling experiments suggest that the reaction proceeds via a metal-catalyzed dehydrogenation of C<sub>α</sub>-OH to afford a carbonyl intermediate, followed by C<sub>β</sub>-O bond cleavage (via hydrogenolysis) to afford monophenols and aromatic ketone products. The hydrogen used for the cleavage of the C<sub>β</sub>-O bond originates from the alcohol moiety in the substrate, and the cascade dehydrogenation and hydrogenolysis steps are highly coupled, rendering it an efficient and atom-economic process.</p></div>","PeriodicalId":15788,"journal":{"name":"Journal of Environmental Sciences-china","volume":null,"pages":null},"PeriodicalIF":5.9000,"publicationDate":"2024-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Sciences-china","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S100107422400264X","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
引用次数: 0
Abstract
Green and atom-economic depolymerization of lignin remains a great challenge due to its complex non-repetitive structure and the inert property for chemo-digestion. A redox-neutral lignin depolymerization system without the use of extra oxidant and/or reductant over a Co-NC catalyst has been developed in this work, providing the first non-noble metal heterogeneous catalytic system for redox-neutral valorization of lignin. Mechanistic studies based on control reactions and deuterium labeling experiments suggest that the reaction proceeds via a metal-catalyzed dehydrogenation of Cα-OH to afford a carbonyl intermediate, followed by Cβ-O bond cleavage (via hydrogenolysis) to afford monophenols and aromatic ketone products. The hydrogen used for the cleavage of the Cβ-O bond originates from the alcohol moiety in the substrate, and the cascade dehydrogenation and hydrogenolysis steps are highly coupled, rendering it an efficient and atom-economic process.
期刊介绍:
The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.