Depolymerization of lignin over heterogeneous Co-NC catalyst

IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Fei Song , Kai Du , Huamei Yang , Qi Luo , Yuxuan Liu , Qian Qiang , Yangming Ding , Qingda An , Changzhi Li
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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.

在异相 Co-NC 催化剂上对木质素进行氧化还原中性解聚反应
由于木质素具有复杂的非重复性结构和化学消化的惰性,因此对其进行绿色和原子经济的解聚仍然是一项巨大的挑战。本研究开发了一种无需使用额外氧化剂和/或还原剂的 Co-NC 催化剂氧化还原中性木质素解聚系统,为木质素氧化还原中性价化提供了首个非贵金属异相催化系统。基于对照反应和氘标记实验的机理研究表明,该反应是通过金属催化 Cα-OH 脱氢生成羰基中间体,然后 Cβ-O 键裂解(通过氢解)生成单酚和芳香酮产物。用于 Cβ-O 键裂解的氢来自底物中的醇分子,级联脱氢和氢解步骤高度耦合,使其成为一种高效、原子经济的工艺。
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来源期刊
Journal of Environmental Sciences-china
Journal of Environmental Sciences-china 环境科学-环境科学
CiteScore
13.70
自引率
0.00%
发文量
6354
审稿时长
2.6 months
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.
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