期刊
FUEL
卷 267, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2020.117100
关键词
Lignin depolymerization; Graphene oxide; Enol ether; Carbocatalyst; Energy diagram
资金
- Biomass Research & Development Initiative Competitive [2001-10006-3058]
- USDA National Institute of Food and Agriculture
- U.S. Department of Energy's International Affairs [DE-PI0000031]
- U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office
- University Research Scholar Fund
- Buckman Chair Fund at the University of New Haven
- National Science Foundation [ACI-1053575]
Many efforts have been devoted to depolymerizing lignin to high-value aromatic monomers. However, a controllable and complete lignin inter-unit bond cleavage remains difficult because of the randomness in lignin structure and low selectivity in catalysis. Herein, we demonstrate that a sole carbocatalyst graphene oxide (GO) can selectively oxidize aryl- and alkyl-hydroxyl groups of lignin without the presence of any additional oxidizers, leading to lignin degradation under mild conditions. The results from lignin dimers, lignin oligomers, and organosolv lignin indicate that the depolymerization is catalyzed via an oxidative mechanism through an enol ether intermediate, a stable intermediate that has been chemically isolated here. Quantum chemistry calculations at the density functional theory level indicate that the phenolic -OH group in lignin facilitates the formation of radical cations and thus prohibits ring opening reactions, leading to the complete conversion of lignin dimers to guaiacol through the enol ether intermediate.
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