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Light-Driven Depolymerization of Native Lignin Enabled by Proton Coupled Electron Transfer
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DOI：10.1021/acscatal.9b04813.png)
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摘要
En 中文
Here, we report a catalytic, light-driven method for the redox-neutral depolymerization of native lignin biomass at ambient temperature. This transformation proceeds via a proton-coupled electron-transfer (PCET) activation of an alcohol O-H bond to generate a key alkoxy radical intermediate, which then facilitates the beta-scission of a vicinal C-C bond. Notably, this single-step depolymerization is driven solely by visible-light irradiation, requires no stoichiometric chemical reagents, and produces no stoichiometric waste. This method exhibits good efficiency and excellent selectivity for the activation and fragmentation of the beta-O-4 linkage in the polymer backbone, even in the presence of numerous other PCET-active functional groups. The feasibility of this protocol in enabling the cleavage of the beta-1 linkage in model lignin dimers was also demonstrated. These results provide further evidence that visible-light photocatalysis can serve as a viable method for the direct conversion of lignin biomass into valuable arene feedstocks.
Keyword:
lignin depolymerization
proton-coupled electron transfer
alkoxy radicals
C-C bond cleavage
photoredox catalysis
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期刊
IF:
13.1
论文数:
1.6W
被引数:
15.0W
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