Journal
ACS CATALYSIS
Volume 8, Issue 6, Pages 4761-4771Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b00022
Keywords
lignin model; photocatalysis; C-C bond cleavage; mesoporous carbon nitride; visible light
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Funding
- National Natural Science Foundation of China [21690082, 21690080]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020300]
- Department of Science and Technology of Liaoning province [2015020086-101]
- DICP [DICP DMTO201406]
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Photocatalysis is a potentially promising approach to harvest aromatic compounds from lignin. However, the development of an active and selective solid photocatalyst is still challenging for lignin transformation under ambient conditions. We herein report a mild photocatalytic oxidative strategy for C-C bond cleavage of lignin beta-O-4 and beta-1 linkages using a mesoporous graphitic carbon nitride catalyst. Identifications by solid-state NMR techniques and density functional theory (DFT) calculations indicate that pi-pi stacking interactions are most likely present between the flexible carbon nitride surface and lignin model molecule. Besides, low charge recombination efficiency and high specific surface area (206.5 m(2) g(-1)) of the catalyst also contribute to its high catalytic activity. Mechanistic investigations reveal that photogenerated holes, as the main active species, trigger the oxidation and C-C bond cleavage of lignin models. This study sheds light on the interaction between complex lignin structures and the catalyst surface and provides a new strategy of photocatalytic cleavage of lignin models with heterogeneous photocatalysts.
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