解聚
键裂
光催化
氧合物
木质素
化学
劈理(地质)
光化学
选择性
催化作用
化学工程
有机化学
材料科学
断裂(地质)
工程类
复合材料
作者
Huan Chen,Donghui Hong,Kun Wan,Junjie Wang,Bo Niu,Yayun Zhang,Donghui Long
标识
DOI:10.1016/j.cclet.2021.11.084
摘要
Selective cleavage of robust C−C bonds to harvest value-added aromatic oxygenates is an intriguing but challenging task in lignin depolymerization. Photocatalysis is a promising technology with the advantages of mild reaction conditions and strong sustainability. Herein, we show a novel urchin-like Nb2O5 hollow microsphere (U-Nb2O5 HM), prepared by one-pot hydrothermal method, are highly active and selective for Cα−Cβ bond cleavage of lignin β-O-4 model compounds under mild conditions, achieving 94% substrate conversion and 96% C−C bond cleavage selectivity. Systematic experimental studies and density functional theory (DFT) calculations revealed that the superior performance of U-Nb2O5 HMs arises from more exposed active sites, more efficient free charge separation and the active (001) facet, which facilitates the activation of Cβ−H bond of lignin models and generate key Cβ radical intermediates by photogenerated holes, further inducing the Cα−Cβ bond cleavage to produce aromatic oxygenates. This work could provide some suggestions for the fabrication of hierarchical photocatalysts in the lignin depolymerization system.
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