Efficient visible-light-driven depolymerization of oxidized lignin to aromatics catalyzed by an iridium complex immobilized on mesocellular silica foams

被引:51
作者
Hao, Zhongkai [1 ]
Li, Shuyuan [1 ]
Sun, Jiarong [2 ]
Li, Song [1 ]
Zhang, Fang [1 ]
机构
[1] Shanghai Normal Univ, Shanghai Key Lab Rare Earth Funct Mat, Educ Minist, Key Lab Resource Chem, Shanghai 200234, Peoples R China
[2] Han Acad, 33-35 Wong Chuk Hang Rd, Hong Kong, Hong Kong, Peoples R China
关键词
Lignin depolymerization; Visible-light photocatalysis; Ir(ppy)(2)(bpy)-MCFs photocatalyst; Mesoporous cellular silica foams; Click chemistry; ORGANOSILICA NANOTUBES; OXIDATION; HYDROGENOLYSIS; THIOL; HYDROGENATION; DEGRADATION; CONVERSION; CHEMICALS; NIOBIUM; MODELS;
D O I
10.1016/j.apcatb.2018.05.072
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A novel Ir(ppy)(2)(bpy) complex-containing mesoporous cellular silica foams (Ir(ppy)(2)(bpy)-MCFs) was prepared by a facile thiol-ene click reaction between the prefabricated thiol-functionalized mesoporous cellular silica foams and vinyl-tagged [Ir(ppy)2(bpy)]PF6 complex. The elaborate Ir(ppy)(2)(bpy)-MCFs material possessed the large surface area (355 cm(2)/g), open foam-like mesoporous structure with 30 nm cell pore size and 3.0 nm window pore size. Importantly, it had the well-defined molecular configuration of Ir(ppy)(2)(bpy) active species. As expected, it exhibited excellent catalytic reactivity and selectivity in the visible-light-driven reductive de polymerization of oxidized lignin beta-O-4 model compounds including p-hydroxyphenyl (H)-, guaiacyl (G)- and syringyl (S)-type units under the mild conditions. Meanwhile, it showed the comparable catalytic efficiency with the corresponding homogeneous [Ir(ppy)(2)(bpy)]PF6 catalyst. These high catalytic performances could be attributed to aerogel-like three-dimensional pore structure and high visible-light transparency, which efficiently decreased the mass transfer resistance and the photon propagation hindrance. Furthermore, it could be easily recycled and reused at least six times without the remarkable loss of catalytic activity.
引用
收藏
页码:366 / 372
页数:7
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