Nanospherical mesoporous carbon-supported gold as an efficient heterogeneous catalyst in the elimination of mass transport limitations

被引:41
作者
Chen, Shangjun [1 ,2 ]
Fu, Haibin [1 ,2 ]
Zhang, Li [1 ,2 ]
Wan, Ying [1 ,2 ]
机构
[1] Shanghai Normal Univ, Key Lab Resource Chem, Shanghai Key Lab Rare Earth Funct Mat, Educ Minist, Shanghai 200234, Peoples R China
[2] Shanghai Normal Univ, Dept Chem, Shanghai 200234, Peoples R China
关键词
Diffusion limitation; Nanosphere; Gold; Carbon; Selective hydrogenation; LIQUID-PHASE OXIDATION; AU NANOPARTICLES; SELECTIVE OXIDATION; REDUCTION; DIFFUSION; SILICA; DESIGN; STABILIZER; PALLADIUM; ALCOHOL;
D O I
10.1016/j.apcatb.2019.02.006
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
This study proposes ordered mesoporous carbon nanosphere-supported gold catalysts to eliminate the diffusion limitation inside the long channels of bulk mesoporous materials. The nanospherical catalysts have a spherical morphology with a diameter of approximately 90 nm, uniform pore sizes of 2.5 nm, and high surface areas of approximately 600 m(2)/g; and the bulk catalysts have similar mesoporous textural properties with nanospherical catalysts but an irregular bulk shape. Metallic gold particles are both intercalated inside carbonaceous walls. The Madon-Boudart (MB) test shows that nanospherical catalysts exhibit no diffusion limitations in the reduction of nitroarenes, even for a large 2,6-dimethylnitrobenzene (2,6-DMNB) molecule. By comparison, the bulk-ordered mesoporous carbon-supported gold catalysts display distinct mass transfer inhibition. The nanospherical mesoporous carbon-supported gold catalysts are highly active and selective for the reduction of nitroarenes to corresponding amines, reaching turnover frequency (TOF) values of 13.7, 16.1, 7.6 and 26.8 min(-1) for converting 4-nitrophenol (4-NP), 2-nitrophenol (2-NP), 4-(tert-butyl)-2-nitrophenol (4-TB-2-NP), and 2,6-DMNB, respectively. The catalysts are stable and can be re-used more than 15 times.
引用
收藏
页码:22 / 30
页数:9
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