Galvanic Deposition of Au on Paperlike Cu Fiber for High-Efficiency, Low-Temperature Gas-Phase Oxidation of Alcohols

被引:21
作者
Zhao, Guofeng [1 ]
Hu, Huanyun [1 ]
Deng, Miaomiao [1 ]
Lu, Yong [1 ]
机构
[1] E China Normal Univ, Dept Chem, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
关键词
alcohols; copper; electrochemistry; gold; heat transfer; COPPER-CONTAINING CATALYSTS; STRUCTURED SILVER CATALYST; SELECTIVE OXIDATION; BENZYL ALCOHOL; REPLACEMENT REACTION; MOLECULAR-OXYGEN; H-2; PRODUCTION; GOLD; STATE; DEHYDROGENATION;
D O I
10.1002/cctc.201100138
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
The highly active and selective gold-on-copper fiber catalysts with excellent heat conductivity were successfully prepared for high-efficiency gas-phase selective oxidation of various alcohols. The Au/Cu-fiber catalysts were obtained by conducting galvanic deposition of Au onto a thin-sheet microfibrous structure that consisted of 5 vol% Cu-fiber (8 mu m diameter), and 95 vol% voidage. The best catalyst was Au-3/Cu-fiber-200 (Au loading: 3 wt%; calcined at 200 degrees C in air), which was effective for acyclic, benzylic, and polynary alcohols using a high weight hourly space velocity of 20 h(-1). Benzyl alcohol conversion of 86% was obtained with 99% selectivity to benzaldehyde at 220 degrees C. Cyclopropanemethanol could be transformed to cyclo-propanecarboxaldehyde, with conversion of 91% and selectivity of 95% at 250 degrees C. 1,2-Propanediol demonstrated a high con-version of 92%, with a medium selectivity of 74% at 340 degrees C. An oxidation of volatile unsaturated alcohols, such as crotyl alcohol and 3-methyl-2-butenol, could also proceed highly selectively with good conversions at 280 degrees C. A low Delta T of less than 10 degrees C between the catalyst bed and the external wall of the reactor was observed in the selective oxidation of benzyl alcohol owing to the enhanced heat-transfer ability that permits rapid dissipation of large quantities of the reaction heat. Special AuCu(alloy)-Cu2O active composites were formed during the reaction, and their cooperative effect contributed to increasing the low-temperature activity. By nature, the AuCu alloy can catalyze the oxidation of Cu2O-H species with O-2 to release active Cu2O sites.
引用
收藏
页码:1629 / 1636
页数:8
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