SBA-15-supported Pd catalysts: The effect of pretreatment conditions on particle size and its application to benzyl alcohol oxidation

被引:46
作者
Liu, Chun-Hsia [1 ]
Lin, Chih-Yu [2 ]
Chen, Jeng-Lung [1 ]
Lu, Kueih-Tzu [1 ]
Lee, Jyh-Fu [1 ]
Chen, Jin-Ming [1 ]
机构
[1] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan
[2] Natl Tsing Hua Univ, Dept Chem, Hsinchu 30013, Taiwan
关键词
Palladium catalyst; Mesoporous material; Alcohol oxidation; X-ray absorption spectra; FREE AEROBIC OXIDATION; SUPPORTED PALLADIUM NANOPARTICLES; SELECTIVE OXIDATION; HETEROGENEOUS CATALYST; MOLECULAR-OXYGEN; SILICA; SBA-15; EFFICIENT; FUNCTIONALIZATION; DECOMPOSITION;
D O I
10.1016/j.jcat.2017.01.019
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
SBA-15-supported Pd catalysts were prepared by impregnation, thermal pretreatment, and H-2 reduction. The pretreatment conditions have an important influence on the resulting size (from 1.3 to 10.3 nm) of the Pd particles; the catalyst prepared under vacuum conditions possessed the smallest particles (size 1.3 nm). X-ray absorption spectra were used to analyze the transformation of the Pd precursor in each step of the preparation. These catalysts were applied to the oxidation of benzyl alcohol by molecular oxygen; the catalyst with the smallest Pd particles exhibited the highest turnover frequency (9684 h(-1)). The catalyst was reusable three times without loss of activity (with conversion >96%). X-ray absorption spectra were recorded ex situ to monitor the oxidation and the coordination structure of Pd at varied temperatures of reaction; when the reaction temperature was above 100 degrees C, the Pd species were in the metallic state. This result indicates that metallic Pd might be the active phase in the oxidation of benzyl alcohol by molecular oxygen. (C) 2017 Elsevier Inc. All rights reserved.
引用
收藏
页码:21 / 29
页数:9
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