Aerobic selective oxidation of alcohols using La1-xCexCoO3 perovskite catalysts

被引:66
|
作者
Zhu, Junjiang [1 ,2 ,3 ]
Zhao, Yanxi [2 ,3 ]
Tang, Duihai [1 ]
Zhao, Zhen [1 ]
Carabineiro, Sonia A. C. [4 ]
机构
[1] Shenyang Normal Univ, Inst Catalysis Energy & Environm, Coll Chem & Chem Engn, Shenyang 110034, Peoples R China
[2] South Cent Univ Nationalities, Key Lab Catalysis & Mat Sci, State Ethn Affairs Commiss, Wuhan 430074, Peoples R China
[3] South Cent Univ Nationalities, Minist Educ, Wuhan 430074, Peoples R China
[4] Univ Porto, Dept Chem Engn, Fac Engn, LCM,Associate Lab LSRE LCM, Rua Dr Roberto Frias, P-4200465 Oporto, Portugal
基金
美国国家科学基金会;
关键词
La1-xCexCoO3; Porous structure; Selective oxidation; Benzyl alcohol; Molecular oxygen; BENZYL ALCOHOL; MOLECULAR-OXYGEN; OXIDE CATALYSTS; DIRECT DECOMPOSITION; DIESEL EXHAUST; CO OXIDATION; PD CATALYSTS; LACOO3; CARBON; NO;
D O I
10.1016/j.jcat.2016.04.013
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 synthesis of porous perovskites with high and stable activity for alcohols oxidation using molecular oxygen as oxidant is reported. La1-xCexCoO3 catalysts are prepared by a sol-gel method using methanol and ethylene glycol as complexing agents. Calcination at 600 degrees C allows the formation of macro- and mesopores, in contrast to similar materials that often show a bulk structure. Catalytic tests show that La0.9Ce0.1CoO3 is highly active for benzyl alcohol oxidation with molecular oxygen, with both conversion and selectivity above 95% (60 min, 88 degrees C, 1 atm). Further tests show that 94% of the original activity can be obtained after surface regeneration of the used catalyst. The good catalytic performance is explained by the presence of cerium, which is able to attract and release adsorbed oxygen on the oxygen vacancies. The electrons donated by alcohols improve the ability of oxygen vacancies to activate molecular oxygen into oxygen anions, which react with the alcohol and increase the reaction rate. A mechanism is proposed. (C) 2016 Elsevier Inc. All rights reserved.
引用
收藏
页码:41 / 48
页数:8
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