Ordered Mesoporous Mixed Metal Oxides: Remarkable Effect of Pore Size on Catalytic Activity

被引:40
作者
Pahalagedara, Madhavi N. [1 ]
Pahalagedara, Lakshitha R. [1 ]
Kuo, Chung-Hao [1 ]
Dharmarathna, Saminda [1 ]
Suib, Steven L. [1 ,2 ]
机构
[1] Univ Connecticut, Dept Chem, Storrs, CT 06269 USA
[2] Univ Connecticut, Inst Mat Sci, Storrs, CT 06269 USA
关键词
LAYERED DOUBLE HYDROXIDE; KNOEVENAGEL CONDENSATION; REUSABLE CATALYST; SILICA; GROWTH; TRANSFORMATION; INTERCALATION; NANOPARTICLES; CRYSTALLINITY; HYDROTALCITE;
D O I
10.1021/la502190b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report the synthesis of ordered mesoporous NiAl mixed metal oxides (MMOs) from NiAl-layered double hydroxides (LDHs) through a soft template method using pluronic-F127 as the structure-directing agent. Ordered mesopores were obtained by the thermal decomposition of as-synthesized LDHs at different temperatures. The effects of the pluronic-F127 amount and the calcination temperature on the pore size distribution of the MMO were investigated. NiAl MMOs exhibited excellent catalytic activity in the Knoevenagel condensation of benzaldehyde with acidic methylene group-containing malononitrile. Finally, the dependence of the catalytic activity on the surface properties of NiAl MMOs was investigated. The pore diameter and the pore volume of NiAl MMOs were well correlated with the performance of the catalysts. MMO obtained from the calcination of NiAl-F127(3%)6LDH at 750 degrees C for 5 h gave the highest conversion (>99%) in the Knoevenagel condensation in 30 min. The optimum pore diameter for the model reaction described here was 7.7 nm, which gave rise to more than 99% conversion with 100% selectivity. Ethanol gave the best conversion at 60 degrees C. The regenerated catalyst showed 93.0 and 89.0% of the initial catalytic activity after the first and the second regeneration cycles, respectively.
引用
收藏
页码:8228 / 8237
页数:10
相关论文
共 62 条
[1]   Sphere-to-rod transition in the shape of anionic surfactant micelles determined by surface tension measurements [J].
Alargova, RG ;
Danov, KD ;
Petkov, JT ;
Kralchevsky, PA ;
Broze, G ;
Mehreteab, A .
LANGMUIR, 1997, 13 (21) :5544-5551
[2]   Growth and Shrinkage of Pluronic Micelles by Uptake and Release of Flurbiprofen: Variation of pH [J].
Alexander, Shirin ;
de Vos, Wiebe M. ;
Castle, Thomas C. ;
Cosgrove, Terence ;
Prescott, Stuart W. .
LANGMUIR, 2012, 28 (16) :6539-6545
[3]   Mesoporous carbon nitride as a metal-free base catalyst in the microwave assisted Knoevenagel condensation of ethylcyanoacetate with aromatic aldehydes [J].
Ansari, Mohd Bismillah ;
Jin, Hailian ;
Parvin, Mst Nargis ;
Park, Sang-Eon .
CATALYSIS TODAY, 2012, 185 (01) :211-216
[4]  
Bennazha J., 2001, CATAL COMMUN, V2, P101, DOI [DOI 10.1016/S1566-7367(01)00015-2, 10.1016/S1566-7367(01)00015-2]
[5]   Montmorillonite KSF as an inorganic, water stable, and reusable catalyst for the knoevenagel synthesis of coumarin-3-carboxylic acids [J].
Bigi, F ;
Chesini, L ;
Maggi, R ;
Sartori, G .
JOURNAL OF ORGANIC CHEMISTRY, 1999, 64 (03) :1033-1035
[6]   Biodiesel Production from Waste Oil Using Mg-Al Layered Double Hydroxide Catalysts [J].
Brito, A. ;
Borges, M. E. ;
Garin, M. ;
Hernandez, A. .
ENERGY & FUELS, 2009, 23 (5-6) :2952-2958
[7]   Ordered meso- and macroporous binary and mixed metal oxides [J].
Carreon, MA ;
Guliants, VV .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2005, (01) :27-43
[8]   Synthesis of ordered, uniform, macroporous carbons with mesoporous walls templated by aggregates of polystyrene spheres and silica particles for use as catalyst supports in direct methanol fuel cells [J].
Chai, GS ;
Shin, IS ;
Yu, JS .
ADVANCED MATERIALS, 2004, 16 (22) :2057-+
[9]   The effect of calcination temperature on the crystallinity of TiO2 nanopowders [J].
Chen, YF ;
Lee, CY ;
Yeng, MY ;
Chiu, HT .
JOURNAL OF CRYSTAL GROWTH, 2003, 247 (3-4) :363-370
[10]   Catalytic benzene alkylation over mesoporous zeolite single crystals: Improving activity and selectivity with a new family of porous materials [J].
Christensen, CH ;
Johannsen, K ;
Schmidt, I ;
Christensen, CH .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (44) :13370-13371