An analysis of the chemical, physical and reactivity features of MgO-SiO2 catalysts for butadiene synthesis with the Lebedev process

被引：88

作者：

Ochoa, Juliana Velasquez ^{[1
]}

Bandinelli, Claudia ^{[1
]}

Vozniuk, Olena ^{[1
]}

Chieregato, Alessandro ^{[1
]}

Malmusi, Andrea ^{[1
]}

Recchi, Carlo ^{[1
]}

Cavani, Fabrizio ^{[1
,2
]}

机构：

[1] Toso Montanari Dept Ind Chem, Viale Risorgimento 4, I-40136 Bologna, Italy

[2] INSTM, Res Unit Bologna, Via G Giusti 9, Florence, Italy

来源：

GREEN CHEMISTRY | 2016年 / 18卷 / 06期

关键词：

BASE PROPERTIES; ETHANOL; OXIDES; CONVERSION;

D O I：

10.1039/c5gc02194d

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

New insights into the transformation of ethanol to butadiene over MgO-SiO2 catalysts, prepared by means of the sol-gel technique, have been gained via characterization, catalytic tests, and in situ infrared diffuse reflectance spectroscopy. Catalysts with low Si-content, i.e., with a Mg/Si atomic ratio in the range between 9 and 15, gave superior butadiene yields, because of the proper combination of strong basic sites, required for ethanol activation, and a moderate number of medium-strength acid sites, needed for the dehydration of intermediately formed alkenols to butadiene. A model of the medium-strength, Lewis-type acid sites, consisting of Mg2+ cations with neighbouring Si4+ atoms, has been proposed; these sites are converted into Bronsted sites in the presence of water, a co-product of the multistep transformation of ethanol into C-4 molecules.

引用

页码：1653 / 1663

页数：11

共 21 条

[1] Influence of acid-base properties on the Lebedev ethanol-to-butadiene process catalyzed by SiO2-MgO materials
Angelici, Carlo
Velthoen, Marjolein E. Z.
Weckhuysen, Bert M.
Bruijnincx, Pieter C. A.
[J]. CATALYSIS SCIENCE & TECHNOLOGY, 2015, 5 (05) : 2869 - 2879
[2] Effect of Preparation Method and CuO Promotion in the Conversion of Ethanol into 1,3-Butadiene over SiO2-MgO Catalysts
Angelici, Carlo
Velthoen, Marjolein E. Z.
Weckhuysen, Bert M.
Bruijnincx, Pieter C. A.
[J]. CHEMSUSCHEM, 2014, 7 (09) : 2505 - 2515
[3] Chemocatalytic Conversion of Ethanol into Butadiene and Other Bulk Chemicals
Angelici, Carlo
Weckhuysen, Bert M.
Bruijnincx, Pieter C. A.
[J]. CHEMSUSCHEM, 2013, 6 (09) : 1595 - 1614
[4] Silica-magnesia mixed oxides prepared by a modified Stober route: Structural and textural aspects
Brambilla, Rodrigo
Radtke, Claudio
dos Santos, Joao H. Z.
Miranda, Marcia S. L.
[J]. POWDER TECHNOLOGY, 2010, 198 (03) : 337 - 346
[5] Spectroscopic characterization of the acid properties of metal oxide catalysts
Busca, G
[J]. CATALYSIS TODAY, 1998, 41 (1-3) : 191 - 206
[6] The surface acidity of solid oxides and its characterization by IR spectroscopic methods. An attempt at systematization
Busca, G
[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1999, 1 (05) : 723 - 736
[7] On the Chemistry of Ethanol on Basic Oxides: Revising Mechanisms and Intermediates in the Lebedev and Guerbet reactions
Chieregato, Alessandro
Ochoa, Juliana Velasquez
Bandinelli, Claudia
Fornasari, Giuseppe
Cavani, Fabrizio
Mella, Massimo
[J]. CHEMSUSCHEM, 2015, 8 (02) : 377 - 388
[8] The sol-gel approach as a method of synthesis of xMgO•ySiO2 powder with defined physicochemical properties including crystalline structure
Ciesielczyk, Filip
Przybysz, Milena
Zdarta, Jakub
Piasecki, Adam
Paukszta, Dominik
Jesionowski, Teofil
[J]. JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY, 2014, 71 (03) : 501 - 513
[9] Site selective hydroxylation of the MgO surface
Diwald, O
Sterrer, M
Knözinger, E
[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2002, 4 (12) : 2811 - 2817
[10] Ternary Ag/MgO-SiO2 Catalysts for the Conversion of Ethanol into Butadiene
Janssens, Wout
Makshina, Ekaterina V.
Vanelderen, Pieter
De Clippel, Filip
Houthoofd, Kristof
Kerkhofs, Stef
Martens, Johan A.
Jacobs, Pierre A.
Sels, Bert F.
[J]. CHEMSUSCHEM, 2015, 8 (06) : 994 - 1008

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