Study of acetaldehyde condensation chemistry over magnesia and zirconia supported on silica

被引：137

作者：

Ordomsky, V. V. ^{[1
]}

Sushkevich, V. L. ^{[1
]}

Ivanova, I. I. ^{[1
]}

机构：

[1] Moscow MV Lomonosov State Univ, Dept Chem, Moscow 119892, Russia

来源：

JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL | 2010年 / 333卷 / 1-2期

关键词：

Aldol condensation; Acetaldehyde; IR spectroscopy; ACID-BASE PROPERTIES; ALDOL CONDENSATION; CARBON-DIOXIDE; CATALYTIC-PROPERTIES; SILANOL GROUPS; FT-IR; ADSORPTION; SURFACE; OXIDES; PHASE;

D O I：

10.1016/j.molcata.2010.10.001

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：

Aldol condensation of acetaldehyde was investigated over silica supported magnesium and zirconium oxides. The acidic and basic properties of the catalysts were studied by TPD of NH3 and CO2 and IR spectroscopy of adsorbed pyridine and CO2. MgO/SiO2 catalyst was characterized by high content of both basic and acidic sites, while ZrO2/SiO2 contained mainly Lewis acid sites. All materials studied were shown to catalyze the aldol condensation of acetaldehyde with selectivity to crotonaldehyde of ca. 85%. The activity of the catalysts was found to be in the following order: ZrO2/SiO2 > MgO/SiO2 >> SiO2. To assess the role of acidic and basic sites in condensation reaction, pyridine and carbon dioxide were used as probe molecules for poisoning of the corresponding active sites during catalytic runs. The results pointed to the key role of Lewis acid sites in acetaldehyde condensation. A concerted mechanism involving Lewis and Bronsted acid sites of the catalysts is proposed on the basis of in situ IR spectroscopic studies. (C) 2010 Elsevier B.V. All rights reserved.

引用

页码：85 / 93

页数：9

共 42 条

[1] THE OLEFIN ALDEHYDE CONDENSATION - THE PRINS REACTION [J].

ARUNDALE, E ;

MIKESKA, LA .

CHEMICAL REVIEWS, 1952, 51 (03) :505-555

[2] MECHANISTIC STUDIES IN STRONG ACIDS .10. ACID-CATALYZED ENOLIZATION AND ALDOL CONDENSATION OF ACETALDEHYDE [J].

BAIGRIE, LM ;

COX, RA ;

SLEBOCKATILK, H ;

TENCER, M ;

TIDWELL, TT .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1985, 107 (12) :3640-3645

[3] A C-13 NMR-STUDY OF THE CONDENSATION CHEMISTRY OF ACETONE AND ACETALDEHYDE ADSORBED AT THE BRONSTED ACID SITES IN H-ZSM-5 [J].

BIAGLOW, AI ;

SEPA, J ;

GORTE, RJ ;

WHITE, D .

JOURNAL OF CATALYSIS, 1995, 151 (02) :373-384

[4] Vapor phase reactions of acetaldehyde over type X zeolites [J].

Chang, YC ;

Ko, AN .

APPLIED CATALYSIS A-GENERAL, 2000, 190 (1-2) :149-155

[5] Facile synthesis and characterization of acid-base bifunctionalized mesoporous silica [J].

Chen, Ying ;

Han, Jinyu ;

Zhang, Haitao .

APPLIED SURFACE SCIENCE, 2008, 254 (18) :5967-5974

[6] SILICA-SUPPORTED ZIRCONIA .1. CHARACTERIZATION BY INFRARED-SPECTROSCOPY, TEMPERATURE-PROGRAMMED DESORPTION, AND X-RAY-DIFFRACTION [J].

DANG, Z ;

ANDERSON, BG ;

AMENOMIYA, Y ;

MORROW, BA .

JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (39) :14437-14443

[7] Structure and surface and catalytic properties of Mg-Al basic oxides [J].

Di Cosimo, JI ;

Diez, VK ;

Xu, M ;

Iglesia, E ;

Apesteguia, CR .

JOURNAL OF CATALYSIS, 1998, 178 (02) :499-510

[8] Acid-base properties and active site requirements for elimination reactions on alkali-promoted MgO catalysts [J].

Díez, VK ;

Apesteguía, CR ;

Di Cosimo, JI .

CATALYSIS TODAY, 2000, 63 (01) :53-62

[9] Influence of the acid-base properties of solid catalysts derived from hydrotalcite-like compounds on the condensation of formaldehyde and acetaldehyde [J].

Dumitriu, E ;

Hulea, V ;

Chelaru, C ;

Catrinescu, C ;

Tichit, D ;

Durand, R .

APPLIED CATALYSIS A-GENERAL, 1999, 178 (02) :145-157

[10] The aldol condensation of lower aldehydes over MFI zeolites with different acidic properties [J].

Dumitriu, E ;

Hulea, V ;

Fechete, I ;

Auroux, A ;

Lacaze, JF ;

Guimon, C .

MICROPOROUS AND MESOPOROUS MATERIALS, 2001, 43 (03) :341-359

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