Synthesis, characterization and activity study of SO42-/CexZr1-x O2 solid superacid catalyst

被引：94

作者：

Reddy, BM ^{[1
]}

Sreekanth, PM ^{[1
]}

Lakshmanan, P ^{[1
]}

Khan, A ^{[1
]}

机构：

[1] Indian Inst Chem Technol, Inorgan & Phys Chem Div, Hyderabad 500007, Andhra Pradesh, India

来源：

JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL | 2006年 / 244卷 / 1-2期

关键词：

solid superacid; sulfated zirconia; ceria-zirconia; sulfated ceria-zirconia; Mannich reaction; ammonia-TPD;

D O I：

10.1016/j.molcata.2005.08.054

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：

Sulfated CexZr1-xO2 catalyst was found to exhibit solid super-acidity and good catalytic activity for synthesis of P-amino ketones by a three-component Mannich type reaction in the liquid phase under solvent free conditions at ambient temperature. To make the sulfated CexZr1-xO2 catalyst, Ce-Zr hydroxide gel was prepared by a coprecipitation method and SO42- ions were deposited by treating the gel with sulfuric acid and calcined at 923 K. Surface and bulk properties of the CexZr1-xO2 and SO42-/CexZr1-xO2 samples were investigated by means of X-ray powder diffraction, thermogravimetry, ammonia-TPD, Raman spectroscopy and BET surface area methods. Characterization results indicate that impregnated SO42- ions strongly influence the physicochemical characteristics of the CexZr1-xO2 solid solution. Powder XRD profiles reveal the presence of cubic Ce0.5Zr0.5O2 in the case of unpromoted sample and tetragonal Ce0.16Zr0.84O2 phase along with zirconium sulfate compounds in the case of SO42- promoted sample. In particular, the XRD and Raman results suggest a selective interaction of the sulfate ions with zirconia portion of the CeZr1-xO2 solid solution leading to the formation of zirconium sulfate compounds. The NH3-TPD profiles indicate significant changes in the distribution of acid sites on the CexZr1-xO2 upon sulfation. The SO42-/CexZr1-xO2 sample exhibits strong as well as super-acidic sites. (c) 2005 Elsevier B.V. All rights reserved.

引用

页码：1 / 7

页数：7

共 56 条

[1] ACID SITES IN SULFATED AND METAL-PROMOTED ZIRCONIUM DIOXIDE CATALYSTS [J].

ADEEVA, V ;

DEHAAN, JW ;

JANCHEN, J ;

LEI, GD ;

SCHUNEMANN, V ;

VANDEVEN, LJM ;

SACHTLER, WMH ;

VANSANTEN, RA .

JOURNAL OF CATALYSIS, 1995, 151 (02) :364-372

[2] HBF4 catalyzed Mannich-type reaction in aqueous media [J].

Akiyama, T ;

Takaya, J ;

Kagoshima, H .

SYNLETT, 1999, (07) :1045-1048

[3] EPOXIDE REARRANGEMENT .3. ISOMERIZATION OF 1-METHYLCYCLOHEXENE OXIDE OVER TIO2-ZRO2, NISO4 AND FESO4 [J].

ARATA, K ;

AKUTAGAWA, S ;

TANABE, K .

BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1976, 49 (02) :390-393

[4] Preparation of superacids by metal oxides for reactions of butanes and pentanes [J].

Arata, K .

APPLIED CATALYSIS A-GENERAL, 1996, 146 (01) :3-32

[5]

Arata K., 1990, ADV CATAL, V37, P165

[6]

Arend M, 1998, ANGEW CHEM INT EDIT, V37, P1044, DOI 10.1002/(SICI)1521-3773(19980504)37:8<1044::AID-ANIE1044>3.0.CO

[7]

2-E

[8] INFLUENCE OF PREPARATION CONDITIONS ON THE STRUCTURE AND CATALYTIC PROPERTIES OF SO42-/ZRO2 SUPERACID CATALYSTS [J].

CORMA, A ;

FORNES, V ;

JUANRAJADELL, MI ;

NIETO, JML .

APPLIED CATALYSIS A-GENERAL, 1994, 116 (1-2) :151-163

[9] Discovery of new paraffin isomerization catalysts based on SO42-/ZrO2 and WOx/ZrO2 applying combinatorial techniques [J].

Corma, A ;

Serra, JM ;

Chica, A .

CATALYSIS TODAY, 2003, 81 (03) :495-506

[10] Highly diastereoselective addition of silyl enolates to chiral imines derived from (S)-valine methyl ester using lanthanide triflate. [J].

Cozzi, PG ;

DiSimone, B ;

UmaniRonchi, A .

TETRAHEDRON LETTERS, 1996, 37 (10) :1691-1694

← 1 2 3 4 5 6 →