Vapour phase isopropylation of phenol over zinc- and iron-containing Al-MCM-41 molecular sieves

被引:29
作者
Savidha, R [1 ]
Pandurangan, A [1 ]
机构
[1] Anna Univ, Dept Chem, Madras 600025, Tamil Nadu, India
关键词
isopropylation; phenol; isopropyl acetate; Al-MCM-41; zinc; iron;
D O I
10.1016/j.apcata.2003.08.018
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
Al-MCM-41 molecular sieves containing zinc and iron are hydrothermally synthesised. The low angle X-ray powder diffraction (XRD) analysis shows that Zn and Fe incorporated Al-MCM-41 retains the hexagonal structure. The higher d-spacing values of Zn- and Fe-Al-MCM-41 catalysts than that of Al-MCM-41 indicate the incorporation of Zn and Fe into the framework. The mesoporous nature of the materials was confirmed by nitrogen adsorption isotherms. Electron paramagnetic resonance (EPR) and diffuse reflectance spectrum (DRS) techniques confirm the tetrahedral co-ordination of iron into the framework. The total acidity of the synthesised catalysts was analysed by both TPD of ammonia and of adsorbed pyridine FT-IR spectroscopy. Acidity measurements indicate that Zn and Fe incorporation increases both Lewis and Bronsted acidity of the catalysts. due to strengthening of Bronsted acid sites by appropriately positioned Zn 2 1 and Fe 31 Lewis acid metals. Vapour phase isopropylation of phenol with a new alkylating agent isopropyl acetate (IPA) was carried out over the H-forms of the above catalysts. On comparison. the Zn and Fe incorporated Al-MCM-41 catalysts show significantly higher phenol conversion and selectivity towards the important product 4-isopropyl phenol (4-IPP). Further, the undesired and dialkylated products selectivity are found to be lower over Zn and Fe incorporated Al-MCM-41 than pure Al-MCM-41 catalysts. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:1 / 11
页数:11
相关论文
共 39 条
[1]   Tertiary butylation of phenol over mesoporous H-FeMCM-41 [J].
Badamali, SK ;
Sakthivel, A ;
Selvam, P .
CATALYSIS LETTERS, 2000, 65 (1-3) :153-157
[2]  
BECK JS, 1992, J AM CHEM SOC, V114, P10835
[3]   ALKYLATION OF PHENOL WITH ANISOLE OVER ZEOLITES OR GAMMA-ALUMINA [J].
BELTRAME, P ;
BELTRAME, PL ;
CARNITI, P ;
CASTELLI, A ;
FORNI, L .
APPLIED CATALYSIS, 1987, 29 (02) :327-334
[4]   SYNTHESIS OF ALUMINUM-RICH MCM-41 [J].
BORADE, RB ;
CLEARFIELD, A .
CATALYSIS LETTERS, 1995, 31 (2-3) :267-272
[5]   Structure and reactivity of framework and extraframework iron in Fe-silicalite as investigated by spectroscopic and physicochemical methods [J].
Bordiga, S ;
Buzzoni, R ;
Geobaldo, F ;
Lamberti, C ;
Giamello, E ;
Zecchina, A ;
Leofanti, G ;
Petrini, G ;
Tozzola, G ;
Vlaic, G .
JOURNAL OF CATALYSIS, 1996, 158 (02) :486-501
[6]   PHYSISORPTION OF ARGON, NITROGEN AND OXYGEN BY MCM-41, A MODEL MESOPOROUS ADSORBENT [J].
BRANTON, PJ ;
HALL, PG ;
SING, KSW ;
REICHERT, H ;
SCHUTH, F ;
UNGER, KK .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1994, 90 (19) :2965-2967
[7]   Control of mesostructured silica particle morphology [J].
Chan, HBS ;
Budd, PM ;
Naylor, TD .
JOURNAL OF MATERIALS CHEMISTRY, 2001, 11 (03) :951-957
[8]  
Chang C.D., 1994, U.S. Patent, Patent No. [5,288,927, 5288927]
[9]   Mesoporous aluminosilicate of the MCM-41 type:: Its catalytic activity in n-hexane isomerization [J].
Chaudhari, K ;
Das, TK ;
Chandwadkar, AJ ;
Sivasanker, S .
JOURNAL OF CATALYSIS, 1999, 186 (01) :81-90
[10]   EPR STUDY OF NATURE AND REMOVAL OF IRON(III) IMPURITIES IN AMMONIUM-EXCHANGED NAY-ZEOLITE [J].
DEROUANE, EG ;
MESTDAGH, M ;
VIELVOYE, L .
JOURNAL OF CATALYSIS, 1974, 33 (02) :169-175