Acetaldehyde as a probe for the chemical properties of aluminophosphate molecular sieves. An in situ FT-IR study

被引:12
作者
Jeong, MS [1 ]
Frei, H [1 ]
机构
[1] Univ Calif Berkeley, Lawrence Berkeley Lab, Calvin Lab, Phys Biosci Div, Berkeley, CA 94720 USA
关键词
aluminophosphate molecular sieve; transition metals; infrared spectroscopy; acetaldehyde; Lewis acid sites;
D O I
10.1016/S1381-1169(99)00421-5
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
Loading of acetaldehyde from the gas phase into transition metal substituted aluminophosphate sieves of AFI structure resulted in mainly physisorbed CH3CH=O in the case of FeAlPO4-5. By contrast, FT-IR spectroscopy revealed extensive chemical reaction upon loading into metal-free AlPO4-5 and CoAlPO4-5 materials at temperatures as low as - 100 degrees C. The low temperature product is identified as acetaldol, which dehydrates to crotonaldehyde upon warm-up to room temperature. The reactive sites are proposed to be Lewis acid sites in the aluminophosphate framework. Using FT-IR monitoring of acetaldehyde in the pores of aluminophosphate sieves as a sensitive method for the detection of Lewis acid sites, we find that their abundance varies substantially with metal substitution. Interestingly, isomorphous Fe substitution of the aluminophosphate framework seems to suppress the formation of such defect sites. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:245 / 253
页数:9
相关论文
共 36 条
[1]  
ARENDS IWC, 1997, ANGEW CHEM INT EDIT, V36, P1145
[2]   X-ray absorption spectroscopic study of Bronsted, Lewis, and redox centers in cobalt-substituted aluminum phosphate catalysts [J].
Barrett, PA ;
Sankar, G ;
Catlow, CRA ;
Thomas, JM .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (21) :8977-8985
[3]   C-13 NMR-STUDIES OF ACETONE IN DEALUMINATED FAUJASITES - A PROBE FOR NONFRAMEWORK ALUMINA [J].
BIAGLOW, AI ;
GORTE, RJ ;
WHITE, D .
JOURNAL OF CATALYSIS, 1994, 150 (01) :221-224
[4]   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
[5]   INTERACTION OF ACETONE WITH SKELETAL HYDROXYLS OF ZEOLITES [J].
BOSACEK, V ;
KUBELKOVA, L .
ZEOLITES, 1990, 10 (01) :64-65
[6]  
CHAVEZDIAZ CD, 1992, ZEOLITES, V12, P851
[7]   FORMATION OF C-2 OXYGENATES ON RHODIUM-CONTAINING CATALYSTS DURING CO+H-2 REACTIONS - FTIR STUDY OF ACETALDEHYDE ADSORPTION [J].
DEMRI, D ;
HINDERMANN, JP ;
DIAGNE, C ;
KIENNEMANN, A .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1994, 90 (03) :501-506
[8]  
GEODAKYA.KT, 1967, RUSS J PHYS CH USSR, V41, P476
[9]   Interactions of chemical species with acid sites in zeolites [J].
Gorte, RJ ;
White, D .
TOPICS IN CATALYSIS, 1997, 4 (1-2) :57-69
[10]   Transition-metal ions in aluminophosphate and silicoaluminophosphate molecular sieves: Location, interaction with adsorbates and catalytic properties [J].
Hartmann, M ;
Kevan, L .
CHEMICAL REVIEWS, 1999, 99 (03) :635-663