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Activation of ethyl acetate over metal substituted MCM-41: application to alkylation and acylation
Authors:S Sudha  S Vishnu Priya  J Herbert Mabel  M Palanichamy  V Murugesan
Affiliation:(1) Department of Chemistry, Anna University, Chennai, 600 025, India
Abstract:Al-MCM-41, Fe,Al-MCM-41 and Zn,Al-MCM-41 materials with different silicon to metal ratios were synthesized hydrothermally and characterized by XRD, BET, FT-IR, Acidity measurement by pyridine adsorbed FT-IR spectroscopy, 29Si and 27Al MAS NMR and ESR techniques. The orderly arrangement of mesoporous materials was clearly revealed from the XRD patterns. 29Si and 27Al MAS NMR established the co-ordination environment of silicon and aluminium. Electron paramagnetic resonance (EPR) study confirmed the co-ordination environment of Fe in Fe,Al-MCM-41 framework. The catalytic activity of these materials was evaluated in the vapour phase alkylation and acylation of ethylbenzene with ethyl acetate in the temperature range between 250 and 400 °C. The products were found to be 1,3-diethylbenzene (1,3-DEB), 1,4-diethylbenzene (1,4-DEB), 1,2-diethylbenzene (1,2-DEB), 4-ethylacetophenone (4-EAP) and acetophenone (AP). The reaction products revealed that activation of ethyl acetate is a convenient route for both alkylation and acylation reactions. The order of the catalysts activity for the reaction is found to be Fe,Al-MCM-41 (50) > Fe,Al-MCM-41 (100) > Zn,Al-MCM-41 (50) > Zn,Al-MCM-41 (100) > Al-MCM-41 (50) > Al-MCM-41 (100). In addition to the density of acid sites, the strength of acid sites is also important for this reaction. The effects of temperature, feed ratio, WHSV and time on stream were also examined and the results are discussed.
Keywords:Al-MCM-41  Isomorphic substitution  Ethylbenzene  Ethyl acetate  1  4-Diethyl benzene  4-Ethylacetophenone  Alkylation  Acylation
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