Journal
JOURNAL OF CATALYSIS
Volume 299, Issue -, Pages 284-297Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2012.12.018
Keywords
Coke characterization; (MA)LDI-TOF MS; EPR; Ethanol transformation; BEA zeolite
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Funding
- IFPEN
- Agence National de la Recherche
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HBEA (11) zeolite was deactivated rapidly by coking during the ethanol transformation into hydrocarbons, at 623 K and 30 bar. The nature of carbonaceous deposit was studied, after zeolite dissolution by hydrofluoric acid both by gas chromatography coupled with mass spectrometry and by matrix-assisted laser desorption/ionization time of flight mass spectrometry (MALDI-TOF MS). The coke on the external zeolite surface was characterized directly on the spent catalyst by laser desorption/ionization time of flight mass spectrometry (LDI-TOF MS). The coke species were identified and classified into 17 families following their unsaturation number (4-23). The coke was polyaromatic, and it was very alkylated (methyl, ethyl, and propyl groups). It is compounded of alkylbenzenes, mainly hexamethylbenzene (HMB), and alkyl-pyrenes, located within the zeolite pore, which could migrate to the external zeolite surface and grow into polyaromatic compounds constituted up to eight aromatic rings and up to 40 carbon atoms. Pulsed electron paramagnetic resonance spectroscopy measurements and molecular simulation by using Cerius(2) software have shown that HMBs are distant of 0.6 nm inside the zeolite pores. (C) 2012 Elsevier Inc. All rights reserved.
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