Journal
AICHE JOURNAL
Volume 58, Issue 11, Pages 3474-3481Publisher
WILEY-BLACKWELL
DOI: 10.1002/aic.13725
Keywords
methanol-to-olefin; ethylene production; formaldehyde coupling; a-Mn2O3 nanocrystals; in situ diffuse reflectance infrared Fourier transform spectroscopy
Categories
Funding
- Chinese Education Ministry 111 project [B08021]
- National Science Foundation [21006068, 21176071, 21106041]
- Program for New Century Excellent Talents in University [NCET-10-0611]
- Program of Introducing Talents of Discipline to Universities [B06006]
- Shanghai PuJiang Talent Program [2010/10PJ1402500, 2011/11PJ1402400]
- Program of Science and Technology Commission of Shanghai Municipality [11JC1402700]
- Innovation Program of Shanghai Municipal Education Commission [11ZZ52, 11ZZ051]
- Shanghai Natural Science Foundation [11ZR1408400]
- Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials (Fudan University) [2010MCIMKF01]
- Creative Team Development Project of Ministry of Education [IRT0721]
- Fundamental Research Funds for the Central Universities
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The synthesis and utilization of an a-Mn2O3 nanocrystal catalyst for methanol-to-olefin reaction is described. A methanol conversion of 35% and a maximum selectivity of 80% toward ethylene were obtained at 250 degrees C. In particular, formaldehyde, a primary intermediate for the reaction, was used to produce ethylene via a coupling reaction. A conversion of 45% and a selectivity of 66% to ethylene were achieved at 150 degrees C in a formaldehyde stream. In situ diffuse reflectance infrared Fourier transform spectra reveal the formation of the surface CH2-containing species during reaction, which implies that the main pathway for formaldehyde coupling is probably through interactions of those intermediates. In addition, the weakly adsorbed oxygen on the alpha-Mn2O3 nanocrystal surface was found to play an important role in this reaction. (c) 2012 American Institute of Chemical Engineers AIChE J, 2012
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