Alumino-mesostructured Ni catalysts for the direct conversion of ethene to propene

• Published in: Journal of catalysis Vol. 305; pp. 154 - 168
• Main Authors: Alvarado Perea, L., Wolff, T., Veit, P., Hilfert, L., Edelmann, F.T., Hamel, C., Seidel-Morgenstern, A.
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier Inc 01.09.2013; Elsevier; Elsevier BV
• Subjects: 1-Butene isomerization; acidity; AlMCM-41; aluminum; Catalysis; Catalysts; catalytic activity; Chemical synthesis; Chemistry; Colloidal state and disperse state; Ethene; ethylene; Exact sciences and technology; General and physical chemistry; MCM-41; nickel; Nickel catalysts; nuclear magnetic resonance spectroscopy; Porous materials; Propene; propylene; silicon; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry; transmission electron microscopy; X-ray diffraction; AlMCM-41; Nickel catalysts; Ethene; Propene; 1-Butene isomerization; MCM-41; Isomerization; Transition metal; Porous material; Conversion; Heterogeneous catalysis; Nickel; Butene; Ethylenic compound; Catalyst
• ISSN: 0021-9517; 1090-2694
• DOI: 10.1016/j.jcat.2013.05.007

In this work, the direct conversion of ethene to propene on Ni/MCM-41 and Ni/AlMCM-41 was studied. The Ni/AlMCM-41 with a Si/Al ratio of 60 revealed the highest conversion of ethene and the highest yield of propene. The combined effect between Ni state and the surface acidity of the catalyst is the responsible of the differences in the catalytic activity. [Display omitted] •Ni/MCM-41 had low conversion of ethene and low selectivity of propene.•Ni/AlMCM-41 provided high conversion of ethene and a selectivity of propene of 39%.•The acidity and the Ni state play a very important role in the catalytic behavior.•Low Si/Al ratio presented a detrimental effect on the catalytic activity.•Propene is involved not only in dimerization, isomerization, and metathesis reactions. Ni/MCM-41 and Ni/AlMCM-41 were synthesized at different Si/Al ratios and tested in the direct conversion of ethene to propene (ETP-reaction). It was intended to evaluate the effect of modifying the catalyst acidity on the ETP-reaction rather than optimizing its performance. All catalysts were characterized by powder XRD, N2-physisorption, 29Si and 27Al MAS NMR, TEM, NH3-TPD, pyridine-DRITFS, H2-TPR, and TPO. Ni/MCM-41 showed low catalytic activity due to its low acidity. Ni/AlMCM-41 catalyst with a Si/Al ratio of 60 had high catalytic activity. Characterization results revealed that the catalyst structure does not have effect on the catalytic activity. Al could be incorporated into the MCM-41 framework up to Si/Al ratio of 16. Two different Ni-composites on the surface of the MCM-41 and AlMCM-41 were observed. Deeper characterization is required to know the Ni state. Important deactivation was observed at 450°C. The nature of the carbonaceous species and reaction mechanism require deeper characterization.