Novel method for the preparation of Cs-containing FAU(Y) catalysts for aniline methylation

Olga A. Ponomareva , Polina A. Shaposhnik , Marina V. Belova , Boris A. Kolozhvari , Irina I. Ivanova

Front. Chem. Sci. Eng. ›› 2018, Vol. 12 ›› Issue (1) : 70 -76.

PDF (286KB)
Front. Chem. Sci. Eng. ›› 2018, Vol. 12 ›› Issue (1) : 70 -76. DOI: 10.1007/s11705-017-1694-3
RESEARCH ARTICLE
RESEARCH ARTICLE

Novel method for the preparation of Cs-containing FAU(Y) catalysts for aniline methylation

Author information +
History +
PDF (286KB)

Abstract

Cs-containing FAU(Y)-type zeolite catalysts were prepared by conventional and novel ion exchange procedures followed by incipient wetness impregnation with CsOH. The novel ion exchange procedure involved hydrothermal treatment of NaY zeolite in aqueous solution of CsCl at 140–200 °C for 6–24 h. The samples were characterized by low-temperature nitrogen adsorption, X-ray fluorescence analysis, X-ray powder diffraction, scanning electron microscopy, 23Na, 27Al and 133Cs magic angle spinning nuclear magnetic resonance, CO2 and NH3-Temperature programmed desorption. The results show that hydrothermal treatment at 200 °C allows to obtain higher degrees of ion-exchange (up to 83%) with respect to conventional method giving maximum 66%–69%. Catalytic properties of Cs-containing FAU(Y) were studied in aniline methylation. The yield of N-methylaniline is shown to correlate with catalyst’s basicity. The best catalyst performance was achieved over the catalyst with the highest ion-exchange degree impregnated with CsOH. The selectivity to N-methylaniline over this catalyst reached 96.4%.

Graphical abstract

Keywords

FAU(Y) zeolite / ion exchange with cesium / aniline alkylation / N-methylaniline

Cite this article

Download citation ▾
Olga A. Ponomareva, Polina A. Shaposhnik, Marina V. Belova, Boris A. Kolozhvari, Irina I. Ivanova. Novel method for the preparation of Cs-containing FAU(Y) catalysts for aniline methylation. Front. Chem. Sci. Eng., 2018, 12(1): 70-76 DOI:10.1007/s11705-017-1694-3

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

Jacobs P AUytterhoeven  J B. Active sites in zeolites: Part 7. Isopropanol dehydrogenation over alkali cation-exchanged X and Y zeolites. Journal of Catalysis197750(1): 109–114

[2]

Hathaway P EDavis  M E. Base catalysis by alkali-modified zeolites: I. Catalytic activity. Journal of Catalysis1989116(1): 263–278

[3]

Hathaway P EDavis  M E. Base catalysis by alkali-modified zeolites: II. Nature of the active site. Journal of Catalysis1989116(1): 279–284

[4]

Cocepcion-Heydorn P Jia CHerein  DPfander N Karge H G Jentoft F C. Structural and catalytic properties of sodium and cesium exchanged X and Y zeolites, and germanium-substituted X zeolite. Journal of Molecular Catalysis A Chemical2000162(1-2): 227–246

[5]

Bordawekar S V Davis R J. Probing the basic character of alkali-modified zeolites by CO2 adsorption microcalorimetry, butene isomerization, and toluene alkylation with ethylene. Journal of Catalysis2000189(1): 79–90

[6]

Kim J CLi  H XChen  C YDavis  M E. Base catalysis by intrazeolitic cesium oxides. Microporous Materials19942(5): 413–423

[7]

Wieland W SDavis  R JGarses  J M. Side-chain alkylation of toluene with methanol over alkali-exchanged zeolites X, Y, L, and β. Journal of Catalysis1998173(2): 490–500

[8]

Borgna ASepulveda  JMagni S I Apesteguia C R. Active sites in the alkylation of toluene with methanol: A study by selective acid–base poisoning. Applied Catalysis A, General2004276(1-2): 207–215

[9]

Palomares A E Eder-mirth G Rep MLercher  J A. Alkylation of toluene over basic catalysts—key requirements for side chain alkylation. Journal of Catalysis1998180(1): 56–65

[10]

Sooknoi TDwyer  J. Role of substrate’s electrophilicity in base catalysis by zeolites: Alkylation of acetonitrile with methanol. Journal of Molecular Catalysis A Chemical2004211(1-2): 155–164

[11]

Su B LBarthomeuf  D. Alkylation of aniline with methanol: Change in selectivity with acido-basicity of faujasite catalysts. Applied Catalysis A, General1995124(1): 73–80

[12]

Ivanova I IPomakhina  E BRebrov  A IWang  WHunger M Weitkamp J. Mechanism of aniline methylation on zeolite catalysts investigated by in situ 13C NMR spectroscopy. Kinetics and Catalysis200344(5): 701–709

[13]

Danuthai TSooknoi  TJongpatiwut S Rirksomboon T Osuwan S Resasco D E. Effect of extra-framework cesium on the deoxygenation of methylester over CsNaX zeolites. Applied Catalysis A, General2004409-410: 74–81

[14]

Tsou JMagnoux  PGuisnet P Orfao J J M Figueiredo J L. Catalytic oxidation of methyl-isobutyl-ketone over basic zeolites. Applied Catalysis B: Environmental200451(2): 129–133

[15]

Sherry H S. The ion-exchange properties of zeolites. I. Univalent ion exchange in synthetic faujasite. Journal of Physical Chemistry196670(4): 1158–1168

[16]

Norby PPoshni  F IGualtiery  A FHanson  J CGrey  C P. Cation migration in zeolites: An in situ  powder diffraction and MAS NMR study of the structure of zeolite Cs(Na)-Y during dehydration. Journal of Physical Chemistry B1998102(5): 839–856

[17]

Koller HBurger  BSchneider A M Engelhardt G Weitkamp J. Location of Na+ and Cs+ cations in CsNaY zeolites studied by 23Na and 133Cs magic-angle spinning nuclear magnetic resonance spectroscopy combined with X-ray structure analysis by Rietveld refinement. Microporous Materials19955(4): 219–232

[18]

Wei RGuo  MWang J. Preparation, characterization and catalytic behavior of 12-molybdophosphoric acid encapsulated in the supercage of Cs+-exchanged Y zeolite. Chinese Journal of Chemical Engineering200917(1): 58–63

[19]

Hunger MEngelhardt  GKoller H Weitkamp J. Characterization of sodium cations in dehydrated faujasites and zeolite EMT by 23Na DOR, 2D nutation, and MAS NMR. Solid State Nuclear Magnetic Resonance19932(3): 111–120

[20]

Hunger MSchenk  UBuchholz A. Mobility of cations and guest compounds in cesium-exchanged and impregnated zeolites Y and X investigated by high-temperature MAS NMR spectroscopy. Journal of Physical Chemistry B2000104(51): 12230–12236

[21]

Jelinek RMalek  AOzin G A. 23Na synchronized double-rotation NMR study of Cs+, Ca2+, and La3+ cation-exchanged sodium zeolite Y. Journal of Physical Chemistry B199599(22): 9236–9240

[22]

Mortier W J. Zeolite electronegativity related to physicochemical properties. Journal of Catalysis197855(2): 138–145

RIGHTS & PERMISSIONS

Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature

AI Summary AI Mindmap
PDF (286KB)

2938

Accesses

0

Citation

Detail

Sections
Recommended

AI思维导图

/