Center for Molecular Modeling - T. Deconinck

How zeolitic acid strength and composition alter the reactivity of alkenes and aromatics towards methanol

michel — Wed, 10 Sep 2014 11:53:49 +0000

M.W. Erichsen, K. De Wispelaere, K. Hemelsoet, S.L. Moors, T. Deconinck, M. Waroquier, S. Svelle, V. Van Speybroeck, U. Olsbye

Journal of Catalysis

328, 186-196

2015

Abstract

This work encompasses a combined experimental and theoretical assessment of how zeolitic acid strength and composition affects acid-catalysed methylation reactions. Overall, higher methylation rates were observed over the material with higher acid strength. Co-reactions of methanol with benzene at 250 degrees C over the two isostructural AFI materials H-SSZ-24 and H-SAPO-5 revealed large differences in selectivity. While the stronger acidic H-SSZ-24 mainly produced toluene and polymethylbenzenes, high yields of C4+ aliphatics were observed over H-SAPO-5. These results strongly suggest that alkene methylation was preferred over H-SAPO-5 even at very low conversion during methanol/benzene co-reactions. Furthermore, a comparison of benzene and propene methylation at 350-400 degrees C revealed a significantly faster rate of benzene than propene methylation in H-SSZ-24, whereas the rates of benzene and propene methylation were similar in H-SAPO-5. The observed difference in reactivity of the two hydrocarbons in both catalysts could be understood by careful analysis of various molecular dynamics simulations of the co-adsorbed complexes. The probability to form protonated methanol was, as expected, higher in the more acidic material. However, in H-SSZ-24, the probability for methanol protonation was higher when co-adsorbed with benzene than when co-adsorbed with propene, while the same was not observed in H-SAPO-5. Furthermore, it was found that benzene and methanol are more likely to form a reactive co-adsorbed complex in H-SSZ-24 compared to propene and methanol, while the opposite was observed for H-SAPO-5. This work shows that molecular dynamics simulations provide insights into the adsorption behaviour of guest molecules in large pore AFI materials. The obtained insights correlate with the experimentally observed reactivities. (C) 2015 Elsevier Inc. All rights reserved.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1016/j.jcat.2015.01.013

Private attachment

15_JCatalysis_328,186_Erichsen.pdf

Combined Theoretical and Experimental Study on the Influence of Zeolitic Acid Strength on the Methanol Conversion Process

kristof — Mon, 26 Oct 2015 15:40:02 +0000

K. De Wispelaere, M. Westgård Erichsen, K. Hemelsoet, S.L. Moors, T. Deconinck, S. Svelle, M. Waroquier, U. Olsbye, V. Van Speybroeck

ISBN/ISSN:

Poster

Conference / event / venue

IAP Annual Meeting

Hasselt, Belgium

Friday, 11 September, 2015

Combined Theoretical and Experimental Study on the Influence of Zeolitic Acid Strength on the Methanol Conversion Process

kristof — Mon, 16 Feb 2015 10:47:56 +0000

K. De Wispelaere, M. Westgård Erichsen, K. Hemelsoet, S.L. Moors, T. Deconinck, S. Svelle, M. Waroquier, U. Olsbye, V. Van Speybroeck

ISBN/ISSN:

Talk

Conference / event / venue

ZMPC2015

Sapporo, Japan

Sunday, 28 June, 2015 to Thursday, 2 July, 2015

Abstract (private)

Abstract_ZMPC_KDW_1.pdf

Conference reference

ZMPC2015

Combined theoretical and experimental study on the influence of catalyst acid strength on the zeolite-catalyzed methanol conversion process

kristof — Wed, 10 Sep 2014 12:06:26 +0000

K. De Wispelaere, M. Westgård Erichsen, K. Hemelsoet, S.L. Moors, T. Deconinck, S. Svelle, M. Waroquier, U. Olsbye, V. Van Speybroeck

ISBN/ISSN:

Poster

Conference / event / venue

DZA14 meeting (Dutch Zeolite Association)

Gent, Belgium

Tuesday, 7 October, 2014

Abstract (private)

DeWispelaere_Kristof.pdf

The influence of catalyst acid strength on reactions relevant for Methanol To Hydrocarbons (MTH) catalysis

kristof — Mon, 28 Apr 2014 14:13:05 +0000

M. Westgård Erichsen, K. De Wispelaere, J. Van der Mynsbrugge, S.L. Moors, T. Deconinck, S. Svelle, K. Hemelsoet, V. Van Speybroeck, U. Olsbye

ISBN/ISSN:

Talk

Conference / event / venue

16th Nordic Symposium on Catalysis (NSC2014)

Oslo, Norway

Sunday, 15 June, 2014 to Tuesday, 17 June, 2014

Abstract (private)

NCS2014_abstract.pdf

Dynamic ab initio study towards new hydrocarbon pool cycles for the MTO-conversion in H-SAPO-5

wim — Mon, 03 Mar 2014 07:58:44 +0000

T. Deconinck, K. De Wispelaere, J. Van der Mynsbrugge, S.L. Moors, M. Westgård Erichsen, S. Svelle, U. Olsbye, K. Hemelsoet, V. Van Speybroeck

ISBN/ISSN:

Poster

Conference / event / venue

XVth Netherlands' Catalysis and Chemistry Conference (NCCC XV)

Noordwijkerhout, The Netherlands

Monday, 10 March, 2014 to Wednesday, 12 March, 2014

Abstract (private)

2014_TDC_abstract NCCC_v3.pdf

Conference reference

15th NCCC conference

wim — Thu, 27 Feb 2014 10:01:25 +0000

Noordwijkerhout, The Netherlands

Monday, 10 March, 2014 to Wednesday, 12 March, 2014

Participant(s)

K. Hemelsoet, S.L. Moors, K. De Wispelaere, T. Bogaerts, J. Hajek, T. Deconinck, P. Cnudde, T. Van Den Heede

Project ref.

FWO mandaat, FWO MOFs (3G048612) B/12561/*, ERC KINPOR B/10761/*

Conference reference

15th NCCC conference

Dynamic ab initio study towards new hydrocarbon pool cycles for the MTO-conversion in H-SAPO-5

wim — Thu, 05 Sep 2013 13:32:52 +0000

T. Deconinck

Master of Science in Chemical Engineering

2014

Supervisors

Prof. Dr. ir. Veronique Van Speybroeck, Dr. ir. Karen Hemelsoet

Attachment (private)

thesis_main_TDeconinck.pdf

Thomas Deconinck

wim — Tue, 20 Aug 2013 14:10:28 +0000