Center for Molecular Modeling - I. Muylaert

Covalent immobilization of the Jacobsen catalyst on mesoporous phenolic polymer: a highly enantioselective and stable asymmetric epoxidation catalyst

bogaerts — Tue, 12 Feb 2013 10:08:02 +0000

J. De Decker, T. Bogaerts, I. Muylaert, S. Delahaye, F. Lynen, V. Van Speybroeck, A. Verberckmoes, P. Van der Voort

Materials Chemistry and Physics

141 (2013), 967-972

2013

Abstract

The Jacobsen catalyst, N,N′-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediaminomanganese (III) chloride is covalently immobilized on mesoporous phenolic resin through a direct and simple procedure. The immobilization is evident from nitrogen sorption and quantitative XRF measurements. A complex loading of 0.09 mmol g−1 is obtained, corresponding to well dispersed Mn-complexes on the surface of the mesoporous phenolic resin. This novel catalytic system shows good catalytic activity and excellent enantioselectivity in the asymmetric epoxidation of 1,2-dialin. The heterogenized Jacobsen catalyst is demonstrated to be a re-usable and non-leaching catalytic system.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1016/j.matchemphys.2013.06.035

Private attachment

13_matchemphys_141_967_DeDecker.pdf

draft_matchemphys.pdf

A coordinative saturated vanadium containing metal organic framework that shows a remarkable catalytic activity

wim — Thu, 08 Dec 2011 14:15:16 +0000

K. Leus, I. Muylaert, V. Van Speybroeck, G.B. Marin, P. Van der Voort

Studies in Surface Science and Catalysis

175, 329-332

2010

Abstract

A completely saturated Metal Organic Framework, MIL-47 was synthesized and tested for its catalytic performance in the oxidation of cyclohexene with tert-butyl hydroperoxide as oxidant. The catalyst was compared to several reference catalysts: namely VAPO-5, supported VOx/SiO2 and the homogeneous catalyst VO(acac)2. MIL-47 shows a remarkable catalytic activity and preserves its crystalline structure and surface area after a catalytic run. Furthermore MIL-47 exhibits a very high activity in successive runs.

DOI

http://dx.doi.org/10.1016/S0167-2991(10)75053-9

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2010_Leus-Proceeding_PREPA_10.pdf

The remarkable catalytic activity of the saturated metal organic framework V-MIL-47 in the cyclohexeneoxidation

wim — Tue, 23 Aug 2011 09:56:41 +0000

K. Leus, I. Muylaert, M. Vandichel, G.B. Marin, M. Waroquier, V. Van Speybroeck, P. Van der Voort

Chemical Communications

46, 5085-5087

2010

Abstract

The remarkable catalytic activity of the saturated metal organic framework MIL-47 in the epoxidation of cyclohexene is elucidated by means of both experimental results and theoretical calculations.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1039/C0CC01506G

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10 chem. commun 46(28)1359 leus.pdf

The coordinatively saturated vanadium MIL-47 as a low leaching heterogeneous catalyst in the oxidation of cyclohexene

wim — Mon, 22 Aug 2011 12:41:31 +0000

K. Leus, M. Vandichel, Y-Y Liu, I. Muylaert, J. Musschoot, H. Vrielinck, F. Callens, G.B. Marin, C. Detavernier, Y.Z. Khimyak, M. Waroquier, V. Van Speybroeck, P. Van der Voort

Journal of Catalysis

285 (1) 196-207

2012

Abstract

A Metal Organic Framework, containing coordinatively saturated V+IV sites linked together by terephthalic linkers (V-MIL-47), is evaluated as a catalyst in the epoxidation of cyclohexene. Different solvents and conditions are tested and compared. If the oxidant TBHP is dissolved in water, a significant leaching of V-species into the solution is observed, and also radical pathways are prominently operative leading to the formation of an adduct between the peroxide and cyclohexene. If, however, the oxidant is dissolved in decane, leaching is negligible and the structural integrity of the V-MIL-47 is maintained during successive runs. The selectivity toward the epoxide is very high in these circumstances. Extensive computational modeling is performed to show that several reaction cycles are possible. EPR and NMR measurements confirm that at least two parallel catalytic cycles are co-existing: one with V+IV sites and one with pre-oxidized V+V sites, and this is in complete agreement with the theoretical predictions.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1016/j.jcat.2011.09.014

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12 j. of catalysis 285 196 Leus.pdf

Development of metal organic frameworks as heterogeneous catalysts

wim — Mon, 17 Oct 2011 14:08:00 +0000

K. Leus, I. Muylaert, M. Vandichel, V. Van Speybroeck, G.B. Marin, P. Van der Voort

Poster

Conference / event / venue

XIth Netherlands' Catalysis and Chemistry Conference (NCCC XI)

Noordwijkerhout, The Netherlands

Monday, 1 March, 2010 to Wednesday, 3 March, 2010

Abstract

2010-Leus-NCCC2010.pdf

A detailed study of the catalytic performance of V, Co and Cu MOFs in the oxidation of cyclohexene

wim — Mon, 17 Oct 2011 13:40:21 +0000

K. Leus, I. Muylaert, A. Verberckmoes, G.B. Marin, Y-Y Liu, V. Van Speybroeck, P. Van der Voort

p. 266

Poster

Conference / event / venue

MOF2010 conference

Marseille, France

Sunday, 5 September, 2010 to Wednesday, 8 September, 2010

Abstract

KLeusMOF2010.pdf

Conference reference

MOF2010

How does alkene epoxidation with TBHP occur in MIL-47?

wim — Mon, 17 Oct 2011 13:38:44 +0000

M. Vandichel, K. Leus, I. Muylaert, P. Van der Voort, M. Waroquier, V. Van Speybroeck

P. 283

Poster

Conference / event / venue

MOF2010 conference

Marseille, France

Sunday, 5 September, 2010 to Wednesday, 8 September, 2010

Abstract

VandichelMOF2010.pdf

Conference reference

MOF2010

The catalytic performance of MIL-47 in the liquid phase oxidation of cyclohexene

wim — Mon, 17 Oct 2011 13:36:20 +0000

K. Leus, I. Muylaert, M. Vandichel, G.B. Marin, M. Waroquier, V. Van Speybroeck, P. Van der Voort

p. 267-270

Poster

Conference / event / venue

MOF2010 conference

Marseille, France

Sunday, 5 September, 2010 to Wednesday, 8 September, 2010

Abstract

KLeusMOF2010_2.pdf

Conference reference

MOF2010

A study of the effect of electron donating and electron withdrawing groups on the catalytic performance of V-MIL-47

wim — Mon, 17 Oct 2011 13:03:33 +0000

K. Leus, Y-Y Liu, M. Vandichel, I. Muylaert, G.B. Marin, M. Waroquier, V. Van Speybroeck, P. Van der Voort

p. 225

Poster

Conference / event / venue

XIIth Netherlands' Catalysis and Chemistry Conference (NCCC XII)

Noordwijkerhout, The Netherlands

Monday, 28 February, 2011 to Wednesday, 2 March, 2011

Abstract

2011 K_Leus_NCCC.pdf

Conference reference

NCCC-XII