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Author Kurttepeli, M.; Locus, R.; Verboekend, D.; de Clippel, F.; Breynaert, E.; Martens, J.; Sels, B.; Bals, S.
Title Synthesis of aluminum-containing hierarchical mesoporous materials with columnar mesopore ordering by evaporation induced self assembly Type A1 Journal article
Year (down) 2016 Publication Microporous and mesoporous materials: zeolites, clays, carbons and related materials Abbreviated Journal Micropor Mesopor Mat
Volume 234 Issue 234 Pages 186-195
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The incorporation of aluminum into the silica columns of hierarchical mesoporous materials (HMMs) was studied. The HMMs were synthesized by a combination of hard and soft templating methods, forming mesoporous SBA-15-type silica columns inside the pores of anodic aluminum oxide membranes via evaporation induced self-assembly (EISA). By adding Al-isopropoxide to the EISA-mixture a full tetrahedral incorporation of Al and thus the creation of acid sites was achieved, which was proved by nuclear magnetic resonance spectroscopy. Electron microscopy showed that the use of Al-isopropoxide as an Al source for the HMMs led to a change in the mesopore ordering of silica material from circular hexagonal (donut-like) to columnar hexagonal and a 37% increase in specific surface (BET surface). These results were confirmed by a combination of nitrogen physisorption and small-angle X-ray scattering experiments and can be attributed to a swelling of the P123 micelles with isopropanol. The columnar mesopore ordering of silica is advantageous towards the pore accessibility and therefore preferential for many possible applications including catalysis and adsorption on the acid tetrahedral Al-sites. (C) 2016 Elsevier Inc. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000383291400020 Publication Date 2016-07-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1387-1811 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.615 Times cited 5 Open Access OpenAccess
Notes ; The Belgian government (Belgian Science Policy Office, Belspo) is acknowledged for financing the Interuniversity Attraction Poles (IAP-PAI). S. B. acknowledges the financial support from the European Research Council (ERC Starting Grant #335078-COLOURATOMS). D. V. acknowledges the Flanders Research Foundation (FWO). ; ecas_Sara Approved Most recent IF: 3.615
Call Number UA @ lucian @ c:irua:137108 Serial 4404
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Author Zhong, R.; Peng, L.; de Clippel, F.; Gommes, C.; Goderis, B.; Ke, X.; Van Tendeloo, G.; Jacobs, P.A.; Sels, B.F.
Title An eco-friendly soft template synthesis of mesostructured silica-carbon nanocomposites for acid catalysis Type A1 Journal article
Year (down) 2015 Publication ChemCatChem Abbreviated Journal Chemcatchem
Volume 7 Issue 7 Pages 3047-3058
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The synthesis of ordered mesoporous silica-carbon composites was explored by employing TEOS and sucrose as the silica and carbon precursor respectively, and the triblock copolymer F127 as a structure-directing agent via an evaporation-induced self-assembly (EISA) process. It is demonstrated that the synthesis procedures allow for control of the textural properties and final composition of these silica-carbon nanocomposites via adjustment of the effective SiO2/C weight ratio. Characterization by SAXS, N-2 physisorption, HRTEM, TGA, and C-13 and Si-29 solid-state MAS NMR show a 2D hexagonal mesostructure with uniform large pore size ranging from 5.2 to 7.6nm, comprising of separate carbon phases in a continuous silica phase. Ordered mesoporous silica and non-ordered porous carbon can be obtained by combustion of the pyrolyzed nanocomposites in air or etching with HF solution, respectively. Sulfonic acid groups can be readily introduced to such kind of silica-carbon nanocomposites by a standard sulfonation procedure with concentrated sulfuric acid. Excellent acid-catalytic activities and selectivities for the dimerization of styrene to produce 1,3-diphenyl-1-butene and dimerization of -methylstyrene to unsaturated dimers were demonstrated with the sulfonated materials.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000361189400037 Publication Date 2015-09-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1867-3880; 1867-3899 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.803 Times cited 13 Open Access
Notes Approved Most recent IF: 4.803; 2015 IF: 4.556
Call Number UA @ lucian @ c:irua:127836 Serial 4138
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Author de Clippel, F.; Harkiolakis, A.; Vosch, T.; Ke, X.; Giebeler, L.; Oswald, S.; Houthoofd, K.; Jammaer, J.; Van Tendeloo, G.; Martens, J.A.; Jacobs, P.A.; Baron, G.V.; Sels, B.F.; Denayer, J.F.M.
Title Graphitic nanocrystals inside the pores of mesoporous silica : synthesis, characterization and an adsorption study Type A1 Journal article
Year (down) 2011 Publication Microporous and mesoporous materials: zeolites, clays, carbons and related materials Abbreviated Journal Micropor Mesopor Mat
Volume 144 Issue 1/3 Pages 120-133
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract This work presents a new carbonsilica hybrid material, denoted as CSM, with remarkable sorption properties. It consists of intraporous graphitic nanocrystals grown in the pores of mesoporous silica. CSM is obtained by a subtle incipient wetness impregnation of Al-containing mesoporous silica with furfuryl alcohol (FA)/hemelitol solutions. Both the volume match of the impregnation solution with that of the silica template pore volume, and the presence of Al3+ in the silica, are crucial to polymerize FA selectively inside the mesopores. Carbonization of the intraporous polymer was then performed by pyrolysis under He up to 1273 K. The resulting CSMs were examined by SEM, HRTEM, 27Al MAS NMR, N2 adsorption, XRD, TGA, TPD, XPS, pycnometry and Raman spectroscopy. Mildly oxidized graphitic-like carbon nanoblocks, consisting of a few graphene-like sheets, were thus identified inside the template mesopores. Random stacking of these carbon crystallites generates microporosity resulting in biporous materials at low carbon content and microporous materials at high carbon loadings. Very narrow pore distributions were obtained when pyrolysis was carried out under slow heating rate, viz. 1 K min−1. Adsorption and shape selective properties of the carbon filled mesoporous silica were studied by performing pulse chromatography and breakthrough experiments, and by measuring adsorption isotherms of linear and branched alkanes. Whereas the parent mesoporous silica shows unselective adsorption, their CSM analogues preferentially adsorb linear alkanes. The sorption capacity and selectivity can be adjusted by changing the pore size of the template or by varying the synthesis conditions. A relation between the carbon crystallites size and the shape selective behaviour of the corresponding CSM for instance is demonstrated. Most interestingly, CSM shows separation factors for linear and branched alkanes up to values comparable to those of zeolitic molecular sieves.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000293435400016 Publication Date 2011-04-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1387-1811; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.615 Times cited 15 Open Access
Notes Approved Most recent IF: 3.615; 2011 IF: 3.285
Call Number UA @ lucian @ c:irua:92325 Serial 1380
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Author Philippaerts, A.; Paulussen, S.; Turner, S.; Lebedev, O.I.; Van Tendeloo, G.; Poelman, H.; Bulut, M.; de Clippel, F.; Smeets, P.; Sels, B.; Jacobs, P.
Title Selectivity in sorption and hydrogenation of methyl oleate and elaidate on MFI zeolites Type A1 Journal article
Year (down) 2010 Publication Journal of catalysis Abbreviated Journal J Catal
Volume 270 Issue 1 Pages 172-184
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Different zeolites were tested for selective removal of methyl elaidate (trans isomer) from an equimolar mixture with methyl oleate (cis isomer). Sorption experiments of the geometric isomers show that only ZSM-5 samples with reduced Al content in the framework are able to discriminate among the bent cis and the linear trans fatty acid methyl esters. Hydrogenation experiments of equimolar methyl oleate and elaidate mixtures at low temperature (65 °C) and high hydrogen pressure (6.0 MPa), using Pt catalysts, confirm this result. Only with a Pt/NaZSM-5 catalyst outspoken selectivity for the hydrogenation of the trans isomer is obtained. In order to prepare a selective Pt/ZSM-5 catalyst, the influence of Pt addition (impregnation, ion-exchange and competitive ion-exchange) and Pt activation (different calcination and reduction temperatures) on the Pt-distribution and Pt particle size was investigated using SEM, bright-field and HR TEM, EDX, electron tomography, CO-chemisorption, XPS, XRD, and UVvis measurements. The best result in terms of hydrogenation activity and selectivity is obtained with a Pt/ZSM-5 catalyst, which is prepared via competitive ion-exchange, followed by slow calcination up to 350 °C under high O2 flow and a reduction up to 500 °C under H2. This preparation method leads to a Pt/ZSM-5 catalyst with the best Pt distribution and the smallest Pt clusters occluded in the zeolite structure. Finally, the influence of zeolite crystal size, morphology, and elemental composition of ZSM-5 on hydrogenation activity and selectivity was investigated in detail.
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Corporate Author Thesis
Publisher Place of Publication San Diego, Calif. Editor
Language Wos 000275966100021 Publication Date 2010-01-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0021-9517; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.844 Times cited 24 Open Access
Notes FWO; IAP-IV; Methusalem Approved Most recent IF: 6.844; 2010 IF: 5.415
Call Number UA @ lucian @ c:irua:82435 Serial 2970
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Author de Clippel, F.; Harkiolakis, A.; Ke, X.; Vosch, T.; Van Tendeloo, G.; Baron, G.V.; Jacobs, P.A.; Denayer, J.F.M.; Sels, B.F.
Title Molecular sieve properties of mesoporous silica with intraporous nanocarbon Type A1 Journal article
Year (down) 2010 Publication Chemical communications Abbreviated Journal Chem Commun
Volume 46 Issue 6 Pages 928-930
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Biporous carbonsilica materials (CSM) with molecular sieve properties and high sorption capacity were developed by synthesizing nano-sized carbon crystallites in the mesopores of Al-MCM-41.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000274070800024 Publication Date 2009-12-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1359-7345;1364-548X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.319 Times cited 21 Open Access
Notes Fwo; Iap Approved Most recent IF: 6.319; 2010 IF: 5.787
Call Number UA @ lucian @ c:irua:80994 Serial 2182
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