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Author Vernimmen, J.; Guidotti, M.; Silvestre-Albero, J.; Jardim, E.O.; Mertens, M.; Lebedev, O.I.; Van Tendeloo, G.; Psaro, R.; Rodríguez-Reinoso, F.; Meynen, V.; Cool, P.
Title Immersion calorimetry as a tool to evaluate the catalytic performance of titanosilicate materials in the epoxidation of cyclohexene Type A1 Journal article
Year 2011 Publication Langmuir: the ACS journal of surfaces and colloids Abbreviated Journal Langmuir
Volume 27 Issue 7 Pages (up) 3618-3625
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract Different types of titanosilicates are synthesized, structurally characterized, and subsequently catalytically tested in the liquid-phase epoxidation of cyclohexene. The performance of three types of combined zeolitic/mesoporous materials is compared with that of widely studied Ti-grafted-MCM-41 molecular sieve and the TS-1 microporous titanosilicate. The catalytic test results are correlated with the structural characteristics of the different catalysts. Moreover, for the first time, immersion calorimetry with the same substrate molecule as in the catalytic test reaction is applied as an extra means to interpret the catalytic results. A good correlation between catalytic performance and immersion calorimetry results is found. This work points out that the combination of catalytic testing and immersion calorimetry can lead to important insights into the influence of the materials structural characteristics on catalysis. Moreover, the potential of using immersion calorimetry as a screening tool for catalysts in epoxidation reactions is shown.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000288970900054 Publication Date 2011-02-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0743-7463;1520-5827; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.833 Times cited 19 Open Access
Notes Approved Most recent IF: 3.833; 2011 IF: 4.186
Call Number UA @ lucian @ c:irua:88366 Serial 1557
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Author Rahemi, V.; Trashin, S.; Hafideddine, Z.; Van Doorslaer, S.; Meynen, V.; Gorton, L.; De Wael, K.
Title Amperometric flow-injection analysis of phenols induced by reactive oxygen species generated under daylight irradiation of titania impregnated with horseradish peroxidase Type A1 Journal article
Year 2020 Publication Analytical Chemistry Abbreviated Journal Anal Chem
Volume 92 Issue 92 Pages (up) 3643-3649
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract Titanium dioxide (TiO2) is a unique material for biosensing applications due to its capability of hosting enzymes. For the first time, we show that TiO2 can accumulate reactive oxygen species (ROS) under daylight irradiation and can support the catalytic cycle of horseradish peroxidase (HRP) without the need of H2O2 to be present in the solution. Phenolic compounds, such as hydroquinone (HQ) and 4-aminophenol (4-AP), were detected amperometrically in flow-injection analysis (FIA) mode via the use of an electrode modified with TiO2 impregnated with HRP. In contrast to the conventional detection scheme, no H2O2 was added to the analyte solution. Basically, the inherited ability of TiO2 to generate reactive oxygen species is used as a strategy to avoid adding H2O2 in the solution during the detection of phenolic compounds. Electron paramagnetic resonance (EPR) spectroscopy indicates the presence of ROS on titania which, in interaction with HRP, initiate the electrocatalysis toward phenolic compounds. The amperometric response to 4-AP was linear in the concentration range between 0.05 and 2 μM. The sensitivity was 0.51 A M–1 cm–2, and the limit of detection (LOD) 26 nM. The proposed sensor design opens new opportunities for the detection of phenolic traces by HRP-based electrochemical biosensors, yet in a more straightforward and sensitive way following green chemistry principles of avoiding the use of reactive and harmful chemical, such as H2O2.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000518234700023 Publication Date 2020-01-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0003-2700; 5206-882x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.4 Times cited 3 Open Access
Notes ; The authors thank Scientific Reseatch-Flanders (F-WO) (grant 12T4219N) for funding. ; Approved Most recent IF: 7.4; 2020 IF: 6.32
Call Number UA @ admin @ c:irua:166241 Serial 5463
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Author Vernimmen, J.; Meynen, V.; Herregods, S.J.F.; Mertens, M.; Lebedev, O.I.; Van Tendeloo, G.; Cool, P.
Title New insights in the formation of combined zeolitic/mesoporous materials by using a one-pot templating synthesis Type A1 Journal article
Year 2011 Publication European journal of inorganic chemistry Abbreviated Journal Eur J Inorg Chem
Volume Issue 27 Pages (up) 4234-4240
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract Zeolitic growth is often absent or occurs in separate phases when synthetic strategies based on the combination of zeolite templates and mesopore templating agents are applied. In this work, zeolitic growth and mesopore formation have been investigated at different temperatures by applying a one-pot templating approach, based on a TS-1 zeolite synthesis whereby part of the microtemplate (tetrapropylammonium hydroxide, TPAOH) is replaced by a mesotemplate (hexadecyltrimethylammonium bromide, CTMABr). Moreover, the synthesis duration and the molar ratio of the microtemplate/mesotemplate have also been studied. The different syntheses clearly show the inherent competitive mechanism between zeolitic growth and mesopore formation. These insights have led to the conclusion that by following a one-pot templating strategy with standard, nonexotic commercial templates, i.e. CTMABr and TPAOH, it is not possible to develop a true hierarchical mesoporous zeolite, meaning a mesoporous siliceous material with highly crystalline zeolitic walls. The resultant materials are instead combined zeolitic/mesoporous composite structures with, however, highly tuneable and controllable porosity characteristics.
Address
Corporate Author Thesis
Publisher Place of Publication Weinheim Editor
Language Wos 000296143500014 Publication Date 2011-08-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1434-1948; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.444 Times cited 7 Open Access
Notes Fwo Approved Most recent IF: 2.444; 2011 IF: 3.049
Call Number UA @ lucian @ c:irua:91574 Serial 2315
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Author Loreto, S.; Cuypers, B.; Brokken, J.; Van Doorslaer, S.; De Wael, K.; Meynen, V.
Title The effect of the buffer solution on the adsorption and stability of horse heart myoglobin on commercial mesoporous titanium dioxide : a matter of the right choice Type A1 Journal article
Year 2017 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 19 Issue 21 Pages (up) 13503-13514
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract Despite the numerous studies on the adsorption of different proteins onto mesoporous titanium dioxide and indications on the important role of buffer solutions in bioactivity, a systematic study on the impact of the buffer on the protein incorporation into porous substrates is still lacking. We here studied the interaction between a commercial mesoporous TiO2 and three of the most used buffers for protein incorporation, i.e. HEPES, Tris and phosphate buffer. In addition, this paper analyzes the adsorption of horse heart myoglobin (hhMb) onto commercial mesoporous TiO2 as a model system to test the influence of buffers on the protein incorporation behavior in mesoporous TiO2. N2 sorption analysis, FT-IR and TGA/DTG measurements were used to evaluate the interaction between the buffers and the TiO2 surface, and the effect of such an interaction on hhMb adsorption. Cyclic voltammetry (CV) and electron paramagnetic resonance (EPR) were used to detect changes in the microenvironment surrounding the heme. The three buffers show a completely different interaction with the TiO2 surface, which drastically affects the adsorption of myoglobin as well as its structure and electrochemical activity. Therefore, special attention is required while choosing the buffer medium to avoid misguided evaluation of protein adsorption on mesoporous TiO2.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000402488300013 Publication Date 2017-04-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076; 1463-9084 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 2 Open Access
Notes ; We are grateful to Gert Nuyts for performing the XRF measurements, and Dr Stanislav Trashin for his assistance during the electrochemical experiments. This work is supported by the Research Foundation – Flanders (FWO) (grant G.0687.13) and the University of Antwerp (BOF project). ; Approved Most recent IF: 4.123
Call Number UA @ admin @ c:irua:143514 Serial 5582
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Author Collart, O.; Cool, P.; van der Voort, P.; Meynen, V.; Vansant, E.F.; Houthoofd, K.J.; Grobet, P.J.; Lebedev, O.I.; Van Tendeloo, G.
Title Aluminum incorporation into MCM-48 toward the creation of Brønsted acidity Type A1 Journal article
Year 2004 Publication The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical Abbreviated Journal J Phys Chem B
Volume 108 Issue Pages (up) 13905-13912
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000224164000003 Publication Date 2004-09-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1520-6106;1520-5207; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.177 Times cited 13 Open Access
Notes Fwo; Iuap P5/01 Approved Most recent IF: 3.177; 2004 IF: 3.834
Call Number UA @ lucian @ c:irua:49014 Serial 92
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Author Satyawali, Y.; Van Roy, S.; Roevens, A.; Meynen, V.; Mullens, S.; Jochems, P.; Doyen, W.; Cauwenberghs, L.; Dejonghe, W.
Title Characterization and analysis of the adsorption immobilization mechanism of \beta-galactosidase on metal oxide powders Type A1 Journal article
Year 2013 Publication RSC advances Abbreviated Journal
Volume 3 Issue 46 Pages (up) 24054-24062
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL)
Abstract Immobilization of the enzymes plays a vital role in enhancing their applicability in a wide range of applications, thus ensuring the use of sustainable enzymatic processes over the conventional chemical processes on an industrial scale. This study provides the background information for the selection and screening of inorganic metal oxide (MO) powders for their use as fillers in mixed matrix membranes for enzyme immobilization as the future aim. A total of 13 MOs, ranging in size from 0.01 μm to <5 μm, were tested for their performance as a support for enzyme (β-galactosidase) immobilization via adsorption. Alumina appeared to be the best performing MO with the amount and activity of the immobilized enzyme being 64 mg g−1 and up to 288 U g−1, respectively. The amount of immobilized enzyme on alumina (α-Al2O3 C and γ-Al2O3) was >3 times higher than ZrO2 (used as a reference MO in this study). Upon heat treatment at 900 °C, up to 15%, 52% and 42% decline was observed in the amount of immobilized enzyme in case of alumina metal oxides (MOs), ZrO2 and TiO2, respectively. The results suggested that both isoelectric point and surface area of the MO influence the immobilization. The most important observation in this study was that the bonding of the enzyme to the MO surface seems to be mediated by the bonding/interaction of the buffer to the enzyme.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000326745100030 Publication Date 2013-10-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2046-2069 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:111300 Serial 7607
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Author Kus, M.; Altantzis, T.; Vercauteren, S.; Caretti, I.; Leenaerts, O.; Batenburg, K.J.; Mertens, M.; Meynen, V.; Partoens, B.; Van Doorslaer, S.; Bals, S.; Cool, P.
Title Mechanistic Insight into the Photocatalytic Working of Fluorinated Anatase {001} Nanosheets Type A1 Journal article
Year 2017 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal J Phys Chem C
Volume 121 Issue 121 Pages (up) 26275-26286
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Laboratory of adsorption and catalysis (LADCA)
Abstract Anatase nanosheets with exposed {001} facets

have gained increasing interest for photocatalytic applications. To

fully understand the structure-to-activity relation, combined

experimental and computational methods have been exploited.

Anatase nanosheets were prepared under hydrothermal conditions

in the presence of fluorine ions. High resolution scanning

transmission electron microscopy was used to fully characterize

the synthesized material, confirming the TiO2 nanosheet

morphology. Moreover, the surface structure and composition

of a single nanosheet could be determined by annular bright-field

scanning transmission electron microscopy (ABF-STEM) and

STEM electron energy loss spectroscopy (STEM-EELS). The photocatalytic activity was tested for the decomposition of organic

dyes rhodamine 6G and methyl orange and compared to a reference TiO2 anatase sample. The anatase nanosheets with exposed

{001} facets revealed a significantly lower photocatalytic activity compared to the reference. In order to understand the

mechanism for the catalytic performance, and to investigate the role of the presence of F−, light-induced electron paramagnetic

resonance (EPR) experiments were performed. The EPR results are in agreement with TEM, proving the presence of Ti3+

species close to the surface of the sample and allowing the analysis of the photoinduced formation of paramagnetic species.

Further, ab initio calculations of the anisotropic effective mass of electrons and electron holes in anatase show a very high effective

mass of electrons in the [001] direction, having a negative impact on the mobility of electrons toward the {001} surface and thus

the photocatalysis. Finally, motivated by the experimental results that indicate the presence of fluorine atoms at the surface, we

performed ab initio calculations to determine the position of the band edges in anatase slabs with different terminations of the

{001} surface. The presence of fluorine atoms near the surface is shown to strongly shift down the band edges, which indicates

another reason why it can be expected that the prepared samples with a large amount of {001} surface, but with fluorine atoms

near the surface, show only a low photocatalytic activity.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000417228500017 Publication Date 2017-11-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.536 Times cited 20 Open Access OpenAccess
Notes The authors acknowledge the University of Antwerp for financial support in the frame of a GOA project. S.B. acknowledges funding from the European Research Council under the Seventh Framework Program (FP7), ERC Grant No. 335078 COLOURATOM. S.V.D. and V.M. acknowledge funding from the Fund for Scientific Research-Flanders (G.0687.13). T.A. acknowledges financial support from the Research Foundation Flanders (FWO, Belgium) through a postdoctoral grant. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); saraecas; ECAS_Sara; Approved Most recent IF: 4.536
Call Number EMAT @ emat @c:irua:147240UA @ admin @ c:irua:147240 Serial 4771
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Author Kaliyappan, P.; Paulus, A.; D’Haen, J.; Samyn, P.; Uytdenhouwen, Y.; Hafezkhiabani, N.; Bogaerts, A.; Meynen, V.; Elen, K.; Hardy, A.; Van Bael, M.K.
Title Probing the impact of material properties of core-shell SiO₂@TiO₂ spheres on the plasma-catalytic CO₂ dissociation using a packed bed DBD plasma reactor Type A1 Journal article
Year 2021 Publication Journal Of Co2 Utilization Abbreviated Journal J Co2 Util
Volume 46 Issue Pages (up) 101468
Keywords A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Plasma catalysis, a promising technology for conversion of CO2 into value-added chemicals near room temperature, is gaining increasing interest. A dielectric barrier discharge (DBD) plasma has attracted attention due to its simple design and operation at near ambient conditions, ease to implement catalysts in the plasma zone and upscaling ability to industrial applications. To improve its main drawbacks, being relatively low conversion and energy efficiency, a packing material is used in the plasma discharge zone of the reactor, sometimes decorated by a catalytic material. Nevertheless, the extent to which different properties of the packing material influence plasma performance is still largely unexplored and unknown. In this study, the particular effect of synthesis induced differences in the morphology of a TiO2 shell covering a SiO2 core packing material on the plasma conversion of CO2 is studied. TiO2 has been successfully deposited around 1.6–1.8 mm sized SiO2 spheres by means of spray coating, starting from aqueous citratoperoxotitanate(IV) precursors. Parameters such as concentration of the Ti(IV) precursor solutions and addition of a binder were found to affect the shells’ properties and surface morphology and to have a major impact on the CO2 conversion in a packed bed DBD plasma reactor. Core-shell SiO2@TiO2 obtained from 0.25 M citratoperoxotitante(IV) precursors with the addition of a LUDOX binder showed the highest CO2 conversion 37.7% (at a space time of 70 s corresponding to an energy efficiency of 2%) and the highest energy efficiency of 4.8% (at a space time of 2.5 s corresponding to a conversion of 3%).
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000634280300004 Publication Date 2021-02-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2212-9820 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.292 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 4.292
Call Number UA @ admin @ c:irua:175958 Serial 6773
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Author Xu, W.; Buelens, L.C.; Galvita, V.V.; Bogaerts, A.; Meynen, V.
Title Improving the performance of gliding arc plasma-catalytic dry reforming via a new post-plasma tubular catalyst bed Type A1 Journal Article
Year 2024 Publication Journal of CO2 Utilization Abbreviated Journal Journal of CO2 Utilization
Volume 83 Issue Pages (up) 102820
Keywords A1 Journal Article; Dry reforming Gliding arc plasma Plasma catalytic DRM Ni-based mixed oxide Post-plasma catalysis; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract A combination of a gliding arc plasmatron (GAP) reactor and a newly designed tubular catalyst bed (N-bed) was applied to investigate the post-plasma catalytic (PPC) effect for dry reforming of methane (DRM). As comparison, a traditional plasma catalyst bed (T-bed) was also utilized. The post-plasma catalytic effect of a Ni-based mixed oxide (Ni/MO) catalyst with a thermal catalytic performance of 77% CO2 and 86% CH4 conversion at 700 ℃ was studied. Although applying the T-bed had little effect on plasma based CO2 and CH4 conversion, an increase in selectivity to H2 was obtained with a maximum value of 89% at a distance of 2 cm. However, even when only α-Al2O3 packing material was used in the N-bed configuration, compared to the plasma alone and the T-bed, an increase of the CO2 and CH4 conversion from 53% and 53% to 69% and 69% to 83% was achieved. Addition of the Ni/MO catalyst further enhanced the DRM reaction, resulting in conversions of 79% for CO2 and 91% for

CH4. Hence, although no insulation nor external heating was applied to the N-bed post plasma, it provides a slightly better conversion than the thermal catalytic performance with the same catalyst, while being fully electrically driven. In addition, an enhanced CO selectivity to 96% was obtained and the energy cost was reduced from ~ 6 kJ/L (plasma alone) to 4.3 kJ/L. To our knowledge, it is the first time that a post-plasma catalytic system achieves this excellent catalytic performance for DRM without extra external heating or insulation.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2024-05-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2212-9820 ISBN Additional Links
Impact Factor 7.7 Times cited Open Access
Notes Wencong Xu, Vladimir V. Galvita, Annemie Bogaerts, and Vera Meynen would like to acknowledge the VLAIO Catalisti Moonshot project D2M and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692). Lukas C. Buelens acknowledges financial support from the Fund for Scientific Research Flanders (FWO Flanders) through a postdoctoral fellowship grant 12E5623N. Vladimir V. Galvita also acknowledges a personal grant from the Research Fund of Ghent University (BOF; 01N16319). Approved Most recent IF: 7.7; 2024 IF: 4.292
Call Number PLASMANT @ plasmant @ Serial 9131
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Author Wang, J.; Zhang, K.; Mertens, M.; Bogaerts, A.; Meynen, V.
Title Plasma-based dry reforming of methane in a dielectric barrier discharge reactor: Importance of uniform (sub)micron packings/catalysts to enhance the performance Type A1 Journal Article
Year 2023 Publication APPLIED CATALYSIS B-ENVIRONMENTAL Abbreviated Journal
Volume 337 Issue Pages (up) 122977
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract This study presents new insights on the effect of (sub)micrometer particle sized materials in plasma-based CO2-

CH4 reforming by investigating the performance of SiO2 spheres (with/without supported metal) of varying

particle sizes. (Sub)micron particles synthesized through the St¨ober method were used instead of (sub)millimeter

particles employed in previous studies. Increasing particle size (from 120 nm to 2390 nm) was found to first

increase and then decrease conversion and energy yield, with optimal performance achieved using 740 nm 5 wt%

Ni loaded SiO2, which improved CO2 and CH4 conversion, and energy yield to 44%, 55%, and 0.271 mmol/kJ,

respectively, compared to 20%, 27%, and 0.116 mmol/kJ in an empty reactor at the same flow rate. This is the

first to achieve significant performance improvement in a fully packed reactor, highlighting the importance of

selecting a suitable particle size. The findings can offer guidance towards rational design of catalysts for plasmabased

reactions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001056527600001 Publication Date 2023-06-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-3373 ISBN Additional Links UA library record; WoS full record
Impact Factor 22.1 Times cited Open Access Not_Open_Access
Notes This work is supported by the China Scholarship Council (No. 201806060123); and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692). K.Z acknowledges the EASiCHEM project funded by the Flemish Strategic Basic Research Program of the Catalisti cluster and Flanders Innovation & Entrepreneurship (HBC.2018.0484). Approved Most recent IF: 22.1; 2023 IF: 9.446
Call Number PLASMANT @ plasmant @c:irua:196955 Serial 8797
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Author Wang, J.; Zhang, K.; Mertens, M.; Bogaerts, A.; Meynen, V.
Title Plasma-based dry reforming of methane in a dielectric barrier discharge reactor: Importance of uniform (sub)micron packings/catalysts to enhance the performance Type A1 Journal Article
Year 2023 Publication APPLIED CATALYSIS B-ENVIRONMENTAL Abbreviated Journal
Volume 337 Issue Pages (up) 122977
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract This study presents new insights on the effect of (sub)micrometer particle sized materials in plasma-based CO2-

CH4 reforming by investigating the performance of SiO2 spheres (with/without supported metal) of varying

particle sizes. (Sub)micron particles synthesized through the St¨ober method were used instead of (sub)millimeter

particles employed in previous studies. Increasing particle size (from 120 nm to 2390 nm) was found to first

increase and then decrease conversion and energy yield, with optimal performance achieved using 740 nm 5 wt%

Ni loaded SiO2, which improved CO2 and CH4 conversion, and energy yield to 44%, 55%, and 0.271 mmol/kJ,

respectively, compared to 20%, 27%, and 0.116 mmol/kJ in an empty reactor at the same flow rate. This is the

first to achieve significant performance improvement in a fully packed reactor, highlighting the importance of

selecting a suitable particle size. The findings can offer guidance towards rational design of catalysts for plasmabased

reactions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001056527600001 Publication Date 2023-06-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-3373 ISBN Additional Links UA library record; WoS full record
Impact Factor 22.1 Times cited Open Access Not_Open_Access
Notes This work is supported by the China Scholarship Council (No. 201806060123); and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692). K.Z acknowledges the EASiCHEM project funded by the Flemish Strategic Basic Research Program of the Catalisti cluster and Flanders Innovation & Entrepreneurship (HBC.2018.0484). Approved Most recent IF: 22.1; 2023 IF: 9.446
Call Number PLASMANT @ plasmant @c:irua:196955 Serial 8798
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Author Uytdenhouwen, Y.; Bal, Km.; Neyts, Ec.; Meynen, V.; Cool, P.; Bogaerts, A.
Title On the kinetics and equilibria of plasma-based dry reforming of methane Type A1 Journal article
Year 2021 Publication Chemical Engineering Journal Abbreviated Journal Chem Eng J
Volume 405 Issue Pages (up) 126630
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Plasma reactors are interesting for gas-based chemical conversion but the fundamental relation between the plasma chemistry and selected conditions remains poorly understood. Apparent kinetic parameters for the loss and formation processes of individual components of gas conversion processes, can however be extracted by performing experiments in an extended residence time range (2–75 s) and fitting the gas composition to a firstorder kinetic model of the evolution towards partial chemical equilibrium (PCE). We specifically investigated the differences in kinetic characteristics and PCE state of the CO2 dissociation and CH4 reforming reactions in a dielectric barrier discharge reactor (DBD), how these are mutually affected when combining both gases in the dry reforming of methane (DRM) reaction, and how they change when a packing material (non-porous SiO2) is added to the reactor. We find that CO2 dissociation is characterized by a comparatively high reaction rate of 0.120 s−1 compared to CH4 reforming at 0.041 s−1; whereas CH4 reforming reaches higher equilibrium conversions, 82% compared to 53.6% for CO2 dissociation. Combining both feed gases makes the DRM reaction to proceed at a relatively high rate (0.088 s−1), and high conversion (75.4%) compared to CO2 dissociation, through accessing new chemical pathways between the products of CO2 and CH4. The addition of the packing material can also distinctly influence the conversion rate and position of the equilibrium, but its precise effect depends strongly on the gas composition. Comparing different CO2:CH4 ratios reveals the delicate balance of the combined chemistry. CO2 drives the loss reactions in DRM, whereas CH4 in the mixture suppresses back reactions. As a result, our methodology provides some of the insight necessary to systematically tune the conversion process.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000621197700003 Publication Date 2020-08-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited Open Access OpenAccess
Notes The authors acknowledge financial support from the European Fund for Regional Development through the cross-border collaborative Interreg V program Flanders-the Netherlands (project EnOp), the Fund for Scientific Research (FWO; grant number: G.0254.14N), a TOP-BOF project and an IOF-SBO (SynCO2Chem) project from the University of Antwerp. Approved Most recent IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:172458 Serial 6411
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Author Wang, J.; Zhang, K.; Bogaerts, A.; Meynen, V.
Title 3D porous catalysts for plasma-catalytic dry reforming of methane : how does the pore size affect the plasma-catalytic performance? Type A1 Journal article
Year 2023 Publication Chemical engineering journal Abbreviated Journal
Volume 464 Issue Pages (up) 142574-12
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract The effect of pore size on plasma catalysis is crucial but still unclear. Studies have shown plasma cannot enter micropores and mesopores, so catalysts for traditional thermocatalysis may not fit plasma catalysis. Here, 3D porous Cu and CuO with different pore sizes were prepared using uniform silica particles (10–2000 nm) as templates, and compared in plasma-catalytic dry reforming. In most cases, the smaller the pore size, the higher the conversion of CH4 and CO2. Large pores reachable by more electrons did not improve the reaction efficiency. We attribute this to the small surface area and large crystallite size, as indicated by N2-sorption, mercury intrusion and XRD. While the smaller pores might not be reachable by electrons, due to the sheath formed in front of them, as predicted by modeling, they can still be reached by radicals formed in the plasma, and ions can even be attracted into these pores. An exception are the samples synthesized from 1 μm silica, which show better performance. We believe this is due to the electric field enhancement for pore sizes close to the Debye length. The performances of CuO and Cu with different pore sizes can provide references for future research on oxide supports and metal components of plasma catalysts.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000966076400001 Publication Date 2023-03-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 15.1; 2023 IF: 6.216
Call Number UA @ admin @ c:irua:194862 Serial 7262
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Author Wang, J.; Zhang, K.; Meynen, V.; Bogaerts, A.
Title Dry reforming in a dielectric barrier discharge reactor with non-uniform discharge gap : effects of metal rings on the discharge behavior and performance Type A1 Journal article
Year 2023 Publication Chemical engineering journal Abbreviated Journal
Volume Issue Pages (up) 142953-29
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract The application of dielectric barrier discharge (DBD) plasma reactors is promising in various environmental and energy processes, but is limited by their low energy yield. In this study, we put a number of stainless steel rings over the inner electrode rod of the DBD reactor to change the local discharge gap and electric field, and we studied the dry reforming performance. At 50 W supplied power, the metal rings mostly have a negative impact on the performance, which we attribute to the non-uniform spatial distribution of the discharges caused by the rings. However, at 30 W supplied power, the energy yield is higher than at 50 W and the placement of the rings improves the performance of the reactor. More rings and with a larger cross-sectional diameter can further improve the performance. The reactor with 20 rings with a 3.2 mm cross-sectional diameter exhibits the best performance in this study. Compared to the reactor without rings, it increases the CO2 conversion from 7% to 16 %, the CH4 conversion from 12% to 23%, and the energy yield from 0.05 mmol/kJ supplied power to 0.1 mmol/kJ (0.19 mmol/kJ if calculated from the plasma power), respectively. The presence of the rings increases the local electric field, the displaced charge and the discharge fraction, and also makes the discharge more stable and with more uniform intensity. It also slightly improves the selectivity to syngas. The performance improvement observed by placing stainless steel rings in this study may also be applicable to other plasma-based processes.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000986051300001 Publication Date 2023-04-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 15.1; 2023 IF: 6.216
Call Number UA @ admin @ c:irua:195603 Serial 7264
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Author Van Dijck, J.G.; Mampuys, P.; Ching, H.Y.V.; Krishnan, D.; Baert, K.; Hauffman, T.; Verbeeck, J.; Van Doorslaer, S.; Maes, B.U.W.; Dorbec, M.; Buekenhoudt, A.; Meynen, V.
Title Synthesis – properties correlation and the unexpected role of the titania support on the Grignard surface modification Type A1 Journal article
Year 2020 Publication Applied Surface Science Abbreviated Journal Appl Surf Sci
Volume 527 Issue Pages (up) 146851-17
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Organic synthesis (ORSY); Applied Electrochemistry & Catalysis (ELCAT)
Abstract While the impact of reaction conditions on surface modification with Grignard reactants has been studied for silica supports, such information is absent for metal oxides like titania. Differences between modified titania and silica are observed, making it paramount to explore the reaction mechanism. A detailed study on the impact of the reaction conditions is reported, with a focus on the chain length of the alkyl Grignard reactant, its concentration, the reaction time and temperature, and the type of titania support. While the increase in the chain length reduces the amount of organic groups on the surface, the concentration, time and temperature show little/no influence on the modification degree. However, the type of titania support used and the percentage of amorphous phase present has a significant impact on the amount of grafted groups. Even though the temperature and concentration show no clear impact on the modification degree, they can cause changes in the surface hydroxyl population, which are thus not linked to the modification degree. Furthermore, the titania support is reduced during functionalization. This reduction dependents on the reaction temperature, the titania support and the chain length of the Grignard reactant. Similarly, this reduction is not linked to the modification degree.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000564205300003 Publication Date 2020-06-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0169-4332 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.7 Times cited 5 Open Access OpenAccess
Notes ; The FWO (Fonds Wetenschappelijk Onderzoek) is gratefully acknowledged for the VITO-FWO grant of fellow Jeroen G. Van Dijck (11W9416N) and the financial support granted in project GO12712N. The E.U. is acknowledged for H.Y. Vincent Ching's H2020-MSCA-IF (grant number 792946, iSPY). Dileep Krishnan and Johan Verbeeck acknowledge funding from GOA project “solarpaint” of the University of Antwerp. ; Approved Most recent IF: 6.7; 2020 IF: 3.387
Call Number UA @ admin @ c:irua:169722 Serial 6712
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Author Ramesha, B.M.; Pawlak, B.; Arenas Esteban, D.; Reekmans, G.; Bals, S.; Marchal, W.; Carleer, R.; Adriaensens, P.; Meynen, V.
Title Partial hydrolysis of diphosphonate ester during the formation of hybrid Tio₂ nanoparticles : role of acid concentration Type A1 Journal article
Year 2023 Publication ChemPhysChem : a European journal of chemical physics and physical chemistry Abbreviated Journal
Volume Issue Pages (up) e202300437-13
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract In the present work, a method was utilized to control the in‐situ partial hydrolysis of a diphosphonate ester in presence of a titania precursor and in function of acid content and its impact on the hybrid nanoparticles was assessed. The hydrolysis degree of organodiphosphonate ester linkers during the formation of hybrid organic‐inorganic metal oxide nanoparticles, are relatively underexplored . Quantitative solution NMR spectroscopy revealed that during the synthesis of TiO2 nanoparticles, an increase in acid concentration introduces a higher degree of partial hydrolysis of the TEPD linker into diverse acid/ester derivatives of TEPD. Increasing the HCl/Ti ratio from 1 to 3, resulted in an increase in degree of partial hydrolysis of the TEPD linker in solution from 4% to 18.8% under the here applied conditions. As a result of the difference in partial hydrolysis, the linker‐TiO2 bonding was altered. Upon subsequent drying of the colloidal TiO2 solution, different textures, at nanoscale and macroscopic scale, were obtained dependent on the HCl/Ti ratio and thus the degree of hydrolysis of TEPD. Understanding such linker‐TiO2 nanoparticle surface dynamics is crucial for making hybrid organic‐inorganic materials (i.e. (porous) metal phosphonates) employed in applications such as electronic/photonic devices, separation technology and heterogeneous catalysts.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001071673900001 Publication Date 2023-09-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1439-4235; 1439-7641 ISBN Additional Links UA library record; WoS full record
Impact Factor 2.9 Times cited Open Access OpenAccess
Notes This work was supported by the Research Foundation-Flanders (FWO Vlaanderen) Project G.0121.17 N. The work was further supported by Hasselt University and the Research Foundation – Flanders (FWO Vlaanderen) via the Hercules project AUHL/15/2 – GOH3816 N. V. M. acknowledges the Research Foundation Flanders (FWO) for project K801621 N. B. M. R. acknowledges, Prof. Dr. Christophe Detavernier and Dr. Davy Deduystche (COCOON, Ghent University) for PXRD and VT-XRD measurements, Prof. Dr. Christophe Van De Velde (iPRACS, University of Antwerp) and Dr. Radu Ciocarlan (LADCA, University of Antwerp) for helpful discussions on PXRD measurements and Dr. Nick Gys (University of Antwerp and VITO) for ICP-OES measurements. Approved Most recent IF: 2.9; 2023 IF: 3.075
Call Number UA @ admin @ c:irua:198934 Serial 8911
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