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Author | Michielsen, I.; Uytdenhouwen, Y.; Pype, J.; Michielsen, B.; Mertens, J.; Reniers, F.; Meynen, V.; Bogaerts, A. | ||||
Title | CO 2 dissociation in a packed bed DBD reactor: First steps towards a better understanding of plasma catalysis | Type | A1 Journal article | ||
Year | 2017 | Publication | Chemical engineering journal | Abbreviated Journal | Chem Eng J |
Volume | 326 | Issue | 326 | Pages | 477-488 |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma catalysis is gaining increasing interest for CO2 conversion, but the interaction between the plasma and catalyst is still poorly understood. This is caused by limited systematic materials research, since most works combine a plasma with commercial supported catalysts and packings. In the present paper, we study the influence of specific material and reactor properties, as well as reactor/bead configuration, on the conversion and energy efficiency of CO2 dissociation in a packed bed dielectric barrier discharge (DBD) reactor. Of the various packing materials investigated, BaTiO3 yields the highest conversion and energy efficiency, i.e., 25% and 4.5%. Our results show that, when evaluating the influence of catalysts, the impact of the packing (support) material itself cannot be neglected, since it can largely affect the conversion and energy efficiency. This shows the large potential for further improvement of packed bed plasma reactors for CO2 conversion and other chemical conversion reactions by adjusting both packing (support) properties and catalytically active sites. Moreover, we clearly prove that comparison of results obtained in different reactor setups should be done with care, since there is a large effect of the reactor setup and reactor/bead configuration. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000406137200047 | Publication Date | 2017-06-01 | |
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 | 49 | Open Access | OpenAccess |
Notes | This research was carried out with financial support of the Institute for the Promotion of Innovation by Science and Technology in Flanders (IWT Flanders) for both I. Michielsen (IWT-141093) and J. Pype (IWT-131229) and of the Walloon region through the excellence programme FLYCOAT (nr. 1318147) for the profilometry measurements. The authors also acknowledge financial support from an IOF-SBO project from the University of Antwerp and from the Fund for Scientific Research (FWO; grant number: G.0254.14 N). This research was carried out in the framework of the network on Physical Chemistry of Plasma-Surface Interactions – Interuniversity Attraction Poles, phase VII (http://psi-iap7.ulb. ac.be/), and supported by the Belgian Science Policy Office (BELSPO). The authors would also like to thank Koen Van Laer for the discussions on this manuscript. | Approved | Most recent IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ c:irua:144802 | Serial | 4626 | ||
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Author | Uytdenhouwen, Y.; Van Alphen, S.; Michielsen, I.; Meynen, V.; Cool, P.; Bogaerts, A. | ||||
Title | A packed-bed DBD micro plasma reactor for CO 2 dissociation: Does size matter? | Type | A1 Journal article | ||
Year | 2018 | Publication | Chemical engineering journal | Abbreviated Journal | Chem Eng J |
Volume | 348 | Issue | Pages | 557-568 | |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | DBD plasma reactors are of great interest for environmental and energy applications, such as CO2 conversion, but they suffer from limited conversion and especially energy efficiency. The introduction of packing materials has been a popular subject of investigation in order to increase the reactor performance. Reducing the discharge gap of the reactor below one millimetre can enhance the plasma performance as well. In this work, we combine both effects and use a packed-bed DBD micro plasma reactor to investigate the influence of gap size reduction, in combination with a packing material, on the conversion and efficiency of CO2 dissociation. Packing materials used in this work were SiO2, ZrO2, and Al2O3 spheres as well as glass wool. The results are compared to a regular size reactor as a benchmark. Reducing the discharge gap can greatly increase the CO2 conversion, although at a lower energy efficiency. Adding a packing material further increases the conversion when keeping a constant residence time, but is greatly dependent on the material composition, gap and sphere size used. Maximum conversions of 50–55% are obtained for very long residence times (30 s and higher) in an empty reactor or with certain packing material combinations, suggesting a balance in CO2 dissociation and recombination reactions. The maximum energy efficiency achieved is 4.3%, but this is for the regular sized reactor at a short residence time (7.5 s). Electrical characterization is performed to reveal some trends in the electrical behaviour of the plasma upon reduction of the discharge gap and addition of a packing material. | ||||
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Language | Wos | 000434467000055 | Publication Date | 2018-05-03 | |
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ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.216 | Times cited | 22 | Open Access | Not_Open_Access: Available from 03.05.2020 |
Notes | We 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) and an IOF-SBO (SynCO2Chem) project from the University of Antwerp. | Approved | Most recent IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:151238 | Serial | 4956 | ||
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Author | Uytdenhouwen, Y.; Bal, Km.; Michielsen, I.; Neyts, Ec.; Meynen, V.; Cool, P.; Bogaerts, A. | ||||
Title | How process parameters and packing materials tune chemical equilibrium and kinetics in plasma-based CO2 conversion | Type | A1 Journal article | ||
Year | 2019 | Publication | Chemical engineering journal | Abbreviated Journal | Chem Eng J |
Volume | 372 | Issue | Pages | 1253-1264 | |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma (catalysis) reactors are increasingly being used for gas-based chemical conversions, providing an alternative method of energy delivery to the molecules. In this work we explore whether classical concepts such as equilibrium constants, (overall) rate coefficients, and catalysis exist under plasma conditions. We specifically investigate the existence of a so-called partial chemical equilibrium (PCE), and how process parameters and packing properties influence this equilibrium, as well as the overall apparent rate coefficient, for CO2 splitting in a DBD plasma reactor. The results show that a PCE can be reached, and that the position of the equilibrium, in combination with the rate coefficient, greatly depends on the reactor parameters and operating conditions (i.e., power, pressure, and gap size). A higher power, higher pressure, or smaller gap size enhance both the equilibrium constant and the rate coefficient, although they cannot be independently tuned. Inserting a packing material (non-porous SiO2 and ZrO2 spheres) in the reactor reveals interesting gap/material effects, where the type of material dictates the position of the equilibrium and the rate (inhibition) independently. As a result, no apparent synergistic effect or plasma-catalytic behaviour was observed for the non-porous packing materials studied in this reaction. Within the investigated parameters, equilibrium conversions were obtained between 23 and 71%, while the rate coefficient varied between 0.027 s−1 and 0.17 s−1. This method of analysis can provide a more fundamental insight in the overall reaction kinetics of (catalytic) plasma-based gas conversion, in order to be able to distinguish plasma effects from true catalytic enhancement. |
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Language | Wos | 000471670400116 | Publication Date | 2019-05-08 | |
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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 | 3 | Open Access | Not_Open_Access: Available from 05.05.2021 |
Notes | European Fund for Regional Development; FWOFWO, G.0254.14N ; University of Antwerp; FWO-FlandersFWO-Flanders, 11V8915N ; 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. K. M. B. was funded as a PhD fellow (aspirant) of the FWOFlanders (Fund for Scientific Research-Flanders), Grant 11V8915N. | Approved | Most recent IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @UA @ admin @ c:irua:159979 | Serial | 5171 | ||
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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 | 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. | ||||
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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 | 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. | ||||
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Language | Wos | 000966076400001 | Publication Date | 2023-03-21 | |
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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 | 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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Language | Wos | 000986051300001 | Publication Date | 2023-04-17 | |
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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 | 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 | 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%). | ||||
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Language | Wos | 000634280300004 | Publication Date | 2021-02-15 | |
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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 | van Oers, C.J.; Kurttepeli, M.; Mertens, M.; Bals, S.; Meynen, V.; Cool, P. | ||||
Title | Zeolite \beta nanoparticles based bimodal structures : mechanism and tuning of the porosity and zeolitic properties | Type | A1 Journal article | ||
Year | 2014 | Publication | Microporous and mesoporous materials: zeolites, clays, carbons and related materials | Abbreviated Journal | Micropor Mesopor Mat |
Volume | 185 | Issue | Pages | 204-212 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) | ||||
Abstract | Despite great efforts in the research area of zeolite nanoparticles and their use in the synthesis of bimodal materials, still little is known about the impact of the synthesis conditions of the zeolite nanoparticles on its own characteristics, and on the properties and the formation mechanism of the final bimodal materials. A zeolite β nanoparticles solution is applied in a mesotemplate-free synthesis method, and the influence of the hydrothermal ageing temperature of the nanoparticles solution on both the zeolitic and porosity characteristics of the final bimodal material has been studied. Transmission electron microscopy in combination with 3-dimensional reconstructions obtained by electron tomography revealed that the zeolite β nanoparticles are connected by neck-like structures, thus creating a wormhole-like mesoporous material. Considering the zeolitic properties, a clear threshold is observed in the synthesis temperature series at 413 K. Below and at this threshold, the biporous materials show no apparent zeolitic characteristics, although these materials exhibit a more condensed and uniform SiOSi network in comparison to Al-MCF. Synthesis temperatures above the threshold lead to bimodal structures with defined zeolitic properties. Moreover, the dimensions of the nanoparticles are studied by TEM, revealing an increasing particle size with increasing temperature under the threshold of 413 K, which is in agreement with a sol-mechanism. This mechanism is disturbed after the threshold due to the start of the crystallisation process. | ||||
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Publisher | Place of Publication | Amsterdam | Editor | ||
Language | Wos | 000330930400025 | Publication Date | 2013-11-21 | |
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ISSN | 1387-1811; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.615 | Times cited | 10 | Open Access | OpenAccess |
Notes | 262348 Esmi | Approved | Most recent IF: 3.615; 2014 IF: 3.453 | ||
Call Number | UA @ lucian @ c:irua:112501 | Serial | 3930 | ||
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Author | Rahemi, V.; Trashin, S.; Hafideddine, Z.; Meynen, V.; Van Doorslaer, S.; De Wael, K. | ||||
Title | Enzymatic sensor for phenols based on titanium dioxide generating surface confined ROS after treatment with H2O2 | Type | A1 Journal article | ||
Year | 2019 | Publication | Sensors and actuators : B : chemical | Abbreviated Journal | Sensor Actuat B-Chem |
Volume | 283 | Issue | 283 | Pages | 343-348 |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) | ||||
Abstract | Titanium dioxide (TiO2) is a popular material as host matrix for enzymes. We now evidence that TiO2 can accumulate and retain reactive oxygen species after treatment by hydrogen peroxide (H2O2) and support redox cycling of a phenolic analyte between horseradish peroxidase (HRP) and an electrode. The proposed detection scheme is identical to that of second generation biosensors, but the measuring solution requires no dissolved H2O2. This significantly simplifies the analysis and overcomes issues related to H2O2 being present (or generated) in the solution. The modified electrodes showed rapid stabilization of the baseline, a low noise level, fast realization of a steady-state current response, and, in addition, improved sensitivity and limit of detection compared to the conventional approach, i.e. in the presence of H2O2 in the measuring solution. Hydroquinone, 4-aminophenol, and other phenolic compounds were successfully detected at sub-μM concentrations. Particularly, a linear response in the concentration range between 0.025 and 2 μM and LOD of 24 nM was demonstrated for 4-aminophenol. The proposed sensor design goes beyond the traditional concept with three sensors generations offering a new possibility for the development of enzymatic sensors based on peroxidases and the formation of ROS on titania after treatment with H2O2. | ||||
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Language | Wos | 000455854000043 | Publication Date | 2018-12-10 | |
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ISSN | 0925-4005 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.401 | Times cited | 1 | Open Access | |
Notes | ; The authors thank the University of Antwerp for GOA funding and the Scientific Research-Flanders (FWO) (grant 12T4219N). V. Rahemi is financially supported through a postdoctoral fellowship of the Research Foundation-Flanders (FWO). ; | Approved | Most recent IF: 5.401 | ||
Call Number | UA @ admin @ c:irua:155665 | Serial | 5605 | ||
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Author | Rahemi, V.; Trashin, S.; Meynen, V.; De Wael, K. | ||||
Title | An adhesive conducting electrode material based on commercial mesoporous titanium dioxide as a support for Horseradish peroxidase for bioelectrochemical applications | Type | A1 Journal article | ||
Year | 2016 | Publication | Talanta : the international journal of pure and applied analytical chemistry | Abbreviated Journal | Talanta |
Volume | 146 | Issue | Pages | 689-693 | |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) | ||||
Abstract | An adhesive conducting electrode material containing of graphite, biocompatible ion exchange polymer nafion® and commercial mesoporous TiO2 impregnated with horseradish peroxidase (HRP) is prepared and characterized by amperometric, UVvis and N2 sorption methods. The factors influencing the performance of the resulting biosensor are studied in detail. The optimal electrode material consists of 45% graphite, 50% impregnated HRPTiO2 and 5% nafion®. The optimum conditions for H2O2 reduction are an applied potential of 0.3 V and 0.1 mM hydroquinone. Sensitivity and limit of detection in the optimum conditions are 1 A M−1 cm−2 and 1 µM correspondingly. The N2 sorption results show that the pore volume of TiO2 decreases sharply upon adsorption of HRP. The preparation process of the proposed enzyme electrode is straightforward and potentially can be used for preparation of carbon paste electrodes for bioelectrochemical detections. | ||||
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Language | Wos | 000363815600093 | Publication Date | 2015-06-24 | |
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ISSN | 0039-9140; 1873-3573 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.162 | Times cited | 7 | Open Access | |
Notes | ; The authors thank the Fund for Scientific Research – Flanders (FWO) (Grant G.0687.13), the GOA-BOF UA 2013-2016 (project-ID 28312) for funding and Ward Huybrechts of the University of Antwerp, Laboratory of Adsorption and Catalysis (LADCA) for help with the N<INF>2</INF> sorption. ; | Approved | Most recent IF: 4.162 | ||
Call Number | UA @ admin @ c:irua:126495 | Serial | 5458 | ||
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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 | 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. | ||||
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Language | Wos | 000518234700023 | Publication Date | 2020-01-27 | |
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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 | 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 | 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. |
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Language | Wos | 000417228500017 | Publication Date | 2017-11-30 | |
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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 | 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 | 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. | ||||
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Language | Wos | 000402488300013 | Publication Date | 2017-04-27 | |
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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 | Uytdenhouwen, Y.; Meynen, V.; Cool, P.; Bogaerts, A. | ||||
Title | The Potential Use of Core-Shell Structured Spheres in a Packed-Bed DBD Plasma Reactor for CO2 Conversion | Type | A1 Journal article | ||
Year | 2020 | Publication | Catalysts | Abbreviated Journal | Catalysts |
Volume | 10 | Issue | 5 | Pages | 530 |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | This work proposes to use core-shell structured spheres to evaluate whether it allows to individually optimize bulk and surface effects of a packing material, in order to optimize conversion and energy efficiency. Different core-shell materials have been prepared by spray coating, using dense spheres (as core) and powders (as shell) of SiO2, Al2O3, and BaTiO3. The materials are investigated for their performance in CO2 dissociation and compared against a benchmark consisting of a packed-bed reactor with the pure dense spheres, as well as an empty reactor. The results in terms of CO2 conversion and energy efficiency show various interactions between the core and shell material, depending on their combination. Al2O3 was found as the best core material under the applied conditions here, followed by BaTiO3 and SiO2, in agreement with their behaviour for the pure spheres. Applying a thin shell layer on the cores showed equal performance between the different shell materials. Increasing the layer thickness shifts this behaviour, and strong combination effects were observed depending on the specific material. Therefore, this method of core-shell spheres has the potential to allow tuning of the packing properties more closely to the application by designing an optimal combination of core and shell. | ||||
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Language | Wos | 000546007000092 | Publication Date | 2020-05-11 | |
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ISSN | 2073-4344 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.9 | Times cited | Open Access | ||
Notes | Interreg, Project EnOp ; Fonds Wetenschappelijk Onderzoek, G.0254.14N ; Universiteit Antwerpen, Project SynCO2Chem ; We want to thank Jasper Lefevre (VITO) for assistance in the development of the coating suspension for the core-shell spheres. | Approved | Most recent IF: 3.9; 2020 IF: 3.082 | ||
Call Number | PLASMANT @ plasmant @c:irua:169222 | Serial | 6364 | ||
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Author | Michielsen, I.; Uytdenhouwen, Y.; Bogaerts, A.; Meynen, V. | ||||
Title | Altering conversion and product selectivity of dry reforming of methane in a dielectric barrier discharge by changing the dielectric packing material | Type | A1 Journal article | ||
Year | 2019 | Publication | Catalysts | Abbreviated Journal | Catalysts |
Volume | 9 | Issue | 1 | Pages | 51 |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We studied the influence of dense, spherical packing materials, with different chemical compositions, on the dry reforming of methane (DRM) in a dielectric barrier discharge (DBD) reactor. Although not catalytically activated, a vast effect on the conversion and product selectivity could already be observed, an influence which is often neglected when catalytically activated plasma packing materials are being studied. The alpha-Al2O3 packing material of 2.0-2.24 mm size yields the highest total conversion (28%), as well as CO2 (23%) and CH4 (33%) conversion and a high product fraction towards CO (similar to 70%) and ethane (similar to 14%), together with an enhanced CO/H-2 ratio of 9 in a 4.5 mm gap DBD at 60 W and 23 kHz. gamma-Al2O3 is only slightly less active in total conversion (22%) but is even more selective in products formed than alpha-Al2O3 BaTiO3 produces substantially more oxygenated products than the other packing materials but is the least selective in product fractions and has a clear negative impact on CO2 conversion upon addition of CH4. Interestingly, when comparing to pure CO2 splitting and when evaluating differences in products formed, significantly different trends are obtained for the packing materials, indicating a complex impact of the presence of CH4 and the specific nature of the packing materials on the DRM process. | ||||
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Language | Wos | 000459732000051 | Publication Date | 2019-01-10 | |
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ISSN | 2073-4344 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles; WoS full record; WoS citing articles | |
Impact Factor | 3.082 | Times cited | 4 | Open Access | OpenAccess |
Notes | Approved | Most recent IF: 3.082 | |||
Call Number | UA @ admin @ c:irua:158666 | Serial | 5268 | ||
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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 | 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. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-05-25 | ||
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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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