“Hybrid plasma-thermal system for methane conversion to ethylene and hydrogen”. Liu R, Hao Y, Wang T, Wang L, Bogaerts A, Guo H, Yi Y, Chemical engineering journal 463, 142442 (2023). http://doi.org/10.1016/j.cej.2023.142442
Abstract: By combining dielectric barrier discharge plasma and external heating, we exploit a two-stage hybrid plasmathermal
system (HPTS), i.e., a plasma stage followed by a thermal stage, for direct non-oxidative coupling of
CH4 to C2H4 and H2, yielding a CH4 conversion of ca. 17 %. In the two-stage HPTS, the plasma first converts CH4
into C2H6 and C3H8, which in the thermal stage leads to a high C2H4 selectivity of ca. 63 % by pyrolysis, with H2
selectivity of ca. 64 %.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/j.cej.2023.142442
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“How process parameters and packing materials tune chemical equilibrium and kinetics in plasma-based CO2 conversion”. Uytdenhouwen Y, Bal Km, Michielsen I, Neyts Ec, Meynen V, Cool P, Bogaerts A, Chemical engineering journal 372, 1253 (2019). http://doi.org/10.1016/j.cej.2019.05.008
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.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
Times cited: 3
DOI: 10.1016/j.cej.2019.05.008
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“How gas flow design can influence the performance of a DBD plasma reactor for dry reforming of methane”. Uytdenhouwen Y, Hereijgers J, Breugelmans T, Cool P, Bogaerts A, Chemical Engineering Journal 405, 126618 (2021). http://doi.org/10.1016/j.cej.2020.126618
Abstract: DBD plasma reactors are commonly used in a static ‘one inlet – one outlet’ design that goes against reactor design principles for multi-component reactions, such as dry reforming of methane (DRM). Therefore, in this paper we have developed a novel reactor design, and investigated how the shape and size of the reaction zone, as well as gradual gas addition, and the method of mixing CO2 and CH4 can influence the conversion and product com position of DRM. Even in the standard ‘one inlet – one outlet’ design, the direction of the gas flow (i.e. short or long path through the reactor, which defines the gas velocity at fixed residence time), as well as the dimensions of the reaction zone and the power delivery to the reactor, largely affect the performance. Using gradual gas addition and separate plasma activation zones for the individual gases give increased conversions within the same operational parameters, by optimising mixing ratios and kinetics. The choice of the main (pre-activated) gas and the direction of gas flow largely affect the conversion and energy cost, while the gas inlet position during separate addition only influences the product distribution.
Keywords: A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 6.216
DOI: 10.1016/j.cej.2020.126618
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“Gliding arc plasma for CO 2 conversion: Better insights by a combined experimental and modelling approach”. Wang W, Mei D, Tu X, Bogaerts A, Chemical engineering journal 330, 11 (2017). http://doi.org/10.1016/j.cej.2017.07.133
Abstract: A gliding arc plasma is a potential way to convert CO2 into CO and O2, due to its non-equilibrium character, but little is known about the underlying mechanisms. In this paper, a self-consistent two-dimensional (2D) gliding arc model is developed, with a detailed non-equilibrium CO2 plasma chemistry, and validated with experiments. Our calculated values of the electron number density in the plasma, the CO2 conversion and energy efficiency show reasonable agreement with the experiments, indicating that the model can provide a realistic picture of the plasma chemistry. Comparison of the results with classical thermal conversion, as well as other plasma-based technologies for CO2 conversion reported in literature, demonstrates the non-equilibrium character of the gliding arc, and indicates that the gliding arc is a promising plasma reactor for CO2 conversion. However, some process modifications should be exploited to further improve its performance. As the model provides a realistic picture of the plasma behaviour, we use it first to investigate the plasma characteristics in a whole gliding arc cycle, which is necessary to understand the underlying mechanisms. Subsequently, we perform a chemical kinetics analysis, to investigate the different pathways for CO2 loss and formation. Based on the revealed discharge properties and the underlying CO2 plasma chemistry, the model allows us to propose solutions on how to further improve the
CO2 conversion and energy efficiency by a gliding arc plasma.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
Times cited: 38
DOI: 10.1016/j.cej.2017.07.133
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“Gas-solid hydrodynamics in a stator-rotor vortex chamber reactor”. Lang X, Ouyang Y, Vandewalle LA, Goshayeshi B, Chen S, Madanikashani S, Perreault P, Van Geem KM, van Geem KM, Chemical engineering journal 446, 137323 (2022). http://doi.org/10.1016/J.CEJ.2022.137323
Abstract: The gas-solid vortex reactor (GSVR) has enormous process intensification potential. However the huge gas consumption can be a serious disadvantage for the GSVR in some applications such as fast pyrolysis. In this work, we demonstrate a recent novel design, where a stator-rotor vortex chamber (STARVOC) is driven by the fluid's kinetic energy, to decouple the solids bed rotation and gas. Gas-solid fluidization by using air and monosized aluminum balls was performed to investigate the hydrodynamics. A constructed fluidization flow regime map for a fixed solids loading of 100 g shows that the bed can only be fluidized for a rotation speed between 200 and 400 RPM. Below 200 RPM, particles settle down on the bottom plate and cannot form a stable bed due to inertia and friction. Above 400 RPM, the bed cannot be fluidized with superficial velocities up to 1.8 m/s (air flow rate of 90 Nm(3)/h). The bed thickness shows some non-uniformities, being smaller at the top of the bed than at the bottom counterpart. However by increasing the air flow rate or rotation speed the axial nonuniformity can be resolved. The bed pressure drop first increases with increasing gas flow rate and then levels off, showing similar characteristics as conventional fluidized beds. Theoretical pressure drops calculated from mathematical models such as Kao et al. model agree well with experimental measurements. Particle velocity discrepancies between the top and bottom particles reveal that the impact of gravity cannot be completely neglected. Design guidelines and possible applications for further development of STARVOC concept are proposed based on fundamental data provided in this work.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2022.137323
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“Gas phase photocatalytic spiral reactor for fast and efficient pollutant degradation”. Blommaerts N, Asapu R, Claes N, Bals S, Lenaerts S, Verbruggen SW, Chemical engineering journal 316, 850 (2017). http://doi.org/10.1016/j.cej.2017.02.038
Abstract: Photocatalytic reactors for the degradation of gaseous organic pollutants often suffer from major limitations such as small reaction area, sub-optimal irradiation conditions and thus limited reaction rate. In this work, an alternative solution is presented that involves a glass tube coated on the inside with (silvermodified) TiO2 and spiraled around a UVA lamp. First, the spiral reactor is coated from the inside with TiO2 using an experimentally verified procedure that is optimized toward UV light transmission. This procedure is kept as simple as possible and involves a single casting step of a 1 wt% suspension of TiO2 in ethanol through the spiral. This results in a coated tube that absorbs nearly all incident UV light under the experimental conditions used. The optimized coated spiral reactor is then benchmarked to a conventional annular photoreactor of the same outer dimensions and total catalyst loading over a broad range of experimental conditions. Although residence time distribution experiments indicate slightly longer dwelling of molecules in the spiral reactor, no significant difference in by-passing of gas between the spiral reactor and the annular reactor can be claimed. Acetaldehyde degradation efficiency of 100% is obtained with the spiral reactor for a residence time as low as 60 s, whereas the annular reactor could not achieve full degradation even at 1000 s residence time. In a final case study, addition of long-term stable silver nanoparticles, protected by an ultra-thin polymer shell applied via the layer-by-layer (LbL) method, to the spiral reactor coating is shown to double the degradation efficiency and provides an interesting strategy to cope with higher pollutant concentrations without changing the overall dimensions.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
Times cited: 30
DOI: 10.1016/j.cej.2017.02.038
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“Effusion nozzle for energy-efficient NOx production in a rotating gliding arc plasma reactor”. Van Alphen S, Ahmadi Eshtehardi H, O'Modhrain C, Bogaerts J, Van Poyer H, Creel J, Delplancke M-P, Snyders R, Bogaerts A, Chemical Engineering Journal 443, 136529 (2022). http://doi.org/10.1016/j.cej.2022.136529
Abstract: Plasma-based NOx production is of interest for sustainable N2 fixation, but more research is needed to improve its performance. One of the current limitations is recombination of NO back into N2 and O2 molecules immediately after the plasma reactor. Therefore, we developed a novel so-called “effusion nozzle”, to improve the performance of a rotating gliding arc plasma reactor for NOx production, but the same principle can also be applied to other plasma types. Experiments in a wide range of applied power, gas flow rates and N2/O2 ratios demonstrate an enhancement in NOx concentration by about 8%, and a reduction in energy cost by 22.5%. In absolute terms, we obtain NOx concentrations up to 5.9%, at an energy cost down to 2.1 MJ/mol, which are the best values reported to date in literature. In addition, we developed four complementary models to describe the gas flow, plasma temperature and plasma chemistry, aiming to reveal why the effusion nozzle yields better performance. Our simulations reveal that the effusion nozzle acts as very efficient heat sink, causing a fast drop in gas temperature when the gas molecules leave the plasma, hence limiting the recombination of NO back into N2 and O2. This yields an overall higher NOx concentration than without the effusion nozzle. This immediate quenching right at the end of the plasma makes our effusion nozzle superior to more conventional cooling options, like water cooling In addition, this higher NOx concentration can be obtained at a slightly lower power, because the effusion nozzle allows for the ignition and sustainment of the plasma at somewhat lower power. Hence, this also explains the lower energy cost. Overall, our experimental results and detailed modeling analysis will be useful to improve plasma-based NOx production in other plasma reactors as well.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/j.cej.2022.136529
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“Dry reforming in a dielectric barrier discharge reactor with non-uniform discharge gap : effects of metal rings on the discharge behavior and performance”. Wang J, Zhang K, Meynen V, Bogaerts A, Chemical engineering journal , 142953 (2023). http://doi.org/10.1016/J.CEJ.2023.142953
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.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2023.142953
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“Development of a novel type activated carbon fiber filter for indoor air purification”. Roegiers J, Denys S, Chemical Engineering Journal 417, 128109 (2021). http://doi.org/10.1016/J.CEJ.2020.128109
Abstract: A novel type of activated carbon fiber filter was developed for indoor air purification. The filter is equipped with electrodes for thermo-electrical regeneration at the point of saturation. The electrodes are arranged in such a way that the filter forms a pleated structure with an electrode in the tip of each pleat. This allows for a uniform temperature distribution on the filter surface during the regeneration process and the pleated structure reduces the overall pressure drop across the filter. The latter was validated by Computational Fluid Dynamics, using Darcy-Forchheimer parameters derived in previous work. The CFD model was further used to perform a virtual sensitivity study in search for the optimal ACF filter design by varying the pleat length, pleat height and filter thickness. Finally, adsorption and desorption properties were investigated with acetaldehyde and toluene as model compounds. Freundlich and Langmuir adsorption parameters, derived in previous work were successfully validated with a Multiphysics model.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
DOI: 10.1016/J.CEJ.2020.128109
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“Determination of intrinsic kinetic parameters in photocatalytic multi-tube reactors by combining the NTUm-method with radiation field modelling”. van Walsem J, Roegiers J, Modde B, Lenaerts S, Denys S, Chemical engineering journal 354, 1042 (2018). http://doi.org/10.1016/J.CEJ.2018.08.010
Abstract: In this work, we propose an adapted Number of Transfer Units (NTUm)-method as an effective tool to determine the Langmuir-Hinshelwood kinetic parameters for a photocatalytic multi-tube reactor. The Langmuir-Hinshelwood rate constant kLH and the Langmuir adsorption constant KL were determined from several experiments under different UV-irradiance conditions, resulting in irradiance depending values for kLH. In order to determine a unique, intrinsic empirical constant k0, valid for all irradiation conditions, we coupled the adapted NTUm-method with a radiation field model to predict UV-irradiance distribution inside the reactor. The final set of kinetic parameters were derived using a Generalized Reduced Gradient (GRG) nonlinear solving method in Matlab which minimizes the differences between model and experimental reactor outlet concentrations of acetaldehyde for various photocatalytic experiments under varying operating conditions, including inlet concentration, flow rate and UV-irradiance. An excellent agreement of the intrinsic empirical constant k0, derived from the coupled NTUm-radiation field model and an earlier published CFD approach was found, emphasizing its validity and reliability.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
Times cited: 2
DOI: 10.1016/J.CEJ.2018.08.010
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“Coupled multi-dimensional modelling of warm plasmas: Application and validation for an atmospheric pressure glow discharge in CO2/CH4/O2”. Maerivoet S, Tsonev I, Slaets J, Reniers F, Bogaerts A, Chemical Engineering Journal 492, 152006 (2024). http://doi.org/10.1016/j.cej.2024.152006
Abstract: To support experimental research into gas conversion by warm plasmas, models should be developed to explain the experimental observations. These models need to describe all physical and chemical plasma properties in a coupled way. In this paper, we present a modelling approach to solve the complete set of assumed relevant equations, including gas flow, heat balance and species transport, coupled with a rather extensive chemistry set, consisting of 21 species, obtained by reduction of a more detailed chemistry set, consisting of 41 species. We apply this model to study the combined CO2 and CH4 conversion in the presence of O2, in a direct current atmospheric pressure glow discharge. Our model can predict the experimental trends, and can explain why higher O2 fractions result in higher CH4 conversion, namely due to the higher gas temperature, rather than just by additional chemical reactions. Indeed, our model predicts that when more O2 is added, the energy required to reach any set temperature (i.e., the enthalpy) drops, allowing the system to reach higher temperatures with similar amounts of energy. This is in turn related to the higher H2O fraction and lower H2 fraction formed in the plasma, as demonstrated by our model. Altogether, our new self-consistent model can capture the main physics and chemistry occurring in this warm plasma, which is an important step towards predictive modelling for plasma-based gas conversion.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 15.1
DOI: 10.1016/j.cej.2024.152006
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“CO 2 dissociation in a packed bed DBD reactor: First steps towards a better understanding of plasma catalysis”. Michielsen I, Uytdenhouwen Y, Pype J, Michielsen B, Mertens J, Reniers F, Meynen V, Bogaerts A, Chemical engineering journal 326, 477 (2017). http://doi.org/10.1016/j.cej.2017.05.177
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.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
Times cited: 49
DOI: 10.1016/j.cej.2017.05.177
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“CFD-modelling of activated carbon fibers for indoor air purification”. Roegiers J, Denys S, Chemical engineering journal 365, 80 (2019). http://doi.org/10.1016/J.CEJ.2019.02.007
Abstract: Activated carbon fibers for indoor air purification were investigated by means of pressure drop and adsorption capacity. The Darcy-Forchheimer law combined with Computational Fluid Dynamics (CFD) modelling was deployed to simulate the pressure drop over an activated carbon fiber (ACF) filter with varying filter thickness. The CFD model was later combined with adsorption modelling to simulate breakthrough profiles of acetaldehyde adsorption on the ACF-filter. The adsorption model incorporates mass transfer resistance and adsorption equilibrium. It assumes local equilibrium between gas phase and solid phase. The latter was investigated for three different adsorption isotherms: linear, Langmuir and Freundlich adsorption. Successful agreement between model simulations and experimental data was obtained, using the Freundlich adsorption model. The numerical model could provide valuable insights and allows to continuously improve the design of filtration devices.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1016/J.CEJ.2019.02.007
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“CFD- and radiation field modeling of a gas phase photocatalytic multi-tube reactor”. Roegiers J, van Walsem J, Denys S, Chemical engineering journal 338, 287 (2018). http://doi.org/10.1016/J.CEJ.2018.01.047
Abstract: This paper focusses on the development of a Multiphysics model as a tool for assessing the performance of a multi-tube photoreactor. The model predicts the transient behavior of acetaldehyde concentration, as a model compound for the organic fraction of the indoor air pollutants, under varying sets of conditions. A 3D-model couples radiation field modeling with reaction kinetics and fluid dynamics in order to simulate the transport of the pollutant as it progresses through the reactor. A model-based approach is proposed to determine the layer thickness and refractive index of different P25-powder modified solgel coatings, using an optimization procedure to estimate these parameters based on UV-irradiance measurements. The radiation field model was able to accurately predict the irradiance on the catalytic surface within the reactor. Consequently, the radiation field model was used to define an irradiance dependent reaction rate constant in a coupled Multiphysics model. An optimization routine was deployed to estimate the adsorption, desorption- and photocatalytic reaction rate constants on the TiO2-surface, using experimentally determined, transient outlet concentrations of acetaldehyde. Additionally, a validation test was performed in an air-tight climate chamber at much higher flow rates, higher irradiance and realistic indoor pollutant concentrations to emphasize the reliability and accuracy of the parameters for adsorption, desorption and photocatalytic reaction. The developed model makes it possible to optimize the reactor design and scale-up for commercial applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1016/J.CEJ.2018.01.047
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“CFD modeling of transient adsorption/desorption behavior in a gas phase photocatalytic fiber reactor”. Verbruggen SW, Keulemans M, van Walsem J, Tytgat T, Lenaerts S, Denys S, Chemical engineering journal 292, 42 (2016). http://doi.org/10.1016/J.CEJ.2016.02.014
Abstract: We present the use of computational fluid dynamics (CFD) for accurately determining the adsorption parameters of acetaldehyde on photocatalytic fiber filter material, integrated in a continuous flow system. Unlike the traditional analytical analysis based on Langmuir adsorption, not only steady-state situations but also transient phenomena can be accounted for. Air displacement effects in the reactor and gas detection cell are investigated and inherently made part of the model. Incorporation of a surface aldol condensation reaction in the CFD analysis further improves the accuracy of the model which enables to extract precise, intrinsic adsorption parameters for situations in which analytical analysis would otherwise fail.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
Times cited: 12
DOI: 10.1016/J.CEJ.2016.02.014
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“CFD investigation of a multi-tube photocatalytic reactor in non-steady-state conditions”. van Walsem J, Verbruggen SW, Modde B, Lenaerts S, Denys S, Chemical engineering journal 304, 808 (2016). http://doi.org/10.1016/J.CEJ.2016.07.028
Abstract: A novel multi-tube photoreactor is presented with a high efficiency (over 90% conversion) toward the degradation of acetaldehyde in air under UV conditions with an incident intensity of 2.1 mW cm−2. A CFD model was developed to simulate the transient adsorption and photocatalytic degradation processes of acetaldehyde in this reactor design and to estimate the corresponding kinetic parameters through an optimization routine using the experimentally determined outlet concentration profiles. The CFD model takes into account the entire reactor geometry and all relevant flow parameters, in contrast to analytical methods that often oversimplify the physical and chemical process characteristics. Using CFD, we show that both adsorption and desorption rate constants increase by respectively one and two orders of magnitude when the UV light is switched on, which clearly affects the transient behavior. The agreement of the experimental and modelled concentration profiles is excellent as evidenced by a coefficient of determination of at least 0.965. To demonstrate the reliability and accuracy of all parameters obtained from the modelling approach, an ultimate validation test was performed using other conditions than the ones used for estimating the kinetic parameters. The model was able to accurately simulate simultaneous adsorption, desorption and photocatalytic degradation.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
Times cited: 10
DOI: 10.1016/J.CEJ.2016.07.028
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“Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions”. Wang Y, Chen Y, Harding J, He H, Bogaerts A, Tu X, Chemical Engineering Journal 450, 137860 (2022). http://doi.org/10.1016/j.cej.2022.137860
Abstract: Direct conversion of CH4 and CO2 to liquid fuels and chemicals under mild conditions is appealing for biogas conversion and utilization but challenging due to the inert nature of both gases. Herein, we report a promising plasma process for the catalyst-free single-step conversion of CH4 and CO2 into higher value oxygenates (i.e., methanol, acetic acid, ethanol, and acetone) at ambient pressure and room temperature using a water-cooled dielectric barrier discharge (DBD) reactor, with methanol being the main liquid product. The distribution of liquid products could be tailored by tuning the discharge power, reaction temperature and residence time. Lower discharge powers (10–15 W) and reaction temperatures (5–20 ◦ C) were favourable for the production of liquid products, achieving the highest methanol selectivity of 43% at 5 ◦ C and 15 W. A higher discharge power and reaction temperature, on the other hand, produced more gaseous products, particularly H2 (up to 26% selectivity) and CO (up to 33% selectivity). In addition, varying these process parameters (discharge power, reaction temperature and residence time) resulted in a simultaneous change in key discharge properties, such as mean electron energy (Ee), electron density (ne) and specific energy input (SEI), all of which are essential determiners of plasma chemical reactions. According to the results of artificial neural network (ANN) models, the relative importance of these process parameters and key discharge indicators on reaction performance follows the order: discharge power > reaction temperature > residence time, and SEI > ne > Ee, respectively. This work provides new insights into the contributions and tuning mechanism of multiple parameters for optimizing the reaction performance (e.g., liquid production) in the plasma gas conversion process.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/j.cej.2022.137860
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“Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream”. Girard-Sahun F, Biondo O, Trenchev G, van Rooij G, Bogaerts A, Chemical Engineering Journal 442, 136268 (2022). http://doi.org/10.1016/j.cej.2022.136268
Abstract: CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/j.cej.2022.136268
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“Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream”. Girard-Sahun F, Biondo O, Trenchev G, van Rooij G, Bogaerts A, Chemical Engineering Journal 442, 136268 (2022). http://doi.org/10.1016/j.cej.2022.136268
Abstract: CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/j.cej.2022.136268
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“Atmospheric pressure glow discharge for CO2 conversion : model-based exploration of the optimum reactor configuration”. Trenchev G, Nikiforov A, Wang W, Kolev S, Bogaerts A, Chemical engineering journal 362, 830 (2019). http://doi.org/10.1016/J.CEJ.2019.01.091
Abstract: We investigate the performance of an atmospheric pressure glow discharge (APGD) reactor for CO2 conversion in three different configurations, through experiments and simulations. The first (basic) configuration utilizes the well-known pin-to-plate design, which offers a limited conversion. The second configuration improves the reactor performance by employing a vortex-flow generator. The third, “confined” configuration is a complete redesign of the reactor, which encloses the discharge in a limited volume, significantly surpassing the conversion rate of the other two designs. The plasma properties are investigated using an advanced plasma model.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
Times cited: 4
DOI: 10.1016/J.CEJ.2019.01.091
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“Angular momentum based-analysis of gas-solid fluidized beds in vortex chambers”. Orozco-Jimenez AJ, Pinilla-Fernandez DA, Pugliese V, Bula A, Perreault P, Gonzalez-Quiroga A, Chemical engineering journal 457, 141222 (2023). http://doi.org/10.1016/J.CEJ.2022.141222
Abstract: Gas-solid vortex chambers are a promising alternative for reactive and non-reactive processes requiring enhanced heat and mass transfer rates and order-of-milliseconds contact time. The conservation of angular momentum is instrumental in understanding how the interactions between gas, particulate solids, and chamber walls influence the formation of a rotating solids bed. Therefore, this work applies the conservation of angular momentum to derive a model that gives the average angular velocity of solids in terms of gas injection velocity, wall-solids bed drag coefficient, gas and particle properties, and chamber geometry. Three datasets from published studies, comprising 1 g-Geldart B- and d-type particles in different vortex chambers, validate the model results. Using a sensitivity analysis, we assessed the effect of input variables on the average angular velocity of solids, average void fraction, and average bed height. Results indicate that the top and bottom end-wall boundaries exert the most significant braking effect on the rotating solids bed compared with the cylindrical outer wall and gas injection boundaries. The wall-solids bed drag coefficient appears independent of the gas injection velocity for a wide range of operating conditions. The proposed model is a valuable tool for analyzing and comparing gas–solid vortex typologies, unraveling improvement opportunities, and scale-up.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2022.141222
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“Analytic versus CFD approach for kinetic modeling of gas phase photocatalysis”. Verbruggen SW, Lenaerts S, Denys S, Chemical engineering journal 262, 1 (2015). http://doi.org/10.1016/J.CEJ.2014.09.041
Abstract: In this work two methods for determining the LangmuirHinshelwood kinetic parameters for a slit-shaped flat bed photocatalytic reactor are compared: an analytic mass transfer based model adapted from literature and a computational fluid dynamics (CFD) approach that was used in conjunction with a simplex optimization routine. Despite the differences between both approaches, similar values for the kinetic parameters and similar trends in terms of their UV intensity dependence were found. Using an effectiveness-NTU (number of transfer units) approach, the analytic mass transfer based method could quantify the relative contributions of the rate limiting steps through a reaction effectiveness parameter. The numeric CFD approach on the other hand could yield the two kinetic parameters that determine the photocatalytic reaction rate simultaneously. Furthermore, it proved to be more accurate as it accounts for the spatial variation of flow rate, reaction rate and concentrations at the surface of the photocatalyst. We elaborate this dual kinetic analysis with regard to the photocatalytic degradation of acetaldehyde in air over a silicon wafer coated with a layer of TiO2 P25 (Evonik) and study the usefulness and limitations of both strategies.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
Times cited: 30
DOI: 10.1016/J.CEJ.2014.09.041
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“Ammonia stripping and scrubbing followed by nitrification and denitrification saves costs for manure treatment based on a calibrated model approach”. Vingerhoets R, Brienza C, Sigurnjak I, Buysse J, Vlaeminck SE, Spiller M, Meers E, Chemical engineering journal 477, 146984 (2023). http://doi.org/10.1016/J.CEJ.2023.146984
Abstract: Resource-efficient nitrogen management is of high environmental and economic interest, and manure represents the major nutrient flow in livestock-intensive regions. Ammonia stripping/scrubbing (SS) is an appealing nitrogen recovery route from manure, yet its real-life implementation has been limited thus far. In nutrient surplus regions like Flanders, treatment of the liquid fraction (LF) of (co–)digested manure typically consists of nitrification/denitrification (NDN) removing most N as nitrogen gas. Integrating SS before NDN in existing plants would expand treatment capacity and recover N while maintaining low N effluent values, yet cost estimations of this novel approach after process optimisation are not yet available. A programming model was developed and calibrated to minimise the treatment costs of this approach and find the balance between N recovery versus N removal. Four crucial operational parameters (CO2 stripping time, NH3 stripping time, temperature and NaOH addition) were optimised for 18 scenarios which were different in terms of technical set-up, influent characteristics and scrubber acid. The model shows that SS before NDN can decrease the costs by 1 to 56% under optimal conditions compared to treatment with NDN only, with 1 to 8% reduction for the LF of manure (22–29% recovered of N treated), and 11 to 56% reduction for the LF of co-digested manure (42–67% recovered of N treated), primarily dependent on resource pricing. This study shows the power of modelling for minimum-cost design and operation of manure treatment yielding savings while producing useful N recovery products with SS followed by NDN.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2023.146984
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“Active site titration of immobilized beta-galactosidase for the determination of active enzymes”. Jochems P, Mueller T, Satyawali Y, Diels L, Dejonghe W, Hanefeld U, Biochemical engineering journal 93, 137 (2015). http://doi.org/10.1016/J.BEJ.2014.10.007
Abstract: In the present study, an active site titration method is demonstrated, to determine the amount of active enzyme (beta-galactosidase), immobilized on a support. Two types of supports were investigated, viz, amino acrylic resin and a mixed matrix membrane. Furthermore, 2',4'-dinitrophenyl 2-deoxy-2-fluoro-beta-D-galactopyranoside was used as an inhibitor for the active site titration of immobilized beta-galactosidase obtained from Kluyveromyces lactis. Using the active site titration, approximately 8.3 mg of active enzyme was found on 1 g of dried commercially available SPRIN imibond, which is an amino acrylic resin with covalently bound beta-galactosidase obtained from K. lactis. However, this method, in its present form, was not effective on the mixed matrix membranes due to the irreversible partial adsorption of the leaving group (2',4'-dinitrophenolate) by the membrane. This observation implied that it is important to investigate interactions between the support and the used inhibitor and leaving group. (C) 2014 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1016/J.BEJ.2014.10.007
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“A packed-bed DBD micro plasma reactor for CO 2 dissociation: Does size matter?”.Uytdenhouwen Y, Van Alphen S, Michielsen I, Meynen V, Cool P, Bogaerts A, Chemical engineering journal 348, 557 (2018). http://doi.org/10.1016/j.cej.2018.04.210
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.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
Times cited: 22
DOI: 10.1016/j.cej.2018.04.210
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“3D porous catalysts for plasma-catalytic dry reforming of methane : how does the pore size affect the plasma-catalytic performance?”.Wang J, Zhang K, Bogaerts A, Meynen V, Chemical engineering journal 464, 142574 (2023). http://doi.org/10.1016/J.CEJ.2023.142574
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.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2023.142574
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