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“Photoresistive gas sensor based on nanocrystalline ZnO sensitized with colloidal perovskite CsPbBr3 nanocrystals”. Chizhov As, Rumyantseva Mn, Drozdov Ka, Krylov Iv, Batuk M, Hadermann J, Filatova Dg, Khmelevsky No, Kozlovsky Vf, Maltseva Ln, Gaskov Am, Sensors And Actuators B-Chemical 329, 129035 (2021). http://doi.org/10.1016/j.snb.2020.129035
Abstract: The development of sensor materials of which gas sensitivity activates under light illumination is of great importance for the design of portable gas analyzers with low power consumption. In the present work a ZnO/CsPbBr3 nanocomposite based on nanocrystalline ZnO and colloidal cubic-shaped perovskite CsPbBr3 nanocrystals (NCs) capped by oleic acide and oleylamine was synthesized. The individual materials and obtained nanocomposite are characterized by x-ray diffraction, low-temperature nitrogen adsorption, x-ray photoelectron spectroscopy, high angle annular dark field scanning transmission electron microscopy with energy-dispersive Xray spectroscopy mapping and UV-vis absorption spectroscopy. The spectral dependence of the photoconductivity of the ZnO/CsPbBr3 nanocomposite reveals a well-defined peak that strongly correlates with the its optical absorption spectrum. The nanocomposite ZnO/CsPbBr3 shows enhanced photoresponse under visible light illumination (lambda(max) = 470 nm, 8 mW/cm(2)) in air, oxygen and argone, compared with pure nanocrystalline ZnO. Under periodic illumination in the temperature range of 25-100 degrees C, the ZnO/CsPbBr3 nanocomposite shows a sensor response to 0.5-3.0 ppm NO2, unlike pure nanocrystalline ZnO matrix, which demonstrates sensor sensitivity to NO2 under the same conditions above 100 degrees C. The effects of humidity on the sensor signal and photoresponse are also discussed.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.401
DOI: 10.1016/j.snb.2020.129035
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“Tuning the turnover frequency and selectivity of photocatalytic CO2 reduction to CO and methane using platinum and palladium nanoparticles on Ti-Beta zeolites”. Blommaerts N, Hoeven N, Arenas Esteban D, Campos R, Mertens M, Borah R, Glisenti A, De Wael K, Bals S, Lenaerts S, Verbruggen SW, Cool P, Chemical Engineering Journal 410, 128234 (2021). http://doi.org/10.1016/j.cej.2020.128234
Abstract: A Ti-Beta zeolite was used in gas phase photocatalytic CO2 reduction to reduce the charge recombination rate and increase the surface area compared to P25 as commercial benchmark, reaching 607 m2 g-1. By adding Pt nanoparticles, the selectivity can be tuned toward CO, reaching a value of 92% and a turnover frequency (TOF) of 96 µmol.gcat-1.h-1, nearly an order of magnitude higher in comparison with P25. By adding Pd nanoparticles the selectivity can be shifted from CO (70% for a bare Ti-Beta zeolite), toward CH4 as the prevalent species (60%). In this way, the selectivity toward CO or CH4 can be tuned by either using Pt or Pd. The TOF values obtained in this work outperform reported state-of-the-art values in similar research. The improved activity by adding the nanoparticles was attributed to an improved charge separation efficiency, together with a plasmonic contribution of the metal nanoparticles under the applied experimental conditions.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL); Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.216
Times cited: 15
DOI: 10.1016/j.cej.2020.128234
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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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“Sub-ppm H2S sensing by tubular ZnO-Co3O4 nanofibers”. Rumyantseva MN, Vladimirova SA, Platonov VB, Chizhov AS, Batuk M, Hadermann J, Khmelevsky NO, Gaskov AM, Sensors And Actuators B-Chemical 307, 127624 (2020). http://doi.org/10.1016/j.snb.2019.127624
Abstract: Tubular ZnO – Co3O4 nanofibers were co-electrospun from polymer solution containing zinc and cobalt acetates. Phase composition, cobalt electronic state and element distribution in the fibers were investigated by XRD, SEM, HRTEM, HAADF-STEM with EDX mapping, and XPS. Bare ZnO has high selective sensitivity to NO and NO2, while ZnO-Co3O4 composites demonstrate selective sensitivity to H2S in dry and humid air. This effect is discussed in terms of transformation of cobalt oxides into cobalt sulfides and change in the acidity of ZnO oxide surface upon cobalt doping. Reduction in response and recovery time is attributed to the formation of a tubular structure facilitating gas transport through the sensitive layer.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.401
DOI: 10.1016/j.snb.2019.127624
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“Conductive imprinted polymers for the direct electrochemical detection of beta-lactam antibiotics: The case of cefquinome”. Moro G, Bottari F, Sleegers N, Florea A, Cowen T, Moretto LM, Piletsky S, De Wael K, Sensors and actuators : B : chemical 297, 126786 (2019). http://doi.org/10.1016/J.SNB.2019.126786
Abstract: A biomimetic sensor for cefquinome (CFQ) was designed at multi-walled carbon nanotubes modified graphite screen-printed electrodes (MWCNTs-G-SPEs) as a proof-of-concept for the creation of a sensors array for beta-lactam antibiotics detection in milk. The sensitive and selective detection of antibiotic residues in food and environment is a fundamental step in the elaboration of prevention strategies to fight the insurgence of antimicrobial resistance (AMR) as recommended by authorities around the world (EU, WHO, FDA). The detection strategy is based on the characteristic electrochemical fingerprint of the target antibiotic cefquinome. A conducive electropolymerized molecularly imprinted polymer (MIP) coupled with MWCNTs was found to be the optimal electrode modifier, able to provide an increased selectivity and sensitivity for CFQ detection. The design of CFQ-MIP was facilitated by the rational selection of the monomer, 4-aminobenzoic acid (4-ABA). The electropolymerization process of 4-ABA have not been fully elucidated yet; for this reason a thorough study and optimization of electropolymerization conditions was performed to obtain a conducive and stable poly(4-ABA) film. The modified electrodes were characterized by electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM) and cyclic voltammetry (CV). CFQ-MIP were synthesized at MWCNT-G-SPEs by electropolyrnerization in pH approximate to 1 (0.1 M sulphuric acid) with a monomer:template ratio of 5:1. Two different analytical protocols were tested (single and double step detection) to minimize unspecific adsorptions and improve the sensitivity. Under optimal conditions, the lowest CFQ concentration detectable by square wave voltammetry (SWV) at the modified sensor was 50 nM in 0.1 M phosphate buffer pH 2.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 5.401
Times cited: 4
DOI: 10.1016/J.SNB.2019.126786
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“On the kinetics and equilibria of plasma-based dry reforming of methane”. Uytdenhouwen Y, Bal Km, Neyts Ec, Meynen V, Cool P, Bogaerts A, Chemical Engineering Journal 405, 126630 (2021). http://doi.org/10.1016/j.cej.2020.126630
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.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
DOI: 10.1016/j.cej.2020.126630
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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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“Pioneering on single-sludge nitrification/denitrification at 50 °C”. Vandekerckhove TGL, Boon N, Vlaeminck SE, Chemosphere 252, 126527 (2020). http://doi.org/10.1016/J.CHEMOSPHERE.2020.126527
Abstract: Thermophilic nitrification has been proven in lab-scale bioreactors at 50 °C. The challenge is now to develop a solution for thermophilic nitrogen removal, integrating nitrification with denitrification and aerobic carbon removal. This pioneering study aimed at a single-sludge nitrification/denitrification process at 50 °C, through exposing nitrification in a step by step approach to anoxia and/or organics. Firstly, recurrent anoxia was tolerated by a nitrifying community during long-term membrane bioreactor (MBR) operation (85 days), with high ammonium oxidation efficiencies (>98%). Secondly, five organic carbon sources did not affect thermophilic ammonium and nitrite oxidation rates in three-day aerobic batch flask incubations. Moving to long-term tests with sequencing batch reactors (SBR) and MBR (>250 days), good nitrification performance was obtained at increasing COD/Ninfluent ratios (0, 0.5, 1, 2 and 3). Thirdly, combining nitrification, recurrent anoxia and presence of organic carbon resulted in a nitrogen removal efficiency of 92–100%, with a COD/Nremoved of 4.8 ± 0.6 and a nitrogen removal rate of 50 ± 14 mg N g−1 VSS d−1. Overall, this is the first proof of principle thermophilic nitrifiers can cope with redox fluctuations (aerobic/anoxic) and the aerobic or anoxic presence of organic carbon, can functionally co-exist with heterotrophs and that single-sludge nitrification/denitrification can be achieved.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 8.8
DOI: 10.1016/J.CHEMOSPHERE.2020.126527
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“Plasma-catalytic dry reforming of methane: Screening of catalytic materials in a coaxial packed-bed DBD reactor”. Andersen Ja, Christensen Jm, Østberg M, Bogaerts A, Jensen Ad, Chemical Engineering Journal 397, 125519 (2020). http://doi.org/10.1016/j.cej.2020.125519
Abstract: The combination of catalysis with non-thermal plasma is a promising alternative to thermal catalysis. A dielectric-barrier discharge reactor was used to study plasma-catalytic dry reforming of methane at ambient pressure and temperature and a fixed plasma power of 45 W. The effect of different catalytic packing materials was evaluated in terms of conversion, product selectivity, and energy efficiency. The conversion of CO2 (~22%) and CH4 (~33%) were found to be similar in plasma-only and when introducing packing materials in plasma. The main reason is the shorter residence time of the gas due to packing geometry, when compared at identical flow rates. H2, CO, C2-C4 hydrocarbons, and oxygenates were identified in the product gas. High selectivity towards H2 and CO were found for all catalysts and plasma-only, with a H2/CO molar ratio of ~0.9. The lowest syngas selectivity was obtained with Cu/Al2O3 (~66%), which instead, had the highest alcohol selectivity (~3.6%).
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
DOI: 10.1016/j.cej.2020.125519
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“Plasma-enabled catalyst-free conversion of ethanol to hydrogen gas and carbon dots near room temperature”. Zhou R, Zhou R, Xian Y, Fang Z, Lu X, Bazaka K, Bogaerts A, Ostrikov K(K), Chemical Engineering Journal 382, 122745 (2020). http://doi.org/10.1016/J.CEJ.2019.122745
Abstract: Selective conversion of bio-renewable ethanol under mild conditions especially at room temperature remains a major challenge for sustainable production of hydrogen and valuable carbon-based materials. In this study, adaptive non-thermal plasma is applied to deliver pulsed energy to rapidly and selectively reform ethanol in the absence of a catalyst. Importantly, the carbon atoms in ethanol that would otherwise be released into the environment in the form of CO or CO2 are effectively captured in the form of carbon dots (CDs). Three modes of non-thermal spark plasma discharges, i.e. single spark mode (SSM), multiple spark mode (MSM) and gliding spark mode (GSM), provide additional flexibility in ethanol reforming by controlling the processes of energy transfer and distribution, thereby affecting the flow rate, gas content, and energy consumption in H-2 production. A favourable combination of low temperature (< 40 degrees C), attractive conversion rate (gas flow rate of similar to 120 mL/min), high hydrogen yield (H-2 content > 90%), low energy consumption (similar to 0.96 kWh/m(3) H-2) and the effective generation of photoluminescent CDs (which are applicable for bioimaging or biolabelling) in the MSM indicate that the proposed strategy may offer a new carbon-negative avenue for comprehensive utilization of alcohols and mitigating the increasingly severe energy and environmental issues.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 15.1
Times cited: 20
DOI: 10.1016/J.CEJ.2019.122745
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“Thermodynamically unconstrained forced concentration cycling of methane catalytic partial oxidation over CeO2FeCralloy catalysts”. Ma Z, Perreault P, Pelegrin DC, Boffito DC, Patience GS, Chemical Engineering Journal 380, 122470 (2020). http://doi.org/10.1016/J.CEJ.2019.122470
Abstract: Converting waste associated natural gas from oil fields is uneconomic with current gas-to-liquid technology. Micro Gas-to-Liquids technology ( GtL) combines process intensification and numbering up economics to reduce capital costs to convert flared and vented natural gas to value-added synthetic fuel: Milli-second contact times in the catalytic partial oxidation of methane (CPOX) integrated with a tandem Fischer-Tropsch (FT) step meets the economic constraints together with remote process control. FeCralloy knitted fibres with high thermal conductivity and low pressure drop, resist thermal and mechanical stresses in the high pressure CPOX step. The FeCralloy catalysts are free of pre-reduction treatments. We deposited Pt and/or CeO2 over the fibre surface via solution combustion synthesis. Methane conversion was higher at ambient pressure compared to 2 MPa while the Pt/CeO2 FeCralloy was relatively inert from 0.1 MPa to 2 MPa. However, both catalysts demonstrated high activity in quasi-chemical looping partial oxidation of methane: during the reduction step while feeding methane, an on-line mass spectrometer only detected H2 while in the oxidation step it detected predominantly CO. Kinetic modeling of the oxidation-reduction cycles suggests that the reaction follows a direct mechanism to produce CO and H2 rather than an indirect mechanism that first produces CO2 and H2O followed by reforming.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2019.122470
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“Effect of cobalt content on the properties of quintuple perovskites Sm₂Ba₃Fe₅-xCoxO₁₅-δ”. Golovachev IB, Mychinko MY, Volkova NE, Gavrilova LY, Raveau B, Maignan A, Cherepanov VA, Journal Of Solid State Chemistry 301, 122324 (2021). http://doi.org/10.1016/J.JSSC.2021.122324
Abstract: Quintuple perovskites Sm2Ba3Fe5-xCoxO15-delta = 0.5, 1.0 and 1.5) have been prepared by glycerin-nitrate tech- nique in air. The phase purity was confirmed by XRD. Partial substitution of Co for Fe decreases the oxygen content and thus the mean oxidation state of 3d-metals. It also slightly decreases the thermal expansion coefficient of oxides. Positive value of the Seebeck coefficient confirmed p-type conductivity, though the thermopower decreases as the Co content increases. The temperature dependence of electrical conductivity reveals a maximum at 550-750 degrees C.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.299
DOI: 10.1016/J.JSSC.2021.122324
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“Proof of concept of an upscaled photocatalytic multi-tube reactor : a combined modelling and experimental study”. van Walsem J, Roegiers J, Modde B, Lenaerts S, Denys S, Chemical engineering journal 378, 122038 (2019). http://doi.org/10.1016/J.CEJ.2019.122038
Abstract: Three upscaled multi-tube photocatalytic reactors designed for integration into HVAC (Heating, Ventilation and Air Conditioning) systems were proposed and evaluated using a CFD modelling approach, with emphasis on the flow, irradiation and concentration distribution in the reactor and hence, photocatalytic performance. Based on the obtained insights, the best reactor design was selected, further characterized and improved by an additional proof of concept study and eventually converted into practice. Subsequently, the scaled-up prototype was experimentally tested according to the CEN-EN-16846-1 standard (2017) for volatile organic compound (VOC) removal by an external scientific research center. The combined modelling and experimental approach used in this work, leads to essential insights into the design and assessment of photocatalytic reactors. Therefore, this study provides an essential step towards the optimization and commercialization of photocatalytic reactors for HVAC applications.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
DOI: 10.1016/J.CEJ.2019.122038
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“Structural and magnetic properties of the perovskites A₂LaFe₂SbO₉, (A = Ca, Sr, Ba)”. Hendrickx M, Tang Y, Hunter EC, Battle PD, Hadermann J, Journal Of Solid State Chemistry 295, 121914 (2021). http://doi.org/10.1016/J.JSSC.2020.121914
Abstract: Polycrystalline samples of A(2)LaFe(2)SbO(9) (A = Ca, Sr, Ba) perovskites appeared monophasic to X-ray or neutron powder diffraction but a single-crystal study utilising transmission electron microscopy revealed a greater level of complexity. Although local charge balance is maintained, compositional and structural variations are present among and within the submicron-sized crystals. Despite the inhomogeneity, A = Ca is monophasic with a partially-ordered distribution of Fe3+ and Sb5+ cations across two crystallographically-distinct octahedral sites, i.e. Ca2La(Fe1.25Sb0.25)(2d) (Fe0.75Sb0.75)(2c)O-9. For A = Sr or Ba, the inhomogeneities result in differences in the filling patterns of the octahedra and the ordering of the B cations. Particles of A = Sr contain a phase (Fe:Sb similar to 2:1) without B cation ordering and one (Fe:Sb similar to 1:1) with B cation ordering. Monophasic A = Ba lacks long-range cation order although ordered nanodomains are present within the disordered phase. The temperature dependence of the magnetic properties of each sample is discussed.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.299
DOI: 10.1016/J.JSSC.2020.121914
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“Preparation of the noncentrosymmetric ferrimagnetic phase La0.9Ba0.1Mn0.96O2.43 by topochemical reduction”. Parsons TG, Hadermann J, Halasyamani PS, Hayward MA, Journal Of Solid State Chemistry 287, 121356 (2020). http://doi.org/10.1016/J.JSSC.2020.121356
Abstract: Topochemical reduction of La0.9Ba0.1MnO3 with NaH at 225 degrees C yields the brownmillerite phase La0.9Ba0.1MnO2.5. However, reduction with CaH2 at 435 degrees C results in the formation of La0.9Ba0.1Mn0.96O2.43 via the deintercalation of both oxide anions and manganese cations from the parent perovskite phase. Electron and neutron diffraction data reveal La0.9Ba0.1Mn0.96O2.43 adopts a complex noncentrosymmetric structure, described in space group I23, confirmed by SHG measurements. Low-temperature neutron diffraction data reveal La0.9Ba0.1Mn0.96O2.43 adopts an ordered magnetic structure in which all the nearest neighbor interactions are antiferromagnetic. However, the presence of ordered manganese cation-vacancies results in a net ferrimagnetic structure with net saturated moment of 0.157(2) mu B per manganese center.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.3
DOI: 10.1016/J.JSSC.2020.121356
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“CaLa2FeCoSbO9 and ALa2FeNiSbO9 (A = Ca, Sr, Ba): cation-ordered, inhomogeneous, ferrimagnetic perovskites”. Hendrickx M, Tang Y, Hunter EC, Battle PD, Cadogan Jm, Hadermann J, Journal Of Solid State Chemistry 285, 121226 (2020). http://doi.org/10.1016/j.jssc.2020.121226
Abstract: Polycrystalline samples of CaLa2FeCoSbO9 and ALa2FeNiSbO9 (A=Ca, Sr, Ba) have been prepared in solid-state reactions and studied by a combination of transmission electron microscopy, magnetometry, X-ray diffraction, neutron diffraction and Mössbauer spectroscopy. Diffraction and TEM showed that each shows 1:1 B-site ordering in which Co2+/Ni2+ and Sb5+ tend to occupy two distinct crystallographic sites while Fe3+ is distributed over both sites. While X-ray and neutron diffraction agreed that all four compositions are monophasic with space group P21/n, TEM revealed different levels of compositional inhomogeneity at the subcrystal scale, which, in the case of BaLa2FeNiSbO9, leads to the occurrence of both a P21/n and an I2/m phase. Magnetometry and neutron diffraction show that these perovskites are ferrimagnets with a G-type magnetic structure. Their relatively low magnetisation can be attributed to their inhomogeneity. This work demonstrates the importance of studying the microstructure of complex compositions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.3
DOI: 10.1016/j.jssc.2020.121226
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“NH3 decomposition for H2 production by thermal and plasma catalysis using bimetallic catalysts”. Meng S, Li S, Sun S, Bogaerts A, Liu Y, Yi Y, Chemical engineering science 283, 119449 (2024). http://doi.org/10.1016/j.ces.2023.119449
Abstract: Plasma catalysis has emerged as a promising approach for driving thermodynamically unfavorable chemical
reactions. Nevertheless, comprehending the mechanisms involved remains a challenge, leading to uncertainty
about whether the optimal catalyst in plasma catalysis aligns with that in thermal catalysis. In this research, we
explore this question by studying monometallic catalysts (Fe, Co, Ni and Mo) and bimetallic catalysts (Fe-Co, Mo-
Co, Fe-Ni and Mo-Ni) in both thermal catalytic and plasma catalytic NH3 decomposition. Our findings reveal that
the Fe-Co bimetallic catalyst exhibits the highest activity in thermal catalysis, the Fe-Ni bimetallic catalyst
outperforms others in plasma catalysis, indicating a discrepancy between the optimal catalysts for the two
catalytic modes in NH3 decomposition. Comprehensive catalyst characterization, kinetic analysis, temperature
program surface reaction experiments and plasma diagnosis are employed to discuss the key factors influencing
NH3 decomposition performance.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.7
DOI: 10.1016/j.ces.2023.119449
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“Analytical techniques for the detection of amphetamine-type substances in different matrices : a comprehensive review”. Drăgan A-M, Parrilla M, Feier B, Oprean R, Cristea C, De Wael K, Trac-Trends In Analytical Chemistry 145, 116447 (2021). http://doi.org/10.1016/J.TRAC.2021.116447
Abstract: This current review focuses on contributions to amphetamine-type substances (ATS) analysis. This type of synthetic illicit drugs has been increasingly present worldwide reaching 5% of the market on illicit drugs in 2019. The increment of their production in many clandestine laboratories and easy distribution among society are two of the main concerns towards the battle against synthetic drugs. Therefore, the first part of this review details the classification and mechanism of action of ATS in the human body. Second, the pharmacological and toxicological effects of ATS on human health are described to motivate the need of early detection of ATS. Subsequently, the most used laboratory-based and portable methods are presented and critically discussed along the review. Finally, a careful discussion on the advantages and disadvantages of portable techniques employed on the field are addressed as potential tools for on-site ATS detection by law enforcement officers.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 8.442
DOI: 10.1016/J.TRAC.2021.116447
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“Mapping the gaps in chemical analysis for the characterisation of aptamer-target interactions”. Daems E, Moro G, Campos R, De Wael K, Trac-Trends In Analytical Chemistry 142, 116311 (2021). http://doi.org/10.1016/J.TRAC.2021.116311
Abstract: Aptamers are promising biorecognition elements with a wide applicability from therapeutics to bio-sensing. However, to successfully use these biomolecules, a complete characterisation of their bindingperformance in the presence of the target is crucial. Several multi-analytical approaches have been re-ported including techniques to describe kinetic and thermodynamic aspects of the aptamer-targetinteraction, and techniques which allow an in-depth understanding of the aptamer-target structures.Recent literature shows the need of a critical data interpretation, a combination of characterisationtechniques and suggests the key role of the characterisation protocol design. Indeed, thefinal applicationof the aptamer should be considered before choosing the characterisation method. All the limitations andcapabilities of the analytical tools in use for aptamer characterisation should be taken into account. Here,we present a critical overview of the current methods and multi-analytical approaches to study aptamer-target binding, aiming to provide researchers with guidelines for the design of characterisation protocols.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 8.442
DOI: 10.1016/J.TRAC.2021.116311
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“Electrochemical identification of hazardous phenols and their complex mixtures in real samples using unmodified screen-printed electrodes”. Barich H, Cánovas R, De Wael K, Journal of electroanalytical chemistry : an international journal devoted to all aspects of electrode kynetics, interfacial structure, properties of electrolytes, colloid and biological electrochemistry. 904, 115878 (2022). http://doi.org/10.1016/J.JELECHEM.2021.115878
Abstract: The electrochemical behavior of some of the most relevant endocrine-disrupting phenols using unmodified carbon screen-printed electrodes (SPEs) is described for the first time. Experiments were made to assess the electrochemical behavior of phenol (PHOH), pentachlorophenol (PCP), 4-tert octylphenol (OP) and bisphenol A (BPA) and their determination in the most favorable conditions, using voltammetric methods such as cyclic voltammetry (CV), linear sweep voltammetry (LSV) and square wave voltammetry (SWV) in Britton Robinson (BR) buffer. Further, the usefulness of the electrochemical approach was validated with real samples from a local river and was compared to commercial phenols test kit, which is commonly used for on-site screening in industrial streams and wastewaters. Finally, the approach was compared with a lab-bench standard method using real samples, i.e., high-performance liquid chromatography with a photodiode array detector (HPLC-DAD).
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 4.5
DOI: 10.1016/J.JELECHEM.2021.115878
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“Voltammetric sensing using an array of modified SPCE coupled with machine learning strategies for the improved identification of opioids in presence of cutting agents”. Ortiz-Aguayo D, De Wael K, del Valle M, Journal Of Electroanalytical Chemistry 902, 115770 (2021). http://doi.org/10.1016/J.JELECHEM.2021.115770
Abstract: This work reports the use of modified screen-printed carbon electrodes (SPCEs) for the identification of three drugs of abuse and two habitual cutting agents, caffeine and paracetamol, combining voltammetric sensing and chemometrics. In order to achieve this goal, codeine, heroin and morphine were subjected to Square Wave Voltammetry (SWV) at pH 7, in order to elucidate their electrochemical fingerprints. The optimized SPCEs electrode array, which have a differentiated response for the three oxidizable compounds, was derived from Carbon, Prussian blue, Cobalt (II) phthalocyanine, Copper (II) oxide, Polypyrrole and Palladium nanoparticles ink-modified carbon electrodes. Finally, Principal Component Analysis (PCA) coupled with Silhouette parameter assessment was used to select the most suitable combination of sensors for identification of drugs of abuse in presence of cutting agents.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 3.012
DOI: 10.1016/J.JELECHEM.2021.115770
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“Abnormal in-plane permittivity and ferroelectricity of confined water : from sub-nanometer channels to bulk”. Hamid I, Jalali H, Peeters FM, Neek-Amal M, Journal Of Chemical Physics 154, 114503 (2021). http://doi.org/10.1063/5.0038359
Abstract: Dielectric properties of nano-confined water are important in several areas of science, i.e., it is relevant in the dielectric double layer that exists in practically all heterogeneous fluid-based systems. Molecular dynamics simulations are used to predict the in-plane dielectric properties of confined water in planar channels of width ranging from sub-nanometer to bulk. Because of suppressed rotational degrees of freedom near the confining walls, the dipole of the water molecules tends to be aligned parallel to the walls, which results in a strongly enhanced in-plane dielectric constant (epsilon (parallel to)) reaching values of about 120 for channels with height 8 angstrom < h < 10 angstrom. With the increase in the width of the channel, we predict that epsilon (parallel to) decreases nonlinearly and reaches the bulk value for h > 70 angstrom. A stratified continuum model is proposed that reproduces the h > 10 angstrom dependence of epsilon (parallel to). For sub-nanometer height channels, abnormal behavior of epsilon (parallel to) is found with two orders of magnitude reduction of epsilon (parallel to) around h similar to 7.5 angstrom, which is attributed to the formation of a particular ice phase that exhibits long-time (similar to mu s) stable ferroelectricity. This is of particular importance for the understanding of the influence of confined water on the functioning of biological systems.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 2.965
Times cited: 13
DOI: 10.1063/5.0038359
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“Free energy barriers from biased molecular dynamics simulations”. Bal KM, Fukuhara S, Shibuta Y, Neyts EC, Journal Of Chemical Physics 153, 114118 (2020). http://doi.org/10.1063/5.0020240
Abstract: Atomistic simulation methods for the quantification of free energies are in wide use. These methods operate by sampling the probability density of a system along a small set of suitable collective variables (CVs), which is, in turn, expressed in the form of a free energy surface (FES). This definition of the FES can capture the relative stability of metastable states but not that of the transition state because the barrier height is not invariant to the choice of CVs. Free energy barriers therefore cannot be consistently computed from the FES. Here, we present a simple approach to calculate the gauge correction necessary to eliminate this inconsistency. Using our procedure, the standard FES as well as its gauge-corrected counterpart can be obtained by reweighing the same simulated trajectory at little additional cost. We apply the method to a number of systems—a particle solvated in a Lennard-Jones fluid, a Diels–Alder reaction, and crystallization of liquid sodium—to demonstrate its ability to produce consistent free energy barriers that correctly capture the kinetics of chemical or physical transformations, and discuss the additional demands it puts on the chosen CVs. Because the FES can be converged at relatively short (sub-ns) time scales, a free energy-based description of reaction kinetics is a particularly attractive option to study chemical processes at more expensive quantum mechanical levels of theory.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.4
DOI: 10.1063/5.0020240
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“Adsorption of molecules on C3N nanosheet : a first-principles calculations”. Bafekry A, Ghergherehchi M, Shayesteh SF, Peeters FM, Chemical physics 526, 110442 (2019). http://doi.org/10.1016/J.CHEMPHYS.2019.110442
Abstract: Using first-principles calculations we investigate the interaction of various molecules, including H-2, N-2, CO, CO2, H2O, H2S, NH3, CH4 with a C3N nanosheet. Due to the weaker interaction between H-2, N-2, CO, CO2, H2O, H2S, NH3, and CH4 molecules with C3N, the adsorption energy is small and does not yield any significant distortion of the C3N lattice and the molecules are physisorbed. Calculated charge transfer shows that these molecules act as weak donors. However, adsorption of O-2, NO, NO2 and SO2 molecules are chemisorbed, they receive electrons from C3N and act as a strong acceptor. They interact strongly through hybridizing its frontier orbitals with the p-orbital of C3N, modifying the electronic structure of C3N. Our theoretical studies indicate that C3N-based sensor has a high potential for O-2, NO, NO2 and SO2 molecules detection.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 1.767
Times cited: 52
DOI: 10.1016/J.CHEMPHYS.2019.110442
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“Distribution of lipid aldehydes in phase-separated membranes: A molecular dynamics study”. Oliveira MC, Yusupov M, Bogaerts A, Cordeiro RM, Archives Of Biochemistry And Biophysics 717, 109136 (2022). http://doi.org/10.1016/j.abb.2022.109136
Abstract: It is well established that lipid aldehydes (LAs) are able to increase the permeability of cell membranes and induce their rupture. However, it is not yet clear how LAs are distributed in phase-separated membranes (PSMs), which are responsible for the transport of selected molecules and intracellular signaling. Thus, we investigate here the distribution of LAs in a PSM by coarse-grained molecular dynamics simulations. Our results reveal that LAs derived from mono-unsaturated lipids tend to accumulate at the interface between the liquid-ordered/liquiddisordered domains, whereas those derived from poly-unsaturated lipids remain in the liquid-disordered domain. These results are important for understanding the effects caused by oxidized lipids in membrane structure, properties and organization.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.9
DOI: 10.1016/j.abb.2022.109136
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“Intensifying mass and heat transfer using a high-g stator-rotor vortex chamber”. Gonzalez-Quiroga A, Shtern V, Perreault P, Vandewalle L, Marin GB, Van Geem KM, Chemical Engineering And Processing 169, 108638 (2021). http://doi.org/10.1016/J.CEP.2021.108638
Abstract: Vortex reactors take advantage of the synergy between enhanced heat and mass transfer rates and multifunctional phenomena at different temporal and spatial scales. Proof-of-concept experiments with our novel and innovative STAtor-Rotor VOrtex Chamber (STARVOC) confirm its advantageous features for the sustainable production of chemicals and fuels. STARVOC is a high-g contactor that uses carrier flow (gas or liquid) tangential injection to drive a rotor attached to low-friction bearings. The vortex chamber inside the rotor contains a secondary phase or phases, such as a solids bed, a liquid layer, or a suspension. Carrier fluid passes through the perforated rotor wall and contacts a densely and uniformly distributed secondary phase with enhanced slip velocities. Experiments focused on pressure profiles, rotor angular velocity, and solids azimuthal velocity. With air as the carrier fluid and different solid particle beds as the secondary phase, STARVOC reached bed azimuthal velocities up to four-fold compared to those reached in Gas-Solid Vortex Units with fully static geometry. These results show its potential to improve interfacial heat and mass transfer rates and take advantage of flow energy and angular momentum. Due to its process intensification capabilities, STARVOC is a promising alternative for the state-of-the-art chemical industry.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 2.234
DOI: 10.1016/J.CEP.2021.108638
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“How do nitrated lipids affect the properties of phospholipid membranes?”.Oliveira MC, Yusupov M, Bogaerts A, Cordeiro RM, Archives Of Biochemistry And Biophysics 695, 108548 (2020). http://doi.org/10.1016/j.abb.2020.108548
Abstract: Biological membranes are under constant attack of free radicals, which may lead to lipid nitro-oxidation, pro ducing a complex mixture of nitro-oxidized lipids that are responsible for structural and dynamic changes on the membrane. Despite the latter, nitro-oxidized lipids are also associated with several inflammatory and neuro degenerative diseases, the underlying mechanisms of which remain elusive. We perform atomistic molecular dynamics simulations using several isomers of nitro-oxidized lipids to study their effect on the structure and permeability of the membrane, as well as the interaction between the mixture of these products in the phospholipid membrane environment. Our results show that the stereo- and positional isomers have a stronger effect on the properties of the membrane composed of oxidized lipids compared to that containing nitrated lipids. Nevertheless, nitrated lipids lead to three-fold increase in water permeability compared to oxidized lipids. In addition, we show that in a membrane consisting of combined nitro-oxidized lipid products, the presence of oxidized lipids protects the membrane from transient pores. Is well stablished that plasma application and photodynamic therapy produces a number of oxidative species used to kill cancer cells, through membrane damage induced by nitro-oxidative stress. This study is important to elucidate the mechanisms and the molecular level properties involving the reactive species produced during that cancer therapies.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.9
DOI: 10.1016/j.abb.2020.108548
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“Preferential photoassimilation of volatile fatty acids by purple non-sulfur bacteria : experimental kinetics and dynamic modelling”. Segura PC, De Meur Q, Alloul A, Tanghe A, Onderwater R, Vlaeminck SE, Vande Wouwer A, Wattiez R, Dewasme L, Leroy B, Biochemical engineering journal 186, 108547 (2022). http://doi.org/10.1016/J.BEJ.2022.108547
Abstract: Purple non-sulfur bacteria (PNSB) are known for their metabolic versatility and thrive as anoxygenic photoheterotrophs. In environmental engineering and resource recovery, cells would grow on mixtures of volatile fatty acids (VFA) generated by anaerobic fermentation of waste streams. In this study, we aim to better understand the behavior of Rhodospirillum rubrum, a model PNSB species, grown using multiple VFA as carbon sources. We highlighted that assimilation of individual VFA follows a sequential pattern. Based on observations in other PNSB, this seems to be specific to isocitrate lyase-lacking organisms. We hypothesized that the inhibition phenomenon could be due to the regulation of the metabolic fluxes in the substrate cycle between acetoacetyl-CoA and crotonyl-CoA. Developed macroscopic dynamic models showed a good predictive capability for substrate competition for every VFA mixture containing acetate, propionate, and/or butyrate. These novel insights provide valuable input for better design and operation of PNSB-based waste treatment solutions.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 3.9
DOI: 10.1016/J.BEJ.2022.108547
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“Effect of oxidative stress on cystine transportation by xC&oline, antiporter”. Ghasemitarei M, Yusupov M, Razzokov J, Shokri B, Bogaerts A, Archives of biochemistry and biophysics 674, 108114 (2019). http://doi.org/10.1016/j.abb.2019.108114
Abstract: We performed computer simulations to investigate the effect of oxidation on the extracellular cystine (CYC) uptake by the xC− antiporter. The latter is important for killing of cancer cells. Specifically, applying molecular dynamics (MD) simulations we studied the transport of CYC across xCT, i.e., the light subunit of the xC− antiporter, in charge of bidirectional transport of CYC and glutamate. We considered the outward facing (OF) configuration of xCT, and to study the effect of oxidation, we modified the Cys327 residue, located in the vicinity of the extracellular milieu, to cysteic acid (CYO327). Our computational results showed that oxidation of Cys327 results in a free energy barrier for CYC translocation, thereby blocking the access of CYC to the substrate binding site of the OF system. The formation of the energy barrier was found to be due to the conformational changes in the channel. Analysis of the MD trajectories revealed that the reorganization of the side chains of the Tyr244 and CYO327 residues play a critical role in the OF channel blocking. Indeed, the calculated distance between Tyr244 and either Cys327 or CYO327 showed a narrowing of the channel after oxidation. The obtained free energy barrier for CYC translocation was found to be 33.9kJmol−1, indicating that oxidation of Cys327, by e.g., cold atmospheric plasma, is more effective in inhibiting the xC− antiporter than in the mutation of this amino acid to Ala (yielding a barrier of 32.4kJmol−1). The inhibition of the xC− antiporter may lead to Cys starvation in some cancer cells, eventually resulting in cancer cell death.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.165
DOI: 10.1016/j.abb.2019.108114
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“Covalent immobilization of delipidated human serum albumin on poly(pyrrole-2-carboxylic) acid film for the impedimetric detection of perfluorooctanoic acid”. Moro G, Bottari F, Liberi S, Covaceuszach S, Cassetta A, Angelini A, De Wael K, Moretto LM, Bioelectrochemistry 134, 107540 (2020). http://doi.org/10.1016/J.BIOELECHEM.2020.107540
Abstract: The immobilization of biomolecules at screen printed electrodes for biosensing applications is still an open challenge. To enrich the toolbox of bioelectrochemists, graphite screen printed electrodes (G-SPE) were modified with an electropolymerized film of pyrrole-2-carboxilic acid (Py-2-COOH), a pyrrole derivative rich in carboxylic acid functional groups. These functionalities are suitable for the covalent immobilization of biomolecular recognition layers. The electropolymerization was first optimized to obtain stable and conductive polymeric films, comparing two different electrolytes: sodium dodecyl sulphate (SDS) and sodium perchlorate. The G-SPE modified with Py-2-COOH in 0.1 M SDS solution showed the required properties and were further tested. A proof-of-concept study for the development of an impedimetric sensor for perfluorooctanoic acid (PFOA) was carried out using the delipidated human serum albumin (hSA) as bioreceptor. The data interpretation was supported by size exclusion chromatography and small-angle X-ray scattering (SEC-SAXS) analysis of the bioreceptor-target complex and the preliminary results suggest the possibility to further develop this biosensing strategy for toxicological and analytical studies.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 5
DOI: 10.1016/J.BIOELECHEM.2020.107540
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