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“Selective bifunctional catalytic conversion of cellulose over reshaped ni particles at the tip of carbon nanofibers”. Van de Vyver S, Geboers J, Dusselier M, Schepers H, Vosch T, Zhang L, Van Tendeloo G, Jacobs PA, Sels BF, Chemsuschem 3, 698 (2010). http://doi.org/10.1002/cssc.201000087
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 136
DOI: 10.1002/cssc.201000087
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“Carbon dioxide splitting in a dielectric barrier discharge plasma : a combined experimental and computational study”. Aerts R, Somers W, Bogaerts A, Chemsuschem 8, 702 (2015). http://doi.org/10.1002/cssc.201402818
Abstract: Plasma technology is gaining increasing interest for the splitting of CO2 into CO and O2. We have performed experiments to study this process in a dielectric barrier discharge (DBD) plasma with a wide range of parameters. The frequency and dielectric material did not affect the CO2 conversion and energy efficiency, but the discharge gap can have a considerable effect. The specific energy input has the most important effect on the CO2 conversion and energy efficiency. We have also presented a plasma chemistry model for CO2 splitting, which shows reasonable agreement with the experimental conversion and energy efficiency. This model is used to elucidate the critical reactions that are mostly responsible for the CO2 conversion. Finally, we have compared our results with other CO2 splitting techniques and we identified the limitations as well as the benefits and future possibilities in terms of modifications of DBD plasmas for greenhouse gas conversion in general.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 131
DOI: 10.1002/cssc.201402818
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“Design of Ru-zeolites for hydrogen-free production of conjugated linoleic acid”. Philippaerts A, Goossens S, Vermandel W, Tromp M, Turner S, Geboers J, Van Tendeloo G, Jacobs PA, Sels BF, Chemsuschem 4, 757 (2011). http://doi.org/10.1002/cssc.201100015
Abstract: While conjugated vegetable oils are currently used as additives in the drying agents of oils and paints, they are also attractive molecules for making bio-plastics. Moreover, conjugated oils will soon be accepted as nutritional additives for functional food products. While current manufacture of conjugated vegetable oils or conjugated linoleic acids (CLAs) uses a homogeneous base as isomerisation catalyst, a heterogeneous alternative is not available today. This contribution presents the direct production of CLAs over Ru supported on different zeolites, varying in topology (ZSM-5, BETA, Y), Si/Al ratio and countercation (H+, Na+, Cs+). Ru/Cs-USY, with a Si/Al ratio of 40, was identified as the most active and selective catalyst for isomerisation of methyl linoleate (cis-9,cis-12 (C18:2)) to CLA at 165 °C. Interestingly, no hydrogen pre-treatment of the catalyst or addition of hydrogen donors is required to achieve industrially relevant isomerisation productivities, namely, 0.7 g of CLA per litre of solvent per minute. Moreover, the biologically most active CLA isomers, namely, cis-9,trans-11, trans-10,cis-12 and trans-9,trans-11, were the main products, especially at low catalyst concentrations. Ex situ physicochemical characterisation with CO chemisorption, extended X-ray absorption fine structure measurements, transmission electron microscopy analysis, and temperature-programmed oxidation reveals the presence of highly dispersed RuO2 species in Ru/Cs-USY(40).
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 24
DOI: 10.1002/cssc.201100015
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“Multimodal zeolite-beta-based catalysts with a hierarchical, three-level pore structure”. Chen L-H, Li X-Y, Tian G, Li Y, Tan H-Y, Van Tendeloo G, Zhu G-S, Qiu S-L, Yang X-Y, Su B-L, Chemsuschem 4, 1452 (2011). http://doi.org/10.1002/cssc.201100181
Abstract: Hole diggers: The hierarchically structured porous solid-acid catalyst described in this report possess a remarkable pore system, encompassing well-defined macrochannels, interconnected mesopores, intracrystalline mesopores, and tunable zeolite micropores. Importantly, the catalyst exhibits very strong acidity and superior catalytic activity for esterification reactions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 33
DOI: 10.1002/cssc.201100181
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“Selective nickel-catalyzed conversion of model and lignin-derived phenolic compounds to cyclohexanone-based polymer building blocks”. Schutyser W, Van den Bosch S, Dijkmans J, Turner S, Meledina M, Van Tendeloo G, Debecker DP, Sels BF, Chemsuschem 8, 1805 (2015). http://doi.org/10.1002/cssc.201403375
Abstract: Valorization of lignin is essential for the economics of future lignocellulosic biorefineries. Lignin is converted into novel polymer building blocks through four steps: catalytic hydroprocessing of softwood to form 4-alkylguaiacols, their conversion into 4-alkylcyclohexanols, followed by dehydrogenation to form cyclohexanones, and Baeyer-Villiger oxidation to give caprolactones. The formation of alkylated cyclohexanols is one of the most difficult steps in the series. A liquid-phase process in the presence of nickel on CeO2 or ZrO2 catalysts is demonstrated herein to give the highest cyclohexanol yields. The catalytic reaction with 4-alkylguaiacols follows two parallel pathways with comparable rates: 1) ring hydrogenation with the formation of the corresponding alkylated 2-methoxycyclohexanol, and 2) demethoxylation to form 4-alkylphenol. Although subsequent phenol to cyclohexanol conversion is fast, the rate is limited for the removal of the methoxy group from 2-methoxycyclohexanol. Overall, this last reaction is the rate-limiting step and requires a sufficient temperature (> 250 degrees C) to overcome the energy barrier. Substrate reactivity (with respect to the type of alkyl chain) and details of the catalyst properties (nickel loading and nickel particle size) on the reaction rates are reported in detail for the Ni/CeO2 catalyst. The best Ni/CeO2 catalyst reaches 4-alkylcyclohexanol yields over 80 %, is even able to convert real softwood-derived guaiacol mixtures and can be reused in subsequent experiments. A proof of principle of the projected cascade conversion of lignocellulose feedstock entirely into caprolactone is demonstrated by using Cu/ZrO2 for the dehydrogenation step to produce the resultant cyclohexanones (approximate to 80%) and tin-containing beta zeolite to form 4-alkyl-e-caprolactones in high yields, according to a Baeyer-Villiger-type oxidation with H2O2.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 71
DOI: 10.1002/cssc.201403375
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“The Quest for Value-Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study”. Snoeckx R, Ozkan A, Reniers F, Bogaerts A, Chemsuschem 10, 409 (2017). http://doi.org/10.1002/cssc.201601234
Abstract: Recycling of carbon dioxide by its conversion into value-added products has gained significant interest owing to the role it can play for use in an anthropogenic carbon cycle. The combined conversion with H2O could even mimic the natural photosynthesis process. An interesting gas conversion technique currently being considered in the field of CO2 conversion is plasma technology. To investigate whether it is also promising for this combined conversion, we performed a series of experiments and developed a chemical kinetics plasma chemistry model for a deeper understanding of the process. The main products formed were the syngas components CO and H2, as well as O2 and H2O2, whereas methanol formation was only observed in the parts-per-billion to parts-per-million range. The syngas ratio, on the other hand, could easily be controlled by varying both the water content and/or energy input. On the basis of the model, which was validated with experimental results, a chemical kinetics analysis was performed, which allowed the construction and investigation of the different pathways leading to the observed experimental results and which helped to clarify these results. This approach allowed us to evaluate this technology on the basis of its underlying chemistry and to propose solutions on how to further improve the formation of value-added products by using plasma technology.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 25
DOI: 10.1002/cssc.201601234
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“The Chemical Route to a Carbon Dioxide Neutral World”. Martens JA, Bogaerts A, De Kimpe N, Jacobs PA, Marin GB, Rabaey K, Saeys M, Verhelst S, Chemsuschem 10, 1039 (2017). http://doi.org/10.1002/cssc.201601051
Abstract: Excessive CO2 emissions in the atmosphere from anthropogenic activity can be divided into point sources and diffuse sources. The capture of CO2 from flue gases of large industrial installations and its conversion into fuels and chemicals with fast catalytic processes seems technically possible. Some emerging technologies are already being demonstrated on an industrial scale. Others are still being tested on a laboratory or pilot scale. These emerging chemical technologies can be implemented in a time window ranging from 5 to 20 years. The massive amounts of energy needed for capturing processes and the conversion of CO2 should come from low-carbon energy sources, such as tidal, geothermal, and nuclear energy, but also, mainly, from the sun. Synthetic methane gas that can be formed from CO2 and hydrogen gas is an attractive renewable energy carrier with an existing distribution system. Methanol offers advantages as a liquid fuel and is also a building block for the chemical industry. CO2 emissions from diffuse sources is a difficult problem to solve, particularly for CO2 emissions from road, water, and air transport, but steady progress in the development of technology for capturing CO2 from air is being made. It is impossible to ban carbon from the entire energy
supply of mankind with the current technological knowledge, but a transition to a mixed carbon–hydrogen economy can reduce net CO2 emissions and ultimately lead to a CO2-neutral world.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 75
DOI: 10.1002/cssc.201601051
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“Nitrogen Fixation by Gliding Arc Plasma: Better Insight by Chemical Kinetics Modelling”. Wang W, Patil B, Heijkers S, Hessel V, Bogaerts A, Chemsuschem 10, 2110 (2017). http://doi.org/10.1002/cssc.201700611
Abstract: The conversion of atmospheric nitrogen into valuable compounds, that is, so-called nitrogen fixation, is gaining increased interest, owing to the essential role in the nitrogen cycle of the biosphere. Plasma technology, and more specifically gliding arc plasma, has great potential in this area, but little is known about the underlying mechanisms. Therefore, we developed a detailed chemical kinetics model for a pulsed-power gliding-arc reactor operating at atmospheric pressure for nitrogen oxide synthesis. Experiments are performed to validate the model and reasonable agreement is reached between the calculated and measured NO and NO2 yields and the corresponding energy efficiency for NOx formation for different N2/O2 ratios, indicating that the model can provide a realistic picture of the plasma chemistry. Therefore, we can use the model to investigate the reaction pathways for the formation and loss of NOx. The results indicate that vibrational excitation of N2 in the gliding arc contributes significantly to activating the N2 molecules, and leads to an energy efficient way of NOx production, compared to the thermal process. Based on the underlying chemistry, the model allows us to propose solutions on how to further improve the NOx formation by gliding arc technology. Although the energy efficiency of the gliding-arc-based nitrogen fixation process at the present stage is not comparable to the world-scale Haber–Bosch process, we believe our study helps us to come up with more realistic scenarios of entering a cutting-edge innovation in new business cases for the decentralised production of fertilisers for agriculture, in which lowtemperature plasma technology might play an important role.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 7.226
DOI: 10.1002/cssc.201700611
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“Gliding Arc Plasmatron: Providing an Alternative Method for Carbon Dioxide Conversion”. Ramakers M, Trenchev G, Heijkers S, Wang W, Bogaerts A, Chemsuschem 10, 2642 (2017). http://doi.org/10.1002/cssc.201700589
Abstract: Low-temperature plasmas are gaining a lot of interest for environmental and energy applications. A large research field in these applications is the conversion of CO2 into chemicals and fuels. Since CO2 is a very stable molecule, a key performance indicator for the research on plasma-based CO2 conversion is the energy efficiency. Until now, the energy efficiency in atmospheric plasma reactors is quite low, and therefore we employ here a novel type of plasma reactor, the gliding arc plasmatron (GAP). This paper provides a detailed experimental and computational study of the CO2 conversion, as well as the energy cost and efficiency in a GAP. A comparison with thermal conversion, other plasma types and other novel CO2 conversion technologies is made to find out whether this novel plasma reactor can provide a significant contribution to the much-needed efficient conversion of CO2. From these comparisons it becomes evident that our results are less than a factor of two away from being cost competitive and already outperform several other new technologies. Furthermore, we indicate how the performance of the GAP can still be improved by further exploiting its non-equilibrium character. Hence, it is clear that the GAP is very promising for CO2 conversion.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 42
DOI: 10.1002/cssc.201700589
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“Nitrogen fixation by gliding arc plasma : better insight by chemical kinetics modelling”. Wang W, Patil B, Heijkers S, Hessel V, Bogaerts A, Chemsuschem 10, 2145 (2017). http://doi.org/10.1002/CSSC.201700095
Abstract: The conversion of atmospheric nitrogen into valuable compounds, that is, so-called nitrogen fixation, is gaining increased interest, owing to the essential role in the nitrogen cycle of the biosphere. Plasma technology, and more specifically gliding arc plasma, has great potential in this area, but little is known about the underlying mechanisms. Therefore, we developed a detailed chemical kinetics model for a pulsed-power gliding-arc reactor operating at atmospheric pressure for nitrogen oxide synthesis. Experiments are performed to validate the model and reasonable agreement is reached between the calculated and measured NO and NO2 yields and the corresponding energy efficiency for NOx formation for different N2/O2 ratios, indicating that the model can provide a realistic picture of the plasma chemistry. Therefore, we can use the model to investigate the reaction pathways for the formation and loss of NOx. The results indicate that vibrational excitation of N2 in the gliding arc contributes significantly to activating the N2 molecules, and leads to an energy efficient way of NOx production, compared to the thermal process. Based on the underlying chemistry, the model allows us to propose solutions on how to further improve the NOx formation by gliding arc technology. Although the energy efficiency of the gliding-arc-based nitrogen fixation process at the present stage is not comparable to the world-scale HaberBosch process, we believe our study helps us to come up with more realistic scenarios of entering a cutting-edge innovation in new business cases for the decentralised production of fertilisers for agriculture, in which low-temperature plasma technology might play an important role.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 42
DOI: 10.1002/CSSC.201700095
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“Dry Reforming of Methane in a Gliding Arc Plasmatron: Towards a Better Understanding of the Plasma Chemistry”. Cleiren E, Heijkers S, Ramakers M, Bogaerts A, Chemsuschem 10, 4025 (2017). http://doi.org/10.1002/cssc.201701274
Abstract: Dry reforming of methane (DRM) in a gliding arc plasmatron is studied for different CH4 fractions in the mixture. The CO2 and CH4 conversions reach their highest values of approximately 18 and 10%, respectively, at 25% CH4 in the gas mixture, corresponding to an overall energy cost of 10 kJ L@1 (or 2.5 eV per molecule) and an energy efficiency of 66%. CO and H2 are the major products, with the formation of smaller fractions of C2Hx (x=2, 4, or 6) compounds and H2O. A chemical kinetics model is used to investigate the underlying chemical processes. The calculated CO2 and CH4 conversion and the energy efficiency are in good agreement with the experimental data. The model calculations reveal that the reaction of CO2 (mainly at vibrationally excited levels) with H radicals is mainly responsible for
the CO2 conversion, especially at higher CH4 fractions in the mixture, which explains why the CO2 conversion increases with increasing CH4 fraction. The main process responsible for CH4 conversion is the reaction with OH radicals. The excellent energy efficiency can be explained by the non-equilibrium character of the plasma, in which the electrons mainly activate the gas molecules, and by the important role of the vibrational kinetics of CO2. The results demonstrate that a gliding arc plasmatron is very promising for DRM.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 23
DOI: 10.1002/cssc.201701274
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“Harvesting hydrogen gas from air pollutants with an un-biased gas phase photo-electrochemical cell”. Verbruggen SW, Van Hal M, Bosserez T, Rongé, J, Hauchecorne B, Martens JA, Lenaerts S, Chemsuschem 10, 1413 (2017). http://doi.org/10.1002/CSSC.201601806
Abstract: The concept of an all-gas-phase photo-electrochemical cell (PEC) producing hydrogen gas from volatile organic contaminated gas and light is presented. Without applying any external bias, organic contaminants are degraded and hydrogen gas is produced in separate electrode compartments. The system works most efficiently with organic pollutants in inert carrier gas. In the presence of oxygen gas, the cell performs less efficiently but still significant photocurrents are generated, showing the cell can be run on organic contaminated air. The purpose of this study is to demonstrate new application opportunities of PEC technology and to encourage further advancement toward photo-electrochemical remediation of air pollution with the attractive feature of simultaneous energy recovery and pollution abatement.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 7.226
Times cited: 6
DOI: 10.1002/CSSC.201601806
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“A non-aqueous synthesis of TiO2SiO2 composites in supercritical CO2 for the photodegradation of pollutants”. Jammaer J, Aprile C, Verbruggen SW, Lenaerts S, Pescarmona PP, Martens JA, Chemsuschem 4, 1457 (2011). http://doi.org/10.1002/CSSC.201100059
Abstract: Titania/silica composites with different Ti/Si ratios are synthesized via a nonconventional synthesis route. The synthesis involves non-aqueous reaction of metal alkoxides and formic acid at 75 °C in supercritical carbon dioxide. The as-prepared composite materials contain nanometer-sized anatase crystallites and amorphous silica. Large specific surface areas are obtained. The composites are evaluated in the photocatalytic degradation of phenol in aqueous medium, and in the elimination of acetaldehyde from air. The highest photocatalytic activity in both processes is achieved with a composite containing 40 wt % TiO2.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 7.226
Times cited: 15
DOI: 10.1002/CSSC.201100059
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“C2-H arylation of indoles catalyzed by palladium-containing metal-organic-framework in γ-valerolactone”. Anastasiou I, Van Velthoven N, Tomarelli E, Lombi A, Lanari D, Liu P, Bals S, De Vos DE, Vaccaro L, Chemsuschem 13 (2020). http://doi.org/10.1002/CSSC.202000378
Abstract: An efficient and selective procedure was developed for the direct C2-H arylation of indoles using a Pd-loaded metal-organic framework (MOF) as a heterogeneous catalyst and the nontoxic biomass-derived solvent gamma-valerolactone (GVL) as a reaction medium. The developed method allows for excellent yields and C-2 selectivity to be achieved and tolerates various substituents on the indole scaffold. The established conditions ensure the stability of the catalyst as well as recoverability, reusability, and low metal leaching into the solution.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 8.4
Times cited: 22
DOI: 10.1002/CSSC.202000378
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“Modeling the physicochemical properties of natural deep eutectic solvents : a review”. Kovács A, Billen P, Cornet I, Wijnants M, Neyts EC, Chemsuschem 13, 3789 (2020). http://doi.org/10.1002/CSSC.202000286
Abstract: Natural deep eutectic solvents (NADES) are mixtures of naturally derived compounds with a significantly decreased melting point due to the specific interactions among the constituents. NADES have benign properties (low volatility, flammability, toxicity, cost) and tailorable physicochemical properties (by altering the type and molar ratio of constituents), hence they are often considered as a green alternative to common organic solvents. Modeling the relation between their composition and properties is crucial though, both for understanding and predicting their behavior. Several efforts were done to this end, yet this review aims at structuring the present knowledge as an outline for future research. First, we reviewed the key properties of NADES and relate them to their structure based on the available experimental data. Second, we reviewed available modeling methods applicable to NADES. At the molecular level, density functional theory and molecular dynamics allow interpreting density differences and vibrational spectra, and computation of interaction energies. Additionally, properties at the level of the bulk media can be explained and predicted by semi-empirical methods based on ab initio methods (COSMO-RS) and equation of state models (PC-SAFT). Finally, methods based on large datasets are discussed; models based on group contribution methods and machine learning. A combination of bulk media and dataset modeling allows qualitative prediction and interpretation of phase equilibria properties on the one hand, and quantitative prediction of melting point, density, viscosity, surface tension and refractive indices on the other hand. In our view, multiscale modeling, combining the molecular and macroscale methods, will strongly enhance the predictability of NADES properties and their interaction with solutes, yielding truly tailorable solvents to accommodate (bio)chemical reactions.
Keywords: A1 Journal article; Engineering sciences. Technology; Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Biochemical Wastewater Valorization & Engineering (BioWaVE)
Impact Factor: 8.4
DOI: 10.1002/CSSC.202000286
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“Energy‐Efficient Small‐Scale Ammonia Synthesis Process with Plasma‐enabled Nitrogen Oxidation and Catalytic Reduction of Adsorbed NOx”. Hollevoet L, Vervloessem E, Gorbanev Y, Nikiforov A, De Geyter N, Bogaerts A, Martens JA, Chemsuschem (2022). http://doi.org/10.1002/cssc.202102526
Abstract: Industrial ammonia production without CO2 emission and with low energy consumption is one of the technological grand challenges of this age. Current Haber-Bosch ammonia mass production processes work with a thermally activated iron catalyst needing high pressure. The need for large volumes of hydrogen gas and the continuous operation mode render electrification of Haber-Bosch plants difficult to achieve. Electrochemical solutions at low pressure and temperature are faced with the problematic inertness of the nitrogen molecule on electrodes. Direct reduction of N2 to ammonia is only possible with very reactive chemicals such as lithium metal, the regeneration of which is energy intensive. Here, the attractiveness of an oxidative route for N2 activation was presented. N2 conversion to NOx in a plasma reactor followed by reduction with H2 on a heterogeneous catalyst at low pressure could be an energy-efficient option for small-scale distributed ammonia production with renewable electricity and without intrinsic CO2 footprint.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 8.4
DOI: 10.1002/cssc.202102526
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“Effect of Gas Composition on Temperature and CO2Conversion in a Gliding Arc Plasmatron reactor: Insights for Post‐Plasma Catalysis from Experiments and Computation”. Xu W, Van Alphen S, Galvita VV, Meynen V, Bogaerts A, ChemSusChem (2024). http://doi.org/10.1002/cssc.202400169
Abstract: Plasma‐based CO<sub>2</sub>conversion has attracted increasing interest. However, to understand the impact of plasma operation on post‐plasma processes, we studied the effect of adding N<sub>2</sub>, N<sub>2</sub>/CH<sub>4</sub>and N<sub>2</sub>/CH<sub>4</sub>/H<sub>2</sub>O to a CO<sub>2</sub>gliding arc plasmatron (GAP) to obtain valuable insights into their impact on exhaust stream composition and temperature, which will serve as feed gas and heat for post‐plasma catalysis (PPC). Adding N<sub>2</sub>improves the CO<sub>2</sub>conversion from 4 % to 13 %, and CH<sub>4</sub>addition further promotes it to 44 %, and even to 61 % at lower gas flow rate (6 L/min), allowing a higher yield of CO and hydrogen for PPC. The addition of H<sub>2</sub>O, however, reduces the CO<sub>2</sub>conversion from 55 % to 22 %, but it also lowers the energy cost, from 5.8 to 3 kJ/L. Regarding the temperature at 4.9 cm post‐plasma, N<sub>2</sub>addition increases the temperature, while the CO<sub>2</sub>/CH<sub>4</sub>ratio has no significant effect on temperature. We also calculated the temperature distribution with computational fluid dynamics simulations. The obtained temperature profiles (both experimental and calculated) show a decreasing trend with distance to the exhaust and provide insights in where to position a PPC bed.
Keywords: A1 Journal Article; CO2 conversion · Plasma · Gliding arc plasmatron · Temperature profiles · Computational modelling; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 8.4
DOI: 10.1002/cssc.202400169
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“Control of the interfacial wettability to synthesize highly dispersed PtPd nanocrystals for efficient oxygen reduction reaction”. Wei H, Hu Z-Y, Xiao Y-X, Tian G, Ying J, Van Tendeloo G, Janiak C, Yang X-Y, Su B-L, Chemistry: an Asian journal 13, 1119 (2018). http://doi.org/10.1002/ASIA.201800191
Abstract: Highly dispersed PtPd bimetallic nanocrystals with enhanced catalytic activity and stability were prepared by adjusting the interfacial wettability of the reaction solution on a commercial carbon support. This approach holds great promise for the development of high-performance and low-cost catalysts for practical applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.083
Times cited: 3
DOI: 10.1002/ASIA.201800191
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“Hierarchical MoS2@TiO2 heterojunctions for enhanced photocatalytic performance and electrocatalytic hydrogen evolution”. Dong Y, Chen S-Y, Lu Y, Xiao Y-X, Hu J, Wu S-M, Deng Z, Tian G, Chang G-G, Li J, Lenaerts S, Janiak C, Yang X-Y, Su B-L, Chemistry: an Asian journal 13, 1609 (2018). http://doi.org/10.1002/ASIA.201800359
Abstract: Hierarchical MoS2@TiO2 heterojunctions were synthesized through a one-step hydrothermal method by using protonic titanate nanosheets as the precursor. The TiO2 nanosheets prevent the aggregation of MoS2 and promote the carrier transfer efficiency, and thus enhance the photocatalytic and electrocatalytic activity of the nanostructured MoS2. The obtained MoS2@TiO2 has significantly enhanced photocatalytic activity in the degradation of rhodamineB (over 5.2times compared with pure MoS2) and acetone (over 2.8times compared with pure MoS2). MoS2@TiO2 is also beneficial for electrocatalytic hydrogen evolution (26times compared with pure MoS2, based on the cathodic current density). This work offers a promising way to prevent the self-aggregation of MoS2 and provides a new insight for the design of heterojunctions for materials with lattice mismatches.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.083
Times cited: 22
DOI: 10.1002/ASIA.201800359
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“Interface control by chemical and dimensional matching in an oxide heterostructure”. O'Sullivan M, Hadermann J, Dyer MS, Turner S, Alaria J, Manning TD, Abakumov AM, Claridge JB, Rosseinsky MJ, Nature chemistry 8, 347 (2016). http://doi.org/10.1038/NCHEM.2441
Abstract: Interfaces between different materials underpin both new scientific phenomena, such as the emergent behaviour at oxide interfaces, and key technologies, such as that of the transistor. Control of the interfaces between materials with the same crystal structures but different chemical compositions is possible in many materials classes, but less progress has been made for oxide materials with different crystal structures. We show that dynamical self-organization during growth can create a coherent interface between the perovskite and fluorite oxide structures, which are based on different structural motifs, if an appropriate choice of cations is made to enable this restructuring. The integration of calculation with experimental observation reveals that the interface differs from both the bulk components and identifies the chemical bonding requirements to connect distinct oxide structures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 25.87
Times cited: 28
DOI: 10.1038/NCHEM.2441
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“Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons”. Zhou Y, Che F, Liu M, Zou C, Liang Z, De Luna P, Yuan H, Li J, Wang Z, Xie H, Li H, Chen P, Bladt E, Quintero-Bermudez R, Sham T-K, Bals S, Hofkens J, Sinton D, Chen G, Sargent EH, Nature chemistry 10, 974 (2018). http://doi.org/10.1038/S41557-018-0092-X
Abstract: The electrochemical reduction of CO2 to multi-carbon products has attracted much attention because it provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the efficiency of CO2 conversion to C-2 products remains below that necessary for its implementation at scale. Modifying the local electronic structure of copper with positive valence sites has been predicted to boost conversion to C-2 products. Here, we use boron to tune the ratio of Cu delta+ to Cu-0 active sites and improve both stability and C-2-product generation. Simulations show that the ability to tune the average oxidation state of copper enables control over CO adsorption and dimerization, and makes it possible to implement a preference for the electrosynthesis of C-2 products. We report experimentally a C-2 Faradaic efficiency of 79 +/- 2% on boron-doped copper catalysts and further show that boron doping leads to catalysts that are stable for in excess of similar to 40 hours while electrochemically reducing CO2 to multi-carbon hydrocarbons.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 25.87
Times cited: 700
DOI: 10.1038/S41557-018-0092-X
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“Charge-ordering transition in iron oxide Fe4O5 involving competing dimer and trimer formation”. Ovsyannikov SV, Bykov M, Bykova E, Kozlenko DP, Tsirlin AA, Karkin AE, Shchennikov VV, Kichanov SE, Gou H, Abakumov AM, Egoavil R, Verbeeck J, McCammon C, Dyadkin V, Chernyshov D, van Smaalen S, Dubrovinsky LS, Nature chemistry 8, 501 (2016). http://doi.org/10.1038/nchem.2478
Abstract: Phase transitions that occur in materials, driven, for instance, by changes in temperature or pressure, can dramatically change the materials' properties. Discovering new types of transitions and understanding their mechanisms is important not only from a fundamental perspective, but also for practical applications. Here we investigate a recently discovered Fe4O5 that adopts an orthorhombic CaFe3O5-type crystal structure that features linear chains of Fe ions. On cooling below approximately 150 K, Fe4O5 undergoes an unusual charge-ordering transition that involves competing dimeric and trimeric ordering within the chains of Fe ions. This transition is concurrent with a significant increase in electrical resistivity. Magnetic-susceptibility measurements and neutron diffraction establish the formation of a collinear antiferromagnetic order above room temperature and a spin canting at 85 K that gives rise to spontaneous magnetization. We discuss possible mechanisms of this transition and compare it with the trimeronic charge ordering observed in magnetite below the Verwey transition temperature.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 25.87
Times cited: 51
DOI: 10.1038/nchem.2478
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“Synthesis and in vitro investigation of halogenated 1,3-bis(4-nitrophenyl)triazenide salts as antitubercular compounds”. Torfs E, Vajs J, Bidart de Macedo M, Cools F, Vanhoutte B, Gorbanev Y, Bogaerts A, Verschaeve L, Caljon G, Maes L, Delputte P, Cos P, Komrlj J, Cappoen D, Chemical biology and drug design , 1 (2017). http://doi.org/10.1111/CBDD.13087
Abstract: The diverse pharmacological properties of the diaryltriazenes have sparked the interest to investigate their potential to be repurposed as antitubercular drug candidates. In an attempt to improve the antitubercular activity of a previously constructed diaryltriazene library, eight new halogenated nitroaromatic triazenides were synthesized and underwent biological evaluation. The potency of the series was confirmed against the Mycobacterium tuberculosis lab strain H37Ra, and for the most potent derivative, we observed a minimal inhibitory concentration of 0.85 μm. The potency of the triazenide derivatives against M. tuberculosis H37Ra was found to be highly dependent on the nature of the halogenated phenyl substituent and less dependent on cationic species used for the preparation of the salts. Although the inhibitory concentration against J774A.1 macrophages was observed at 3.08 μm, the cellular toxicity was not mediated by the generation of nitroxide intermediate as confirmed by electron paramagnetic resonance spectroscopy, whereas no in vitro mutagenicity could be observed for the new halogenated nitroaromatic triazenides when a trifluoromethyl substituent was present on both the aryl moieties.
Keywords: A1 Journal article; Pharmacology. Therapy; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 2.396
Times cited: 5
DOI: 10.1111/CBDD.13087
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“Computer simulations of a dielectric barrier discharge used for analytical spectrometry”. Martens T, Bogaerts A, Brok W, van Dijk J, Analytical and bioanalytical chemistry 388, 1583 (2007). http://doi.org/10.1007/s00216-007-1269-0
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.431
Times cited: 28
DOI: 10.1007/s00216-007-1269-0
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“Unraveling the effect of the aptamer complementary element on the performance of duplexed aptamers : a thermodynamic study”. Dillen A, Vandezande W, Daems D, Lammertyn J, Analytical And Bioanalytical Chemistry 413, 4739 (2021). http://doi.org/10.1007/S00216-021-03444-Y
Abstract: Duplexed aptamers (DAs) are widespread aptasensor formats that simultaneously recognize and signal the concentration of target molecules. They are composed of an aptamer and aptamer complementary element (ACE) which consists of a short oligonucleotide that partially inhibits the aptamer sequence. Although the design principles to engineer DAs are straightforward, the tailored development of DAs for a particular target is currently based on trial and error due to limited knowledge of how the ACE sequence affects the final performance of DA biosensors. Therefore, we have established a thermodynamic model describing the influence of the ACE on the performance of DAs applied in equilibrium assays and demonstrated that this relationship can be described by the binding strength between the aptamer and ACE. To validate our theoretical findings, the model was applied to the 29-mer anti-thrombin aptamer as a case study, and an experimental relation between the aptamer-ACE binding strength and performance of DAs was established. The obtained results indicated that our proposed model could accurately describe the effect of the ACE sequence on the performance of the established DAs for thrombin detection, applied for equilibrium assays. Furthermore, to characterize the binding strength between the aptamer and ACEs evaluated in this work, a set of fitting equations was derived which enables thermodynamic characterization of DNA-based interactions through thermal denaturation experiments, thereby overcoming the limitations of current predictive software and chemical denaturation experiments. Altogether, this work encourages the development, characterization, and use of DAs in the field of biosensing.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 3.431
DOI: 10.1007/S00216-021-03444-Y
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“Advantages of combined mu-XRF and mu-XRD for phase characterization of Ti-B-C ceramics compared with conventional X-ray diffraction”. Jaroszewicz J, de Nolf W, Janssens K, Michalski A, Falkenberg G, Analytical and bioanalytical chemistry 391, 1129 (2008). http://doi.org/10.1007/S00216-008-2097-6
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 3.431
Times cited: 7
DOI: 10.1007/S00216-008-2097-6
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“Compositional analysis of Tuscan glass samples: in search of raw materials fingerprints”. Cagno S, Janssens K, Mendera M, Analytical and bioanalytical chemistry 391, 1389 (2008). http://doi.org/10.1007/S00216-008-1945-8
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 3.431
Times cited: 26
DOI: 10.1007/S00216-008-1945-8
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“Euroanalysis 14: the European Conference on Analytical Chemistry”. Janssens K, van Espen P, Van 't dack L, Analytical and bioanalytical chemistry 391, 1107 (2008). http://doi.org/10.1007/S00216-008-2114-9
Keywords: Editorial; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Chemometrics (Mitac 3)
Impact Factor: 3.431
DOI: 10.1007/S00216-008-2114-9
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“Investigating morphological changes in treated vs. untreated stone building materials by x-ray micro-CT”. Bugani S, Camaiti M, Morselli L, Van de Casteele E, Janssens K, Analytical and bioanalytical chemistry 391, 1343 (2008). http://doi.org/10.1007/S00216-008-1946-7
Keywords: A1 Journal article; Vision lab; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 3.431
Times cited: 25
DOI: 10.1007/S00216-008-1946-7
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“Spatially resolved (semi)quantitative determination of iron (Fe) in plants by means of synchrotron micro X-ray fluorescence”. Terzano R, Alfeld M, Janssens K, Vekemans B, Schoonjans T, Vincze L, Tomasi N, Pinton R, Cesco S, Analytical and bioanalytical chemistry 405, 3341 (2013). http://doi.org/10.1007/S00216-013-6768-6
Abstract: Iron (Fe) is an essential element for plant growth and development; hence determining Fe distribution and concentration inside plant organs at the microscopic level is of great relevance to better understand its metabolism and bioavailability through the food chain. Among the available microanalytical techniques, synchrotron mu-XRF methods can provide a powerful and versatile array of analytical tools to study Fe distribution within plant samples. In the last years, the implementation of new algorithms and detection technologies has opened the way to more accurate (semi)quantitative analyses of complex matrices like plant materials. In this paper, for the first time the distribution of Fe within tomato roots has been imaged and quantified by means of confocal mu-XRF and exploiting a recently developed fundamental parameter-based algorithm. With this approach, Fe concentrations ranging from few hundreds of ppb to several hundreds of ppm can be determined at the microscopic level without cutting sections. Furthermore, Fe (semi)quantitative distribution maps were obtained for the first time by using two opposing detectors to collect simultaneously the XRF radiation emerging from both sides of an intact cucumber leaf.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 3.431
Times cited: 27
DOI: 10.1007/S00216-013-6768-6
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