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“A Ricardian analysis of climate change impacts on Japan's agriculture : accounting for solar radiation”. Okamura I, Van Passel S, Fabri C, Senda T, Climate change economics 14, 2350022 (2023). http://doi.org/10.1142/S2010007823500227
Abstract: This study evaluates the effects of climate change on the net revenue of farmers in Japan. We adopted the Ricardian model, which implicitly accounts for farmers’ full adaptation. The main findings of this study are as follows. First, the Ricardian regression shows that changes in temperature significantly impact farmers’ net revenue. In contrast, changes in precipitation have limited effects on farmers’ net revenue. The results of future predictions showed that the effects of climate change are positive across the country, with varying degrees between north and south. These results are more optimistic than those in the existing literature, which frequently reveal negative climate change impacts in southern Japan. However, it should be noted that this model assumes full adaptation and does not consider the transition costs of farmers, and understanding the actual adaptive measures is an important remaining issue.
Keywords: A1 Journal article; Economics; Engineering Management (ENM)
DOI: 10.1142/S2010007823500227
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“Adaptive capacity of smallholder farmers toward climate change: evidence from Hamadan province in Iran”. Jamshidi O, Asadi A, Kalantari K, Movahhed Moghaddam S, Dadrass Javan F, Azadi H, Van Passel S, Witlox F, Climate And Development , 1 (2020). http://doi.org/10.1080/17565529.2019.1710097
Abstract: The global climate is changing, and farmers must increase their adaptive capacity to avoid negative impacts. This study aimed to examine the adaptive capacity of farmers’ household to tolerate climate changes and identify factors affecting the climate in Hamadan province, Iran. The adaptive capacity was evaluated quantitatively by using 23 indicators and was categorized into high, moderate, low, and very low adaptive capacity. The study was based on a cross sectional survey and was conducted with a random sample of 280 household farmers distributed in five counties of Hamadan province in the west of the country whose climatic data revealed signs of climate change. The result showed that farmers’ negative perception toward climate change generally increases during dry seasons and decreases when the precipitation and water resources are more available. Regarding the available information, only 15% of farmers had a high level of adaptive capacity, while 10% of them were highly adapted, and 27.5% showed a very low level of adaptive capacity. Adaptive capacity in the current study was influenced by some socio-economic variables including total farm size, irrigated farm size, number of agricultural land plots, and perception and knowledge of climate change.
Keywords: A1 Journal Article; Adaptive capacity; cross sectional survey; socio-economic variables; adaptation strategies; Hamadan province; Engineering Management (ENM) ;
Impact Factor: 2.051
DOI: 10.1080/17565529.2019.1710097
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“A techno-economic assessment of an algal-based biorefinery”. Thomassen G, Egiguren Vila U, Van Dael M, Lemmens B, Van Passel S, Clean Technologies And Environmental Policy 18, 1849 (2016). http://doi.org/10.1007/S10098-016-1159-2
Abstract: Economic and technological assessments have identified difficulties with the commercialization of bulk products from microalgae, like biofuels. To overcome these problems, a multi-product algal-based biorefinery has been proposed. This paper performs a techno-economic assessment of such a biorefinery. Four production pathways, ranging from a base case with commercial technologies to an improved case with innovative technologies, are analyzed. All region-specific parameters were adapted to Belgian conditions. Three scenarios result in techno-economically viable production plants. The most profitable scenario is the scenario which uses a specialized membrane for medium recycling and an open pond algae cultivation. Although the inclusion of a photobioreactor decreases the culture medium costs, the higher investment costs result in lower economic profits. The carotenoid content and price are identified as critical parameters. Furthermore, the economies of scale assumption for the photobioreactor is critical for the feasibility of this cultivation technology. The techno-economic assessment is an important methodology to guide and evaluate further improvements in research and shorten the time-to-market for innovative technologies in this field.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 3.331
Times cited: 24
DOI: 10.1007/S10098-016-1159-2
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“Cost-efficient emission abatement of energy and transportation technologies : mitigation costs and policy impacts for Belgium”. De Schepper E, Van Passel S, Lizin S, Achten WMJ, Van Acker K, Clean Technologies And Environmental Policy 16, 1107 (2014). http://doi.org/10.1007/S10098-014-0713-Z
Abstract: In the light of global warming, this paper develops a framework to compare energy and transportation technologies in terms of cost-efficient GHG emission reduction. We conduct a simultaneous assessment of economic and environmental performances through life cycle costing and life cycle assessment. To calculate the GHG mitigation cost, we create reference systems within the base scenario. Further, we extend the concept of the mitigation cost, allowing (i) comparision of technologies given a limited investment resource, and (ii) evaluation of the direct impact of policy measures by means of the subsidized mitigation cost. The framework is illustrated with a case of solar photovoltaics (PV), grid powered battery electric vehicles (BEVs), and solar powered BEVs for a Belgian small and medium sized enterprise. The study's conclusions are that the mitigation cost of solar PV is high, even though this is a mature technology. The emerging mass produced BEVs on the other hand are found to have a large potential for cost-efficient GHG mitigation as indicated by their low cost of mitigation. Finally, based on the subsidized mitigation cost, we conclude that the current financial stimuli for all three investigated technologies are excessive when compared to the CO2 market value under the EU Emission Trading Scheme.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 3.331
Times cited: 14
DOI: 10.1007/S10098-014-0713-Z
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“Combining Monte Carlo simulations and experimental design for incorporating risk and uncertainty in investment decisions for cleantech : a fast pyrolysis case study”. Kuppens T, Rafiaani P, Vanreppelen K, Yperman J, Carleer R, Schreurs S, Thewys T, Van Passel S, Clean Technologies And Environmental Policy 20, 1195 (2018). http://doi.org/10.1007/S10098-018-1543-1
Abstract: The value of phytoextracting crops (plants cultivated for soil remediation) depends on the profitability of the sequential investment in a conversion technology aimed at the economic valorization of the plants. However, the net present value (NPV) of an investment in such an innovative technology is risky due to technical and economic uncertainties. Therefore, decision makers want to dispose of information about the probability of a positive NPV, the largest possible loss, and the crucial economic and technical parameters influencing the NPV. This paper maps the total uncertainty in the NPV of an investment in fast pyrolysis for the production of combined heat and power from willow cultivated for phytoextraction in the Belgian Campine. The probability of a positive NPV has been calculated by performing Monte Carlo simulations. Information about possible losses has been provided by means of experimental design. Both methods are then combined in order to identify the key economic and technical parameters influencing the project's profitability. It appears that the case study has a chance of 87% of generating a positive NPV with an expected value of 3 million euro (MEUR), while worst-case scenarios predict possible losses of 7 MEUR. The amount of arable land, the biomass yield, the purchase price of the crop, the policy support, and the product yield of fast pyrolysis are identified as the most influential parameters. It is concluded that both methods, i.e., Monte Carlo simulations and experimental design, provide decision makers with complementary information with regard to economic risk.
Keywords: A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 3.331
Times cited: 5
DOI: 10.1007/S10098-018-1543-1
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“Geochemical assessment of a subtropical reservoir : a case study in Curitiba, Southern Brazil”. Godoi RHM, Hirata PY, Bitterncourt AVL, Godoi AFL, Potgieter-Vermaak S, Gatto Rotondo G, Van Grieken R, et al, Clean : soil, air, water 40, 364 (2012). http://doi.org/10.1002/CLEN.201000610
Abstract: Suspended particles and dissolved substances in water provide reactive surfaces, influence metabolic activity and contribute to the net sediment deposition. It therefore plays an important part in the ecology and quality of the water mass. The water quality in reservoirs is crucial and it is naturally maintained by flushing and sedimentation, which continuously remove phosphorus from the water. In some reservoirs, however, these removal processes are countered by recycling of ions which could play a key role to start and/or maintain the eutrophic state. The combination of macro-, trace- and microanalysis techniques can be useful to trace pollution sources through a chemical fingerprint, whether be during an acute environmental disaster or a long-term release of pollutants. The water quality and total metal content of reservoir sediments were assessed in a reservoir, situated in the capital of the Paraná State, in the South-Eastern part of Brazil. The goal of this paper was to determine the metal presence in the sediment and metal and ionic speciation in the Green River reservoir water. Water and bed sediment samples, collected from various sites during 2008 and 2009, were investigated using XRF, ICP-OES, ICP-MS, XRD and zeta potential measurements. Based on the results, the heavy metal concentration and chemical composition of the suspended matter in the water samples, as well as the sediment's chemical composition will be discussed.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
DOI: 10.1002/CLEN.201000610
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“Trace elements in the atmospheric aerosols and soils in and around Recife, N.E. Brasil”. Costa Dantas C, Moura de Amorim W, Van 't dack L, Van Grieken R, Ciencia e cultura 32, 1525 (1980)
Keywords: A3 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
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“Spatial variation behaviors of argon inductively coupled plasma during discharge mode transition”. Fei G, Xue-Chun L, Zhao S-X, You-Nian W, Chinese physics B 21, 075203 (2012). http://doi.org/10.1088/1674-1056/21/7/075203
Abstract: A Langmuir probe and an ICCD are employed to study the discharge mode transition in Ar inductively coupled plasma. Electron density and plasma emission intensity are measured during the E (capacitive discharge) to H (inductive discharge) mode transitions at different pressures. It is found that plasma exists with a low electron density and a weak emission intensity in the E mode, while it has a high electron density and a strong emission intensity in the H mode. Meanwhile, the plasma emission intensity spatial (2D image) profile is symmetrical in the H mode, but the 2D image is an asymmetric profile in the E mode. Moreover, the electron density and emission intensity jump up discontinuously at high pressure, but increase almost continuously at the E to H mode transition under low pressure.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.223
Times cited: 11
DOI: 10.1088/1674-1056/21/7/075203
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“Atomic defects, functional groups and properties in MXenes”. Cui W, Hu Z-Y, Unocic RR, Van Tendeloo G, Sang X, Chinese Chemical Letters 32, 339 (2021). http://doi.org/10.1016/J.CCLET.2020.04.024
Abstract: MXenes, a new family of functional two-dimensional (2D) materials, have shown great potential for an extensive variety of applications within the last decade. Atomic defects and functional groups in MXenes are known to have a tremendous influence on the functional properties. In this review, we focus on recent progress in the characterization of atomic defects and functional group chemistry in MXenes, and how to control them to directly influence various properties (e.g., electron transport, Li' adsorption, hydrogen evolution reaction (HER) activity, and magnetism) of 2D MXenes materials. Dynamic structural transformations such as oxidation and growth induced by atomic defects in MXenes are also discussed. The review thus provides perspectives on property optimization through atomic defect engineering, and bottom-up synthesis methods based on defect-assisted homoepitaxial growth of MXenes. (C) 2020 Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences. Published by Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.932
DOI: 10.1016/J.CCLET.2020.04.024
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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 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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“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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“Recent trends in plasmon‐assisted photocatalytic CO₂, reduction”. Ciocarlan R-G, Blommaerts N, Lenaerts S, Cool P, Verbruggen SW, Chemsuschem 16, e202201647 (2023). http://doi.org/10.1002/CSSC.202201647
Abstract: Direct photocatalytic reduction of CO2 has become an highly active field of research. It is thus of utmost importance to maintain an overview of the various materials used to sustain this process, find common trends, and, in this way, eventually improve the current conversions and selectivities. In particular, CO2 photoreduction using plasmonic photocatalysts under solar light has gained tremendous attention, and a wide variety of materials has been developed to reduce CO2 towards more practical gases or liquid fuels (CH4, CO, CH3OH/CH3CH2OH) in this manner. This Review therefore aims at providing insights in current developments of photocatalysts consisting of only plasmonic nanoparticles and semiconductor materials. By classifying recent studies based on product selectivity, this Review aims to unravel common trends that can provide effective information on ways to improve the photoreduction yield or possible means to shift the selectivity towards desired products, thus generating new ideas for the way forward.
Keywords: A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 8.4
DOI: 10.1002/CSSC.202201647
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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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“Fluorescent nanodiamonds with bioorthogonally reactive protein-resistant polymeric coatings”. Rehor I, Mackova H, Filippov SK, Kucka J, Proks V, Slegerova J, Turner S, Van Tendeloo G, Ledvina M, Hruby M, Cigler P;, ChemPlusChem 79, 21 (2014). http://doi.org/10.1002/cplu.201300339
Abstract: The novel synthesis of a polymeric interface grown from the surface of bright fluorescent nanodiamonds is reported. The polymer enables bioorthogonal attachment of various molecules by click chemistry; the particles are resistant to nonspecific protein adsorption and show outstanding colloidal stability in buffers and biological media. The coating fully preserves the unique optical properties of the nitrogen-vacancy centers that are crucial for bioimaging and sensoric applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.797
Times cited: 34
DOI: 10.1002/cplu.201300339
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“On the Origin of Damped Electrochemical Oscillations at Silicon Anodes (Revisited)”. Proost J, Blaffart F, Turner S, Idrissi H, ChemPhysChem : a European journal of chemical physics and physical chemistry 15, 3116 (2014). http://doi.org/10.1002/cphc.201402207
Abstract: Electrochemical oscillations accompanying the formation of anodic silica have been shown in the past to be correlated with rather abrupt changes in the mechanical stress state of the silica film, commonly associated with some kind of fracture or porosification of the oxide. To advance the understanding on the origin of such oscillations in fluoride-free electrolytes, we have revisited a seminal experiment reported by Lehmann almost two decades ago. We thereby demonstrate that the oscillations are not stress-induced, and do not originate from a morphological transformation of the oxide in the course of anodisation. Alternatively, the mechanical features accompanying the oscillations can be explained by a partial relaxation of the field-induced electrostrictive stress. Furthermore, our observations suggest that the oscillation mechanism more likely results from a periodic depolarisation of the anodic silica.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.075
Times cited: 5
DOI: 10.1002/cphc.201402207
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“Rational design of Ag/TiO2 nanosystems by a combined RF-sputtering/sol-gel approach”. Armelao L, Barreca D, Bottaro G, Gasparotto A, Maccato C, Tondello E, Lebedev OI, Turner S, Van Tendeloo G, Štangar UL, ChemPhysChem : a European journal of chemical physics and physical chemistry 10, 3249 (2009). http://doi.org/10.1002/cphc.200900571
Abstract: The present work is devoted to the preparation of Ag/TiO2 nanosystems by an original synthetic strategy, based on the radio-frequency (RF) sputtering of silver particles on titania-based xerogels prepared by the sol-gel (SG) route. This approach takes advantage of the synergy between the microporous xerogel structure and the infiltration power characterizing RF-sputtering, whose combination enables the obtainment of a tailored dispersion of Ag-containing particles into the titania matrix. In addition, the systems chemico-physical features can be tuned further through proper ex situ thermal treatments in air at 400 and 600 °C. The synthesized composites are extensively characterized by the joint use of complementary techniques, that is, X-ray photoelectron and X-ray excited Auger electron spectroscopies (XPS, XE-AES), secondary ion mass spectrometry (SIMS), glancing incidence X-ray diffraction (GIXRD), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), electron diffraction (ED), high-angle annular dark field scanning TEM (HAADF-STEM), energy-filtered TEM (EF-TEM) and optical absorption spectroscopy. Finally, the photocatalytic performances of selected samples in the decomposition of the azo-dye Plasmocorinth B are preliminarily investigated. The obtained results highlight the possibility of tailoring the system characteristics over a broad range, directly influencing their eventual functional properties.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.075
Times cited: 56
DOI: 10.1002/cphc.200900571
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