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“A new generalized empirical correlation for predicting methane hydrate equilibrium conditions in pure water”. Kummamuru NB, Perreault P, Lenaerts S, Industrial &, Engineering Chemistry Research 60, 3474 (2021). http://doi.org/10.1021/ACS.IECR.0C05833
Abstract: This work contributes to a new generalized empirical correlation for predicting methane (CH4) hydrate equilibrium conditions in pure water. Unlike the conventional thermodynamic approach that involves complex reckoning, the proposed empirical equation is developed by regressing 215 experimental data points from the literature and validating with 45 data points for predicting methane hydrate equilibrium conditions in pure water. The new correlation is proposed for a temperature and pressure range of 273.2–303.48 K and 2.63–72.26 MPa, respectively. The accuracy and performance of the proposed correlation is quantitatively evaluated using statistical error analysis. The proposed correlation was able to estimate CH4 hydrate equilibrium conditions satisfactorily with an R2 of 0.99987. The overall error analysis for the proposed correlation shows fair agreement with the experimental data reported within the literature. Concurrently, the new correlation showed better performance in predicting equilibrium conditions compared to those calculated by other empirical correlations available in the literature within the investigated range. In addition, the proposed empirical equation is also checked to evaluate its efficacy in fitting each set of experimental binary/ternary methane hydrates (BTMH) and binary hydrogen hydrates (BHH) for an accurate representation of equilibrium data over a wide range of composition, pressure, and temperature conditions. A maximum percentage deviation of 0.58% and 0.24% was observed between experimental and calculated equilibrium conditions for BTMH and BHH, respectively.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 2.843
DOI: 10.1021/ACS.IECR.0C05833
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“Analysis and comparison of the co2 and co dielectric barrier discharge solid products”. Belov I, Paulussen S, Bogaerts A, Hakone Xv: International Symposium On High Pressure Low Temperature Plasma Chemistry: With Joint Cost Td1208 Workshop: Non-equilibrium Plasmas With Liquids For Water And Surface Treatment (2016)
Abstract: The CO and CO2 Dielectric Barrier Discharges (DBD) and their solid products were analyzed keeping similar energy input regimes. Gas chromatography analysis revealed the presence of CO2, CO and O-2 mixture in the exhaust of the CO2 DBD, while no O-2 was found when CO was used as a feed gas. It was shown that the C-2 Swan lines observed with optical emission spectroscopy were distinct in the CO plasma while they were not observed in the CO2 emission spectrum. Also the solid products of the plasmas exhibited remarkable differences. Nanoparticles with a diameter between10 and 300 nm, composed of Fe, O and C (Fe: O: C similar to 13: 50: 30) were produced by the CO2 DBD, while microscopic dendrite-like carbon structure (C: O similar to 73: 27) were formed in the CO plasma. The growth rate in the CO2 and CO DBDs was evaluated to be on the level of 0.15 mg/min and 15 mg/min, respectively. The difference of the CO and CO2 discharges and their products might be attributed to the oxygen content in the latter (6.4 mol.% O-2 in the exhaust) and subsequent etching of the carbonaceous film.
Keywords: P1 Proceeding; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
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“Plasma based co2 conversion: a combined modeling and experimental study”. Bogaerts A, Snoeckx R, Berthelot A, Heijkers S, Wang W, Sun S, Van Laer K, Ramakers M, Michielsen I, Uytdenhouwen Y, Meynen V, Cool P, Hakone Xv: International Symposium On High Pressure Low Temperature Plasma Chemistry: With Joint Cost Td1208 Workshop: Non-equilibrium Plasmas With Liquids For Water And Surface Treatment (2016)
Abstract: In recent years there is increased interest in plasma-based CO2 conversion. Several plasma setups are being investigated for this purpose, but the most commonly used ones are a dielectric barrier discharge (DBD), a microwave (MW) plasma and a gliding arc (GA) reactor. In this proceedings paper, we will show results from our experiments in a (packed bed) DBD reactor and in a vortex-flow GA reactor, as well as from our model calculations for the detailed plasma chemistry in a DBD, MW and GA, for pure CO2 as well as mixtures of CO2 with N-2, CH4 and H2O.
Keywords: P1 Proceeding; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
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“Pd-catalyzed decarboxylation of glutamic acid and pyroglutamic acid to bio-based 2-pyrrolidone”. De Schouwer F, Claes L, Claes N, Bals S, Degrève J, De Vos DE, Green chemistry : cutting-edge research for a greener sustainable future 17, 2263 (2015). http://doi.org/10.1039/c4gc02194k
Abstract: In order to recycle nitrogen from nitrogen-rich waste streams, particularly protein waste, we studied the decarboxylation of pyroglutamic acid and glutamic acid in a one-pot reaction to bio-based 2-pyrrolidone. After the screening of a wide range of supported Pd and Pt catalysts, 5 wt% Pd/Al2O3 displayed the highest yield (70%) and selectivity (81%) for the decarboxylation of pyroglutamic acid in water at 250 °C and under an inert atmosphere. Side products originate from consecutive reactions of 2-pyrrolidone; different reaction pathways are proposed to explain the presence of degradation products like propionic acid, γ-hydroxybutyric acid, γ-butyrolactone and methylamine. An extensive study of the reaction parameters was performed to check their influence on selectivity and conversion. This heterogeneous catalytic system was successfully extended to the conversion of glutamic acid.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.125
Times cited: 47
DOI: 10.1039/c4gc02194k
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“Catalytic upcycling of PVC waste-derived phthalate esters into safe, hydrogenated plasticizers”. Windels S, Diefenhardt T, Jain N, Marquez C, Bals S, Schlummer M, De Vos DE, Green chemistry : cutting-edge research for a greener sustainable future 24, 754 (2022). http://doi.org/10.1039/D1GC03864H
Abstract: Recycling of end-of-life polyvinyl chloride (PVC) calls for solutions to deal with the vast amounts of harmful phthalate plasticizers that have historically been incorporated in PVC. Here, we report on the upcycling of such waste-extracted phthalate esters into analogues of the much safer diisononyl 1,2-cyclohexanedicarboxylate plasticizer (DINCH), via a catalytic one-pot (trans)esterification-hydrogenation process. For most of the virgin phthalates, Ru/Al2O3 is a highly effective hydrogenation catalyst, yielding >99% ring-hydrogenated products under mild reaction conditions (0.1 mol% Ru, 80 degrees C, 50 bar H-2). However, applying this reaction to PVC-extracted phthalates proved problematic, (1) as benzyl phthalates are hydrogenolyzed to benzoic acids that inhibit the Ru-catalyst, and (2) because impurities in the plasticizer extract (PVC, sulfur) further retard the hydrogenation. These complications were solved by coupling the hydrogenation to an in situ (trans)esterification with a higher alcohol, and by pretreating the extract with an activated carbon adsorbent. In this way, a real phthalate extract obtained from post-consumer PVC waste was eventually completely (>99%) hydrogenated to phthalate-free, cycloaliphatic plasticizers.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 9.8
Times cited: 8
DOI: 10.1039/D1GC03864H
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“Enzyme immobilization on/in polymeric membranes : status, challenges and perspectives in biocatalytic membrane reactors (BMRs)”. Jochems P, Satyawali Y, Diels L, Dejonghe W, Green chemistry : cutting-edge research for a greener sustainable future 13, 1609 (2011). http://doi.org/10.1039/C1GC15178A
Abstract: Immobilization of enzymes is beneficial in terms of improving the process economics by enabling enzyme re-use and enhancing overall productivity and robustness. Increasingly, membranes are thought to be good supports for enzyme immobilization. These resulting biocatalytic membranes are integrated in reactors known as biocatalytic membrane reactors (BMRs) which enable the integration of biocatalysis and separation. Often the available commercial membranes require modifications to make them suitable for enzyme immobilization. Different immobilization techniques can be used on such suitable membranes, but no general rules exist for making a choice between them. Despite the advantages of BMR application, there are some issues which need to be addressed in order to achieve up-scaling of such systems. In this review, the different aspects of enzyme immobilization on membranes are discussed to show the complexity of this interdisciplinary technology. In addition, the existing issues which require further investigation are highlighted.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1039/C1GC15178A
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“Plasma-catalytic one-step steam reforming of CH₄, to CH₃OH and H₂, promoted by oligomerized [Cu-O-Cu] species on zeolites”. Fang W, Wang X, Li S, Hao Y, Yang Y, Zhao W, Liu R, Li D, Li C, Gao X, Wang L, Guo H, Yi Y, Green chemistry : cutting-edge research for a greener sustainable future 26, 5150 (2024). http://doi.org/10.1039/D4GC00265B
Abstract: Oligomerized [Cu-O-Cu] species are reported to be efficient in promoting plasma catalytic one-step steam reforming of methane to methanol and hydrogen, achieving 6.8% CH4 conversion and 73.1% CH3OH selectivity without CO2.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 9.8
DOI: 10.1039/D4GC00265B
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“A multi-objective optimization-extended techno-economic assessment : exploring the optimal microalgal-based value chain”. Thomassen G, Van Dael M, You F, Van Passel S, Green Chemistry 21, 5945 (2019). http://doi.org/10.1039/C9GC03071A
Abstract: The use of fossil-based products induces a large environmental burden. To lighten this burden, green technologies are required that can replace their fossil-based counterparts. To enable the development of economically viable green technologies, an optimization towards both economic and environmental objectives is required. To perform this multi-objective optimization (MOO), the environmental techno-economic assessment (ETEA) methodology is extended towards a MOO-extended ETEA. The development of this MOO-extended ETEA is the main objective of this manuscript. As an example of a green technology, the concept of microalgae biorefineries is used as a case study to illustrate the MOO-extended ETEA. According to the results, all optimal value chains include open pond cultivation, a membrane for medium recycling and spray drying. The optimal economic value chain uses Nannochloropsis sp. in a one-stage cultivation to produce fish larvae feed, while the optimal environmental design uses Dunaliella salina or Haematococcus pluvialis to produce carotenoids and fertilizer or energy products, by means of anaerobic digestion or gasification. The crucial parameters for both environmental and economic feasibility are the content, price and reference impact of the main end product, the growth parameters and the biomass and carotenoid recovery efficiency alongside the different process steps. By identifying the economic and environmentally optimal algal-based value chain and the crucial drivers, the MOO-extended ETEA provides insights on how algae-based value chains can be developed in the most economic and environmentally-friendly way. For example, the inclusion of a medium recycling step to lower the water and salt consumption is required in all Pareto-optimal scenarios. Another major insight is the requirement of high-value products such as carotenoids or specialty food to obtain and economically and environmentally feasible algal-based value chain. Due to the modular nature of the MOO-extended ETEA, multiple processes can be included or excluded from the superstructure. Although this case study is limited to current microalgae biorefinery technologies, the MOO-extended ETEA can also be used to assess the economic and environmental effect of more innovative technologies. This way, the MOO-extended ETEA provides a methodology to assess the economic and environmental potential of innovative green technologies and shorten their time-to-market.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 9.125
Times cited: 1
DOI: 10.1039/C9GC03071A
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“How to assess the potential of emerging green technologies? Towards a prospective environmental and techno-economic assessment framework”. Thomassen G, Van Dael M, Van Passel S, You F, Green Chemistry 21, 4868 (2019). http://doi.org/10.1039/C9GC02223F
Abstract: For sustainable production and consumption, emerging green technologies need to be optimized towards a minimal environmental impact and a maximal economic impact. In an early stage of technology development, more flexibility is available to adapt the technology. Therefore, a prospective environmental and techno-economic assessment is required. The prospective assessment differs at the different stages of technology development, as also the data availability and accuracy evolves. This paper reviews the different prospective technological, economic and environmental assessment methods which have been used to assess the potential of new green chemical technologies. Based on the current best practices, an overarching framework is introduced to assess the technological, economic and environmental potential of an emerging green chemical technology at the different stages of technology development.
Keywords: A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 9.125
Times cited: 5
DOI: 10.1039/C9GC02223F
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“CO2and CH4conversion in “real&rdquo, gas mixtures in a gliding arc plasmatron: how do N2and O2affect the performance?”.Slaets J, Aghaei M, Ceulemans S, Van Alphen S, Bogaerts A, Green Chemistry 22, 1366 (2020). http://doi.org/10.1039/C9GC03743H
Abstract: In this paper we study dry reforming of methane (DRM) in a gliding arc plasmatron (GAP) in the presence of N<sub>2</sub>and O<sub>2</sub>. N<sub>2</sub>is added to create a stable plasma at equal fractions of CO<sub>2</sub>and CH<sub>4</sub>, and because emissions from industrial plants typically contain N<sub>2</sub>, while O<sub>2</sub>is added to enhance the process. We test different gas mixing ratios to evaluate the conversion and energy cost. We obtain conversions between 31 and 52% for CO<sub>2</sub>and between 55 and 99% for CH<sub>4</sub>, with total energy costs between 3.4 and 5.0 eV per molecule, depending on the gas mixture. This is very competitive when benchmarked with the literature. In addition, we present a chemical kinetics model to obtain deeper insight in the underlying plasma chemistry. This allows determination of the major reaction pathways to convert CO<sub>2</sub>and CH<sub>4</sub>, in the presence of O<sub>2</sub>and N<sub>2</sub>, into CO and H<sub>2</sub>. We show that N<sub>2</sub>assists in the CO<sub>2</sub>conversion, but part of the applied energy is also wasted in N<sub>2</sub>excitation. Adding O<sub>2</sub>enhances the CH<sub>4</sub>conversion, and lowers the energy cost, while the CO<sub>2</sub>conversion remains constant, and only slightly drops at the highest O<sub>2</sub>fractions studied, when CH<sub>4</sub>is fully oxidized into CO<sub>2</sub>.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 9.8
DOI: 10.1039/C9GC03743H
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“Plasma-driven catalysis: green ammonia synthesis with intermittent electricity”. Rouwenhorst KHR, Engelmann Y, van ‘t Veer K, Postma RS, Bogaerts A, Lefferts L, Green Chemistry 22, 6258 (2020). http://doi.org/10.1039/D0GC02058C
Abstract: Ammonia is one of the most produced chemicals, mainly synthesized from fossil fuels for fertilizer applications. Furthermore, ammonia may be one of the energy carriers of the future, when it is produced from renewable electricity. This has spurred research on alternative technologies for green ammonia production. Research on plasma-driven ammonia synthesis has recently gained traction in academic literature. In the current review, we summarize the literature on plasma-driven ammonia synthesis. We distinguish between mechanisms for ammonia synthesis in the presence of a plasma, with and without a catalyst, for different plasma conditions. Strategies for catalyst design are discussed, as well as the current understanding regarding the potential plasma-catalyst synergies as function of the plasma conditions and their implications on energy efficiency. Finally, we discuss the limitations in currently reported models and experiments, as an outlook for research opportunities for further unravelling the complexities of plasma-catalytic ammonia synthesis, in order to bridge the gap between the currently reported models and experimental results.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
Impact Factor: 9.8
Times cited: 4
DOI: 10.1039/D0GC02058C
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“Avoiding solid carbon deposition in plasma-based dry reforming of methane”. Biondo O, van Deursen CFAM, Hughes A, van de Steeg A, Bongers W, van de Sanden MCM, van Rooij G, Bogaerts A, Green Chemistry 25, 10485 (2023). http://doi.org/10.1039/D3GC03595F
Abstract: Solid carbon deposition is a persistent challenge in dry reforming of methane (DRM), affecting both classical and plasma-based processes. In this work, we use a microwave plasma in reverse vortex flow configuration to overcome this issue in CO<sub>2</sub>/CH<sub>4</sub>plasmas. Indeed, this configuration efficiently mitigates carbon deposition, enabling operation even with pure CH<sub>4</sub>feed gas, in contrast to other configurations. At the same time, high reactor performance is achieved, with CO<sub>2</sub>and CH<sub>4</sub>conversions reaching 33% and 44% respectively, at an energy cost of 14 kJ L<sup>−1</sup>for a CO<sub>2</sub> : CH<sub>4</sub>ratio of 1 : 1. Laser scattering and optical emission imaging demonstrate that the shorter residence time in reverse vortex flow lowers the gas temperature in the discharge, facilitating a shift from full to partial CH<sub>4</sub>pyrolysis. This underscores the pivotal role of flow configuration in directing process selectivity, a crucial factor in complex chemistries like CO<sub>2</sub>/CH<sub>4</sub>mixtures and very important for industrial applications.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 9.8
DOI: 10.1039/D3GC03595F
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“NOxproduction in a rotating gliding arc plasma: potential avenue for sustainable nitrogen fixation”. Jardali F, Van Alphen S, Creel J, Ahmadi Eshtehardi H, Axelsson M, Ingels R, Snyders R, Bogaerts A, Green Chemistry 23, 1748 (2021). http://doi.org/10.1039/D0GC03521A
Abstract: The fast growing world population demands food to survive, and nitrogen-based fertilizers are essential to ensure sufficient food production. Today, fertilizers are mainly produced from non-sustainable fossil fuels<italic>via</italic>the Haber–Bosch process, leading to serious environmental problems. We propose here a novel rotating gliding arc plasma, operating in air, for direct NO<sub>x</sub>production, which can yield high nitrogen content organic fertilizers without pollution associated with ammonia emission. We explored the efficiency of NO<sub>x</sub>production in a wide range of feed gas ratios, and for two arc modes: rotating and steady. When the arc is in steady mode, record-value NO<sub>x</sub>concentrations up to 5.5% are achieved which are 1.7 times higher than the maximum concentration obtained by the rotating arc mode, and with an energy consumption of 2.5 MJ mol<sup>−1</sup>(or<italic>ca.</italic>50 kW h kN<sup>−1</sup>);<italic>i.e.</italic>the lowest value so far achieved by atmospheric pressure plasma reactors. Computer modelling, using a combination of five different complementary approaches, provides a comprehensive picture of NO<sub>x</sub>formation in both arc modes; in particular, the higher NO<sub>x</sub>production in the steady arc mode is due to the combined thermal and vibrationally-promoted Zeldovich mechanisms.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 9.125
DOI: 10.1039/D0GC03521A
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“Sustainable NOxproduction from air in pulsed plasma: elucidating the chemistry behind the low energy consumption”. Vervloessem E, Gorbanev Y, Nikiforov A, De Geyter N, Bogaerts A, Green Chemistry 24, 916 (2022). http://doi.org/10.1039/D1GC02762J
Abstract: N-Based fertilisers are paramount to support our still-growing world population. Current industrial N<sub>2</sub>fixation is heavily fossil fuel-dependent, therefore, a lot of work is put into the development of fossil-free pathways. Plasma technology offers a fossil-free and flexible method for N<sub>2</sub>fixation that is compatible with renewable energy sources. We present here a pulsed plasma jet for direct NO<sub><italic>x</italic></sub>production from air. The pulsed power allows for a record-low energy consumption (EC) of 0.42 MJ (mol N)<sup>−1</sup>. This is the lowest reported EC in plasma-based N<sub>2</sub>fixation at atmospheric pressure thus far. We compare our experimental data with plasma chemistry modelling, and obtain very good agreement. Hence, we can use our model to explain the underlying mechanisms responsible for this low EC. The pulsed power and the corresponding pulsed gas temperature are the reason for the very low EC: they provide a strong vibrational–translational non-equilibrium and promote the non-thermal Zeldovich mechanism. This insight is important for the development of the next generation of plasma sources for energy-efficient NO<sub><italic>x</italic></sub>production.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 9.8
DOI: 10.1039/D1GC02762J
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“An integrated techno-sustainability assessment (TSA) framework for emerging technologies”. Van Schoubroeck S, Thomassen G, Van Passel S, Malina R, Springael J, Lizin S, Venditti RA, Yao Y, Van Dael M, Green Chemistry 23, 1700 (2021). http://doi.org/10.1039/D1GC00036E
Abstract: A better understanding of the drivers of the economic, environmental, and social sustainability of emerging (biobased) technologies and products in early development phases can help decision-makers to identify sustainability hurdles and opportunities. Furthermore, it guides additional research and development efforts and investment decisions, that will, ultimately, lead to more sustainable products and technologies entering a market. To this end, this study developed a novel techno-sustainability assessment (TSA) framework with a demonstration on a biobased chemical application. The integrated TSA compares the potential sustainability performance of different (technology) scenarios and helps to make better-informed decisions by evaluating and trading-off sustainability impacts in one holistic framework. The TSA combines methods for comprehensive indicator selection and integration of technological and country-specific data with environmental, economic, and social data. Multi-criteria decision analysis (MCDA) is used to address data uncertainty and to enable scenario comparison if indicators are expressed in different units. A hierarchical, stochastic outranking approach is followed that compares different weighting schemes and preference structures to check for the robustness of the results. The integrated TSA framework is demonstrated on an application for which the sustainability of a production and harvesting plant of microalgae-based food colorants is assessed. For a set of scenarios that vary with regard to the algae feedstock, production technology, and location, the sustainability performance is quantified and compared, and the underlying reasons for this performance are explored.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 9.125
DOI: 10.1039/D1GC00036E
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“Disproportionation of nitrogen induced by DC plasma-driven electrolysis in a nitrogen atmosphere”. Pattyn C, Maira N, Buddhadasa M, Vervloessem E, Iseni S, Roy NC, Remy A, Delplancke M-P, De Geyter N, Reniers F, Green Chemistry 24, 7100 (2022). http://doi.org/10.1039/D2GC01013E
Abstract: Nitrogen disproportionation i.e. its simultaneous conversion to compounds of higher (NOx) and lower (NH3) oxidation states in a N-2 DC plasma-driven electrolysis process with a plasma cathode is investigated. This type of plasma-liquid interaction exhibits a growing interest for many applications, in particular nitrogen fixation where it represents a green alternative to the Haber-Bosch process. Optical emission spectroscopy, FTIR and electrochemical sensing systems are used to characterize the gas phase physico-chemistry while the liquid phase is analyzed via ionic chromatography and colorimetric assays. Experiments suggest that lowering the discharge current enhances nitrogen reduction and facilitates the transfer of nitrogen compounds to the liquid phase. Large amounts of water vapor appear to impact the gas discharge physico-chemistry and to favor the vibrational excitation of N-2, a key parameter for an energy-efficient nitrogen fixation.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 9.8
DOI: 10.1039/D2GC01013E
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“A biobased, bioactive, low CO₂, impact coating for soil improvers”. Wei&beta, R, Gritsch S, Brader G, Nikolic B, Spiller M, Santolin J, Weber HK, Schwaiger N, Pluchon S, Dietel K, Guebitz G, Nyanhongo G, Green Chemistry 23, 6501 (2021). http://doi.org/10.1039/D1GC02221K
Abstract: Lignosulfonate-based bioactive coatings as soil improvers for lawns were developed using laccase as a biocatalyst. Incorporation of glycerol, xylitol and sorbitol as plasticizers considerably reduced the brittleness of the synthesized coatings of marine carbonate granules while thermal enzyme inactivation at 100 degrees C enabled the production of stable coatings. Heat inactivation produced stable coatings with a molecular weight of 2000 kDa and a viscosity of 4.5 x 10(-3) Pas. The desired plasticity for the spray coating of soil improver granules was achieved by the addition of 2.7% of xylitol. Agriculture beneficial microorganisms (four different Bacillus species) were integrated into the coatings. The stable coatings protected the marine calcium carbonate granules, maintained the viability of the microorganisms and showed no toxic effects on the germination and growth of model plants including corn, wheat, salad, and tomato despite a slight delay in germination. Moreover, the coatings reduced the dust formation of soil improvers by 70%. CO2 emission analysis showed potential for the reduction of up to 3.4 kg CO2-eq. kg(-1) product, making it a viable alternative to fossil-based coatings.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 9.125
DOI: 10.1039/D1GC02221K
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“Can post-plasma CH4injection improve plasma-based dry reforming of methane? A modeling study”. Albrechts M, Tsonev I, Bogaerts A, Green Chemistry 26, 9712 (2024). http://doi.org/10.1039/D4GC02889A
Abstract: Thermal plasma-driven dry reforming of methane (DRM) has gained increased attention in recent years due to its high conversion and energy conversion efficiency (ECE). Recent experimental work investigated the performance of a pure CO<sub>2</sub>plasma with post-plasma CH<sub>4</sub>injection. The rationale behind this strategy is that by utilizing a pure CO<sub>2</sub>plasma, all plasma energy can be used to dissociate CO<sub>2</sub>, while CH<sub>4</sub>reforming proceeds post-plasma in the reforming reactor with residual heat, potentially improving the energy efficiency compared to injecting both CO<sub>2</sub>and CH<sub>4</sub>into the plasma. To assess whether post-plasma CH<sub>4</sub>injection indeed improves the DRM performance, we developed a chemical kinetics model describing the post-plasma conversion process. We first validated our model by reproducing the experimental results of the pure CO<sub>2</sub>plasma with post-plasma CH<sub>4</sub>injection. Subsequently, we compared both strategies: injecting only CO<sub>2</sub>inside the plasma while injecting CH<sub>4</sub>post-plasma,<italic>vs.</italic>classical plasma-based DRM. Our modeling results indicate that below specific energy inputs (SEI) of 220 kJ mol<sup>−1</sup>, the total conversion slightly improves (<italic>ca.</italic>5%) with the first strategy. However, the ECE is slightly lower due to the low H<sub>2</sub>selectivity caused by substantial H<sub>2</sub>O formation. The highest conversion and ECE are obtained at SEI values of 240–280 kJ mol<sup>−1</sup>, where both strategies yield nearly identical results, indicating the limited potential of improving the performance of DRM by pure CO<sub>2</sub>plasma with post-plasma CH<sub>4</sub>injection. Nevertheless, the approach is still very valuable to allow higher CH<sub>4</sub>/CO<sub>2</sub>ratios without problems of coke formation within the plasma, and thus, to improve plasma stability and reach higher syngas ratios, which is more useful for further Fischer–Tropsch or methanol synthesis.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 9.8
DOI: 10.1039/D4GC02889A
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“The role of ions in plasma catalytic carbon nanotube growth : a review”. Neyts EC, Frontiers of Chemical Science and Engineering 9, 154 (2015). http://doi.org/10.1007/s11705-015-1515-5
Abstract: While it is well-known that the plasma-enhanced catalytic chemical vapor deposition (PECVD) of carbon nanotubes (CNTs) offers a number of advantages over thermal CVD, the influence of the various individual contributing factors is not well understood. Especially the role of ions is unclear, since ions in plasmas are generally associated with sputtering rather than with growing a material. Even so, various studies have demonstrated the beneficial effects of ion bombardment during the growth of CNTs. This review looks at the role of the ions in plasma-enhanced CNT growth as deduced from both experimental and simulation studies. Specific attention is paid to the beneficial effects of ion bombardment. Based on the available literature, it can be concluded that ions can be either beneficial or detrimental for carbon nanotube growth, depending on the exact conditions and the control over the growth process.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.712
Times cited: 8
DOI: 10.1007/s11705-015-1515-5
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“Atomistic simulations of plasma catalytic processes”. Neyts EC, Frontiers of Chemical Science and Engineering 12, 145 (2018). http://doi.org/10.1007/S11705-017-1674-7
Abstract: There is currently a growing interest in the realisation and optimization of hybrid plasma/catalyst systems for a multitude of applications, ranging from nanotechnology to environmental chemistry. In spite of this interest, there is, however, a lack in fundamental understanding of the underlying processes in such systems. While a lot of experimental research is already being carried out to gain this understanding, only recently the first simulations have appeared in the literature. In this contribution, an overview is presented on atomic scale simulations of plasma catalytic processes as carried out in our group. In particular, this contribution focusses on plasma-assisted catalyzed carbon nanostructure growth, and plasma catalysis for greenhouse gas conversion. Attention is paid to what can routinely be done, and where challenges persist.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.712
Times cited: 5
DOI: 10.1007/S11705-017-1674-7
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“Plasma for cancer treatment: How can RONS penetrate through the cell membrane? Answers from computer modeling”. Bogaerts A, Yusupov M, Razzokov J, Van der Paal J, Frontiers of Chemical Science and Engineering (2019). http://doi.org/10.1007/s11705-018-1786-8
Abstract: Plasma is gaining increasing interest for cancer
treatment, but the underlying mechanisms are not yet fully
understood. Using computer simulations at the molecular
level, we try to gain better insight in how plasma-generated
reactive oxygen and nitrogen species (RONS) can
penetrate through the cell membrane. Specifically, we
compare the permeability of various (hydrophilic and
hydrophobic) RONS across both oxidized and nonoxidized cell membranes. We also study pore formation,
and how it is hampered by higher concentrations of
cholesterol in the cell membrane, and we illustrate the
much higher permeability of H2O2 through aquaporin
channels. Both mechanisms may explain the selective
cytotoxic effect of plasma towards cancer cells. Finally, we
also discuss the synergistic effect of plasma-induced
oxidation and electric fields towards pore formation.
Keywords plasma medicine, cancer treatment, computer
modelling, cell membrane, reactive oxygen and nitrogen
species
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.712
Times cited: 5
DOI: 10.1007/s11705-018-1786-8
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“Molecular dynamics simulations of initial Pd and PdO nanocluster growth in a magnetron gas aggregation source”. Brault P, Chamorro-Coral W, Chuon S, Caillard A, Bauchire J-M, Baranton S, Coutanceau C, Neyts E, Frontiers of Chemical Science and Engineering 13, 324 (2019). http://doi.org/10.1007/S11705-019-1792-5
Abstract: Molecular dynamics simulations are carried out for describing growth of Pd and PdO nanoclusters using the ReaxFF force field. The resulting nanocluster structures are successfully compared to those of nanoclusters experimentally grown in a gas aggregation source. The PdO structure is quasi-crystalline as revealed by high resolution transmission microscope analysis for experimental PdO nanoclusters. The role of the nanocluster temperature in the molecular dynamics simulated growth is highlighted.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.712
Times cited: 3
DOI: 10.1007/S11705-019-1792-5
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“Special Issue on future directions in plasma nanoscience”. Neyts EC, Frontiers of Chemical Science and Engineering 13, 199 (2019). http://doi.org/10.1007/S11705-019-1843-Y
Keywords: Editorial; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.712
DOI: 10.1007/S11705-019-1843-Y
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“Probing oxygen activation on plasmonic photocatalysts”. Dingenen F, Borah R, Ninakanti R, Verbruggen SW, Frontiers in Chemistry 10, 988542 (2022). http://doi.org/10.3389/FCHEM.2022.988542
Abstract: In this work we present an assay to probe the oxygen activation rate on plasmonic nanoparticles under visible light. Using a superoxide-specific XTT molecular probe, the oxygen activation rate on bimetallic gold-silver “rainbow” nanoparticles with a broadband visible light (> 420 nm) response, is determined at different light intensities by measuring its conversion into the colored XTT-formazan derivate. A kinetic model is applied to enable a quantitative estimation of the rate constant, and is shown to match almost perfectly with the experimental data. Next, the broadband visible light driven oxygen activation capacity of this plasmonic rainbow system, supported on nano-sized SiO 2 , is demonstrated towards the oxidation of aniline to azobenzene in DMSO. To conclude, a brief theoretical discussion is devoted to the possible mechanisms behind such plasmon-driven reactions.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 5.5
DOI: 10.3389/FCHEM.2022.988542
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“Cyclodextrin-appended superparamagnetic iron oxide nanoparticles as cholesterol-mopping agents”. Puglisi A, Bassini S, Reimhult E, Frontiers In Chemistry 9, 795598 (2021). http://doi.org/10.3389/FCHEM.2021.795598
Abstract: Cholesterol plays a crucial role in major cardiovascular and neurodegenerative diseases, including Alzheimer’s disease and rare genetic disorders showing altered cholesterol metabolism. Cyclodextrins (CDs) have shown promising therapeutic efficacy based on their capacity to sequester and mobilise cholesterol. However, the administration of monomeric CDs suffers from several drawbacks due to their lack of specificity and poor pharmacokinetics. We present core-shell superparamagnetic iron oxide nanoparticles (SPIONs) functionalised with CDs appended to poly (2-methyl-2-oxazoline) polymers grafted in a dense brush to the iron oxide core. The CD-decorated nanoparticles (CySPIONs) are designed so that the macrocycle is specifically cleaved off the nanoparticle’s shell at a slightly acidic pH. In the intended use, free monomeric CDs will then mobilise cholesterol out of the lysosome to the cytosol and beyond through the formation of an inclusion complex. Hence, its suitability as a therapeutic platform to remove cholesterol in the lysosomal compartment. Synthesis and full characterization of the polymer as well as of the core-shell SPION are presented. Cholesterol-binding activity is shown through an enzymatic assay.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 3.994
DOI: 10.3389/FCHEM.2021.795598
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“Electrochemical fingerprints of illicit drugs on graphene and multi-walled carbon nanotubes”. Dragan A-M, Truta FM, Tertis M, Florea A, Schram J, Cernat A, Feier B, De Wael K, Cristea C, Oprean R, Frontiers In Chemistry 9, 641147 (2021). http://doi.org/10.3389/FCHEM.2021.641147
Abstract: Illicit drugs use and abuse remains an increasing challenge for worldwide authorities and, therefore, it is important to have accurate methods to detect them in seized samples, biological fluids and wastewaters. They are recently classified as the latest group of emerging pollutants as their consumption increased tremendously in recent years. Nanomaterials have gained much attention over the last decade in the development of sensors for a myriad of applications. The applicability of these nanomaterials, functionalized or not, significantly increases and it is therefore highly suitable for use in the detection of illicit drugs. We have assessed the suitability of various nanoplatforms, such as graphene (GPH), multi-walled carbon nanotubes (MWCNTs), gold nanoparticles (AuNPs) and platinum nanoparticles (PtNPs) for the electrochemical detection of illicit drugs. GPH and MWCNTs were chosen as the most suitable platforms and cocaine, 3,4-methylendioxymethamfetamine (MDMA), 3-methylmethcathinone (MMC) and alpha-pyrrolidinovalerophenone (PVP) were tested. Due to the hydrophobicity of the nanomaterials-based platforms which led to low signals, two strategies were followed namely, pretreatment of the electrodes in sulfuric acid by cyclic voltammetry and addition of Tween 20 to the detection buffer. Both strategies led to an increase in the oxidation signal of illicit drugs. Binary mixtures of illicit drugs with common adulterants found in street samples were also investigated. The proposed strategies allowed the sensitive detection of illicit drugs in the presence of most adulterants. The suitability of the proposed sensors for the detection of illicit drugs in spiked wastewaters was finally assessed.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 3.994
DOI: 10.3389/FCHEM.2021.641147
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“Tackling the problem of sensing commonly abused drugs through nanomaterials and (bio)recognition approaches”. Truta F, Florea A, Cernat A, Tertis M, Hosu O, De Wael K, Cristea C, Frontiers In Chemistry 8, 561638 (2020). http://doi.org/10.3389/FCHEM.2020.561638
Abstract: We summarize herein the literature in the last decade, involving the use of nanomaterials and various (bio)recognition elements, such as antibodies, aptamers and molecularly imprinted polymers, for the development of sensitive and selective (bio)sensors for illicit drugs with a focus on electrochemical transduction systems. The use and abuse of illicit drugs remains an increasing challenge for worldwide authorities and, therefore, it is important to have accurate methods to detect them in seized samples, biological fluids and wastewaters. They are recently classified as the latest group of “emerging pollutants,” as their consumption has increased tremendously in recent years. Nanomaterials, antibodies, aptamers and molecularly imprinted polymers have gained much attention over the last decade in the development of (bio)sensors for a myriad of applications. The applicability of these (nano)materials, functionalized or not, has significantly increased, and are therefore highly suitable for use in the detection of drugs. Lately, such functionalized nanoscale materials have assisted in the detection of illicit drugs fingerprints, providing large surface area, functional groups and unique properties that facilitate sensitive and selective sensing. The review discusses the types of commonly abused drugs and their toxicological implications, classification of functionalized nanomaterials (graphene, carbon nanotubes), their fabrication, and their application on real samples in different fields of forensic science. Biosensors for drugs of abuse from the last decade's literature are then exemplified. It also offers insights into the prospects and challenges of bringing the functionalized nanobased technology to the end user in the laboratories or in-field.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 5.5
DOI: 10.3389/FCHEM.2020.561638
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“Analysis of geothermal waters by spark source mass spectrometry”. Vandelannoote R, Blommaert W, Gijbels R, van Grieken R, Fresenius' Zeitschrift für analytische Chemie 309, 291 (1981). http://doi.org/10.1007/BF00488604
Abstract: Although the analysis of thermal water by spark-source mass spectrometry (SSMS) is rather timeconsuming, it allows the detection of about 20 elements of geochemical interest down to the ppb-level. A physical preconcentration is proposed in order to collect elements having quite different chemical properties, e.g. alkalis, transition elements, and elements occurring in anionic form. The relative sensitivity factors appear to be rather independent of the salt content of the graphite electrodes. Contrary to neutron activation analysis, SSMS has a quite uniform elemental sensitivity, and allows to determine elements for which neutron activation is not suitable, e.g. Sn and Pb. The precision of SSMS is however by a factor of about 2 worse than that obtained for neutron activation.
Keywords: A3 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Times cited: 8
DOI: 10.1007/BF00488604
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“2,2′-Diaminodiethylamine cellulose powder for trace metal preconcentrations from water”. Reggers C, Van Grieken R, Fresenius' Zeitschrift für analytische Chemie 317, 520 (1984). http://doi.org/10.1007/BF00511918
Abstract: Cellulose powder with 2,2′-diaminodiethylamine (DEN) functional groups exhibits efficient complexation of transition metal cations. Collection yields above 85 % are obtained up to a chelation capacity of 1.5 meq per gram. Since a good collection is obtained for a pH up from 5, no pH adjustments have to be made for natural water samples. The cellulose-DEN powder is insensitive to abundant substances like alkali and alkaline earth ions, and humic matter. Some cations can be eluted efficiently in a small volume of HNO3. Blank concentration levels from the cellulose-DEN powder are reported.
Keywords: A3 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
DOI: 10.1007/BF00511918
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“Energy-dispersive X-ray spectrometry : present state and trends”. Van Grieken R, Markowicz A, Török S, Fresenius' Zeitschrift für analytische Chemie 324, 825 (1986). http://doi.org/10.1007/BF00473177
Abstract: Recent development, present state and expected future developments in energy-dispersive X-ray spectrometry are discussed. Attention is paid to the improvements in analytical selectivity, sensitivity, detection limit, quantitative character and applicability range, which are the result of new or better excitation sources, detectors, instrument design, automation, computer software and theoretical developments.
Keywords: A3 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
DOI: 10.1007/BF00473177
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