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Author | Liu, Y.; Ngo, H.H.; Guo, W.; Zhou, J.; Peng, L.; Wang, D.; Chen, X.; Sun, J.; Ni, B.-J. | ||||
Title | Optimizing sulfur-driven mixotrophic denitrification process : system performance and nitrous oxide emission | Type | A1 Journal article | ||
Year | 2017 | Publication | Chemical engineering science | Abbreviated Journal | |
Volume | 172 | Issue | Pages | 414-422 | |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | Nitrate contamination of groundwater has been recognized as a significant environmental problem world widely. Sulfur-driven mixotrophic denitrification has been demonstrated as a promising groundwater treatment process, which though plays an important role in nitrous oxide (N2O) emissions, significantly contributing to the overall carbon footprint of the system. However, the current process optimizations only focus on nitrate removal and excess sulfate control, with the N2O emission being ignored. In this work, an integrated mathematical model was proposed to evaluate the N2O emission as well as the excess sulfate production and carbon source utilization in sulfur-driven mixotrophic denitrification process. In this model, autotrophic and heterotrophic denitrifiers use their corresponding electron donors (sulfur and organic matter, respectively) to reduce nitrate to nitrogen gas, with each modeled as three-step denitrification (NO3 to N-2 via NO2 and N2O) driven by sulfur or organic matter to describe all potential N2O accumulation steps. The developed model, employing model parameters previously reported in literature, was successfully validated using N2O and sulfate data from two mixotrophic denitrification systems with different initial conditions. Modeling results revealed substantial N2O accumulation due to the relatively low autotrophic N2O reduction activity as compared to heterotrophic N2O reduction activity, explaining the observation that higher carbon source addition resulted in lower N2O accumulation in sulfur-driven mixotrophic denitrifying system. Based on the validated model, optimizations of the overall system performance were carried out. Application of the model to simulate long-term operations of sulfur-driven mixotrophic denitrification process indicates that longer sludge retention time reduces N2O emission due to better retention of active biomass. High-level total nitrogen removal with significant N2O emission mitigation, appropriate excess sulfate control and maximized COD utilization can be achieved simultaneously through controlling the influent nitrate and COD concentrations. (C) 2017 Elsevier Ltd. All rights reserved. | ||||
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Language | Wos | 000410833900034 | Publication Date | 2017-07-03 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 0009-2509 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:146634 | Serial | 8344 | ||
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Author | Desmet, N.J.S.; van Belleghem, S.; Seuntjens, P.; Bouma, T.J.; Buis, K.; Meire, P. | ||||
Title | Quantification of the impact of macrophytes on oxygen dynamics and nitrogen retention in a vegetated lowland river | Type | A1 Journal article | ||
Year | 2011 | Publication | Physics and chemistry of the earth, parts A/B/C | Abbreviated Journal | |
Volume | 36 | Issue | 12 | Pages | 479-489 |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | When macrophytes are growing in the river, the vegetation induces substantial changes to the water quality. Some effects are the result of direct interactions, such as photosynthetic activity or nutrient uptake, whereas others may be attributed to indirect effects of the water plants on hydrodynamics and river processes. This research focused on the direct effect of macrophytes on oxygen dynamics and nutrient cycling. Discharge, macrophyte biomass density, basic water quality, dissolved oxygen and nutrient concentrations were in situ monitored throughout the year in a lowland river (Nete catchment, Belgium). In addition, various processes were investigated in more detail in multiple ex situ experiments. The field and aquaria measurement results clearly demonstrated that aquatic plants can exert considerable impact on dissolved oxygen dynamics in a lowland river. When the river was dominated by macrophytes, dissolved oxygen concentrations varied from 5 to 10 mg l−1. Considering nutrient retention, it was shown that the investigated in-stream macrophytes could take up dissolved inorganic nitrogen (DIN) from the water column at rates of View the MathML source. And DIN fluxes towards the vegetation were found to vary from 0.03 to 0.19 g N ha−1 h−1 in spring and summer. Compared to the measured changes in DIN load over the river stretch, it means that about 313% of the DIN retention could be attributed to direct nitrogen uptake from the water by macrophytes. Yet, the role of macrophytes in rivers should not be underrated as aquatic vegetation also exerts considerable indirect effects that may have a greater impact than the direct fixation of nutrients into the plant biomass. | ||||
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Language | Wos | 000295862600001 | Publication Date | 2008-06-15 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1474-7065 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:92439 | Serial | 8436 | ||
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Author | Zankowski, S.P.; Van Hoecke, L.; Mattelaer, F.; de Raedt, M.; Richard, O.; Detavernier, C.; Vereecken, P.M. | ||||
Title | Redox layer deposition of thin films of MnO2 on nanostructured substrates from aqueous solutions | Type | A1 Journal article | ||
Year | 2019 | Publication | Chemistry of materials | Abbreviated Journal | |
Volume | 31 | Issue | 13 | Pages | 4805-4816 |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | In this work, we report a new method for depositing thin films of MnO2 on planar and complex nanostructured surfaces, with high precision and conformality. The method is based on repeating cycles of adsorption of an unsaturated alcohol on a surface, followed by its oxidation with aqueous KMnO4 and formation of thin, solid MnO2. The amount of manganese oxide formed in each cycle is limited by the quantity of the adsorbed alcohol; thus, the growth exhibits the self-limiting characteristics of atomic layer deposition (ALD). Contrary to the typical ALD, however, the new redox layer deposition is performed in air, at room temperature, using common chemicals and simple laboratory glassware, which greatly reduces its cost and complexity. We also demonstrate application of the method for the fabrication of a nanostructured MnO2/Ni electrode, which was not possible with thermal ALD because of the rapid decomposition of the gaseous precursor on the high surface-area substrate. Thanks to its simplicity, the conformal deposition of MnO2 can be easily upscaled and thus exploited for its numerous (electro)chemical applications. | ||||
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Language | Wos | 000475408400021 | Publication Date | 2019-06-12 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:161225 | Serial | 8465 | ||
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Author | Haest, P.J.; Springael, D.; Seuntjens, P.; Smolders, E. | ||||
Title | Self-inhibition can limit biologically enhanced TCE dissolution from a TCE DNAPL | Type | A1 Journal article | ||
Year | 2012 | Publication | Chemosphere | Abbreviated Journal | |
Volume | 89 | Issue | 11 | Pages | 1369-1375 |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | Biodegradation of trichloroethene (TCE) near a Dense Non Aqueous Phase Liquid (DNAPL) can enhance the dissolution rate of the DNAPL by increasing the concentration gradient at the DNAPL-water interface. Two-dimensional flow-through sand boxes containing a ICE DNAPL and inoculated with a TCE dechlorinating consortium were set up to measure this bio-enhanced dissolution under anaerobic conditions. The total mass of TCE and daughter products in the effluent of the biotic boxes was 3-6 fold larger than in the effluent of the abiotic box. However, the mass of daughter products only accounted for 19-55% of the total mass of chlorinated compounds in the effluent, suggesting that bio-enhanced dissolution factors were maximally 1.3-2.2. The enhanced dissolution most likely primarily resulted from variable DNAPL distribution rather than biodegradation. Specific dechlorination rates previously determined in a stirred liquid medium were used in a reactive transport model to identify the rate limiting factors. The model adequately simulated the overall TCE degradation when predicted resident microbial numbers approached observed values and indicated an enhancement factor for TCE dissolution of 1.01. The model shows that dechlorination of TCE in the 20 box was limited due to the short residence time and the self-inhibition of the TCE degradation. A parameter sensitivity analysis predicts that the bio-enhanced dissolution factor for this TCE source zone can only exceed a value of 2 if the TCE self-inhibition is drastically reduced (when a TCE tolerant dehalogenating community is present) or if the DNAPL is located in a low-permeable layer with a small Darcy velocity. (C) 2012 Elsevier Ltd. All rights reserved. | ||||
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Language | Wos | 000310112600015 | Publication Date | 2012-06-30 | |
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ISSN | 0045-6535; 1879-1298 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:102142 | Serial | 8512 | ||
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Author | Chen, Y.; Wu, Y.; Wang, D.; Li, H.; Wang, Q.; Liu, Y.; Peng, L.; Yang, Q.; Li, X.; Zeng, G.; Chen, Y. | ||||
Title | Understanding the mechanisms of how poly aluminium chloride inhibits short-chain fatty acids production from anaerobic fermentation of waste activated sludge | Type | A1 Journal article | ||
Year | 2018 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 334 | Issue | Pages | 1351-1360 | |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | Poly aluminum chloride (PAC) is accumulated in waste activated sludge at high levels. However, details of how PAC affects short-chain fatty acids (SCFA) production from anaerobic sludge fermentation has not been documented. This work therefore aims to fill this knowledge gap by analyzing the impact of PAC on the aggregate of sludge flocs, disruption of extracellular polymeric substances (EPS), and the bio-processes of hydrolysis, acid-ogenesis, and methanogenesis. The relationship between SCFA production and different aluminum species (i.e., Ala, Alb, and Alc) was also identified by controlling different OH/Al ratio and pH in different fermentation systems. Experimental results showed that with the increase of PAC addition from 0 to 40 mg Al per gram of total suspended solids, SCFA yield decreased from 212.2 to 138.4 mg COD/g volatile suspended solids. Mechanism exploration revealed that PAC benefited the aggregates of sludge flocs and caused more loosely-and tightly-bound extracellular polymeric substances remained in sludge cells. Besides, it was found that the hydrolysis, acidiogenesis, and methanogenesis processes were all inhibited by PAC. Although three types of Al species, i.e., Ala (Al monomers, dimer, and trimer), Alb (Al-13(AlO4Al12(OH)(24)(H2O) 7+ 12), and Alc (Al polymer molecular weight normally larger than 3000 Da), were co-existed in fermentation systems, their impacts on SCFA production were different. No correlation was found between SCFA and Ala, whereas SCFA production decreased with the contents of Alb and Alc. Compared with Alb, Alc was the major contributor to the decreased SCFA production ( R-2 = 0.5132 vs R-2 = 0.98). This is the first report revealing the underlying mechanism of how PAC affects SCFA production and identifying the contribution of different Al species to SCFA inhibition. | ||||
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Language | Wos | 000418533400135 | Publication Date | 2017-11-13 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947; 1873-3212 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:148413 | Serial | 8708 | ||
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Author | Scandura, G.; Kumari, P.; Palmisano, G.; Karanikolos, G.N.; Orwa, J.; Dumee, L.F. | ||||
Title | Nanoporous Dealloyed Metal Materials Processing and Applications?A Review | Type | A1 Journal article | ||
Year | 2023 | Publication | Industrial and engineering chemistry research | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | The development of porous metal materials with pore geometries and sizes at the nanoscale offers promising opportunities for the development of smart responsive interfaces for separation and catalytic applications and as building blocks for complex composite materials. Dealloying is an innovative technique based on selective removal of a sacrificial metal from a metal alloy to engineer surface textures and pores across significant thicknesses. Dealloyed structures may be processed over large scales and for a range of source alloys, offering unprecedented manufacturing opportunities. This review presents the operations and challenges of dealloying routes and discusses avenues for process optimizations and improvements, aiming at the development of scalable nanoporous materials. The potential of dealloyed materials for catalytic and sensing applications is expanded and benchmarked against reference materials. Future prospects and applications of dealloyed materials toward surface reactivity control and pore architecture development are highlighted. | ||||
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Language | Wos | 000918107700001 | Publication Date | 2023-01-13 | |
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ISSN | 0888-5885; 1520-5045 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.2 | Times cited | Open Access | Not_Open_Access | |
Notes | Approved | Most recent IF: 4.2; 2023 IF: 2.843 | |||
Call Number | UA @ admin @ c:irua:199419 | Serial | 8904 | ||
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Author | Vingerhoets, R.; Brienza, C.; Sigurnjak, I.; Buysse, J.; Vlaeminck, S.E.; Spiller, M.; Meers, E. | ||||
Title | Ammonia stripping and scrubbing followed by nitrification and denitrification saves costs for manure treatment based on a calibrated model approach | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 477 | Issue | Pages | 146984-14 | |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | Resource-efficient nitrogen management is of high environmental and economic interest, and manure represents the major nutrient flow in livestock-intensive regions. Ammonia stripping/scrubbing (SS) is an appealing nitrogen recovery route from manure, yet its real-life implementation has been limited thus far. In nutrient surplus regions like Flanders, treatment of the liquid fraction (LF) of (co–)digested manure typically consists of nitrification/denitrification (NDN) removing most N as nitrogen gas. Integrating SS before NDN in existing plants would expand treatment capacity and recover N while maintaining low N effluent values, yet cost estimations of this novel approach after process optimisation are not yet available. A programming model was developed and calibrated to minimise the treatment costs of this approach and find the balance between N recovery versus N removal. Four crucial operational parameters (CO2 stripping time, NH3 stripping time, temperature and NaOH addition) were optimised for 18 scenarios which were different in terms of technical set-up, influent characteristics and scrubber acid. The model shows that SS before NDN can decrease the costs by 1 to 56% under optimal conditions compared to treatment with NDN only, with 1 to 8% reduction for the LF of manure (22–29% recovered of N treated), and 11 to 56% reduction for the LF of co-digested manure (42–67% recovered of N treated), primarily dependent on resource pricing. This study shows the power of modelling for minimum-cost design and operation of manure treatment yielding savings while producing useful N recovery products with SS followed by NDN. | ||||
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Language | Wos | 001108935900001 | Publication Date | 2023-10-28 | |
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ISSN | 1385-8947; 1873-3212 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | |||
Call Number | UA @ admin @ c:irua:200649 | Serial | 9003 | ||
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Author | Maerivoet, S.; Wanten, B.; De Meyer, R.; Van Hove, M.; Van Alphen, S.; Bogaerts, A. | ||||
Title | Effect of O2on Plasma-Based Dry Reforming of Methane: Revealing the Optimal Gas Composition via Experiments and Modeling of an Atmospheric Pressure Glow Discharge | Type | A1 Journal Article | ||
Year | 2024 | Publication | ACS Sustainable Chemistry & Engineering | Abbreviated Journal | ACS Sustainable Chem. Eng. |
Volume | 12 | Issue | 30 | Pages | 11419-11434 |
Keywords | A1 Journal Article; plasma-based conversion, thermal plasma, syngas production, CO2 conversion, CH4 conversio; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma technology is gaining increasing interest for the conversion of greenhouse gases, such as CO2 and CH4, into value-added chemicals using (renewable) electricity. In this paper, we study the effect of O2 addition to the combined conversion of CO2 and CH4 in an atmospheric pressure glow discharge plasma. This process is called “oxidative CO2 reforming of methane”, and we search for the optimal gas mixing ratio in terms of conversion, energy cost, product output and plasma stability. A mixing ratio of 42.5:42.5:15 CO2/CH4/O2 yields the best performance, with a CO2 and CH4 conversion of 50 and 74%, respectively, and an energy cost as low as 2 eV molecule−1 (corresponding to 7.9 kJ L−1 and 190 kJ mol−1), i.e., clearly below the target defined to be competitive with other technologies. The syngas components (CO and H2) are the most important products, with a syngas ratio, H2/CO, being 0.8. Plasma destabilization at high CH4 fractions due to solid carbon formation is the limiting factor for further improving this syngas ratio. The solid carbon material is found to be contaminated with steel particles originating from the electrode material, rendering it unappealing as a side product. Therefore, O2 addition helps to remove the carbon formation. Besides the experiments, we developed a 2D axisymmetric fluid dynamics model, which can successfully predict the experimental trends in conversion, product composition and temperatures, while providing unique insights in the formation of CxHy species. | ||||
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Language | Wos | https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001280 | Publication Date | 2024-07-29 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.4 | Times cited | Open Access | ||
Notes | Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 40007511 G0I1822N ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2024 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:207488 | Serial | 9257 | ||
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Author | Wang, K.; Ceulemans, S.; Zhang, H.; Tsonev, I.; Zhang, Y.; Long, Y.; Fang, M.; Li, X.; Yan, J.; Bogaerts, A. | ||||
Title | Inhibiting recombination to improve the performance of plasma-based CO2 conversion | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 481 | Issue | Pages | 148684 | |
Keywords | A1 Journal Article; Plasma-based CO2 splitting Recombination reactions In-situ gas sampling Fluid dynamics modeling Kinetics modeling Afterglow quenching; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Warm plasma offers a promising route for CO2 splitting into valuable CO, yet recombination reactions of CO with oxygen, forming again CO2, have recently emerged as critical limitation. This study combines experiments and fluid dynamics + chemical kinetics modelling to comprehensively analyse the recombination reactions upon CO2 splitting in an atmospheric plasmatron. We introduce an innovative in-situ gas sampling technique, enabling 2D spatial mapping of gas product compositions and temperatures, experimentally confirming for the first time the substantial limiting effect of CO recombination reactions in the afterglow region. Our results show that the CO mole fraction at a 5 L/min flow rate drops significantly from 11.9 % at a vertical distance of z = 20 mm in the afterglow region to 8.6 % at z = 40 mm. We constructed a comprehensive 2D model that allows for spatial reaction rates analysis incorporating crucial reactions, and we validated it to kinetically elucidate this phenomenon. CO2 +M⇌O+CO+M and CO2 +O⇌CO+O2 are the dominant reactions, with the forward reactions prevailing in the plasma region and the backward reactions becoming prominent in the afterglow region. These results allow us to propose an afterglow quenching strategy for performance enhancement, which is further demonstrated through a meticulously developed plasmatron reactor with two-stage cooling. Our approach substantially increases the CO2 conversion (e.g., from 6.6 % to 19.5 % at 3 L/min flow rate) and energy efficiency (from 13.5 % to 28.5 %, again at 3 L/min) and significantly shortens the startup time (from ~ 150 s to 25 s). Our study underscores the critical role of inhibiting recombination reactions in plasma-based CO2 conversion and offers new avenues for performance enhancement. | ||||
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Language | Wos | 001168999200001 | Publication Date | 2024-01-10 | |
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ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 15.1 | Times cited | Open Access | Not_Open_Access | |
Notes | Key Research and Development Program of Zhejiang Province, 2023C03129 ; Vlaamse regering; European Research Council; National Natural Science Foundation of China, 51976191 52276214 ; Horizon 2020 Framework Programme; Fonds De La Recherche Scientifique – FNRS; Fonds Wetenschappelijk Onderzoek, 1101524N ; Vlaams Supercomputer Centrum; Horizon 2020, 101081162 810182 ; European Research Council; | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:204352 | Serial | 8993 | ||
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Author | Fedirchyk, I.; Tsonev, I.; Quiroz Marnef, R.; Bogaerts, A. | ||||
Title | Plasma-assisted NH3 cracking in warm plasma reactors for green H2 production | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 499 | Issue | Pages | 155946 | |
Keywords | A1 Journal Article; Plasma-assisted NH3 cracking Plasma reactors Warm plasma H2 production from NH3; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | renewable energy. Plasma technology is promising for this purpose, as it can crack NH3 without the need for a catalyst and is highly compatible with renewable electricity, reducing the environmental footprint of the cracking process. This work investigates the NH3 cracking performance of four different warm plasma reactors with different configurations and operating in a wide range of conditions. We show that the NH3 conversion in warm plasma reactors is primarily determined by the specific energy input, with the main difference observed in the energy cost (EC) of cracking. The lowest EC obtained is 146 kJ/mol but at a conversion of only 8 %. A more reasonable conversion of around 50 % yields an EC of around 200 kJ/mol in two of the reactors investigated. Plasma reactors operating at higher feed flow rates are more efficient and yield a higher H2 production rate. Our data indicate that NH3 cracking in these warm plasma reactors occurs mainly via thermal chemistry, with nonthermal plasma chemistry playing a less prominent role. NH3 decomposes not only inside the plasma core but also in a hot volume around it, which reduces the EC. Our study shows that warm plasmas are significantly more efficient for NH3 cracking than cold plasmas, even when the latter are combined with catalysts. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-09-19 | ||
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ISSN | 1385-8947 | ISBN | Additional Links | ||
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | Belgian Federal Government; European Commission Marie Sklodowska-Curie Actions; | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9267 | ||
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Author | Wang, W.; Patil, B.; Heijkers, S.; Hessel, V.; Bogaerts, A. | ||||
Title | Nitrogen Fixation by Gliding Arc Plasma: Better Insight by Chemical Kinetics Modelling | Type | A1 Journal Article | ||
Year | 2017 | Publication | Chemsuschem | Abbreviated Journal | Chemsuschem |
Volume | 10 | Issue | 10 | Pages | 2110-2110 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
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. | ||||
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Language | Wos | Publication Date | 2017-05-11 | ||
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ISSN | 1864-5631 | ISBN | Additional Links | ||
Impact Factor | 7.226 | Times cited | Open Access | Not_Open_Access | |
Notes | This research was supported by the European Marie Skłodowska- Curie Individual Fellowship “GlidArc” within Horizon 2020 (Grant No.657304), by the FWO project (grant G.0383.16 N) and by the EU project MAPSYN: Microwave, Acoustic and Plasma assisted SYNthesis, under the grant agreement no. CP-IP 309376 of the European Community’s Seventh Framework Program. The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. | Approved | Most recent IF: 7.226 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 4573 | ||
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Author | Huygh, S.; Bogaerts, A.; Bal, K.M.; Neyts, E.C. | ||||
Title | High Coke Resistance of a TiO2Anatase (001) Catalyst Surface during Dry Reforming of Methane | Type | A1 Journal Article | ||
Year | 2018 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 122 | Issue | 17 | Pages | 9389-9396 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | The resistance of a TiO2 anatase (001) surface to coke formation was studied in the context of dry reforming of methane using density functional theory (DFT) calculations. As carbon atoms act as precursors for coke formation, the resistance to coke formation can be measured by the carbon coverage of the surface. This is related to the stability of different CHx (x = 0−3) species and their rate of hydrogenation and dehydrogenation on the TiO2 surface. Therefore, we studied the reaction mechanisms and their corresponding rates as a function of the temperature for the dehydrogenation of the species on the surface. We found that the stabilities of C and CH are significantly lower than those of CH3 and CH2. The hydrogenation rates of the different species are significantly higher than the dehydrogenation rates in a temperature range of 300−1000 K. Furthermore, we found that dehydrogenation of CH3, CH2, and CH will only occur at appreciable rates starting from 600, 900, and 900 K, respectively. On the basis of these results, it is clear that the anatase (001) surface has a high coke resistance, and it is thus not likely that the surface will become poisoned by coke during dry reforming of methane. As the rate limiting step in dry reforming is the dissociative adsorption of CH4, we studied an alternative approach to thermal catalysis. We found that the temperature threshold for dry reforming is at least 700 K. This threshold temperature may be lowered by the use of plasma-catalysis, where the appreciable rates of adsorption of plasma-generated CHx radicals result in bypassing the rate limiting step of the reaction. | ||||
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Language | Wos | 000431723700014 | Publication Date | 2018-05-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.536 | Times cited | 1 | Open Access | OpenAccess |
Notes | Federaal Wetenschapsbeleid, IAP/7 ; Fonds Wetenschappelijk Onderzoek, G.0217.14N ; Onderzoeksfonds, Universiteit Antwerpen, 32249 ; | Approved | Most recent IF: 4.536 | ||
Call Number | PLASMANT @ plasmant @c:irua:151529c:irua:152816 | Serial | 5000 | ||
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Author | Vermeiren, V.; Bogaerts, A. | ||||
Title | Supersonic Microwave Plasma: Potential and Limitations for Energy-Efficient CO2Conversion | Type | A1 Journal Article | ||
Year | 2018 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 122 | Issue | 45 | Pages | 25869-25881 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Supersonic flows provide a high thermodynamic nonequilibrium, which is crucial for energy-efficient conversion of CO 2 in microwave plasmas and are therefore of great interest. However, the effect of the flow on the chemical reactions is poorly understood. In this work, we present a combined flow and plasma chemical kinetics model of a microwave CO 2 plasma in a Laval nozzle setup. The effects of the flow field on the different dissociation and recombination mechanisms, the vibrational distribution, and the vibrational transfer mechanism are discussed. In addition, the effect of experimental parameters, like position of power deposition, outlet pressure, and specific energy input, on the CO 2 conversion and energy efficiency is examined. The short residence time of the gas in the plasma region, the shockwave, and the maximum critical heat, and thus power, that can be added to the flow to avoid thermal choking are the main obstacles to reaching high energy efficiencies. |
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000451101400016 | Publication Date | 2018-11-15 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.536 | Times cited | 5 | Open Access | Not_Open_Access |
Notes | Fonds Wetenschappelijk Onderzoek, G.0383.16N ; | Approved | Most recent IF: 4.536 | ||
Call Number | PLASMANT @ plasmant @c:irua:155412 | Serial | 5070 | ||
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Author | Gorbanev, Y.; Privat-Maldonado, A.; Bogaerts, A. | ||||
Title | Analysis of Short-Lived Reactive Species in Plasma–Air–Water Systems: The Dos and the Do Nots | Type | A1 Journal Article | ||
Year | 2018 | Publication | Analytical Chemistry | Abbreviated Journal | Anal Chem |
Volume | 90 | Issue | 22 | Pages | 13151-13158 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | This Feature addresses the analysis of the reactive species generated by nonthermal atmospheric pressure plasmas, which are widely employed in industrial and biomedical research, as well as first clinical applications. We summarize the progress in detection of plasma-generated short-lived reactive oxygen and nitrogen species in aqueous solutions, discuss the potential and limitations of various analytical methods in plasma−liquid systems, and provide an outlook on the possible future research goals in development of short-lived reactive species analysis methods for a general nonspecialist audience. |
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000451246100002 | Publication Date | 2018-11-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2700 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.32 | Times cited | 17 | Open Access | Not_Open_Access |
Notes | European Commission, 743151 ; This work was supported by the European Marie Sklodowska- Curie Individual Fellowship within Horizon2020 (“LTPAM”, Grant No. 743151). | Approved | Most recent IF: 6.32 | ||
Call Number | PLASMANT @ plasmant @c:irua:156301 | Serial | 5152 | ||
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Author | Hoffman, B.M.; Lukoyanov, D.; Yang, Z.-Y.; Dean, D.R.; Seefeldt, L.C. | ||||
Title | Mechanism of Nitrogen Fixation by Nitrogenase: The Next Stage | Type | A1 Journal Article | ||
Year | 2014 | Publication | Chemical Reviews | Abbreviated Journal | Chem. Rev. |
Volume | 114 | Issue | 8 | Pages | 4041-4062 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Ammonia is a crucial nutrient used for plant growth and as a building block in pharmaceutical and chemical industry, produced via nitrogen fixation of the ubiquitous atmospheric N2. Current industrial ammonia production relies heavily on fossil resources, but a lot of work is put into developing non-fossil based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as H source for nitrogen fixation into NH3 by non-equilibrium plasma. The highest selectivity towards NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2014-04-23 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0009-2665 | ISBN | Additional Links | ||
Impact Factor | Times cited | Open Access | |||
Notes | We would like to thank Sylvia Dewilde (Department of Biomedical Sciences) for providing analytical equipment. | Approved | no | ||
Call Number | PLASMANT @ plasmant @ | Serial | 6337 | ||
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Author | Biondo, O.; van Deursen, C.F.A.M.; Hughes, A.; van de Steeg, A.; Bongers, W.; van de Sanden, M.C.M.; van Rooij, G.; Bogaerts, A. | ||||
Title | Avoiding solid carbon deposition in plasma-based dry reforming of methane | Type | A1 Journal Article | ||
Year | 2023 | Publication | Green Chemistry | Abbreviated Journal | Green Chem. |
Volume | 25 | Issue | 24 | Pages | 10485-10497 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
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. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 001110100100001 | Publication Date | 2023-11-24 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1463-9262 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 9.8 | Times cited | Open Access | ||
Notes | Universiteit Antwerpen; Nederlandse Organisatie voor Wetenschappelijk Onderzoek; HORIZON EUROPE Marie Sklodowska-Curie Actions, 813393 ; | Approved | Most recent IF: 9.8; 2023 IF: 9.125 | ||
Call Number | PLASMANT @ plasmant @c:irua:202138 | Serial | 8978 | ||
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Author | Oliveira, M.C.; Yusupov, M.; Bogaerts, A.; Cordeiro, R.M. | ||||
Title | Lipid Oxidation: Role of Membrane Phase-Separated Domains | Type | A1 Journal Article | ||
Year | 2021 | Publication | Journal Of Chemical Information And Modeling | Abbreviated Journal | J Chem Inf Model |
Volume | 61 | Issue | 6 | Pages | 2857-2868 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Lipid oxidation is associated with several inflammatory and neurodegenerative diseases, but many questions to unravel its effects on biomembranes are still open due to the complexity of the topic. For instance, recent studies indicated that phase-separated domains can have a significant effect on membrane function. It is reported that domain interfaces are “hot spots” for pore formation, but the underlying mechanisms and the effect of oxidation-induced phase separation on membranes remain elusive. Thus, to evaluate the permeability of the membrane coexisting of liquid-ordered (Lo) and liquid-disordered (Ld) domains, we performed atomistic molecular dynamics simulations. Specifically, we studied the membrane permeability of nonoxidized or oxidized homogeneous membranes (single-phase) and at the Lo/Ld domain interfaces of heterogeneous membranes, where the Ld domain is composed of either oxidized or nonoxidized lipids. Our simulation results reveal that the addition of only 1.5% of lipid aldehyde molecules at the Lo/Ld domain interfaces of heterogeneous membranes increases the membrane permeability, whereas their addition at homogeneous membranes does not have any effect. This study is of interest for a better understanding of cancer treatment methods based on oxidative stress (causing among others lipid oxidation), such as plasma medicine and photodynamic therapy. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000669541400034 | Publication Date | 2021-06-28 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1549-9596 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.76 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, 1200219N ; Coordenação de Aperfeiçoamento de Pessoal de NÃvel Superior; We thank Universidade Federal do ABC for providing the computational resources needed for completion of this work and CAPES for the scholarship granted. M.Y. acknowledges the Flanders Research Foundation (grant 1200219N) for financial support. | Approved | Most recent IF: 3.76 | ||
Call Number | PLASMANT @ plasmant @c:irua:179766 | Serial | 6806 | ||
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Author | Loenders, B.; Michiels, R.; Bogaerts, A. | ||||
Title | Is a catalyst always beneficial in plasma catalysis? Insights from the many physical and chemical interactions | Type | A1 Journal Article | ||
Year | 2023 | Publication | Journal of Energy Chemistry | Abbreviated Journal | Journal of Energy Chemistry |
Volume | 85 | Issue | Pages | 501-533 | |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma-catalytic dry reforming of CH4 (DRM) is promising to convert the greenhouse gasses CH4 and CO2 into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products, because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex, as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, highlighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems. Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures, at which vibrational excitation can enhance the surface reactions. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2023-06-30 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2095-4956 | ISBN | Additional Links | UA library record | |
Impact Factor | 13.1 | Times cited | Open Access | Not_Open_Access | |
Notes | This research was supported by the FWO-SBO project PlasMa- CatDESIGN (FWO grant ID S001619N), the FWO fellowship of R. Michiels (FWO grant ID 1114921N), and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project). The computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. | Approved | Most recent IF: 13.1; 2023 IF: 2.594 | ||
Call Number | PLASMANT @ plasmant @c:irua:198159 | Serial | 8806 | ||
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Author | Wanten, B.; Vertongen, R.; De Meyer, R.; Bogaerts, A. | ||||
Title | Plasma-based CO2 conversion: How to correctly analyze the performance? | Type | A1 journal article | ||
Year | 2023 | Publication | Journal of Energy Chemistry | Abbreviated Journal | Journal of Energy Chemistry |
Volume | 86 | Issue | Pages | 180-196 | |
Keywords | A1 journal article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | |||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 001070885000001 | Publication Date | 2023-07-22 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2095-4956 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.1 | Times cited | Open Access | Not_Open_Access | |
Notes | We acknowledge financial support from the Fund for Scientific Research (FWO) Flanders (Grant ID 110221N), the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement No 810182 – SCOPE ERC Synergy project), and the Methusalem funding of the University of Antwerp. We acknowledge the icons from the graphical abstract made by dDara, geotatah, Spashicons and Freepik on www.flaticon.com. We also thank Stein Maerivoet, Joachim Slaets, Elizabeth Mercer, Colín Ó’Modráin, Joran Van Turnhout, Pepijn Heirman, dr. Yury Gorbanev, dr. Fanny Girard-Sahun and dr. Sean Kelly for the interesting discussions and feedback. | Approved | Most recent IF: 13.1; 2023 IF: 2.594 | ||
Call Number | PLASMANT @ plasmant @c:irua:198709 | Serial | 8816 | ||
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Author | Li, S.; Sun, J.; Gorbanev, Y.; van’t Veer, K.; Loenders, B.; Yi, Y.; Kenis, T.; Chen, Q.; Bogaerts, A. | ||||
Title | Plasma-Assisted Dry Reforming of CH4: How Small Amounts of O2Addition Can Drastically Enhance the Oxygenate Production─Experiments and Insights from Plasma Chemical Kinetics Modeling | Type | A1 Journal Article | ||
Year | 2023 | Publication | ACS Sustainable Chemistry & Engineering | Abbreviated Journal | ACS Sustainable Chem. Eng. |
Volume | 11 | Issue | 42 | Pages | 15373-15384 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma-based dry reforming of methane (DRM) into high-value-added oxygenates is an appealing approach to enable otherwise thermodynamically unfavorable chemical reactions at ambient pressure and near room temperature. However, it suffers from coke deposition due to the deep decomposition of CH4. In this work, we assess the DRM performance upon O2 addition, as well as varying temperature, CO2/CH4 ratio, discharge power, and gas residence time, for optimizing oxygenate production. By adding O2, the main products can be shifted from syngas (CO + H2) toward oxygenates. Chemical kinetics modeling shows that the improved oxygenate production is due to the increased concentration of oxygen-containing radicals, e.g., O, OH, and HO2, formed by electron impact dissociation [e + O2 → e + O + O/O(1D)] and subsequent reactions with H atoms. Our study reveals the crucial role of oxygen-coupling in DRM aimed at oxygenates, providing practical solutions to suppress carbon deposition and at the same time enhance the oxygenates production in plasma-assisted DRM. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001082603900001 | Publication Date | 2023-10-23 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | Open Access | Not_Open_Access | |
Notes | Fonds Wetenschappelijk Onderzoek, S001619N ; China Scholarship Council, 202006060029 ; National Natural Science Foundation of China, 21975018 ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:201013 | Serial | 8966 | ||
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Author | Bogaerts, A. | ||||
Title | Special Issue on “Dielectric Barrier Discharges and their Applications” in Commemoration of the 20th Anniversary of Dr. Ulrich Kogelschatz’s Work | Type | A1 Journal Article | ||
Year | 2023 | Publication | Plasma Chemistry and Plasma Processing | Abbreviated Journal | Plasma Chem Plasma Process |
Volume | 43 | Issue | 6 | Pages | 1281-1285 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | n/a | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 001110371000001 | Publication Date | 2023-11-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0272-4324 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 3.6 | Times cited | Open Access | Not_Open_Access | |
Notes | n/a | Approved | Most recent IF: 3.6; 2023 IF: 2.355 | ||
Call Number | PLASMANT @ plasmant @c:irua:201387 | Serial | 8969 | ||
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Author | Gerrits, N.; Jackson, B.; Bogaerts, A. | ||||
Title | Accurate Reaction Probabilities for Translational Energies on Both Sides of the Barrier of Dissociative Chemisorption on Metal Surfaces | Type | A1 Journal Article | ||
Year | 2024 | Publication | The Journal of Physical Chemistry Letters | Abbreviated Journal | J. Phys. Chem. Lett. |
Volume | 15 | Issue | 9 | Pages | 2566-2572 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Molecular dynamics simulations are essential for a better understanding of dissociative chemisorption on metal surfaces, which is often the rate-controlling step in heterogeneous and plasma catalysis. The workhorse quasi-classical trajectory approach ubiquitous in molecular dynamics is able to accurately predict reactivity only for high translational and low vibrational energies. In contrast, catalytically relevant conditions generally involve low translational and elevated vibrational energies. Existing quantum dynamics approaches are intractable or approximate as a result of the large number of degrees of freedom present in molecule−metal surface reactions. Here, we extend a ring polymer molecular dynamics approach to fully include, for the first time, the degrees of freedom of a moving metal surface. With this approach, experimental sticking probabilities for the dissociative chemisorption of methane on Pt(111) are reproduced for a large range of translational and vibrational energies by including nuclear quantum effects and employing full-dimensional simulations. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001177959900001 | Publication Date | 2024-03-07 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1948-7185 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 5.7 | Times cited | Open Access | ||
Notes | Nick Gerrits has been financially supported through a Dutch Research Council (NWO) Rubicon grant (019.202EN.012). The computational resources and services used in this work were provided by the high performance computing (HPC) core facility CalcUA of the Universiteit Antwerpen and the Flemish Supercomputer Center (VSC) funded by the Research Foundation−Flanders (FWO) and the Flemish Government. The authors thank Mark Somers for useful discussions. | Approved | Most recent IF: 5.7; 2024 IF: 9.353 | ||
Call Number | PLASMANT @ plasmant @c:irua:204818 | Serial | 9114 | ||
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Author | Maerivoet, S.; Tsonev, I.; Slaets, J.; Reniers, F.; Bogaerts, A. | ||||
Title | Coupled multi-dimensional modelling of warm plasmas: Application and validation for an atmospheric pressure glow discharge in CO2/CH4/O2 | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 492 | Issue | Pages | 152006 | |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | To support experimental research into gas conversion by warm plasmas, models should be developed to explain the experimental observations. These models need to describe all physical and chemical plasma properties in a coupled way. In this paper, we present a modelling approach to solve the complete set of assumed relevant equations, including gas flow, heat balance and species transport, coupled with a rather extensive chemistry set, consisting of 21 species, obtained by reduction of a more detailed chemistry set, consisting of 41 species. We apply this model to study the combined CO2 and CH4 conversion in the presence of O2, in a direct current atmospheric pressure glow discharge. Our model can predict the experimental trends, and can explain why higher O2 fractions result in higher CH4 conversion, namely due to the higher gas temperature, rather than just by additional chemical reactions. Indeed, our model predicts that when more O2 is added, the energy required to reach any set temperature (i.e., the enthalpy) drops, allowing the system to reach higher temperatures with similar amounts of energy. This is in turn related to the higher H2O fraction and lower H2 fraction formed in the plasma, as demonstrated by our model. Altogether, our new self-consistent model can capture the main physics and chemistry occurring in this warm plasma, which is an important step towards predictive modelling for plasma-based gas conversion. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-05-09 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | ||
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID G0I1822N; EOS ID 40007511) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 810182–SCOPE ERC Synergy project, and grant agreement No. 101081162–PREPARE ERC Proof of Concept project). computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9132 | ||
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Author | Cai, Y.; Michiels, R.; De Luca, F.; Neyts, E.; Tu, X.; Bogaerts, A.; Gerrits, N. | ||||
Title | Improving Molecule–Metal Surface Reaction Networks Using the Meta-Generalized Gradient Approximation: CO2Hydrogenation | Type | A1 Journal Article | ||
Year | 2024 | Publication | The Journal of Physical Chemistry C | Abbreviated Journal | J. Phys. Chem. C |
Volume | 128 | Issue | 21 | Pages | 8611-8620 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Density functional theory is widely used to gain insights into molecule−metal surface reaction networks, which is important for a better understanding of catalysis. However, it is well-known that generalized gradient approximation (GGA) density functionals (DFs), most often used for the study of reaction networks, struggle to correctly describe both gas-phase molecules and metal surfaces. Also, GGA DFs typically underestimate reaction barriers due to an underestimation of the selfinteraction energy. Screened hybrid GGA DFs have been shown to reduce this problem but are currently intractable for wide usage. In this work, we use a more affordable meta-GGA (mGGA) DF in combination with a nonlocal correlation DF for the first time to study and gain new insights into a catalytically important surface reaction network, namely, CO2 hydrogenation on Cu. We show that the mGGA DF used, namely, rMS-RPBEl-rVV10, outperforms typical GGA DFs by providing similar or better predictions for metals and molecules, as well as molecule−metal surface adsorption and activation energies. Hence, it is a better choice for constructing molecule−metal surface reaction networks. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-05-30 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1932-7447 | ISBN | Additional Links | ||
Impact Factor | 3.7 | Times cited | Open Access | ||
Notes | H2020 Marie Sklodowska-Curie Actions, 813393 ; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 019.202EN.012 ; | Approved | Most recent IF: 3.7; 2024 IF: 4.536 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9248 | ||
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Author | Michiels, R.; Gerrits, N.; Neyts, E.; Bogaerts, A. | ||||
Title | Plasma Catalysis Modeling: How Ideal Is Atomic Hydrogen for Eley–Rideal? | Type | A1 Journal Article | ||
Year | 2024 | Publication | The Journal of Physical Chemistry C | Abbreviated Journal | J. Phys. Chem. C |
Volume | 128 | Issue | 27 | Pages | 11196-11209 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma catalysis is an emerging technology, but a lot of questions about the underlying surface mechanisms remain unanswered. One of these questions is how important Eley−Rideal (ER) reactions are, next to Langmuir−Hinshelwood reactions. Most plasma catalysis kinetic models predict ER reactions to be important and sometimes even vital for the surface chemistry. In this work, we take a critical look at how ER reactions involving H radicals are incorporated in kinetic models describing CO2 hydrogenation and NH3 synthesis. To this end, we construct potential energy surface (PES) intersections, similar to elbow plots constructed for dissociative chemisorption. The results of the PES intersections are in agreement with ab initio molecular dynamics (AIMD) findings in literature while being computationally much cheaper. We find that, for the reactions studied here, adsorption is more probable than a reaction via the hot atom (HA) mechanism, which in turn is more probable than a reaction via the ER mechanism. We also conclude that kinetic models of plasma-catalytic systems tend to overestimate the importance if ER reactions. Furthermore, as opposed to what is often assumed in kinetic models, the choice of catalyst will influence the ER reaction probability. Overall, the description of ER reactions is too much “ideal” in models. Based on our indings, we make a number of recommendations on how to incorporate ER reactions in kinetic models to avoid overestimation of their importance. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-07-11 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1932-7447 | ISBN | Additional Links | ||
Impact Factor | 3.7 | Times cited | Open Access | ||
Notes | Fonds Wetenschappelijk Onderzoek, 1114921N ; Horizon 2020 Framework Programme, 810182 ; | Approved | Most recent IF: 3.7; 2024 IF: 4.536 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9251 | ||
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Author | Albrechts, M.; Tsonev, I.; Bogaerts, A. | ||||
Title | Can post-plasma CH4injection improve plasma-based dry reforming of methane? A modeling study | Type | A1 Journal Article | ||
Year | 2024 | Publication | Green Chemistry | Abbreviated Journal | Green Chem. |
Volume | 26 | Issue | 18 | Pages | 9712-9728 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
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. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-08-24 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1463-9262 | ISBN | Additional Links | ||
Impact Factor | 9.8 | Times cited | Open Access | ||
Notes | HORIZON EUROPE Framework Programme, 101069491 ; | Approved | Most recent IF: 9.8; 2024 IF: 9.125 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9265 | ||
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Author | Vertongen, R.; De Felice, G.; van den Bogaard, H.; Gallucci, F.; Bogaerts, A.; Li, S. | ||||
Title | Sorption-Enhanced Dry Reforming of Methane in a DBD Plasma Reactor for Single-Stage Carbon Capture and Utilization | Type | A1 Journal Article | ||
Year | 2024 | Publication | ACS Sustainable Chemistry & Engineering | Abbreviated Journal | ACS Sustainable Chem. Eng. |
Volume | 12 | Issue | 29 | Pages | 10841-10853 |
Keywords | A1 Journal Article; plasma, dry reforming of methane, dielectric barrier discharge, sorbent, carbon capture and utilization, zeolite; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma−sorbent systems are a novel technology for single-stage carbon capture and utilization (CCU), where the plasma enables the desorption of CO2 from a sorbent and the simultaneous conversion to CO. In this study, we test the flexibility of a plasma−sorbent system in a single unit, specifically for sorption-enhanced dry reforming of methane (DRM). The experimental results indicate the selective adsorption of CO2 by the sorbent zeolite 5A in the first step, and CH4 addition during the plasma-based desorption of CO2 enables DRM to various value-added products in the second step, such as H2, CO, hydrocarbons, and the byproduct H2O. Furthermore, our work also demonstrates that zeolite has the potential to increase the conversion of CO2 and CH4, attributed to its capability to capture H2O. Aside from the notable carbon deposition, material analysis shows that the zeolite remains relatively stable under plasma exposure. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-07-22 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | ||
Impact Factor | 8.4 | Times cited | Open Access | ||
Notes | Fonds Wetenschappelijk Onderzoek, 110221N V404823N ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2024 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9264 | ||
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Author | Gorbanev, Y.; Fedirchyk, I.; Bogaerts, A. | ||||
Title | Plasma catalysis in ammonia production and decomposition: Use it, or lose it? | Type | A1 Journal Article | ||
Year | 2024 | Publication | Current Opinion in Green and Sustainable Chemistry | Abbreviated Journal | Current Opinion in Green and Sustainable Chemistry |
Volume | 47 | Issue | Pages | 100916 | |
Keywords | A1 Journal Article; Plasma Nitrogen fixation Ammonia Plasma catalysis Production and decomposition; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | The combination of plasma with catalysis for the synthesis and decomposition of NH3 is an attractive route to the production of carbon-neutral fertiliser and energy carriers and its conversion into H2. Recent years have seen fast developments in the field of plasma-catalytic NH3 life cycle. This work summarises the most recent advances in plasma-catalytic and related NH3-focussed processes, identifies some of the most important discoveries, and addresses plausible strategies for future developments in plasma-based NH3 technology. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-03-29 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2452-2236 | ISBN | Additional Links | ||
Impact Factor | 9.3 | Times cited | Open Access | ||
Notes | The work was supported by the Fund for Scientific Research (FWO) Flanders Bioeconomy project (grant G0G2322N) funded by the European Union-NextGe- nerationEU, the HyPACT project funded by the Belgian Energy Transition Fund, and the MSCA4Ukraine project 1233629 funded by the European Union. | Approved | Most recent IF: 9.3; 2024 IF: NA | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9117 | ||
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Author | Gregory, C.L.; Nullens, H.A.; Gijbels, R.H.; van Espen, P.J.; Geuens, I.; de Keyzer, R. | ||||
Title | Automated particle analysis of populations of silver halide microcrystals by electron probe microanalysis under cryogenic conditions | Type | A1 Journal article | ||
Year | 1998 | Publication | Analytical chemistry | Abbreviated Journal | Anal Chem |
Volume | 70 | Issue | Pages | 2551-2559 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Chemometrics (Mitac 3) | ||||
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Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | 000074584700047 | Publication Date | 2002-07-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2700;1520-6882; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.32 | Times cited | 12 | Open Access | |
Notes | Approved | Most recent IF: 6.32; 1998 IF: 4.580 | |||
Call Number | UA @ lucian @ c:irua:21308 | Serial | 210 | ||
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Author | Verlinden, G.; Janssens, G.; Gijbels, R.; van Espen, P.; Geuens, I. | ||||
Title | Three-dimensional chemical characterization of complex silver halide microcrystals by scanning ion microprobe mass analysis | Type | A1 Journal article | ||
Year | 1997 | Publication | Analytical chemistry | Abbreviated Journal | Anal Chem |
Volume | 69 | Issue | Pages | 3773-3779 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Chemometrics (Mitac 3) | ||||
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Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | A1997XV71200019 | Publication Date | 2002-07-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2700;1520-6882; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.32 | Times cited | 6 | Open Access | |
Notes | Approved | Most recent IF: 6.32; 1997 IF: 4.743 | |||
Call Number | UA @ lucian @ c:irua:16959 | Serial | 3647 | ||
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