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“Predicted Influence of Plasma Activation on Nonoxidative Coupling of Methane on Transition Metal Catalysts”. Engelmann Y, Mehta P, Neyts EC, Schneider WF, Bogaerts A, Acs Sustainable Chemistry &, Engineering 8, 6043 (2020). http://doi.org/10.1021/acssuschemeng.0c00906
Abstract: The combination of catalysis and nonthermal plasma holds promise for enabling difficult chemical conversions. The possible synergy between both depends strongly on the nature of the reactive plasma species and the catalyst material. In this paper, we show how vibrationally excited species and plasma-generated radicals interact with transition metal catalysts and how changing the catalyst material can improve the conversion rates and product selectivity. We developed a microkinetic model to investigate the impact of vibrational excitations and plasma-generated radicals on the nonoxidative coupling of methane over transition metal surfaces. We predict a significant increase in ethylene formation for vibrationally excited methane. Plasma-generated radicals have a stronger impact on the turnover frequencies with high selectivity toward ethylene on noble catalysts and mixed selectivity on non-noble catalysts. In general, we show how the optimal catalyst material depends on the desired products as well as the plasma conditions.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
Impact Factor: 8.4
DOI: 10.1021/acssuschemeng.0c00906
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“Plasma-Based N2Fixation into NOx: Insights from Modeling toward Optimum Yields and Energy Costs in a Gliding Arc Plasmatron”. Vervloessem E, Aghaei M, Jardali F, Hafezkhiabani N, Bogaerts A, Acs Sustainable Chemistry &, Engineering 8, 9711 (2020). http://doi.org/10.1021/acssuschemeng.0c01815
Abstract: Plasma technology provides a sustainable, fossil-free method for N2 fixation, i.e., the conversion of inert atmospheric N2 into valuable substances, such as NOx or ammonia. In this work, we present a novel gliding arc plasmatron at atmospheric pressure for NOx production at different N2/O2 gas feed ratios, offering a promising NOx yield of 1.5% with an energy cost of 3.6 MJ/mol NOx produced. To explain the underlying mechanisms, we present a chemical kinetics model, validated by experiments, which provides insight into the NOx formation pathways and into the ambivalent role of the vibrational kinetics. This allows us to pinpoint the factors limiting the yield and energy cost, which can help to further improve the process.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 8.4
DOI: 10.1021/acssuschemeng.0c01815
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“Nitrogen fixation with water vapor by nonequilibrium plasma : toward sustainable ammonia production”. Gorbanev Y, Vervloessem E, Nikiforov A, Bogaerts A, Acs Sustainable Chemistry &, Engineering 8, 2996 (2020). http://doi.org/10.1021/ACSSUSCHEMENG.9B07849
Abstract: Ammonia is a crucial nutrient used for plant growth and as a building block in the 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 nonfossil-based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as a H source for nitrogen fixation into NH3 by nonequilibrium plasma. The highest selectivity toward NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor contents. We also studied the role of H2O vapor and of the plasma-exposed liquid H2O in nitrogen fixation by using isotopically labeled water to distinguish between these two sources of H2O. We show that added H2O vapor, and not liquid H2O, is the main source of H for NH3 generation. The studied catalyst- and H2-free method offers excellent selectivity toward NH3 (up to 96%), with energy consumption (ca. 95–118 MJ/mol) in the range of many plasma-catalytic H2-utilizing processes.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 8.4
Times cited: 14
DOI: 10.1021/ACSSUSCHEMENG.9B07849
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Engelmann Y, van &rsquo,t Veer K, Gorbanev Y, Neyts EC, Schneider WF, Bogaerts A (2021) Plasma Catalysis for Ammonia Synthesis: A Microkinetic Modeling Study on the Contributions of Eley–Rideal Reactions. 13151–13163
Abstract: Plasma catalysis is an emerging new technology for the electrification and downscaling of NH3 synthesis. Increasing attention is being paid to the optimization of plasma catalysis with respect to the plasma conditions, the catalyst material, and their mutual interaction. In this work we use microkinetic models to study how the total conversion process is impacted by the combination of different plasma conditions and transition metal catalysts. We study how plasma-generated radicals and vibrationally excited N2 (present in a dielectric barrier discharge plasma) interact with the catalyst and impact the NH3 turnover frequencies (TOFs). Both filamentary and uniform plasmas are studied, based on plasma chemistry models that provided plasma phase speciation and vibrational distribution functions. The Langmuir−Hinshelwood reaction rate coefficients (i.e., adsorption reactions and subsequent reactions among adsorbates) are determined using conventional scaling relations. An additional set of Eley−Rideal reactions (i.e., direct reactions of plasma radicals with adsorbates) was added and a sensitivity analysis on the assumed reaction rate coefficients was performed. We first show the impact of different vibrational distribution functions on the catalytic dissociation of N2 and subsequent production of NH3, and we gradually include more radical reactions, to illustrate the contribution of these species and their corresponding reaction pathways. Analysis over a large range of catalysts indicates that different transition metals (metals such as Rh, Ni, Pt, and Pd) optimize the NH3TOFs depending on the population of the vibrational levels of N2. At higher concentrations of plasma-generated radicals, the NH3 TOFs become less dependent on the catalyst material, due to radical adsorptions on the more noble catalysts and Eley−Rideal reactions on the less noble catalysts.
Keywords: A1 Journal Article;Plasma catalysis; Eley−Rideal reactions; Volcano plots; Vibrational excitation; Radical reactions; Dielectric barrier discharge; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 5.951
DOI: 10.1021/acssuschemeng.1c02713
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“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”. Li S, Sun J, Gorbanev Y, van’t Veer K, Loenders B, Yi Y, Kenis T, Chen Q, Bogaerts A, ACS Sustainable Chemistry &, Engineering 11, 15373 (2023). http://doi.org/10.1021/acssuschemeng.3c04352
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.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 8.4
DOI: 10.1021/acssuschemeng.3c04352
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“Effect of O2on Plasma-Based Dry Reforming of Methane: Revealing the Optimal Gas Composition via Experiments and Modeling of an Atmospheric Pressure Glow Discharge”. Maerivoet S, Wanten B, De Meyer R, Van Hove M, Van Alphen S, Bogaerts A, ACS Sustainable Chemistry &, Engineering 12, 11419 (2024). http://doi.org/10.1021/acssuschemeng.4c04283
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.
Keywords: A1 Journal Article; plasma-based conversion, thermal plasma, syngas production, CO2 conversion, CH4 conversio; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 8.4
DOI: 10.1021/acssuschemeng.4c04283
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“Sorption-Enhanced Dry Reforming of Methane in a DBD Plasma Reactor for Single-Stage Carbon Capture and Utilization”. Vertongen R, De Felice G, van den Bogaard H, Gallucci F, Bogaerts A, Li S, ACS Sustainable Chemistry &, Engineering 12, 10841 (2024). http://doi.org/10.1021/acssuschemeng.4c02502
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.
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) ;
Impact Factor: 8.4
DOI: 10.1021/acssuschemeng.4c02502
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“Molecular dynamics simulation of temperature effects on CF(3)(+) etching of Si surface”. Jian-Ping N, Xiao-Dan L, Cheng-Li Z, You-Min Q, Ping-Ni H, Bogaerts A, Fu-Jun G, Wuli xuebao 59, 7225 (2010)
Abstract: Molecular dynamics method was employed to investigate the effects of the reaction layer formed near the surface region on CF(3)(+) etching of Si at different temperatures. The simulation results show that the coverages of F and C are sensitive to the surface temperature. With increasing temperature, the physical etching is enhanced, while the chemical etching is weakened. It is found that with increasing surface temperature, the etching rate of Si increases. As to the etching products, the yields of SiF and SiF(2) increase with temperature, whereas the yield of SiF(3) is not sensitive to the surface temperature. And the increase of the etching yield is mainly due to the increased desorption of SiF and SiF(2). The comparison shows that the reactive layer plays an important part in the subsequeat impacting, which enhances the etching rate of Si and weakens the chemical etching intensity.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 0.624
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“Catalyst design by NH4OH treatment of USY zeolite”. Van Aelst J, Verboekend D, Philippaerts A, Nuttens N, Kurttepeli M, Gobechiya E, Haouas M, Sree SP, Denayer JFM, Martens JA, Kirschhock CEA, Taulelle F, Bals S, Baron GV, Jacobs PA, Sels BF, Advanced functional materials 25, 7130 (2015). http://doi.org/10.1002/adfm.201502772
Abstract: Hierarchical zeolites are a class of superior catalysts which couples the intrinsic zeolitic properties to enhanced accessibility and intracrystalline mass transport to and from the active sites. The design of hierarchical USY (Ultra-Stable Y) catalysts is achieved using a sustainable postsynthetic room temperature treatment with mildly alkaline NH4OH ( 0.02(M)) solutions. Starting from a commercial dealuminated USY zeolite (Si/Al = 47), a hierarchical material is obtained by selective and tuneable creation of interconnected and accessible small mesopores (2- 6 nm). In addition, the treatment immediately yields the NH4+ form without the need for additional ion exchange. After NH4OH modification, the crystal morphology is retained, whereas the microporosity and relative crystallinity are decreased. The gradual formation of dense amorphous phases throughout the crystal without significant framework atom leaching rationalizes the very high material yields (>90%). The superior catalytic performance of the developed hierarchical zeolites is demonstrated in the acid-catalyzed isomerization of alpha-pinene and the metal-catalyzed conjugation of safflower oil. Significant improvements in activity and selectivity are attained, as well as a lowered susceptibility to deactivation. The catalytic performance is intimately related to the introduced mesopores, hence enhanced mass transport capacity, and the retained intrinsic zeolitic properties.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 64
DOI: 10.1002/adfm.201502772
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“Injectable Plasma‐Treated Alginate Hydrogel for Oxidative Stress Delivery to Induce Immunogenic Cell Death in Osteosarcoma”. Živanić, M, Espona‐Noguera A, Verswyvel H, Smits E, Bogaerts A, Lin A, Canal C, Advanced functional materials (2023). http://doi.org/10.1002/adfm.202312005
Abstract: Cold atmospheric plasma (CAP) is a source of cell‐damaging oxidant molecules that may be used as low‐cost cancer treatment with minimal side effects. Liquids treated with cold plasma and enriched with oxidants are a modality for non‐invasive treatment of internal tumors with cold plasma via injection. However, liquids are easily diluted with body fluids which impedes high and localized delivery of oxidants to the target. As an alternative, plasma‐treated hydrogels (PTH) emerge as vehicles for the precise delivery of oxidants. This study reports an optimal protocol for the preparation of injectable alginate PTH that ensures the preservation of plasma‐generated oxidants. The generation, storage, and release of oxidants from the PTH are assessed. The efficacy of the alginate PTH in cancer treatment is demonstrated in the context of cancer cell cytotoxicity and immunogenicity–release of danger signals and phagocytosis by immature dendritic cells, up to now unexplored for PTH. These are shown in osteosarcoma, a hard‐to‐treat cancer. The study aims to consolidate PTH as a novel cold plasma treatment modality for non‐invasive or postoperative tumor treatment. The results offer a rationale for further exploration of alginate‐based PTHs as a versatile platform in biomedical engineering.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Center for Oncological Research (CORE)
Impact Factor: 19
DOI: 10.1002/adfm.202312005
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“Tiling silicalite-1 nanoslabs into 3D mosaics”. Kremer SPB, Kirschhock CEA, Aerts A, Villani K, Martens JA, Lebedev OI, Van Tendeloo G, Advanced materials 15, 1705 (2003). http://doi.org/10.1002/adma.200305266
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 19.791
Times cited: 82
DOI: 10.1002/adma.200305266
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“In Situ Plasma Studies Using a Direct Current Microplasma in a Scanning Electron Microscope”. Grünewald L, Chezganov D, De Meyer R, Orekhov A, Van Aert S, Bogaerts A, Bals S, Verbeeck J, Advanced Materials Technologies (2024). http://doi.org/10.1002/admt.202301632
Abstract: Microplasmas can be used for a wide range of technological applications and to improve the understanding of fundamental physics. Scanning electron microscopy, on the other hand, provides insights into the sample morphology and chemistry of materials from the mm‐ down to the nm‐scale. Combining both would provide direct insight into plasma‐sample interactions in real‐time and at high spatial resolution. Up till now, very few attempts in this direction have been made, and significant challenges remain. This work presents a stable direct current glow discharge microplasma setup built inside a scanning electron microscope. The experimental setup is capable of real‐time in situ imaging of the sample evolution during plasma operation and it demonstrates localized sputtering and sample oxidation. Further, the experimental parameters such as varying gas mixtures, electrode polarity, and field strength are explored and experimental<italic>V</italic>–<italic>I</italic>curves under various conditions are provided. These results demonstrate the capabilities of this setup in potential investigations of plasma physics, plasma‐surface interactions, and materials science and its practical applications. The presented setup shows the potential to have several technological applications, for example, to locally modify the sample surface (e.g., local oxidation and ion implantation for nanotechnology applications) on the µm‐scale.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.8
DOI: 10.1002/admt.202301632
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“Non‐Thermal Plasma as a Unique Delivery System of Short‐Lived Reactive Oxygen and Nitrogen Species for Immunogenic Cell Death in Melanoma Cells”. Lin A, Gorbanev Y, De Backer J, Van Loenhout J, Van Boxem W, Lemière F, Cos P, Dewilde S, Smits E, Bogaerts A, Advanced Science 6, 1802062 (2019). http://doi.org/10.1002/advs.201802062
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Center for Oncological Research (CORE)
Impact Factor: 9.034
Times cited: 39
DOI: 10.1002/advs.201802062
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“Plasma‐driven<scp>CO2</scp>hydrogenation to<scp>CH3OH</scp>over<scp>Fe2O3</scp>/<scp>γ‐Al2O3</scp>catalyst”. Meng S, Wu L, Liu M, Cui Z, Chen Q, Li S, Yan J, Wang L, Wang X, Qian J, Guo H, Niu J, Bogaerts A, Yi Y, AIChE Journal 69, e18154 (2023). http://doi.org/10.1002/aic.18154
Abstract: We report a plasma‐assisted CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH over Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>catalysts, achieving 12% CO<sub>2</sub>conversion and 58% CH<sub>3</sub>OH selectivity at a temperature of nearly 80°C atm pressure. We investigated the effect of various supports and loadings of the Fe‐based catalysts, as well as optimized reaction conditions. We characterized catalysts by X‐ray powder diffraction (XRD), hydrogen temperature programmed reduction (H<sub>2</sub>‐TPR), CO<sub>2</sub>and CO temperature programmed desorption (CO<sub>2</sub>/CO‐TPD), high‐resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM), x‐ray photoelectron spectroscopy (XPS), Mössbauer, and Fourier transform infrared<bold>(</bold>FTIR). The XPS results show that the enhanced CO<sub>2</sub>conversion and CH<sub>3</sub>OH selectivity are attributed to the chemisorbed oxygen species on Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>. Furthermore, the diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) and TPD results illustrate that the catalysts with stronger CO<sub>2</sub>adsorption capacity exhibit a higher reaction performance.<italic>In situ</italic>DRIFTS gain insight into the specific reaction pathways in the CO<sub>2</sub>/H<sub>2</sub>plasma. This study reveals the role of chemisorbed oxygen species as a key intermediate, and inspires to design highly efficient catalysts and expand the catalytic systems for CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH.
Keywords: A1 Journal Article; chemisorbed oxygen, CO2 hydrogenation, iron-based catalyst, methanol production, plasma catalysis; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 3.7
DOI: 10.1002/aic.18154
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“Computer simulations of a dielectric barrier discharge used for analytical spectrometry”. Martens T, Bogaerts A, Brok W, van Dijk J, Analytical and bioanalytical chemistry 388, 1583 (2007). http://doi.org/10.1007/s00216-007-1269-0
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.431
Times cited: 28
DOI: 10.1007/s00216-007-1269-0
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“Modeling plasmas in analytical chemistry—an example of cross-fertilization”. Bogaerts A, Analytical And Bioanalytical Chemistry 412, 6059 (2020). http://doi.org/10.1007/s00216-020-02587-8
Abstract: This paper gives an overview of the modeling work developed in our group in the last 25 years for various plasmas used in analytical spectrochemistry, i.e., glow discharges (GDs), inductively coupled plasmas (ICPs), and laser ablation (LA) for sample introduction in the ICP and for laser-induced breakdown spectroscopy (LIBS). The modeling approaches are briefly presented, which are different for each case, and some characteristic results are illustrated. These plasmas are used not only in analytical chemistry but also in other applications, and the insights obtained in these other fields were quite helpful for us to develop models for the analytical plasmas. Likewise, there is now a huge interest in plasma–liquid interaction, atmospheric pressure glow discharges (APGDs), and dielectric barrier discharges (DBDs) for environmental, medical, and materials applications of plasmas. The insights obtained in these fields are also very relevant for ambient desorption/ionization sources and for liquid sampling, which are nowadays very popular in analytical chemistry, and they could be very helpful in developing models for these sources as well.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.3
DOI: 10.1007/s00216-020-02587-8
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“Atomic spectroscopy”. Bings NH, Bogaerts A, Broekaert JAC, Analytical chemistry 85, 670 (2013). http://doi.org/10.1021/ac3031459
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 29
DOI: 10.1021/ac3031459
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“Atomic spectroscopy”. Bings NH, Bogaerts A, Broekaert JAC, Analytical chemistry 80, 4317 (2008). http://doi.org/10.1021/ac8006297
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 53
DOI: 10.1021/ac8006297
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“Atomic spectroscopy”. Bings NH, Bogaerts A, Broekaert JAC, Analytical chemistry 78, 3917 (2006). http://doi.org/10.1021/ac060597m
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 112
DOI: 10.1021/ac060597m
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“Atomic spectroscopy”. Bings NH, Bogaerts A, Broekaert JAC, Analytical chemistry 76, 3313 (2004). http://doi.org/10.1021/ac040052x
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 32
DOI: 10.1021/ac040052x
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“Atomic spectroscopy”. Bings NH, Bogaerts A, Broekaert JAC, Analytical chemistry 74, 2691 (2002). http://doi.org/10.1021/ac020190r
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 18
DOI: 10.1021/ac020190r
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“Atomic spectroscopy: a review”. Bings NH, Bogaerts A, Broekaert JAC, Analytical chemistry 82, 4653 (2010). http://doi.org/10.1021/ac1010469
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 65
DOI: 10.1021/ac1010469
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“Optimized transport setup for high repetition rate pulse-separated analysis in laser ablation-inductively coupled plasma mass spectrometry”. Lindner H, Autrique D, Garcia CC, Niemax K, Bogaerts A, Analytical chemistry 81, 4241 (2009). http://doi.org/10.1021/ac802627x
Abstract: An optimized laser ablation setup, proposed for high repetition rate inductively coupled plasma mass spectrometry (ICPMS) analyses such as 2D imaging or depth profiling, is presented. For such applications, the particle washout time needs to be as short as possible to allow high laser pulse frequencies for reduced analysis time. Therefore, it is desirable to have an ablation setup that operates as a laminar flow reactor (LFR). A top-down strategy was applied that resulted in the present design. In the first step, a previously applied ablation setup was analyzed on the basis of computational fluid dynamics (CFD) results presented by D. Autrique et al. (Spectrochim. Acta, B 2008, 63, 257−270). By means of CFD simulations, the design was modified in such a way that it operated in the LFR regime. Experimental results demonstrate that the current design can indeed be regarded as an LFR. Furthermore, the operation under LFR conditions allowed some insight into the initial radial concentration distribution if the experimental ICPMS signal and analytical expressions are taken into account. Recommendations for a modified setup for more resilient spatial distributions are given. With the present setup, a washout time of 140 ms has been achieved for a 3% signal area criterion. Therefore, 7 Hz repetition rates can be applied with the present setup. Using elementary formulas of the analytical model, an upper bound for the washout times for similar setups can be predicted. The authors believe that the presented setup geometry comes close to the achievable limit for reliable short washout times.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 18
DOI: 10.1021/ac802627x
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“Simulation and experimental studies on plasma temperature, flow velocity, and injector diameter effects for an inductively coupled plasma”. Lindner H, Murtazin A, Groh S, Niemax K, Bogaerts A, Analytical chemistry 83, 9260 (2011). http://doi.org/10.1021/ac201699q
Abstract: An inductively coupled plasma (ICP) is analyzed by means of experiments and numerical simulation. Important plasma properties are analyzed, namely, the effective temperature inside the central channel and the mean flow velocity inside the plasma. Furthermore, the effect of torches with different injector diameters is studied by the model. The temperature inside the central channel is determined from the end-on collected line-to-background ratio in dependence of the injector gas flow rates. Within the limits of 3% deviation, the results of the simulation and the experiments are in good agreement in the range of flow rates relevant for the analysis of relatively large droplets, i.e., 50 μm. The deviation increases for higher gas flow rates but stays below 6% for all flow rates studied. The velocity of the gas inside the coil region was determined by side-on analyte emission measurements with single monodisperse droplet introduction and by the analysis of the injector gas path lines in the simulation. In the downstream region significantly higher velocities were found than in the upstream region in both the simulation and the experiment. The quantitative values show good agreement in the downstream region. In the upstream region, deviations were found in the absolute values which can be attributed to the flow conditions in that region and because the methods used for velocity determination are not fully consistent. Eddy structures are found in the simulated flow lines. These affect strongly the way taken by the path lines of the injector gas and they can explain the very long analytical signals found in the experiments at low flow rates. Simulations were performed for different injector diameters in order to find conditions where good analyte transport and optimum signals can be expected. The results clearly show the existence of a transition flow rate which marks the lower limit for effective analyte transport conditions through the plasma. A rule-of-thumb equation was extracted from the results from which the transition flow rate can be estimated for different injector diameters and different injector gas compositions.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 34
DOI: 10.1021/ac201699q
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“Theoretical characterization of an atmospheric pressure glow discharge used for analytical spectrometry”. Martens T, Mihailova D, van Dijk J, Bogaerts A, Analytical chemistry 81, 9096 (2009). http://doi.org/10.1021/ac9017742
Abstract: We have investigated the plasma processes in an atmospheric pressure glow discharge (APGD) in He used for analytical spectrometry by means of fluid and Monte Carlo (MC) simulations. Typical results include the potential and electric field distributions in the plasma, the density profiles of the various plasma species throughout the discharge, the mean electron energy, as well as the rates of the various collision processes in the plasma, and the relative importance of the different production and loss rates for the various species. The similarities and differences with low-pressure glow discharges are discussed. The main differences are a very small cathode dark space region and a large positive column as well as the dominant role of molecular ions. Some characteristic features of the APGD, such as the occurrence of the different spatial zones in the discharge, are illustrated, with links to experimental observations.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 15
DOI: 10.1021/ac9017742
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“Two-dimensional model of a direct current glow discharge : description of the argon metastable atoms, sputtered atoms and ions”. Bogaerts A, Gijbels R, Analytical chemistry 68, 2676 (1996). http://doi.org/10.1021/ac951206z
Abstract: A two-dimensional model is presented that describes the behavior of argon metastable atoms, copper atoms, and copper ions in an argon direct. current glow discharge, in the standard cell of the VG9000 glow discharge mass spectrometer for analyzing flat samples. The model is combined with a previously developed model for the electrons, argon ions, and atoms in the same cell to obtain an overall picture of the glow discharge, The results of the present model comprise the number densities of the described plasma species, the relative contributions of different production and loss processes for the argon metastable atoms, the thermalization profile of the sputtered copper atoms, the relative importance of the different ionization mechanisms for the copper atoms, the ionization degree of copper, the copper ion-to-argon ion density ratio, and the relative roles of copper ions, argon ions, and atoms in the sputtering process. All these quantities are calculated for a range of voltages and pressures, Moreover, since the sticking coefficient of copper atoms on solid surfaces is not well-known in the literature, the influence of this parameter on the results is briefly discussed.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 5.636
Times cited: 57
DOI: 10.1021/ac951206z
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“Two-dimensional model of a direct current glow discharge: description of the electrons, argon ions and fast argon atoms”. Bogaerts A, Gijbels R, Goedheer WJ, Analytical chemistry 68, 2296 (1996). http://doi.org/10.1021/ac9510651
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 5.636
Times cited: 70
DOI: 10.1021/ac9510651
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“Ion Clouds in the Inductively Coupled Plasma Torch: A Closer Look through Computations”. Aghaei M, Lindner H, Bogaerts A, Analytical chemistry 88, 8005 (2016). http://doi.org/10.1021/acs.analchem.6b01189
Abstract: We have computationally investigated the introduction of copper elemental particles in an inductively coupled plasma torch connected to a sampling cone, including for the first time the ionization of the sample. The sample is inserted as liquid particles, which are followed inside the entire torch, i.e., from the injector inlet up to the ionization and reaching the sampler. The spatial position of the ion clouds inside the torch as well as detailed information on the copper species fluxes at the position of the sampler orifice and the exhausts of the torch are provided. The effect of on- and off-axis injection is studied. We clearly show that the ion clouds of on-axis injected material are located closer to the sampler with less radial diffusion. This guarantees a higher transport efficiency through the sampler cone. Moreover, our model reveals the optimum ranges of applied power and flow rates, which ensure the proper position of ion clouds inside the torch, i.e., close enough to the sampler to increase the fraction that can enter the mass spectrometer and with minimum loss of material toward the exhausts as well as a sufficiently high plasma temperature for efficient ionization.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 9
DOI: 10.1021/acs.analchem.6b01189
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“Impact of the Particle Diameter on Ion Cloud Formation from Gold Nanoparticles in ICPMS”. Fuchs J, Aghaei M, Schachel TD, Sperling M, Bogaerts A, Karst U, Analytical chemistry 90, 10271 (2018). http://doi.org/10.1021/acs.analchem.8b02007
Abstract: The unique capabilities of microsecond dwell time (DT) single-particle inductively coupled plasma mass spectrometry (spICPMS) were utilized to characterize the cloud of ions generated from the introduction of suspensions of gold nanoparticles (AuNPs) into the plasma. A set of narrowly distributed particles with diameters ranging from 15.4 to 100.1 nm was synthesized and characterized according to established protocols. Statistically significant numbers of the short transient spICPMS events were evaluated by using 50 μs DT for their summed intensity, maximum intensity, and duration, of which all three were found to depend on the particle diameter. The summed intensity increases from 10 to 1661 counts and the maximum intensity from 6 to 309 counts for AuNPs with diameters from 15.4 to 83.2 nm. The event duration rises from 322 to 1007 μs upon increasing AuNP diameter. These numbers represent a comprehensive set of key data points of the ion clouds generated in ICPMS from AuNPs. The extension of event duration is of high interest to appoint the maximum possible particle number concentration at which separation of consecutive events in spICPMS can still be achieved. Moreover, the combined evaluation of all above-mentioned ion cloud characteristics can explain the regularly observed prolonged single-particle events. The transport and ionization behavior of AuNPs in the ICP was also computationally modeled to gain insight into the size-dependent signal generation. The simulated data reveals that the plasma temperature, and therefore the point of ionization of the particles, is the same for all diameters. However, the maximum number density of Au+, as well as the extent of the ion cloud, depends on the particle diameter, in agreement with the experimental data, and it provides an adequate explanation for the observed ion cloud characteristics.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.32
Times cited: 5
DOI: 10.1021/acs.analchem.8b02007
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“Analysis of Short-Lived Reactive Species in Plasma–Air–Water Systems: The Dos and the Do Nots”. Gorbanev Y, Privat-Maldonado A, Bogaerts A, Analytical Chemistry 90, 13151 (2018). http://doi.org/10.1021/acs.analchem.8b03336
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.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 6.32
Times cited: 17
DOI: 10.1021/acs.analchem.8b03336
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