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| Author | Vermeiren, V.; Bogaerts, A. | ||||
| Title | Plasma-Based CO2Conversion: To Quench or Not to Quench? | Type | A1 Journal article | ||
| Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 124 | Issue | 34 | Pages | 18401-18415 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma technology is gaining increasing interest for CO2 conversion. The gas temperature in (and after) the plasma reactor largely affects the performance. Therefore, we examine the effect of cooling/quenching, during and after the plasma, on the CO2 conversion and energy efficiency, for typical “warm” plasmas, by means of chemical kinetics modeling. For plasmas at low specific energy input (SEI ∼ 0.5 eV/molecule), it is best to quench at the plasma end, while for high-SEI plasmas (SEI ∼ 4 eV/molecule), quenching at maximum conversion is better. For low-SEI plasmas, quenching can even increase the conversion beyond the dissociation in the plasma, known as superideal quenching. To better understand the effects of quenching at different plasma conditions, we study the dissociation and recombination rates, as well as the vibrational distribution functions (VDFs) of CO2, CO, and O2. When a high vibrational−translational (VT) nonequilibrium exists at the moment of quenching, the dissociation and recombination reaction rates both increase. Depending on the conversion degree at the moment of quenching, this can lead to a net increase or decrease of CO2 conversion. In general, however, and certainly for equilibrium plasmas at high temperature, quenching after the plasma helps prevent recombination reactions and clearly enhances the final CO2 conversion. We also investigate the effect of different quenching cooling rates on the CO2 conversion and energy efficiency. Finally, we compare plasma-based conversion to purely thermal conversion. For warm plasmas with typical temperatures of 3000−4000 K, the conversion is roughly thermal. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000566481000003 | Publication Date | 2020-08-27 | |
| 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 | 3.7 | Times cited | Open Access | OpenAccess | |
| Notes | Fonds Wetenschappelijk Onderzoek, G.0383.16N ; H2020 European Research Council, 810182 ; This research was supported by the FWO project (grant no. G.0383.16N) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement no. 810182SCOPE ERC Synergy project). 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: 3.7; 2020 IF: 4.536 | ||
| Call Number | PLASMANT @ plasmant @c:irua:172052 | Serial | 6407 | ||
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| Author | van ‘t Veer, K.; Engelmann, Y.; Reniers, F.; Bogaerts, A. | ||||
| Title | Plasma-Catalytic Ammonia Synthesis in a DBD Plasma: Role of Microdischarges and Their Afterglows | Type | A1 Journal article | ||
| Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 124 | Issue | 42 | Pages | 22871-22883 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
| Abstract | Plasma-catalytic ammonia synthesis is receiving ever increasing attention, especially in packed bed dielectric barrier discharge (DBD) reactors. The latter typically operate in the filamentary regime when used for gas conversion applications. While DBDs are in principle well understood and already applied in the industry, the incorporation of packing materials and catalytic surfaces considerably adds to the complexity of the plasma physics and chemistry governing the ammonia formation. We employ a plasma kinetics model to gain insights into the ammonia formation mechanisms, paying special attention to the role of filamentary microdischarges and their afterglows. During the microdischarges, the synthesized ammonia is actually decomposed, but the radicals created upon electron impact dissociation of N2 and H2 and the subsequent catalytic reactions cause a net ammonia gain in the afterglows of the microdischarges. Under our plasma conditions, electron impact dissociation of N2 in the gas phase followed by the adsorption of N atoms is identified as a rate-limiting step, instead of dissociative adsorption of N2 on the catalyst surface. Both elementary Eley−Rideal and Langmuir−Hinshelwood reaction steps can be found important in plasma-catalytic NH3 synthesis. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000585970300002 | Publication Date | 2020-10-22 | |
| 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 | 3.7 | Times cited | Open Access | OpenAccess | |
| Notes | Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique – FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ;This research was supported by the Excellence of Science FWOFNRS project (FWO grant ID GoF9618n, EOS ID 30505023) and by 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 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. The authors would also like to thank Järi Van den Hoek and Dr. Yury Gorbanev for providing the experimentally measured electrical characteristics and Dr. Fatme Jardali for creating the TOC graphics. | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
| Call Number | PLASMANT @ plasmant @c:irua:173587 | Serial | 6428 | ||
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| Author | Michiels, R.; Engelmann, Y.; Bogaerts, A. | ||||
| Title | Plasma Catalysis for CO2Hydrogenation: Unlocking New Pathways toward CH3OH | Type | A1 Journal article | ||
| Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 124 | Issue | 47 | Pages | 25859-25872 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
| Abstract | We developed a microkinetic model to reveal the effects of plasma-generated radicals, intermediates, and vibrationally excited species on the catalytic hydrogenation of CO2 to CH3OH on a Cu(111) surface. As a benchmark, we first present the mechanisms of thermal catalytic CH3OH formation. Our model predicts that the reverse water-gas shift reaction followed by CO hydrogenation, together with the formate path, mainly contribute to CH3OH formation in thermal catalysis. Adding plasma-generated radicals and intermediates results in a higher CH3OH turnover frequency (TOF) by six to seven orders of magnitude, showing the potential of plasma-catalytic CO2 hydrogenation into CH3OH, in accordance with the literature. In addition, CO2 vibrational excitation further increases the CH3OH TOF, but the effect is limited due to relatively low vibrational temperatures under typical plasma catalysis conditions. The predicted increase in CH3OH formation by plasma catalysis is mainly attributed to the increased importance of the formate path. In addition, the conversion of plasma-generated CO to HCO* and subsequent HCOO* or H2CO* formation contribute to CH3OH formation. Both pathways bypass the HCOO* formation from CO2, which is the main bottleneck in the process. Hence, our model points toward the important role of CO, but also O, OH, and H radicals, as they influence the reactions that consume CO2 and CO. In addition, our model reveals that the H pressure should not be smaller than ca. half of the O pressure in the plasma as this would cause O* poisoning, which would result in very small product TOFs. Thus, plasma conditions should be targeted with a high CO and H content as this is favorable for CH3OH formation, while the O content should be minimized. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000595545800023 | Publication Date | 2020-11-25 | |
| 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 | 3.7 | Times cited | Open Access | Not_Open_Access: Available from 15.07.2021 | |
| Notes | Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; We acknowledge the financial support from the Fund for Scientific Research (FWO-Vlaanderen; grant ID 1114921N) and from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 810182 − SCOPE ERC Synergy project) as well as from the DOC-PRO3 and the TOPBOF projects of the University of Antwerp. | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
| Call Number | PLASMANT @ plasmant @c:irua:173864 | Serial | 6443 | ||
| Permanent link to this record | |||||
| Author | Loenders, B.; Engelmann, Y.; Bogaerts, A. | ||||
| Title | Plasma-Catalytic Partial Oxidation of Methane on Pt(111): A Microkinetic Study on the Role of Different Plasma Species | Type | A1 Journal article | ||
| Year | 2021 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 125 | Issue | 5 | Pages | 2966-2983 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
| Abstract | We use microkinetic modeling to examine the potential of plasma-catalytic partial oxidation (POX) of CH4 as a promising new approach to produce oxygenates. We study how different plasma species affect POX of CH4 on the Pt(111) surface, and we discuss the associated kinetic and mechanistic changes. We discuss the effect of vibrationally excited CH4 and O2, as well as plasma-generated radicals and stable intermediates. Our results show that vibrational excitation enhances the turnover frequency (TOF) of catalytic CH4 dissociation and has good potential for improving the selectivities toward CH3OH, HCOOH, and C2 hydrocarbons. Nevertheless, when also considering plasma-generated radicals, we find that these species mainly govern the surface chemistry. Additionally, we find that plasma-generated radicals and stable intermediates enhance the TOFs of COx and oxygenates, increase the selectivity toward oxygenates, and make the formation of HCOOH more significant on Pt(111). We also briefly illustrate the potential impact of Eley−Rideal reactions that involve plasma-generated radicals. Finally, we reveal how various radicals affect the catalyst surface chemistry and we link this to the formation of different products. This allows us to make suggestions on how the plasma composition should be altered to improve the formation of desired products. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000619760700017 | Publication Date | 2021-02-11 | |
| 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 | Open Access | OpenAccess | |
| Notes | Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, S001619N ; H2020 European Research Council, 810182 ; We thank Tom Butterworth for the interesting discussions regarding the calculation of the vibrational populations of methane and for taking the time to share his thoughts and experiences on the matter. This research is supported by the FWO-SBO project PLASMACATDesign (grant number S001619N). We also acknowledge financial support from the TOP-BOF project of the University of Antwerp and from the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement no. 810182SCOPE ERC Synergy project). The calculations were carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (Department EWI), and the University of Antwerp. | Approved | Most recent IF: 4.536 | ||
| Call Number | PLASMANT @ plasmant @c:irua:175873 | Serial | 6672 | ||
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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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| Corporate Author | Thesis | ||||
| 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 | Grubova, I.Y.; Surmeneva, M.A.; Huygh, S.; Surmenev, R.A.; Neyts, E.C. | ||||
| Title | Density functional theory study of interface interactions in hydroxyapatite/rutile composites for biomedical applications | Type | A1 Journal article | ||
| Year | 2017 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 121 | Issue | 29 | Pages | 15687-15695 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | To gain insight into the nature of the adhesion mechanism between hydroxyapatite (HA) and rutile (rTiO(2)), the mutual affinity between their surfaces was systematically studied using density functional theory (DFT). We calculated both bulk and surface properties of HA and rTiO(2), and explored the interfacial bonding mechanism of amorphous HA (aHA) surface onto amorphous as well as stoichiometric and nonstoichiometric crystalline rTiO(2). Formation energies of bridging and subbridging oxygen vacancies considered in the rTiO(2)(110) surface were evaluated and compared with other theoretical and experimental results. The interfacial interaction was evaluated through the work of adhesion. For the aHA/rTiO(2)(110) interfaces, the work of adhesion is found to depend strongly on the chemical environment of the rTiO(2)(110) surface. Electronic analysis indicates that the charge transfer is very small in the case of interface formation between aHA and crystalline rTiO(2)(110). In contrast, significant charge transfer occurs between aHA and amorphous rTiO(2) (aTiO(2)) slabs during the formation of the interface. Charge density difference (CDD) analysis indicates that the dominant interactions in the interface have significant covalent character, and in particular the Ti-O and Ca-O bonds. Thus, the obtained results reveal that the aHA/aTiO(2) interface shows a more preferable interaction and is thermodynamically more stable than other interfaces. These results are particularly important for improving the long-term stability of HA-based implants. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000406726200022 | Publication Date | 2017-06-27 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | 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 | Approved | Most recent IF: 4.536 | |||
| Call Number | UA @ lucian @ c:irua:145195 | Serial | 4715 | ||
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| Author | Vets, C.; Neyts, E.C. | ||||
| Title | Stabilities of bimetallic nanoparticles for chirality-selective carbon nanotube growth and the effect of carbon interstitials | Type | A1 Journal article | ||
| Year | 2017 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 121 | Issue | 28 | Pages | 15430-15436 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Bimetallic nanoparticles play a crucial role in various applications. A better understanding of their properties would facilitate these applications and possibly even enable chirality-specific growth of carbon nanotubes (CNTs). We here examine the stabilities of NiFe, NiGa, and FeGa nanoparticles and the effect of carbon dissolved in NiFe nanoparticles through density functional theory (DFT) calculations and Born Oppenheimer molecular dynamics (BOMD) simulations. We establish that nanoparticles with more Fe in the core and more Ga on the surface are more stable and compare these results with well-known properties such as surface energy and atom size. Furthermore, we find that the nanoparticles become more stable with increasing carbon content, both at 0 K and at 700 K. These results provide a basis for further research into the chirality-specific growth of CNT's. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000406355700050 | Publication Date | 2017-06-23 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 2 | Open Access | Not_Open_Access |
| Notes | Approved | Most recent IF: 4.536 | |||
| Call Number | UA @ lucian @ c:irua:145206 | Serial | 4725 | ||
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| Author | Jafarzadeh, A.; Bal, K.M.; Bogaerts, A.; Neyts, E.C. | ||||
| Title | CO2 activation on TiO2-supported Cu5 and Ni5 nanoclusters : effect of plasma-induced surface charging | Type | A1 Journal article | ||
| Year | 2019 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 123 | Issue | 11 | Pages | 6516-6525 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Surface charging is an often overlooked factor in many plasma-surface interactions and in particular in plasma catalysis. In this study, we investigate the effect of excess electrons induced by a plasma on the adsorption properties of CO2 on titania-supported Cu-5 and Ni-5 clusters using spin-polarized and dispersion-corrected density functional theory calculations. The effect of excess electrons on the adsorption of Ni and Cu pentamers as well as on CO2 adsorption on a pristine anatase TiO2(101) slab is studied. Our results indicate that adding plasma-induced excess electrons to the system leads to further stabilization of the bent CO2 structure. Also, dissociation of CO2 on charged clusters is energetically more favorable than on neutral clusters. We hypothesize that surface charge is a plausible cause for the synergistic effects sometimes observed in plasma catalysis. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000462260700024 | Publication Date | 2019-02-21 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 4 | Open Access | OpenAccess |
| Notes | Approved | Most recent IF: 4.536 | |||
| Call Number | UA @ admin @ c:irua:159422 | Serial | 5281 | ||
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| Author | Mehta, A.N.; Mo, J.; Pourtois, G.; Dabral, A.; Groven, B.; Bender, H.; Favia, P.; Caymax, M.; Vandervorst, W. | ||||
| Title | Grain-boundary-induced strain and distortion in epitaxial bilayer MoS₂ lattice | Type | A1 Journal article | ||
| Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 124 | Issue | 11 | Pages | 6472-6478 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Grain boundaries between 60 degrees rotated and twinned crystals constitute the dominant type of extended line defects in two-dimensional transition metal dichalcogenides (2D MX2) when grown on a single crystalline template through van der Waals epitaxy. The two most common 60 degrees grain boundaries in MX2 layers, i.e., beta- and gamma-boundaries, introduce distinct distortion and strain into the 2D lattice. They impart a localized tensile or compressive strain on the subsequent layer, respectively, due to van der Waals coupling in bilayer MX2 as determined by combining atomic resolution electron microscopy, geometric phase analysis, and density functional theory. Based on these observations, an alternate route to strain engineering through controlling intrinsic van der Waals forces in homobilayer MX2 is proposed. In contrast to the commonly used external means, this approach enables the localized application of strain to tune the electronic properties of the 2D semiconducting channel in ultra-scaled nanoelectronic applications. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000526396000067 | Publication Date | 2020-02-21 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.7 | Times cited | 2 | Open Access | |
| Notes | ; ; | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
| Call Number | UA @ admin @ c:irua:168625 | Serial | 6528 | ||
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| Author | Nematollahi, P.; Neyts, E.C. | ||||
| Title | Identification of a unique pyridinic FeN4Cx electrocatalyst for N₂ reduction : tailoring the coordination and carbon topologies | Type | A1 Journal article | ||
| Year | 2022 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 126 | Issue | 34 | Pages | 14460-14469 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Although the heterogeneity of pyrolyzed Fe???N???C materials is known and has been reported previously, the atomic structure of the active sites and their detailed reaction mechanisms are still unknown. Here, we identified two pyridinic Fe???N4-like centers with different local C coordinates, i.e., FeN4C8 and FeN4C10, and studied their electrocatalytic activity for the nitrogen reduction reaction (NRR) based on density functional theory (DFT) calculations. We also discovered the influence of the adsorption of NH2 as a functional ligand on catalyst performance on the NRR. We confirmed that the NRR selectivity of the studied catalysts is essentially governed either by the local C coordination or by the dynamic structure associated with the FeII/FeIII. Our investigations indicate that the proposed traditional pyridinic FeN4C10 has higher catalytic activity and selectivity for the NRR than the robust FeN4C8 catalyst, while it may have outstanding activity for promoting other (electro)catalytic reactions. <comment>Superscript/Subscript Available</comment | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000859545200001 | Publication Date | 2022-08-17 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 3.7 | Times cited | Open Access | OpenAccess | |
| Notes | Approved | Most recent IF: 3.7 | |||
| Call Number | UA @ admin @ c:irua:191469 | Serial | 7268 | ||
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| Author | Van de Sompel, P.; Khalilov, U.; Neyts, E.C. | ||||
| Title | Contrasting H-etching to OH-etching in plasma-assisted nucleation of carbon nanotubes | Type | A1 Journal article | ||
| Year | 2021 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 125 | Issue | 14 | Pages | 7849-7855 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | To gain full control over the growth of carbon nanotubes (CNTs) using plasma-enhanced chemical vapor deposition (PECVD), a thorough understanding of the underlying plasma-catalyst mechanisms is required. Oxygen-containing species are often used as or added to the growth precursor gas, but these species also yield various radicals and ions, which may simultaneously etch the CNT during the growth. At present, the effect of these reactive species on the growth onset has not yet been thoroughly investigated. We here report on the etching mechanism of incipient CNT structures from OH and O radicals as derived from combined (reactive) molecular dynamics (MD) and force-bias Monte Carlo (tfMC) simulations. Our results indicate that the oxygen-containing radicals initiate a dissociation process. In particular, we show how the oxygen species weaken the interaction between the CNT and the nanocluster. As a result of this weakened interaction, the CNT closes off and dissociates from the cluster in the form of a fullerene. Beyond the specific systems studied in this work, these results are generically important in the context of PECVD-based growth of CNTs using oxygen-containing precursors. | ||||
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| Language | Wos | 000641307100032 | Publication Date | 2021-04-06 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 4.536 | Times cited | Open Access | OpenAccess | |
| Notes | Approved | Most recent IF: 4.536 | |||
| Call Number | UA @ admin @ c:irua:178393 | Serial | 7729 | ||
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| Author | Nematollahi, P.; Ma, H.; Schneider, W.F.; Neyts, E.C. | ||||
| Title | DFT and microkinetic comparison of ru-doped porphyrin-like graphene and nanotubes toward catalytic formic acid decomposition and formation | Type | A1 Journal article | ||
| Year | 2021 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 125 | Issue | 34 | Pages | 18673-18683 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Immobilization of single metal atoms on a solid host opens numerous possibilities for catalyst designs. If that host is a two-dimensional sheet, sheet curvature becomes a design parameter potentially complementary to host and metal composition. Here, we use a combination of density functional theory calculations and microkinetic modeling to compare the mechanisms and kinetics of formic acid decomposition and formation, chosen for their relevance as a potential hydrogen storage medium, over single Ru atoms anchored to pyridinic nitrogen in a planar graphene flake (RuN4-G) and curved carbon nanotube (RuN4-CNT). Activation barriers are lowered and the predicted turnover frequencies are increased over RuN4-CNT relative to RuN4-CNT. The results highlight the potential of curvature control as a means to achieve high performance and robust catalysts. | ||||
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| Language | Wos | 000693413400013 | Publication Date | 2021-08-22 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | Open Access | OpenAccess | |
| Notes | Approved | Most recent IF: 4.536 | |||
| Call Number | UA @ admin @ c:irua:181538 | Serial | 7805 | ||
| Permanent link to this record | |||||
| Author | Tchakoua, T.; Powell, A.D.; Gerrits, N.; Somers, M.F.; Doblhoff-Dier, K.; Busnengo, H.F.; Kroes, G.-J. | ||||
| Title | Simulating highly activated sticking of H₂ on Al(110) : quantum versus quasi-classical dynamics | Type | A1 Journal article | ||
| Year | 2023 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | |
| Volume | 127 | Issue | 11 | Pages | 5395-5407 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | We evaluate the importance of quantum effects on the sticking of H2 on Al(110) for conditions that are close to those of molecular beam experiments that have been done on this system. Calculations with the quasi-classical trajectory (QCT) method and with quantum dynamics (QD) are performed using a model in which only motion in the six molecular degrees of freedom is allowed. The potential energy surface used has a minimum barrier height close to the value recently obtained with the quantum Monte Carlo method. Monte Carlo averaging over the initial rovibrational states allowed the QD calculations to be done with an order of magnitude smaller computational expense. The sticking probability curve computed with QD is shifted to lower energies relative to the QCT curve by 0.21 to 0.05 kcal/mol, with the highest shift obtained for the lowest incidence energy. Quantum effects are therefore expected to play a small role in calculations that would evaluate the accuracy of electronic structure methods for determining the minimum barrier height to dissociative chemisorption for H2 + Al(110) on the basis of the standard procedure for comparing results of theory with molecular beam experiments. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000971346700001 | Publication Date | 2023-03-14 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.7 | Times cited | Open Access | OpenAccess | |
| Notes | Approved | Most recent IF: 3.7; 2023 IF: 4.536 | |||
| Call Number | UA @ admin @ c:irua:196071 | Serial | 8525 | ||
| Permanent link to this record | |||||
| Author | Huygh, S.; Neyts, E.C. | ||||
| Title | Adsorption of C and CHx radicals on anatase (001) and the influence of oxygen vacancies | Type | A1 Journal article | ||
| Year | 2015 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 119 | Issue | 119 | Pages | 4908-4921 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | The adsorption of C and CHx radicals on anatase (001) was studied using DFT within the generalized gradient approximation using the Perde-Burke-Ernzerhof (PBE) functional. We have studied the influence of oxygen vacancies in and at the surface on the adsorption properties of the radicals. For the oxygen vacancies in anatase (001), the most stable vacancy is located at the surface. For this vacancy, the maximal adsorption strength of C and CH decreases compared to the adsorption on the stoichiometric surface, but it increases for CH2 and CH3. If an oxygen vacancy is present in the first subsurface layer, the maximal adsorption strength increases for C, CH, CH2, and CH3. When the vacancy is present in the next subsurface layer, we find that only the CH3 adsorption is enhanced, while the maximal adsorption energies for the other radical species decrease. Not only does the precise location of the oxygen vacancy determine the maximal adsorption interaction, it also influences the adsorption strengths of the radicals at different surface configurations. This determines the probability of finding a certain adsorption configuration at the surface, which in turn influences the possible surface reactions. We find that C preferentially adsorbs far away from the oxygen vacancy, while CH2 and CH3 adsorb preferentially at the oxygen vacancy site. A fraction of CH partially adsorbs at the oxygen vacancy, and another fraction adsorbs further away from the vacancy. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000350840700052 | Publication Date | 2015-02-18 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 13 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2015 IF: 4.772 | |||
| Call Number | c:irua:124909 | Serial | 63 | ||
| Permanent link to this record | |||||
| Author | Phung, Q.M.; Vancoillie, S.; Pourtois, G.; Swerts, J.; Pierloot, K.; Delabie, A. | ||||
| Title | Atomic layer deposition of ruthenium on a titanium nitride surface : a density functional theory study | Type | A1 Journal article | ||
| Year | 2013 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 117 | Issue | 38 | Pages | 19442-19453 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Because of its excellent properties in nanotechnology applications, atomic layer deposition of ruthenium (Ru) has been the subject of numerous experimental studies. Recently, two different Ru precursors were compared for plasma-enhanced atomic layer deposition (PEALD) of Ru, and their reactivity was found to be different. Inhibition was observed for bis(ethylcyclopentadienyl)ruthenium (Ru(EtCp)(2)), while nearly linear growth behavior was observed for (methylcyclopentadienyl-pyrrolyl)ruthenium (Ru(MeCp)Py). To understand this difference in reactivity, we investigate the adsorption of RuCp, and RuCpPy (i.e., without substituents) on a TiN surface using calculations based on periodic boundary conditions density functional theory (DFT) combined with experiments based on Rutherford backscattering spectroscopy (RBS). The calculations demonstrate that the RuCpPy precursor chemisorbs on the TiN(100) surface while the RuCp2 precursor only physisorbs. We propose a reaction mechanism for the chemisorption of RuCpPy. The area density of the calculated RuCpPy surface species is compared with the experimental values from RBS. The impact of a H-plasma is also investigated. The DFT calculations and experimental results from RBS provide insight into the adsorption processes of the RuCpPy and RuCp2 precursors on the TiN(100) surface. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000330162500022 | Publication Date | 2013-08-28 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 6 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2013 IF: 4.835 | |||
| Call Number | UA @ lucian @ c:irua:114855 | Serial | 170 | ||
| Permanent link to this record | |||||
| Author | Quan Manh, P.; Pourtois, G.; Swerts, J.; Pierloot, K.; Delabie, A. | ||||
| Title | Atomic layer deposition of Ruthenium on Ruthenium surfaces : a theoretical study | Type | A1 Journal article | ||
| Year | 2015 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 119 | Issue | 119 | Pages | 6592-6603 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Atomic, layer deposition,(ALD of ruthenium using two ruthenium precursors, i.e., Ru(C5H5)(2) (RuCp2) and Ru(C5H5)(C4H4N) (RuCpPy), is studied using density functional theory. By investigating the reaction mechanisms On bare ruthenium surfaces, i.e., (001), (101), and (100), and H-terminated surfaces, an atomistic insight in the Ru ALD is provided. The calculated results show that on the Ru surfaces both RuCp2 and RuCpPy an undergo dehydrogenation and ligand dissociation reactions. RuCpPy is more reactive than RuCp2. By forming a, strong, bond between N of Py and Ru of the surface, RuCpPy can easily chemisorb on the surfaces. The reactions of RuCp2,On the Surfaces are less favorable the adsorption is not strong enough This could be a,factor contributing to the higher growth-per-cycle of Ru using RuCpPy, as observed experimentally. By Studying, the adsorption on H-terminated Ru surfaces, We showed that H Can prevent the adsorption of the precursors, thus inhibiting the growth of Ru. Our calculations indicate that the H content on the surface can have an impact on the growth-per-cycle. Finally, our simulations also demonstrate large impacts of the surface structure on the reaction mechanisms. Of the three surfaces, the (100) surface, which is the less stable and has a zigzag surface structure, is also the most reactive one. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000351970800015 | Publication Date | 2015-03-04 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 10 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2015 IF: 4.772 | |||
| Call Number | c:irua:125544 | Serial | 171 | ||
| Permanent link to this record | |||||
| Author | Khalilov, U.; Neyts, E.C.; Pourtois, G.; van Duin, A.C.T. | ||||
| Title | Can we control the thickness of ultrathin silica layers by hyperthermal silicon oxidation at room temperature? | Type | A1 Journal article | ||
| Year | 2011 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 115 | Issue | 50 | Pages | 24839-24848 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Using reactive molecular dynamics simulations by means of the ReaxFF potential, we studied the growth mechanism of ultrathin silica (SiO2) layers during hyperthermal oxidation at room temperature. Oxidation of Si(100){2 × 1} surfaces by both atomic and molecular oxygen was investigated in the energy range 15 eV. The oxidation mechanism, which differs from thermal oxidation, is discussed. In the case of oxidation by molecular O2, silica is quickly formed and the thickness of the formed layers remains limited compared to oxidation by atomic oxygen. The Si/SiO2 interfaces are analyzed in terms of partial charges and angle distributions. The obtained structures of the ultrathin SiO2 films are amorphous, including some intrinsic defects. This study is important for the fabrication of silica-based devices in the micro- and nanoelectronics industry, and more specifically for the fabrication of metal oxide semiconductor devices. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000297947700050 | Publication Date | 2011-11-16 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 36 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2011 IF: 4.805 | |||
| Call Number | UA @ lucian @ c:irua:94303 | Serial | 273 | ||
| Permanent link to this record | |||||
| Author | Wendelen, W.; Dzhurakhalov, A.A.; Peeters, F.M.; Bogaerts, A. | ||||
| Title | Combined molecular dynamics: continuum study of phase transitions in bulk metals under ultrashort pulsed laser irradiation | Type | A1 Journal article | ||
| Year | 2010 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 114 | Issue | 12 | Pages | 5652-5660 |
| Keywords | A1 Journal article; Integrated Molecular Plant Physiology Research (IMPRES); Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | The phase transition processes induced by ultrashort, 100 fs pulsed laser irradiation of Au, Cu, and Ni are studied by means of a combined atomistic-continuum approach. A moderately low absorbed laser fluence range, from 200 to 600 J/m2 is considered to study phase transitions by means of a local and a nonlocal order parameter. At low laser fluences, the occurrence of layer-by-layer evaporation has been observed, which suggests a direct solid to vapor transition. The calculated amount of molten material remains very limited under the conditions studied, especially for Ni. Therefore, our results show that a kinetic equation that describes a direct solid to vapor transition might be the best approach to model laser-induced phase transitions by continuum models. Furthermore, the results provide more insight into the applicability of analytical superheating theories that were implemented in continuum models and help the understanding of nonequilibrium phase transitions. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000275855600044 | Publication Date | 2010-01-26 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 2 | Open Access | |
| Notes | ; A.D. gratefully acknowledges Professor M. Hot (ULB, Brussels) for the basic MD-code that was modified further for the laser-induced melting processes. W.W, and A.D. are thankful to Professor L.V. Zhigilei for useful discussions and advices. The calculations were performed on the CALCUA computing facility of the University of Antwerp. This work was supported by the Belgian Science Policy (IAP). ; | Approved | Most recent IF: 4.536; 2010 IF: 4.524 | ||
| Call Number | UA @ lucian @ c:irua:81391 | Serial | 402 | ||
| Permanent link to this record | |||||
| Author | Tinck, S.; Neyts, E.C.; Bogaerts, A. | ||||
| Title | Fluorinesilicon surface reactions during cryogenic and near room temperature etching | Type | A1 Journal article | ||
| Year | 2014 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 118 | Issue | 51 | Pages | 30315-30324 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Cyrogenic etching of silicon is envisaged to enable better control over plasma processing in the microelectronics industry, albeit little is known about the fundamental differences compared to the room temperature process. We here present molecular dynamics simulations carried out to obtain sticking probabilities, thermal desorption rates, surface diffusion speeds, and sputter yields of F, F2, Si, SiF, SiF2, SiF3, SiF4, and the corresponding ions on Si(100) and on SiF13 surfaces, both at cryogenic and near room temperature. The different surface behavior during conventional etching and cryoetching is discussed. F2 is found to be relatively reactive compared to other species like SiF03. Thermal desorption occurs at a significantly lower rate under cryogenic conditions, which results in an accumulation of physisorbed species. Moreover, ion incorporation is often observed for ions with energies of 30400 eV, which results in a relatively low net sputter yield. The obtained results suggest that the actual etching of Si, under both cryogenic and near room temperature conditions, is based on the complete conversion of the Si surface to physisorbed SiF4, followed by subsequent sputtering of these molecules, instead of direct sputtering of the SiF03 surface. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000347360200101 | Publication Date | 2014-11-25 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 11 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2014 IF: 4.772 | |||
| Call Number | UA @ lucian @ c:irua:122957 | Serial | 1239 | ||
| Permanent link to this record | |||||
| Author | Khalilov, U.; Pourtois, G.; van Duin, A.C.T.; Neyts, E.C. | ||||
| Title | Hyperthermal oxidation of Si(100)2x1 surfaces : effect of growth temperature | Type | A1 Journal article | ||
| Year | 2012 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 116 | Issue | 15 | Pages | 8649-8656 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Using reactive molecular dynamics simulations based on the ReaxFF potential, we studied the growth mechanism of ultrathin silica (SiO2) layers during hyperthermal oxidation as a function of temperature in the range 100-1300 K. Oxidation of Si(100){2 x 1} surfaces by both atomic and molecular oxygen was investigated for hyperthermal impact energies in the range of 1 to 5 eV. Two different growth mechanisms are found, corresponding to a low temperature oxidation and a high temperature one. The transition temperature between these mechanisms is estimated to be about 700 K. Also, the initial step of the Si oxidation process is analyzed in detail. Where possible, we validated our results with experimental and ab initio data, and good agreement was obtained. This study is important for the fabrication of silica-based devices in the micro- and nanoelectronics industry and, more specifically, for the fabrication of metal oxide semiconductor devices. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000302924900035 | Publication Date | 2012-03-26 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 32 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2012 IF: 4.814 | |||
| Call Number | UA @ lucian @ c:irua:98259 | Serial | 1542 | ||
| Permanent link to this record | |||||
| Author | Neyts, E.C.; Khalilov, U.; Pourtois, G.; van Duin, A.C.T. | ||||
| Title | Hyperthermal oxygen interacting with silicon surfaces : adsorption, implantation, and damage creation | Type | A1 Journal article | ||
| Year | 2011 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 115 | Issue | 15 | Pages | 4818-4823 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Using reactive molecular dynamics simulations, we have investigated the effect of single-impact, low-energy (thermal-100 eV) bombardment of a Si(100){2 × 1} surface by atomic and molecular oxygen. Penetration probability distributions, as well as defect formation distributions, are presented as a function of the impact energy for both species. It is found that at low impact energy, defects are created chemically due to the chemisorption process in the top layers of the surface, while at high impact energy, additional defects are created by a knock-on displacement of Si. These results are of particular importance for understanding device performances of silica-based microelectronic and photovoltaic devices. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000288401200060 | Publication Date | 2011-03-02 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 28 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2011 IF: 4.805 | |||
| Call Number | UA @ lucian @ c:irua:89858 | Serial | 1543 | ||
| Permanent link to this record | |||||
| Author | Aerts, R.; Martens, T.; Bogaerts, A. | ||||
| Title | Influence of vibrational states on CO2 splitting by dielectric barrier discharges | Type | A1 Journal article | ||
| Year | 2012 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 116 | Issue | 44 | Pages | 23257-23273 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | In this paper, the splitting of CO2 in a pulsed plasma system, such as a dielectric barrier discharge (DBD), is evaluated from a chemical point of view by means of numerical modeling. For this purpose, a chemical reaction set of CO2 in an atmospheric pressure plasma is developed, including the vibrational states of CO2, O2, and CO. The simulated pulses are matched to the conditions of a filament (or microdischarge) and repeated with intervals of 1 μs. The influence of vibrationally excited CO2 as well as other neutral species, ions, and electrons on the CO2 splitting is discussed. Our calculations predict that the electrons have the largest contribution to the CO2 splitting at the conditions under study, by electron impact dissociation. The contribution of vibrationally excited CO2 levels in the splitting of CO2 is found be 6.4%, when only considering one microdischarge pulse and its afterglow, but it can be much higher for consecutive discharge pulses, as is typical for a filamentary DBD, when the interpulse time is short enough and accumulation effects in the vibrationally excited CO2 densities can occur. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000310769300012 | Publication Date | 2012-10-19 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 112 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2012 IF: 4.814 | |||
| Call Number | UA @ lucian @ c:irua:101764 | Serial | 1659 | ||
| Permanent link to this record | |||||
| Author | Kato, T.; Neyts, E.C.; Abiko, Y.; Akama, T.; Hatakeyama, R.; Kaneko, T. | ||||
| Title | Kinetics of energy selective Cs encapsulation in single-walled carbon nanotubes for damage-free and position-selective doping | Type | A1 Journal article | ||
| Year | 2015 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 119 | Issue | 119 | Pages | 11903-11908 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | A method has been developed for damage-free cesium (Cs) encapsulation within single-walled carbon nanotubes (SWNTs) with fine position selectivity. Precise energy tuning of Cs-ion irradiation revealed that there is a clear energy window (2060 eV) for the efficient encapsulation of Cs through the hexagonal network of SWNT sidewalls without causing significant damage. This minimum energy threshold of Cs-ion encapsulation (∼20 eV) matches well with the value obtained by ab initio simulation (∼22 eV). Furthermore, position-selective Cs encapsulation was carried out, resulting in the successful formation of pn-junction SWNT thin films with excellent environmental stability. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000355495600072 | Publication Date | 2015-05-06 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 3 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2015 IF: 4.772 | |||
| Call Number | c:irua:125928 | Serial | 1760 | ||
| Permanent link to this record | |||||
| Author | Delabie, A.; Sioncke, S.; Rip, J.; van Elshocht, S.; Caymax, M.; Pourtois, G.; Pierloot, K. | ||||
| Title | Mechanisms for the trimethylaluminum reaction in aluminum oxide atomic layer deposition on sulfur passivated germanium | Type | A1 Journal article | ||
| Year | 2011 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 115 | Issue | 35 | Pages | 17523-17532 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Germanium combined with high-κ dielectrics is investigated for the next generations of CMOS devices. Therefore, we study reaction mechanisms for Al2O3 atomic layer deposition on sulfur passivated Ge using calculations based on density functional theory and total reflection X-ray fluorescence (TXRF). TXRF indicates 6 S/nm2 and 4 Al/nm2 after the first TMA/H2O reaction cycle, and growth inhibition from the second reaction cycle on. Calculations are performed on molecular clusters representing −GeSH surface sites. The calculations confirm that the TMA reaction does not affect the S content. On fully SH-terminated Ge, TMA favorably reacts with up to three −GeSH sites, resulting in a near tetrahedral Al coordination. Electron deficient structures with a GeS site shared between two Al atoms are proposed. The impact of the cluster size on the structures and reaction energetics is systematically investigated. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000294386000037 | Publication Date | 2011-08-01 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 9 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2011 IF: 4.805 | |||
| Call Number | UA @ lucian @ c:irua:91714 | Serial | 1980 | ||
| Permanent link to this record | |||||
| Author | Khalilov, U.; Pourtois, G.; Huygh, S.; van Duin, A.C.T.; Neyts, E.C.; Bogaerts, A. | ||||
| Title | New mechanism for oxidation of native silicon oxide | Type | A1 Journal article | ||
| Year | 2013 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 117 | Issue | 19 | Pages | 9819-9825 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Continued miniaturization of metal-oxide-semiconductor field-effect transistors (MOSFETs) requires an ever-decreasing thickness of the gate oxide. The structure of ultrathin silicon oxide films, however, critically depends on the oxidation mechanism. Using reactive atomistic simulations, we here demonstrate how the oxidation mechanism in hyperthermal oxidation of such structures may be controlled by the oxidation temperature and the oxidant energy. Specifically, we study the interaction of hyperthermal oxygen with energies of 15 eV with thin SiOx (x ≤ 2) films with a native oxide thickness of about 10 Å. We analyze the oxygen penetration depth probability and compare with results of the hyperthermal oxidation of a bare Si(100){2 × 1} (c-Si) surface. The temperature-dependent oxidation mechanisms are discussed in detail. Our results demonstrate that, at low (i.e., room) temperature, the penetrated oxygen mostly resides in the oxide region rather than at the SiOx|c-Si interface. However, at higher temperatures, starting at around 700 K, oxygen atoms are found to penetrate and to diffuse through the oxide layer followed by reaction at the c-Si boundary. We demonstrate that hyperthermal oxidation resembles thermal oxidation, which can be described by the DealGrove model at high temperatures. Furthermore, defect creation mechanisms that occur during the oxidation process are also analyzed. This study is useful for the fabrication of ultrathin silicon oxide gate oxides for metal-oxide-semiconductor devices as it links parameters that can be straightforwardly controlled in experiment (oxygen temperature, velocity) with the silicon oxide structure. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000319649100032 | Publication Date | 2013-04-23 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 24 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2013 IF: 4.835 | |||
| Call Number | UA @ lucian @ c:irua:107989 | Serial | 2321 | ||
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| Author | Kolev, I.; Bogaerts, A. | ||||
| Title | Numerical study of the sputtering in a dc magnetron | Type | A1 Journal article | ||
| Year | 2009 | Publication | Journal of vacuum science and technology: A: vacuum surfaces and films | Abbreviated Journal | J Phys Chem C |
| Volume | 27 | Issue | 1 | Pages | 20-28 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Molecular dynamics simulations were used to investigate the size-dependent melting mechanism of nickel nanoclusters of various sizes. The melting process was monitored by the caloric curve, the overall cluster Lindemann index, and the atomic Lindemann index. Size-dependent melting temperatures were determined, and the correct linear dependence on inverse diameter was recovered. We found that the melting mechanism gradually changes from dynamic coexistence melting to surface melting with increasing cluster size. These findings are of importance in better understanding carbon nanotube growth by catalytic chemical vapor deposition as the phase state of the catalyst nanoparticle codetermines the growth mechanism. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | New York, N.Y. | Editor | ||
| Language | Wos | 000263299600018 | Publication Date | 2009-02-03 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 66 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2009 IF: 4.224 | |||
| Call Number | UA @ lucian @ c:irua:71634 | Serial | 2411 | ||
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| Author | Khalilov, U.; Pourtois, G.; van Duin, A.C.T.; Neyts, E.C. | ||||
| Title | On the c-Si\mid a-SiO2 interface in hyperthermal Si oxidation at room temperature | Type | A1 Journal article | ||
| Year | 2012 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 116 | Issue | 41 | Pages | 21856-21863 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | The exact structure and properties of the Si vertical bar SiO2 interface are very important in microelectronics and photovoltaic devices such as metal-oxide-semiconductor field-effect transistors (MOSFETs) and solar cells. Whereas Si vertical bar SiO2 structures are traditionally produced by thermal oxidation, hyperthermal oxidation shows a number of promising advantages. However, the Si vertical bar SiO2 interface induced in hyperthermal Si oxidation has not been properly investigated yet. Therefore, in this work, the interface morphology and interfacial stresses during hyperthermal oxidation at room temperature are studied using reactive molecular dynamics simulations based on the ReaxFF potential. Interface thickness and roughness, as well as the bond length and bond angle distributions in the interface are discussed and compared with other models developed for the interfaces induced by traditional thermal oxidation. The formation of a compressive stress is observed. This compressive stress, which at the interface amounts about 2 GPa, significantly slows down the inward silica growth. This value is close to the experimental value in the Si vertical bar SiO2 interface obtained in traditional thermal oxidation. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000309902100026 | Publication Date | 2012-09-26 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 27 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2012 IF: 4.814 | |||
| Call Number | UA @ lucian @ c:irua:102167 | Serial | 2458 | ||
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| Author | De Bie, C.; van Dijk, J.; Bogaerts, A. | ||||
| Title | The Dominant Pathways for the Conversion of Methane into Oxygenates and Syngas in an Atmospheric Pressure Dielectric Barrier Discharge | Type | A1 Journal article | ||
| Year | 2015 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 119 | Issue | 119 | Pages | 22331-22350 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | A one-dimensional fluid model for a dielectric barrier discharge in CH4/O2 and CH4/CO2 gas mixtures is developed. The model describes the gas-phase chemistry for partial oxidation and for dry reforming of methane. The spatially averaged densities of the various plasma species are presented as a function of time and initial gas mixing ratio. Besides, the conversion of the inlet gases and the selectivities of the reaction products are calculated. Syngas, higher hydrocarbons, and higher oxygenates are typically found to be important reaction products. Furthermore, the main underlying reaction pathways for the formation of syngas, methanol, formaldehyde, and other higher oxygenates are determined. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000362385700010 | Publication Date | 2015-09-10 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 46 | Open Access | |
| Notes | This work was carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI), and the Universiteit Antwerpen. The authors also acknowledge financial support from the IAP/7 (Interuniversity Attraction Pole) program “PSI-Physical Chemistry of Plasma- Surface Interactions” by the Belgian Federal Office for Science Policy (BELSPO) and from the Fund for Scientific Research Flanders (FWO). | Approved | Most recent IF: 4.536; 2015 IF: 4.772 | ||
| Call Number | c:irua:128774 | Serial | 3960 | ||
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| Author | Snoeckx, R.; Aerts, R.; Tu, X.; Bogaerts, A. | ||||
| Title | Plasma-based dry reforming : a computational study ranging from the nanoseconds to seconds time scale | Type | A1 Journal article | ||
| Year | 2013 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 117 | Issue | 10 | Pages | 4957-4970 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | We present a computational study for the conversion of CH4 and CO2 into value-added chemicals, i.e., the so-called dry reforming of methane, in a dielectric barrier discharge reactor. A zero-dimensional chemical kinetics model is applied to study the plasma chemistry in a 1:1 CH4/CO2 mixture. The calculations are first performed for one microdischarge pulse and its afterglow, to study in detail the chemical pathways of the conversion. Subsequently, long time-scale simulations are carried out, corresponding to real residence times in the plasma, assuming a large number of consecutive microdischarge pulses, to mimic the conditions of the filamentary discharge regime in a dielectric barrier discharge (DBD) reactor. The conversion of CH4 and CO2 as well as the selectivity of the formed products and the energy cost and energy efficiency of the process are calculated and compared to experiments for a range of different powers and gas flows, and reasonable agreement is reached. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000316308400010 | Publication Date | 2013-02-18 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 118 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2013 IF: 4.835 | |||
| Call Number | UA @ lucian @ c:irua:106516 | Serial | 2628 | ||
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| Author | Yusupov, M.; Bogaerts, A.; Huygh, S.; Snoeckx, R.; van Duin, A.C.T.; Neyts, E.C. | ||||
| Title | Plasma-induced destruction of bacterial cell wall components : a reactive molecular dynamics simulation | Type | A1 Journal article | ||
| Year | 2013 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 117 | Issue | 11 | Pages | 5993-5998 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Nonthermal atmospheric pressure plasmas are gaining increasing attention for biomedical applications. However, very little fundamental information on the interaction mechanisms between the plasma species and biological cells is currently available. We investigate the interaction of important plasma species, such as OH, H2O2, O, O3, as well as O2 and H2O, with bacterial peptidoglycan by means of reactive molecular dynamics simulations, aiming for a better understanding of plasma disinfection. Our results show that OH, O, O3, and H2O2 can break structurally important bonds of peptidoglycan (i.e., CO, CN, or CC bonds), which consequently leads to the destruction of the bacterial cell wall. The mechanisms behind these breakups are, however, dependent on the impinging plasma species, and this also determines the effectiveness of the cell wall destruction. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Washington, D.C. | Editor | ||
| Language | Wos | 000316773000056 | Publication Date | 2013-02-23 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN |
1932-7447;1932-7455; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | 59 | Open Access | |
| Notes | Approved | Most recent IF: 4.536; 2013 IF: 4.835 | |||
| Call Number | UA @ lucian @ c:irua:107154 | Serial | 2636 | ||
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