NANOlab Center of Excellence literature database -- Query Results

<< 1 2 3 4 5 6 >>

Details

Records
Author	Neyts, E.C.; Brault, P.
Title	Molecular Dynamics Simulations for Plasma-Surface Interactions: Molecular Dynamics Simulations…			Type	A1 Journal article
Year	2017	Publication	Plasma processes and polymers	Abbreviated Journal	Plasma Process Polym
Volume	14	Issue	14	Pages	1600145
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Plasma-surface interactions are in general highly complex due to the interplay of many concurrent processes. Molecular dynamics simulations provide insight in some of these processes, subject to the accessible time and length scales, and the availability of suitable force fields. In this introductory tutorial-style review, we aim to describe the current capabilities and limitations of molecular dynamics simulations in this field, restricting ourselves to low-temperature nonthermal plasmas. Attention is paid to the simulation of the various fundamental processes occurring, including sputtering, etching, implantation, and deposition, as well as to what extent the basic plasma components can be accounted for, including ground state and excited species, electric fields, ions, photons, and electrons. A number of examples is provided, giving an bird’s eye overview of the current state of the field.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000393184600009	Publication Date	2016-09-07
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1612-8850	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	2.846	Times cited	13	Open Access	Not_Open_Access
Notes				Approved	Most recent IF: 2.846
Call Number	PLASMANT @ plasmant @ c:irua:141758			Serial	4488
Permanent link to this record



Author	Schoeters, B.; Neyts, E.C.; Khalilov, U.; Pourtois, G.; Partoens, B.
Title	Stability of Si epoxide defects in Si nanowires : a mixed reactive force field/DFT study			Type	A1 Journal article
Year	2013	Publication	Physical chemistry, chemical physics	Abbreviated Journal	Phys Chem Chem Phys
Volume	15	Issue	36	Pages	15091-15097
Keywords	A1 Journal article; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Modeling the oxidation process of silicon nanowires through reactive force field based molecular dynamics simulations suggests that the formation of Si epoxide defects occurs both at the Si/SiOx interface and at the nanowire surface, whereas for flat surfaces, this defect is experimentally observed to occur only at the interface as a result of stress. In this paper, we argue that the increasing curvature stabilizes the defect at the nanowire surface, as suggested by our density functional theory calculations. The latter can have important consequences for the opto-electronic properties of thin silicon nanowires, since the epoxide induces an electronic state within the band gap. Removing the epoxide defect by hydrogenation is expected to be possible but becomes increasingly difficult with a reduction of the diameter of the nanowires.
Address
Corporate Author				Thesis
Publisher		Place of Publication	Cambridge	Editor
Language		Wos	000323520600029	Publication Date	2013-07-16
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1463-9076;1463-9084;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.123	Times cited	3	Open Access
Notes	; BS gratefully acknowledges financial support of the IWT, Institute for the Promotion of Innovation by Science and Technology in Flanders, via the SBO project “SilaSol”. 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 and the Universiteit Antwerpen. ;			Approved	Most recent IF: 4.123; 2013 IF: 4.198
Call Number	UA @ lucian @ c:irua:110793			Serial	3130
Permanent link to this record



Author	Grubova, I.Y.; Surmeneva, M.A.; Surmenev, R.A.; Neyts, E.C.
Title	Effect of van der Waals interactions on the adhesion strength at the interface of the hydroxyapatite-titanium biocomposite : a first-principles study			Type	A1 Journal article
Year	2020	Publication	RSC advances	Abbreviated Journal
Volume	10	Issue	62	Pages	37800-37805
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Hydroxyapatite (HAP) is frequently used as biocompatible coating on Ti-based implants. In this context, the HAP-Ti adhesion is of crucial importance. Here, we report ab initio calculations to investigate the influence of Si incorporation into the amorphous calcium-phosphate (a-HAP) structure on the interfacial bonding mechanism between the a-HAP coating and an amorphous titanium dioxide (a-TiO2) substrate, contrasting two different density functionals: PBE-GGA, and DFT-D3, which are capable of describing the influence of the van der Waals (vdW) interactions. In particular, we discuss the effect of dispersion on the work of adhesion (W-ad), equilibrium geometries, and charge density difference (CDD). We find that replacement of P by Si in a-HAP (a-Si-HAP) with the creation of OH vacancies as charge compensation results in a significant increase in the bond strength between the coating and substrate in the case of using the PBE-GGA functional. However, including the vdW interactions shows that these forces considerably contribute to the W-ad. We show that the difference (W-ad – W-ad(vdW)) is on average more than 1.1 J m(-2) and 0.5 J m(-2) for a-HAP/a-TiO2 and a-Si-HAP/a-TiO2, respectively. These results reveal that including vdW interactions is essential for accurately describing the chemical bonding at the a-HAP/a-TiO2 interface.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000583523300025	Publication Date	2020-10-14
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN		ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor		Times cited		Open Access
Notes	; The authors gratefully acknowledge financial support from the Russian president's grant MK-330.2020.8 and BOF Fellowships for International Joint PhD students funded by University of Antwerp (UAntwerp, project number 32545). The work was carried out at Tomsk Polytechnic University within the framework of Tomsk Polytechnic University Competitiveness Enhancement Program grant and in part using the Turing HPC infrastructure of the CalcUA core facility of the UAntwerp, a division of the Flemish Supercomputer Centre (VSC), funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerp, Belgium. ;			Approved	Most recent IF: NA
Call Number	UA @ admin @ c:irua:173603			Serial	6499
Permanent link to this record



Author	Nematollahi, P.; Neyts, E.C.
Title	Direct oxidation of methane to methanol on Co embedded N-doped graphene: Comparing the role of N₂O and O₂ as oxidants			Type	A1 Journal article
Year	2020	Publication	Applied Catalysis A-General	Abbreviated Journal	Appl Catal A-Gen
Volume	602	Issue		Pages	117716-10
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	In this work, the effects of N-doping into the Co-doped single vacancy (Co-SV-G) and di-vacancy graphene flake (Co-dV-G) are investigated and compared toward direct oxidation of methane to methanol (DOMM) employing two different oxidants (N2O and O-2) using density functional theory (DFT) calculation. We found that DOMM on CoN3-G utilizing the N2O molecule as oxygen-donor proceeds via a two-step reaction with low activation energies. In addition, we found that although CoN3-G might be a good catalyst for methane conversion, it can also catalyze the oxidation of methanol to CO2 and H2O due to the required low activation barriers. Moreover, the adsorption behaviors of CHx (x = 0-4) species and dehydrogenation of CHx (x = 1-4) species on CoN3-G are investigated. We concluded that CoN3-G can be used as an efficient catalyst for DOMM and N-2O reduction at ambient conditions which may serve as a guide for fabricating effective C/N catalysts in energy-related devices.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000554006800046	Publication Date	2020-06-27
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0926-860x	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	5.5	Times cited		Open Access
Notes	; This work was performed with the financial support from the Doctoral Fund of the Antwerp University (NO. BOFLP33099). All the simulations are performed on resources provided by the high-performance computing center of Antwerp University. ;			Approved	Most recent IF: 5.5; 2020 IF: 4.339
Call Number	UA @ admin @ c:irua:171219			Serial	6485
Permanent link to this record



Author	Dabaghmanesh, S.; Neek-Amal, M.; Partoens, B.; Neyts, E.C.
Title	The formation of Cr₂O₃ nanoclusters over graphene sheet and carbon nanotubes			Type	A1 Journal article
Year	2017	Publication	Chemical physics letters	Abbreviated Journal	Chem Phys Lett
Volume	687	Issue		Pages	188-193
Keywords	A1 Journal article; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract
Address
Corporate Author				Thesis
Publisher		Place of Publication	Amsterdam	Editor
Language		Wos	000412453700030	Publication Date	2017-09-06
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0009-2614	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	1.815	Times cited	2	Open Access	Not_Open_Access: Available from 01.11.2019
Notes	; This work was supported by SIM vzw, Technologiepark 935, BE-9052 Zwijnaarde, Belgium, within the InterPoCo project of the H-INT-S horizontal program. The computational resources and services used in this work were provided by the Vlaams Supercomputer Centrum (VSC) and the HPC infrastructure of the University of Antwerp. ;			Approved	Most recent IF: 1.815
Call Number	UA @ lucian @ c:irua:146646			Serial	4795
Permanent link to this record



Author	Dabaghmanesh, S.; Sarmadian, N.; Neyts, E.C.; Partoens, B.
Title	A first principles study of p-type defects in LaCrO₃			Type	A1 Journal article
Year	2017	Publication	Physical chemistry, chemical physics	Abbreviated Journal	Phys Chem Chem Phys
Volume	19	Issue	34	Pages	22870-22876
Keywords	A1 Journal article; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Recently, Sr-doped LaCrO3 has been experimentally introduced as a new p-type transparent conducting oxide. It is demonstrated that substituting Sr for La results in inducing p-type conductivity in LaCrO3. Performing first principles calculations we study the electronic structure and formation energy of various point defects in LaCrO3. Our results for the formation energies show that in addition to Sr, two more divalent defects, Ca and Ba, substituting for La in LaCrO3, behave as shallow acceptors in line with previous experimental reports. We further demonstrate that under oxygen-poor growth conditions, these shallow acceptors will be compensated by intrinsic donor-like defects (an oxygen vacancy and Cr on an oxygen site), but in the oxygen-rich growth regime the shallow acceptors have the lowest formation energies between all considered defects and will lead to p-type conductivity.
Address
Corporate Author				Thesis
Publisher		Place of Publication	Cambridge	Editor
Language		Wos	000408671600026	Publication Date	2017-08-01
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1463-9076; 1463-9084	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.123	Times cited	16	Open Access	OpenAccess
Notes	; This work was supported by SIM vzw, Technologiepark 935, BE-9052 Zwijnaarde, Belgium, within the InterPoCo project of the H-INT-S horizontal program. The computational resources and services were provided by the Flemish Supercomputer Center and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government. ;			Approved	Most recent IF: 4.123
Call Number	UA @ lucian @ c:irua:145621			Serial	4735
Permanent link to this record



Author	Dabaghmanesh, S.; Neyts, E.C.; Partoens, B.
Title	van der Waals density functionals applied to corundum-type sesquioxides : bulk properties and adsorption of CH₃ and C₆H₆ on (0001) surfaces			Type	A1 Journal article
Year	2016	Publication	Physical chemistry, chemical physics	Abbreviated Journal	Phys Chem Chem Phys
Volume	18	Issue	18	Pages	23139-23146
Keywords	A1 Journal article; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	van der Waals (vdW) forces play an important role in the adsorption of molecules on the surface of solids. However, the choice of the most suitable vdW functional for different systems is an essential problem which must be addressed for different systems. The lack of a systematic study on the performance of the vdW functionals in the bulk and adsorption properties of metal-oxides motivated us to examine different vdW approaches and compute the bulk and molecular adsorption properties of alpha-Cr2O3, alpha-Fe2O3, and alpha-Al2O3. For the bulk properties, we compared our results for the heat of formation, cohesive energy, lattice parameters and bond distances between the different vdW functionals and available experimental data. Next we studied the adsorption of benzene and CH3 molecules on top of different oxide surfaces. We employed different approximations to exchange and correlation within DFT, namely, the Perdew-Burke-Ernzerhof (PBE) GGA, (PBE)+U, and vdW density functionals [ DFT(vdW-DF/DF2/optPBE/optB86b/optB88)+U] as well as DFT-D2/D3(+U) methods of Grimme for the bulk calculations and optB86b-vdW(+U) and DFT-D2(+U) for the adsorption energy calculations. Our results highlight the importance of vdW interactions not only in the adsorption of molecules, but importantly also for the bulk properties. Although the vdW contribution in the adsorption of CH3 (as a chemisorption interaction) is less important compared to the adsorption of benzene (as a physisorption interaction), this contribution is not negligible. Also adsorption of benzene on ferryl/chromyl terminated surfaces shows an important chemisorption contribution in which the vdW interactions become less significant.
Address
Corporate Author				Thesis
Publisher		Place of Publication	Cambridge	Editor
Language		Wos	000382109300040	Publication Date	2016-07-27
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1463-9076; 1463-9084	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.123	Times cited	6	Open Access
Notes	; This work was supported by the Strategic Initiative Materials in Flanders (SIM). The computational resources and services used in this work were provided by the Vlaams Supercomputer Centrum (VSC) and the HPC infrastructure of the University of Antwerp. ;			Approved	Most recent IF: 4.123
Call Number	UA @ lucian @ c:irua:135701			Serial	4311
Permanent link to this record



Author	Nematollahi, P.; Barbiellini, B.; Bansil, A.; Lamoen, D.; Qingying, J.; Mukerjee, S.; Neyts, E.C.
Title	Identification of a Robust and Durable FeN₄C_xCatalyst for ORR in PEM Fuel Cells and the Role of the Fifth Ligand			Type	A1 Journal article
Year	2022	Publication	ACS catalysis	Abbreviated Journal	Acs Catal
Volume		Issue		Pages	7541-7549
Keywords	A1 Journal article; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Although recent studies have advanced the understanding of pyrolyzed Fe−N−C materials as oxygen reduction reaction (ORR) catalysts, the atomic and electronic structures of the active sites and their detailed reaction mechanisms still remain unknown. Here, based on first-principles density functional theory (DFT) computations, we discuss the electronic structures of three FeN4 catalytic centers with different local topologies of the surrounding C atoms with a focus on unraveling the mechanism of their ORR activity in acidic electrolytes. Our study brings back a forgotten, synthesized pyridinic Fe−N coordinate to the community’s attention, demonstrating that this catalyst can exhibit excellent activity for promoting direct four-electron ORR through the addition of a fifth ligand such as −NH2, −OH, and −SO4. We also identify sites with good stability properties through the combined use of our DFT calculations and Mössbauer spectroscopy data.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000823193100001	Publication Date	2022-06-10
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	2155-5435	ISBN		Additional Links	UA library record; WoS full record; WoS full record; WoS citing articles
Impact Factor	12.9	Times cited		Open Access	OpenAccess
Notes	Basic Energy Sciences, DE-FG02-07ER46352 ; Fonds Wetenschappelijk Onderzoek, 1261721N ; Opetus- ja Kulttuuriministeri?; Department of Energy, DE-EE0008416 ;			Approved	Most recent IF: 12.9
Call Number	EMAT @ emat @c:irua:189000			Serial	7073
Permanent link to this record



Author	Engelmann, Y.; van ’t Veer, K.; Gorbanev, Y.; Neyts, E.C.; Schneider, W.F.; Bogaerts, A.
Title	Plasma Catalysis for Ammonia Synthesis: A Microkinetic Modeling Study on the Contributions of Eley–Rideal Reactions			Type	A1 Journal Article;Plasma catalysis
Year	2021	Publication	Acs Sustainable Chemistry & Engineering	Abbreviated Journal	Acs Sustain Chem Eng
Volume	9	Issue	39	Pages	13151-13163
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) ;
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.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000705367800004	Publication Date	2021-10-04
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	2168-0485	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	5.951	Times cited		Open Access	OpenAccess
Notes	Basic Energy Sciences, DE-SC0021107 ; Vlaamse regering, HBC.2019.0108 ; H2020 European Research Council, 810182 ; Methusalem project – University of Antwerp; Excellence of science FWO-FNRS, GoF9618n ; TOP-BOF – University of Antwerp; DOCPRO3 – University of Antwerp; We acknowledge the ﬁnancial support from the DOC-PRO3, the TOP-BOF, and the Methusalem project of the University of Antwerp, as well as from the European Research Council (ERC) (grant agreement No, 810182−SCOPE ERC Synergy project), under the European Union’s Horizon 2020 research and innovation programme, the Flemish Government through the Moonshot cSBO project P2C (HBC.2019.0108), and the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023). 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), 13162			Approved	Most recent IF: 5.951
Call Number	PLASMANT @ plasmant @c:irua:182482			Serial	6811
Permanent link to this record



Author	Jafarzadeh, A.; Bal, K.M.; Bogaerts, A.; Neyts, E.C.
Title	Activation of CO₂on Copper Surfaces: The Synergy between Electric Field, Surface Morphology, and Excess Electrons			Type	A1 Journal article
Year	2020	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
Volume	124	Issue	12	Pages	6747-6755
Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	In this work, we use density functional theory calculations to study the combined eﬀect of external electric ﬁelds, surface morphology, and surface charge on CO2 activation over Cu(111), Cu(211), Cu(110), and Cu(001) surfaces. We observe that the binding energy of the CO2 molecule on Cu surfaces increases signiﬁcantly upon increasing the applied electric ﬁeld strength. In addition, rougher surfaces respond more eﬀectively to the presence of the external electric ﬁeld toward facilitating the formation of a carbonate-like CO2 structure and the transformation of the most stable adsorption mode from physisorption to chemisorption. The presence of surface charges further strengthens the electric ﬁeld eﬀect and consequently causes an improved bending of the CO2 molecule and C−O bond length elongation. On the other hand, a net charge in the absence of an externally applied electric ﬁeld shows only a marginal eﬀect on CO2 binding. The chemisorbed CO2 is more stable and further activated when the eﬀects of an external electric ﬁeld, rough surface, and surface charge are combined. These results can help to elucidate the underlying factors that control CO2 activation in heterogeneous and plasma catalysis, as well as in electrochemical processes.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000526396900030	Publication Date	2020-03-26
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
Notes	Bijzonder Onderzoeksfonds, 32249 ; The ﬁnancial support from the TOP research project of the Research Fund of the University of Antwerp (grant ID: 32249) is highly acknowledged by the authors. The computational resources used in this study were provided by the VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Governmentdepartment EWI.			Approved	Most recent IF: 3.7; 2020 IF: 4.536
Call Number	PLASMANT @ plasmant @c:irua:168606			Serial	6361
Permanent link to this record



Author	Verlackt, C.C.W.; Neyts, E.C.; Jacob, T.; Fantauzzi, D.; Golkaram, M.; Shin, Y.-K.; van Duin, A.C.T.; Bogaerts, A.
Title	Atomic-scale insight into the interactions between hydroxyl radicals and DNA in solution using the ReaxFF reactive force field			Type	A1 Journal article
Year	2015	Publication	New journal of physics	Abbreviated Journal	New J Phys
Volume	17	Issue	17	Pages	103005
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Cold atmospheric pressure plasmas have proven to provide an alternative treatment of cancer by targeting tumorous cells while leaving their healthy counterparts unharmed. However, the underlying mechanisms of the plasma–cell interactions are not yet fully understood. Reactive oxygen species, and in particular hydroxyl radicals (OH), are known to play a crucial role in plasma driven apoptosis of malignant cells. In this paper we investigate the interaction of OH radicals, as well as H2O2 molecules and HO2 radicals, with DNA by means of reactive molecular dynamics simulations using the ReaxFF force field. Our results provide atomic-scale insight into the dynamics of oxidative stress on DNA caused by the OH radicals, while H2O2 molecules appear not reactive within the considered timescale. Among the observed processes are the formation of 8-OH-adduct radicals, forming the first stages towards the formation of 8-oxoGua and 8-oxoAde, H-abstraction reactions of the amines, and the partial opening of loose DNA ends in aqueous solution.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000367328100001	Publication Date	2015-10-02
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1367-2630;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	3.786	Times cited	18	Open Access
Notes	CCWV,ECN and AB acknowledge the contribution of J Van Beeck who is investigating the interaction between H2O2 andDNAusingrMDsimulations. Furthermore, they acknowledge financial support from the Fund for Scientific Research—Flanders (project number G012413N). The calculations were performed using the Turing HPCinfrastructure 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. TJ and DF gratefully acknowledge support from the European Research Council through the ERC-Starting GrantTHEOFUN(Grant Agreement No. 259608).			Approved	Most recent IF: 3.786; 2015 IF: 3.558
Call Number	c:irua:129178			Serial	3955
Permanent link to this record



Author	Berdiyorov, G.R.; Khalilov, U.; Hamoudi, H.; Neyts, E.C.
Title	Effect of chemical modification on electronic transport properties of carbyne			Type	A1 Journal article
Year	2021	Publication	Journal Of Computational Electronics	Abbreviated Journal	J Comput Electron
Volume		Issue		Pages
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Using density functional theory in combination with the Green’s functional formalism, we study the effect of surface functionalization on the electronic transport properties of 1D carbon allotrope—carbyne. We found that both hydrogenation and fluorination result in structural changes and semiconducting to metallic transition. Consequently, the current in the functionalization systems increases significantly due to strong delocalization of electronic states along the carbon chain. We also study the electronic transport in partially hydrogenated carbyne and interface structures consisting of pristine and functionalized carbyne. In the latter case, current rectification is obtained in the system with rectification ratio up to 50%. These findings can be useful for developing carbyne-based structures with tunable electronic transport properties.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000617664900001	Publication Date	2021-02-13
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1569-8025	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	1.526	Times cited		Open Access	OpenAccess
Notes	Computational resources were provided by the research computing facilities of Qatar Environment and Energy Research Institute. Calculations are also conducted using the Turing HPC infrastructure of the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Centre VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the University of Antwerp. U. Khalilov gratefully acknowledges financial support from the Fund of Scientific Research Flanders (FWO), Belgium, Grant number 12M1315N.			Approved	Most recent IF: 1.526
Call Number	PLASMANT @ plasmant @c:irua:176169			Serial	6708
Permanent link to this record



Author	Marinov, D.; de Marneffe, J.-F.; Smets, Q.; Arutchelvan, G.; Bal, K.M.; Voronina, E.; Rakhimova, T.; Mankelevich, Y.; El Kazzi, S.; Nalin Mehta, A.; Wyndaele, P.-J.; Heyne, M.H.; Zhang, J.; With, P.C.; Banerjee, S.; Neyts, E.C.; Asselberghs, I.; Lin, D.; De Gendt, S.
Title	Reactive plasma cleaning and restoration of transition metal dichalcogenide monolayers			Type	A1 Journal article
Year	2021	Publication	npj 2D Materials and Applications	Abbreviated Journal	npj 2D Mater Appl
Volume	5	Issue	1	Pages	17
Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	The cleaning of two-dimensional (2D) materials is an essential step in the fabrication of future devices, leveraging their unique physical, optical, and chemical properties. Part of these emerging 2D materials are transition metal dichalcogenides (TMDs). So far there is limited understanding of the cleaning of “monolayer” TMD materials. In this study, we report on the use of downstream H<sub>2</sub>plasma to clean the surface of monolayer WS<sub>2</sub>grown by MOCVD. We demonstrate that high-temperature processing is essential, allowing to maximize the removal rate of polymers and to mitigate damage caused to the WS<sub>2</sub>in the form of sulfur vacancies. We show that low temperature in situ carbonyl sulfide (OCS) soak is an efficient way to resulfurize the material, besides high-temperature H<sub>2</sub>S annealing. The cleaning processes and mechanisms elucidated in this work are tested on back-gated field-effect transistors, confirming that transport properties of WS<sub>2</sub>devices can be maintained by the combination of H<sub>2</sub>plasma cleaning and OCS restoration. The low-damage plasma cleaning based on H<sub>2</sub>and OCS is very reproducible, fast (completed in a few minutes) and uses a 300 mm industrial plasma etch system qualified for standard semiconductor pilot production. This process is, therefore, expected to enable the industrial scale-up of 2D-based devices, co-integrated with silicon technology.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000613258900001	Publication Date	2021-01-28
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	2397-7132	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor		Times cited		Open Access	OpenAccess
Notes	Daniil Marinov has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No 752164. Ekaterina Voronina, Yuri Mankelevitch, and Tatyana Rakhimova are thankful to the Russian Science Foundation (RSF) for financial support (Grant No. 16-12-10361). This study was carried out using the equipment of the shared research facilities of high-performance computing resources at Lomonosov Moscow State University and the computational resources and services of the HPC core facility CalcUA of the University of Antwerp, and VSC (Flemish Supercomputer Center), funded by the Research Foundation-Flanders (FWO) and the Flemish Government. Patrick With gratefully acknowledges imec’s CTO office for financial support during his stay at imec. The authors thank Mr. Surajit Sutar (imec) for his help during sample electrical characterization, and Patrick Verdonck for lab processing. Jean-François de Marneffe thank Prof. Simone Napolitano from the Free University of Brussels for useful discussions on irreversibly adsorbed polymer layers, and Cédric Huyghebaert (imec) for his continuous support in the framework of the Graphene FET Flagship core project. All authors acknowledge the support of imec’s pilot line and materials characterization and analysis (MCA) group, namely Jonathan Ludwig, Stefanie Sergeant, Thomas Nuytten, Olivier Richard, and Thierry Conard. Finally, Daniil Marinov thank Mikhail Krishtab (imec/KU Leuven) for his help in selecting the optimal plasma etch system for this work. Part of this project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 649953.			Approved	Most recent IF: NA
Call Number	PLASMANT @ plasmant @c:irua:175871			Serial	6671
Permanent link to this record



Author	Aussems, D.U.B.; Bal, K.M.; Morgan, T.W.; van de Sanden, M.C.M.; Neyts, E.C.
Title	Mechanisms of elementary hydrogen ion-surface interactions during multilayer graphene etching at high surface temperature as a function of flux			Type	A1 Journal article
Year	2018	Publication	Carbon	Abbreviated Journal	Carbon
Volume	137	Issue		Pages	527-532
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	In order to optimize the plasma-synthesis and modification process of carbon nanomaterials for applications such as nanoelectronics and energy storage, a deeper understanding of fundamental hydrogengraphite/graphene interactions is required. Atomistic simulations by Molecular Dynamics have proven to be indispensable to illuminate these phenomena. However, severe time-scale limitations restrict them to very fast processes such as reflection, while slow thermal processes such as surface diffusion and molecular desorption are commonly inaccessible. In this work, we could however reach these thermal processes for the first time at time-scales and surface temperatures (1000 K) similar to high-flux plasma exposure experiments during the simulation of multilayer graphene etching by 5 eV H ions. This was achieved by applying the Collective Variable-Driven Hyperdynamics biasing technique, which extended the inter-impact time over a range of six orders of magnitude, down to a more realistic ion-flux of 1023m2s1. The results show that this not only causes a strong shift from predominant ion-to thermally induced interactions, but also significantly affects the hydrogen uptake and surface evolution. This study thus elucidates H ion-graphite/graphene interaction mechanisms and stresses the importance of including long time-scales in atomistic simulations at high surface temperatures to understand the dynamics of the ion-surface system.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000440661700056	Publication Date	2018-05-24
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0008-6223	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	6.337	Times cited	4	Open Access	Not_Open_Access: Available from 25.05.2020
Notes	DIFFER is part of the Netherlands Organisation for Scientific Research (NWO). K.M.B. is funded as PhD fellow (aspirant) of the FWO-Flanders (Fund for Scientific Research-Flanders), Grant 11V8915N. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Government e department EWI.			Approved	Most recent IF: 6.337
Call Number	PLASMANT @ plasmant @c:irua:152172			Serial	4993
Permanent link to this record



Author	Aussems, D.U.B.; Bal, K. M.; Morgan, T.W.; van de Sanden, M.C.M.; Neyts, E.C.
Title	Atomistic simulations of graphite etching at realistic time scales			Type	A1 Journal article
Year	2017	Publication	Chemical science	Abbreviated Journal	Chem Sci
Volume	8	Issue	10	Pages	7160-7168
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Hydrogen–graphite interactions are relevant to a wide variety of applications, ranging from astrophysics to fusion devices and nano-electronics. In order to shed light on these interactions, atomistic simulation using Molecular Dynamics (MD) has been shown to be an invaluable tool. It suffers, however, from severe timescale limitations. In this work we apply the recently developed Collective Variable-Driven Hyperdynamics (CVHD) method to hydrogen etching of graphite for varying inter-impact times up to a realistic value of 1 ms, which corresponds to a flux of 1020 m2 s1. The results show that the erosion yield, hydrogen surface coverage and species distribution are significantly affected by the time between impacts. This can be explained by the higher probability of C–C bond breaking due to the prolonged exposure to thermal stress and the subsequent transition from ion- to thermal-induced etching. This latter regime of thermal-induced etching – chemical erosion – is here accessed for the first time using atomistic simulations. In conclusion, this study demonstrates that accounting for long time-scales significantly affects ion bombardment simulations and should not be neglected in a wide range of conditions, in contrast to what is typically assumed.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000411730500055	Publication Date	2017-08-24
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	2041-6520	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	8.668	Times cited	3	Open Access	OpenAccess
Notes	DIFFER is part of the Netherlands Organisation for Scientic Research (NWO). K. M. B. is funded as a PhD fellow (aspirant) of the FWO-Flanders (Fund for Scientic Research-Flanders), Grant 11V8915N. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government – department EWI.			Approved	Most recent IF: 8.668
Call Number	PLASMANT @ plasmant @c:irua:145519			Serial	4707
Permanent link to this record



Author	Neyts, E.C.; Ostrikov, K.K.; Sunkara, M.K.; Bogaerts, A.
Title	Plasma Catalysis: Synergistic Effects at the Nanoscale			Type	A1 Journal article
Year	2015	Publication	Chemical reviews	Abbreviated Journal	Chem Rev
Volume	115	Issue	115	Pages	13408-13446
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Thermal-catalytic gas processing is integral to many current industrial processes. Ever-increasing demands on conversion and energy efficiencies are a strong driving force for the development of alternative approaches. Similarly, synthesis of several functional materials (such as nanowires and nanotubes) demands special processing conditions. Plasma catalysis provides such an alternative, where the catalytic process is complemented by the use of plasmas that activate the source gas. This combination is often observed to result in a synergy between plasma and catalyst. This Review introduces the current state-of-the-art in plasma catalysis, including numerous examples where plasma catalysis has demonstrated its benefits or shows future potential, including CO2 conversion, hydrocarbon reforming, synthesis of nanomaterials, ammonia production, and abatement of toxic waste gases. The underlying mechanisms governing these applications, as resulting from the interaction between the plasma and the catalyst, render the process highly complex, and little is known about the factors leading to the often-observed synergy. This Review critically examines the catalytic mechanisms relevant to each specific application.
Address	Department of Chemistry, Research Group PLASMANT, Universiteit Antwerpen , Universiteitsplein 1, 2610 Wilrijk-Antwerp, Belgium
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language	English	Wos	000367563000006	Publication Date	2015-11-30
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0009-2665	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	47.928	Times cited	204	Open Access
Notes	ECN and AB gratefully acknowledge financial support from the Fund of Scientific Research Flanders (FWO), Belgium, Grant Number G.0217.14N. KO acknowledges partial support by the Australian Research Council and CSIRO’s OCE Science Leaders Program. MKS acknowledges partial support from US National Science Foundation through grants DMS 1125909 and EPSCoR 1355448 and also PhD students Babajide Ajayi, Apolo Nambo and Maria Carreon for their help.			Approved	Most recent IF: 47.928; 2015 IF: 46.568
Call Number	c:irua:130001			Serial	3993
Permanent link to this record



Author	Huygh, S.; Bogaerts, A.; Bal, K.M.; Neyts, E.C.
Title	High Coke Resistance of a TiO₂Anatase (001) Catalyst Surface during Dry Reforming of Methane			Type	A1 Journal Article
Year	2018	Publication	Journal Of Physical Chemistry C	Abbreviated Journal	J Phys Chem C
Volume	122	Issue	17	Pages	9389-9396
Keywords	A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract	The resistance of a TiO2 anatase (001) surface to coke formation was studied in the context of dry reforming of methane using density functional theory (DFT) calculations. As carbon atoms act as precursors for coke formation, the resistance to coke formation can be measured by the carbon coverage of the surface. This is related to the stability of different CHx (x = 0−3) species and their rate of hydrogenation and dehydrogenation on the TiO2 surface. Therefore, we studied the reaction mechanisms and their corresponding rates as a function of the temperature for the dehydrogenation of the species on the surface. We found that the stabilities of C and CH are significantly lower than those of CH3 and CH2. The hydrogenation rates of the different species are significantly higher than the dehydrogenation rates in a temperature range of 300−1000 K. Furthermore, we found that dehydrogenation of CH3, CH2, and CH will only occur at appreciable rates starting from 600, 900, and 900 K, respectively. On the basis of these results, it is clear that the anatase (001) surface has a high coke resistance, and it is thus not likely that the surface will become poisoned by coke during dry reforming of methane. As the rate limiting step in dry reforming is the dissociative adsorption of CH4, we studied an alternative approach to thermal catalysis. We found that the temperature threshold for dry reforming is at least 700 K. This threshold temperature may be lowered by the use of plasma-catalysis, where the appreciable rates of adsorption of plasma-generated CHx radicals result in bypassing the rate limiting step of the reaction.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000431723700014	Publication Date	2018-05-03
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.536	Times cited	1	Open Access	OpenAccess
Notes	Federaal Wetenschapsbeleid, IAP/7 ; Fonds Wetenschappelijk Onderzoek, G.0217.14N ; Onderzoeksfonds, Universiteit Antwerpen, 32249 ;			Approved	Most recent IF: 4.536
Call Number	PLASMANT @ plasmant @c:irua:151529c:irua:152816			Serial	5000
Permanent link to this record



Author	Shirazi, M.; Bogaerts, A.; Neyts, E.C.
Title	A DFT study of H-dissolution into the bulk of a crystalline Ni(111) surface: a chemical identifier for the reaction kinetics			Type	A1 Journal article
Year	2017	Publication	Physical chemistry, chemical physics	Abbreviated Journal	Phys Chem Chem Phys
Volume	19	Issue	19	Pages	19150-19158
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	In this study, we investigated the diffusion of H-atoms to the subsurface and their further diffusion into the bulk of a Ni(111) crystal by means of density functional theory calculations in the context of thermal and plasma-assisted catalysis. The H-atoms at the surface can originate from the dissociative adsorption of H2 or CH4 molecules, determining the surface H-coverage. When a threshold H-coverage is passed, corresponding to 1.00 ML for the crystalline Ni(111) surface, the surface-bound H-atoms start to diffuse to the subsurface. A similar threshold coverage is observed for the interstitial H-coverage. Once the interstitial sites are filled up with a coverage above 1.00 ML of H, dissolution of interstitial H-atoms to the layer below the interstitial sites will be initiated. Hence, by applying a high pressure or inducing a reactive plasma and high temperature, increasing the H-flux to the surface, a large amount of hydrogen can diffuse in a crystalline metal like Ni and can be absorbed. The formation of metal hydride may modify the entire reaction kinetics of the system. Equivalently, the H-atoms in the bulk can easily go back to the surface and release a large amount of heat. In a plasma process, H-atoms are formed in the plasma, and therefore the energy barrier for dissociative adsorption is dismissed, thus allowing achievement of the threshold coverage without applying a high pressure as in a thermal process. As a result, depending on the crystal plane and type of metal, a large number of H-atoms can be dissolved (absorbed) in the metal catalyst, explaining the high efficiency of plasma-assisted catalytic reactions. Here, the mechanism of H-dissolution is established as a chemical identifier for the investigation of the reaction kinetics of a chemical process.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000406334300034	Publication Date	2017-06-22
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1463-9076	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.123	Times cited	10	Open Access	OpenAccess
Notes	Financial support from the Reactive Atmospheric Plasma processIng – eDucation (RAPID) network, through the EU 7th Framework Programme (grant agreement no. 606889), is gratefully acknowledged. The calculations were performed 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.			Approved	Most recent IF: 4.123
Call Number	PLASMANT @ plasmant @ c:irua:144794			Serial	4633
Permanent link to this record



Author	Shirazi, M.; Neyts, E.C.; Bogaerts, A.
Title	DFT study of Ni-catalyzed plasma dry reforming of methane			Type	A1 Journal article
Year	2017	Publication	Applied catalysis : B : environmental	Abbreviated Journal	Appl Catal B-Environ
Volume	205	Issue	205	Pages	605-614
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	tWe investigated the plasma-assisted catalytic reactions for the production of value-added chemicalsfrom Ni-catalyzed plasma dry reforming of methane by means of density functional theory (DFT). Weinspected many activation barriers, from the early stage of adsorption of the major chemical fragmentsderived fromCH4andCO2molecules up to the formation of value-added chemicals at the surface, focusingon the formation of methanol, as well as the hydrogenation of C1and C2hydrocarbon fragments. Theactivation barrier calculations show that the presence of surface-bound H atoms and in some cases alsoremaining chemical fragments at the surface facilitates the formation of products. This implies that thehydrogenation of a chemical fragment on the hydrogenated crystalline surface is energetically favouredcompared to the simple hydrogenation of the chemical fragment at the bare Ni(111) surface. Indeed, thepresence of hydrogen modifies the electronic structure of the surface and the course of the reactions.We therefore conclude that surface-bound H atoms, and to some extent also the remaining chemicalfragments at the crystalline surface, induce the following effects: they facilitate associative desorption ofmethanol and ethane by increasing the rate of H-transfer to the adsorbed fragments while they impedehydrogenation of ethylene to ethane, thus promoting again the desorption of ethylene. Overall, they thusfacilitate the catalytic conversion of the formed fragments from CH4and CO2, into value-added chemicals.Finally, we believe that the retention of methane fragments, especially CH3, in the presence of surface-boundHatoms (as observed here for Ni) can be regarded as an identifier for the proper choice of a catalystfor the production of value-added chemicals.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000393931000063	Publication Date	2017-01-05
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0926-3373	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	9.446	Times cited	26	Open Access	OpenAccess
Notes	Financial support from the Reactive Atmospheric Plasmaprocessing –eDucation network (RAPID), through the EU 7thFramework Programme (grant agreement no. 606889) is grate-fully acknowledged. The calculations were performed using theTuring HPC infrastructure at the CalcUA core facility of the Univer-siteit Antwerpen, a division of the Flemish Supercomputer CenterVSC, funded by the Hercules Foundation, the Flemish			Approved	Most recent IF: 9.446
Call Number	PLASMANT @ plasmant @ c:irua:139514			Serial	4343
Permanent link to this record



Author	Bal, K.M.; Neyts, E.C.
Title	Overcoming Old Scaling Relations and Establishing New Correlations in Catalytic Surface Chemistry: Combined Effect of Charging and Doping			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	10	Pages	6141-6147
Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Optimization of catalytic materials for a given application is greatly constrained by linear scaling relations. Recently, however, it has been demonstrated that it is possible to reversibly modulate the chemisorption of molecules on nanomaterials by charging (i.e., injection or removal of electrons) and hence reversibly and selectively modify catalytic activity beyond structure−activity correlations. The fundamental physical relation between the properties of the material, the charging process, and the chemisorption energy, however, remains unclear, and a systematic exploration and optimization of charge-switchable sorbent materials is not yet possible. Using hybrid DFT calculations of CO2 chemisorption on hexagonal boron nitride nanosheets with several types of defects and dopants, we here reveal the existence of fundamental correlations between the electron aﬃnity of a material and charge-induced chemisorption, show how defect engineering can be used to modulate the strength and eﬃciency of the adsorption process, and demonstrate that excess electrons stabilize many topological defects. We then show how these insights could be exploited in the development of new electrocatalytic materials and the synthesis of doped nanomaterials. Moreover, we demonstrate that calculated chemical properties of charged materials are highly sensitive to the employed computational methodology because of the self-interaction error, which underlines the theoretical challenge posed by such systems.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000461537400035	Publication Date	2019-03-14
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.536	Times cited	5	Open Access	Not_Open_Access: Available from 21.02.2020
Notes	Fonds Wetenschappelijk Onderzoek, 11V8915N ;			Approved	Most recent IF: 4.536
Call Number	PLASMANT @ plasmant @UA @ admin @ c:irua:158117			Serial	5160
Permanent link to this record



Author	Razzokov, J.; Yusupov, M.; Vanuytsel, S.; Neyts, E.C.; Bogaerts, A.
Title	Phosphatidylserine flip-flop induced by oxidation of the plasma membrane: a better insight by atomic scale modeling			Type	A1 Journal article
Year	2017	Publication	Plasma processes and polymers	Abbreviated Journal	Plasma Process Polym
Volume	14	Issue	10	Pages	1700013
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	We perform molecular dynamics simulations to study the flip-flop motion of phosphatidylserine (PS) across the plasma membrane upon increasing oxidation degree of the membrane. Our computational results show that an increase of the oxidation degree in the lipids leads to a decrease of the free energy barrier for translocation of PS through the membrane. In other words, oxidation of the lipids facilitates PS flip-flop motion across the membrane, because in native phospholipid bilayers this is only a “rare event” due to the high energy barriers for the translocation of PS. The present study provides an atomic-scale insight into the mechanisms of the PS flip-flop upon oxidation of lipids, as produced for example by cold atmospheric plasma, in living cells.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000413045800010	Publication Date	2017-04-05
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1612-8850	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	2.846	Times cited	9	Open Access	Not_Open_Access
Notes	Fonds Wetenschappelijk Onderzoek, 1200216N ;			Approved	Most recent IF: 2.846
Call Number	PLASMANT @ plasmant @c:irua:149567			Serial	4910
Permanent link to this record



Author	Khalilov, U.; Bogaerts, A.; Neyts, E.C.
Title	Toward the Understanding of Selective Si Nano-Oxidation by Atomic Scale Simulations			Type	A1 Journal article
Year	2017	Publication	Accounts of chemical research	Abbreviated Journal	Accounts Chem Res
Volume	50	Issue	50	Pages	796-804
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	The continuous miniaturization of nanodevices, such as transistors, solar cells, and optical fibers, requires the controlled synthesis of (ultra)thin gate oxides (<10 nm), including Si gate-oxide (SiO2) with high quality at the atomic scale. Traditional thermal growth of SiO2 on planar Si surfaces, however, does not allow one to obtain such ultrathin oxide due to either the high oxygen diffusivity at high temperature or the very low sticking ability of incident oxygen at low temperature. Two recent techniques, both operative at low (room) temperature, have been put forward to overcome these obstacles: (i) hyperthermal oxidation of planar Si surfaces and (ii) thermal or plasma-assisted oxidation of nonplanar Si surfaces, including Si nanowires (SiNWs). These nanooxidation processes are, however, often difficult to study experimentally, due to the key intermediate processes taking place on the nanosecond time scale. In this Account, these Si nano-oxidation techniques are discussed from a computational point of view and compared to both hyperthermal and thermal oxidation experiments, as well as to well-known models of thermal oxidation, including the Deal−Grove, Cabrera−Mott, and Kao models and several alternative mechanisms. In our studies, we use reactive molecular dynamics (MD) and hybrid MD/Monte Carlo simulation techniques, applying the Reax force field. The incident energy of oxygen species is chosen in the range of 1−5 eV in hyperthermal oxidation of planar Si surfaces in order to prevent energy-induced damage. It turns out that hyperthermal growth allows for two growth modes, where the ultrathin oxide thickness depends on either (1) only the kinetic energy of the incident oxygen species at a growth temperature below Ttrans = 600 K, or (2) both the incident energy and the growth temperature at a growth temperature above Ttrans. These modes are specific to such ultrathin oxides, and are not observed in traditional thermal oxidation, nor theoretically considered by already existing models. In the case of thermal or plasma-assisted oxidation of small Si nanowires, on the other hand, the thickness of the ultrathin oxide is a function of the growth temperature and the nanowire diameter. Below Ttrans, which varies with the nanowire diameter, partially oxidized SiNW are formed, whereas complete oxidation to a SiO2 nanowire occurs only above Ttrans. In both nano-oxidation processes at lower temperature (T < Ttrans), final sandwich c-Si\|SiOx\|a-SiO2 structures are obtained due to a competition between overcoming the energy barrier to penetrate into Si subsurface layers and the compressive stress (∼2−3 GPa) at the Si crystal/oxide interface. The overall atomic-simulation results strongly indicate that the thickness of the intermediate SiOx (x < 2) region is very limited (∼0.5 nm) and constant irrespective of oxidation parameters. Thus, control over the ultrathin SiO2 thickness with good quality is indeed possible by accurately tuning the oxidant energy, oxidation temperature and surface curvature. In general, we discuss and put in perspective these two oxidation mechanisms for obtaining controllable ultrathin gate-oxide films, offering a new route toward the fabrication of nanodevices via selective nano-oxidation.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000399859800016	Publication Date	2017-04-18
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0001-4842	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	20.268	Times cited	5	Open Access	OpenAccess
Notes	Fonds Wetenschappelijk Onderzoek, 12M1315N ;			Approved	Most recent IF: 20.268
Call Number	PLASMANT @ plasmant @ c:irua:142638			Serial	4561
Permanent link to this record



Author	Khalilov, U.; Vets, C.; Neyts, E.C.
Title	Molecular evidence for feedstock-dependent nucleation mechanisms of CNTs			Type	A1 Journal article
Year	2019	Publication	Nanoscale Horizons	Abbreviated Journal	Nanoscale Horiz.
Volume	4	Issue	3	Pages	674-682
Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Atomic scale simulations have been shown to be a powerful tool for elucidating the growth mechanisms of carbon nanotubes. The growth picture is however not entirely clear yet due to the gap between current simulations and real experiments. We here simulate for the first time the nucleation and subsequent growth of single-wall carbon nanotubes (SWNTs) from oxygen-containing hydrocarbon feedstocks using the hybrid Molecular Dynamics/Monte Carlo technique. The underlying nucleation mechanisms of Ni-catalysed SWNT growth are discussed in detail. Specifically, we find that as a function of the feedstock, different carbon fractions may emerge as the main growth species, due to a competition between the feedstock decomposition, its rehydroxylation and its contribution to etching of the growing SWNT. This study provides a further understanding of the feedstock effects in SWNT growth in comparison with available experimental evidence as well as with<italic>ab initio</italic>and other simulation data, thereby reducing the simulation–experiment gap.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000471816500011	Publication Date	2019-01-02
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	2055-6756	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor		Times cited	1	Open Access	Not_Open_Access: Available from 03.01.2020
Notes	Fonds Wetenschappelijk Onderzoek, 12M1318N 1S22516N ; The authors gratefully acknowledge financial support from the Research Foundation Flanders (FWO), Belgium (Grant numbers 12M1318N and 1S22516N). The work was carried out in part using the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Centre VSC, funded by FWO and the Flemish Government (Department EWI). We thank Prof. A. C. T. van Duin for sharing the reax-code and forcefield parameters.			Approved	Most recent IF: NA
Call Number	PLASMANT @ plasmant @UA @ admin @ c:irua:159658			Serial	5169
Permanent link to this record



Author	Bal, K.M.; Neyts, E.C.
Title	Quantifying the impact of vibrational nonequilibrium in plasma catalysis: insights from a molecular dynamics model of dissociative chemisorption			Type	A1 Journal Article;plasma catalysis
Year	2021	Publication	Journal Of Physics D-Applied Physics	Abbreviated Journal	J Phys D Appl Phys
Volume	54	Issue	39	Pages	394004
Keywords	A1 Journal Article;plasma catalysis; vibrational nonequilibrium; dissociative chemisorption; free energy barriers; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract	The rate, selectivity and efficiency of plasma-based conversion processes is strongly affected by nonequilibrium phenomena. High concentrations of vibrationally excited molecules are such a plasma-induced effect. It is frequently assumed that vibrationally excited molecules are important in plasma catalysis because their presence lowers the apparent activation energy of dissociative chemisorption reactions and thus increases the conversion rate. A detailed atomic-level understanding of vibrationally stimulated catalytic reactions in the context of plasma catalysis is however lacking. Here, we couple a recently developed statistical model of a plasma-induced vibrational nonequilibrium to molecular dynamics simulations, enhanced sampling methods, and machine learning techniques. We quantify the impact of a vibrational nonequilibrium on the dissociative chemisorption barrier of H2 and CH4 on nickel catalysts over a wide range of vibrational temperatures. We investigate the effect of surface structure and compare the role of different vibrational modes of methane in the dissociation process. For low vibrational temperatures, very high vibrational efficacies are found, and energy in bend vibrations appears to dominate the dissociation of methane. The relative impact of vibrational nonequilibrium is much higher on terrace sites than on surface steps. We then show how our simulations can help to interpret recent experimental results, and suggest new paths to a better understanding of plasma catalysis.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000674464100001	Publication Date	2021-09-30
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0022-3727	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	2.588	Times cited		Open Access	OpenAccess
Notes	Fonds Wetenschappelijk Onderzoek, 12ZI420N ; K M B was funded as a junior postdoctoral fellow of the FWO (Research Foundation—Flanders), Grant 12ZI420N. The computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Government. HLDA calculations were performed with a script provided by G Piccini.			Approved	Most recent IF: 2.588
Call Number	PLASMANT @ plasmant @c:irua:179830			Serial	6808
Permanent link to this record



Author	Izadi, M.E.; Bal, K.M.; Maghari, A.; Neyts, E.C.
Title	Reaction mechanisms of C(³P_J) and C⁺(²P_J) with benzene in the interstellar medium from quantum mechanical molecular dynamics simulations			Type	A1 Journal article
Year	2021	Publication	Physical Chemistry Chemical Physics	Abbreviated Journal	Phys Chem Chem Phys
Volume	23	Issue	7	Pages	4205-4216
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	While spectroscopic data on small hydrocarbons in interstellar media in combination with crossed molecular beam (CMB) experiments have provided a wealth of information on astrochemically relevant species, much of the underlying mechanistic pathways of their formation remain elusive. Therefore, in this work, the chemical reaction mechanisms of C(<sup>3</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>and C<sup>+</sup>(<sup>2</sup>P) + C<sub>6</sub>H<sub>6</sub>systems using the quantum mechanical molecular dynamics (QMMD) technique at the PBE0-D3(BJ) level of theory is investigated, mimicking a CMB experiment. Both the dynamics of the reactions as well as the electronic structure for the purpose of the reaction network are evaluated. The method is validated for the first reaction by comparison to the available experimental data. The reaction scheme for the C(<sup>3</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>system covers the literature data,<italic>e.g.</italic>the major products are the 1,2-didehydrocycloheptatrienyl radical (C<sub>7</sub>H<sub>5</sub>) and benzocyclopropenyl radical (C<sub>6</sub>H<sub>5</sub>–CH), and it reveals the existence of less common pathways for the first time. The chemistry of the C<sup>+</sup>(<sup>2</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>system is found to be much richer, and we have found that this is because of more exothermic reactions in this system in comparison to those in the C(<sup>3</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>system. Moreover, using the QMMD simulation, a number of reaction paths have been revealed that produce three distinct classes of reaction products with different ring sizes. All in all, at all the collision energies and orientations, the major product is the heptagon molecular ion for the ionic system. It is also revealed that the collision orientation has a dominant effect on the reaction products in both systems, while the collision energy mostly affects the charged system. These simulations both prove the applicability of this approach to simulate crossed molecular beams, and provide fundamental information on reactions relevant for the interstellar medium.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000621595300016	Publication Date	2021-01-18
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1463-9076	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.123	Times cited		Open Access	OpenAccess
Notes	Fonds Wetenschappelijk Onderzoek, 12ZI420N ; Ministry of Science Research and Technology; Universiteit Antwerpen; The financial support from the Iran Ministry of Science, Research and Technology and PLASMANT Research Group University of Antwerp is highly acknowledged by the authors. K.M.B. was funded as a junior postdoctoral fellow of the FWO (Research Foundation – Flanders), Grant 12ZI420N. The computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Government.			Approved	Most recent IF: 4.123
Call Number	PLASMANT @ plasmant @c:irua:176672			Serial	6742
Permanent link to this record



Author	Verlackt, C.C.W.; Van Boxem, W.; Dewaele, D.; Lemière, F.; Sobott, F.; Benedikt, J.; Neyts, E.C.; Bogaerts, A.
Title	Mechanisms of Peptide Oxidation by Hydroxyl Radicals: Insight at the Molecular Scale			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	121	Pages	5787-5799
Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Molecular dynamics (MD) simulations were performed to provide atomic scale insight in the initial interaction between hydroxyl radicals (OH) and peptide systems in solution. These OH radicals are representative reactive oxygen species produced by cold atmospheric plasmas. The use of plasma for biomedical applications is gaining increasing interest, but the fundamental mechanisms behind the plasma modifications still remain largely elusive. This study helps to gain more insight in the underlying mechanisms of plasma medicine but is also more generally applicable to peptide oxidation, of interest for other applications. Combining both reactive and nonreactive MD simulations, we are able to elucidate the reactivity of the amino acids inside the peptide systems and their effect on their structure up to 1 μs. Additionally, experiments were performed, treating the simulated peptides with a plasma jet. The computational results presented here correlate well with the obtained experimental data and highlight the importance of the chemical environment for the reactivity of the individual amino acids, so that specific amino acids are attacked in higher numbers than expected. Furthermore, the long time scale simulations suggest that a single oxidation has an effect on the 3D conformation due to an increase in hydrophilicity and intra- and intermolecular interactions.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000396969900037	Publication Date	2017-03-16
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	1932-7447	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	4.536	Times cited	5	Open Access	OpenAccess
Notes	Fonds Wetenschappelijk Onderzoek, G012413N ;			Approved	Most recent IF: 4.536
Call Number	PLASMANT @ plasmant @ c:irua:142202			Serial	4537
Permanent link to this record



Author	Khalilov, U.; Vets, C.; Neyts, E.C.
Title	Catalyzed growth of encapsulated carbyne			Type	A1 Journal article
Year	2019	Publication	Carbon	Abbreviated Journal	Carbon
Volume	153	Issue		Pages	1-5
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Carbyne is a novel material of current interest in nanotechnology. As is typically the case for nanomaterials, the growth process determines the resulting properties. While endohedral carbyne has been successfully synthesized, its catalyst and feedstock-dependent growth mechanism is still elusive. We here study the nucleation and growth mechanism of different carbon chains in a Ni-containing double walled carbon nanotube using classical molecular dynamics simulations and ﬁrst-principles calculations. We ﬁnd that the understanding the competitive role of the metal catalyst and the hydrocarbon is important to control the growth of 1-dimensional carbon chains, including Ni or H-terminated carbyne. Also, we ﬁnd that the electronic property of the Ni-terminated carbyne can be tuned by steering the H concentration along the chain. These results suggest catalyst-containing carbon nanotubes as a possible synthesis route for carbyne formation.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000485054200001	Publication Date	2019-07-01
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0008-6223	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	6.337	Times cited		Open Access	Not_Open_Access
Notes	Fund of Scientific Research Flanders (FWO), Belgium, 12M1318N 1S22516N ; Flemish Supercomputer Centre VSC; Hercules Foundation; Flemish Government; University of Antwerp; The authors gratefully acknowledge the ﬁnancial support from the Fund of Scientiﬁc Research Flanders (FWO), Belgium, Grant numbers 12M1318N and 1S22516N. The work was carried out in part using the Turing HPC infrastructure of the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Centre VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the University of Antwerp.			Approved	Most recent IF: 6.337
Call Number	PLASMANT @ plasmant @c:irua:160695			Serial	5187
Permanent link to this record



Author	Khalilov, U.; Neyts, E.C.
Title	Mechanisms of selective nanocarbon synthesis inside carbon nanotubes			Type	A1 Journal article
Year	2021	Publication	Carbon	Abbreviated Journal	Carbon
Volume	171	Issue		Pages	72-78
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	The possibility of conﬁnement effects inside a carbon nanotube provides new application opportunities, e.g., growth of novel carbon nanostructures. However, the understanding the precise role of catalystfeedstock in the nanostructure synthesis is still elusive. In our simulation-based study, we investigate the Ni-catalyzed growth mechanism of encapsulated carbon nanostructures, viz. double-wall carbon nanotube and graphene nanoribbon, from carbon and hydrocarbon growth precursors, respectively. Speciﬁcally, we ﬁnd that the tube and ribbon growth is determined by a catalyst-vs-feedstock competition effect. We compare our results, i.e., growth mechanism and structure morphology with all available theoretical and experimental data. Our calculations show that all encapsulated nanostructures contain metal (catalyst) atoms and such structures are less stable than their pure counterparts. Therefore, we study the puriﬁcation mechanism of these structures. In general, this study opens a possible route to the controllable synthesis of tubular and planar carbon nanostructures for today’s nanotechnology.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000598371500009	Publication Date	2020-09-02
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0008-6223	ISBN		Additional Links	UA library record; WoS full record
Impact Factor	6.337	Times cited		Open Access	OpenAccess
Notes	Fund of Scientific Research Flanders, 12M1318N ; Universiteit Antwerpen; Flemish Supercomputer Centre; Hercules Foundation; Flemish Government; The authors gratefully acknowledge the ﬁnancial support from the Fund of Scientiﬁc Research Flanders (FWO), Belgium, Grant number 12M1318N. The work was carried out in part using the Turing HPC infrastructure of the CalcUA core facility of the Universiteit Antwerpen (UA), a division of the Flemish Supercomputer Centre (VSC), funded by the Hercules Foundation, the Flemish Government (department EWI) and the UA, Belgium.			Approved	Most recent IF: 6.337
Call Number	PLASMANT @ plasmant @c:irua:172459			Serial	6414
Permanent link to this record



Author	Bogaerts, A.; Neyts, E.C.; Guaitella, O.; Murphy, A.B.
Title	Foundations of plasma catalysis for environmental applications			Type	A1 Journal article
Year	2022	Publication	Plasma Sources Science & Technology	Abbreviated Journal	Plasma Sources Sci T
Volume		Issue		Pages
Keywords	A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract	Plasma catalysis is gaining increasing interest for various applications, but the underlying mechanisms are still far from understood. Hence, more fundamental research is needed to understand these mechanisms. This can be obtained by both modelling and experiments. This foundations paper describes the fundamental insights in plasma catalysis, as well as efforts to gain more insights by modelling and experiments. Furthermore, it discusses the state-of-the-art of the major plasma catalysis applications, as well as successes and challenges of technology transfer of these applications.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000804396200001	Publication Date	2022-03-21
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	0963-0252	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	3.8	Times cited		Open Access	OpenAccess
Notes	H2020 Marie Skłodowska-Curie Actions, 823745 ; H2020 European Research Council, 810182 ; We acknowldege financial support 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) and the European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie Grant Agreement No. 813393 (PIONEER).			Approved	Most recent IF: 3.8
Call Number	PLASMANT @ plasmant @c:irua:188539			Serial	7070
Permanent link to this record



Author	Engelmann, Y.; Mehta, P.; Neyts, E.C.; Schneider, W.F.; Bogaerts, A.
Title	Predicted Influence of Plasma Activation on Nonoxidative Coupling of Methane on Transition Metal Catalysts			Type	A1 Journal article
Year	2020	Publication	Acs Sustainable Chemistry & Engineering	Abbreviated Journal	Acs Sustain Chem Eng
Volume	8	Issue	15	Pages	6043-6054
Keywords	A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
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.
Address
Corporate Author				Thesis
Publisher		Place of Publication		Editor
Language		Wos	000526884000025	Publication Date	2020-04-20
Series Editor		Series Title		Abbreviated Series Title
Series Volume		Series Issue		Edition
ISSN	2168-0485	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
Impact Factor	8.4	Times cited		Open Access
Notes	Herculesstichting; University of Notre Dame; Universiteit Antwerpen; Division of Engineering Education and Centers, EEC-1647722 ; We would like to thank Tom Butterworth for his work on methane vibrational distribution functions (VDF) and for sharing his thoughts and experiences on this matter, specifically regarding the VDF of the degenerate modes of methane. We ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Research Article https://dx.doi.org/10.1021/acssuschemeng.0c00906 ACS Sustainable Chem. Eng. 2020, 8, 6043−6054 6052 also acknowledge financial support from the DOC-PRO3 and the TOP-BOF projects of the University of Antwerp. This work was carried out in part 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. Support for W.F.S. was provided by the National Science Foundation under cooperative agreement no. EEC-1647722, an Engineering Research Center for the Innovative and Strategic Transformation of Alkane Resources (CISTAR). P.M. acknowledges support through the Eilers Graduate Fellowship of the University of Notre Dame.			Approved	Most recent IF: 8.4; 2020 IF: 5.951
Call Number	PLASMANT @ plasmant @c:irua:169228			Serial	6366
Permanent link to this record