|
Records |
Links |
|
Author |
Neyts, E.C.; Bogaerts, A. |
|
|
Title |
Understanding plasma catalysis through modelling and simulation : a review |
Type |
A1 Journal article |
|
Year |
2014 |
Publication |
Journal of physics: D: applied physics |
Abbreviated Journal |
J Phys D Appl Phys |
|
|
Volume |
47 |
Issue |
22 |
Pages |
224010 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
Plasma catalysis holds great promise for environmental applications, provided that the process viability can be maximized in terms of energy efficiency and product selectivity. This requires a fundamental understanding of the various processes taking place and especially the mutual interactions between plasma and catalyst. In this review, we therefore first examine the various effects of the plasma on the catalyst and of the catalyst on the plasma that have been described in the literature. Most of these studies are purely experimental. The urgently needed fundamental understanding of the mechanisms underpinning plasma catalysis, however, may also be obtained through modelling and simulation. Therefore, we also provide here an overview of the modelling efforts that have been developed already, on both the atomistic and the macroscale, and we identify the data that can be obtained with these models to illustrate how modelling and simulation may contribute to this field. Last but not least, we also identify future modelling opportunities to obtain a more complete understanding of the various underlying plasma catalytic effects, which is needed to provide a comprehensive picture of plasma catalysis. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
Iop publishing ltd |
Place of Publication |
Bristol |
Editor |
|
|
|
Language |
|
Wos |
000336207900011 |
Publication Date |
2014-05-14 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0022-3727;1361-6463; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
2.588 |
Times cited |
130 |
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 2.588; 2014 IF: 2.721 |
|
|
Call Number |
UA @ lucian @ c:irua:116920 |
Serial |
3803 |
|
Permanent link to this record |
|
|
|
|
Author |
Dufour, T.; Minnebo, J.; Abou Rich, S.; Neyts, E.C.; Bogaerts, A.; Reniers, F. |
|
|
Title |
Understanding polyethylene surface functionalization by an atmospheric He/O2 plasma through combined experiments and simulations |
Type |
A1 Journal article |
|
Year |
2014 |
Publication |
Journal of physics: D: applied physics |
Abbreviated Journal |
J Phys D Appl Phys |
|
|
Volume |
47 |
Issue |
22 |
Pages |
224007 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
High density polyethylene surfaces were exposed to the atmospheric post-discharge of a radiofrequency plasma torch supplied in helium and oxygen. Dynamic water contact angle measurements were performed to evaluate changes in surface hydrophilicity and angle resolved x-ray photoelectron spectroscopy was carried out to identify the functional groups responsible for wettability changes and to study their subsurface depth profiles, up to 9 nm in depth. The reactions leading to the formation of CO, C = O and OC = O groups were simulated by molecular dynamics. These simulations demonstrate that impinging oxygen atoms do not react immediately upon impact but rather remain at or close to the surface before eventually reacting. The simulations also explain the release of gaseous species in the ambient environment as well as the ejection of low molecular weight oxidized materials from the surface. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
London |
Editor |
|
|
|
Language |
|
Wos |
000336207900008 |
Publication Date |
2014-05-14 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0022-3727;1361-6463; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
2.588 |
Times cited |
13 |
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 2.588; 2014 IF: 2.721 |
|
|
Call Number |
UA @ lucian @ c:irua:116919 |
Serial |
3804 |
|
Permanent link to this record |
|
|
|
|
Author |
Mees, M.J.; Pourtois, G.; Neyts, E.C.; Thijsse, B.J.; Stesmans, A. |
|
|
Title |
Uniform-acceptance force-bias Monte Carlo method with time scale to study solid-state diffusion |
Type |
A1 Journal article |
|
Year |
2012 |
Publication |
Physical review : B : condensed matter and materials physics |
Abbreviated Journal |
Phys Rev B |
|
|
Volume |
85 |
Issue |
13 |
Pages |
134301-134301,9 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
Monte Carlo (MC) methods have a long-standing history as partners of molecular dynamics (MD) to simulate the evolution of materials at the atomic scale. Among these techniques, the uniform-acceptance force-bias Monte Carlo (UFMC) method [ G. Dereli Mol. Simul. 8 351 (1992)] has recently attracted attention [ M. Timonova et al. Phys. Rev. B 81 144107 (2010)] thanks to its apparent capacity of being able to simulate physical processes in a reduced number of iterations compared to classical MD methods. The origin of this efficiency remains, however, unclear. In this work we derive a UFMC method starting from basic thermodynamic principles, which leads to an intuitive and unambiguous formalism. The approach includes a statistically relevant time step per Monte Carlo iteration, showing a significant speed-up compared to MD simulations. This time-stamped force-bias Monte Carlo (tfMC) formalism is tested on both simple one-dimensional and three-dimensional systems. Both test-cases give excellent results in agreement with analytical solutions and literature reports. The inclusion of a time scale, the simplicity of the method, and the enhancement of the time step compared to classical MD methods make this method very appealing for studying the dynamics of many-particle systems. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000302290500001 |
Publication Date |
2012-04-03 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
1098-0121;1550-235X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
3.836 |
Times cited |
31 |
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 3.836; 2012 IF: 3.767 |
|
|
Call Number |
UA @ lucian @ c:irua:97160 |
Serial |
3809 |
|
Permanent link to this record |
|
|
|
|
Author |
Neyts, E.; Bogaerts, A.; van de Sanden, M.C.M. |
|
|
Title |
Unraveling the deposition mechanism in a-C:H thin-film growth: a molecular-dynamics study for the reaction behavior of C3 and C3H radicals with a-C:H surfaces |
Type |
A1 Journal article |
|
Year |
2006 |
Publication |
Journal of applied physics |
Abbreviated Journal |
J Appl Phys |
|
|
Volume |
99 |
Issue |
1 |
Pages |
014902,1-8 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
|
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
American Institute of Physics |
Place of Publication |
New York, N.Y. |
Editor |
|
|
|
Language |
|
Wos |
000234607200071 |
Publication Date |
2006-01-23 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0021-8979; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
2.068 |
Times cited |
25 |
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 2.068; 2006 IF: 2.316 |
|
|
Call Number |
UA @ lucian @ c:irua:55831 |
Serial |
3815 |
|
Permanent link to this record |
|
|
|
|
Author |
Heyne, M.H.; Chiappe, D.; Meersschaut, J.; Nuytten, T.; Conard, T.; Bender, H.; Huyghebaert, C.; Radu, I.P.; Caymax, M.; de Marneffe, J.F.; Neyts, E.C.; De Gendt, S.; |
|
|
Title |
Multilayer MoS2 growth by metal and metal oxide sulfurization |
Type |
A1 Journal article |
|
Year |
2016 |
Publication |
Journal of materials chemistry C : materials for optical and electronic devices |
Abbreviated Journal |
J Mater Chem C |
|
|
Volume |
4 |
Issue |
4 |
Pages |
1295-1304 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
We investigated the deposition of MoS2 multilayers on large area substrates. The pre-deposition of metal or metal oxide with subsequent sulfurization is a promising technique to achieve layered films. We distinguish a different reaction behavior in metal oxide and metallic films and investigate the effect of the temperature, the H2S/H-2 gas mixture composition, and the role of the underlying substrate on the material quality. The results of the experiments suggest a MoS2 growth mechanism consisting of two subsequent process steps. At first, the reaction of the sulfur precursor with the metal or metal oxide occurs, requiring higher temperatures in the case of metallic film compared to metal oxide. At this stage, the basal planes assemble towards the diffusion direction of the reaction educts and products. After the sulfurization reaction, the material recrystallizes and the basal planes rearrange parallel to the substrate to minimize the surface energy. Therefore, substrates with low roughness show basal plane assembly parallel to the substrate. These results indicate that the substrate character has a significant impact on the assembly of low dimensional MoS2 films. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000370723300020 |
Publication Date |
2016-01-05 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2050-7526; 2050-7534 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
5.256 |
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 5.256 |
|
|
Call Number |
UA @ lucian @ c:irua:132327 |
Serial |
4211 |
|
Permanent link to this record |
|
|
|
|
Author |
Neyts, E.C. |
|
|
Title |
The role of ions in plasma catalytic carbon nanotube growth : a review |
Type |
A1 Journal article |
|
Year |
2015 |
Publication |
Frontiers of Chemical Science and Engineering |
Abbreviated Journal |
Front Chem Sci Eng |
|
|
Volume |
9 |
Issue |
9 |
Pages |
154-162 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
While it is well-known that the plasma-enhanced catalytic chemical vapor deposition (PECVD) of carbon nanotubes (CNTs) offers a number of advantages over thermal CVD, the influence of the various individual contributing factors is not well understood. Especially the role of ions is unclear, since ions in plasmas are generally associated with sputtering rather than with growing a material. Even so, various studies have demonstrated the beneficial effects of ion bombardment during the growth of CNTs. This review looks at the role of the ions in plasma-enhanced CNT growth as deduced from both experimental and simulation studies. Specific attention is paid to the beneficial effects of ion bombardment. Based on the available literature, it can be concluded that ions can be either beneficial or detrimental for carbon nanotube growth, depending on the exact conditions and the control over the growth process. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000360319600003 |
Publication Date |
2015-06-11 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2095-0179 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
1.712 |
Times cited |
8 |
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 1.712; 2015 IF: NA |
|
|
Call Number |
UA @ lucian @ c:irua:127815 |
Serial |
4239 |
|
Permanent link to this record |
|
|
|
|
Author |
Ali, S.; Myasnichenko, V.S.; Neyts, E.C. |
|
|
Title |
Size-dependent strain and surface energies of gold nanoclusters |
Type |
A1 Journal article |
|
Year |
2016 |
Publication |
Physical chemistry, chemical physics |
Abbreviated Journal |
Phys Chem Chem Phys |
|
|
Volume |
18 |
Issue |
18 |
Pages |
792-800 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
Gold nanocluster properties exhibit unique size-dependence. In this contribution, we employ reactive molecular dynamics simulations to calculate the size- and temperature-dependent surface energies, strain energies and atomic displacements for icosahedral, cuboctahedral, truncated octahedral and decahedral Au-nanoclusters. The calculations demonstrate that the surface energy decreases with increasing cluster size at 0 K but increases with size at higher temperatures. The calculated melting curves as a function of cluster size demonstrate the Gibbs-Thomson effect. Atomic displacements and strain are found to strongly depend on the cluster size and both are found to increase with increasing cluster size. These results are of importance for understanding the size-and temperature-dependent surface processes on gold nanoclusters. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
Cambridge |
Editor |
|
|
|
Language |
|
Wos |
000369480600017 |
Publication Date |
2015-11-18 |
|
|
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 |
37 |
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 4.123 |
|
|
Call Number |
UA @ lucian @ c:irua:131626 |
Serial |
4243 |
|
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 |
Neyts, E. |
|
|
Title |
Algemene chemie : van atomen tot thermodynamica |
Type |
MA2 Book as author |
|
Year |
2014 |
Publication |
|
Abbreviated Journal |
|
|
|
Volume |
|
Issue |
|
Pages |
317 p. |
|
|
Keywords |
MA2 Book as author; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
|
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
Acco |
Place of Publication |
Leuven |
Editor |
|
|
|
Language |
|
Wos |
|
Publication Date |
|
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
|
ISBN |
978-90-334-9628-8 |
Additional Links |
UA library record |
|
|
Impact Factor |
|
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: NA |
|
|
Call Number |
UA @ lucian @ c:irua:128094 |
Serial |
4514 |
|
Permanent link to this record |
|
|
|
|
Author |
Nematollahi, P.; Neyts, E.C. |
|
|
Title |
Direct methane conversion to methanol on M and MN4 embedded graphene (M = Ni and Si): a comparative DFT study |
Type |
A1 Journal article |
|
Year |
2019 |
Publication |
Applied surface science |
Abbreviated Journal |
Appl Surf Sci |
|
|
Volume |
496 |
Issue |
496 |
Pages |
143618 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
The ever increasing global production and dispersion of methane requires novel chemistry to transform it into easily condensable energy carriers that can be integrated into the chemical infrastructure. In this context, single atom catalysts have attracted considerable interest due to their outstanding catalytic activity. We here use density functional theory (DFT) computations to compare the reaction and activation energies of M and MN4 embedded graphene (M = Ni and Si) on the methane-to-methanol conversion near room temperature. Thermodynamically, conversion of methane to methanol is energetically favorable at ambient conditions. Both singlet and triplet spin state of the studied systems are considered in all of the calculations. The DFT results show that the barriers are significantly lower when the complexes are in the triplet state than in the singlet state. In particular, Si-G with the preferred spin multiplicity of triplet seems to be viable catalysts for methane oxidation thanks to the corresponding lower energy barriers and higher stability of the obtained configurations. Our results provide insights into the nature of methane conversion and may serve as guidance for fabricating cost-effective graphene-based single atom catalysts. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000488957400004 |
Publication Date |
2019-08-12 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0169-4332 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
3.387 |
Times cited |
2 |
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 3.387 |
|
|
Call Number |
UA @ admin @ c:irua:163695 |
Serial |
6294 |
|
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 |
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 |
Kovács, A.; Billen, P.; Cornet, I.; Wijnants, M.; Neyts, E.C. |
|
|
Title |
Modeling the physicochemical properties of natural deep eutectic solvents : a review |
Type |
A1 Journal article |
|
Year |
2020 |
Publication |
Chemsuschem |
Abbreviated Journal |
Chemsuschem |
|
|
Volume |
13 |
Issue |
15 |
Pages |
3789-3804 |
|
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Biochemical Wastewater Valorization & Engineering (BioWaVE) |
|
|
Abstract |
Natural deep eutectic solvents (NADES) are mixtures of naturally derived compounds with a significantly decreased melting point due to the specific interactions among the constituents. NADES have benign properties (low volatility, flammability, toxicity, cost) and tailorable physicochemical properties (by altering the type and molar ratio of constituents), hence they are often considered as a green alternative to common organic solvents. Modeling the relation between their composition and properties is crucial though, both for understanding and predicting their behavior. Several efforts were done to this end, yet this review aims at structuring the present knowledge as an outline for future research. First, we reviewed the key properties of NADES and relate them to their structure based on the available experimental data. Second, we reviewed available modeling methods applicable to NADES. At the molecular level, density functional theory and molecular dynamics allow interpreting density differences and vibrational spectra, and computation of interaction energies. Additionally, properties at the level of the bulk media can be explained and predicted by semi-empirical methods based on ab initio methods (COSMO-RS) and equation of state models (PC-SAFT). Finally, methods based on large datasets are discussed; models based on group contribution methods and machine learning. A combination of bulk media and dataset modeling allows qualitative prediction and interpretation of phase equilibria properties on the one hand, and quantitative prediction of melting point, density, viscosity, surface tension and refractive indices on the other hand. In our view, multiscale modeling, combining the molecular and macroscale methods, will strongly enhance the predictability of NADES properties and their interaction with solutes, yielding truly tailorable solvents to accommodate (bio)chemical reactions. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000541499100001 |
Publication Date |
2020-05-07 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
1864-5631 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
8.4 |
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 8.4; 2020 IF: 7.226 |
|
|
Call Number |
UA @ admin @ c:irua:168851 |
Serial |
6770 |
|
Permanent link to this record |
|
|
|
|
Author |
Surmenev, R.A.; Grubova, I.Y.; Neyts, E.; Teresov, A.D.; Koval, N.N.; Epple, M.; Tyurin, A.I.; Pichugin, V.F.; Chaikina, M.V.; Surmeneva, M.A. |
|
|
Title |
Ab initio calculations and a scratch test study of RF-magnetron sputter deposited hydroxyapatite and silicon-containing hydroxyapatite coatings |
Type |
A1 Journal article |
|
Year |
2020 |
Publication |
Surfaces and interfaces |
Abbreviated Journal |
|
|
|
Volume |
21 |
Issue |
|
Pages |
|
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
A crucial property for implants is their biocompatibility. To ensure biocompatibility, thin coatings of hydroxyapatite (HA) are deposited on the actual implant. In this study, we investigate the effects of the addition of silicate anions to the structure of hydroxyapatite coatings on their adhesion strength via a scratch test and ab initio calculations. We find that both the grain size and adhesion strength decrease with the increase in the silicon content in the HA coating (SiHA). The increase in the silicon content to 1.2 % in the HA coating leads to a decrease in the average crystallite size from 28 to 21 nm, and in the case of 4.6 %, it leads to the formation of an amorphous or nanocrystalline film. The decreases in the grain and crystallite sizes lead to peeling and destruction of the coating from the titanium substrate at lower loads. Further, our ab initio simulations demonstrate an increased number of molecular bonds at the amorphous SiHA-TiO2 interface. However, the experimental results revealed that the structure and grain size have more pronounced effects on the adhesion strength of the coatings. In conclusion, based on the results of the ab initio simulations and the experimental results, we suggest that the presence of Si in the form of silicate ions in the HA coating has a significant impact on the structure, grain size, and number of molecular bonds at the interface and on the adhesion strength of the SiHA coating to the titanium substrate. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
000697616300009 |
Publication Date |
2020-10-02 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2468-0230 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
6.2 |
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 6.2; 2020 IF: NA |
|
|
Call Number |
UA @ admin @ c:irua:181685 |
Serial |
7400 |
|
Permanent link to this record |
|
|
|
|
Author |
Kovács, A.; Janssens, N.; Mielants, M.; Cornet, I.; Neyts, E.C.; Billen, P. |
|
|
Title |
Biocatalyzed vinyl laurate transesterification in natural deep eutectic solvents |
Type |
A1 Journal article |
|
Year |
2023 |
Publication |
Waste and biomass valorization |
Abbreviated Journal |
|
|
|
Volume |
|
Issue |
|
Pages |
1-12 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Biochemical Wastewater Valorization & Engineering (BioWaVE); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) |
|
|
Abstract |
Purpose Natural deep eutectic solvents (NADES) represent a green alternative to conventional organic solvents as reaction medium, offering more benign properties. To efficiently design NADES for biocatalysis, a better understanding of their effect on these reactions is needed. We hypothesize that this effect can be described by separately considering (1) the solvent interactions with the substrates, (2) the solvent viscosities and (3) the enzyme stability in NADES. Methods We investigated the effect of substrate solvation and viscosity on the reaction rate; and the stability of the enzyme in NADES. To this end, we monitored the conversion over time of the transesterification of vinyl laurate with 1- butanol by the lipase enzyme Candida antarctica B in NADES of different compounds and molar ratios. Results The initial reaction rate is higher in most NADES ( varying between 1.14 and 15.07 mu mol min(-1) mg(-1)) than in the reference n-hexane (4.0 mu mol min(-1) mg(-1))), but no clear relationship between viscosity and initial reaction rate was found. The increased reaction rate is most likely related to the solvation of the substrate due to a change in the activation energy of the reaction or a change in the conformation of the substrate. The enzyme retained part of its activity after the first 2 h of reaction (on average 20 % of the substrate reacted in the 2-24 h period). Enzyme incubation in ethylene glycol-based NADES resulted in a reduced reaction rate ( 15.07 vs. 3.34 mu mol min(-1) mg(-1)), but this may also be due to slow dissolution of the substrate. Conclusions The effect of viscosity seems to be marginal next to the effect of solvation and possible enzyme-NADES interaction. The enzyme retains some of its activity during the 24-hour measurements, but the enzyme incubation experiments did not yield accurate, comparable values. [GRAPHICS] . |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
001117290800003 |
Publication Date |
2023-12-07 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
1877-2641; 1877-265x |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
3.2 |
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 3.2; 2023 IF: 1.337 |
|
|
Call Number |
UA @ admin @ c:irua:202709 |
Serial |
9005 |
|
Permanent link to this record |
|
|
|
|
Author |
Grubova, I.Y.; Surmenev, R.A.; Neyts, E.C.; Koptyug, A.V.; Volkova, A.P.; Surmeneva, M.A. |
|
|
Title |
Combined first-principles and experimental study on the microstructure and mechanical characteristics of the multicomponent additive-manufactured Ti-35Nb-7Zr-5Ta alloy |
Type |
A1 Journal article |
|
Year |
2023 |
Publication |
ACS Omega |
Abbreviated Journal |
|
|
|
Volume |
8 |
Issue |
30 |
Pages |
27519-27533 |
|
|
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
|
Abstract |
New & beta;-stabilizedTi-based alloys are highly promising forbone implants, thanks in part to their low elasticity. The natureof this elasticity, however, is as yet unknown. We here present combinedfirst-principles DFT calculations and experiments on the microstructure,structural stability, mechanical characteristics, and electronic structureto elucidate this origin. Our results suggest that the studied & beta;Ti-35Nb-7Zr-5Ta wt % (TNZT) alloy manufacturedby the electron-beam powder bed fusion (E-PBF) method has homogeneousmechanical properties (H = 2.01 & PLUSMN; 0.22 GPa and E = 69.48 & PLUSMN; 0.03 GPa) along the building direction,which is dictated by the crystallographic texture and microstructuremorphologies. The analysis of the structural and electronic properties,as the main factors dominating the chemical bonding mechanism, indicatesthat TNZT has a mixture of strong metallic and weak covalent bonding.Our calculations demonstrate that the softening in the Cauchy pressure(C & PRIME; = 98.00 GPa) and elastic constant C ̅ ( 44 ) = 23.84 GPa is the originof the low elasticity of TNZT. Moreover, the nature of this softeningphenomenon can be related to the weakness of the second and thirdneighbor bonds in comparison with the first neighbor bonds in theTNZT. Thus, the obtained results indicate that a carefully designedTNZT alloy can be an excellent candidate for the manufacturing oforthopedic internal fixation devices. In addition, the current findingscan be used as guidance not only for predicting the mechanical propertiesbut also the nature of elastic characteristics of the newly developedalloys with yet unknown properties. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
001031269000001 |
Publication Date |
2023-07-18 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2470-1343 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
4.1 |
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 4.1; 2023 IF: NA |
|
|
Call Number |
UA @ admin @ c:irua:198313 |
Serial |
9011 |
|
Permanent link to this record |
|
|
|
|
Author |
Cassimon, J.; Kovács, A.; Neyts, E.; Cornet, I.; Billen, P. |
|
|
Title |
Deacetylation of mannosylerythritol lipids in hydrophobic natural deep eutectic solvents |
Type |
A1 Journal article |
|
Year |
2023 |
Publication |
European journal of organic chemistry |
Abbreviated Journal |
|
|
|
Volume |
27 |
Issue |
5 |
Pages |
e202300934-10 |
|
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Biochemical Wastewater Valorization & Engineering (BioWaVE); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) |
|
|
Abstract |
Mannosylerythritol lipids (MELs) are a promising group of biosurfactants due to their high fermentation yield, selfassembly and biological activity. During fermentation by Pseudozyma aphidis, a mixture of MELs with different levels of acylation is formed, of which the fully deacetylated form is the most valuable. In order to reduce the environmental impact of deacetylation, an enzymatic process using natural deep eutectic solvents (NADES) has been developed. We tested the deacetylation of a purified MELs mixture with immobilized Candida antarctica lipase B enzyme and 2-ethylhexanol as co-substrate in 140 h reactions with different NADES. We identified hydrophobic NADES systems with similar yields and kinetics as in pure 2-ethylhexanol solvent. Our results indicate that deacetylation of MELs mixtures in NADES as a solvent is possible with yields comparable to pure co-substrate and that hydrophobic NADES without carboxylic acid compounds facilitate the reaction to the greatest extent. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
|
Publication Date |
2023-12-12 |
|
|
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
1434-193x; 1099-0690 |
ISBN |
|
Additional Links |
UA library record |
|
|
Impact Factor |
2.8 |
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 2.8; 2023 IF: 2.834 |
|
|
Call Number |
UA @ admin @ c:irua:201382 |
Serial |
9017 |
|
Permanent link to this record |
|
|
|
|
Author |
Gogoi, A.; Neyts, E.C.; Peeters, F.M. |
|
|
Title |
Reduction-enhanced water flux through layered graphene oxide (GO) membranes stabilized with H3O+ and OH- ions |
Type |
A1 Journal article |
|
Year |
2024 |
Publication |
Physical chemistry, chemical physics |
Abbreviated Journal |
|
|
|
Volume |
26 |
Issue |
13 |
Pages |
10265-10272 |
|
|
Keywords |
A1 Journal article; Condensed Matter Theory (CMT); Modelling and Simulation in Chemistry (MOSAIC) |
|
|
Abstract |
Graphene oxide (GO) is one of the most promising candidates for next generation of atomically thin membranes. Nevertheless, one of the major issues for real world application of GO membranes is their undesirable swelling in an aqueous environment. Recently, we demonstrated that generation of H3O+ and OH- ions (e.g., with an external electric field) in the interlayer gallery could impart aqueous stability to the layered GO membranes (A. Gogoi, ACS Appl. Mater. Interfaces, 2022, 14, 34946). This, however, compromises the water flux through the membrane. In this study, we report on reducing the GO nanosheets as a solution to this issue. With the reduction of the GO nanosheets, the water flux through the layered GO membrane initially increases and then decreases again beyond a certain degree of reduction. Here, two key factors are at play. Firstly, the instability of the H-bond network between water molecules and the GO nanosheets, which increases the water flux. Secondly, the pore size reduction in the interlayer gallery of the membranes, which decreases the water flux. We also observe a significant improvement in the salt rejection of the membranes, due to the dissociation of water molecules in the interlayer gallery. In particular, for the case of 10% water dissociation, the water flux through the membranes can be enhanced without altering its selectivity. This is an encouraging observation as it breaks the traditional tradeoff between water flux and salt rejection of a membrane. |
|
|
Address |
|
|
|
Corporate Author |
|
Thesis |
|
|
|
Publisher |
|
Place of Publication |
|
Editor |
|
|
|
Language |
|
Wos |
001186465400001 |
Publication Date |
2024-03-15 |
|
|
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 |
|
|
Impact Factor |
3.3 |
Times cited |
|
Open Access |
|
|
|
Notes |
|
Approved |
Most recent IF: 3.3; 2024 IF: 4.123 |
|
|
Call Number |
UA @ admin @ c:irua:204792 |
Serial |
9168 |
|
Permanent link to this record |