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“A first-principles study of the effects of atom impurities, defects, strain, electric field and layer thickness on the electronic and magnetic properties of the C2N nanosheet”. Bafekry A, Stampfl C, Ghergherehchi M, Shayesteh SF, Carbon 157, 371 (2020). http://doi.org/10.1016/J.CARBON.2019.10.038
Abstract: Using the first-principles calculations, we explore the structural and novel electronic/optical properties of the C2N nanosheet. To this goal, we systematically investigate the affect of layer thickness, electrical field and strain on the electronic properties of the C2N nanosheet. By increasing the thickness of C2N, we observed that the band gap decreases. Moreover, by applying an electrical field to bilayer C2N, the band gap decreases and a semiconductor-to-metal transition can occur. Our results also confirm that uniaxial and biaxial strain can effectively alter the band gap of C2N monolayer. Furthermore, we show that the electronic and magnetic properties of C2N can be modified by the adsorption and substitution of various atoms. Depending on the species of embedded atoms, they may induce semiconductor (O, C, Si and Be), metal (S, N, P, Na, K, Mg and Ca), dilute-magnetic semiconductor (H, F, B), or ferro-magnetic-metal (Cl, Li) character in C2N monolayer. It was also found that the inclusion of hydrogen or oxygen impurities and nitrogen vacancies, can induce magnetism in the C2N monolayer. These extensive calculations can be useful to guide future studies to modify the electronic/optical properties of two-dimensional materials. (C) 2019 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 10.9
Times cited: 49
DOI: 10.1016/J.CARBON.2019.10.038
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“Mechanisms of selective nanocarbon synthesis inside carbon nanotubes”. Khalilov U, Neyts EC, Carbon 171, 72 (2021). http://doi.org/10.1016/j.carbon.2020.08.060
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.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.337
DOI: 10.1016/j.carbon.2020.08.060
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“Entropic and enthalpic factors determining the thermodynamics and kinetics of carbon segregation from transition metal nanoparticles”. Fukuhara S, Bal KM, Neyts EC, Shibuta Y, Carbon 171, 806 (2021). http://doi.org/10.1016/j.carbon.2020.09.059
Abstract: The free energy surface (FES) for carbon segregation from nickel nanoparticles is obtained from advanced molecular dynamics simulations. A suitable reaction coordinate is developed that can distinguish dissolved carbon atoms from segregated dimers, chains and junctions on the nanoparticle surface. Because of the typically long segregation time scale (up to ms), metadynamics simulations along the developed reaction coordinate are used to construct FES over a wide range of temperatures and carbon concentrations. The FES revealed the relative stability of different stages in the segregation process, and free energy barriers and rates of the individual steps could then be calculated and decomposed into enthalpic and entropic contributions. As the carbon concentration in the nickel nanoparticle increases, segregated carbon becomes more stable in terms of both enthalpy and entropy. The activation free energy of the reaction also decreases with the increase of carbon concentration, which can be mainly attributed to entropic effects. These insights and the methodology developed to obtain them improve our understanding of carbon segregation process across materials science in general, and the nucleation and growth of carbon nanotube in particular.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.337
DOI: 10.1016/j.carbon.2020.09.059
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“Electro-optical properties of monolayer and bilayer boron-doped C₃N: Tunable electronic structure via strain engineering and electric field”. Bafekry A, Yagmurcukardes M, Shahrokhi M, Ghergherehchi M, Carbon 168, 220 (2020). http://doi.org/10.1016/J.CARBON.2020.06.082
Abstract: In this work, the structural, electronic and optical properties of monolayer and bilayer of boron doped C3N are investigated by means of density functional theory-based first-principles calculations. Our results show that with increasing the B dopant concentration from 3.1% to 12.5% in the hexagonal pattern, an indirect-to-direct band gap (0.8 eV) transition occurs. Furthermore, we study the effect of electric field and strain on the B doped C3N bilayer (B-C3N@2L). It is shown that by increasing E-field strength from 0.1 to 0.6V/angstrom, the band gap displays almost a linear decreasing trend, while for the > 0.6V/angstrom, we find dual narrow band gap with of 50 meV (in parallel E-field) and 0.4 eV (in antiparallel E-field). Our results reveal that in-plane and out-of-plane strains can modulate the band gap and band edge positions of the B-C3N@2L. Overall, we predict that B-C3N@2L is a new platform for the study of novel physical properties in layered two-dimensional materials (2DM) which may provide new opportunities to realize high-speed low-dissipation devices. (C) 2020 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 10.9
Times cited: 21
DOI: 10.1016/J.CARBON.2020.06.082
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“PAI-graphene : a new topological semimetallic two-dimensional carbon allotrope with highly tunable anisotropic Dirac cones”. Chen X, Bouhon A, Li L, Peeters FM, Sanyal B, Carbon 170, 477 (2020). http://doi.org/10.1016/J.CARBON.2020.08.012
Abstract: Using evolutionary algorithm for crystal structure prediction, we present a new stable two-dimensional (2D) carbon allotrope composed of polymerized as-indacenes (PAI) in a zigzag pattern, namely PAI-graphene whose energy is lower than most of the reported 2D allotropes of graphene. Crucially, the crystal structure realizes a nonsymmorphic layer group that enforces a nontrivial global topology of the band structure with two Dirac cones lying perfectly at the Fermi level. The absence of electron/hole pockets makes PAI-graphene a pristine crystalline topological semimetal having anisotropic Fermi velocities with a high value of 7.0 x 10(5) m/s. We show that while the semimetallic property of the allotrope is robust against the application of strain, the positions of the Dirac cone and the Fermi velocities can be modified significantly with strain. Moreover, by combining strain along both the x- and y-directions, two band inversions take place at G leading to the annihilation of the Dirac nodes demonstrating the possibility of strain-controlled conversion of a topological semimetal into a semiconductor. Finally we formulate the bulk-boundary correspondence of the topological nodal phase in the form of a generalized Zak-phase argument finding a perfect agreement with the topological edge states computed for different edge-terminations. (C) 2020 The Author(s). Published by Elsevier Ltd.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 10.9
Times cited: 43
DOI: 10.1016/J.CARBON.2020.08.012
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“Carbon single-electron point source controlled by Coulomb blockade”. Kleshch VI, Porshyn V, Orekhov AS, Orekhov AS, Lützenkirchen-Hecht D, Obraztsov AN, Carbon 171, 154 (2021). http://doi.org/10.1016/j.carbon.2020.09.008
Abstract: The Coulomb blockade effect is commonly used in solid state electronics for the control of electron flow
at the single-particle level. Potentially, it allows the creation of single-electron point sources demanded
for prospective electron microscopy instruments and other vacuum electronics devices. Here we realize
this potential via creation of a stable point electron source composed of a carbon nanowire electrically
coupled to a diamond nanotip by a tunnel junction. Using energy spectroscopy analysis, we characterize
the electrons liberated from the nanometer scale carbon heterostructures in time and energy domains.
Our experimental results demonstrate perfect agreement with theory prediction of Coulomb oscillations
of the Fermi level in the nanowire and allow to determine the mechanisms of their suppression.
Persistence of the oscillations at room temperature, high intensity field emission with currents up to
1 mA, and other characteristics of our emitters are very promising for practical realization of coherent
single-electron guns.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.337
DOI: 10.1016/j.carbon.2020.09.008
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“Tuning flexoelectricty and electronic properties of zig-zag graphene nanoribbons by functionalization”. Pandey T, Covaci L, Peeters FM, Carbon 171, 551 (2021). http://doi.org/10.1016/J.CARBON.2020.09.028
Abstract: The flexoelectric and electronic properties of zig-zag graphene nanoribbons are explored under mechanical bending using state of the art first principles calculations. A linear dependence of the bending induced out of plane polarization on the applied strain gradient is found. The inferior flexoelectric properties of graphene nanoribbons can be improved by more than two orders of magnitude by hydrogen and fluorine functionalization (CH and CF nanoribbons). A large out of plane flexoelectric effect is predicted for CF nanoribbons. The origin of this enhancement lies in the electro-negativity difference between carbon and fluorine atoms, which breaks the out of plane charge symmetry even for a small strain gradient. The flexoelectric effect can be further improved by co-functionalization with hydrogen and fluorine (CHF Janus-type nanoribbon), where a spontaneous out of plane dipole moment is formed even for flat nanoribbons. We also find that bending can control the charge localization of valence band maxima and therefore enables the tuning of the hole effective masses and band gaps. These results present an important advance towards the understanding of flexoelectric and electronic properties of hydrogen and fluorine functionalized graphene nanoribbons, which can have important implications for flexible electronic applications. (C) 2020 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Impact Factor: 6.337
Times cited: 15
DOI: 10.1016/J.CARBON.2020.09.028
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“3D arrangement of epitaxial graphene conformally grown on porousified crystalline SiC”. Veronesi S, Pfusterschmied G, Fabbri F, Leitgeb M, Arif O, Esteban DA, Bals S, Schmid U, Heun S, Carbon 189, 210 (2022). http://doi.org/10.1016/j.carbon.2021.12.042
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 10.9
Times cited: 3
DOI: 10.1016/j.carbon.2021.12.042
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“Tunable natural terahertz and mid-infrared hyperbolic plasmons in carbon phosphide”. Dehdast M, Valiollahi Z, Neek-Amal M, Van Duppen B, Peeters FM, Pourfath M, Carbon 178, 625 (2021). http://doi.org/10.1016/J.CARBON.2021.03.040
Abstract: Hyperbolic polaritons in ultra thin materials such as few layers of van derWaals heterostructures provide a unique control over light-matter interaction at the nanoscale and with various applications in flat optics. Natural hyperbolic surface plasmons have been observed on thin films of WTe2 in the light wavelength range of 16-23 mu m (similar or equal to 13-18 THz) [Nat. Commun. 11, 1158 (2020)]. Using time-dependent density functional theory, it is found that carbon doped monolayer phosphorene (beta-allotrope of carbon phosphide monolayer) exhibits natural hyperbolic plasmons at frequencies above similar or equal to 5 THz which is not observed in its parent materials, i.e. monolayer of black phosphorous and graphene. Furthermore, we found that by electrostatic doping the plasmonic frequency range can be extended to the mid-infrared. (C) 2021 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 6.337
Times cited: 11
DOI: 10.1016/J.CARBON.2021.03.040
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“A cyclic catalyst pretreatment in CO2 for high yield production of Carbon nanofibers with narrow diameter distribution”. Corthals S, van Noyen J, Liang D, Ke X, Van Tendeloo G, Jacobs P, Sels B, Catalysis letters 141, 1621 (2011). http://doi.org/10.1007/s10562-011-0690-3
Abstract: This paper presents a cyclic catalyst pretreatment process to improve the CNF yield with narrow size distribution by sequentially feeding the CVD reactor with CH4/CO2 mixtures (carbon deposition) and CO2 (carbon removal) prior to the actual growth process. A mechanism based on a break-up of large Ni particles tentatively explains the beneficial effect of the cyclic carbon deposition/removal CVD procedure.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.799
Times cited: 1
DOI: 10.1007/s10562-011-0690-3
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“One-pot synthesis of Pt catalysts based on layered double hydroxides: an application in propane dehydrogenation”. Filez M, Redekop EA, Poelman H, Galvita VV, Meledina M, Turner S, Van Tendeloo G, Detavernier C, Marin GB, Catalysis science &, technology 6, 1863 (2016). http://doi.org/10.1039/C5CY01274K
Abstract: Simple methods for producing noble metal catalysts with well-defined active sites and improved performance are highly desired in the chemical industry. However, the development of such methods still presents a formidable synthetic challenge. Here, we demonstrate a one-pot synthesis route for the controlled production of bimetallic Pt–In catalysts based on the single-step formation of Mg,Al,Pt,In-containing layered double hydroxides (LDHs). Besides their simple synthesis, these Pt–In catalysts exhibit superior propane dehydrogenation activity compared to their multi-step synthesized analogs. The presented material serves as a showcase for the one-pot synthesis of a broader class of LDH-derived mono- and multimetallic Pt catalysts. The compositional flexibility provided by LDH materials can pave the way towards highperforming Pt-based catalysts with tunable physicochemical properties.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.773
Times cited: 12
DOI: 10.1039/C5CY01274K
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“Towards biolubricant compatible vegetable oils by pore mouth hydrogenation with shape-selective Pt/ZSM-5 catalysts”. Van Aelst J, Philippaerts A, Bartholomeeusen E, Fayad E, Thibault-Starzyk F, Lu J, Schryvers D, Ooms R, Verboekend D, Jacobs P, Sels B, Catalysis science &, technology 6, 2820 (2016). http://doi.org/10.1039/C6CY00498A
Abstract: Pt/ZSM-5 catalysts with various crystal sizes were prepared via competitive ion-exchange, followed by a slow activation procedure. Even when using very large ZSM-5 crystals, highly dispersed Pt nano-clusters were contained within the zeolite crystal's voids, as ascertained by 2D pressure-jump IR spectroscopy of adsorbed CO and focussed ion-beam transmission electron microscopy. The shape-selective properties of the Pt/ZSM-5 catalysts were evaluated in the partial hydrogenation of soybean oil. Unique hydrogenation selectivities were observed, as the fatty acids located at the central position of the triacylglycerol (TAG) molecules were preferentially hydrogenated. The resulting oil has therefore high levels of intermediately melting TAGs, which are compatible with biolubricants due to their improved oxidative stability and still appropriate low-temperature fluidity. The TAG distribution in the partially hydrogenated soybean oil samples was independent from the zeolite crystal size, while the hydrogenation activity linearly increases with the crystal's external surface area. This trend was confirmed with a Pt loaded mesoporous ZSM-5 zeolite, obtained via a mild alkaline treatment. These observations imply and confirm a genuine pore mouth catalysis mechanism, in which only one fatty acid chain of the TAG is able to enter the micropores of ZSM-5, where the double bonds are hydrogenated by the crystal encapsulated Pt-clusters.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.773
Times cited: 5
DOI: 10.1039/C6CY00498A
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“Factors driving the activity of commercial titanium dioxide powders towards gas phase photocatalytic oxidation of acetaldehyde”. Verbruggen SW, Masschaele K, Moortgat E, Korany TE, Hauchecorne B, Martens JA, Lenaerts S, Catalysis science &, technology 2, 2311 (2012). http://doi.org/10.1039/C2CY20123B
Abstract: The photocatalytic activity of two commercial titanium dioxide powders (Cristal Global, Millennium PC500 and Evonik, P25) is compared towards acetaldehyde degradation in the gas phase. In contrast to the extensive literature available, we found a higher activity for the PC500 than for the P25 coating. Here, we present a comprehensive characterization of the bulk and surface properties of both powders. Our comparison shows that the material properties that dominate the overall photocatalytic activity in gas phase differ from those required for the photodegradation of water-borne pollutants.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 5.773
Times cited: 33
DOI: 10.1039/C2CY20123B
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“Observation of surface species in plasma-catalytic dry reforming of methane in a novel atmospheric pressure dielectric barrier discharge in situ IR cell”. Van Turnhout J, Aceto D, Travert A, Bazin P, Thibault-Starzyk F, Bogaerts A, Azzolina-Jury F, Catalysis Science &, Technology 12, 6676 (2022). http://doi.org/10.1039/D2CY00311B
Abstract: We developed a novel in situ (i.e. inside plasma and during operation) IR dielectric barrier discharge cell allowing investigation of plasma catalysis in transmission mode, atmospheric pressure, flow conditions (WHSV similar to 0-50 000 mL g(-1) h(-1)), at relevant discharge voltages (similar to 0-50 kV) and frequencies (similar to 0-5 kHz). We applied it to study the IR-active surface species formed on a SiO2 support and on a 3 wt% Ru/SiO2 catalyst, which can help to reveal the important surface reaction mechanisms during the plasma-catalytic dry reforming of methane (DRM). Moreover, we present a technique for the challenging task of estimating the temperature of a catalyst sample in a plasma-catalytic system in situ and during plasma operation. We found that during the reaction, water is immediately formed at the SiO2 surface, and physisorbed formic acid is formed with a delay. As Ru/SiO2 is subject to greater plasma-induced heating than SiO2 (with a surface temperature increase in the range of 70-120 degrees C, with peaks up to 150 degrees C), we observe lower amounts of physisorbed water on Ru/SiO2, and less physisorbed formic acid formation. Importantly, the formation of surface species on the catalyst sample in our plasma-catalytic setup, as well as the observed conversions and selectivities in plasma conditions, can not be explained by plasma-induced heating of the catalyst surface, but must be attributed to other plasma effects, such as the adsorption of plasma-generated radicals and molecules, or the occurrence of Eley-Rideal reactions.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 5
DOI: 10.1039/D2CY00311B
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“Catalytic and molecular separation properties of Zeogrids and Zeotiles”. Martens JA, Thybaut JW, Denayer JFM, Sree SP, Aerts A, Reyniers M-F, van Speybroeck V, Waroquier M, Buekenhoudt A, Vankelecom I, Buijs W, Persoons J, Baron GV, Bals S, Van Tendeloo G, Marin GB, Jacobs PA, Kirschhock CEA, Catalysis today 168, 17 (2011). http://doi.org/10.1016/j.cattod.2011.01.036
Abstract: Zeogrids and Zeotiles are hierarchical materials built from assembled MFI zeolite precursor units. Permanent secondary porosity in these materials is obtained through self assembly of nanoparticles encountered in MFI zeolite synthesis in the presence of supramolecular templates. Hereon, the aggregated species are termed nanoslabs. Zeogrids are layered materials with lateral spacings between nanoslabs creating galleries qualifying as supermicropores. Zeotiles present a diversity of tridimensional nanoslab assemblies with mesopores. Zeotile-1, -4 and -6 are hexagonal mesostructures. Zeotile-1 has triangular and hexagonal channels; Zeotile-4 has hexagonal channels interconnected via slits. Zeotile-2 has a cubic structure with gyroid type mesoporosity. The behavior of Zeogrids and Zeotiles in adsorption, membrane and chromatographic separation and catalysis has been characterized and compared with zeolites and mesoporous materials derived from unstructured silica sources. Shape selectivity was detected via adsorption of n- and iso-alkanes. The mesoporosity of Zeotiles can be exploited in chromatographic separation of biomolecules. Zeotiles present attractive separation properties relevant to CO2 sequestration. Because of its facile synthesis procedure without hydrothermal steps Zeogrid is convenient for membrane synthesis. The performance of Zeogrid membrane in gas separation, nanofiltration and pervaporation is reported. In the Beckmann rearrangement of cyclohexanone oxime Zeogrids and Zeotiles display a catalytic activity characteristic of silicalite-1 zeolites. Introduction of acidity and redox catalytic activity can be achieved via incorporation of Al and Ti atoms in the nanoslabs during synthesis. Zeogrids are active in hydrocracking, catalytic cracking, alkylation and epoxidation reactions. Zeogrids and Zeotiles often behave differently from ordered mesoporous materials as well as from zeolites and present a valuable extension of the family of hierarchical silicate based materials.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.636
Times cited: 13
DOI: 10.1016/j.cattod.2011.01.036
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“Molecular dynamics simulations of supported metal nanocatalyst formation by plasma sputtering”. Brault P, Neyts EC, Catalysis today 256, 3 (2015). http://doi.org/10.1016/j.cattod.2015.02.004
Abstract: Magnetron sputtering is a widely used physical vapor deposition technique for deposition and formation of nanocatalyst thin films and clusters. Nevertheless, so far only few studies investigated this formation process at the fundamental level. We here review atomic scale molecular dynamics simulations aimed at elucidating the nanocatalyst growth process through magnetron sputtering. We first introduce the basic magnetron sputtering background and machinery of molecular dynamics simulations, and then describe the studies conducted in this field so far. We also present a perspective view on how the field may be developed further.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.636
Times cited: 18
DOI: 10.1016/j.cattod.2015.02.004
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“Nanoscale thermodynamic aspects of plasma catalysis”. Neyts EC, Ostrikov K(K), Catalysis today 256, 23 (2015). http://doi.org/10.1016/j.cattod.2015.02.025
Abstract: Plasma catalysis continues to gain increasing scientific interest, both in established fields like toxic waste abatement and emerging fields like greenhouse gas conversion into value-added chemicals. Attention is typically focused on the obtained conversion process selectivity, rates and energy efficiency. Much less attention is usually paid to the underlying mechanistic aspects of the processes that occur. In this contribution, we critically examine a number of fundamentally important nanoscale thermodynamic aspects of plasma catalysis, which are very relevant to these processes but so far have been overlooked or insufficiently covered in the plasma catalysis literature.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.636
Times cited: 14
DOI: 10.1016/j.cattod.2015.02.025
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“Novel MoVSbOx-type catalysts for selective isobutane oxidation”. Paul JS, Groothaert MH, Kirschhock CEA, Lebedev OI, Jacobs PA, Maier WF, Catalysis today
T2 –, 7th European Workshop Meeting on Selective Oxidation, AUG 31-SEP 04, 2003, Innsbruck, AUSTRIA 91-2, 265 (2004). http://doi.org/10.1016/j.cattod.2004.03.041
Abstract: A new sol-gel synthesis procedure is proposed for the preparation of MoVSbOx catalysts for the selective oxidation of isobutane. Physico-chemical characterization of the materials calcined at 400 degreesC, showed essentially amorphous catalysts, with long-range order. Increase of calcination temperature, however, resulted in the formation of small crystalline regions, confirmed through TEM. EPR measurements on the calcined samples pointed to the presence of isolated and magnetically interacting V(IV) species. The reported catalysts proved to be much more selective for partial oxidation compared to a literature reference catalyst. Furthermore, it is shown that this versatile synthesis recipe forms an excellent start for high-throughput and combinatorial studies. (C) 2004 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.636
Times cited: 12
DOI: 10.1016/j.cattod.2004.03.041
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“Preparation of sulfonated ordered mesoporous carbon and its use for the esterification of fatty acids”. Peng L, Philippaerts A, Ke X, van Noyen J, de Cleppel F, Van Tendeloo G, Jacobs PA, Sels BF, Catalysis today 150, 140 (2010). http://doi.org/10.1016/j.cattod.2009.07.066
Abstract: Mesoporous carbon, which can be replicated from mesoporous silica and whose surface is hydrophobic, can be an ideal catalyst for the esterification of fatty acids. Here we report an easy and low cost way to prepare sulfonic acid group-functionalized mesoporous carbon. A sample of calcined mesoporous silica SBA-15 was added to an aqueous sucrose solution followed by drying and calcination at different temperatures. In contrast to existing procedures, the obtained hybrid Si/C material was then first sulfonated in H2SO4, before the final removal of the silica template in order to stabilize the porous structure towards the liquid phase sulfonation treatment. Thus the silicacarbon composites, instead of the mesoporous carbon, were successfully sulfonated to introduce SO3H groups, while keeping the ordered mesoporous structure intact. The influence of carbonization temperature was investigated, suggesting an optimum temperature of 873 K. The SO3H group-functionalized mesoporous carbon, denoted as CMK-3-873-SO3H, was characterized by means of XRD, N2 physisorption, SEM, FT-IR, elemental analysis and TEM. It followed that a uniform mesoporous carbon was obtained with an average pore size of 3.89 nm, a specific surface of 807 m2/g and a SO3H group loading of 0.39 meq/g of dry material. Compared with other solid acid catalysts, the resulting material shows enhanced activity in the acid-catalyzed esterification of oleic acid with methanol, and can be used repeatedly. The increased catalytic performance is attributed to the hydrophobic surface and larger pore size of the new catalyst. It can effectively accommodate long chain fatty acids and reject formed water, making the active sites easily accessible.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.636
Times cited: 132
DOI: 10.1016/j.cattod.2009.07.066
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“Temperature influence on the reactivity of plasma species on a nickel catalyst surface : an atomic scale study”. Somers W, Bogaerts A, van Duin ACT, Huygh S, Bal KM, Neyts EC, Catalysis today 211, 131 (2013). http://doi.org/10.1016/j.cattod.2013.02.010
Abstract: In recent years, the potential use of hydrogen as a clean energy source has gained considerable attention. Especially H2 formation by Ni-catalyzed reforming of methane at elevated temperatures is an attractive process. However, a more fundamental knowledge at the atomic level is needed for a full comprehension of the reactions at the catalyst surface. In this contribution, we therefore investigate the H2 formation after CHx impacts on a Ni(1 1 1) surface in the temperature range 4001600 K, by means of reactive molecular dynamics (MD) simulations using the ReaxFF potential. While some H2 formation is already observed at the lower temperatures, substantial H2 formation is only obtained at elevated temperatures of 1400 K and above. At 1600 K, the H2 molecules are even the most frequently formed species. In direct correlation with the increasing dehydrogenation at elevated temperatures, an increased surface-to-subsurface C-diffusivity is observed as well. This study highlights the major importance of the temperature on the H2 formation.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.636
Times cited: 27
DOI: 10.1016/j.cattod.2013.02.010
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“Burning questions of plasma catalysis: Answers by modeling”. Bogaerts A, Zhang Q-Z, Zhang Y-R, Van Laer K, Wang W, Catalysis today 337, 3 (2019). http://doi.org/10.1016/j.cattod.2019.04.077
Abstract: Plasma catalysis is promising for various environmental, energy and chemical synthesis applications, but the underlying mechanisms are far from understood. Modeling can help to obtain a better insight in these mechanisms. Some burning questions relate to the plasma behavior inside packed bed reactors and whether plasma can penetrate into catalyst pores. In this paper, we try to provide answers to these questions, by means of both fluid modeling and particle-in-cell/Monte Carlo collision simulations. We present a short overview of recent findings obtained in our group by means of modeling, i.e., the enhanced electric field near the contact points and the streamer propagation through the packing in packed bed reactors, as well as the plasma behavior in catalyst pores, to determine the minimum pore size in which plasma streamers can penetrate.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.636
Times cited: 7
DOI: 10.1016/j.cattod.2019.04.077
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“Improvement in the coating homogeneity in electrosynthesized Rh structured catalysts for the partial oxidation of methane”. Benito P, Monti M, de Nolf W, Nuyts G, Janssens K, et al, Catalysis today 246, 154 (2015). http://doi.org/10.1016/J.CATTOD.2014.10.003
Abstract: The precipitation of Rh/Mg/Al and Rh/Al hydroxides on the surface of FeCrAlloy foams by a base electrogeneration method was investigated to improve the properties of the deposited film (homogeneity and composition) and therefore the performances of the structured catalysts, obtained by calcination, in the Catalytic Partial Oxidation of CH4 to syngas. The work focussed on decreasing current gradients within open-cell foam cylinders by increasing the number of electrical contacts from 1 to 3 points to promote a more homogeneous precipitation of the hydroxides. Electrochemical and catalytic tests as well as SEM/EDS and mu-XRFIXRD analyses allowed to correlate the effect of the number of electrical contact points with materials properties. Lastly, syntheses were performed on Pt plates to study the effect of the electrical behaviour and shape of the support on the composition of the film. A more homogeneous coating of the foam surface was achieved by adopting a configuration with 3 contact points since the reduction of nitrates and water molecules that generates the basic media in the vicinity of the support was enhanced. Layer thicknesses up to 5-15 mu m were deposited; however, the sequential precipitation of a film with composition closer to the expected one and a layer enriched in Al and Rh (outer layer) was not avoided. The improvement in the coating gave rise to enhanced performances for a sample prepared at -1.1 V for 3000 s. Contrarily, the low adherence of the outer layer in a sample prepared at -1.2 V for 2000 s during both calcination and catalytic tests may be responsible of the unexpected decrease in catalytic performances. The same sequential precipitation was observed by performing the syntheses on Pt plates, showing that the electrical nature the support did not play a key role on this phenomenon. (C) 2014 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 4.636
Times cited: 14
DOI: 10.1016/J.CATTOD.2014.10.003
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“Effect of process parameters on the photocatalytic soot degradation on self-cleaning cementitious materials”. Smits M, Huygh D, Craeye B, Lenaerts S, Catalysis today 230, 250 (2014). http://doi.org/10.1016/J.CATTOD.2013.10.001
Abstract: Soot deposition has the negative ability to devalue the aesthetic appearance of buildings. Titanium dioxide applied on the building material is one way to counteract this problem as it provides air-purifying and self-cleaning properties due to its photocatalytic activity. In literature, photocatalytic soot oxidation was described, but until now, little information was available about the influence of process parameters on the photocatalytic degradation efficiency. The influence of three process parameters was tested in this study, namely TiO2 concentration, soot concentration and water-to-cement ratio (WIC-ratio) of the mortar substrates. The results revealed 50 mu gTiO(2) cm(-2) is better to use on the cementitious materials than 250 mu gTiO(2) cm(-2). The soot concentrations occurring in real-world situations will not inhibit the photocatalyst to be activated by light. Furthermore, the photonic efficiency increases slightly for lower WIC-ratios. This can be of interest for structural building applications, since a lower WIC-ratio results in a lower porosity of the samples and consequently in an increase in mortar strength. (C) 2013 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL); Energy and Materials in Infrastructure and Buildings (EMIB)
Impact Factor: 4.636
Times cited: 14
DOI: 10.1016/J.CATTOD.2013.10.001
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“Fabrication of perovskite capillary membranes for high temperature gas separation”. Van Noyen J, Middelkoop V, Buysse C, Kovalevsky A, Snijkers F, Buekenhoudt A, Mullens S, Luyten J, Kretzschmar J, Lenaerts S, Catalysis today 193, 172 (2012). http://doi.org/10.1016/J.CATTOD.2012.03.005
Abstract: Oxygen-permeable perovskites with mixed ionic-electronic conducting properties can play an important role in carbon capture and storage techniques. Their ability to separate oxygen from air is needed, more specifically, in oxy-fuel and pre-combustion technologies. In this work, the first detailed comparative analysis and new results are reported on four types of Ba0.5Sr0.5Co0.8Fe0.2O3-delta (BSCF) capillary membranes: non-coated sulphur-containing; catalyst-coated sulphur-containing; non-coated sulphur-free and catalyst-coated sulphur-free. The fabrication of BSCF capillaries by a spinning technique based on phase inversion is further discussed and their oxygen separation performances are interpreted. The comparison of the performance of these different generations of BSCF capillaries of similar dimensions demonstrates a significant impact of the sulphur contamination on both the oxygen flux through the membrane and the activation energy of the overall oxygen transport mechanism. Careful attention is paid to the effect of activation layers on both sulphur-free and sulphur-containing types of capillaries. Additional long-term testing of the sulphur-free BSCF capillaries is presented, where partial decomposition of the membrane surface was observed due to kinetic demixing. (c) 2012 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.636
Times cited: 9
DOI: 10.1016/J.CATTOD.2012.03.005
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“Surface photovoltage measurements : a quick assessment of the photocatalytic activity?”.Verbruggen SW, Dirckx JJJ, Martens JA, Lenaerts S, Catalysis today 209, 215 (2013). http://doi.org/10.1016/J.CATTOD.2012.11.010
Abstract: Surface photovoltage (SPV) measurements can contribute to a better understanding of electronic properties of photocatalysts under illumination. Direct linking of SPV data to the actual photocatalytic activity remains troublesome. This work aims to discuss SPV measurements from a photocatalytic point of view. By means of several application-based scenarios we illustrate that the trend between SPV and photocatalysis strongly depends on parameters such as the crystal structure, surface modifications, morphology and humidity. This makes the interpretation far from straightforward.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.636
Times cited: 8
DOI: 10.1016/J.CATTOD.2012.11.010
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“Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene”. de la Croix T, Claes N, Eyley S, Thielemans W, Bals S, De Vos D, Catalysis Science &, Technology (2023). http://doi.org/10.1039/D3CY00370A
Abstract: The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.
Keywords: A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Impact Factor: 5
DOI: 10.1039/D3CY00370A
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“Mode Transition of Filaments in Packed-Bed Dielectric Barrier Discharges”. Gao M, Zhang Y, Wang H, Guo B, Zhang Q, Bogaerts A, Catalysts 8, 248 (2018). http://doi.org/10.3390/catal8060248
Abstract: We investigated the mode transition from volume to surface discharge in a packed bed dielectric barrier discharge reactor by a two-dimensional particle-in-cell/Monte Carlo collision method. The calculations are performed at atmospheric pressure for various driving voltages and for gas mixtures with different N2 and O2 compositions. Our results reveal that both a change of the driving voltage and gas mixture can induce mode transition. Upon increasing voltage, a mode transition from hybrid (volume+surface) discharge to pure surface discharge occurs, because the charged species can escape much more easily to the beads and charge the bead surface due to the strong electric field at high driving voltage. This significant surface charging will further enhance the tangential component of the electric field along the dielectric bead surface, yielding surface ionization waves (SIWs). The SIWs will give rise to a high concentration of reactive species on the surface, and thus possibly enhance the surface activity of the beads, which might be of interest for plasma catalysis. Indeed, electron impact excitation and ionization mainly take place near the bead surface. In addition, the propagation speed of SIWs becomes faster with increasing N2 content in the gas mixture, and slower with increasing O2 content, due to the loss of electrons by attachment to O2
molecules. Indeed, the negative O-2 ion density produced by electron impact attachment is much higher than the electron and positive O+2 ion density. The different ionization rates between N2 and O2 gases will create different amounts of electrons and ions on the dielectric bead surface, which might also have effects in plasma catalysis.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.082
Times cited: 7
DOI: 10.3390/catal8060248
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“Hydrogenation of Carbon Dioxide to Value-Added Chemicals by Heterogeneous Catalysis and Plasma Catalysis”. Liu M, Yi Y, Wang L, Guo H, Bogaerts A, Catalysts 9, 275 (2019). http://doi.org/10.3390/catal9030275
Abstract: Due to the increasing emission of carbon dioxide (CO2), greenhouse effects are becoming more and more severe, causing global climate change. The conversion and utilization of CO2 is one of the possible solutions to reduce CO2 concentrations. This can be accomplished, among other methods, by direct hydrogenation of CO2, producing value-added products. In this review, the progress of mainly the last five years in direct hydrogenation of CO2 to value-added chemicals (e.g., CO, CH4, CH3OH, DME, olefins, and higher hydrocarbons) by heterogeneous catalysis and plasma catalysis is summarized, and research priorities for CO2 hydrogenation are proposed.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.082
DOI: 10.3390/catal9030275
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“Altering conversion and product selectivity of dry reforming of methane in a dielectric barrier discharge by changing the dielectric packing material”. Michielsen I, Uytdenhouwen Y, Bogaerts A, Meynen V, Catalysts 9, 51 (2019). http://doi.org/10.3390/CATAL9010051
Abstract: We studied the influence of dense, spherical packing materials, with different chemical compositions, on the dry reforming of methane (DRM) in a dielectric barrier discharge (DBD) reactor. Although not catalytically activated, a vast effect on the conversion and product selectivity could already be observed, an influence which is often neglected when catalytically activated plasma packing materials are being studied. The alpha-Al2O3 packing material of 2.0-2.24 mm size yields the highest total conversion (28%), as well as CO2 (23%) and CH4 (33%) conversion and a high product fraction towards CO (similar to 70%) and ethane (similar to 14%), together with an enhanced CO/H-2 ratio of 9 in a 4.5 mm gap DBD at 60 W and 23 kHz. gamma-Al2O3 is only slightly less active in total conversion (22%) but is even more selective in products formed than alpha-Al2O3 BaTiO3 produces substantially more oxygenated products than the other packing materials but is the least selective in product fractions and has a clear negative impact on CO2 conversion upon addition of CH4. Interestingly, when comparing to pure CO2 splitting and when evaluating differences in products formed, significantly different trends are obtained for the packing materials, indicating a complex impact of the presence of CH4 and the specific nature of the packing materials on the DRM process.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.082
Times cited: 4
DOI: 10.3390/CATAL9010051
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“The Potential Use of Core-Shell Structured Spheres in a Packed-Bed DBD Plasma Reactor for CO2 Conversion”. Uytdenhouwen Y, Meynen V, Cool P, Bogaerts A, Catalysts 10, 530 (2020). http://doi.org/10.3390/catal10050530
Abstract: This work proposes to use core-shell structured spheres to evaluate whether it allows to individually optimize bulk and surface effects of a packing material, in order to optimize conversion and energy efficiency. Different core-shell materials have been prepared by spray coating, using dense spheres (as core) and powders (as shell) of SiO2, Al2O3, and BaTiO3. The materials are investigated for their performance in CO2 dissociation and compared against a benchmark consisting of a packed-bed reactor with the pure dense spheres, as well as an empty reactor. The results in terms of CO2 conversion and energy efficiency show various interactions between the core and shell material, depending on their combination. Al2O3 was found as the best core material under the applied conditions here, followed by BaTiO3 and SiO2, in agreement with their behaviour for the pure spheres. Applying a thin shell layer on the cores showed equal performance between the different shell materials. Increasing the layer thickness shifts this behaviour, and strong combination effects were observed depending on the specific material. Therefore, this method of core-shell spheres has the potential to allow tuning of the packing properties more closely to the application by designing an optimal combination of core and shell.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.9
DOI: 10.3390/catal10050530
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