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“Synthesis, structure, and electrochemical properties of k-based sulfates K2M2(SO4)3) with M = Fe and Cu”. Lander L, Rousse G, Batuk D, Colin CV, Dalla Corte DA, Tarascon J-M, Inorganic chemistry 56, 2013 (2017). http://doi.org/10.1021/ACS.INORGCHEM.6B02526
Abstract: Stabilizing new host structures through potassium extraction from K-based polyanionic materials has been proven to be an interesting approach to develop new Li+/Na+ insertion materials. Pursuing the same trend, we here report the feasibility of preparing langbeinite “Fe-2(SO4)(3)” via electrochemical and chemical oxidation of K2Fe2(SO4)(3). Additionally, we succeeded in stabilizing a new K2Cu2(SO4)(3) phase via a solid-state synthesis approach. This novel compound crystallizes in a complex orthorhombic structure that differs from that of langbeinite as deduced from synchrotron X-ray and neutron powder diffraction. Electrochemically, the performance of this new phase is limited, which we explain in terms of sluggish diffusion kinetics. We further show that K2Cu2(SO4)(3) decomposes into K2Cu3O(SO4)(3) on heating, and we report for the first time the synthesis of fedotovite K2Cu3O(SO4)(3). Finally, the fundamental attractiveness of these S = 1/2 systems for physicists is examined by neutron magnetic diffraction, which reveals the absence of a long-range ordering of Cu2+ magnetic moments down to 1.5 K.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 13
DOI: 10.1021/ACS.INORGCHEM.6B02526
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“Molybdenum oxide nitrides of the Mo2(O,N,\square)5 type : on the way to Mo2O5”. Weber D, Huber M, Gorelik TE, Abakumov AM, Becker N, Niehaus O, Schwickert C, Culver SP, Boysen H, Senyshyn A, Poettgen R, Dronskowski R, Ressler T, Kolb U, Lerch M, Inorganic chemistry 56, 8782 (2017). http://doi.org/10.1021/ACS.INORGCHEM.7B00551
Abstract: Blue-colored molybdenum oxide nitrides of the Mo-2(O,N,square)(5) type were synthesized by direct nitridation of commercially available molybdenum trioxide with a mixture of gaseous ammonia and oxygen. Chemical composition, crystal structure, and stability of the obtained and hitherto unknown compounds are studied extensively. The average oxidation state of +5 for molybdenum is proven by Mo K near-edge X-ray absorption spectroscopy; the magnetic behavior is in agreement with compounds exhibiting (MoO6)-O-v units. The new materials are stable up to similar to 773 K in an inert gas atmosphere. At higher temperatures, decomposition is observed. X-ray and neutron powder diffraction, electron diffraction, and high-resolution transmission electron microscopy reveal the structure to be related to VNb9O24.9-type phases, however, with severe disorder hampering full structure determination. Still, the results demonstrate the possibility of a future synthesis of the potential binary oxide Mo2O5. On the basis of these findings, a tentative suggestion on the crystal structure of the potential compound Mo2O5, backed by electronic-structure and phonon calculations from first principles, is given.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 3
DOI: 10.1021/ACS.INORGCHEM.7B00551
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“The influence of branched alkyl side chains in A-D-A oligothiophenes on the photovoltaic performance and morphology of solution-processed bulk-heterojunction solar cells”. Ata I, Ben Dkhil S, Pfannmoeller M, Bals S, Duche D, Simon J-J, Koganezawa T, Yoshimoto N, Videlot-Ackermann C, Margeat O, Ackermann J, Baeuerle P, Organic chemistry frontiers : an international journal of organic chemistry 4, 1561 (2017). http://doi.org/10.1039/C7QO00222J
Abstract: Besides providing sufficient solubility, branched alkyl chains also affect the film-forming and packing properties of organic semiconductors. In order to avoid steric hindrance as it is present in wide-spread alkyl chains comprising a branching point position at the C2-position, i.e., 2-ethylhexyl, the branching point can be moved away from the pi-conjugated backbone. In this report, we study the influence of the modification of the branching point position from the C2-position in 2-hexyldecylamine (1) to the C4-position in 4-hexyldecylamine (2) connected to the central dithieno[3,2-b: 2', 3'-d] pyrrole (DTP) moiety in a well-studied A-D-A oligothiophene on the optoelectronic properties and photovoltaic performance in solution- processed bulk heterojunction solar cells (BHJSCs) with [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) as the acceptor material. Post-treatment of the photoactive layers is performed via solvent vapor annealing (SVA) in order to improve the film microstructure of the bulk heterojunction. The time evolution of nanoscale morphological changes is followed by combining scanning transmission electron microscopy with low-energy-loss spectroscopic imaging (STEM-SI), solid-state absorption spectroscopy, and two-dimensional grazing incidence X-ray diffraction (2D-GIXRD). Our results show an improvement of the photovoltaic performance that is dependent on the branching point position in the donor oligomer. Optical spacers are utilized to increase light absorption inside the co-oligomer 2-based BHJSCs leading to increased power conversion efficiencies (PCEs) of 8.2% when compared to the corresponding co-oligomer 1-based devices. A STEM-SI analysis of the respective device cross-sections of active layers containing 1 and 2 as donor materials indeed reveals significant differences in their respective active layer morphologies.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.955
Times cited: 24
DOI: 10.1039/C7QO00222J
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“Mechanical behavior of ultrathin sputter deposited porous amorphous Al2O3 films”. van der Rest A, Idrissi H, Henry F, Favache A, Schryvers D, Proost J, Raskin J-P, Van Overmeere Q, Pardoen T, Acta materialia 125, 27 (2017). http://doi.org/10.1016/j.actamat.2016.11.037
Abstract: The determination of the mechanical properties of porous amorphous Al2O3 thin films is essential to address reliability issues in wear-resistant, optical and electronic coating applications. Testing the mechanical properties of Al2O3 films thinner than 200 nm is challenging, and the link between the mechanical behavior and the microstructure of such films is largely unknown. Herein, we report on the elastic and viscoplastic mechanical properties of amorphous Al2O3 thin films synthesized by reactive magnetron sputtering using a combination of internal stress, nanoindentation, and on-chip uniaxial tensile testing, together with mechanical homogenization models to separate the effect of porosity from intrinsic variations of the response of the sound material. The porosity is made of voids with 2e30 nm diameter. The Young's modulus and hardness of the films decrease by a factor of two when the deposition pressure increases from 1.2 to 8 mTorr. The contribution of porosity was found to be small, and a change in the atomic structure of the amorphous Al2O3 matrix is hypothesized to be the main contributing factor. The activation volume associated to the viscoplastic deformation mechanism is around 100 Å3. Differences in the atomic structure of the films could not be revealed by electron diffraction, pointing to a minute effect of atomic arrangement on the elastic properties.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.301
Times cited: 5
DOI: 10.1016/j.actamat.2016.11.037
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“Homogeneous flow and size dependent mechanical behavior in highly ductile Zr 65 Ni 35 metallic glass films”. Ghidelli M, Idrissi H, Gravier S, Blandin J-J, Raskin J-P, Schryvers D, Pardoen T, Acta materialia 131, 246 (2017). http://doi.org/10.1016/j.actamat.2017.03.072
Abstract: Motivated by recent studies demonstrating a high strength – high ductility potential of nano-scale metallic glass samples, the mechanical response of freestanding Zr65Ni35 film with sub-micron thickness has been investigated by combining advanced on-chip tensile testing and electron microscopy. Large deformation up to 15% is found for specimen thicknesses below 500 nm with variations depending on specimen size and frame compliance. The deformation is homogenous until fracture, with no evidence of shear banding. The yield stress is doubled when decreasing the specimen cross-section, reaching ~3 GPa for small cross-sections. The fracture strain variation is related to both the stability of the test device and to the specimen size. The study concludes on clear disconnect between the mechanisms controlling the onset of plasticity and the fracture process.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.301
Times cited: 42
DOI: 10.1016/j.actamat.2017.03.072
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“Direct nucleation of hexagonal boron nitride on diamond : crystalline properties of hBN nanowalls”. Hoang D-Q, Korneychuk S, Sankaran KJ, Pobedinskas P, Drijkoningen S, Turner S, Van Bael MK, Verbeeck J, Nicley SS, Haenen K, Acta materialia 127, 17 (2017). http://doi.org/10.1016/J.ACTAMAT2017.01.002
Abstract: Hexagonal boron nitride (hBN) nanowalls were deposited by unbalanced radio frequency sputtering on (100)-oriented silicon, nanocrystalline diamond films, and amorphous silicon nitride (Si3N4) membranes. The hBN nanowall structures were found to grow vertically with respect to the surface of all of the substrates. To provide further insight into the nucleation phase and possible lattice distortion of the deposited films, the structural properties of the different interfaces were characterized by transmission electron microscopy. For Si and Si3N4 substrates, turbostratic and amorphous BN phases form a clear transition zone between the substrate and the actual hBN phase of the bulk nanowalls. However, surprisingly, the presence of these phases was suppressed at the interface with a nanocrystalline diamond film, leading to a direct coupling of hBN with the diamond surface, independent of the vertical orientation of the diamond grain. To explain these observations, a growth mechanism is proposed in which the hydrogen terminated surface of the nanocrystalline diamond film leads to a rapid formation of the hBN phase during the initial stages of growth, contrary to the case of Si and Si3N4 substrates. (C) 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.301
DOI: 10.1016/J.ACTAMAT2017.01.002
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“Encapsulation of bimetallic metal nanoparticles into robust zirconium-based metal-organic frameworks : evaluation of the catalytic potential for size-selective hydrogenation”. Roesler C, Dissegna S, Rechac VL, Kauer M, Guo P, Turner S, Ollegott K, Kobayashi H, Yamamoto T, Peeters D, Wang Y, Matsumura S, Van Tendeloo G, Kitagawa H, Muhler M, Llabres i Xamena FX, Fischer RA, Chemistry: a European journal 23, 3583 (2017). http://doi.org/10.1002/CHEM.201603984
Abstract: The realization of metal nanoparticles (NPs) with bimetallic character and distinct composition for specific catalytic applications is an intensively studied field. Due to the synergy between metals, most bimetallic particles exhibit unique properties that are hardly provided by the individual monometallic counterparts. However, as small-sized NPs possess high surface energy, agglomeration during catalytic reactions is favored. Sufficient stabilization can be achieved by confinement of NPs in porous support materials. In this sense, metal-organic frameworks (MOFs) in particular have gained a lot of attention during the last years; however, encapsulation of bimetallic species remains challenging. Herein, the exclusive embedding of preformed core-shell PdPt and RuPt NPs into chemically robust Zr-based MOFs is presented. Microstructural characterization manifests partial retention of the core-shell systems after successful encapsulation without harming the crystallinity of the microporous support. The resulting chemically robust NP@UiO-66 materials exhibit enhanced catalytic activity towards the liquid-phase hydrogenation of nitrobenzene, competitive with commercially used Pt on activated carbon, but with superior size-selectivity for sterically varied substrates.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.317
Times cited: 13
DOI: 10.1002/CHEM.201603984
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“p -CoO x / n -SnO 2 nanostructures: New highly selective materials for H 2 S detection”. Rumyantseva MN, Vladimirova SA, Vorobyeva NA, Giebelhaus I, Mathur S, Chizhov AS, Khmelevsky NO, Aksenenko AY, Kozlovsky VF, Karakulina OM, Hadermann J, Abakumov AM, Gaskov AM, Sensors and actuators : B : chemical (2017). http://doi.org/10.1016/j.snb.2017.08.096
Abstract: Nanostructures p-CoOx/n-SnO2 based on tin oxide nanowires have been prepared by two step CVD technique and characterized in detail by XRD, XRF, XPS, HAADF-STEM imaging and EDX-STEM mapping. Depending on the temperature of decomposition of cobalt complex during the second step of CVD synthesis of nanostructures cobalt oxide forms a coating and/or isolated nanoparticles on SnO2 nanowire surface. It was found that cobalt presents in +2 and +3 oxidation states. The measurements of gas sensor properties have been carried out during exposure to CO (14 ppm), NH3 (21 ppm), and H2S (2 ppm) in dry air. The opposite trends were observed in the effect of cobalt oxide on the SnO2 gas sensitivity when detecting CO or NH3 in comparison to H2S. The decrease of sensor signal toward CO and NH3 was attributed to high catalytic activity of Co3O4 in oxidation of these gases. Contrary, the significant increase of sensor signal in the presence of H2S was attributed to the formation of metallic cobalt sulfide and removal of the barrier between p-CoOx and n-SnO2. This effect provides an excellent selectivity of p-CoOx/n-SnO2 nanostructures in H2S detection.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.401
Times cited: 13
DOI: 10.1016/j.snb.2017.08.096
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“A joint action of aptamers and gold nanoparticles chemically trapped on a glassy carbon support for the electrochemical sensing of ofloxacin”. Pilehvar S, Reinemann C, Bottari F, Vanderleyden E, Van Vlierberghe S, Blust R, Strehlitz B, De Wael K, Sensors and actuators : B : chemical 240, 1024 (2017). http://doi.org/10.1016/J.SNB.2016.09.075
Abstract: A joint action of ssDNA aptamers and electrochemistry is a key element in developing successful biosensing platforms, since aptamers are capable of binding various targets with high specificity, and electrochemistry is one of the most sensitive techniques for on-site detections. A continuous search for improved immobilization and sensing strategies of aptamers on transducer surfaces resulted in the strategy presented in this article. The strategy is based on the covalent attachment of gold nanoparticles on the surface of glassy carbon electrodes through sulfhydryl-terminated monolayer, acting as a glue to connect AuNPs on the electrode. The covalently attached gold nanoparticles modified glassy carbon electrodes have been applied for the efficient immobilization of thiolated ssDNA probes, with a surface coverage of about 8.54 × 1013 molecules cm−2 which was 7-fold higher than that on the electrochemically deposited gold nanoparticles. Consequently, improved sensitivity, good reproducibility and stability are achieved for electrochemical aptasensor. Combined with the high affinity and specificity of an aptamer, a simple, novel, rapid, sensitive and label-free electrochemical aptasensor was successfully fabricated for ofloxacin (OFL) detection. The linear dynamic range of the sensor varies between 5 × 10−8 to 2 × 10−5 M OFL with a detection limit of 1 × 10−9 M OFL. A potential application in environmental monitoring was demonstrated by using this sensing strategy for the determination of OFL in (experimentally spiked) real samples such as tap water and effluent of sewage treatment plant. The proposed nanoaptasensor combines the advantages of the covalent attachment of neatly arranged AuNPs (enlarged active surface area and strengthened electrochemical signal) and the elimination of labels for the amplified detection of OFL, with the covalent attachment of highly specific aptamers to the surface of the modified electrode.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 5.401
Times cited: 21
DOI: 10.1016/J.SNB.2016.09.075
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“Cooperative electrocatalytic and chemoselective alcohol oxidation by Shvo's catalyst”. Lybaert J, Trashin S, Maes BUW, De Wael K, Abbaspour Tehrani K, Advanced synthesis and catalysis 359, 919 (2017). http://doi.org/10.1002/ADSC.201600783
Abstract: A new electrocatalytic conversion of alcohols to ketones and aldehydes was developed based on an electrochemical study of Shvos complex. The oxidation of secondary alcohols was efficiently performed under mild conditions using a catalytic amount of Shvos catalyst, in combination with a sub-stoichiometric amount of 2,6-dimethoxy-1,4- benzoquinone in N,N-dimethylformamide at 80 8C. The hydroquinone thus formed is continuously reoxidized with the aid of an electrochemical device. Excellent yields for different ketones, aromatic as well as aliphatic and a,b-unsaturated ketones, are obtained. In addition, chemoselectivity towards oxidation of the secondary alcohol is achieved when converting vicinal diols such as 1,2-octanediol and 1,2-decanediol.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Organic synthesis (ORSY)
Impact Factor: 5.646
Times cited: 4
DOI: 10.1002/ADSC.201600783
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“Thiol-ethylene bridged PMO: A high capacity regenerable mercury adsorbent via intrapore mercury thiolate crystal formation”. Esquivel D, Ouwehand J, Meledina M, Turner S, Tendeloo GV, Romero-Salguero FJ, Clercq JD, Voort PVD, Journal of hazardous materials 339, 368 (2017). http://doi.org/10.1016/j.jhazmat.2017.06.051
Abstract: Highly ordered thiol-ethylene bridged Periodic Mesoporous Organosilicas were synthesized directly from a homemade thiol-functionalized bis-silane precursor. These high surface area materials contain up to 4.3 mmol/g sulfur functions in the walls and can adsorb up to 1183 mg/g mercury ions. Raman spectroscopy reveals the existence of thiol and disulfide moieties. These groups have been evaluated by a combination of Raman spectroscopy, Ellman’s reagent and elemental analysis. The adsorption of mercury ions was evidenced by different techniques, including Raman, XPS and porosimetry, which indicate that thiol groups are highly accessible to mercury. Scanning transmission electron microscopy combined with EDX showed an even homogenous distribution of the sulfur atoms throughout the structure, and have revealed for the first time that a fraction of the adsorbed mercury is forming thiolate nanocrystals in the pores. The adsorbent is highly selective for mercury and can be regenerated and reused multiple times, maintaining its structure and functionalities and showing only a marginal loss of adsorption capacity after several runs.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.065
Times cited: 12
DOI: 10.1016/j.jhazmat.2017.06.051
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“Ship-in-a-bottle CMPO in MIL-101(Cr) for selective uranium recovery from aqueous streams through adsorption”. De Decker J, Folens K, De Clercq J, Meledina M, Van Tendeloo G, Du Laing G, Van Der Voort P, Journal of hazardous materials 335, 1 (2017). http://doi.org/10.1016/J.JHAZMAT.2017.04.029
Abstract: Mesoporous MIL-101(Cr) is used as host for a ship-in-a-bottle type adsorbent for selective U(VI) recovery from aqueous environments. The acid-resistant cage-type MOF is built in-situ around N,N-Diisobutyl-2-(octylphenylphosphoryl)acetamide (CMPO), a sterically demanding ligand with high U(VI) affinity. This one-step procedure yields an adsorbent which is an ideal compromise between homogeneous and heterogeneous systems, where the ligand can act freely within the pores of MIL-101, without leaching, while the adsorbent is easy separable and reusable. The adsorbent was characterized by XRD, FTIR spectroscopy, nitrogen adsorption, XRF, ADF-STEM and EDX, to confirm and quantify the successful encapsulation of the CMPO in MIL-101, and the preservation of the host. Adsorption experiments with a central focus on U(VI) recovery were performed. Very high selectivity for U(VI) was observed, while competitive metal adsorption (rare earths, transition metals...) was almost negligible. The adsorption capacity was calculated at 5.32 mg U/g (pH 3) and 27.99 mg U/g (pH 4), by fitting equilibrium data to the Langmuir model. Adsorption kinetics correlated to the pseudo-second-order model, where more than 95% of maximum uptake is achieved within 375 min. The adsorbed U(VI) is easily recovered by desorption in 0.1 M HNO3. Three adsorption/desorption cycles were performed. (C) 2017 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.065
Times cited: 35
DOI: 10.1016/J.JHAZMAT.2017.04.029
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“Electrochemical reduction of nalidixic acid at glassy carbon electrodemodified with multi-walled carbon nanotubes”. Patiño Y, Pilehvar S, Díaz E, Ordóñez S, De Wael K, Journal of hazardous materials 323, 621 (2017). http://doi.org/10.1016/J.JHAZMAT.2016.10.023
Abstract: The aqueous phase electrochemical degradation of nalidixic acid (NAL) is studied in this work, using cyclic voltammetry (CV) and differential pulse voltammetry (DPV) as instrumental techniques. The promotional effect of multi-walled carbon nanotubes (MWCNT) on the the performance of glassy carbon electrodes is demonstrated, being observed that these materials catalyze the NAL reduction. The effect of surface functional groups on MWCNT −MWCNT-COOH and MWCNT-NH2was also studied. The modification of glassy carbon electrode (GCE) with MWCNT leads to an improved performance for NAL reduction following the order of MWCNT > MWCNT-NH2 > MWCNT-COOH. The best behavior at MWCNT-GCE is mainly due to both the increased electrode active area and the enhanced MWCNT adsorption properties. The NAL degradation was carried out under optimal conditions (pH = 5.0, deposition time = 20 s and volume of MWCNT = 10 μL) using MWCNT-GCE obtaining an irreversible reduction of NAL to less toxic products. Paramaters as the number of DPV cycles and the volume/area (V/A) ratio were optimized for maximize pollutant degradation. It was observed that after 15 DPV scans and V/A = 8, a complete reduction was obtained, obtaining two sub-products identified by liquid chromatography-mass spectrometry (LCMS).
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.065
Times cited: 4
DOI: 10.1016/J.JHAZMAT.2016.10.023
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“Gas phase photocatalytic spiral reactor for fast and efficient pollutant degradation”. Blommaerts N, Asapu R, Claes N, Bals S, Lenaerts S, Verbruggen SW, Chemical engineering journal 316, 850 (2017). http://doi.org/10.1016/j.cej.2017.02.038
Abstract: Photocatalytic reactors for the degradation of gaseous organic pollutants often suffer from major limitations such as small reaction area, sub-optimal irradiation conditions and thus limited reaction rate. In this work, an alternative solution is presented that involves a glass tube coated on the inside with (silvermodified) TiO2 and spiraled around a UVA lamp. First, the spiral reactor is coated from the inside with TiO2 using an experimentally verified procedure that is optimized toward UV light transmission. This procedure is kept as simple as possible and involves a single casting step of a 1 wt% suspension of TiO2 in ethanol through the spiral. This results in a coated tube that absorbs nearly all incident UV light under the experimental conditions used. The optimized coated spiral reactor is then benchmarked to a conventional annular photoreactor of the same outer dimensions and total catalyst loading over a broad range of experimental conditions. Although residence time distribution experiments indicate slightly longer dwelling of molecules in the spiral reactor, no significant difference in by-passing of gas between the spiral reactor and the annular reactor can be claimed. Acetaldehyde degradation efficiency of 100% is obtained with the spiral reactor for a residence time as low as 60 s, whereas the annular reactor could not achieve full degradation even at 1000 s residence time. In a final case study, addition of long-term stable silver nanoparticles, protected by an ultra-thin polymer shell applied via the layer-by-layer (LbL) method, to the spiral reactor coating is shown to double the degradation efficiency and provides an interesting strategy to cope with higher pollutant concentrations without changing the overall dimensions.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 6.216
Times cited: 30
DOI: 10.1016/j.cej.2017.02.038
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“Gliding arc plasma for CO 2 conversion: Better insights by a combined experimental and modelling approach”. Wang W, Mei D, Tu X, Bogaerts A, Chemical engineering journal 330, 11 (2017). http://doi.org/10.1016/j.cej.2017.07.133
Abstract: A gliding arc plasma is a potential way to convert CO2 into CO and O2, due to its non-equilibrium character, but little is known about the underlying mechanisms. In this paper, a self-consistent two-dimensional (2D) gliding arc model is developed, with a detailed non-equilibrium CO2 plasma chemistry, and validated with experiments. Our calculated values of the electron number density in the plasma, the CO2 conversion and energy efficiency show reasonable agreement with the experiments, indicating that the model can provide a realistic picture of the plasma chemistry. Comparison of the results with classical thermal conversion, as well as other plasma-based technologies for CO2 conversion reported in literature, demonstrates the non-equilibrium character of the gliding arc, and indicates that the gliding arc is a promising plasma reactor for CO2 conversion. However, some process modifications should be exploited to further improve its performance. As the model provides a realistic picture of the plasma behaviour, we use it first to investigate the plasma characteristics in a whole gliding arc cycle, which is necessary to understand the underlying mechanisms. Subsequently, we perform a chemical kinetics analysis, to investigate the different pathways for CO2 loss and formation. Based on the revealed discharge properties and the underlying CO2 plasma chemistry, the model allows us to propose solutions on how to further improve the
CO2 conversion and energy efficiency by a gliding arc plasma.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
Times cited: 38
DOI: 10.1016/j.cej.2017.07.133
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“CO 2 dissociation in a packed bed DBD reactor: First steps towards a better understanding of plasma catalysis”. Michielsen I, Uytdenhouwen Y, Pype J, Michielsen B, Mertens J, Reniers F, Meynen V, Bogaerts A, Chemical engineering journal 326, 477 (2017). http://doi.org/10.1016/j.cej.2017.05.177
Abstract: Plasma catalysis is gaining increasing interest for CO2 conversion, but the interaction between the plasma and catalyst is still poorly understood. This is caused by limited systematic materials research, since most works combine a plasma with commercial supported catalysts and packings. In the present paper, we study the influence of specific material and reactor properties, as well as reactor/bead configuration, on the conversion and energy efficiency of CO2 dissociation in a packed bed dielectric barrier discharge (DBD) reactor. Of the various packing materials investigated, BaTiO3 yields the highest conversion and energy efficiency, i.e., 25% and 4.5%.
Our results show that, when evaluating the influence of catalysts, the impact of the packing (support) material itself cannot be neglected, since it can largely affect the conversion and energy efficiency. This shows the large potential for further improvement of packed bed plasma reactors for CO2 conversion and other chemical conversion reactions by adjusting both packing (support) properties and catalytically active sites. Moreover, we clearly prove that comparison of results obtained in different reactor setups should be done with care, since there is a large effect of the reactor setup and reactor/bead configuration.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.216
Times cited: 49
DOI: 10.1016/j.cej.2017.05.177
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“Simultaneous creation of metal nanoparticles in metal organic frameworks via spray drying technique”. Gholampour N, Chaemchuen S, Hu Z-Y, Mousavi B, Van Tendeloo G, Verpoort F, Chemical engineering journal 322, 702 (2017). http://doi.org/10.1016/J.CEJ.2017.04.085
Abstract: In-situ fabrication of palladium(0) nanoparticles inside zeolitic imidazolate frameworks (ZIF-8) has been established via one-step facile spray-dry technique. Crystal structures and morphologies of the Pd@ZIF-8 samples are investigated by powder XRD, TEM, SAED, STEM, and EDX techniques. High angle annular dark field scanning transmission electron microscopy (HAAD-STEM) and 3D tomographic analysis confirm the presence of palladium nanoparticles inside the ZIF-8 structure. The porosity, surface area and N-2 physisorption properties are evaluated for Pd@ZIF-8 with various palladium contents. Furthermore, Pd@ZIF-8 samples are effectively applied as heterogeneous catalysts in alkenes hydrogenation. This straightforward method is able to speed up the synthesis of encapsulation of metal nanoparticles in metal organic frameworks. (C) 2017 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.216
Times cited: 14
DOI: 10.1016/J.CEJ.2017.04.085
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“Polydopamine nanocoated whole-cell asymmetric biocatalysts”. Wang L, Hu Z-Y, Yang X-Y, Zhang B-B, Geng W, Van Tendeloo G, Su B-L, Chemical communications 53, 6617 (2017). http://doi.org/10.1039/C7CC01283G
Abstract: Our whole-cell biocatalyst with a polydopamine nanocoating shows high catalytic activity (5 times better productivity than the native cell) and reusability (84% of the initial yield after 5 batches, 8 times higher than the native cell) in asymmetric reduction. It also integrates with titania, silica, and magnetic nanoparticles for multi-functionalization.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.319
Times cited: 15
DOI: 10.1039/C7CC01283G
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“Disentangling the effect of seed size and crystal habit on gold nanoparticle seeded growth”. González-Rubio G, de Oliveira TM, Altantzis T, La Porta A, Guerrero-Martínez A, Bals S, Scarabelli L, Liz-Marzán LM, Chemical communications 53, 11360 (2017). http://doi.org/10.1039/C7CC06854A
Abstract: Oxidative etching was used to produce gold seeds of different sizes and crystal habits. Following detailed characterization, the seeds were grown under different conditions. Our results bring new insights toward understanding the effect of size and crystallinity on the growth of anisotropic particles, whilst identifying guidelines for the optimisation of new synthetic protocols of predesigned seeds.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.319
Times cited: 29
DOI: 10.1039/C7CC06854A
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“Unique opto-electronic structure and photo reduction properties of sulfur doped lead chromates explaining their instability in paintings”. Rahemi V, Sarmadian N, Anaf W, Janssens K, Lamoen D, Partoens B, De Wael K, Analytical chemistry 89, 3326 (2017). http://doi.org/10.1021/ACS.ANALCHEM.6B03803
Abstract: Chrome yellow refers to a group of synthetic inorganic pigments that became popular as an artists material from the second quarter of the 19th century. The color of the pigment, in which the chromate ion acts as a chromophore, is related to its chemical composition (PbCr1-xSxO4, with 0≤x≤0.8) and crystalline structure (monoclinic/orthorhombic). Their shades range from the yellow-orange to the paler yellow tones with increasing sulfate amount. These pigments show remarkable signs of degradation after limited time periods. Pure PbCrO4 (crocoite in its natural form) has a deep yellow color and is relatively stable, while the co-precipitate with lead sulfate (PbCr1-xSxO4) has a paler shade and seems to degrade faster. This degradation is assumed to be related to the reduction of Cr(VI) to Cr(III). We show that on increasing the sulfur(S)-content in chrome yellow, the band gap increases. Typically, when increasing the band gap, one might assume that a decrease in photo activity is the result. However, the photo activity relative to the Cr content, and thus Cr reduction, of sulfur-rich PbCr1-xSxO4 is found to be much higher compared to the sulfur-poor or non-doped lead chromates. This discrepancy can be explained by the evolution of the crystal and electronic structure as function of the sulfur content: first-principles density functional theory calculations show that both the absorption coefficient and reflection coefficients of the lead chromates change as a result of the sulfate doping in such a way that the generation of electron-hole pairs under illumination relative to the total Cr content increases. These changes in the material properties explain why paler shade yellow colors of this pigment are more prone to discoloration. The electronic structure calculations also demonstrate that lead chromate and its co-precipitates are p-type semiconductors, which explains the observed reduction reaction. As understanding this phenomenon is valuable in the field of cultural heritage, this study is the first joint action of photo-electrochemical measurements and first-principles calculations to approve the higher tendency of sulfur-rich lead chromates to darken.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.32
Times cited: 7
DOI: 10.1021/ACS.ANALCHEM.6B03803
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“Combined computed nanotomography and nanoscopic x-ray fluorescence imaging of cobalt nanoparticles in caenorhabditis elegans”. Cagno S, Brede DA, Nuyts G, Vanmeert F, Pacureanu A, Tucoulou R, Cloetens P, Falkenberg G, Janssens K, Salbu B, Lind OC, Analytical chemistry 89, 11435 (2017). http://doi.org/10.1021/ACS.ANALCHEM.7B02554
Abstract: Synchrotron radiation phase-contrast computed nanotomography (nano-CT) and two-and three-dimensional (2D and 3D) nanoscopic X-ray fluorescence (nano-XRF) were used to investigate the internal distribution of engineered-cobalt nanoparticles (Co NPs) in exposed individuals of the nematode Caenorhabditis elegans. Whole-nematodes and selected tissues and organs were 3D-rendered: anatomical 3D renderings with 50 nm voxel size enabled the visualization of spherical nanoparticle aggregates. with size tip to 200 nm within intact C. elegans. A 20 X 37 nm(2) high-brilliance beam was employed to obtain XRF elemental distribution maps of entire nematodes or anatomical details such as embryos, which could be compared with the CT data, These maps showed Co NPs to be predominantly present within the intestine and the epithelium, and they were not colocalized with Zn granules found in the lysosonie-containing vesicles or Fe agglomerates in the intestine. Iterated XRF scanning of a specimen at 0 degrees and 90 degrees angles suggested that NP aggregates were translocated into tissues outside of the intestinal lumen. Virtual-slicing by means of 2D XRF tomography, combined with holotomography, indicated presumable presence of individual NP aggregates inside the uterus and within embryos.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.32
Times cited: 13
DOI: 10.1021/ACS.ANALCHEM.7B02554
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“Atomic-scale mechanisms of plasma-assisted elimination of nascent base-grown carbon nanotubes”. Khalilov U, Bogaerts A, Neyts EC, Carbon 118, 452 (2017). http://doi.org/10.1016/j.carbon.2017.03.068
Abstract: Selective etching allows for obtaining carbon nanotubes with a specific chirality. While plasma-assisted etching has already been used to separate metallic tubes from their semiconducting counterparts, little is known about the nanoscale mechanisms of the etching process. We combine (reactive) molecular dynamics (MD) and force-bias Monte Carlo (tfMC) simulations to study H-etching of CNTs. In particular, during the hydrogenation and subsequent etching of both the carbon cap and the tube, they sequentially transform to different carbon nanostructures, including carbon nanosheet, nanowall, and polyyne chains, before they are completely removed from the surface of a substrate-bound Ni-nanocluster.We also found that onset of the etching process is different in the cases of the cap and the tube, although the overall etching scenario is similar in both cases. The entire hydrogenation/etching process for both cases is analysed in detail, comparing with available theoretical and experimental evidences.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.337
Times cited: 2
DOI: 10.1016/j.carbon.2017.03.068
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“Carbon-rich carbon nitride monolayers with Dirac cones : Dumbbell C4N”. Li L, Kong X, Leenaerts O, Chen X, Sanyal B, Peeters FM, Carbon 118, 285 (2017). http://doi.org/10.1016/J.CARBON.2017.03.045
Abstract: Two-dimensional (2D) carbon nitride materials play an important role in energy-harvesting, energy-storage and environmental applications. Recently, a new carbon nitride, 2D polyaniline (C3N) was proposed [PNAS 113 (2016) 7414-7419]. Based on the structure model of this C3N monolayer, we propose two new carbon nitride monolayers, named dumbbell (DB) C4N-I and C4N-II. Using first-principles calculations, we systematically study the structure, stability, and band structure of these two materials. In contrast to other carbon nitride monolayers, the orbital hybridization of the C/N atoms in the DB C4N monolayers is sp(3). Remarkably, the band structures of the two DB C4N monolayers have a Dirac cone at the K point and their Fermi velocities (2.6/2.4 x 10(5) m/s) are comparable to that of graphene. This makes them promising materials for applications in high-speed electronic devices. Using a tight-binding model, we explain the origin of the Dirac cone. (C) 2017 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 6.337
Times cited: 36
DOI: 10.1016/J.CARBON.2017.03.045
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Chirumamilla CS, Palagani A, Kamaraj B, Declerck K, Verbeek MWC, Ryabtsova O, De Bosscher K, Bougarne N, Ruttens B, Gevaert K, Houtman R, De Vos WH, Joossens J, van der Veken P, Augustyns K, van Ostade X, Bogaerts A, De Winter H, Vanden Berghe W (2017) Selective glucocorticoid receptor properties of GSK866 analogs with cysteine reactive warheads. Place of publication unknown, 1324
Abstract: Synthetic glucocorticoids (GC) are the mainstay therapy for treatment of acute and chronic inflammatory disorders. Due to the high adverse effects associated with long-term use, GC pharmacology has focused since the nineties on more selective GC ligand-binding strategies, classified as selective glucocorticoid receptor (GR) agonists (SEGRAs) or selective glucocorticoid receptor modulators (SEGRMs). In the current study, GSK866 analogs with electrophilic covalent-binding warheads were developed with potential SEGRA properties to improve their clinical safety profile for long-lasting topical skin disease applications. Since the off-rate of a covalently binding drug is negligible compared to that of a non-covalent drug, its therapeutic effects can be prolonged and typically, smaller doses of the drug are necessary to reach the same level of therapeutic efficacy, thereby potentially reducing systemic side effects. Different analogs of SEGRA GSK866 coupled to cysteine reactive warheads were characterized for GR potency and selectivity in various biochemical and cellular assays. GR- and NFκB-dependent reporter gene studies show favorable anti-inflammatory properties with reduced GR transactivation of two non-steroidal GSK866 analogs UAMC-1217 and UAMC-1218, whereas UAMC-1158 and UAMC-1159 compounds failed to modulate cellular GR activity. These results were further supported by GR immuno-localization and S211 phospho-GR western analysis, illustrating significant GR phosphoactivation and nuclear translocation upon treatment of GSK866, UAMC-1217, or UAMC-1218, but not in case of UAMC-1158 or UAMC-1159. Furthermore, mass spectrometry analysis of tryptic peptides of recombinant GR ligand-binding domain (LBD) bound to UAMC-1217 or UAMC-1218 confirmed covalent cysteine-dependent GR binding. Finally, molecular dynamics simulations, as well as glucocorticoid receptor ligand-binding domain (GR-LBD) coregulator interaction profiling of the GR-LBD bound to GSK866 or its covalently binding analogs UAMC-1217 or UAMC-1218 revealed subtle conformational differences that might underlie their SEGRA properties. Altogether, GSK866 analogs UAMC-1217 and UAMC-1218 hold promise as a novel class of covalent-binding SEGRA ligands for the treatment of topical inflammatory skin disorders.
Keywords: Administrative Services; A1 Journal article; Pharmacology. Therapy; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Medicinal Chemistry (UAMC)
Impact Factor: 6.429
Times cited: 2
DOI: 10.3389/FIMMU.2017.01324
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“Quantitative determination of residual silver distribution in nanoporous gold and its influence on structure and catalytic performance”. Mahr C, Kundu P, Lackmann A, Zanaga D, Thiel K, Schowalter M, Schwan M, Bals S, Wittstock A, Rosenauer A, Journal of catalysis 352, 52 (2017). http://doi.org/10.1016/j.jcat.2017.05.002
Abstract: Large efforts have been made trying to understand the origin of the high catalytic activity of dealloyed nanoporous gold as a green catalyst for the selective promotion of chemical reactions at low temperatures. Residual silver, left in the sample after dealloying of a gold-silver alloy, has been shown to have a strong influence on the activity of the catalyst. But the question of how the silver is distributed within the porous structure has not finally been answered yet. We show by quantitative energy dispersive X-ray tomography measurements that silver forms clusters that are distributed irregularly, both on the surface and inside the ligaments building up the porous structure. Furthermore, we find that the role of the residual silver is ambiguous. Whereas CO oxidation is supported by more residual silver, methanol oxidation to methyl formate is hindered. Structural characterisation reveals larger ligaments and pores for decreasing residual silver concentration.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.844
Times cited: 42
DOI: 10.1016/j.jcat.2017.05.002
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“Gate induced monolayer behavior in twisted bilayer black phosphorus”. Sevik C, Wallbank JR, Gulseren O, Peeters FM, Çakir D, 2D materials 4, 035025 (2017). http://doi.org/10.1088/2053-1583/AA80C4
Abstract: Optical and electronic properties of black phosphorus strongly depend on the number of layers and type of stacking. Using first-principles calculations within the framework of density functional theory, we investigate the electronic properties of bilayer black phosphorus with an interlayer twist angle of 90 degrees. These calculations are complemented with a simple (k) over right arrow . (p) over right arrow model which is able to capture most of the low energy features and is valid for arbitrary twist angles. The electronic spectrum of 90 degrees twisted bilayer black phosphorus is found to be x-y isotropic in contrast to the monolayer. However x-y anisotropy, and a partial return to monolayer-like behavior, particularly in the valence band, can be induced by an external out-of-plane electric field. Moreover, the preferred hole effective mass can be rotated by 90 degrees simply by changing the direction of the applied electric field. In particular, a +0.4 (-0.4) V angstrom(1) out-of-plane electric field results in a similar to 60% increase in the hole effective mass along the y (x) axis and enhances the m(y)*/m(x)* (m(x)*/m(y)*) ratio as much as by a factor of 40. Our DFT and (k) over right arrow . (p) over right arrow simulations clearly indicate that the twist angle in combination with an appropriate gate voltage is a novel way to tune the electronic and optical properties of bilayer phosphorus and it gives us a new degree of freedom to engineer the properties of black phosphorus based devices.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 6.937
Times cited: 13
DOI: 10.1088/2053-1583/AA80C4
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“Thermal activated rotation of graphene flake on graphene”. Peymanirad F, Singh SK, Ghorbanfekr-Kalashami H, Novoselov KS, Peeters FM, Neek-Amal M, 2D materials 4, 025015 (2017). http://doi.org/10.1088/2053-1583/AA58A4
Abstract: The self rotation of a graphene flake over graphite is controlled by the size, initial misalignment and temperature. Using both ab initio calculations and molecular dynamics simulations, we investigate annealing effects on the self rotation of a graphene flake on a graphene substrate. The energy barriers for rotation and drift of a graphene flake over graphene is found to be smaller than 25 meV/atom which is comparable to thermal energy. We found that small flakes (of about similar to 4 nm) are more sensitive to temperature and initial misorientation angles than larger one (beyond 10 nm). The initial stacking configuration of the flake is found to be important for its dynamics and time evolution of misalignment. Large flakes, which are initially in the AA-or AB-stacking state with small misorientation angle, rotate and end up in the AB-stacking configuration. However small flakes can they stay in an incommensurate state specially when the initial misorientation angle is larger than 2 degrees. Our results are in agreement with recent experiments.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 6.937
Times cited: 16
DOI: 10.1088/2053-1583/AA58A4
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“The Quest for Value-Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study”. Snoeckx R, Ozkan A, Reniers F, Bogaerts A, Chemsuschem 10, 409 (2017). http://doi.org/10.1002/cssc.201601234
Abstract: Recycling of carbon dioxide by its conversion into value-added products has gained significant interest owing to the role it can play for use in an anthropogenic carbon cycle. The combined conversion with H2O could even mimic the natural photosynthesis process. An interesting gas conversion technique currently being considered in the field of CO2 conversion is plasma technology. To investigate whether it is also promising for this combined conversion, we performed a series of experiments and developed a chemical kinetics plasma chemistry model for a deeper understanding of the process. The main products formed were the syngas components CO and H2, as well as O2 and H2O2, whereas methanol formation was only observed in the parts-per-billion to parts-per-million range. The syngas ratio, on the other hand, could easily be controlled by varying both the water content and/or energy input. On the basis of the model, which was validated with experimental results, a chemical kinetics analysis was performed, which allowed the construction and investigation of the different pathways leading to the observed experimental results and which helped to clarify these results. This approach allowed us to evaluate this technology on the basis of its underlying chemistry and to propose solutions on how to further improve the formation of value-added products by using plasma technology.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 25
DOI: 10.1002/cssc.201601234
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“The Chemical Route to a Carbon Dioxide Neutral World”. Martens JA, Bogaerts A, De Kimpe N, Jacobs PA, Marin GB, Rabaey K, Saeys M, Verhelst S, Chemsuschem 10, 1039 (2017). http://doi.org/10.1002/cssc.201601051
Abstract: Excessive CO2 emissions in the atmosphere from anthropogenic activity can be divided into point sources and diffuse sources. The capture of CO2 from flue gases of large industrial installations and its conversion into fuels and chemicals with fast catalytic processes seems technically possible. Some emerging technologies are already being demonstrated on an industrial scale. Others are still being tested on a laboratory or pilot scale. These emerging chemical technologies can be implemented in a time window ranging from 5 to 20 years. The massive amounts of energy needed for capturing processes and the conversion of CO2 should come from low-carbon energy sources, such as tidal, geothermal, and nuclear energy, but also, mainly, from the sun. Synthetic methane gas that can be formed from CO2 and hydrogen gas is an attractive renewable energy carrier with an existing distribution system. Methanol offers advantages as a liquid fuel and is also a building block for the chemical industry. CO2 emissions from diffuse sources is a difficult problem to solve, particularly for CO2 emissions from road, water, and air transport, but steady progress in the development of technology for capturing CO2 from air is being made. It is impossible to ban carbon from the entire energy
supply of mankind with the current technological knowledge, but a transition to a mixed carbon–hydrogen economy can reduce net CO2 emissions and ultimately lead to a CO2-neutral world.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 75
DOI: 10.1002/cssc.201601051
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“Nitrogen Fixation by Gliding Arc Plasma: Better Insight by Chemical Kinetics Modelling”. Wang W, Patil B, Heijkers S, Hessel V, Bogaerts A, Chemsuschem 10, 2110 (2017). http://doi.org/10.1002/cssc.201700611
Abstract: The conversion of atmospheric nitrogen into valuable compounds, that is, so-called nitrogen fixation, is gaining increased interest, owing to the essential role in the nitrogen cycle of the biosphere. Plasma technology, and more specifically gliding arc plasma, has great potential in this area, but little is known about the underlying mechanisms. Therefore, we developed a detailed chemical kinetics model for a pulsed-power gliding-arc reactor operating at atmospheric pressure for nitrogen oxide synthesis. Experiments are performed to validate the model and reasonable agreement is reached between the calculated and measured NO and NO2 yields and the corresponding energy efficiency for NOx formation for different N2/O2 ratios, indicating that the model can provide a realistic picture of the plasma chemistry. Therefore, we can use the model to investigate the reaction pathways for the formation and loss of NOx. The results indicate that vibrational excitation of N2 in the gliding arc contributes significantly to activating the N2 molecules, and leads to an energy efficient way of NOx production, compared to the thermal process. Based on the underlying chemistry, the model allows us to propose solutions on how to further improve the NOx formation by gliding arc technology. Although the energy efficiency of the gliding-arc-based nitrogen fixation process at the present stage is not comparable to the world-scale Haber–Bosch process, we believe our study helps us to come up with more realistic scenarios of entering a cutting-edge innovation in new business cases for the decentralised production of fertilisers for agriculture, in which lowtemperature plasma technology might play an important role.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 7.226
DOI: 10.1002/cssc.201700611
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