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“Functionalization of MWCNTs with atomic nitrogen”. Ruelle B, Felten A, Ghijsen J, Drube W, Johnson RL, Liang D, Erni R, Van Tendeloo G, Sophie P, Dubois P, Godfroid T, Hecq M, Bittencourt C;, Micron 40, 85 (2009). http://doi.org/10.1016/j.micron.2008.01.003
Abstract: In this study of the changes induced by exposing MWCNTs to a nitrogen plasma, it was found by HRTEM that the atomic nitrogen exposure does not significantly etch the surface of the carbon nanotube (CNT). Nevertheless, the atomic nitrogen generated by a microwave plasma effectively grafts amine, nitrile, amide, and oxime groups onto the CNT surface, as observed by XPS, altering the density of valence electronic states, as seen in UPS. (C) 2008 Elsevier Ltd. All fights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.98
Times cited: 24
DOI: 10.1016/j.micron.2008.01.003
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“Ultrastructure and composition of cell wall appositions in the roots of Asplenium (Polypodiales)”. Leroux O, Leroux F, Bagniewska-Zadworna, Knox JP, Claeys M, Bals S, Viane RLL, Micron 42, 863 (2011). http://doi.org/10.1016/j.micron.2011.06.002
Abstract: Cell wall appositions (CWAs), formed by the deposition of extra wall material at the contact site with microbial organisms, are an integral part of the response of plants to microbial challenge. Detailed histological studies of CWAs in fern roots do not exist. Using light and electron microscopy we examined the (ultra)structure of CWAs in the outer layers of roots of Asplenium species. All cell walls studded with CWAs were impregnated with yellow-brown pigments. CWAs had different shapes, ranging from warts to elongated branched structures, as observed with scanning and transmission electron microscopy. Ultrastructural study further showed that infecting fungi grow intramurally and that they are immobilized by CWAs when attempting to penetrate intracellularly. Immunolabelling experiments using monoclonal antibodies indicated pectic homogalacturonan, xyloglucan, mannan and cellulose in the CWAs, but tests for lignins and callose were negative. We conclude that these appositions are defense-related structures made of a non-lignified polysaccharide matrix on which phenolic compounds are deposited in order to create a barrier protecting the root against infections.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.98
Times cited: 20
DOI: 10.1016/j.micron.2011.06.002
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“Imaging from atomic structure to electronic structure”. Xu Q, Zandbergen HW, van Dyck D, Micron 43, 524 (2012). http://doi.org/10.1016/j.micron.2011.10.024
Abstract: This paper discusses the possibility of retrieving the electron distribution (with highlighted valence electron distribution information) of materials from recorded HREM images. This process can be achieved by solving two inverse problems: reconstruction of the exit wave and reconstruction of the electron distribution from exit waves. The first inverse problem can be solved using a focal series reconstruction method. We show that the second inverse problem can be solved by combining a series of exit waves recorded at different thickness conditions. This process is designed based on an improved understanding of the dynamical scattering process. It also explains the fundamental difficulty of obtaining the valence electron distribution information and the basis of our solution.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 1.98
DOI: 10.1016/j.micron.2011.10.024
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“Model-based electron microscopy : from images toward precise numbers for unknown structure parameters”. Van Aert S, van den Broek W, Goos P, van Dyck D, Micron 43, 509 (2012). http://doi.org/10.1016/j.micron.2011.10.019
Abstract: Statistical parameter estimation theory is proposed as a method to quantify electron microscopy images. It aims at obtaining precise and accurate values for the unknown structure parameters including, for example, atomic column positions and types. In this theory, observations are purely considered as data planes, from which structure parameters have to be determined using a parametric model describing the images. The method enables us to measure positions of atomic columns with a precision of the order of a few picometers even though the resolution of the electron microscope is one or two orders of magnitude larger. Moreover, small differences in averaged atomic number, which cannot be distinguished visually, can be quantified using high-angle annular dark field scanning transmission electron microscopy images. Finally, it is shown how to optimize the experimental design so as to attain the highest precision. As an example, the optimization of the probe size for nanoparticle radius measurements is considered. It is also shown how to quantitatively balance signal-to-noise ratio and resolution by adjusting the probe size.
Keywords: A1 Journal article; Engineering Management (ENM); Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 1.98
Times cited: 7
DOI: 10.1016/j.micron.2011.10.019
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“The effect of probe inaccuracies on the quantitative model-based analysis of high angle annular dark field scanning transmission electron microscopy images”. Martinez GT, de Backer A, Rosenauer A, Verbeeck J, Van Aert S, Micron 63, 57 (2014). http://doi.org/10.1016/j.micron.2013.12.009
Abstract: Quantitative structural and chemical information can be obtained from high angle annular dark field scanning transmission electron microscopy (HAADF STEM) images when using statistical parameter estimation theory. In this approach, we assume an empirical parameterized imaging model for which the total scattered intensities of the atomic columns are estimated. These intensities can be related to the material structure or composition. Since the experimental probe profile is assumed to be known in the description of the imaging model, we will explore how the uncertainties in the probe profile affect the estimation of the total scattered intensities. Using multislice image simulations, we analyze this effect for Cs corrected and non-Cs corrected microscopes as a function of inaccuracies in cylindrically symmetric aberrations, such as defocus and spherical aberration of third and fifth order, and non-cylindrically symmetric aberrations, such as 2-fold and 3-fold astigmatism and coma.
Keywords: A1 Journal article; Engineering Management (ENM); Electron microscopy for materials research (EMAT)
Impact Factor: 1.98
Times cited: 25
DOI: 10.1016/j.micron.2013.12.009
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“Do you believe that atoms stay in place when you observe them in HREM?”.van Dyck D, Lobato I, Chen F-R, Kisielowski C, Micron 68, 158 (2015). http://doi.org/10.1016/j.micron.2014.09.003
Abstract: Recent advancements in aberration-corrected electron microscopy allow for an evaluation of unexpectedly large atom displacements beyond a resolution limit of similar to 0.5 angstrom, which are found to be dose-rate dependent in high resolution images. In this paper we outline a consistent description of the electron scattering process, which explains these unexpected phenomena. Our approach links thermal diffuse scattering to electron beam-induced object excitation and relaxation processes, which strongly contribute to the image formation process. The effect can provide an explanation for the well-known contrast mismatch (“Stobbs factor”) between image calculations and experiments. (C) 2014 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 1.98
Times cited: 11
DOI: 10.1016/j.micron.2014.09.003
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“Focused electron beam induced deposition as a tool to create electron vortices”. Béché, A, Winkler R, Plank H, Hofer F, Verbeeck J, Micron 80, 34 (2015). http://doi.org/10.1016/j.micron.2015.07.011
Abstract: Focused electron beam induced deposition (FEBID) is a microscopic technique that allows geometrically controlled material deposition with very high spatial resolution. This technique was used to create a spiral aperture capable of generating electron vortex beams in a transmission electron microscope (TEM). The vortex was then fully characterized using different TEM techniques, estimating the average orbital angular momentum to be approximately 0.8variant Planck's over 2pi per electron with almost 60% of the beam ending up in the l=1 state.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.98
Times cited: 21
DOI: 10.1016/j.micron.2015.07.011
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“One-step synthesis of a suspended ultrathin graphene oxide film: Application in transmission electron microscopy”. Kirilenko DA, Dideykin AT, Aleksenskiy AE, Sitnikova AA, Konnikov SG, Vul' AY, Micron 68, 23 (2015). http://doi.org/10.1016/j.micron.2014.08.006
Abstract: Ultrathin graphene films find their use as advantageous support for nano- and biomaterials investigations. Thin film causes a very slight deterioration to measured signals, thus providing more details of the object's structure at nanoscale. The ultimate thinness of graphene works in the best way for this purpose. However, obtaining suspended thin film of a large-area, which is convenient for applications, is often a relatively complicated and time-consuming task. Here we present a one-step 1-min technique for synthesis of an extremely thin (about 1-2 nm) continuous film suspended over cells of a conventional copper grid (50-400 mu m mesh). This technique enables us to acquire a large-area film which is water-resistant, stable in organic solvents and can act as a support when studying nanoparticles or biomaterials. Moreover, the very mechanism of the film formation can be interesting from the point of view of other applications of ultrathin graphene oxide papers. (C) 2014 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.98
Times cited: 13
DOI: 10.1016/j.micron.2014.08.006
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“Secondary ion formation of low molecular weight organic dyes in time-of-flight static secondary ion mass spectrometry”. Lenaerts J, van Vaeck L, Gijbels R, Rapid communications in mass spectrometry 17, 2115 (2003). http://doi.org/10.1002/rcm.1160
Abstract: Time-of-flight static secondary ion mass spectrometry (TOF-S-SIMS) was used to characterize thin layers of oxy- and thiocarbocyanine dyes on Ag and Si. Apart from adduct ions a variety of structural fragment ions were detected for which a fragmentation pattern is proposed. Peak assignments were confirmed by comparing spectra of dyes with very similar structures. All secondary ions were assigned with a mass accuracy better than 50 ppm. The intensity of molecular ions as well as fragment ions has been studied as a function of the type of organic dye, the substrate, the layer thickness and the type of primary ion. A large yield difference of two orders of magnitude was observed between the precursor ions of cationic carbocyanine dyes and the protonated molecules of the anionic dyes. Fragment ions, on the other hand, yielded similar intensities for both types of dye. As the dye layers deposited on an Ag substrate yielded higher secondary ion intensities than those deposited on a Si substrate, the Ag metal clearly acts as a promoting agent for secondary ion formation. The effect was more pronounced for precursor signals than for fragment ions. The promoting effect decreased as the deposited layer thickness of the organic dye layer was increased. Copyright (C) 2003 John Wiley Sons, Ltd.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.998
Times cited: 10
DOI: 10.1002/rcm.1160
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“Comparison of mono- and polyatomic primary ions for the characterization of organic dye overlayers with static secondary ion mass spectrometry”. Lenaerts J, van Vaeck L, Gijbels R, Van Luppen J, Rapid communications in mass spectrometry 18, 257 (2004). http://doi.org/10.1002/rcm.1320
Abstract: Organic carbocyanine dye coatings have been analyzed by time-of-flight static secondary ion mass spectrometry (TOF-S-SIMS) using three types of primary ions: Ga+ operating at 25 keV, and Xe+ and SF5+ both operating at 9 keV. Secondary ion yields obtained with these three primary ions have been compared for coatings with different layer thickness, varying from (sub)-monolayer to multilayers, on different substrates (Si, Ag and AgBr cubic microcrystals). For (sub)-monolayers deposited on Ag, Xe+ and SF5+ primary ions generate similar precursor ion intensities, but with Ga+ slightly lower precursor ion intensities were obtained. Thick coatings on Ag as well as mono- and multilayers on Si produce the highest precursor and fragment ion intensities with the polyatomic primary ion. The yield difference between SF5+ and Xe+ can reach a factor of 6. In comparison with Ga+, yield enhancements by up to a factor of 180 are observed with SF5+. For the mass spectrometric analysis of dye layers on AgBr microcrystals, SF5+ again proves to be the primary ion of choice. Copyright (C) 2004 John Wiley Sons, Ltd.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.998
Times cited: 5
DOI: 10.1002/rcm.1320
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“Matrix-enhanced secondary ion mass spectrometry: the influence of MALDI matrices on molecular ion yields of thin organic films”. Adriaensen L, Vangaever F, Lenaerts J, Gijbels R, Rapid communications in mass spectrometry 19, 1017 (2005). http://doi.org/10.1002/rcm.1881
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 1.998
Times cited: 24
DOI: 10.1002/rcm.1881
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“Large-volume injection combined with gas chromatography/isotope ratio mass spectrometry for the analysis of polycyclic aromatic hydrocarbons”. Buczyńska AJ, Geypens B, Van Grieken R, De Wael K, Rapid communications in mass spectrometry 28, 1 (2014). http://doi.org/10.1002/RCM.6769
Abstract: RATIONALE: Compound-specific stable isotope analyses of carbon require relatively large amounts of sample for reliable analyses. Commonly applied injections of 1 μL may thus be inefficient for samples with low concentrations of pollutants (e.g. air particulate matter) or when the amount of a sample is limited. METHODS: A Large-Volume Injection (LVI) method for carbon stable isotope ratio analysis of Polycyclic Aromatic Hydrocarbons (PAHs) was optimized in this study. Gas chromatography/combustion/isotope ratio mass spectrometry (GCCIRMS) and ion trap mass spectrometry (ITMS) were used for the determination of stable carbon isotope ratios and quantification of compounds, respectively. RESULTS: The optimized method resulted in very good reproducibility, even for the most volatile PAH, naphthalene, when a small amount of higher boiling co-solvent was used. No significant fractionation of isotope ratios could be seen and the recoveries of analytes were similar to or better than that of a splitless cold injection. CONCLUSIONS: Injection of 100 μL, instead of the commonly used 1 μL, increases the detection limit for PAHs significantly and/or simplifies the sample preparation step. Using our optimized method, stable carbon isotope ratios can be reliably measured in samples with concentrations of PAHs down to 0.050.1 ng μL1.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.998
Times cited: 5
DOI: 10.1002/RCM.6769
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“A XANES study of chromophores : the case of black glass”. Ceglia A, Nuyts G, Cagno S, Meulebroeck W, Baert K, Cosyns P, Nys K, Thienpont H, Janssens K, Terryn H, Analytical methods 6, 2662 (2014). http://doi.org/10.1039/C3AY42029A
Abstract: We studied the Fe K-edge X-ray absorption near edge (XANES) spectra of several Roman black glass fragments in order to determine the Fe3+/ΣFe ratio of these materials. The selected archaeological glass samples cover the period 1st5th century AD in nine different sites of the North Western provinces of the Roman Empire. The fragments belong to two different compositional groups demonstrating a diachronic evolution: early Roman HMG (High Magnesia Glass) and Roman Imperial LMG (Low Magnesia Glass). The first group contains natural Fe levels (below 2 wt% as Fe2O3), while the LMG has concentrations above 5 wt%. This difference is also reflected by Fe3+/ΣFe values. Low iron glass was produced under strongly reducing conditions in order to obtain the black colour, with average Fe3+/ΣFe values ≈ 0.17. LMG glass is somewhat more oxidised (Fe3+/ΣFe ≈ 0.40.5). While HMG glass required active control of the furnace environment, LMG was made under ambient atmosphere and its higher oxidation degree is mainly determined by the chemistry of the raw glass.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.9
Times cited: 14
DOI: 10.1039/C3AY42029A
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“Spin polarization in monolayer MoS₂, in the presence of proximity-induced interactions”. Zhao XN, Xu W, Xiao YM, Van Duppen B, International Journal Of Modern Physics C 31, 2050143 (2020). http://doi.org/10.1142/S0129183120501430
Abstract: When monolayer (ML) MoS2 is placed on a substrate, the proximity-induced interactions such as the Rashba spin-orbit coupling (RSOC) and exchange interaction (EI) can be introduced. Thus, the electronic system can behave like a spintronic device. In this study, we present a theoretical study on how the presence of the RSCO and EI can lead to the band splitting, the lifting of the valley degeneracy and to the spin polarization in n- and p-type ML MoS2. We find that the maxima of the in-plane spin orientation in the conduction and valence bands in ML MoS2 depend on the Rashba parameter and the effective Zeeman field factor. At a fixed Rashba parameter, the minima of the split conduction band and the maxima of the split valence band along with the spin polarization in ML MoS2 can be tuned effectively by varying the effective Zeeman field factor. On the basis that the EI can be induced by placing the ML MoS2 on a ferromagnetic substrate or by magnetic doping in ML MoS2, we predict that the interesting spintronic effects can be observed in n- and p-type ML MoS2. This work can be helpful to gain an in-depth understanding of the basic physical properties of ML MoS2 for application in advanced electronic and optoelectronic devices.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 1.9
DOI: 10.1142/S0129183120501430
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“Metal-based nanoparticles : an alternative treatment for biofilm infection in hard-to-heal wounds”. Iungin O, Shydlovska O, Moshynets O, Vasylenko V, Sidorenko M, Mickevicius S, Potters G, Journal of wound care 33, 99 (2024). http://doi.org/10.12968/JOWC.2024.33.SUP4A.XCIX
Abstract: Metal-based nanoparticles (MNPs) are promoted as effective compounds in the treatment of bacterial infections and as possible alternatives to antibiotics. These MNPs are known to affect a broad spectrum of microorganisms using a multitude of strategies, including the induction of reactive oxygen species and interaction with the inner structures of the bacterial cells. The aim of this review was to summarise the latest studies about the effect of metal-based nanoparticles on pathogenic bacterial biofilm formed in wounds, using the examples of Gram-positive bacterium Staphylococcus aureus and Gram-negative bacterium Pseudomonas aeruginosa, as well as provide an overview of possible clinical applications. Declaration of interest: The authors have no conflicts of interest.
Keywords: A1 Journal article; Antwerp engineering, PhotoElectroChemistry & Sensing (A-PECS)
Impact Factor: 1.9
DOI: 10.12968/JOWC.2024.33.SUP4A.XCIX
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“Rational design of an XNA ligase through docking of unbound nucleic acids to toroidal proteins”. Vanmeert M, Razzokov J, Mirza MU, Weeks SD, Schepers G, Bogaerts A, Rozenski J, Froeyen M, Herdewijn P, Pinheiro VB, Lescrinier E, Nucleic acids research 47, 7130 (2019). http://doi.org/10.1093/nar/gkz551
Abstract: Xenobiotic nucleic acids (XNA) are nucleic acid analogues not present in nature that can be used for the storage of genetic information. In vivo XNA applications could be developed into novel biocontainment strategies, but are currently limited by the challenge of developing XNA processing enzymes such as polymerases, ligases and nucleases. Here, we present a structure-guided modelling-based strategy for the rational design of those enzymes essential for the development of XNA molecular biology. Docking of protein domains to unbound double-stranded nucleic acids is used to generate a first approximation of the extensive interaction of nucleic acid processing enzymes with their substrate. Molecular dynamics is used to optimise that prediction allowing, for the first time, the accurate prediction of how proteins that form toroidal complexes with nucleic acids interact with their substrate. Using the Chlorella virus DNA ligase as a proof of principle, we recapitulate the ligase's substrate specificity and successfully predict how to convert it into an XNA-templated XNA ligase.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 10.162
Times cited: 1
DOI: 10.1093/nar/gkz551
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“Morphotropic phase boundary in pure perovskite lead titanate at room temperature”. Zhang Z, Chen X, Shi X, Hu Y, Huang J, Liu S, Ren Z, Huang H, Han G, Van Tendeloo G, Tian H, Materials Today Nano 20, 100275 (2022). http://doi.org/10.1016/J.MTNANO.2022.100275
Abstract: For many decades, great efforts have been devoted to pursue a large piezoelectric response by an intelligent design of morphotropic phase boundaries (MPB) in solid solutions, where tetragonal (T) and rhombohedral (R) structures coexist. For example, classical PbZrxTi1-xO3 and Pb(Mg1/3Nb2/3)O-3-PbTiO3 single crystals demonstrate a giant piezoelectric response near MPB. However, as the end member of these solids, perovskite-structured PbTiO3 always adopts the T phase at room temperature. Here, we report a pathway to create room temperature MPB in a single-phase PbTiO3. The uniaxial stress along the c-axis drives a T-R phase transition bridged by a monoclinic (M) phase, which facilitates a polarization rotation in the monodomain PbTiO3. Meanwhile, we demonstrate that the coexistence of T and R phases at room temperature can be achieved via an extremely mismatched heterointerface system. The uniaxial pressure is proved as an efficient way to break the inherent symmetry and able to substantially tailor the phase transition temperature Tc. These findings provide new insights into MPB, offering the opportunity to explore the giant piezoelectric response in single-phase materials. (c) 2022 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 10.3
DOI: 10.1016/J.MTNANO.2022.100275
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“Sustainability analysis of methane-to-hydrogen-to-ammonia conversion by integration of high-temperature plasma and non-thermal plasma processes”. Osorio-Tejada J, van't Veer K, Long NVD, Tran NN, Fulcheri L, Patil BS, Bogaerts A, Hessel V, Energy Conversion And Management 269, 116095 (2022). http://doi.org/10.1016/j.enconman.2022.116095
Abstract: The Covid era has made us aware of the need for resilient, self-sufficient, and local production. We are likely willing to pay an extra price for that quality. Ammonia (NH3) synthesis accounts for 2 % of global energy production and is an important point of attention for the development of green energy technologies. Therefore, we propose a thermally integrated process for H2 production and NH3 synthesis using plasma technology, and we evaluate its techno-economic performance and CO2 footprint by life cycle assessment (LCA). The key is to integrate energy-wise a high-temperature plasma (HTP) process, with a (low-temperature) non-thermal plasma (NTP) process and to envision their joint economic potential. This particularly means raising the temperature of the NTP process, which is typically below 100 ◦ C, taking advantage of the heat released from the HTP process. For that purpose, we proposed the integrated process and conducted chemical kinetics simulations in the NTP section to determine the thermodynamically feasible operating window of this novel combined plasma process. The results suggest that an NH3 yield of 2.2 mol% can be attained at 302 ◦ C at an energy yield of 1.1 g NH3/kWh. Cost calculations show that the economic performance is far from commercial, mainly because of the too low energy yield of the NTP process. However, when we base our costs on the best literature value and plausible future scenarios for the NTP energy yield, we reach a cost prediction below 452 $/tonne NH3, which is competitive with conventional small-scale Haber-Bosch NH3 synthesis for distributed production. In addition, we demonstrate that biogas can be used as feed, thus allowing the proposed integrated reactor concept to be part of a biogas-to-ammonia circular concept. Moreover, by LCA we demonstrate the environmental benefits of the proposed plant, which could cut by half the carbon emissions when supplied by photovoltaic electricity, and even invert the carbon balance when supplied by wind power due to the avoided emissions of the carbon black credits.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 10.4
DOI: 10.1016/j.enconman.2022.116095
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“Feasibility study of a small-scale fertilizer production facility based on plasma nitrogen fixation”. Manaigo F, Rouwenhorst K, Bogaerts A, Snyders R, Energy Conversion and Management 302, 118124 (2024). http://doi.org/10.1016/j.enconman.2024.118124
Keywords: A1 Journal Article; Plasma-based nitrogen fixation Haber-Bosch Feasibility study Fertilizer production; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 10.4
DOI: 10.1016/j.enconman.2024.118124
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“A Pareto aggregation approach for environmental-economic multi-objective optimization applied on a second-generation bioethanol production model”. Vasilakou K, Billen P, Van Passel S, Nimmegeers P, Energy conversion and management 303, 118184 (2024). http://doi.org/10.1016/J.ENCONMAN.2024.118184
Abstract: Multi-objective optimization is an important decision-making tool for energy processes, as multiple targets need to be achieved. These objectives are usually conflicting since a single solution cannot be optimal for all objectives, resulting in a set of Pareto-optimal solutions. Multiple indicators might be available to describe a sustainability objective, such as the environmental impact which is commonly evaluated by performing a life cycle assessment. In this study, Pareto aggregation is proposed as a method which employs a novel multi-objective optimization-based approach as an alternative to the classically used aggregation in life cycle assessment. This method identifies conflicting environmental indicators and performs an aggregation among those that require a trade-off. An environmental-economic optimization of a second-generation bioethanol plant is used to illustrate and evaluate the proposed method. Process parameters from a biochemical conversion pathway flowsheet simulation model are chosen as optimization variables. To reduce the computational time, surrogate models, based on artificial neural networks, are used. Out of the eighteen ReCiPe Midpoint environmental indicators, five were identified as conflicting, resulting in an aggregated environmental objective, which was then traded off with the economic objective function, chosen as the levelized cost of ethanol. Comparison with the widely used single-score EcoIndicator99 showed that the Pareto aggregation method can reduce most of the environmental indicators by up to 6.5%. This research provides an insight on non-redundant objective functions, aiming at reducing the dimensionality of multi-objective optimization problems, while taking into consideration decision-makers’ preferences.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS)
Impact Factor: 10.4
DOI: 10.1016/J.ENCONMAN.2024.118184
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“The acute effect of budesonide/formoterol in COPD : a multi-slice computed tomography and lung function study”. De Backer LA, Vos W, de Backer J, Van Holsbeke C, Vinchurkar S, de Backer W, European Respiratory Journal 40, 298 (2012). http://doi.org/10.1183/09031936.00072511
Abstract: The Global Initiative for Chronic Obstructive Lung Disease (GOLD) classification of chronic obstructive pulmonary disease (COPD) does not always match with other clinical disease descriptors such as exacerbation frequency and quality of life, indicating that forced expiratory volume in 1 s (FEV1) is not a perfect descriptor of the disease. The aim of this study was to find out whether changes in airway geometry after inhalation of the most commonly used inhalation therapy in severe COPD can more adequately be described with an image-based approach than with spirometry. 10 COPD GOLD stage III patients were assessed in a double-blind crossover study. Airway volumes were analysed using segmentation of multi-slice computed tomography (MSCT) images; airway resistance was determined using computational fluid dynamics (CFD). Distal airway volume significantly increased (p=0.011) in patients 4 h after receiving a budesonide/formoterol combination from 9.6+/-4.67 cm(3) to 10.14+/-4.81 cm(3). Also CFD-determined airway resistance significantly decreased (p=0.047) from 0.051+/-0.021 kPa.s.L-1 to 0.043+/- 0.019 kPa.s.L-1. None of the lung function parameters showed a significant change. Only functional residual capacity (FRC) showed a trend to decline (p=0.056). Only the image-based parameters were able to predict the visit at which the combination product was administered. This study showed that imaging is a sensitive, complementary tool to describe changes in airway structure.
Keywords: A1 Journal article; Biophysics and Biomedical Physics; Condensed Matter Theory (CMT); Laboratory Experimental Medicine and Pediatrics (LEMP)
Impact Factor: 10.569
Times cited: 37
DOI: 10.1183/09031936.00072511
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de Backer W, Vos W, Van Holsbeke C, Vinchurkar S, Claes R, Hufkens A, Parizel PM, Bedert L, de Backer J (2014) The effect of roflumilast in addition to LABA/LAMA/ICS treatment in COPD patients. Copenhagen, 527–529
Keywords: L1 Letter to the editor; Biophysics and Biomedical Physics; Condensed Matter Theory (CMT); Antwerp Surgical Training, Anatomy and Research Centre (ASTARC); Laboratory Experimental Medicine and Pediatrics (LEMP)
Impact Factor: 10.569
Times cited: 26
DOI: 10.1183/09031936.00011714
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“Electrochemical behavior of electrodeposited nanoporous Pt catalysts for the oxygen reduction reaction”. Geboes B, Ustarroz J, Sentosun K, Vanrompay H, Hubin A, Bals S, Breugelmans T, ACS catalysis 6, 5856 (2016). http://doi.org/10.1021/acscatal.6b00668
Abstract: Nanoporous Pt based nanoparticles (NP's) are promising fuel cell catalysts due to their high surface area and increased electrocatalytic activity toward the ORR In this work a direct double-pulse electrodeposition procedure at room temperature is applied to obtain dendritic Pt structures (89 nm diameter) with a high level of porosity (ca. 25%) and nanopores of 2 nm protruding until the center of the NP's. The particle morphology is characterized using aberration corrected high angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and electron tomography (ET) combined with field emission scanning electron microscopy (FESEM) and macroscopic electrochemical measurements to assess their activity and stability toward the ORR. Macroscopic determination of the active surface area through hydrogen UPD measurements in combination with FESEM and ET showed that a considerable amount of the active sites inside the pores of the low overpotential NP's were accessible to oxygen species. As a result of this accessibility, up to a 9-fold enhancement of the Pt mass corrected ORR activity at 0.85 V vs RHE was observed at the highly porous structures. After successive potential cycling upward to 1.5 V vs RHE in a deaerated HClO4 solution a negative shift of 71 mV in half-wave potential occurred. This decrease in ORR activity could be correlated to the partial collapse of the nanopores, visible in both the EASA values and 3D ET reconstructions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 10.614
Times cited: 48
DOI: 10.1021/acscatal.6b00668
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“PdPb-catalyzed decarboxylation of proline to pyrrolidine : highly selective formation of a biobased amine in water”. Verduyckt J, Van Hoof M, De Schouwer F, Wolberg M, Kurttepeli M, Eloy P, Gaigneaux EM, Bals S, Kirschhock CEA, De Vos DE, ACS catalysis 6, 7303 (2016). http://doi.org/10.1021/ACSCATAL.6B02561
Abstract: Amino acids have huge potential as platform chemicals in the biobased industry. Pd-catalyzed decarboxylation is a very promising route for the valorization of these natural compounds derived from protein waste or fermentation. We report that the highly abundant and nonessential amino acid L-proline is very reactive in the Pd-catalyzed decarboxylation. Full conversions are obtained with Pd/C and different Pd/MeOx catalysts; this allowed the identification of the different side reactions and the mapping of the reaction network. Due to the high reactivity of pyrrolidine, the selectivity for pyrrolidine was initially low. By carefully modifying Pd/ZrO2 with Pb in a controlled manner-via two incipient wetness impregnation steps-the selectivity increased remarkably. Finally, a thorough investigation of the reaction parameters resulted in an increased activity of this modified catalyst and an even further enhanced selectivity under a low H-2 pressure of 4 bar at 235 degrees C in water. This results in a very selective and sustainable production route for the highly interesting pyrrolidine.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 10.614
Times cited: 27
DOI: 10.1021/ACSCATAL.6B02561
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“Catalyst preparation with plasmas : how does it work?”.Wang Z, Zhang Y, Neyts EC, Cao X, Zhang X, Jang BW-L, Liu C-jun, ACS catalysis 8, 2093 (2018). http://doi.org/10.1021/ACSCATAL.7B03723
Abstract: Catalyst preparation with plasmas is increasingly attracting interest. A plasma is a partially ionized gas, consisting of electrons, ions, molecules, radicals, photons, and excited species, which are all active species for catalyst preparation and treatment. Under the influence of plasma, nucleation and crystal growth in catalyst preparation can be very different from those in the conventional thermal approach. Some thermodynamically unfavorable reactions can easily take place with plasmas. Compounds such as sulfides, nitrides, and phosphides that are produced under harsh conditions can be synthesized by plasma under mild conditions. Plasmas can produce catalysts with smaller particle sizes and controllable structure. Plasma is also a facile tool for reduction, oxidation, doping, etching, coating, alloy formation, surface treatment, and surface cleaning in a simple and direct way. A rapid and convenient plasma template removal has thus been established for zeolite synthesis. It can operate at room temperature and allows the catalyst preparation on temperature-sensitive supporting materials. Plasma is typically effective for the production of various catalysts on metallic substrates. In addition, plasma-prepared transition-metal catalysts show enhanced low-temperature activity with improved stability. This provides a useful model catalyst for further improvement of industrial catalysts. In this review, we aim to summarize the recent advances in catalyst preparation with plasmas. The present understanding of plasma-based catalyst preparation is discussed. The challenges and future development are addressed.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 10.614
Times cited: 81
DOI: 10.1021/ACSCATAL.7B03723
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“Fe-containing magnesium aluminate support for stability and carbon control during methane reforming”. Theofanidis SA, Galvita VV, Poelman H, Dharanipragada NVRA, Longo A, Meledina M, Van Tendeloo G, Detavernier C, Marin GB, ACS catalysis 8, 5983 (2018). http://doi.org/10.1021/ACSCATAL.8B01039
Abstract: We report a MgFexAl2-xO4 synthetic spinel, where x varies from 0 to 0.26, as support for Ni-based catalysts, offering stability and carbon control under various conditions of methane reforming. By incorporation of Fe into a magnesium aluminate spine!, a support is created with redox functionality and high thermal stability, as concluded from temporal analysis of products (TAP) experiments and redox cycling, respectively. A diffusion coefficient of 3 x 10(-17) m(2) s(-1) was estimated for lattice oxygen at 993 K from TAP experiments. X-ray diffraction (XRD) and extended X-ray absorption fine structure (EXAFS) modeling identified that the incorporation of iron occurs as Fe3+ in the octahedral sites of the spinel lattice, replacing aluminum. Simulation of the X-ray absorption near edge structure (XANES) spectrum of the reduced support showed that 60 +/- 10% of iron was reduced from 3+ to 2+ at 1073 K, while there was no formation of metallic iron. A series of Ni/MgFexAl2-xO4 catalysts, where x varies from 0 to 0.26, was synthesized and reduced, yielding a supported Ni-Fe alloy. The evolution of the catalyst structure during H-2 temperature-programmed reduction (TPR) and CO2 temperature-programmed oxidation (TPO) was examined using time-resolved in situ XRD and XANES. During reforming, iron in both the support and alloy keeps control of carbon accumulation, as confirmed by O-2-TPO on the spent catalysts. By fine tuning the amount of Fe in MgFexAl2-xO4, a supported alloy was obtained with a Ni/Fe molar ratio of similar to 10, which was active for reforming and stable. By comparison of the performance of Ni-based catalysts with Fe either incorporated into or deposited onto the support, the location of Fe within the support proved crucial for the stability and carbon mitigation under reforming conditions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 10.614
Times cited: 18
DOI: 10.1021/ACSCATAL.8B01039
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“Pr/ZrO2 prepared by atomic trapping : an efficient catalyst for the conversion of glycerol to lactic acid with concomitant transfer hydrogenation of cyclohexene”. Tang Z, Liu P, Cao H, Bals S, Heeres HJ, Pescarmona PP, ACS catalysis 9, 9953 (2019). http://doi.org/10.1021/ACSCATAL.9B02139
Abstract: A series of heterogeneous catalysts consisting of highly dispersed Pt nanoparticles supported on nanosized ZrO2 (20 to 60 nm) was synthesized and investigated for the one-pot transfer hydrogenation between glycerol and cyclohexene to produce lactic acid and cyclohexane, without any additional H-2. Different preparation methods were screened, by varying the calcination and reduction procedures with the purpose of optimizing the dispersion of Pt species (i.e., as single-atom sites or extra-fine Pt nanoparticles) on the ZrO2 support. The Pt/ZrO2 catalysts were characterized by means of transmission electron microscopy techniques (HAADF-STEM, TEM), elemental analysis (ICP-OES, EDX mapping), N-2-physisorption, H-2 temperature-programmed-reduction (H-2-TPR), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). Based on this combination of techniques it was possible to correlate the temperature of the calcination and reduction treatments with the nature of the Pt species. The best catalyst consisted of subnanometer Pt clusters (<1 nm) and atomically dispersed Pt (as Pt2+ and Pt4+) on the ZrO2 support, which were converted into extra-fine Pt nanoparticles (average size = 1.4 nm) upon reduction. These nanoparticles acted as catalytic species for the transfer hydrogenation of glycerol with cyclohexene, which gave an unsurpassed 95% yield of lactic acid salt at 96% glycerol conversion (aqueous glycerol solution, NaOH as promoter, 160 degrees C, 4.5 h, at 20 bar N-2). This is the highest yield and selectivity of lactic acid (salt) reported in the literature so far. Reusability experiments showed a partial and gradual loss of activity of the Pt/ZrO2 catalyst, which was attributed to the experimentally observed aggregation of Pt nanoparticles.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 10.614
Times cited: 46
DOI: 10.1021/ACSCATAL.9B02139
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“Plasma-Catalytic Ammonia Reforming of Methane over Cu-Based Catalysts for the Production of HCN and H2at Reduced Temperature”. Yi Y, Wang X, Jafarzadeh A, Wang L, Liu P, He B, Yan J, Zhang R, Zhang H, Liu X, Guo H, Neyts EC, Bogaerts A, Acs Catalysis 11, 1765 (2021). http://doi.org/10.1021/acscatal.0c04940
Abstract: Industrial production of HCN from NH3 and CH4 not only uses precious Pt or Pt−Rh catalysts but also requires extremely high temperatures (∼1600 K). From an energetic, operational, and safety perspective, a drastic decrease in temperature is highly desirable. Here, we report ammonia reforming of methane for the production of HCN and H2 at 673 K by the combination of CH4/NH3 plasma and a supported Cu/silicalite-1 catalyst. 30% CH4 conversion has been achieved with 79% HCN selectivity. Catalyst characterization and plasma diagnostics reveal that the excellent reaction performance is attributed to metallic Cu active sites. In addition, we propose a possible reaction pathway, viz. E-R reactions with N, NH, NH2, and CH radicals produced in the plasma, for the production of HCN, based on density functional theory calculations. Importantly, the Cu/silicalite-1 catalyst costs less than 5% of the commercial Pt mesh catalyst.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 10.614
DOI: 10.1021/acscatal.0c04940
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“Gold and silver-catalyzed reductive amination of aromatic carboxylic acids to benzylic amines”. Coeck R, Meeprasert J, Li G, Altantzis T, Bals S, Pidko EA, De Vos DE, Acs Catalysis 11, 7672 (2021). http://doi.org/10.1021/ACSCATAL.1C01693
Abstract: The reductive amination of benzoic acid and its derivatives would be an effective addition to current synthesis methods for benzylamine. However, with current technology it is very difficult to keep the aromaticity intact when starting from benzoic acid, and salt wastes are often generated in the process. Here, we report a heterogeneous catalytic system for such a reductive amination, requiring solely H-2 and NH3 as the reactants. The Ag/TiO2 or Au/TiO2 catalysts can be used multiple times, and very little noble metal is required, only 0.025 mol % Au. The catalysts are bifunctional: the support catalyzes the dehydration of both the ammonium carboxylate to the amide and of the amide to the nitrile, while the sites at the metal-support interface promote the hydrogenation of the in situ generated nitrile. Yields of up to 92% benzylamine were obtained.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 10.614
Times cited: 16
DOI: 10.1021/ACSCATAL.1C01693
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“Atomic-level understanding for the enhanced generation of hydrogen peroxide by the introduction of an aryl amino group in polymeric carbon nitrides”. Zhang T, Schilling W, Khan SU, Ching HYV, Lu C, Chen J, Jaworski A, Barcaro G, Monti S, De Wael K, Slabon A, Das S, Acs Catalysis 11, 14087 (2021). http://doi.org/10.1021/ACSCATAL.1C03733
Abstract: Heterogeneous catalysts are often & ldquo;black boxes & rdquo; due to the insufficient understanding of the detailed mechanisms at the catalytic sites. An atomic-level elucidation of the processes taking place in those regions is, thus, mandatory to produce robust and selective heterogeneous catalysts. We have improved the description of the whole reactive scenario for polymeric carbon nitrides (PCN) by combining atomic-level characterizations with magic-angle spinning (MAS) solid-state nuclear magnetic resonance (NMR) spectroscopy, classical reactive molecular dynamics (RMD) simulations, and quantum chemistry (QC) calculations. We disclose the structure & minus;property relationships of an ad hoc modified PCN by inserting an aryl amino group that turned out to be very efficient for the production of H2O2. The main advancement of this work is the development of a difluoromethylene-substituted aryl amino PCN to generate H2O2 at a rate of 2.0 mM & middot;h & minus;1 under the irradiation of household blue LEDs and the identification of possible active catalytic sites with the aid of 15N and 19F MAS solid-state NMR without using any expensive labeling reagent. RMD simulations and QC calculations confirm and further extend the experimental descriptions by revealing the role and locations of the identified functionalities, namely, NH linkers, & minus;NH2 terminal groups, and difluoromethylene units, reactants, and products. <comment>Superscript/Subscript Available</comment
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Organic synthesis (ORSY); Applied Electrochemistry & Catalysis (ELCAT); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 10.614
DOI: 10.1021/ACSCATAL.1C03733
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