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“X-ray spectrometry”. Markowicz AA, Van Grieken RE, Analytical chemistry 58, 279r (1986). http://doi.org/10.1021/AC00296A019
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
DOI: 10.1021/AC00296A019
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“X-ray spectrometry”. Markowicz AA, Van Grieken RE, Reviews in analytical chemistry 56, 241r (1984)
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
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“Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets”. Kavak S, Kadu AA, Claes N, Sánchez-Iglesias A, Liz-Marzán LM, Batenburg KJ, Bals S, The journal of physical chemistry: C : nanomaterials and interfaces 127, 9725 (2023). http://doi.org/10.1021/acs.jpcc.3c02017
Abstract: Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.7
Times cited: 2
DOI: 10.1021/acs.jpcc.3c02017
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“Is a catalyst always beneficial in plasma catalysis? Insights from the many physical and chemical interactions”. Loenders B, Michiels R, Bogaerts A, Journal of Energy Chemistry 85, 501 (2023). http://doi.org/10.1016/j.jechem.2023.06.016
Abstract: Plasma-catalytic dry reforming of CH4 (DRM) is promising to convert the greenhouse gasses CH4 and CO2 into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products, because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex, as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, highlighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems. Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures, at which vibrational excitation can enhance the surface reactions.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 13.1
DOI: 10.1016/j.jechem.2023.06.016
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“Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods”. Sa J, Hu N, Heyvaert W, Van Gordon K, Li H, Wang L, Bals S, Liz-Marzán LM, Ni W, Chemistry of materials (2023). http://doi.org/10.1021/acs.chemmater.3c01044
Abstract: Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.6
DOI: 10.1021/acs.chemmater.3c01044
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“Atomic level mechanisms of graphene healing by methane-based plasma radicals”. Khalilov U, Yusupov M, Eshonqulov Gb, Neyts Ec, Berdiyorov Gr, FlatChem 39, 100506 (2023). http://doi.org/10.1016/j.flatc.2023.100506
Keywords: A1 Journal article; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 6.2
DOI: 10.1016/j.flatc.2023.100506
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“Plasma-based CO2 conversion: How to correctly analyze the performance?”.Wanten B, Vertongen R, De Meyer R, Bogaerts A, Journal of Energy Chemistry 86, 180 (2023). http://doi.org/10.1016/j.jechem.2023.07.005
Keywords: A1 journal article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 13.1
DOI: 10.1016/j.jechem.2023.07.005
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“High thermoelectric figure of merit in p-type Mg₃Si₂Te₆: role of multi-valley bands and high anharmonicity”. Pandey T, Peeters FM, Milošević, MV, Journal of materials chemistry C : materials for optical and electronic devices 11, 11185 (2023). http://doi.org/10.1039/D3TC02169F
Abstract: Silicon-based materials are attractive for thermoelectric applications due to their thermal stability, chemical inertness, and natural abundance of silicon. Here, using a combination of first-principles and Boltzmann transport calculations we report the thermoelectric properties of the recently synthesized compound Mg3Si2Te6. Our analysis reveals that Mg3Si2Te6 is a direct bandgap semiconductor with a bandgap of 1.6 eV. The combination of heavy and light valence bands, along with a high valley degeneracy, results in a large power factor under p-type doping. We also find that Mg is weakly bonded both within and between the layers, leading to low phonon group velocities. The vibrations of the Mg atoms are localized and make a significant contribution to phonon-phonon scattering. This high anharmonicity, coupled with low phonon group velocity, results in a low lattice thermal conductivity of & kappa;(l) = 0.5 W m(-1) K-1 at room temperature, along the cross-plane direction. Combining excellent electronic transport properties and low & kappa;(l), p-type Mg3Si2Te6 achieves figure-of-merit (zT) values greater than 1 at temperatures above 600 K. Specifically, a zT of 2.0 is found at 900 K along the cross-plane direction. Our findings highlight the importance of structural complexity and chemical bonding in electronic and phonon transport, providing guiding insights for further design of Si-based thermoelectrics.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 6.4
Times cited: 1
DOI: 10.1039/D3TC02169F
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“3D-printed microneedle-based potentiometric sensor for pH monitoring in skin interstitial fluid”. Parrilla M, Vanhooydonck A, Johns M, Watts R, De Wael K, Sensors and actuators : B : chemical 378, 133159 (2023). http://doi.org/10.1016/J.SNB.2022.133159
Abstract: Wearable electrochemical sensors are driven by the user-friendly capability of continuous monitoring of key biomarkers for diagnostic or therapeutic operations. Particularly, microneedle (MN)-based sensors can access the interstitial fluid (ISF) in the dermis layer of skin to carry out on-body transdermal detection of analytes. Interestingly, 3D-printing technology allows for rapid and versatile prototyping reaching micrometer resolution. Herein, for the first time, we explore 3D-printed hollow MN patches (1 mm height x 1 mm base with 0.3 mm hole) which are modified with conductive inks to develop a potentiometric sensor for pH monitoring. First, the piercing capability of 3D-printed MN patches is demonstrated by using the parafilm model and their insertion in porcine skin. Subsequently, the hollow MNs are filled with conductive inks to engineer a set of microelectrodes. Thereafter, the working and reference electrodes are properly modified with polyaniline and polyvinyl butyral, respectively, toward a highly stable potentiometric cell. A full in vitro characterization is performed within a broad range of pH (i.e. pH 4 to pH 9). Besides, the MN sensor is analytically assessed in phantom gel and pierced on porcine skin to evaluate the resilience of the MN sensor. Finally, the MN sensor is pierced on the forearm of a subject and tested for its on-body monitoring capability. Overall, 3D-printed MN-based potentiometric sensing brings a versatile and affordable technology to minimally-invasively monitor key physiological parameters in the body.
Keywords: A1 Journal article; Engineering sciences. Technology; Internet Data Lab (IDLab); Product development; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
DOI: 10.1016/J.SNB.2022.133159
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“3D characterization of the structural transformation undergone by Cu@Ag core-shell nanoparticles following CO₂, reduction reaction”. Arenas Esteban D, Pacquets L, Choukroun D, Hoekx S, Kadu AA, Schalck J, Daems N, Breugelmans T, Bals S, Chemistry of materials 35, 6682 (2023). http://doi.org/10.1021/ACS.CHEMMATER.3C00649
Abstract: The increasing use of metallic nanoparticles (NPs) is significantly advancing the field of electrocatalysis. In particular, Cu/Ag bimetallic interfaces are widely used to enhance the electrochemical CO2 reduction reaction (eCO(2)RR) toward CO and, more recently, C-2 products. However, drastic changes in the product distribution and performance when Cu@Ag core-shell configurations are used can often be observed under electrochemical reaction conditions, especially during the first few minutes of the reaction. Possible structural changes that generate these observations remain underexplored; therefore, the structure-property relationship is hardly understood. In this study, we use electron tomography to investigate the structural transformation mechanism of Cu@Ag core-shells NPs during the critical first minutes of the eCO(2)RR. In this manner, we found that the crystallinity of the Cu seed determines whether the formation of a complete and homogeneous Ag shell is possible. Moreover, by tracking the particles' transformations, we conclude that modifications of the Cu-Ag interface and Cu2O enrichment at the surface of the NPs are key factors contributing to the product generation changes. These insights provide a better understanding of how bimetallic core-shell NPs transform under electrochemical conditions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 8.6
Times cited: 1
DOI: 10.1021/ACS.CHEMMATER.3C00649
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“An atomically dispersed Mn-photocatalyst for generating hydrogen peroxide from seawater via the Water Oxidation Reaction (WOR)”. Ren P, Zhang T, Jain N, Ching HYV, Jaworski A, Barcaro G, Monti S, Silvestre-Albero J, Celorrio V, Chouhan L, Rokicinska A, Debroye E, Kustrowski P, Van Doorslaer S, Van Aert S, Bals S, Das S, Journal of the American Chemical Society 145, 16584 (2023). http://doi.org/10.1021/JACS.3C03785
Abstract: In this work, we have fabricatedan aryl amino-substitutedgraphiticcarbon nitride (g-C3N4) catalyst with atomicallydispersed Mn capable of generating hydrogen peroxide (H2O2) directly from seawater. This new catalyst exhibitedexcellent reactivity, obtaining up to 2230 & mu;M H2O2 in 7 h from alkaline water and up to 1800 & mu;Mfrom seawater under identical conditions. More importantly, the catalystwas quickly recovered for subsequent reuse without appreciable lossin performance. Interestingly, unlike the usual two-electron oxygenreduction reaction pathway, the generation of H2O2 was through a less common two-electron water oxidation reaction(WOR) process in which both the direct and indirect WOR processesoccurred; namely, photoinduced h(+) directly oxidized H2O to H2O2 via a one-step 2e(-) WOR, and photoinduced h(+) first oxidized a hydroxide (OH-) ion to generate a hydroxy radical ((OH)-O-& BULL;), and H2O2 was formed indirectly by thecombination of two (OH)-O-& BULL;. We have characterized thematerial, at the catalytic sites, at the atomic level using electronparamagnetic resonance, X-ray absorption near edge structure, extendedX-ray absorption fine structure, high-resolution transmission electronmicroscopy, X-ray photoelectron spectroscopy, magic-angle spinningsolid-state NMR spectroscopy, and multiscale molecular modeling, combiningclassical reactive molecular dynamics simulations and quantum chemistrycalculations.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY); Theory and Spectroscopy of Molecules and Materials (TSM²)
Impact Factor: 15
Times cited: 21
DOI: 10.1021/JACS.3C03785
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“Bioinspired noncyclic transfer pathway electron donors for unprecedented hydrogen production”. Liu J, Wang C, Yu W, Zhao H, Hu Z-Y, Liu F, Hasan T, Li Y, Van Tendeloo G, Li C, Su B-L, CCS chemistry 5, 1470 (2023). http://doi.org/10.31635/CCSCHEM.022.202202071
Abstract: Electron donors are widely exploited in visible-light photocatalytic hydrogen production. As a typical electron donor pair and often the first choice for hydrogen production, the sodium sulfide-sodium sulfite pair has been extensively used. However, the resultant thiosulfate ions consume the photogenerated electrons to form an undesirable pseudocyclic electron transfer pathway during the photocatalytic process, strongly limiting the solar energy conversion efficiency. Here, we report novel and bioinspired electron donor pairs offering a noncyclic electron transfer pathway that provides more electrons without the consumption of the photogenerated electrons. Compared to the state-of-the-art electron donor pair Na2S-Na2SO3, these novel Na2S-NaH2PO2 and Na2S-NaNO2 electron donor pairs enable an unprecedented enhancement of up to 370% and 140% for average photocatalytic H-2 production over commercial CdS nanoparticles, and they are versatile for a large series of photocatalysts for visible-light water splitting. The discovery of these novel electron donor pairs can lead to a revolution in photocatalysis and is of great significance for industrial visible-light-driven H-2 production. [GRAPHICS] .
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
DOI: 10.31635/CCSCHEM.022.202202071
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“Black titania by sonochemistry : a critical evaluation of existing methods”. Raes A, Ninakanti R, Van den Bergh L, Borah R, Van Doorslaer S, Verbruggen SW, Ultrasonics sonochemistry 100, 106601 (2023). http://doi.org/10.1016/J.ULTSONCH.2023.106601
Abstract: In the field of photocatalysis, the fabrication of black titania is a booming topic, as it offers a system with improved solar light harvesting properties and increased overall efficiency. The darkening of white TiO2 powders can be ascribed to surface hydroxylation, oxygen vacancies, Ti3+ centres, or a combination thereof. A handful of studies suggests these defects can be conveniently introduced by acoustic cavitation, generated during sonochemical treatment of pristine TiO2 powders. In reproducing these studies, P25 TiO2 samples were ultrasonicated for various hours with a power density of 8000 W/L, resulting in powders that indeed became gradually darker with increasing sonication time. However, HAADF–STEM revealed that extensive erosion of the sonotrode tip took place and contaminated the samples, which appeared to be the primary reason for the observed colour change. This was confirmed by UV–Vis DRS and DRIFTS, that showed no significant alteration of the catalyst surface after sonication. EPR measurements showed that only an insignificant fraction of Ti3+ centres were produced, far less than in a TiO2 sample that was chemically reduced with NaBH4. No evidence of the presence oxygen vacancies could be found. The enhanced photocatalytic activities of ultrasonicated materials reported in literature can therefore not be ascribed to the synthesis of actual black (defected) TiO2, but rather to specific changes in morphology as a result of acoustic cavitation. Also, this study underlines the importance of considering probe erosion in sonochemical catalyst synthesis, which is an unavoidable side effect that can have an important impact on the catalyst appearance, properties and performance.
Keywords: A1 Journal article; Theory and Spectroscopy of Molecules and Materials (TSM²); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 8.4
DOI: 10.1016/J.ULTSONCH.2023.106601
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“Critical challenges towards the commercial rollouts of a LOHC-based H2 economy”. Perreault P, Van Hoecke L, Pourfallah H, Kummamuru NB, Boruntea C-R, Preuster P, Current opinion in green and sustainable chemistry 41, 100836 (2023). http://doi.org/10.1016/J.COGSC.2023.100836
Abstract: This short review discusses recent developments related to the storage and release of hydrogen from liquid organic hydrogen carriers (LOHCs). It focusses on three areas of recent literature: the application and development of novel, alternative LOHC systems, process development and process integration in the storage and release of hydrogen from LOHCs, and the electrochemical conversion of LOHCs. For the novel LOHC systems, we briefly focus on reaction enthalpy and storage capacity as main KPIs for the comparison of those systems and discuss the technical availability on a relevant scale. In the field of process- and reactor development our emphasis lies on the power density of the chemical conversion units. The LOHC technology still requires further development to reach the necessary energy efficiency, flexibility and overall research maturity for market competitivity and commercial impact.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 9.3
DOI: 10.1016/J.COGSC.2023.100836
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“Development of an electrochemiluminescent oligonucleotide-based assay for the quantification of prostate cancer associated miR-141-3p in human serum”. Campos R, Thiruvottriyur Shanmugam S, Daems E, Ribeiro R, De Wael K, Bioelectrochemistry: an international journal devoted to electrochemical aspects of biology and biological aspects of electrochemistry 153, 108495 (2023). http://doi.org/10.1016/J.BIOELECHEM.2023.108495
Abstract: MicroRNAs (miRNAs) are small oligonucleotides (18–25 bases), biologically relevant for epigenetic regulation of key processes, particularly in association with cancer. Research effort has therefore been directed towards the monitoring and detection of miRNAs to progress (early) cancer diagnoses. Traditional detection strategies for miRNAs are expensive, with a lengthy time-to-result. In this study we develop an oligonucleotide-based assay using electrochemistry for the specific, selective and sensitive detection of a circulating miRNA (miR-141) associated with prostate cancer. In the assay, the excitation and readout of the signal are independent: an electrochemical stimulation followed by an optical readout. A ‘sandwich’ approach is incorporated, consisting of a biotinylated capture probe immobilised on streptavidin-functionalised surfaces and a detection probe labelled with digoxigenin. We show that the assay allows the detection of miR-141 in human serum, even in the presence of other miRNAs, with a LOD of 0.25 pM. The developed electrochemiluminescent assay has, therefore, the potential for efficient universal oligonucleotide target detection via the redesign of capture and detection probes.
Keywords: A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 5
DOI: 10.1016/J.BIOELECHEM.2023.108495
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“Editorial hydrogen production storage and use”. Perreault P, Preuster P, Current opinion in green and sustainable chemistry 44, 100861 (2023). http://doi.org/10.1016/J.COGSC.2023.100861
Abstract: In the pursuit of clean and sustainable energy sources, hydrogen has emerged as a key contender, offering high energy density and the potential to serve as a carbon-neutral fuel. However, one of the major challenges associated with hydrogen is efficient and safe storage and transportation. In this Special Edition, we delve into the exciting developments in the upcoming hydrogen economy, from its sustainable production to chemical hydrogen storage. Some of our reviews focus on particular technologies namely on liquid organic hydrogen carriers (LOHCs) and the utilization of ammonia as a hydrogen carrier.
Keywords: Editorial; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 9.3
DOI: 10.1016/J.COGSC.2023.100861
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“Editorial overview : photocatalysis 2022 shining light on a diversity of research opportunities”. Verbruggen SW, Mul G, Current opinion in green and sustainable chemistry 42, 100838 (2023). http://doi.org/10.1016/J.COGSC.2023.100838
Keywords: Editorial; Engineering sciences. Technology
Impact Factor: 9.3
DOI: 10.1016/J.COGSC.2023.100838
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“Haem-mediated albumin biosensing : towards voltammetric detection of PFOA”. Moro G, Campos R, Daems E, Moretto LM, De Wael K, Bioelectrochemistry: an international journal devoted to electrochemical aspects of biology and biological aspects of electrochemistry 152, 108428 (2023). http://doi.org/10.1016/J.BIOELECHEM.2023.108428
Abstract: The haem group is a promising redox probe for the design of albumin-based voltammetric sensors. Among the endogenous ligands carried by human serum albumin (hSA), haem is characterised by a reversible redox behaviour and its binding kinetics strongly depend on hSA’s conformation, which, in turn, depends on the presence of other ligands. In this work, the potential applicability of haem, especially hemin, as a redox probe was first tested in a proof-of-concept study using perfluorooctanoic acid (PFOA) as model analyte. PFOA is known to bind hSA by occupying Sudlow’s I site (FA7) which is spatially related to the haem-binding site (FA1). The latter undergoes a conformational change, which is expected to affect hemin’s binding kinetics. To verify this hypothesis, hemin:albumin complexes in the presence/absence of PFOA were first screened by UV–Vis spectroscopy. Once the complex formation was verified, haem was further characterised via electrochemical methods to estimate its electron transfer kinetics. The hemin:albumin:PFOA system was studied in solution, with the aim of describing the multiple equilibria at stake and designing an electrochemical assay for PFOA monitoring. This latter could be integrated with protein-based bioremediation approaches for the treatment of per- and polyfluoroalkyl substances polluted waters. Overall, our preliminary results show how hemin can be applied as a redox probe in albumin-based voltammetric sensing strategies.
Keywords: A1 Journal article; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 5
DOI: 10.1016/J.BIOELECHEM.2023.108428
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“Hierarchical zeolites containing embedded Cd0.2Zn0.8S as a photocatalyst for hydrogen production from seawater”. Yuan Y, Wu F-J, Xiao S-T, Wang Y-T, Yin Z-W, Van Tendeloo G, Chang G-G, Tian G, Hu Z-Y, Wu S-M, Yang X-Y, Chemical communications 59, 7275 (2023). http://doi.org/10.1039/D3CC01409F
Abstract: Uncovering an efficient and stable photocatalytic system for seawater splitting is a highly desirable but challenging goal. Herein, Cd0.2Zn0.8S@Silicalite-1 (CZS@S-1) composites, in which CZS is embedded in the hierarchical zeolite S-1, were prepared and show remarkably high activity, stability and salt resistance in seawater.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.9
DOI: 10.1039/D3CC01409F
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“Impact of anionic ordering on the iron site distribution and valence states in oxyfluoride Sr2FeO3+xF1-x(x=0.08, 0.2) with a layered Perovskite network”. Gamon J, Bassat J-M, Villesuzanne A, Duttine M, Batuk M, Vandemeulebroucke D, Hadermann J, Alassani F, Weill F, Durand E, Demourgues A, Inorganic chemistry 62, 10822 (2023). http://doi.org/10.1021/ACS.INORGCHEM.3C01455
Abstract: Sr2FeO3+x F1-x (x = 0.08, 0.2), an n = 1 Ruddlesden-Popperphase, was synthesized from the oxidationof Sr2FeO3F in air at high temperature followinga fluorine for oxygen substitution and Fe3+ to Fe4+ oxidation. A structural investigation of both compounds was performedusing complementary and high-resolution techniques (Synchrotron X-rayand electron diffraction, Mo''ssbauer spectroscopy, HR-STEM)coupled to DFT calculation. This study reveals that oxidation leadsto a high degree of apical anion disorder coupled to antiphase boundaries. Sr2FeO3F, an oxyfluoride compoundwith an n = 1 Ruddlesden-Popper structure,was identifiedas a potential interesting mixed ionic and electronic conductor (MIEC).The phase can be synthesized under a range of different pO(2) atmospheres, leading to various degrees of fluorinefor oxygen substitution and Fe4+ content. A structuralinvestigation and thorough comparison of both argon- and air-synthesizedcompounds were performed by combining high-resolution X-ray and electrondiffraction, high-resolution scanning transmission electron microscopy,Mo''ssbauer spectroscopy, and DFT calculations. While the argon-synthesizedphase shows a well-behaved O/F ordered structure, this study revealedthat oxidation leads to averaged large-scale anionic disorder on theapical site. In the more oxidized Sr2FeO3.2F0.8 oxyfluoride, containing 20% of Fe4+, two differentFe positions can be identified with a 32%/68% occupancy (P4/nmm space group). This originates due to the presenceof antiphase boundaries between ordered domains within the grains.Relations between site distortion and valence states as well as stabilityof apical anionic sites (O vs F) are discussed. This study paves theway for further studies on both ionic and electronic transport propertiesof Sr2FeO3.2F0.8 and its use in MIEC-baseddevices, such as solid oxide fuel cells.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.6
DOI: 10.1021/ACS.INORGCHEM.3C01455
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“Impact of soot deposits on waste gas-to-electricity conversion in a TiO₂/WO₃-based photofuel cell”. Ag KR, Minja AC, Ninakanti R, Van Hal M, Dingenen F, Borah R, Verbruggen SW, Chemical engineering journal 470, 144390 (2023). http://doi.org/10.1016/J.CEJ.2023.144390
Abstract: An unbiased photo-fuel cell (PFC) is a device that integrates the functions of a photoanode and a cathode to achieve simultaneous light-driven oxidation and dark reduction reactions. As such, it generates electricity while degrading pollutants like volatile organic compounds (VOCs). The photoanode is excited by light to generate electron-hole pairs, which give rise to a photocurrent, and are utilized to oxidise organic pollutants simultaneously. Here we have systematically studied various TiO2/WO3 photoanodes towards their photocatalytic soot degradation performance, PFC performance in the presence of VOCs, and the combination of both. The latter thus mimics an urban environment where VOCs and soot are present simultaneously. The formation of a type-II heterojunction after the addition of a thin TiO2 top layer over a dense WO3 bottom layer, improved both soot oxidation efficiency as well as photocurrent generation, thus paving the way towards low-cost PFC technology for energy recovery from real polluted air.
Keywords: A1 Journal article; Engineering sciences. Technology
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2023.144390
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“Integrated poultry waste management by co-digestion with perennial grass : effects of mixing ratio, pretreatments, reaction temperature, and effluent recycle on biomethanation yield”. Phuttaro C, Krishnan S, Saritpongteeraka K, Charnnok B, Diels L, Chaiprapat S, Biochemical engineering journal 196, 108937 (2023). http://doi.org/10.1016/J.BEJ.2023.108937
Abstract: This work aims to enhance the efficiency of integrated poultry waste management in bio-circular-green economy by maximizing the co-digestion of chicken manure and its digestate-grown biomass. In a series of batch assays, Napier grass (NG) was mixed with chicken manure (CM) at various proportions (100:0, 80:20, 60:40, 50:50, 40:60, 20:80 and 0:100) to identify co-substrate synergism, followed by physiochemical conditioning (size reduction and ultrasonication) of NG before co-digestion. Results indicated that NG mix of at least 80% was required to gain a full methanation potential of the individual substrates; no synergistic ratio above unity was found. However, the combined effect of size reduction and sonication was found to markedly improve the cosubstrate's biodegradability by 88.7%. The findings were then used to run continuous co-digestion at various operating regimes. In optimal continuous co-digestion condition, NG particle size of 0.6-2.4 mm combined with sonication intensity at 1111 kJ/kgTS improved biomethanation yield as high as 106.3%. Sub-thermophilic digestion at 45 degrees C was shown to give a higher and more stable CH4 yield than at 55 degrees C. Finally, it was also found that recycling liquid effluent at 40% to replace freshwater in feed, although showed no significant difference in CH4 yield (& alpha; = 0.05), noticeably increased system buffer capacity. This optimized biodegradation regime could give co-digestion waste management a higher overall plant efficiency and economic return.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 3.9
DOI: 10.1016/J.BEJ.2023.108937
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“Investigating the electrochemical profile of methamphetamine to enable fast on-site detection in forensic analysis”. Drăgan A-M, Parrilla M, Sleegers N, Slosse A, Van Durme F, van Nuijs A, Oprean R, Cristea C, De Wael K, Talanta : the international journal of pure and applied analytical chemistry 255, 124208 (2023). http://doi.org/10.1016/J.TALANTA.2022.124208
Abstract: Methamphetamine (MA) is a synthetic psychoactive drug which is consumed both licitly and illicitly. In some countries it is prescribed for attention-deficit and hyperactivity disorder, and short-term treatment of obesity. More often though, it is abused for its psychostimulant properties. Unfortunately, the spread and abuse of this synthetic drug have increased globally, being reported as the most widely consumed synthetic psychoactive drug in the world in 2019. Attempting to overcome the shortcomings of the currently used on-site methods for MA detection in suspected cargos, the present study explores the potential of electrochemical identification of MA by means of square wave voltammetry on disposable graphite screen-printed electrodes. Hence, the analytical characterization of the method was evaluated under optimal conditions exhibiting a linear range between 50 mu M and 2.5 mM MA, a LOD of 16.7 mu M, a LOQ of 50.0 mu M and a sensitivity of 5.3 mu A mM-1. Interestingly, two zones in the potential window were identified for the detection of MA, depending on its concentration in solution. Furthermore, the oxidative pathway of MA was elucidated employing liquid chromatography – mass spectrometry to understand the change in the electrochemical profile. Thereafter, the selectivity of the method towards MA in mixtures with other drugs of abuse as well as common adulterants/cutting agents was evaluated. Finally, the described method was employed for the analysis of MA in confiscated samples and compared with forensic methods, displaying its potential as a fast and easy-to-use method for on-site analysis.
Keywords: A1 Journal article; Toxicological Centre; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 6.1
DOI: 10.1016/J.TALANTA.2022.124208
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“Investigating the technical and economic potential of solid-state fungal pretreatment at nonsterile conditions for sugar production from poplar wood”. Wittner N, Vasilakou K, Broos W, Vlaeminck SE, Nimmegeers P, Cornet I, Industrial and engineering chemistry research , 1 (2023). http://doi.org/10.1021/ACS.IECR.3C02316
Abstract: Pretreatment is crucial for the conversion of lignocellulose to biofuels. Unlike conventional chemical/physicochemical methods, fungal pretreatment uses white-rot fungi and mild reaction conditions. However, challenges, including substrate sterilization, long duration, and low sugar yields associated with this method, contribute to lower techno-economic performance, an aspect that has rarely been investigated. This study aimed to evaluate the feasibility of fungal pretreatment of nonsterilized poplar wood. Various factors, including inoculum types, fermentation supplements, and cultivation methods, were investigated to optimize the process. A techno-economic assessment of the optimized processes was performed at a full biorefinery scale. The scenario using nonsterilized wood as a substrate, precolonized wood as an inoculum, and a 4 week pretreatment showed a 14.5% reduction in sugar production costs (€2.15/kg) compared to using sterilized wood. Although the evaluation of nonsterilized wood pretreatment showed promising cost reductions, fungal pretreatment remained more expensive than conventional methods due to the significant capital investment required.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM); Sustainable Energy, Air and Water Technology (DuEL); Biochemical Wastewater Valorization & Engineering (BioWaVE); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS)
Impact Factor: 4.2
DOI: 10.1021/ACS.IECR.3C02316
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“Low-viscosity nonaqueous sulfolane–amine–methanol solvent blend for reversible CO2 capture”. Wagaarachchige JD, Idris Z, Arstad B, Kummamuru NB, Sætre KAS, Halstensen M, Jens K-J, Industrial and engineering chemistry research 61, 5942 (2022). http://doi.org/10.1021/ACS.IECR.1C04946
Abstract: In this work, the absorption–desorption performance of CO2 in six new solvent blends of amine (diisopropylamine (DPA), 2-amino-2-methyl-1-propanol (AMP), methyldiethanolamine (MDEA), diethanolamine (DEA), diisopropanolamine (DIPA), and ethanolamine (MEA)), sulfolane, and methanol has been monitored using ATR-FTIR spectroscopy. Additionally, NMR-based species confirmation and solvent viscosity analysis were done for DPA solvent samples. The identified CO2 capture products are monomethyl carbonate (MMC), carbamate, carbonate, and bicarbonate anions in different ratios. The DPA solvent formed MMC entirely with 0.88 molCO2/molamine capture capacity, 0.48 molCO2/molamine cyclic capacity, and 3.28 mPa·s CO2-loaded solvent viscosity. MEA, DEA, DIPA, and MDEA were shown to produce a low or a negligible amount of MMC while AMP occupied an intermediate position.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1021/ACS.IECR.1C04946
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“Micro to nano : multiscale IR analyses reveal zinc soap heterogeneity in a 19th-century painting by Corot”. Ma X, Pavlidis G, Dillon E, Beltran V, Schwartz JJ, Thoury M, Borondics F, Sandt C, Kjoller K, Berrie BH, Centrone A, Analytical chemistry 94, 3103 (2022). http://doi.org/10.1021/ACS.ANALCHEM.1C04182
Abstract: Formation and aggregation of metal carboxylates (metal soaps) can degrade the appearance and integrity of oil paints, challenging efforts to conserve painted works of art. Endeavors to understand the root cause of metal soap formation have been hampered by the limited spatial resolution of Fourier transform infrared microscopy (mu-FTIR). We overcome this limitation using optical photothermal infrared spectroscopy (O-PTIR) and photothermal-induced resonance (PTIR), two novel methods that provide IR spectra with approximate to 500 and approximate to 10 nm spatial resolutions, respectively. The distribution of chemical phases in thin sections from the top layer of a 19th-century painting is investigated at multiple scales (mu-FTIR approximate to 10(2) mu m(3), O-PTIR approximate to 10(-1) mu m(3), PTIR approximate to 10(-5) mu m(3)). The paint samples analyzed here are found to be mixtures of pigments (cobalt green, lead white), cured oil, and a rich array of intermixed, small (often << 0.1 mu m(3)) zinc soap domains. We identify Zn stearate and Zn oleate crystalline soaps with characteristic narrow IR peaks (approximate to 1530-1558 cm(-1)) and a heterogeneous, disordered, water-permeable, tetrahedral zinc soap phase, with a characteristic broad peak centered at approximate to 1596 cm(-1). We show that the high signal-to-noise ratio and spatial resolution afforded by O-PTIR are ideal for identifying phase-separated (or locally concentrated) species with low average concentration, while PTIR provides an unprecedented nanoscale view of distributions and associations of species in paint. This newly accessible nanocompositional information will advance our knowledge of chemical processes in oil paint and will stimulate new art conservation practices.
Keywords: A1 Journal article; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
DOI: 10.1021/ACS.ANALCHEM.1C04182
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“Microneedle array-based electrochemical sensor functionalized with SWCNTs for the highly sensitive monitoring of MDMA in interstitial fluid”. Drăgan A-M, Parrilla M, Cambré, S, Domínguez-Robles J, Detamornrat U, Donnelly RF, Oprean R, Cristea C, De Wael K, Microchemical journal 193, 109257 (2023). http://doi.org/10.1016/J.MICROC.2023.109257
Abstract: Illicit drug consumption constitutes a great concern worldwide due to its increased spread and abuse, and the negative consequences exerted on society. For instance, 3,4-methylenedioxymethamphetamine (MDMA), a synthetic amphetamine-type substance, was abused by 20 million people worldwide in 2020. This psychoactive substance exerts a myriad of effects on the human body being dangerous for the consumer’s health. Besides, MDMA has been used in the treatment of some psychiatric conditions. Therefore, the development of wearable devices for MDMA sensing in biological fluids is of great importance for forensic toxicology (e.g., monitoring of patients with suspected or known MDMA consumption) as well as for therapeutic management of patients. Herein, we report the development of a wearable electrochemical platform based on a hollow microneedle (MN) array sensor for the monitoring of MDMA in the interstitial fluid by square-wave voltammetry. First, the holes of the MN array were modified with conductive pastes to devise a MN patch with a three-electrode system. Subsequently, the functionalization of the working electrode with nanomaterials enhanced MDMA detection. Thereafter, analytical parameters were evaluated exhibiting a slope of 0.05 µA µM−1 within a linear range from 1 to 50 µM and a limit of detection of 0.75 µM in artificial interstitial fluid. Importantly, critical parameters such as selectivity, piercing capability, temperature, reversibility and stability were assessed. Overall, the obtained MN sensor exhibited excellent analytical performance, making it a promising tool for MDMA tracking in interstitial fluid for individuals on probation or under therapeutic treatment.
Keywords: A1 Journal article; Pharmacology. Therapy; Nanostructured and organic optical and electronic materials (NANOrOPT); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 4.8
DOI: 10.1016/J.MICROC.2023.109257
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“Multi-scale X-ray imaging of the pigment discoloration processes triggered by chlorine compounds in the Upper Basilica of Saint Francis of Assisi”. Avranovich Clerici E, De Meyer S, Vanmeert F, Legrand S, Monico L, Miliani C, Janssens K, Molecules: a journal of synthetic chemistry and natural product chemistry 28, 6106 (2023). http://doi.org/10.3390/MOLECULES28166106
Abstract: In this paper, the chromatic alteration of various types of paints, present on mural painting fragments derived from the vaults of The Upper Basilica of Saint Francis of Assisi in Italy (12th-13th century), is studied using synchrotron radiation. Six painted mural fragments, several square centimeters in size, were available for analysis, originating from the ceiling paintings attributed to Cimabue and Giotto; they correspond to originally white, blue/green, and brown/yellow/orange areas showing discoloration. As well as collecting macroscopic X-ray fluorescence and diffraction maps from the entire fragments in the laboratory and at the SOLEIL synchrotron, corresponding paint cross-sections were also analyzed using microscopic X-ray fluorescence and powder diffraction mapping at the PETRA-III synchrotron. Numerous secondary products were observed on the painted surfaces, such as (a) copper tri-hydroxychloride in green/blue areas; (b) corderoite and calomel in vermillion red/cinnabar-rich paints; (c) plattnerite and/or scrutinyite assumed to be oxidation products of (hydro)cerussite (2PbCO(3)center dot Pb(OH)(2)) in the white areas, and (d) the calcium oxalates whewellite and weddellite. An extensive presence of chlorinated metal salts points to the central role of chlorine-containing compounds during the degradation of the 800-year-old paint, leading to, among other things, the formation of the rare mineral cumengeite (21PbCl(2)center dot 20Cu(OH) (2) center dot 6H(2)O).
Keywords: A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 4.6
DOI: 10.3390/MOLECULES28166106
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“NanoMIPs-based electrochemical sensors for selective detection of amphetamine”. Truta F, Cruz AG, Tertis M, Zaleski C, Adamu G, Allcock NS, Suciu M, Stefan M-G, Kiss B, Piletska E, De Wael K, Piletsky SA, Cristea C, Microchemical journal 191, 108821 (2023). http://doi.org/10.1016/J.MICROC.2023.108821
Abstract: A highly sensitive and portable electrochemical sensor based on molecularly imprinted nanoparticles (nanoMIPs) was developed. NanoMIPs were computationally designed for specific recognition of amphetamine, and then synthetized using solid phase synthesis. NanoMIPs were immobilized onto screen-printed carbon electrodes using a composite film comprising chitosan, nanoMIPs, and graphene oxide.Ferrocenylmethyl methacrylate was incorporated in nanoMIPs allowing electrochemical detection. The signal recorded for the electrochemical oxidation of ferrocene has proven to be dependent on the presence of amphetamine interacting with nanMIPs. The sensor was tested successfully with street samples, with high sensitivity and satisfactory recoveries (from 100.9% to 107.6%). These results were validated with UPL-MS/MS. The present technology is suitable for forensic applications in selective determination of amphetamine in street samples.
Keywords: A1 Journal article; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 4.8
DOI: 10.1016/J.MICROC.2023.108821
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“Nanoporous Dealloyed Metal Materials Processing and Applications?A Review”. Scandura G, Kumari P, Palmisano G, Karanikolos GN, Orwa J, Dumee LF, Industrial and engineering chemistry research (2023). http://doi.org/10.1021/ACS.IECR.2C03952
Abstract: The development of porous metal materials with pore geometries and sizes at the nanoscale offers promising opportunities for the development of smart responsive interfaces for separation and catalytic applications and as building blocks for complex composite materials. Dealloying is an innovative technique based on selective removal of a sacrificial metal from a metal alloy to engineer surface textures and pores across significant thicknesses. Dealloyed structures may be processed over large scales and for a range of source alloys, offering unprecedented manufacturing opportunities. This review presents the operations and challenges of dealloying routes and discusses avenues for process optimizations and improvements, aiming at the development of scalable nanoporous materials. The potential of dealloyed materials for catalytic and sensing applications is expanded and benchmarked against reference materials. Future prospects and applications of dealloyed materials toward surface reactivity control and pore architecture development are highlighted.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.2
DOI: 10.1021/ACS.IECR.2C03952
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