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“Synthesis, structure, and electrochemical properties of k-based sulfates K2M2(SO4)3) with M = Fe and Cu”. Lander L, Rousse G, Batuk D, Colin CV, Dalla Corte DA, Tarascon J-M, Inorganic chemistry 56, 2013 (2017). http://doi.org/10.1021/ACS.INORGCHEM.6B02526
Abstract: Stabilizing new host structures through potassium extraction from K-based polyanionic materials has been proven to be an interesting approach to develop new Li+/Na+ insertion materials. Pursuing the same trend, we here report the feasibility of preparing langbeinite “Fe-2(SO4)(3)” via electrochemical and chemical oxidation of K2Fe2(SO4)(3). Additionally, we succeeded in stabilizing a new K2Cu2(SO4)(3) phase via a solid-state synthesis approach. This novel compound crystallizes in a complex orthorhombic structure that differs from that of langbeinite as deduced from synchrotron X-ray and neutron powder diffraction. Electrochemically, the performance of this new phase is limited, which we explain in terms of sluggish diffusion kinetics. We further show that K2Cu2(SO4)(3) decomposes into K2Cu3O(SO4)(3) on heating, and we report for the first time the synthesis of fedotovite K2Cu3O(SO4)(3). Finally, the fundamental attractiveness of these S = 1/2 systems for physicists is examined by neutron magnetic diffraction, which reveals the absence of a long-range ordering of Cu2+ magnetic moments down to 1.5 K.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 13
DOI: 10.1021/ACS.INORGCHEM.6B02526
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“Molybdenum oxide nitrides of the Mo2(O,N,\square)5 type : on the way to Mo2O5”. Weber D, Huber M, Gorelik TE, Abakumov AM, Becker N, Niehaus O, Schwickert C, Culver SP, Boysen H, Senyshyn A, Poettgen R, Dronskowski R, Ressler T, Kolb U, Lerch M, Inorganic chemistry 56, 8782 (2017). http://doi.org/10.1021/ACS.INORGCHEM.7B00551
Abstract: Blue-colored molybdenum oxide nitrides of the Mo-2(O,N,square)(5) type were synthesized by direct nitridation of commercially available molybdenum trioxide with a mixture of gaseous ammonia and oxygen. Chemical composition, crystal structure, and stability of the obtained and hitherto unknown compounds are studied extensively. The average oxidation state of +5 for molybdenum is proven by Mo K near-edge X-ray absorption spectroscopy; the magnetic behavior is in agreement with compounds exhibiting (MoO6)-O-v units. The new materials are stable up to similar to 773 K in an inert gas atmosphere. At higher temperatures, decomposition is observed. X-ray and neutron powder diffraction, electron diffraction, and high-resolution transmission electron microscopy reveal the structure to be related to VNb9O24.9-type phases, however, with severe disorder hampering full structure determination. Still, the results demonstrate the possibility of a future synthesis of the potential binary oxide Mo2O5. On the basis of these findings, a tentative suggestion on the crystal structure of the potential compound Mo2O5, backed by electronic-structure and phonon calculations from first principles, is given.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 3
DOI: 10.1021/ACS.INORGCHEM.7B00551
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“Ferrimagnetism as a consequence of unusual cation ordering in the Perovskite SrLa2FeCoSbO9”. Tang Y, Hunter EC, Battle PD, Hendrickx M, Hadermann J, Cadogan JM, Inorganic chemistry 57, 7438 (2018). http://doi.org/10.1021/ACS.INORGCHEM.8B01012
Abstract: A polycrystalline sample of SrLa2FeCoSbO9 has been prepared in a solid-state reaction and studied by a combination of electron microscopy, magnetometry, Mossbauer spectroscopy, X-ray diffraction, and neutron diffraction. The compound adopts a monoclinic (space group P2(1)/n; a = 5.6218(6), b = 5.6221(6), c = 7.9440(8) angstrom, beta = 90.050(7)degrees at 300 K) perovskite-like crystal structure with two crystallographically distinct six-coordinate sites. One of these sites is occupied by 2/3 Co-2(+),1/3 Fe3+ and the other by 2/3 Sb5+, 1/3 Fe3+. This pattern of cation ordering results in a transition to a ferrimagnetic phase at 215 K. The magnetic moments on nearest-neighbor, six-coordinate cations align in an antiparallel manner, and the presence of diamagnetic Sb5+ on only one of the two sites results in a nonzero remanent magnetization of similar to 1 mu(B) per formula unit at 5 K.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 6
DOI: 10.1021/ACS.INORGCHEM.8B01012
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“Layered CeSO and LiCeSO oxide chalcogenides obtained via topotactic oxidative and reductive transformations”. Cassidy SJ, Pitcher MJ, Lim JJK, Hadermann J, Allen JP, Watson GW, Britto S, Chong EJ, Free DG, Grey CP, Clarke SJ, Inorganic chemistry 58, 3838 (2019). http://doi.org/10.1021/ACS.INORGCHEM.8B03485
Abstract: The chemical accessibility of the Celv oxidation state enables redox chemistry to be performed on the naturally coinagemetal -deficient phases CeM1-xSO (M = Cu, Ag). A metastable black compound with the PbFC1 structure type (space group P4/nmm: a = 3.8396(1) angstrom, c = 6.607(4) angstrom, V = 97.40(6) angstrom(3)) and a composition approaching CeSO is obtained by deintercalation of Ag from CeAg0.8SO. High-resolution transmission electron microscopy reveals the presence of large defect-free regions in CeSO, but stacking faults are also evident which can be incorporated into a quantitative model to account for the severe peak anisotropy evident in all the highresolution X-ray and neutron diffractograms of bulk CeSO samples; these suggest that a few percent of residual Ag remains. A strawcolored compound with the filled PbFCI (i.e., ZrSiCuAs- or HfCuSi2type) structure (space group P4/nmm: a = 3.98171(1) angstrom, c = 8.70913(5) angstrom, V = 138.075(1) angstrom 3) and a composition close to LiCeSO, but with small amounts of residual Ag, is obtained by direct reductive lithiation of CeAga8S0 or by insertion of Li into CeSO using chemical or electrochemical means. Computation of the band structure of pure, stoichiometric CeSO predicts it to be a Ce' compound with the 4f-states lying approximately 1 eV above the sulfide-dominated valence band maximum. Accordingly, the effective magnetic moment per Ce ion measured in the CeSO samples is much reduced from the value found for the Ce3+-containing LiCeSO, and the residual paramagnetism corresponds to the Ce3+ ions remaining due to the presence of residual Ag, which presumably reflects the difficulty of stabilizing Ce' in the presence of sulfide (S2-). Comparison of the behavior of CeCu0.8SO with that of CeCu0.8SO reveals much slower reaction kinetics associated with the Cu,_xS layers, and this enables intermediate CeCui LixSO phases to be isolated.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
DOI: 10.1021/ACS.INORGCHEM.8B03485
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“Exsolution of SrO during the Topochemical Conversion of LaSr3CoRuO8to the Oxyhydride LaSr3CoRuO4H4”. Jin L, Batuk M, Kirschner FKK, Lang F, Blundell SJ, Hadermann J, Hayward MA, Inorganic chemistry 58, 14863 (2019). http://doi.org/10.1021/acs.inorgchem.9b02552
Abstract: Reaction of the n = 1 Ruddlesden-Popper oxide LaSr3CoRuO8 with CaH2 yields the oxyhydride phase LaSr3CoRuO4H4 via topochemical anion-exchange. Close inspection of X-ray and neutron powder diffraction data in combination with HAADF-STEM images reveals that nanoparticles of SrO are exsolved from the system during the reaction, with the change in cation stoichiometry accommodated by the inclusion of n > 1 (Co/Ru)nOn+1H2n ‘perovskite’ layers into the Ruddlesden-Popper stacking sequence. This novel pseudo-topochemical process offers a new route for the formation of n > 1 Ruddlesden-Popper structured materials. Magnetization data are consistent with a LaSr3Co1+Ru2+O4H4 (Co1+, d8, S = 1; Ru2+, d6, S = 0) oxidation/spin state combination. Neutron diffraction and μ+SR data show no evidence for long-range magnetic order down to 2 K, suggesting the diamagnetic Ru2+ centers impede the Co-Co magnetic exchange interactions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 1
DOI: 10.1021/acs.inorgchem.9b02552
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“Magnetic Ordering in the Layered Cr(II) Oxide Arsenides Sr2CrO2Cr2As2and Ba2CrO2Cr2As2”. Xu X, Jones MA, Cassidy SJ, Manuel P, Orlandi F, Batuk M, Hadermann J, Clarke SJ, Inorganic Chemistry 59, 15898 (2020). http://doi.org/10.1021/acs.inorgchem.0c02415
Abstract: Sr2CrO2Cr2As2 and Ba2CrO2Cr2As2 with Cr2+ ions in CrO2 sheets and in CrAs layers crystallize with the Sr2Mn3Sb2O2 structure (space group I4/mmm, Z = 2) and lattice parameters a = 4.00800(2) Å, c = 18.8214(1) Å (Sr2CrO2Cr2As2) and a = 4.05506(2) Å, c = 20.5637(1) Å (Ba2CrO2Cr2As2) at room temperature. Powder neutron diffraction reveals checkerboard-type antiferromagnetic ordering of the Cr2+ ions in the arsenide layers below TN1Sr, of 600(10) K (Sr2CrO2Cr2As2) and TN1Ba 465(5) K (Ba2CrO2Cr2As2) with the moments initially directed perpendicular to the layers in both compounds. Checkerboard-type antiferromagnetic ordering of the Cr2+ ions in the oxide layer below 230(5) K for Ba2CrO2Cr2As2 occurs with these moments also perpendicular to the layers, consistent with the orientation preferences of d4 moments in the two layers. In contrast, below 330(5) K in Sr2CrO2Cr2As2, the oxide layer Cr2+ moments are initially oriented in the CrO2 plane; but on further cooling, these moments rotate to become perpendicular to the CrO2 planes, while the moments in the arsenide layers rotate by 90° with the moments on the two sublattices remaining orthogonal throughout [behavior recently reported independently by Liu et al. [Liu et al. Phys. Rev. B 2018, 98, 134416]]. In Sr2CrO2Cr2As2, electron diffraction and high resolution powder X-ray diffraction data show no evidence for a structural distortion that would allow the two Cr2+ sublattices to couple, but high resolution neutron powder diffraction data suggest a small incommensurability between the magnetic structure and the crystal structure, which may account for the coupling of the two sublattices and the observed spin reorientation. The saturation values of the Cr2+ moments in the CrO2 layers (3.34(1) μB (for Sr2CrO2Cr2As2) and 3.30(1) μB (for Ba2CrO2Cr2As2)) are larger than those in the CrAs layers (2.68(1) μB for Sr2CrO2Cr2As2 and 2.298(8) μB for Ba2CrO2Cr2As2) reflecting greater covalency in the arsenide layers.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.6
DOI: 10.1021/acs.inorgchem.0c02415
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“Ambient and high pressure CuNiSb₂, : metal-ordered and metal-disordered NiAs-type derivative pnictides”. Skaggs CM, Kang C-J, Perez CJ, Hadermann J, Emge TJ, Frank CE, Pak C, Lapidus SH, Walker D, Kotliar G, Kauzlarich SM, Tan X, Greenblatt M, Inorganic Chemistry 59, 14058 (2020). http://doi.org/10.1021/ACS.INORGCHEM.0C01848
Abstract: The mineral Zlatogorite, CuNiSb2, was synthesized in the laboratory for the first time by annealing elements at ambient pressure (CuNiSb2-AP). Rietveld refinement of synchrotron powder X-ray diffraction data indicates that CuNiSb2-AP crystallizes in the NiAs-derived structure (P (3) over bar m1, #164) with Cu and Ni ordering. The structure consists of alternate NiSb6 and CuSb6 octahedral layers via face-sharing. The formation of such structure instead of metal disordered NiAs-type structure (P6(3)/mmc, #194) is validated by the lower energy of the ordered phase by first-principle calculations. Interatomic crystal orbital Hamilton population, electron localization function, and charge density analysis reveal strong Ni-Sb, Cu-Sb, and Cu-Ni bonding and long weak Sb-Sb interactions in CuNiSb2-AP. The magnetic measurement indicates that CuNiSb2-AP is Pauli paramagnetic. First-principle calculations and experimental electrical resistivity measurements reveal that CuNiSb2-AP is a metal. The low Seebeck coefficient and large thermal conductivity suggest that CuNiSb2 is not a potential thermoelectric material. Single crystals were grown by chemical vapor transport. The high pressure sample (CuNiSb2-8 GPa) was prepared by pressing CuNiSb2-AP at 700 degrees C and 8 GPa. However, the structures of single crystal and CuNiSb2-8 GPa are best fit with a disordered metal structure in the P (3) over bar m1 space group, corroborated by transmission electron microscopy.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.6
DOI: 10.1021/ACS.INORGCHEM.0C01848
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“Charge Localization and Magnetic Correlations in the Refined Structure of U3O7”. Leinders G, Baldinozzi G, Ritter C, Saniz R, Arts I, Lamoen D, Verwerft M, Inorganic Chemistry 60, 10550 (2021). http://doi.org/10.1021/acs.inorgchem.1c01212
Abstract: Atomic arrangements in the mixed-valence oxide U3O7 are refined from high-resolution neutron scattering data. The crystallographic model describes a long-range structural order in a U60O140 primitive cell (space group P42/n) containing distorted cuboctahedral oxygen clusters. By combining experimental data and electronic structure calculations accounting for spin–orbit interactions, we provide robust evidence of an interplay between charge localization and the magnetic moments carried by the uranium atoms. The calculations predict U3O7 to be a semiconducting solid with a band gap of close to 0.32 eV, and a more pronounced charge-transfer insulator behavior as compared to the well-known Mott insulator UO2. Most uranium ions (56 out of 60) occur in 9-fold and 10-fold coordinated environments, surrounding the oxygen clusters, and have a tetravalent (24 out of 60) or pentavalent (32 out of 60) state. The remaining uranium ions (4 out of 60) are not contiguous to the oxygen cuboctahedra and have a very compact, 8-fold coordinated environment with two short (2 × 1.93(3) Å) “oxo-type” bonds. The higher Hirshfeld charge and the diamagnetic character point to a hexavalent state for these four uranium ions. Hence, the valence state distribution corresponds to 24/60 × U(IV) + 32/60 U(V) + 4/60 U(VI). The tetravalent and pentavalent uranium ions are predicted to carry noncollinear magnetic moments (with amplitudes of 1.6 and 0.8 μB, respectively), resulting in canted ferromagnetic order in characteristic layers within the overall fluorite-related structure.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
DOI: 10.1021/acs.inorgchem.1c01212
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“Chemistry, local molybdenum clustering, and electrochemistry in the Li2+xMo1-xO3 solid solutions”. Savina AA, Saiutina VV, Morozov AV, Boev AO, Aksyonov DA, Dejoie C, Batuk M, Bals S, Hadermann J, Abakumov AM, Inorganic chemistry 61, 5637 (2022). http://doi.org/10.1021/ACS.INORGCHEM.2C00420
Abstract: A broad range of cationic nonstoichiometry has been demonstratedfor the Li-rich layered rock-salt-type oxide Li2MoO3, which has generally been considered as a phase with a well-defined chemical composition. Li2+xMo1-xO3(-0.037 <= x <= 0.124) solid solutions were synthesized via hydrogen reduction ofLi2MoO4in the temperature range of 650-1100 degrees C, withxdecreasing with theincrease of the reduction temperature. The solid solutions adopt a monoclinicallydistorted O3-type layered average structure and demonstrate a robust localordering of the Li cations and Mo3triangular clusters within the mixed Li/Mocationic layers. The local structure was scrutinized in detail by electron diffractionand aberration-corrected scanning transmission electron microcopy (STEM),resulting in an ordering model comprising a uniform distribution of the Mo3clusters compatible with local electroneutrality and chemical composition. The geometry of the triangular clusters with their oxygenenvironment (Mo3O13groups) has been directly visualized using differential phase contrast STEM imaging. The established localstructure was used as input for density functional theory (DFT)-based calculations; they support the proposed atomic arrangementand provide a plausible explanation for the staircase galvanostatic charge profiles upon electrochemical Li+extraction fromLi2+xMo1-xO3in Li cells. According to DFT, all electrochemical capacity in Li2+xMo1-xO3solely originates from the cationic Moredox process, which proceeds via oxidation of the Mo3triangular clusters into bent Mo3chains where the electronic capacity of the clusters depends on the initial chemical composition and Mo oxidation state defining the width of the first charge low-voltageplateau. Further oxidation at the high-voltage plateau proceeds through decomposition of the Mo3chains into Mo2dimers and further into individual Mo6+cations
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.6
Times cited: 3
DOI: 10.1021/ACS.INORGCHEM.2C00420
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“Structures and magnetic ordering in layered Cr oxide arsenides Sr₂CrO₂Cr₂OAs₂, and Sr₂CrO₃CrAs”. Sheath BC, Xu X, Manuel P, Hadermann J, Batuk M, O'Sullivan J, Bonilla RS, Clarke SJ, Inorganic chemistry 61, 10 (2022). http://doi.org/10.1021/ACS.INORGCHEM.2C01773
Abstract: Two novel chromium oxide arsenide materials have been synthesized, Sr2CrO2Cr2OAs2 (i.e., Sr2Cr3As2O3) and Sr2CrO3CrAs (i.e., Sr2Cr2AsO3), both of which contain chromium ions in two distinct layers. Sr2CrO2Cr2OAs2 was targeted following electron microscopy measurements on a related phase. It crystallizes in the space group P4/mmm and accommodates distorted CrO4As2 octahedra containing Cr2+ and distorted CrO(2)As(4 )octahedra containing Cr3+. In contrast, Sr2CrO3CrAs incorporates Cr3+ in CrO5 square-pyramidal coordination in [Sr2CrO3](+) layers and Cr2+ ions in CrAs(4 )tetrahedra in [CrAs](-) layers and crystallizes in the space group P4/nmm. Powder neutron diffraction data reveal antiferromagnetic ordering in both compounds. In Sr2CrO3CrAs the Cr2+ moments in the [CrAs](-) layers exhibit long-range ordering, while the Cr3+ moments in the [Sr2CrO3](+) layers only exhibit short-range ordering. However, in Sr2CrO2Cr2OAs2, both the Cr(2+ )moments in the CrO4As2 environments and the Cr3+ moments in the CrO2As4 polyhedra are long-range-ordered below 530(10) K. Above this temperature, only the Cr3+ moments are ordered with a Neel temperature slightly in excess of 600 K. A subtle structural change is evident in Sr2CrO2Cr2OAs2 below the magnetic ordering transitions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.6
DOI: 10.1021/ACS.INORGCHEM.2C01773
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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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“Defective biphenylene as high-efficiency hydrogen evolution catalysts”. Luo Y, He Y, Ding Y, Zuo L, Zhong C, Ma Y, Sun M, Inorganic chemistry 63, 1136 (2023). http://doi.org/10.1021/ACS.INORGCHEM.3C03503
Abstract: Electrocatalysts play a pivotal role in advancing the application of water splitting for hydrogen production. This research unveils the potential of defective biphenylenes as high-efficiency catalysts for the hydrogen evolution reaction. Using first-principles simulations, we systematically investigated the structure, stability, and catalytic performance of defective biphenylenes. Our findings unveil that defect engineering significantly enhances the electrocatalytic activity for hydrogen evolution. Specifically, biphenylene with a double-vacancy defect exhibits an outstanding Gibbs free energy of -0.08 eV, surpassing that of Pt, accompanied by a remarkable exchange current density of -3.08 A cm(-2), also surpassing that of Pt. Furthermore, we find the preference for the Volmer-Heyrovsky mechanism in the hydrogen evolution reaction, with a low energy barrier of 0.80 eV. This research provides a promising avenue for developing novel metal-free electrocatalysts for water splitting with earth-abundant carbon elements, making a significant step toward sustainable hydrogen production.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 4.6
DOI: 10.1021/ACS.INORGCHEM.3C03503
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“Functional Respiratory Imaging as a tool to personalize respiratory treatment in subjects with unilateral diaphragmatic paralysis”. Van Holsbeke CS, Leemans G, Vos WG, de Backer JW, Vinchurkar SC, Geldof M, Verdonck PR, Parizel PM, van Schil PE, de Backer WA, Respiratory care , 1 (2013). http://doi.org/10.4187/respcare.02756
Abstract: In two subjects with a unilateral diaphragmatic paralysis and complaints of dyspnea, a completely different treatment approach was chosen despite similar anatomical and physiological abnormalities. These decisions were supported by the results generated by Functional Respiratory Imaging (FRI). FRI was able to generate functional information with respect to lobar ventilation and local drug deposition. In one subject, it was found that some lobes were poorly ventilated and drug deposition simulation showed that some regions were undertreated. This subject underwent a diaphragm plication to restore the ventilation. In the other subject, it was found that all lobes were still ventilated. A conservative approach with regular follow-up was chosen to wait for spontaneous recovery of the diaphragmatic function. Both subjects improved subjectively and objectively. These cases demonstrate how novel medical imaging techniques such as FRI can be used to personalize respiratory treatment in subjects with unilateral diaphragmatic paralysis.
Keywords: A1 Journal article; Condensed Matter Theory (CMT); Antwerp Surgical Training, Anatomy and Research Centre (ASTARC); Laboratory Experimental Medicine and Pediatrics (LEMP)
Impact Factor: 1.733
Times cited: 5
DOI: 10.4187/respcare.02756
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“High-resolution X-ray fluorescence microtomography of homogeneous samples”. Simionovici AS, Chukalina M, Schroer C, Drakopoulos M, Snigirev A, Snigireva I, Lengeler B, Janssens K, Adams F, IEEE transactions on nuclear science 47, 2736 (2000). http://doi.org/10.1109/23.901180
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.171
DOI: 10.1109/23.901180
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“Modeling of electroporation induced by pulsed electric fields in irregularly shaped cells”. Mescia L, Chiapperino MA, Bia P, Gielis J, Caratelli D, IEEE transactions on biomedical engineering 65, 414 (2018). http://doi.org/10.1109/TBME.2017.2771943
Abstract: During the past decades, the poration of cell membrane induced by pulsed electric fields has been widely investigated. Since the basic mechanisms of this process have not yet been fully clarified, many research activities are focused on the development of suitable theoretical and numerical models. To this end, a nonlinear, nonlocal, dispersive, and space-time numerical algorithm has been developed and adopted to evaluate the transmembrane voltage and pore density along the perimeter of realistic irregularly shaped cells. The presented model is based on the Maxwell's equations and the asymptotic Smoluchowski's equation describing the pore dynamics. The dielectric dispersion of the media forming the cell has been modeled by using a general multirelaxation Debye-based formulation. The irregular shape of the cell is described by using the Gielis' superformula. Different test cases pertaining to red blood cells, muscular cells, cell in mitosis phase, and cancer-like cell have been investigated. For each type of cell, the influence of the relevant shape, the dielectric properties, and the external electric pulse characteristics on the electroporation process has been analyzed. The numerical results demonstrate that the proposed model is an efficient numerical tool to study the electroporation problem in arbitrary-shaped cells.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1109/TBME.2017.2771943
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“SEM-EDX hyperspectral data analysis for the study of soil aggregates”. Allegretta I, Legrand S, Alfeld M, Gattullo CE, Porfido C, Spagnuolo M, Janssens K, Terzano R, Geoderma: an international journal of soil science 406 (2022). http://doi.org/10.1016/J.GEODERMA.2021.115540
Abstract: Scanning electron microscopy coupled with microanalysis (SEM-EDX) is an important analytical tool for the morphological and chemical characterization of different types of materials. In many applications, SEM-EDX elemental maps are usually used and processed as images, thus flattening and reducing the spectroscopic information contained in EDX hyperspectral data cubes. The exploitation of the full hyperspectral dataset could be indeed very useful for the study of complex matrices like soil. In order to maximize the information attainable by SEM-EDX data cubes analysis, the software package “Datamuncher Gamma” was implemented and applied to study soil aggregates. By using this approach, different phases (silicates, aluminosilicates, Ca-carbonates, Ca-phosphates, organic matter, iron oxides) inside soil aggregates were successfully identified and segmented. The advantages of this method over the common ROI imaging approach are presented. Finally, this method was used to compare different aggregates in a Cr-polluted soil and understand their possible pedological history. The present method can be used for the analysis of every type of SEM-EDX data cubes, allowing its application to different types of samples and fields of study.
Keywords: A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 6.1
DOI: 10.1016/J.GEODERMA.2021.115540
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“Post-plasma quenching to improve conversion and energy efficiency in a CO2 microwave plasma”. Mercer Er, Van Alphen S, van Deursen Cfam, Righart Twh, Bongers Wa, Snyders R, Bogaerts A, van de Sanden Mcm, Peeters Fjj, Fuel 334, 126734 (2023). http://doi.org/10.1016/j.fuel.2022.126734
Abstract: Transforming CO2 into value-added chemicals is crucial to realizing a carbon–neutral economy, and plasma-based conversion, a Power-2-X technology, offers a promising route to realizing an efficient and scalable process. This paper investigates the effects of post-plasma placement of a converging–diverging nozzle in a vortex-stabilized 2.45 GHz CO2 microwave plasma reactor to increase energy efficiency and conversion. The CDN leads to a 21 % relative increase in energy efficiency (31 %) and CO2 conversion (13 %) at high flow rates and near-atmospheric conditions. The most significant performance improvement was seen at low flow rates and sub-atmospheric pressure (300 mbar), where energy efficiency was 23 % and conversion was 28 %, a 71 % relative increase over conditions without the CDN. Using CFD simulations, we found that the CDN produces a change in the flow geometry, leading to a confined temperature profile at the height of the plasma, and forced extraction of CO to the post-CDN region.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.4
DOI: 10.1016/j.fuel.2022.126734
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“Trace metal analysis of sediments and particulate matter in sea water by energy-dispersive X-ray fluorescence”. Vanderstappen M, Van Grieken R, Fresenius' Zeitschrift für analytische Chemie 282, 25 (1976). http://doi.org/10.1007/BF00443774
Abstract: The capability of energy-dispersive X-ray fluorescence was investigated for fast and simple chemical analysis of trace elements in sediments and particulate matter in sea water. Nuclepore 0.4 μm pore-size membranes are recommended as optimal filters for a straightforward collection of suspended material. The collection of suspended trace metals by filtration seemed to give a sufficiently homogeneous filter load (s% <2.5). Data are presented on the concentrations of K, Ca, Ti, Cr, Mn, Fe, Ni, Cu, Zn, Br, Pb, Rb and Sr with a fair precision (s% < 5.6) and accuracy.
Keywords: A3 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
DOI: 10.1007/BF00443774
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“Crystallization of PZT in porous alumina membrane channels”. Zhigalina OM, Mishina ED, Sherstyuk NE, Vorotilov KA, Vasiljev VA, Sigov AS, Lebedev OI, Grigoriev YV, de Santo MP, Barberi R, Rasing T, Ferroelectrics 336, 247 (2006). http://doi.org/10.1080/00150190600697756
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 0.551
Times cited: 10
DOI: 10.1080/00150190600697756
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“Extended stability region for large bipolarons through interaction with multiple phonon branches”. Verbist G, Peeters FM, Devreese JT, Ferroelectrics 130, 27 (1992). http://doi.org/10.1080/00150199208019532
Abstract: The large (bi)polaron is investigated for the case where the electron interacts with multiple LO-phonon branches. Explicit expressions for the groundstate energy and the effective mass are obtained within the Feynman polaron model approximation and they are applied to the material SrTiO3. The results of an effective LO-phonon branch approximation are compared with the results in which all LO-phonon branches are explicitly included. We show how the stability region for large bipolaron formation is enlarged when the electrons interact with multiple LO-phonon branches. The possible relevance of this result for the high-T(c) superconductors is pointed out.
Keywords: A1 Journal article; Condensed Matter Theory (CMT); Theory of quantum systems and complex systems
Impact Factor: 0.469
Times cited: 19
DOI: 10.1080/00150199208019532
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“Twin boundary structure of Au-doped YBa2Cu3O7-x single crystals”. Rosova A, Krekels T, Van Tendeloo G, Darriet B, Chambon M, Ferroelectrics 141, 87 (1993)
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 0.469
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“Chabazite : stable cation-exchanger in hyper alkaline concrete pore water”. Van Tendeloo L, Wangermez W, Kurttepeli M, de Blochouse B, Bals S, Van Tendeloo G, Martens JA, Maes A, Kirschhock CEA, Breynaert E, Environmental science and technology 49, 2358 (2015). http://doi.org/10.1021/es505346j
Abstract: To avoid impact on the environment, facilities for permanent disposal of hazardous waste adopt multibarrier design schemes. As the primary barrier very often consists of cement-based materials, two distinct aspects are essential for the selection of suitable complementary barriers: (1) selective sorption of the contaminants in the repository and (2) long-term chemical stability in hyperalkaline concrete-derived media. A multidisciplinary approach combining experimental strategies from environmental chemistry and materials science is therefore essential to provide a reliable assessment of potential candidate materials. Chabazite is typically synthesized in 1 M KOH solutions but also crystallizes in simulated young cement pore water, a pH 13 aqueous solution mainly containing K+ and Na+ cations. Its formation and stability in this medium was evaluated as a function of temperature (60 and 85 °C) over a timeframe of more than 2 years and was also asessed from a mechanistic point of view. Chabazite demonstrates excellent cation-exchange properties in simulated young cement pore water. Comparison of its Cs+ cation exchange properties at pH 8 and pH 13 unexpectedly demonstrated an increase of the KD with increasing pH. The combined results identify chabazite as a valid candidate for inclusion in engineered barriers for concrete-based waste disposal.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.198
Times cited: 13
DOI: 10.1021/es505346j
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“Confocal micrometer-scale X-ray fluorescence and X-ray absorption fine structure studies of uranium speciation in a tertiary sediment from a waste disposal natural analogue site”. Denecke MA, Janssens K, Proost K, Rothe J, Noseck U, Environmental science and technology 39, 2049 (2005). http://doi.org/10.1021/ES048644K
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.198
Times cited: 47
DOI: 10.1021/ES048644K
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“Copper stabilization by zeolite synthesis in polluted soils treated with coal fly ash”. Terzano R, Spagnuolo M, Medici L, Vekemans B, Vincze L, Janssens K, Ruggiero P, Environmental science and technology 39, 6280 (2005). http://doi.org/10.1021/ES050079D
Abstract: This study deals with the process of zeolite formation in an agricultural soil artificially polluted by high amounts of Cu (15 mg of Cu/g of soil dry weight) and treated with fused coal fly ash at 30 and 60 degrees C and how this process affects the mobility and availability of the metal. As a consequence of the treatment, the amount of dissolved Cu, and thus its mobility, was strongly reduced, and the percentage of the metal stabilized in the solid phase increased over time, reaching values of 30% at 30 degrees C and 40% at 60 degrees C. The physicochemical phenomena responsible for Cu stabilization in the solid phase have been evaluated by EDTA sequential extractions and synchrotron radiation based X-ray microanalytical techniques. These techniques were used for the visualization of the spatial distribution and the speciation of Cu in and/or on the neo-formed zeolite particles. In particular, micro XRF (X-ray fluorescence) tomography showed direct evidence that Cu can be entrapped as clusters inside the porous zeolitic structures while,mu-XANES (X-ray absorption near edge structure) spectroscopy determinations revealed Cu to be present mainly as Cu(II) hydroxide and Cu(II) oxide. The reported results could be useful as a basic knowledge for planning new technologies for the on site physicochemical stabilization of heavy metals in heavily polluted soils.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.198
Times cited: 39
DOI: 10.1021/ES050079D
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“Microstructure characterization of oceanic polyethylene debris”. Rowenczyk L, Dazzi A, Deniset-Besseau A, Beltran V, Goudounèche D, Wong-Wah-Chung P, Boyron O, George M, Fabre P, Roux C, Mingotaud AF, ter Halle A, Environmental Science &, Technology 54, 4102 (2020). http://doi.org/10.1021/ACS.EST.9B07061
Abstract: Plastic pollution has become a worldwide concern. It was demonstrated that plastic breaks down to nanoscale particles in the environment, forming so-called nanoplastics. It is important to understand their ecological impact, but their structure is not elucidated. In this original work, we characterize the microstructure of oceanic polyethylene debris and compare it to the nonweathered objects. Cross sections are analyzed by several emergent mapping techniques. We highlight deep modifications of the debris within a layer a few hundred micrometers thick. The most intense modifications are macromolecule oxidation and a considerable decrease in the molecular weight. The adsorption of organic pollutants and trace metals is also confined to this outer layer. Fragmentation of the oxidized layer of the plastic debris is the most likely source of nanoplastics. Consequently the nanoplastic chemical nature differs greatly from plastics.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 11.4
Times cited: 3
DOI: 10.1021/ACS.EST.9B07061
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“Return-sludge treatment with endogenous free nitrous acid limits nitrate production and N₂O emission for mainstream partial nitritation/anammox”. Peng L, Xie Y, Van Beeck W, Zhu W, Van Tendeloo M, Tytgat T, Lebeer S, Vlaeminck SE, Environmental Science &, Technology 54, 5822 (2020). http://doi.org/10.1021/ACS.EST.9B06404
Abstract: Nitrite oxidizing bacteria (NOB) and nitrous oxide (N2O) hinder the development of mainstream partial nitritation/anammox. To overcome these, endogenous free ammonia (FA) and free nitrous acid (FNA), which can be produced in the sidestream, were used for return-sludge treatment for two integrated-film activated sludge reactors containing biomass in flocs and on carriers. The repeated exposure of biomass from one reactor to FA shocks had a limited impact on NOB suppression but inhibited anammox bacteria (AnAOB). In the other reactor, repeated FNA shocks to the separated flocs failed to limit the system’s nitrate production since NOB activity was still high on the biofilms attached to the unexposed carriers. In contrast, the repeated FNA treatment of flocs and carriers favored aerobic ammonium-oxidizing bacteria (AerAOB) over NOB activity with AnAOB negligibly affected. It was further revealed that return-sludge treatment with higher FNA levels led to lower N2O emissions under similar effluent nitrite concentrations. On this basis, weekly 4 h FNA shocks of 2.0 mg of HNO2-N/L were identified as an optimal and realistic treatment, which not only enabled nitrogen removal efficiencies of ∼65% at nitrogen removal rates of ∼130 mg of N/L/d (20 °C) but also yielded the lowest cost and carbon footprint.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 11.4
Times cited: 1
DOI: 10.1021/ACS.EST.9B06404
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“Synchrotron XRF analysis identifies cerium accumulation colocalized with pharyngeal deformities in CeO₂, NP-exposed caenorhabditis elegans”. Rossbach LM, Brede DA, Nuyts G, Cagno S, Olsson RMS, Oughton DH, Falkenberg G, Janssens K, Lind OC, Environmental science and technology 56, 5081 (2022). http://doi.org/10.1021/ACS.EST.1C08509
Abstract: A combination of synchrotron radiation-based elementalimaging, in vivo redox status analysis, histology, and toxic responses was usedto investigate the uptake, biodistribution, and adverse effects of Cenanoparticles (CeO2NP; 10 nm; 0.5-34.96 mg Ce L-1) or Ce(NO3)3(2.3-26 mg Ce L-1)inCaenorhabditis elegans. Elemental mapping of theexposed nematodes revealed Ce uptake in the alimentary canal prior todepuration. Retention of CeO2NPs was low compared to that of Ce(NO3)3in depurated individuals. X-rayfluorescence (XRF) mapping showed that Cetranslocation was confined to the pharyngeal valve and foregut. Ce(NO3)3exposure significantly decreased growth, fertility, and reproduction, causedslightly reduced fecundity. XRF mapping and histological analysis revealedsevere tissue deformities colocalized with retained Ce surrounding thepharyngeal valve. Both forms of Ce activated the sod-1 antioxidant defense,particularly in the pharynx, whereas no significant effects on the cellular redox balance were identified. The CeO2NP-induceddeformities did not appear to impair the pharyngeal function or feeding ability as growth effects were restricted to Ce(NO3)3exposure. The results demonstrate the utility of integrated submicron-resolution SR-based XRF elemental mapping of tissue-specificdistribution and adverse effect analysis to obtain robust toxicological evaluations of metal-containing contaminants.
Keywords: A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 11.4
DOI: 10.1021/ACS.EST.1C08509
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“Synchrotron XRF and histological analyses identify damage to digestive tract of uranium NP-exposed Daphnia magna”. Byrnes I, Rossbach LM, Jaroszewicz J, Grolimund D, Sanchez DF, Gomez-Gonzalez MA, Nuyts G, Reinoso-Maset E, Janssens K, Salbu B, Brede DA, Lind OC, Environmental science and technology 57, 1071 (2023). http://doi.org/10.1021/ACS.EST.2C07174
Abstract: Micro-and nanoscopic X-ray techniques were used to investigate the relationship between uranium (U) tissue distributions and adverse effects to the digestive tract of aquatic model organism Daphnia magna following uranium nanoparticle (UNP) exposure. X-ray absorption computed tomography measure-ments of intact daphnids exposed to sublethal concentrations of UNPs or a U reference solution (URef) showed adverse morphological changes to the midgut and the hepatic ceca. Histological analyses of exposed organisms revealed a high proportion of abnormal and irregularly shaped intestinal epithelial cells. Disruption of the hepatic ceca and midgut epithelial tissues implied digestive functions and intestinal barriers were compro-mised. Synchrotron-based micro X-ray fluorescence (XRF) elemental mapping identified U co-localized with morphological changes, with substantial accumulation of U in the lumen as well as in the epithelial tissues. Utilizing high-resolution nano-XRF, 400-1000 nm sized U particulates could be identified throughout the midgut and within hepatic ceca cells, coinciding with tissue damages. The results highlight disruption of intestinal function as an important mode of action of acute U toxicity in D. magna and that midgut epithelial cells as well as the hepatic ceca are key target organs.
Keywords: A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 11.4
DOI: 10.1021/ACS.EST.2C07174
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“Capture-ferment-upgrade : a three-step approach for the valorization of sewage organics as commodities”. Alloul A, Ganigue R, Spiller M, Meerburg F, Cagnetta C, Rabaey K, Vlaeminck SE, Environmental science and technology 52, 6729 (2018). http://doi.org/10.1021/ACS.EST.7B05712
Abstract: This critical review outlines a roadmap for the conversion of chemical oxygen demand (COD) contained in sewage to commodities based on three-steps: capture COD as sludge, ferment it to volatile fatty acids (VFA), and upgrade VFA to products. The article analyzes the state-of-the-art of this three step approach and discusses the bottlenecks and challenges. The potential of this approach is illustrated for the European Union's 28 member states (EU-28) through Monte Carlo simulations. High-rate contact stabilization captures the highest amount of COD (66-86 g COD person equivalent(-1) day(-1) in 60% of the iterations). Combined with thermal hydrolysis, this would lead to a VFA-yield of 23-44 g COD person equivalent(-1) day(-1). Upgrading VFA generated by the EU-28 would allow, in 60% of the simulations, for a yearly production of 0.2-2.0 megatonnes of esters, 0.7-1.4 megatonnes of polyhydroxyalkanoates or 0.6-2.2 megatonnes of microbial protein substituting, respectively, 20-273%, 70-140% or 21-72% of their global counterparts (i.e., petrochemical-based esters, bioplastics or fishmeal). From these flows, we conclude that sewage has a strong potential as biorefinery feedstock, although research is needed to enhance capture, fermentation and upgrading efficiencies. These developments need to be supported by economic/environmental analyses and policies that incentivize a more sustainable management of our resources.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1021/ACS.EST.7B05712
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“Determination of methanesulfonic acid and non-sea-salt sulfate in single marine aerosol particles”. Kolaitis LN, Bruynseels FJ, Van Grieken RE, Andreae MO, Environmental science and technology 23, 236 (1989). http://doi.org/10.1021/ES00179A018
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
DOI: 10.1021/ES00179A018
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