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- ItemAddressing the Reproducibility of Photocatalytic Carbon Dioxide Reduction(Weinheim : Wiley-VCH Verlag, 2019) Marx, Maximilian; Mele, Andrea; Spannenberg, Anke; Steinlechner, Christoph; Junge, Henrik; Schollhammer, Philippe; Beller, MatthiasReproducibility of photocatalytic reactions, especially when conducted on small scale for improved turnover numbers with in situ formed catalysts can prove challenging. Herein, we showcase the problematic reproducibility on the example of attractive photocatalytic CO2 reduction utilizing [FeFe] hydrogenase mimics. These Fe complexes, well-known for their application in proton reduction reactions, were combined with a heteroleptic Cu photosensitizer and produced CO/H2/HCO2H mixtures of variable constitution. However, the reactions indicated a poor reproducibility, even when conducted with well-defined complexes. Based on our experience, we make suggestions for scientists working in the field of photocatalysis on how to address and report the reproducibility of novel photocatalytic reaction protocols. In addition, we would like to highlight the importance of studying reproducibility of novel reaction protocols, especially in the fields of photocatalytic water splitting and CO2 reduction, where TONs are widely used as the comparable measure for catalytic activity. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemAerobic iron-catalyzed site-selective C(sp3)–C(sp3) bond cleavage in N-heterocycles(Amsterdam : Elsevier, 2021) Leonard, David K.; Li, Wu; Rockstroh, Nils; Junge, Kathrin; Beller, MatthiasThe kinetic and thermodynamic stability of C(sp3)–C(sp3) bonds makes the site-selective activation of these motifs a real synthetic challenge. In view of this, herein a site-selective method of C(sp3)–C(sp3) bond scission of amines, specifically morpholine and piperazine derivatives, using a cheap iron catalyst and air as a sustainable oxidant is reported. Furthermore, a statistical design of experiments (DoE) is used to evaluate multiple reaction parameters thereby allowing for the rapid development of a catalytic process. © 2021
- ItemDecomposition of methane over alumina supported Fe and Ni–Fe bimetallic catalyst: Effect of preparation procedure and calcination temperature(Amsterdam [u.a.] : Elsevier, 2016) Al-Fatesh, A.S.; Fakeeha, A.H.; Ibrahim, A.A.; Khan, W.U.; Atia, H.; Eckelt, R.; Seshan, K.; Chowdhury, B.Catalytic decomposition of methane has been studied extensively as the production of hydrogen and formation of carbon nanotube is proven crucial from the scientific and technological point of view. In that context, variation of catalyst preparation procedure, calcination temperature and use of promoters could significantly alter the methane conversion, hydrogen yield and morphology of carbon nanotubes formed after the reaction. In this work, Ni promoted and unpromoted Fe/Al2O3 catalysts have been prepared by impregnation, sol–gel and co-precipitation method with calcination at two different temperatures. The catalysts were characterized by X-ray diffraction (XRD), N2 physisorption, temperature programmed reduction (TPR) and thermogravimetric analysis (TGA) techniques. The catalytic activity was tested for methane decomposition reaction. The catalytic activity was high when calcined at 500 °C temperature irrespective of the preparation method. However while calcined at high temperature the catalyst prepared by impregnation method showed a high activity. It is found from XRD and TPR characterization that disordered iron oxides supported on alumina play an important role for dissociative chemisorptions of methane generating molecular hydrogen. The transmission electron microscope technique results of the spent catalysts showed the formation of carbon nanotube which is having length of 32–34 nm. The Fe nanoparticles are present on the tip of the carbon nanotube and nanotube grows by contraction–elongation mechanism. Among three different methodologies impregnation method was more effective to generate adequate active sites in the catalyst surface. The Ni promotion enhances the reducibility of Fe/Al2O3 oxides showing a higher catalytic activity. The catalyst is stable up to six hours on stream as observed in the activity results.
- ItemInter-granular effects at high magnetic fields of cuprate and iron chalcogenide superconducting materials(Bristol : Institute of Physics Publishing, 2019) Buchkov, K.; Valkovski, M.; Gajda, D.; Nenkov, K.; Nazarova, E.The weak links effects are one of the main challenges for effective power applications of high temperature superconducting materials. Studies of these effects help for their better understanding and subsequent improvement. An overview analysis of the intergranular properties of cuprate (Y0.8Ca0.2Ba2Cu3O7-δ) and iron-based chalcogenide (FeSe0.5Te0.5) polycrystalline samples was carried out, by means of series of electro-transport experiments at different magnetic fields. The temperature evolution of the Josephson coupling and intrinsic superconductivity effects for the both systems was constructed. The FeSe0.5Te0.5 compound shows very stable and superior behavior compared to Y0.8Ca0.2BCO up to the highest magnetic fields (14T) used. We have explored FeSe0.5Te0.5 Josephson weak links influence (as a non-linear process) over the resistive transition using different AC current amplitudes and applying the sensitive AC transport third harmonics technique.
- ItemIron-assisted ion beam patterning of Si(001) in the crystalline regime(Bristol : IOP, 2012) Macko, S.; Grenzer, J.; Frost, F.; Engler, M.; Hirsch, D.; Fritzsche, M.; Mücklich, A.; Michely, T.We present ion beam erosion experiments on Si(001) with simultaneous sputter co-deposition of steel at 660 K. At this temperature, the sample remains within the crystalline regime during ion exposure and pattern formation takes place by phase separation of Si and iron-silicide. After an ion fluence of F ≈ 5.9×10 21 ions m -2, investigations by atomic force microscopy and scanning electron microscopy identify sponge, segmented wall and pillar patterns with high aspect ratios and heights of up to 200 nm. Grazing incidence x-ray diffraction and transmission electron microscopy reveal the structures to be composed of polycrystalline iron-silicide. The observed pattern formation is compared to that in the range of 140-440K under otherwise identical conditions, where a thin amorphous layer forms due to ion bombardment.
- ItemSoil conditions and the iron chlorosis of mature vine(London [u.a.] : Institute of Physics, 2019) Yutsis, A.E.; Zhelezova, S.V.; Dammer, K.-H.Iron-deficiency chlorosis is a usual routine problem on calcareous carbonated soils of Crimea. Different reasons cause vine chlorosis: soil properties, physiological status of plants and others. It was shown that chlorosis spot in the vineyard has constant location. Chlorosis can be identified visually and instrumentally. In this study, an attempt was made to find the relationship between soil electrical resistance and the spread of vine chlorosis.
- ItemReducing conditions favor magnetosome production in magnetospirillum magneticum AMB-1(Lausanne : Frontiers Media, 2019) Olszewska-Widdrat, Agata; Schiro, Gabriele; Reichel, Victoria E.; Faivre, DamienMagnetotactic bacteria (MTB) are a heterogeneous group of Gram-negative prokaryotes, which all produce special magnetic organelles called magnetosomes. The magnetosome consists of a magnetic nanoparticle, either magnetite (Fe3O4) or greigite (Fe3S4), embedded in a membrane, which renders the systems colloidaly stable, a desirable property for biotechnological applications. Although these bacteria are able to regulate the formation of magnetosomes through a biologically-controlled mechanism, the environment in general and the physico-chemical conditions surrounding the cells in particular also influence biomineralization. This work thus aims at understanding how such external conditions, in particular the extracellular oxidation reduction potential, influence magnetite formation in the strain Magnetospirillum magneticum AMB-1. Controlled cultivation of the microorganisms was performed at different redox potential in a bioreactor and the formation of magnetosomes was assessed by microscopic and spectroscopic techniques. Our results show that the formation of magnetosomes is inhibited at the highest potential tested (0 mV), whereas biomineralization is facilitated under reduced conditions (-500 mV). This result improves the understanding of the biomineralization process in MTB and provides useful information in sight of a large scale production of magnetosomes for different applications. © 2019 Olszewska-Widdrat, Schiro, Reichel and Faivre.
- ItemHydraulic characterisation of iron-oxide-coated sand and gravel based on nuclear magnetic resonance relaxation mode analyses(Munich : EGU, 2018) Costabel, Stephan; Weidner, Christoph; Müller-Petke, Mike; Houben, GeorgThe capability of nuclear magnetic resonance (NMR) relaxometry to characterise hydraulic properties of iron-oxide-coated sand and gravel was evaluated in a laboratory study. Past studies have shown that the presence of paramagnetic iron oxides and large pores in coarse sand and gravel disturbs the otherwise linear relationship between relaxation time and pore size. Consequently, the commonly applied empirical approaches fail when deriving hydraulic quantities from NMR parameters. Recent research demonstrates that higher relaxation modes must be taken into account to relate the size of a large pore to its NMR relaxation behaviour in the presence of significant paramagnetic impurities at its pore wall. We performed NMR relaxation experiments with water-saturated natural and reworked sands and gravels, coated with natural and synthetic ferric oxides (goethite, ferrihydrite), and show that the impact of the higher relaxation modes increases significantly with increasing iron content. Since the investigated materials exhibit narrow pore size distributions, and can thus be described by a virtual bundle of capillaries with identical apparent pore radius, recently presented inversion approaches allow for estimation of a unique solution yielding the apparent capillary radius from the NMR data. We found the NMR-based apparent radii to correspond well to the effective hydraulic radii estimated from the grain size distributions of the samples for the entire range of observed iron contents. Consequently, they can be used to estimate the hydraulic conductivity using the well-known Kozeny–Carman equation without any calibration that is otherwise necessary when predicting hydraulic conductivities from NMR data. Our future research will focus on the development of relaxation time models that consider pore size distributions. Furthermore, we plan to establish a measurement system based on borehole NMR for localising iron clogging and controlling its remediation in the gravel pack of groundwater wells.
- ItemMechanisms of stress generation and relaxation during pulsed laser deposition of epitaxial Fe-Pd magnetic shape memory alloy films on MgO(Milton Park : Taylor & Francis, 2008) Edler, Tobias; Buschbeck, Jörg; Mickel, Christine; Fähler, Sebastian; Mayr, S.G.Mechanical stress generation during epitaxial growth of Fe–Pd thin films on MgO from pulsed laser deposition is a key parameter for the suitability in shape memory applications. By employing in situ substrate curvature measurements, we determine the stress states as a function of film thickness and composition. Depending on composition, different stress states are observed during initial film growth, which can be attributed to different misfits. Compressive stress generation by atomic peening is observed in the later stages of growth. Comparison with ex situ x-ray based strain measurements allows integral and local stress to be distinguished and yields heterogeneities of the stress state between coherent and incoherent regions. In combination with cross-sectional TEM measurements the relevant stress relaxation mechanism is identified to be stress-induced martensite formation with (111) twinning.
- ItemMagnetization Dynamics of an Individual Single-Crystalline Fe-Filled Carbon Nanotube(Weinheim : Wiley-VCH, 2019) Lenz, Kilian; Narkowicz, Ryszard; Wagner, Kai; Reiche, Christopher F.; Körner, Julia; Schneider, Tobias; Kákay, Attila; Schultheiss, Helmut; Weissker, Uhland; Wolf, Daniel; Suter, Dieter; Büchner, Bernd; Fassbender, Jürgen; Mühl, Thomas; Lindner, JürgenThe magnetization dynamics of individual Fe-filled multiwall carbon-nanotubes (FeCNT), grown by chemical vapor deposition, are investigated by microresonator ferromagnetic resonance (FMR) and Brillouin light scattering (BLS) microscopy and corroborated by micromagnetic simulations. Currently, only static magnetometry measurements are available. They suggest that the FeCNTs consist of a single-crystalline Fe nanowire throughout the length. The number and structure of the FMR lines and the abrupt decay of the spin-wave transport seen in BLS indicate, however, that the Fe filling is not a single straight piece along the length. Therefore, a stepwise cutting procedure is applied in order to investigate the evolution of the ferromagnetic resonance lines as a function of the nanowire length. The results show that the FeCNT is indeed not homogeneous along the full length but is built from 300 to 400 nm long single-crystalline segments. These segments consist of magnetically high quality Fe nanowires with almost the bulk values of Fe and with a similar small damping in relation to thin films, promoting FeCNTs as appealing candidates for spin-wave transport in magnonic applications. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim