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- ItemSelf-Activation of Inorganic-Organic Hybrids Derived through Continuous Synthesis of Polyoxomolybdate and para-Phenylenediamine Enables Very High Lithium-Ion Storage Capacity(Weinheim : Wiley-VCH, 2023) Mohamed, Mana Abdirahman; Arnold, Stefanie; Janka, Oliver; Quade, Antje; Presser, Volker; Kickelbick, GuidoInorganic-organic hybrid materials with redox-active components were prepared by an aqueous precipitation reaction of ammonium heptamolybdate (AHM) with para-phenylenediamine (PPD). A scalable and low-energy continuous wet chemical synthesis process, known as the microjet process, was used to prepare particles with large surface area in the submicrometer range with high purity and reproducibility on a large scale. Two different crystalline hybrid products were formed depending on the ratio of molybdate to organic ligand and pH. A ratio of para-phenylenediamine to ammonium heptamolybdate from 1 : 1 to 5 : 1 resulted in the compound [C6H10N2]2[Mo8O26] ⋅ 6 H2O, while higher PPD ratios from 9 : 1 to 30 : 1 yielded a composition of [C6H9N2]4[NH4]2[Mo7O24] ⋅ 3 H2O. The electrochemical behavior of the two products was tested in a battery cell environment. Only the second of the two hybrid materials showed an exceptionally high capacity of 1084 mAh g−1 at 100 mA g−1 after 150 cycles. The maximum capacity was reached after an induction phase, which can be explained by a combination of a conversion reaction with lithium to Li2MoO4 and an additional in situ polymerization of PPD. The final hybrid material is a promising material for lithium-ion battery (LIB) applications.
- ItemHighly active heterogeneous hydrogenation catalysts prepared from cobalt complexes and rice husk waste(London : RSC Publ., 2022) Unglaube, Felix; Schlapp, Janina; Quade, Antje; Schäfer, Jan; MejÃa, EstebanThe utilization and valorization of agricultural waste is a key strategy for the implementation of a sustainable economy to lessen the environmental footprint of human activities on Earth. This work describes the use of rice husk (RH) from agricultural waste to prepare a highly active catalyst for the reduction of nitro compounds. RH was impregnated with various cobalt complexes bearing N-donor ligands, then pyrolyzed and the resulting composite was etched with a base to remove the silica domains. The composition and morphology of the prepared materials were investigated by IR, AAS, ICP-OES, XRD, BET, XPS and SEM technics. The material showed excellent activity and selectivity in the hydrogenation of nitro groups in aromatic and aliphatic substrates. A remarkable selectivity towards nitro groups was found in the presence of various reactive functionalities, including halogens, carbonyls, borates, and nitriles. Apart from their excellent activity and selectivity, these catalysts showed remarkable stability, allowing their easy recovery and multiple reuse without requiring re-activation.
- ItemOxidative Esterification of 5-Hydroxymethylfurfural under Flow Conditions Using a Bimetallic Co/Ru Catalyst(Weinheim : Wiley-VCH Verlag, 2020) Salazar, Abel; Linke, Alexander; Eckelt, Reinhard; Quade, Antje; Kragl, Udo; MejÃa, EstebanFuranic di-carboxylate derivatives of 5-Hydroxymethylfurfural (HMF) are nowadays important in the polymer industry as they are used as building blocks for bio-based polyesters. The high reactivity of HMF compels to avoid harsh synthetic conditions. Therefore, developing mild catalytic processes for its selective oxidation is a challenging task. Herein, we report the first oxidative esterification of HMF to dimethyl furan-2,5-dicarboxylate (FDCM) under flow conditions using oxygen as oxidant. For that purpose, a new series of nitrogen-doped carbon-supported bimetallic Co/Ru heterogeneous catalysts were prepared and characterized by XRD, XPS and N2 physisorption. These analyses revealed that the porosity of the materials and order of impregnation of the metals to the carbon supports lead to varying catalytic activities. Under optimized conditions the flow reactor showed a 15-fold increase on the production of FDCM compared to batch conditions. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemVanadia–titania multilayer nanodecoration of carbon onions via atomic layer deposition for high performance electrochemical energy storage(Cambridge : Royal Society of Chemistry, 2016) Fleischamann, Simon; Tolosa, Aura; Zieger, Marco; Krüner, Benjamin; Peter, Nicolas J.; Grobelsek, Ingrid; Quade, Antje; Kruth, Angela; Presser, VolkerAtomic layer deposition has proven to be a particularly attractive approach for ecorating mesoporous carbon substrates with redox active metal oxides for lectrochemical energy storage. This study, for the first time, capitalizes on the cyclic character of atomic layer deposition to obtain highly conformal and atomically controlled decoration of carbon onions with alternating stacks of vanadia and titania. The addition of 25 mass% TiO2 leads to expansion of the VO2 unit cell, thus greatly enhancing lithium intercalation capacity and kinetics. Electrochemical characterization revealed an ultrahigh discharge capacity of up to 382 mA h g^-1 of the composite electrode (554 mA h g^-1 per metal oxide) with an impressive capacity retention of 82 mA h g^-1 (120 mA h g^-1 per metal oxide) at a high discharge rate of 20 A g^-1 or 52C. Stability benchmarking showed stability over 3000 cycles when discharging to a reduced potential of ^-1.8 V vs. carbon. These capacity values are among the highest reported for any metal oxide system, while in addition, upercapacitor-like power performance and longevity are achieved. At a device level, high specific energy and power of up to 110 W h kg^-1 and 6 kW kg^-1, respectively, were achieved when employing the hybrid material as anode versus activated carbon cathode.
- ItemHelixJet: An innovative plasma source for next-generation additive manufacturing (3D printing)(Hoboken, NJ : Wiley Interscience, 2020) Schäfer, Jan; Quade, Antje; Abrams, Kerry J.; Sigeneger, Florian; Becker, Markus M.; Majewski, Candice; Rodenburg, CorneliaA novel plasma source (HelixJet) for use in additive manufacturing (AM)/3D printing is proposed. The HelixJet is a capacitively coupled radio frequency plasma with a double-helix electrode configuration that generates a surprisingly stable and homogeneous glow plasma at low flow rates of argon and its mixtures at atmospheric pressure. The HelixJet was tested on three polyamide powders usually used to produce parts by laser sintering, a powder-based AM process, to form local deposits. The chemical composition of such plasma-printed samples is compared with thermally produced and laser-sintered samples with respect to differences in morphology that result from the different thermal cycles on several length scales. Plasma prints exhibit unique features attributable to the nonequilibrium chemistry and to the high-speed heat exchange.
- ItemContinuous wet chemical synthesis of Mo(C,N,O)x as anode materials for Li-ion batteries(London [u.a.] : RSC, 2023) Abdirahman Mohamed, Mana; Arnold, Stefanie; Janka, Oliver; Quade, Antje; Schmauch, Jörg; Presser, Volker; Kickelbick, GuidoMolybdenum carbides, oxides, and mixed anionic carbide–nitride–oxides Mo(C,N,O)x are potential anode materials for lithium-ion batteries. Here we present the preparation of hybrid inorganic–organic precursors by a precipitation reaction of ammonium heptamolybdate ((NH4)6Mo7O24) with para-phenylenediamine in a continuous wet chemical process known as a microjet reactor. The mixing ratio of the two components has a crucial influence on the chemical composition of the obtained material. Pyrolysis of the precipitated precursor compounds preserved the size and morphology of the micro- to nanometer-sized starting materials. Changes in pyrolysis conditions such as temperature and time resulted in variations of the final compositions of the products, which consisted of mixtures of Mo(C,N,O)x, MoO2, Mo2C, Mo2N, and Mo. We optimized the reaction conditions to obtain carbide-rich phases. When evaluated as an anode material for application in lithium-ion battery half-cells, one of the optimized materials shows a remarkably high capacity of 933 mA h g−1 after 500 cycles. The maximum capacity is reached after an activation process caused by various conversion reactions with lithium.
- ItemX-ray Ptychographic Imaging and Spectroscopic Studies of Plasma-Treated Plastic Films(Basel : MDPI, 2022) Ravandeh, Mehdi; Mehrjoo, Masoud; Kharitonov, Konstantin; Schäfer, Jan; Quade, Antje; Honnorat, Bruno; Ruiz-Lopez, Mabel; Keitel, Barbara; Kreis, Svea; Pan, Rui; Gang, Seung-gi; Wende, Kristian; Plönjes, ElkePolyethylene terephthalate (PET) is a thermoplastic polyester with numerous applications in industry. However, it requires surface modification on an industrial scale for printing and coating processes and plasma treatment is one of the most commonly used techniques to increase the hydrophilicity of the PET films. Systematic improvement of the surface modification by adaption of the plasma process can be aided by a comprehensive understanding of the surface morphology and chemistry. However, imaging large surface areas (tens of microns) with a resolution that allows understanding the surface quality and modification is challenging. As a proof-of-principle, plasma-treated PET films were used to demonstrate the capabilities of X-ray ptychography, currently under development at the soft X-ray free-electron laser FLASH at DESY, for imaging macroscopic samples. In combination with scanning electron microscopy (SEM), this new technique was used to study the effects of different plasma treatment processes on PET plastic films. The studies on the surface morphology were complemented by investigations of the surface chemistry using X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR). While both imaging techniques consistently showed an increase in roughness and change in morphology of the PET films after plasma treatment, X-ray ptychography can provide additional information on the three-dimensional morphology of the surface. At the same time, the chemical analysis shows an increase in the oxygen content and polarity of the surface without significant damage to the polymer, which is important for printing and coating processes.
- ItemA novel characterisation approach to reveal the mechano-chemical effects of oxidation and dynamic distension on polypropylene surgical mesh(London : RSC Publishing, 2021) Farr, Nicholas T. H.; Roman, Sabiniano; Schäfer, Jan; Quade, Antje; Lester, Daniel; Hearnden, Vanessa; MacNeil, Sheila; Rodenburg, CorneliaPolypropylene (PP) surgical mesh, used successfully for the surgical repair of abdominal hernias, is associated with serious clinical complications when used in the pelvic floor for repair of stress urinary incontinence or support of pelvic organ prolapse. While manufacturers claim that the material is inert and non-degradable, there is a growing body of evidence that asserts PP fibres are subject to oxidative damage and indeed explanted material from patients suffering with clinical complications has shown some evidence of fibre cracking and oxidation. It has been proposed that a pathological cellular response to the surgical mesh contributes to the medical complications; however, the mechanisms that trigger the specific host response against the material are not well understood. Specifically, this study was constructed to investigate the mechano-chemical effects of oxidation and dynamic distension on polypropylene surgical mesh. To do this we used a novel advanced spectroscopical characterisation technique, secondary electron hyperspectral imaging (SEHI), which is based on the collection of secondary electron emission spectra in a scanning electron microscope (SEM) to reveal mechanical-chemical reactions within PP meshes. This journal is
- ItemSimultaneous Treatment of Both Sides of the Polymer with a Conical-Shaped Atmospheric Pressure Plasma Jet(Basel : MDPI, 2023) Kodaira, Felipe Vicente de Paula; Leal, Bruno Henrique Silva; Tavares, Thayna Fernandes; Quade, Antje; Hein, Luis Rogerio de Oliveira; Chiappim, William; Kostov, Konstantin GeorgievA conical-shaped atmospheric pressure plasma jet (CS-APPJ) was developed to overcome a standard limitation of APPJs, which is their small treatment area. The CS-APPJs increase the treatment area but use the same gas flow. In the present work, polypropylene samples were treated by CS-APPJ and characterized by scanning electron microscope (SEM), the contact angle, Fourier-transformed infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). It was observed that the treatment co-occurs on the face directly in contact with the plasma and on the opposite face (OF) of the samples, i.e., no contact. However, the treatment changed the chemical composition on each side; the OF is rougher than the direct contact face (DCF), probably due to the oxygen groups in excess at the DCF and nitrogen in quantity at the OF. Although simultaneous treatment of both sides of the sample occurs for most atmospheric plasma treatments, this phenomenon is not explored in the literature.
- ItemDifferent Radial Modification Profiles Observed on APPJ-Treated Polypropylene Surfaces according to the Distance between Plasma Outlet and Target(Basel : MDPI, 2022) do Nascimento, Fellype; Silva Leal, Bruno; Quade, Antje; Kostov, Konstantin GeorgievThe plasma jet transfer technique relies on a conductive wire at floating potential, which, upon entering in contact with a primary discharge, is capable of igniting a small plasma plume at the distal end of a long flexible plastic tube. In this work, two different long tube configurations were employed for the surface modification of polypropylene (PP) samples using argon as the working gas. One of the jet configurations has a thin copper (Cu) wire, which was installed inside the long tube. In the other configuration, the floating electrode is a metallic mesh placed between two plastic tubes in a coaxial arrangement. In the first case, the tip of the Cu wire is in direct contact with the working gas at the plasma outlet, whereas, in the second, the inner plastic tube provides an additional dielectric barrier that prevents the conductor from being in contact with the gas. Water contact angle (WCA) measurements on treated PP samples revealed that different surface modification radial profiles are formed when the distance (d) between the plasma outlet and target is changed. Moreover, it was found that the highest WCA reduction does not always occur at the point where the plasma impinges the surface of the material, especially when the d value is small. Through X-ray photoelectron spectroscopy (XPS) analysis, it was confirmed that the WCA values are directly linked to the oxygen-functional groups formed on the PP surfaces after the plasma treatment. An analysis of the WCA measurements along the surface, as well as their temporal evolution, together with the XPS data, suggest that, when the treatment is performed at small d values, the plasma jet removes some functional groups at the point where the plasma hits the surface, thus leading to peculiar WCA profiles.