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End date: 2023 × Start date: 2020 × DDC: 540 × DDC: 660 × WGL Institute: IPF ×

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Now showing 1 - 10 of 21
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    Funktionalisierte Kern-Schale-Partikel als Träger zur Enzymimmobilisierung und deren Anwendung
    (Weinheim : Wiley-VCH Verl., 2020) Matura, Anke; Köpke, Dorina; Marschelke, Claudia; Kramer, Julius; Synytska, Alla; Sallat, Marco
    Mono- und bifunktionale hybride Kern-Schale-Partikel wurden für die Enzymimmobilisierung eingesetzt. An monofunktionalen Poly(2-dimethylamino)ethylmethacrylat-modifizierten Partikeln wurden die idealen Bedingungen für die Immobilisierung untersucht. Anschließend erfolgte die Übertragung auf bifunktionale Janus-Partikel-Systeme, mit denen gleichzeitig die schaltbare Abtrennung und der erneute Einsatz der Enzyme möglich waren. Abschließend wurde der mehrfache Einsatz der enzymbeladenen Partikel modellhaft am Beispiel der Prozesswasserentfärbung aus der Textilindustrie mit Laccase gezeigt und eine Kostenrechnung durchgeführt.
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    Freestanding Nanolayers of a Wide-Gap Topological Insulator through Liquid-Phase Exfoliation
    (Weinheim : Wiley-VCH, 2021) Lê Anh, Mai; Potapov, Pavel; Wolf, Daniel; Lubk, Axel; Glatz, Bernhard; Fery, Andreas; Doert, Thomas; Ruck, Michael
    The layered salt Bi14Rh3I9 is a weak three-dimensional (3D) topological insulator (TI), that is, a stack of two-dimensional (2D) TIs. It has a wide non-trivial band gap of 210 meV, which is generated by strong spin-orbit coupling, and possesses protected electronic edge-states. In the structure, charged layers of (Formula presented.) (Bi4Rh)3I]2+ honeycombs and (Formula presented.) Bi2I8]2− chains alternate. The non-trivial topology of Bi14Rh3I9 is an inherent property of the 2D intermetallic fragment. Here, the exfoliation of Bi14Rh3I9 was performed using two different chemical approaches: (a) through a reaction with n-butyllithium and poly(vinylpyrrolidone), (b) through a reaction with betaine in dimethylformamide at 55 °C. The former yielded few-layer sheets of the new compound Bi12Rh3I, while the latter led to crystalline sheets of Bi14Rh3I9 with a thickness down to 5 nm and edge-lengths up to several ten microns. X-ray diffraction and electron microscopy proved that the structure of Bi14Rh3I9 remained intact. Thus, it was assumed that the particles are still TIs. Dispersions of these flakes now allow for next steps towards the envisioned applications in nanoelectronics, such as the study of quantum coherence in deposited films, the combination with superconducting particles or films for the generation of Majorana fermions, or studies on their behavior under the influence of magnetic or electric fields or in contact with various materials occurring in devices. The method presented generally allows to exfoliate layers with high specific charges and thus the use of layered starting materials beyond van der Waals crystals. © 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH
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    Semi-Interpenetrating Polymer Networks Based on N-isopropylacrylamide and 2-acrylamido-2-methylpropane Sulfonic Acid for Intramolecular Force-Compensated Sensors
    (Bristol : IOP Publishing, 2021) Binder, Simon; Zschoche, Stefan; Voit, Brigitte; Gerlach, Gerald
    Stimulus-responsive hydrogels are swellable polymers that take up a specific volume depending on a measured variable present in solution. Hydrogel-based chemical sensors make use of this ability by converting the resulting swelling pressure, which depends on the measured variable, into an electrical value. Due to the tedious swelling processes, the measuring method of intramolecular force compensation is used to suppress these swelling processes and, thus, significantly increase the sensor's response time. However, intramolecular force compensation requires a bisensitive hydrogel. In addition to the sensitivity of the measured variable the gel has to provide a second sensitivity for intrinsic compensation of the swelling pressure. At the same time, this hydrogel has to meet further requirements, e.g. high compressive strength. Until now, interpenetrating polymer networks (IPN) have been used for such a force-compensatory effective hydrogel, which are complex to manufacture. In order to significantly simplify the sensor design and production, a simpler synthesis of the bisensitive hydrogel is desirable. This paper presents a new bisensitive hydrogel based on semi-interpenetrating polymer networks. It is based on a copolymer network consisting of N-isopropylacrylamide (NiPAAm) and 2-acrylamido-2-methylpropane sulfonic acid (AMPS) and long PAMPS strands that permeate it. Measurements show, that this hydrogel meets all essential requirements for intramolecular force compensation and is at the same time much easier to synthesize than previously used IPN hydrogels. © 2021 The Author(s).
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    Tailoring Magnetic Features in Zigzag-Edged Nanographenes by Controlled Diels–Alder Reactions
    (Weinheim : Wiley-VCH, 2020) Ajayakumar, M.R.; Fu, Yubin; Liu, Fupin; Komber, Hartmut; Tkachova, Valeriya; Xu, Chi; Zhou, Shengqiang; Popov, Alexey A.; Liu, Junzhi; Feng, Xinliang
    Nanographenes (NGs) with tunable electronic and magnetic properties have attracted enormous attention in the realm of carbon-based nanoelectronics. In particular, NGs with biradical character at the ground state are promising building units for molecular spintronics. However, most of the biradicaloids are susceptible to oxidation under ambient conditions and photolytic degradation, which hamper their further applications. Herein, we demonstrated the feasibility of tuning the magnetic properties of zigzag-edged NGs in order to enhance their stability via the controlled Diels–Alder reactions of peri-tetracene (4-PA). The unstable 4-PA (y0=0.72; half-life, t1/2=3 h) was transformed into the unprecedented benzo-peri-tetracenes (BPTs) by a one-side Diels–Alder reaction, which featured a biradical character at the ground state (y0=0.60) and exhibited remarkable stability under ambient conditions for several months. In addition, the fully zigzag-edged circumanthracenes (CAs) were achieved by two-fold or stepwise Diels–Alder reactions of 4-PA, in which the magnetic properties could be controlled by employing the corresponding dienophiles. Our work reported herein opens avenues for the synthesis of novel zigzag-edged NGs with tailor-made magnetic properties. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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    Examining the early stages of thermal oxidative degradation in epoxy-amine resins
    (Amsterdam [u.a.] : Elsevier Science, 2020) Morsch, Suzanne; Liu, Yanwen; Lyon, S.B.; Gibbon, S.R.; Gabriele, Benjamin; Malanin, Mikhail; Eichhorn, Klaus-Jochen
    Epoxy-amine resins continue to find widespread use as the binders in protective and decorative organic coatings, as the matrix in composite materials, and as adhesives. In service, exposure to the environment ultimately results in oxidative deterioration of these materials, limiting the performance lifetime. Defining this auto-oxidation process is therefore a key challenge in developing more durable high-performance materials. In this study, we investigate oxidative degradation of a model resin based on diglycidyl ether of bisphenol-A (DGEBA) and an aliphatic amine hardener, triethylenetetraamine (TETA). Using infrared spectroscopy, we find that prior to the expected detection of formate groups (corresponding to the well-known radical oxidation mechanism of DGEBA), a band at 1658 cm−1 forms, associated with amine cross-linker oxidation. Infrared microspectroscopy, in-situ heated ATR-infrared, Raman spectroscopy and AFM-IR techniques are thus employed to investigate the early stages of resin oxidation and demonstrate strong parallels between the initial stages of cured resin degradation and the auto-oxidation of TETA cross-linker molecules.
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    Dehydropolymerisation of Methylamine Borane and an N-Substituted Primary Amine Borane Using a PNP Fe Catalyst
    (Weinheim : Wiley-VCH, 2020) Anke, Felix; Boye, Susanne; Spannenberg, Anke; Lederer, Albena; Heller, Detlef; Beweries, Torsten
    Dehydropolymerisation of methylamine borane (H3B⋅NMeH2) using the well-known iron amido complex [(PNP)Fe(H)(CO)] (PNP=N(CH2CH2PiPr2)2) (1) gives poly(aminoborane)s by a chain-growth mechanism. In toluene, rapid dehydrogenation of H3B⋅NMeH2 following first-order behaviour as a limiting case of a more general underlying Michaelis–Menten kinetics is observed, forming aminoborane H2B=NMeH, which selectively couples to give high-molecular-weight poly(aminoborane)s (H2BNMeH)n and only traces of borazine (HBNMe)3 by depolymerisation after full conversion. Based on a series of comparative experiments using structurally related Fe catalysts and dimethylamine borane (H3B⋅NMe2H) polymer formation is proposed to occur by nucleophilic chain growth as reported earlier computationally and experimentally. A silyl functionalised primary borane H3B⋅N(CH2SiMe3)H2 was studied in homo- and co-dehydropolymerisation reactions to give the first examples for Si containing poly(aminoborane)s. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
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    Synthesis and characterization of poly(1,2,3-triazole)s with inherent high sulfur content for optical applications
    (Hoboken, NJ : Wiley, 2023) Mazumder, Kajari; Komber, Hartmut; Bittrich, Eva; Voit, Brigitte; Banerjee, Susanta
    The synthesis of solution-processable sulfur-containing polytriazoles for optoelectronic applications is a relatively less explored domain in polymer research. The synthesis of novel bifunctional (DA) and trifunctional (TA) azido-monomers with inherent high sulfur content and of organo-soluble high refractive index poly(1,2,3-triazole)s using the azido-monomers via Cu(I) assisted click polymerization reactions are reported in this work. The azido-monomers were synthesized by the conversion of previously reported amine-functionalized compounds to azides using azidotrimethylsilane in a polar aprotic solvent. Dialkyne monomers were also synthesized and reacted with the azides to prepare a series of five linear and two hyperbranched poly(1,2,3-triazole)s. Fourier transform infrared spectroscopy, nuclear magnetic resonance spectroscopy, differential scanning calorimetry and thermogravimetric analysis were used to characterize the synthesized polymers. It was also demonstrated that the use of the trifunctional azide in optimized conditions resulted in increased solubility of an otherwise insoluble linear poly(1,2,3-triazole). The optical characterization of the polymers was carried out on thin polymer films with thickness in the nanometer range, which were successfully prepared by spin-coating on silicon wafers. It was found that the increase in the sulfur and aromatic content in the polymer backbone successfully increased the refractive index of the polymers up to 1.743 at 589 nm.
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    Bioinspired Polydopamine Coating as an Adhesion Enhancer Between Paraffin Microcapsules and an Epoxy Matrix
    (Washington, DC : ACS Publications, 2020) Fredi, Giulia; Simon, Frank; Sychev, Dmitrii; Melnyk, Inga; Janke, Andreas; Scheffler, Christina; Zimmerer, Cordelia
    Microencapsulated phase change materials (PCMs) are attracting increasing attention as functional fillers in polymer matrices, to produce smart thermoregulating composites for applications in thermal energy storage (TES) and thermal management. In a polymer composite, the filler–matrix interfacial adhesion plays a fundamental role in the thermomechanical properties. Hence, this work aims to modify the surface of commercial PCM microcapsules through the formation of a layer of polydopamine (PDA), a bioinspired polymer that is emerging as a powerful tool to functionalize chemically inert surfaces due to its versatility and great adhesive potential in many different materials. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) evidenced that after PDA coating, the surface roughness increased from 9 to 86 nm, which is beneficial, as it allows a further increase in the interfacial interaction by mechanical interlocking. Spectroscopic techniques allowed investigating the surface chemistry and identifying reactive functional groups of the PDA layer and highlighted that, unlike the uncoated microcapsules, the PDA layer is able to react with oxirane groups, thereby forming a covalent bond with the epoxy matrix. Hot-stage optical microscopy and differential scanning calorimetry (DSC) highlighted that the PDA modification does not hinder the melting/crystallization process of the paraffinic core. Finally, SEM micrographs of the cryofracture surface of epoxy composites containing neat or PDA-modified microcapsules clearly evidenced improved adhesion between the capsule shell and the epoxy matrix. These results showed that PDA is a suitable coating material with considerable potential for increasing the interfacial adhesion between an epoxy matrix and polymer microcapsules with low surface reactivity. This is remarkably important not only for this specific application but also for other classes of composite materials. Future studies will investigate how the deposition parameters affect the morphology, roughness, and thickness of the PDA layer and how the layer properties influence the capsule–matrix adhesion.
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    DNAzymes as Catalysts for l-Tyrosine and Amyloid β Oxidation
    (Washington, DC : ACS Publications, 2020) Köhler, Tony; Patsis, Panagiotis A.; Hahn, Dominik; Ruland, André; Naas, Carolin; Müller, Martin; Thiele, Julian
    Single-stranded deoxyribonucleic acids have an enormous potential for catalysis by applying tailored sequences of nucleotides for individual reaction conditions and substrates. If such a sequence is guanine-rich, it may arrange into a three-dimensional structure called G-quadruplex and give rise to a catalytically active DNA molecule, a DNAzyme, upon addition of hemin. Here, we present a DNAzyme-mediated reaction, which is the oxidation of l-tyrosine toward dityrosine by hydrogen peroxide. With an optimal stoichiometry between DNA and hemin of 1:10, we report an activity of 101.2 ± 3.5 μUnits (μU) of the artificial DNAzyme Dz-00 compared to 33.0 ± 1.8 μU of free hemin. Exemplarily, DNAzymes may take part in neurodegeneration caused by amyloid beta (Aβ) aggregation due to l-tyrosine oxidation. We show that the natural, human genome-derived DNAzyme In1-sp is able to oxidize Aβ peptides with a 4.6% higher yield and a 33.3% higher velocity of the reaction compared to free hemin. As the artificial DNAzyme Dz-00 is even able to catalyze Aβ peptide oxidation with a 64.2% higher yield and 337.1% higher velocity, an in-depth screening of human genome-derived DNAzymes may identify further candidates with similarly high catalytic activity in Aβ peptide oxidation.
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    The role of winding pattern on filament wound composite cylinders under radial compression
    (Brookfield, Conn. : Society of Plastic Engineers, 2020) Lisbôa, Tales V.; Almeida Jr, José Humberto S.; Dalibor, Ingo H.; Spickenheuer, Axel; Marczak, Rogério J.; Amico, Sandro C.
    Filament wound (FW) structures present a geometric characteristic in their helical layers: the winding pattern. The pattern, however, is usually disregarded in conventional experimental or numerical approaches even though it can affect the behavior of FW structures, and most studies that account for the pattern are only theoretical. This study aims at deepening the understanding of pattern effects via a comprehensive experimental campaign focusing on composites cylinders under radial compression. Ten winding patterns were considered, from 1 to 10 units along the circumferential direction. Strength, stiffness, absorbed energy and failure mechanisms were evaluated. The results show that the pattern may have a strong influence on both maximum bearing load and absorbed energy, whereas stiffness is less affected.