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- ItemEnergy-dependent dielectric tensor axes in monoclinic α-3,4,9,10-perylene tetracarboxylic dianhydride(Amsterdam [u.a.] : Elsevier, 2023) Alonso, M.I.; Garriga, M.; Ossó, J.O.; Schreiber, F.; Scholz, R.We have determined the complex dielectric tensor of single crystalline 3,4,9,10-perylene tetracarboxylic dianhydride (α-PTCDA) as a function of energy in the range between 1.4 and 5.0 eV. The results obtained reflect the monoclinic symmetry of the crystal: The principal axes of the real and the imaginary part of the tensor in general do not coincide and show chromatic dispersion. Monoclinic behavior allows rotation of the components ɛX and ɛZ in the plane perpendicular to the unique symmetry axis Y. The experimental results indicate that the energies of the optical transitions observed in the weak ɛX component coincide with energies in which a resonance effect due to coupling with the stronger ɛZ component occurs. These resonances appear at energies close to electronic excitations such as the optical gap, the transport gap and the highest occupied molecular orbital–lowest unoccupied molecular orbital (HOMO–LUMO) peak-to-peak gap and their assignments are discussed based on theoretical calculations.
- ItemGreen hydrogen from anion exchange membrane water electrolysis: A review of recent developments in critical materials and operating conditions(Cambridge : Royal Society of Chemistry, 2020) Miller, Hamish Andrew; Bouzek, Karel; Hnat, Jaromir; Loos, Stefan; Bernäcker, Christian Immanuel; Weißgärber, Thomas; Röntzsch, Lars; Meier-Haack, JochenHydrogen production using water electrolysers equipped with an anion exchange membrane (AEM), a pure water feed and cheap components such as platinum group metal-free catalysts and stainless steel bipolar plates (BPP) can challenge proton exchange membrane (PEM) electrolysis systems as the state of the art. For this to happen the performance of the AEM electrolyzer must match the compact design, stability, H2purity and high current densities of PEM systems. Current research aims at bringing AEM water electrolysis technology to an advanced level in terms of electrolysis cell performance. Such technological advances must be accompanied by demonstration of the cost advantages of AEM systems. The current state of the art in AEM water electrolysis is defined by sporadic reports in the academic literature mostly dealing with catalyst or membrane development. The development of this technology requires a future roadmap for systematic development and commercialization of AEM systems and components. This will include basic and applied research, technology development & integration, and testing at a laboratory scale of small demonstration units (AEM electrolyzer shortstacks) that can be used to validate the technology (from TRL 2-3 currently to TRL 4-5). This review paper gathers together recent important research in critical materials development (catalysts, membranes and MEAs) and operating conditions (electrolyte composition, cell temperature, performance achievements). The aim of this review is to identify the current level of materials development and where improvements are required in order to demonstrate the feasibility of the technology. Once the challenges of materials development are overcome, AEM water electrolysis can drive the future use of hydrogen as an energy storage vector on a large scale (GW) especially in developing countries. © The Royal Society of Chemistry 2020.
- ItemSemi-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, GeraldStimulus-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).
- ItemSynthesis 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, SusantaThe 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.
- ItemBioinspired 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, CordeliaMicroencapsulated 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.
- ItemDNAzymes 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, JulianSingle-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.
- ItemExamining 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-JochenEpoxy-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.
- ItemThe 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.
- ItemComplex Metal Nanostructures with Programmable Shapes from Simple DNA Building Blocks(Weinheim : Wiley-VCH, 2021) Ye, Jingjing; Aftenieva, Olha; Bayrak, Türkan; Jain, Archa; König, Tobias A.F.; Erbe, Artur; Seidel, RalfAdvances in DNA nanotechnology allow the design and fabrication of highly complex DNA structures, uisng specific programmable interactions between smaller nucleic acid building blocks. To convey this concept to the fabrication of metallic nanoparticles, an assembly platform is developed based on a few basic DNA structures that can serve as molds. Programming specific interactions between these elements allows the assembly of mold superstructures with a range of different geometries. Subsequent seeded growth of gold within the mold cavities enables the synthesis of complex metal structures including tightly DNA-caged particles, rolling-pin- and dumbbell-shaped particles, as well as T-shaped and loop particles with high continuity. The method further supports the formation of higher-order assemblies of the obtained metal geometries. Based on electrical and optical characterizations, it is expected that the developed platform is a valuable tool for a self-assembly-based fabrication of nanoelectronic and nanooptic devices. © 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH
- ItemAmphiphilic Copolymers for Versatile, Facile, and In Situ Tunable Surface Biofunctionalization(Weinheim : Wiley-VCH, 2021) Ruland, André; Schenker, Saskia; Schirmer, Lucas; Friedrichs, Jens; Meinhardt, Andrea; Schwartz, Véronique B.; Kaiser, Nadine; Konradi, Rupert; MacDonald, William; Helmecke, Tina; Sikosana, Melissa K.L.N.; Valtin, Juliane; Hahn, Dominik; Renner, Lars D.; Werner, Carsten; Freudenberg, UwePrecision surface engineering is key to advanced biomaterials. A new platform of PEGylated styrene-maleic acid copolymers for adsorptive surface biofunctionalization is reported. Balanced amphiphilicity renders the copolymers water-soluble but strongly affine for surfaces. Fine-tuning of their molecular architecture provides control over adsorptive anchorage onto specific materials-which is why they are referred to as "anchor polymers" (APs)-and over structural characteristics of the adsorbed layers. Conjugatable with an array of bioactives-including cytokine-complexing glycosaminoglycans, cell-adhesion-mediating peptides and antimicrobials-APs can be applied to customize materials for demanding biotechnologies in uniquely versatile, simple, and robust ways. Moreover, homo- and heterodisplacement of adsorbed APs provide unprecedented means of in situ alteration and renewal of the functionalized surfaces. The related options are exemplified with proof-of-concept experiments of controlled bacterial adhesion, human umbilical vein endothelial cell, and induced pluripotent cell growth on AP-functionalized surfaces.
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