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- ItemConformations of a Long Polymer in a Melt of Shorter Chains: Generalizations of the Flory Theorem(Washington, DC : ACS, 2015) Lang, Michael; Rubinstein, Michael; Sommer, Jens-UweLarge-scale simulations of the swelling of a long N-mer in a melt of chemically identical P-mers are used to investigate a discrepancy between theory and experiments. Classical theory predicts an increase of probe chain size R ∼ P–0.18 with decreasing degree of polymerization P of melt chains in the range of 1 < P < N1/2. However, both experiment and simulation data are more consistent with an apparently slower swelling R ∼ P–0.1 over a wider range of melt degrees of polymerization. This anomaly is explained by taking into account the recently discovered long-range bond correlations in polymer melts and corrections to excluded volume. We generalize the Flory theorem and demonstrate that it is in excellent agreement with experiments and simulations.
- ItemProtein-Assisted Assembly of Modular 3D Plasmonic Raspberry-like Core/Satellite Nanoclusters: Correlation of Structure and Optical Properties(Washington, DC : Soc., 2016) Höller, Roland P. M.; Dulle, Martin; Thomä, Sabrina; Mayer, Martin; Steiner, Anja Maria; Förster, Stephan; Fery, Andreas; Kuttner, Christian; Chanana, MunishWe present a bottom-up assembly route for a large-scale organization of plasmonic nanoparticles (NPs) into three-dimensional (3D) modular assemblies with core/satellite structure. The protein-assisted assembly of small spherical gold or silver NPs with a hydrophilic protein shell (as satellites) onto larger metal NPs (as cores) offers high modularity in sizes and composition at high satellite coverage (close to the jamming limit). The resulting dispersions of metal/metal nanoclusters exhibit high colloidal stability and therefore allow for high concentrations and a precise characterization of the nanocluster architecture in dispersion by small-angle X-ray scattering (SAXS). Strong near-field coupling between the building blocks results in distinct regimes of dominant satellite-to-satellite and core-to-satellite coupling. High robustness against satellite disorder was proved by UV/vis diffuse reflectance (integrating sphere) measurements. Generalized multiparticle Mie theory (GMMT) simulations were employed to describe the electromagnetic coupling within the nanoclusters. The close correlation of structure and optical property allows for the rational design of core/satellite nanoclusters with tailored plasmonics and well-defined near-field enhancement, with perspectives for applications such as surface-enhanced spectroscopies.
- ItemInfluence of microwave plasma treatment on the surface properties of carbon fibers and their adhesion in a polypropylene matrix(London [u.a.] : Institute of Physics, 2016) Scheffler, C.; Wölfel, E.; Förster, T.; Poitzsch, C.; Kotte, L.; Mäder, G.; Madsen, Bo; Biel, A.; Kusano, Y.; Lilholt, H.; Mikkelsen, L.P.; Mishnaevsky Jr., L.; Sørensen, B.F.A commercially available carbon fiber (CF) with an epoxy-based sizing (EP-sized CF) and an unsized CF have been plasma treated to study the effect on the fiber-matrix adhesion towards a polypropylene matrix. The EP-sized fiber was chosen because of its predictable low adhesion in a polypropylene (PP) matrix. The fibers have been modified using a microwave low-pressure O2/CO2/N2-gas plasma source (Cyrannus®) developed at IWS in a batch process. One aim of this study was the evaluation of parameters using high energies and short time periods in the plasma chamber to see the effect on mechanical performance of CF. These results will be the fundamental work for a planned continuous plasma modification line. The CF surface was characterized by determining the surface energies, single fiber tensile strength and XPS analysis. The adhesion behavior before and after plasma treatment was studied by single fiber pull-out test (SFPO) and scanning electron microscopy (SEM). It was shown that the CO2- and O2-plasma increases the number of functional groups on the fiber surface during short time plasma treatment of 30 s. Carboxylic groups on the unsized CF surface resulting from O2-plasma treatment lead to an enhanced fiber-matrix adhesion, whereas the fiber strength was merely reduced.
- ItemEffects of high energy electrons on the properties of polyethylene / multiwalled carbon nanotubes composites: Comparison of as-grown and oxygen-functionalised MWCNT(Melville, NY : AIP, 2014) Krause, Beate; Pötschke, Petra; Gohs, U.Polymer modification with high energy electrons (EB) is well established in different applications for many years. It is used for crosslinking, curing, degrading, grafting of polymeric materials and polymerisation of monomers. In contrast to this traditional method, electron induced reactive processing (EIReP) combines the polymer modification with high energy electrons and the melt mixing process. This novel reactive method was used to prepare polymer blends and composites. In this study, both methods were used for the preparation of polyethylene (PE)/ multiwalled carbon nanotubes (MWCNT) composites in the presence of a coupling agent. The influence of MWCNT and type of electron treatment on the gel content, the thermal conductivity, rheological, and electrical properties was investigated whereby as-grown and oxidised MWCNT were used. In the presence of a coupling agent and at an absorbed dose of 40 kGy, the gel content increased from 57 % for the pure PE to 74 % or 88 % by the addition of as-grown (Baytubes® C150P) or oxidised MWCNT, respectively. In comparison to the composites containing the as-grown MWCNTs, the use of the oxidised MWCNTs led to higher melt viscosity and higher storage modulus due to higher yield of filler polymer couplings. The melt viscosity increased due to the addition of MWCNT and crosslinking of PE. The thermal conductivity increased to about 150 % and showed no dependence on the kind of MWCNT and the type of electron treatment. In contrast, the lowest value of electrical volume resistivity was found for the non-irradiated samples and after state of the art electron treatment without any influence of the type of MWCNT. In the case of EIReP, the volume resistivity increased by 2 (as-grown MWCNT) or 3 decades (oxidised MWCNT) depending on the process parameters. © 2014 American Institute of Physics.
- ItemStimuli‐responsive microjets with reconfigurable shape(Hoboken, NJ : Wiley, 2014) Magdanz, Veronika; Stoychev, Georgi; Ionov, Leonid; Sanchez, Samuel; Schmidt, Oliver.G.Flexible thermoresponsive polymeric microjets are formed by the self‐folding of polymeric layers containing a thin Pt film used as catalyst for self‐propulsion in solutions containing hydrogen peroxide. The flexible microjets can reversibly fold and unfold in an accurate manner by applying changes in temperature to the solution in which they are immersed. This effect allows microjets to rapidly start and stop multiple times by controlling the radius of curvature of the microjet. This work opens many possibilities in the field of artificial nanodevices, for fundamental studies on self‐propulsion at the microscale, and also for biorelated applications.
- ItemSurface, interphase and tensile properties of unsized, sized and heat treated basalt fibres(London [u.a.] : Institute of Physics, 2016) Förster, T.; Sommer, G.S.; Mäder, E.; Scheffler, C.Recycling of fibre reinforced polymers is in the focus of several investigations. Chemical and thermal treatments of composites are the common ways to separate the reinforcing fibres from the polymer matrices. However, most sizings on glass and basalt fibre are not designed to resist high temperatures. Hence, a heat treatment might also lead to a sizing removal, a decrease of mechanical performance and deterioration in fibre-matrix adhesion. Different basalt fibres were investigated using surface analysis methods as well as single fibre tensile tests and single fibre pull-out tests in order to reveal the possible causes of these issues. Heat treatment in air reduced the fibre tensile strength in the same level like heat treatment in nitrogen atmosphere, but it influenced the wetting capability. Re-sizing by a coupling agent slightly increased the adhesion strength and reflected a decreased post-debonding friction.
- ItemPhoto-Cross-Linked Dual-Responsive Hollow Capsules Mimicking Cell Membrane for Controllable Cargo Post-Encapsulation and Release(Weinheim : Wiley-VCH, 2016) Liu, Xiaoling; Appelhans, Dietmar; Wei, Qiang; Voit, BrigitteMultifunctional and responsive hollow capsules are ideal candidates to establish highly sophisticated compartments mimicking cell membranes for controllable bio-inspired functions. For this purpose pH and temperature dual-responsive and photo-cross-linked hollow capsules, based on silica-templated layer-by-layer approach by using poly(N-isopropyl acrylamide)-blockpolymethacrylate) and polyallylamine, have been prepared to use them for the subsequent and easily available post-encapsulation process of proteinlike macromolecules at room temperature and pH 7.4 and their controllable release triggered by stimuli. The uptake and release properties of the hollow capsules for cargos are highly affected by changes in the external stimuli temperature (25, 37, or 45 °C) and internal stimuli pH of the phosphate-containing buffer solution (5.5 or 7.4), by the degree of photo-cross-linking, and the size of cargo. The photo-cross-linked and dual stimuli-responsive hollow capsules with different membrane permeability can be considered as attractive material for mimicking cell functions triggered by controllable uptake and release of different up to 11 nm sized biomolecules.
- ItemA hyperbranched dopamine-containing PEG-based polymer for the inhibition of α-synuclein fibrillation(Orlando, Fla. : Academic Press, 2015) Breydo, Leonid; Newland, Ben; Zhang, Hong; Rosser, Anne; Werner, Carsten; Uversky, Vladimir N.; Wang, WenxinAggregation of α-synuclein is believed to play an important role in Parkinson's disease and in other neurodegenerative maladies. Small molecule inhibitors of this process are among the most promising drug candidates for neurodegenerative diseases. Dendrimers have also been studied for anti-fibrillation applications but they can be difficult and expensive to synthetize. Here we show that RAFT polymerization can be used to produce a hyperbranched polyethylene glycol structure via a one-pot reaction. This polymer included a dopamine moiety, a known inhibitor of α-synuclein fibril formation. Dopamine within the polymer structure was capable of aggregation inhibition, although not to the same degree as free dopamine. This result opens up new avenues for the use of controlled radical polymerizations as a means of preparing hyperbranched polymers for anti-fibrillation activity, but shows that the incorporation of functional groups from known small molecules within polymers may alter their biological activity.
- ItemProbing carbonyl-water hydrogen-bond interactions in thin polyoxazoline brushes(Melville, NY : AIP Publishing, 2016) Kroning, Annika; Furchner, Andreas; Adam, Stefan; Uhlmann, Petra; Hinrichs, KarstenTemperature-responsive oxazoline-based polymer brushes have gained increased attention as biocompatible surfaces. In aqueous environment, they can be tuned between hydrophilic and hydrophobic behavior triggered by a temperature stimulus. This transition is connected with changes in molecule–solvent interactions and results in a switching of the brushes between swollen and collapsed states. This work studies the temperature-dependent interactions between poly(2-oxazoline) brushes and water. In detail, thermoresponsive poly(2-cyclopropyl-2-oxazoline), nonresponsive hydrophilic poly(2-methyl-2-oxazoline), as well as a copolymer of the two were investigated with in situ infrared ellipsometry. Focus was put on interactions of the brushes' carbonyl groups with water molecules. Different polymer–water interactions could be observed and assigned to hydrogen bonding between C=O groups and water molecules. The switching behavior of the brushes in the range of 20–45 °C was identified by frequency shifts and intensity changes of the amide I band.
- ItemDevelopment of a polymer composite with high electrical conductivity and improved impact strength for the application as bipolar plate(Melville, NY : AIP, 2016) Hopmann, C.; Windeck, C.; Cohnen, A.; Onken, J.; Krause, Beate; Pötschke, Petra; Hickmann, T.Bipolar plates constitute the most important structural component in fuel cell stacks. Highly filled thermoplastic composites with high electrical conductivity obtain an increasing importance in the design of bipolar plates as alternative to conventional metallic systems. Thermoplastics (e.g. PP) have suitable properties such as a good processability, chemical resistance, light weight and low production costs. As thermoplastics have low electrical conductivities, conductive fillers have to be included in the matrix. A high content of such fillers (e.g. graphite) in excess of 80 wt.-% is necessary to achieve the desired electrical properties. However, materials with such high filler contents embrittle readily. The workability in injection and compression molding is difficult and the mechanical stability is insufficient in case of strain deformation. As consequence, material failure and an inacceptable amount of damaged goods can be observed during the processing. As no suitable thermoplastic system is available for better mechanical properties, the induction and dispersion of a rubber phase in the thermoplastic matrix can be used to increase the impact strength of the conductive composite. In this research work a ternary composite, based on PP as matrix, EPDM as impact modifier and synthetic graphite as conductive filler, was developed. The material was produced using a 26 mm co-rotating, intermeshing twin-screw extruder. The amounts of PP, EPDM and graphite were varied systematically and a process window was defined that enables improved impact strength and high electrical conductivity of the new material. The results indicate that impact strength can be enhanced by about 99 % with an EPDM content of 30 wt.-% in the PP matrix. The electrical conductivity decreases in a small range with increasing content of EPDM, but the conductivity is still excellent for producing bipolar plates.