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- ItemFe3O4 Nanoparticles Grown on Cellulose/GO Hydrogels as Advanced Catalytic Materials for the Heterogeneous Fenton-like Reaction(Washington, DC : ACS Publications, 2019) Chen, Yian; Pötschke, Petra; Pionteck, Jürgen; Voit, Brigitte; Qi, HaisongCellulose/graphene oxide (GO)/iron oxide (Fe3O4) composites were prepared by coprecipitating iron salts onto cellulose/GO hydrogels in a basic solution. X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared, and X-ray diffraction characterization showed that Fe3O4 was successfully coated on GO sheets and cellulose. Cellulose/GO/Fe3O4 composites showed excellent catalytic activity by maintaining almost 98% of the removal of acid orange 7 (AO7) and showed stability over 20 consecutive cycles. This performance is attributable to the synergistic effect of Fe3O4 and GO during the heterogeneous Fenton-like reaction. Especially, the cellulose/GO/Fe3O4 composites preserve their activity by keeping the ratio of Fe3+/Fe2+ at 2 even after 20 catalysis cycles, which is supported by XPS analysis.
- ItemToward Functional Synthetic Cells: In-Depth Study of Nanoparticle and Enzyme Diffusion through a Cross-Linked Polymersome Membrane(Weinheim : Wiley-VCH, 2019) Gumz, Hannes; Boye, Susanne; Iyisan, Banu; Krönert, Vera; Formanek, Petr; Voit, Brigitte; Lederer, Albena; Appelhans, DietmarUnderstanding the diffusion of nanoparticles through permeable membranes in cell mimics paves the way for the construction of more sophisticated synthetic protocells with control over the exchange of nanoparticles or biomacromolecules between different compartments. Nanoparticles postloading by swollen pH switchable polymersomes is investigated and nanoparticles locations at or within polymersome membrane and polymersome lumen are precisely determined. Validation of transmembrane diffusion properties is performed based on nanoparticles of different origin—gold, glycopolymer protein mimics, and the enzymes myoglobin and esterase—with dimensions between 5 and 15 nm. This process is compared with the in situ loading of nanoparticles during polymersome formation and analyzed by advanced multiple-detector asymmetrical flow field-flow fractionation (AF4). These experiments are supported by complementary i) release studies of protein mimics from polymersomes, ii) stability and cyclic pH switches test for in polymersome encapsulated myoglobin, and iii) cryogenic transmission electron microscopy studies on nanoparticles loaded polymersomes. Different locations (e.g., membrane and/or lumen) are identified for the uptake of each protein. The protein locations are extracted from the increasing scaling parameters and the decreasing apparent density of enzyme-containing polymersomes as determined by AF4. Postloading demonstrates to be a valuable tool for the implementation of cell-like functions in polymersomes.
- 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.
- ItemDendritic glycopolymers based on dendritic polyamine scaffolds: view on their synthetic approaches, characteristics and potential for biomedical applications(London : Soc., 2014) Appelhans, Dietmar; Klajnert-Maculewicz, Barbara; Janaszewska, Anna; Lazniewska, Joanna; Voit, BrigitteIn this review we highlight the potential for biomedical applications of dendritic glycopolymers based on polyamine scaffolds. The complex interplay of the molecular characteristics of the dendritic architectures and their specific interactions with various (bio)molecules are elucidated with various examples. A special role of the individual sugar units attached to the dendritic scaffolds and their density is identified, which govern ionic and H-bond interactions, and biological targeting, but to a large extent are also responsible for the significantly reduced toxicity of the dendritic glycopolymers compared to their polyamine scaffolds. Thus, the application of dendritic glycopolymers in drug delivery systems for gene transfection but also as therapeutics in neurodegenerative diseases has great promise.
- ItemOrganic vapor sensing behavior of polycarbonate/polystyrene/multi-walled carbon nanotube blend composites with different microstructures(Amsterdam [u.a.] : Elsevier Science, 2019) Li, Yilong; Pionteck, Jürgen; Pötschke, Petra; Voit, BrigitteWith the focus on the use as leakage detectors, the vapor sensing behavior of conductive polymer composites (CPCs) based on polycarbonate/polystyrene/multi-walled carbon nanotube (PC/PS/MWCNT) blends with different blend ratios was studied as well as their morphological and electrical properties. In the melt mixed blend composites, the MWCNTs are preferentially localized in PC. At the PC/PS ratio of 70/30 wt%, the composites showed a sea-island structure, while for blends containing 40 wt% or 50 wt% PS co-continuous structures were developed resulting in a reduction in the MWCNT percolation threshold. The saturated vapors of the selected solvents have good interactions to PS but different interactions to PC. At 0.75 wt% MWCNT, sea-island CPCs showed high relative resistance change (Rrel) but poor reversibility towards moderate vapors like ethyl acetate and toluene, while CPCs with co-continuous structure exhibited lower Rrel and better reversibility. All CPCs showed poor reversibility towards vapor of the good solvent dichloromethane due to strong interactions between polymers and vapor. In the vapor of the poor solvent cyclohexane, CPCs with higher PS content showed increased Rrel. After extraction of the PS component by cyclohexane, the sensing response was decreased and the Rrel of the co-continuous blend even reached negative values.
- ItemTuning the Properties and Self-Healing Behavior of Ionically Modified Poly(isobutylene-co-isoprene) Rubber(Washington, DC : Soc., 2017) Suckow, Marcus; Mordvinkin, Anton; Roy, Manta; Singha, Nikhil K.; Heinrich, Gert; Voit, Brigitte; Saalwächter, Kay; Böhme, FrankThe focus of this work is on the nature of self-healing of ionically modified rubbers obtained by reaction of brominated poly(isobutylene-co-isoprene) rubber (BIIR) with various alkylimidazoles such as 1-methylimidazole, 1-butylimidazole, 1-hexylimidazole, 1-nonylimidazole, and 1-(6-chlorohexyl)-1H-imidazole. Based on stress-strain and temperature dependent DMA measurements, a structural influence of the introduced ionic imidazolium moieties on the formation of ionic clusters and, as a consequence, on the mechanical strength and self-healing behavior of the samples could be evidenced. These results are fully supported by a molecular-level assessment of the network structure (cross-link and constraint density) and the dynamics of the ionic clusters using an advanced proton low-field NMR technique. The results show distinct correlations between the macroscopic behavior and molecular chain dynamics of the modified rubbers. In particular, it is shown that the optimization of material properties with regard to mechanical and self-healing behavior is limited by opposing tendencies. Samples with reduced chain dynamics exhibit superior mechanical behavior but lack on self-healing behavior. In spite of these limitations, the overall performance of some of our samples including self-healing behavior exceeds distinctly that of other self-healing rubbers described in the literature so far.
- ItemConjugated Polymers as a New Class of Dual-Mode Matrices for MALDI Mass Spectrometry and Imaging(Washington, DC : ACS Publications, 2018) Horatz, Kilian; Giampà, Marco; Karpov, Yevhen; Sahre, Karin; Bednarz, Hanna; Kiriy, Anton; Voit, Brigitte; Niehaus, Karsten; Hadjichristidis, Nikos; Michels, Dominik L.; Lissel, FranziskaMatrix-assisted laser desorption/ionization mass spectrometry (MALDI MS) and MALDI MS imaging are ubiquitous analytical methods in medical, pharmaceutical, biological, and environmental research. Currently, there is a strong interest in the investigation of low molecular weight compounds (LMWCs), especially to trace and understand metabolic pathways, requiring the development of new matrix systems that have favorable optical properties and a high ionization efficiency and that are MALDI silent in the LMWC area. In this paper, five conjugated polymers, poly{[N,N'-bis(2-octyldodecyl)-naphtalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5'(2,2'-bithiophene)} (PNDI(T2)), poly(3-dodecylthiophene-2,5-diyl) (P3DDT), poly{[2,3-bis(3-octyloxyphenyl)quinoxaline-5,8-diyl]-alt-(thiophene-2,5-diyl)} (PTQ1), poly{[N,N'-bis(2-octyldodecyl)-isoindigo-5,5'-diyl]-alt-5,5'(2,2'-bithiophene)} (PII(T2)), and poly(9,9-di-n-octylfluorenyl-2,7-diyl) (P9OFl) are investigated as matrices. The polymers have a strong optical absorption, are solution processable, and can be coated into thin films, allowing a vast reduction in the amount of matrix used. All investigated polymers function as matrices in both positive and negative mode MALDI, classifying them as rare dual-mode matrices, and show a very good analyte ionization ability in both modes. PNDI(T2), P3DDT, PTQ1, and PII(T2) are MALDI silent in the full measurement range (>m/z = 150k), except at high laser intensities. In MALDI MS experiments of single analytes and a complex biological sample, the performance of the polymers was found to be as good as two commonly used matrices (2,5-DHB for positive and 9AA for negative mode measurements). The detection limit of two standard analytes was determined as being below 164 pmol for reserpine and below 245 pmol for cholic acid. Additionally P3DDT was used successfully in first MALDI MS imaging experiments allowing the visualization of the tissue morphology of rat brain sections.
- ItemSugar-Modified Poly(propylene imine) Dendrimers Stimulate the NF-κB Pathway in a Myeloid Cell Line(Dordrecht [u.a.] : Springer Science + Business Media B.V, 2016) Jatczak-Pawlik, Izabela; Gorzkiewicz, Michal; Studzian, Maciej; Appelhans, Dietmar; Voit, Brigitte; Pulaski, Lukasz; Klajnert-Maculewicz, BarbaraPurpose: Fourth-generation poly(propylene imine) dendrimers fully surface-modified by maltose (dense shell, PPI-m DS) were shown to be biocompatible in cellular models, which is important for their application in drug delivery. We decided to verify also their inherent bioactivity, including immunomodulatory activity, for potential clinical applications. We tested their effects on the THP-1 monocytic cell line model of innate immunity effectors. Methods: To estimate the cytotoxicity of dendrimers the reasazurin assay was performed. The expression level of NF-κB targets: IGFBP3, TNFAIP3 and TNF was determined by quantitative real-time RT-PCR. Measurement of NF-κB p65 translocation from cytoplasm to nucleus was conducted with a high-content screening platform and binding of NF-κB to a consensus DNA probe was determined by electrophoretic mobility shift assay. The cytokine assay was performed to measure protein concentration of TNFalpha and IL-4. Results: We found that PPI-m DS did not impact THP-1 viability and growth even at high concentrations (up to 100 μM). They also did not induce expression of genes for important signaling pathways: Jak/STAT, Keap1/Nrf2 and ER stress. However, high concentrations of 4th generation PPI-m DS (25–100 μM), but not their 3rd generation counterparts, induced nuclear translocation of p65 NF-κB protein and its DNA-binding activity, leading to NF-κB-dependent increased expression of mRNA for NF-κB targets: IGFBP3, TNFAIP3 and TNF. However, no increase in pro-inflammatory cytokine secretion was detected. Conclusion: We conclude that maltose-modified PPI dendrimers of specific size could exert a modest immunomodulatory effect, which may be advantageous in clinical applications (e.g. adjuvant effect in anti-cancer vaccines).
- ItemInterfacial chemistry using a bifunctional coupling agent for enhanced electrical properties of carbon nanotube based composites(Oxford : Elsevier Science, 2013) Socher, Robert; Jakisch, Lothar; Krause, Beate; Oertel, Ulrich; Voit, Brigitte; Pötschke, PetraA bifunctional coupling agent (BCA) containing one oxazoline and one benzoxazinone group was applied to promote a reaction between polyamide 12 (PA12) and multiwalled carbon nanotubes (MWCNTs) during melt mixing. With this modification, the MWCNT content needed for the electrical percolation was significantly reduced by more than a factor of three. For amino functionalized MWCNT-PA12 composites adding 1 wt.% BCA electrical percolation was reached at only 0.37 wt.% MWCNTs compared to 1.0 wt.% without BCA. With the help of a model reaction, the covalent attachment of the BCA to the MWCNTs could be shown by thermogravimetric analysis (TGA) and via fluorescence spectroscopy. Model compounds were applied containing either only the oxazoline or the benzoxazinone group to show that the better electrical properties in the PA12-MWCNT composites were a result of a covalent bond between the polymer and the nanotube which only takes place when the BCA was used. In addition, significantly higher electrical conductivity values were obtained by the addition of BCA as well with amino functionalized as with nonmodified commercial MWCNTs. This surprising result was attributed to the significant hydroxy group content on the surface of those commercial MWCNTs. © 2013 Elsevier Ltd. All rights reserved.
- ItemPolypropylene-based melt mixed composites with singlewalled carbon nanotubes for thermoelectric applications: Switching from p-type to n-type by the addition of polyethylene glycol(Oxford : Elsevier Science, 2017) Luo, Jinji; Cerretti, Giacomo; Krause, Beate; Zhang, Long; Otto, Thomas; Jenschke, Wolfgang; Ullrich, Mathias; Tremel, Wolfgang; Voit, Brigitte; Pötschke, PetraThe thermoelectric properties of melt processed conductive nanocomposites consisting of an insulating polypropylene (PP) matrix filled with singlewalled carbon nanotubes (CNTs) and copper oxide (CuO) were evaluated. An easy and cheap route to switch p-type composites into n-type was developed by adding polyethylene glycol (PEG) during melt mixing. At the investigated CNT concentrations of 0.8 wt% and 2 wt% (each above the electrical percolation threshold of ∼0.1 wt%), and a fixed CuO content of 5 wt%, the PEG addition converted p-type composites (positive Seebeck coefficient (S)) into n-type (negative S). PEG was also found to improve the filler dispersion inside the matrix. Two composites were prepared: P-type polymer/CNT composites with high S (up to 45 μV/K), and n-type composites (with S up to −56 μV/K) through the addition of PEG. Two prototypes with 4 and 49 thermocouples of these p- and n-type composites were fabricated, and delivered an output voltage of 21 mV and 110 mV, respectively, at a temperature gradient of 70 K.