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Highly Conductive, Stretchable, and Cell-Adhesive Hydrogel by Nanoclay Doping
Electrically conductive materials that mimic physical and biological properties of tissues are urgently required for seamless brain-machine interfaces. Here, a multinetwork hydrogel combining electrical conductivity of 26 S m-1 , stretchability of 800%, and tissue-like elastic modulus of 15 kPa with mimicry of the extracellular matrix is reported. Engineering this unique set of properties is enabled by a novel in-scaffold polymerization approach. Colloidal hydrogels of the nanoclay Laponite are employed as supports for the assembly of secondary polymer networks. Laponite dramatically increases the conductivity of in-scaffold polymerized poly(ethylene-3,4-diethoxy thiophene) in the absence of other dopants, while preserving excellent stretchability. The scaffold is coated with a layer containing adhesive peptide and polysaccharide dextran sulfate supporting the attachment, proliferation, and neuronal differentiation of human induced pluripotent stem cells directly on the surface of conductive hydrogels. Due to its compatibility with simple extrusion printing, this material promises to enable tissue-mimetic neurostimulating electrodes.
Achieving electrical conductive tracks by laser treatment of non-conductive polypropylene/polycarbonate blends filled with MWCNTs
Electrical non-conductive polymer blends consisting of a polypropylene (PP) matrix and dispersed particles of polycarbonate (PC) were melt compounded with 3 wt.% multiwalled carbon nanotubes (MWCNTs) loading and processed into plates by injection molding. The morphological analysis confirmed the selective localization of the MWCNTs in the PC component. By local irradiation with a CO2 laser beam, depending on the laser conditions, conductive tracks with dimensions of about 2 mm width, 80 to 370 μm depth and line resistances as low as 1.5 kΩ · cm-1 were created on the surface of the non-conductive plates. The factors affecting the line resistance are the PC content, the laser speed and laser power, as well as laser direction with respect to the melt flow direction. After the irradiation an enrichment of MWCNTs in the laser lines was detected indicating that conductive paths were generated by percolation of nanotubes selectively within these lines in otherwise non-conductive plates. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Sperm-Driven Micromotors Moving in Oviduct Fluid and Viscoelastic Media
Biohybrid micromotors propelled by motile cells are fascinating entities for autonomous biomedical operations on the microscale. Their operation under physiological conditions, including highly viscous environments, is an essential prerequisite to be translated to in vivo settings. In this work, a sperm-driven microswimmer, referred to as a spermbot, is demonstrated to operate in oviduct fluid in vitro. The viscoelastic properties of bovine oviduct fluid (BOF), one of the fluids that sperm cells encounter on their way to the oocyte, are first characterized using passive microrheology. This allows to design an artificial oviduct fluid to match the rheological properties of oviduct fluid for further experiments. Sperm motion is analyzed and it is confirmed that kinetic parameters match in real and artificial oviduct fluids, respectively. It is demonstrated that sperm cells can efficiently couple to magnetic microtubes and propel them forward in media of different viscosities and in BOF. The flagellar beat pattern of coupled as well as of free sperm cells is investigated, revealing an alteration on the regular flagellar beat, presenting an on–off behavior caused by the additional load of the microtube. Finally, a new microcap design is proposed to improve the overall performance of the spermbot in complex biofluids. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
A Tunable Polymer–Metal Based Anti-Reflective Metasurface
Anti-reflective surfaces are of great interest for optical devices, sensing, photovoltaics, and photocatalysis. However, most of the anti-reflective surfaces lack in situ tunability of the extinction with respect to wavelength. This communication demonstrates a tunable anti-reflective surface based on colloidal particles comprising a metal core with an electrochromic polymer shell. Random deposition of these particles on a reflective surface results in a decrease in the reflectance of up to 99.8% at the localized surface plasmon resonance frequency. This narrow band feature can be tuned by varying the pH or by application of an electric potential, resulting in wavelength shifts of up to 30 nm. Electrophoretic particle deposition is shown to be an efficient method for controlling the interparticle distance and thereby further optimizing the overall efficiency of the anti-reflective metasurface. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Light-Driven Proton Transfer for Cyclic and Temporal Switching of Enzymatic Nanoreactors
Temporal activation of biological processes by visible light and subsequent return to an inactive state in the absence of light is an essential characteristic of photoreceptor cells. Inspired by these phenomena, light-responsive materials are very attractive due to the high spatiotemporal control of light irradiation, with light being able to precisely orchestrate processes repeatedly over many cycles. Herein, it is reported that light-driven proton transfer triggered by a merocyanine-based photoacid can be used to modulate the permeability of pH-responsive polymersomes through cyclic, temporally controlled protonation and deprotonation of the polymersome membrane. The membranes can undergo repeated light-driven swelling-contraction cycles without losing functional effectiveness. When applied to enzyme loaded-nanoreactors, this membrane responsiveness is used for the reversible control of enzymatic reactions. This combination of the merocyanine-based photoacid and pH-switchable nanoreactors results in rapidly responding and versatile supramolecular systems successfully used to switch enzymatic reactions ON and OFF on demand.
Multivalent Protein-Loaded pH-Stable Polymersomes: First Step toward Protein Targeted Therapeutics
Synthetic platforms for mimicking artificial organelles or for designing multivalent protein therapeutics for targeting cell surface, extracellular matrix, and tissues are in the focus of this study. Furthermore, the availability of a multi-functionalized and stimuli-responsive carrier system is required that can be used for sequential in situ and/or post loading of different proteins combined with post-functionalization steps. Until now, polymersomes exhibit excellent key characteristics to fulfill those requirements, which allow specific transport of proteins and the integration of proteins in different locations of polymeric vesicles. Herein, different approaches to fabricate multivalent protein-loaded, pH-responsive, and pH-stable polymersomes are shown, where a combination of therapeutic action and targeting can be achieved, by first choosing two model proteins such as human serum albumin and avidin. Validation of the molecular parameters of the multivalent biohybrids is performed by dynamic light scattering, cryo-TEM, fluorescence spectroscopy, and asymmetrical flow-field flow fractionation combined with light scattering techniques. To demonstrate targeting functions of protein-loaded polymersomes, avidin post-functionalized polymersomes are used for the molecular recognition of biotinylated cell surface receptors. These versatile protein-loaded polymersomes present new opportunities for designing sophisticated biomolecular nanoobjects in the field of (extracellular matrix) protein therapeutics.
Metal Plastic Hybrids: Optimisation in model experiments [Metall-Kunststoff-Verbunde: Modellversuche zur Optimierung]
Metal plastic hybrids will become more important as components for lightweight constructions. It is reported about optimisation of making three layer hybrids consisted of a steel plate, an adhesion layer based of uretdione powder coating material and a flexible component polyurethane in model experiments. Hybrid formation is performed in a compression moulding process. The adhesion layer and the polyurethane are modified to increase the hybrid bond strength. Peel test are conducted to quantitatively characterize the bond strength and an apparent energy release rate is calculated based on the peel force. For hybrids with widths of 2 mm polyurethane stripes it is possible to increase the apparent energy release rate for about 30 % to 16 N/mm in comparison with a hybrid with unmodified components. These hybrids have the same high bond strength level as the strongest hybrids reported in literature. Concluding the optimisation results are discussed related to their relevancy for the interpretation of the adhesion mechanisms in the interface between adhesion layer and polyurethane. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
AB- Versus AA+BB-Suzuki Polycondensation: A Palladium/Tris(tert-butyl)phosphine Catalyst Can Outperform Conventional Catalysts
A Pd/Pt-Bu3 catalyst having bulky, electron-rich ligands significantly outperforms conventional “step-growth catalysts” Pd(PPh3)4 and Pd(Po-Tol3)3 in the Suzuki polycondensation of the AB-type arylene-based monomers, such as some of the substituted fluorenes, carbazoles, and phenylenes. In the AA+BB polycondensation, Pd/Pt-Bu3 also performs better under homogeneous reaction conditions, in combination with the organic base Et4NOH. The superior performance of Pd/Pt-Bu3 is discussed in terms of its higher reactivity in the oxidative addition step and inherent advantages of the intramolecular catalyst transfer, which is a key step joining catalytic cycles of the AB-polycondensation. These findings are applied to the synthesis of a carbazole-based copolymer designed for the use as a hole conductor in solution-processed organic light-emitting diodes. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Casting of Gold Nanoparticles with High Aspect Ratios inside DNA Molds
DNA nanostructures provide a powerful platform for the programmable assembly of nanomaterials. Here this approach is extended to synthesize rod-like gold nanoparticles in a full DNA controlled manner. The approach is based on DNA molds containing elongated cavities. Gold is deposited inside the molds using a seeded-growth procedure. By carefully exploring the growth parameters it is shown that gold nanostructures with aspect ratios of up to 7 can be grown from single seeds. The highly anisotropic growth is in this case controlled only by the rather soft and porous DNA walls. The optimized seeded growth procedure provides a robust and simple routine to achieve continuous gold nanostructures using DNA templating.
Long-Term Retarded Release for the Proteasome Inhibitor Bortezomib through Temperature-Sensitive Dendritic Glycopolymers as Drug Delivery System from Calcium Phosphate Bone Cement
For the local treatment of bone defects, highly adaptable macromolecular architectures are still required as drug delivery system (DDS) in solid bone substitute materials. Novel DDS fabricated by host–guest interactions between β-cyclodextrin-modified dendritic glycopolymers and adamantane-modified temperature-sensitive polymers for the proteasome inhibitor bortezomib (BZM) is presented. These DDS induce a short- and long-term (up to two weeks) retarded release of BZM from calcium phosphate bone cement (CPC) in comparison to a burst release of the drug alone. Different release parameters of BZM/DDS/CPC are evaluated in phosphate buffer at 37 °C to further improve the long-term retarded release of BZM. This is achieved by increasing the amount of drug (50–100 µg) and/or DDS (100–400 µg) versus CPC (1 g), by adapting the complexes better to the porous bone cement environment, and by applying molar ratios of excess BZM toward DDS with 1:10, 1:25, and 1:100. The temperature-sensitive polymer shells of BZM/DDS complexes in CPC, which allow drug loading at room temperature but are collapsed at body temperature, support the retarding long-term release of BZM from DDS/CPC. Thus, the concept of temperature-sensitive DDS for BZM/DDS complexes in CPC works and matches key points for a local therapy of osteolytic bone lesions.