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- ItemGas-Phase Fluorination on PLA Improves Cell Adhesion and Spreading(Washington, DC : Soc., 2020) Schroepfer, Michaela; Junghans, Frauke; Voigt, Diana; Meyer, Michael; Breier, Anette; Schulze-Tanzil, Gundula; Prade, InaFor the regeneration or creation of functional tissues, biodegradable biomaterials including polylactic acid (PLA) are widely preferred. Modifications of the material surface are quite common to improve cell-material interactions and thereby support the biological outcome. Typical approaches include a wet chemical treatment with mostly hazardous substances or a functionalization with plasma. In the present study, gas-phase fluorination was applied to functionalize the PLA surfaces in a simple and one-step process. The biological response including biocompatibility, cell adhesion, cell spreading, and proliferation was analyzed in cell culture experiments with fibroblasts L929 and correlated with changes in the surface properties. Surface characterization methods including surface energy and isoelectric point measurements, X-ray photoelectron spectroscopy, and atomic force microscopy were applied to identify the effects of fluorination on PLA. Gas-phase fluorination causes the formation of C-F bonds in the PLA backbone, which induce a shift to a more hydrophilic and polar surface. The slightly negatively charged surface dramatically improves cell adhesion and spreading of cells on the PLA even with low fluorine content. The results indicate that this improved biological response is protein-but not integrin-dependent. Gas-phase fluorination is therefore an efficient technique to improve cellular response to biomaterial surfaces without losing cytocompatibility. Copyright © 2020 American Chemical Society.
- ItemElectron Transport across Vertical Silicon/MoS2/Graphene Heterostructures: Towards Efficient Emitter Diodes for Graphene Base Hot Electron Transistors(Washington, DC : ACS Publications, 2020) Belete, Melkamu; Engström, Olof; Vaziri, Sam; Lippert, Gunther; Lukosius, Mindaugas; Kataria, Satender; Lemme, Max C.Heterostructures comprising silicon, molybdenum disulfide (MoS2), and graphene are investigated with respect to the vertical current conduction mechanism. The measured current-voltage (I-V) characteristics exhibit temperature-dependent asymmetric current, indicating thermally activated charge carrier transport. The data are compared and fitted to a current transport model that confirms thermionic emission as the responsible transport mechanism across devices. Theoretical calculations in combination with the experimental data suggest that the heterojunction barrier from Si to MoS2 is linearly temperature-dependent for T = 200-300 K with a positive temperature coefficient. The temperature dependence may be attributed to a change in band gap difference between Si and MoS2, strain at the Si/MoS2 interface, or different electron effective masses in Si and MoS2, leading to a possible entropy change stemming from variation in density of states as electrons move from Si to MoS2. The low barrier formed between Si and MoS2 and the resultant thermionic emission demonstrated here make the present devices potential candidates as the emitter diode of graphene base hot electron transistors for future high-speed electronics. Copyright © 2020 American Chemical Society.
- ItemWet-Spinning of Biocompatible Core–Shell Polyelectrolyte Complex Fibers for Tissue Engineering(Weinheim : Wiley-VCH, 2020) Cui, Qing; Bell, Daniel Josef; Rauer, Sebastian Bernhard; Wessling, MatthiasPolyelectrolyte complex fibers (PEC fibers) have great potential with regard to biomedical applications as they can be fabricated from biocompatible and water-soluble polyelectrolytes under mild process conditions. The present publication describes a novel method for the continuous fabrication of PEC fibers in a water-based wet-spinning process by interfacial complexation within a core–shell spinneret. This process combines the robustness and flexibility of nonsolvent-induced phase separation (NIPS) spinning processes conventionally used in the membrane industry with the complexation between oppositely charged polyelectrolytes. The produced fibers demonstrate a core–shell structure with a low-density core and a highly porous polyelectrolyte complex shell of ≈800 μm diameter. In the case of chitosan and polystyrene sulfonate (PSS), mechanical fiber properties could be enhanced by doping the PSS with poly(ethylene oxide) (PEO). The resulting CHI/PSS-PEO fibers present a Young modulus of 3.78 GPa and a tensile strength of 165 MPa, which is an excellent combination of elongation at break and break stress compared to literature. The suitability of the CHI/PSS-PEO fibers as a scaffold for cell culture applications is verified by a four-day cultivation of human HeLa cells on PEO-reinforced fibers with a subsequent analysis of cell viability by fluorescence-based live/dead assay. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemHighly Symmetric and Extremely Compact Multiple Winding Microtubes by a Dry Rolling Mechanism(Weinheim : Wiley-VCH, 2020) Moradi, Somayeh; Naz, Ehsan Saei Ghareh; Li, Guodong; Bandari, Nooshin; Bandari, Vineeth Kumar; Zhu, Feng; Wendrock, Horst; Schmidt, Oliver G.Rolled-up nanotechnology has received significant attention to self-assemble planar nanomembranes into 3D micro and nanotubular architectures. These tubular structures have been well recognized as novel building blocks in a variety of applications ranging from microelectronics and nanophotonics to microbatteries and microrobotics. However, fabrication of multiwinding microtubes with precise control over the winding interfaces, which is crucial for many complex applications, is not easy to achieve by existing materials and technologies. Here, a dry rolling approach is introduced to tackle this challenge and create tight windings in compact and highly symmetric cylindrical microstructures. This technique exploits hydrophobicity of fluorocarbon polymers and the thermal expansion mismatch of polymers and inorganic films upon thermal treatment. Quality parameters for rolled-up microtubes, against which different fabrication technologies can be benchmarked are defined. The technique offers to fabricate long freestanding multiwinding microtubes as well as hierarchical architectures incorporating rolled-up wrinkled nanomembranes. This work presents an important step forward toward the fabrication of more complex but well-controlled microtubes for advanced high-quality device architectures. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemThe Electronic Conductivity of Single Crystalline Ga-Stabilized Cubic Li7La3Zr2O12: A Technologically Relevant Parameter for All-Solid-State Batteries(Weinheim : Wiley-VCH, 2020) Philipp, Martin; Gadermaier, Bernhard; Posch, Patrick; Hanzu, Ilie; Ganschow, Steffen; Meven, Martin; Rettenwander, Daniel; Redhammer, Günther J.; Wilkening, H. Martin R.The next-generation of all-solid-state lithium batteries need ceramic electrolytes with very high ionic conductivities. At the same time a negligible electronic conductivity σeon is required to eliminate self-discharge in such systems. A non-negligible electronic conductivity may also promote the unintentional formation of Li dendrites, being currently one of the key issues hindering the development of long-lasting all-solid-state batteries. This interplay is suggested recently for garnet-type Li7La3Zr2O12 (LLZO). It is, however, well known that the overall macroscopic electronic conductivity may be governed by a range of extrinsic factors such as impurities, chemical inhomogeneities, grain boundaries, morphology, and size effects. Here, advantage of Czochralski-grown single crystals, which offer the unique opportunity to evaluate intrinsic properties of a chemically homogeneous matrix, is taken to measure the electronic conductivity σeon. Via long-time, high-precision potentiostatic polarization experiments an upper limit of σeon in the order of 5 × 10−10 S cm−1 (293 K) is estimated. This value is by six orders of magnitude lower than the corresponding total conductivity σtotal = 10−3 S cm−1 of Ga-LLZO. Thus, it is concluded that the high values of σeon recently reported for similar systems do not necessarily mirror intragrain bulk properties of chemically homogenous systems but may originate from chemically inhomogeneous interfacial areas. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemTuning of Smart Multifunctional Polymer Coatings Made by Zwitterionic Phosphorylcholines(Weinheim : Wiley-VCH, 2020) Münch, Alexander S.; Adam, Stefan; Fritzsche, Tina; Uhlmann, PetraIn the last years, the generation of multifunctional coatings has been moved into the focus of interface modifications to expand the spectrum of material applications and to introduce new smart properties. Herein a promising multifunctional and universally usable coating with simultaneous antifouling, easy-to-clean, and anti-fog functionality is presented based on smart polymer films consisting of copolymers with 2-methacryloyloxyethyl phosphorylcholine (MPC), realizing the function of the film and photoreactive 4-benzophenyl methacrylate (BPO), which is responsible for stability and crosslinking. The easy-to-clean effect is demonstrated qualitatively and quantitatively by oil droplet detachment experiments. The antifouling behavior against different germs is investigated by cell adhesion experiments. Furthermore the anti-fog performance is shown by breathing on the surfaces. To study the influence of the different amounts of copolymerized BPO, the grafted films are characterized by atomic force microscopy (AFM), infrared spectroscopy (ATR-FTIR), as well as contact angle measurements. In situ spectroscopic ellipsometry is performed to investigate the swelling behavior of the thin films as a function of the time of UV-irradiation. It is found that a degree of swelling of 15 and a water contact angle of less than 12° are the key parameters necessary for the generation of multifunctional coatings. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemAdvances and Trends in Chemically Doped Graphene(Weinheim : Wiley-VCH, 2020) Ullah, Sami; Shi, Qitao; Zhou, Junhua; Yang, Xiaoqin; Ta, Huy Q.; Hasan, Maria; Ahmad, Nasir Mahmood; Fu, Lei; Bachmatiuk, Alicja; Rümmeli, Mark H.Chemically doped graphene materials are fascinating because these have different desirable attributes with possible synergy. The inert and gapless nature of graphene can be changed by adding a small number of heteroatoms to substitute carbon in the lattice. The doped material may display superior catalytic activities; durable, fast, and selective sensing; improved magnetic moments; photoresponses; and activity in chemical reactions. In the current review, recent advances are covered in chemically doped graphene. First, the different types of heteroatoms, their bonding configurations, and briefly their properties are discussed. This is followed by the description of various synthesis and analytical methods essential for assessing the characteristics of heterographene with specific focus on the selected graphene materials of different dopants (particularly, single dopants, including N, B, S, P, first three halogens, Ge, and Ga, and codopants, such as N/O), and more importantly, up-to-date applications enabled by the intentional doping. Finally, outlook and perspectives section review the existing challenges, future opportunities, and possible ways to improve the graphitic materials. The goal is to update and inspire the readers to establish novel doped graphene with valuable properties and for current and futuristic applications. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemIncreasing Antibacterial Efficiency of Cu Surfaces by targeted Surface Functionalization via Ultrashort Pulsed Direct Laser Interference Patterning(Weinheim : Wiley-VCH, 2020) Müller, Daniel W.; Lößlein, Sarah; Terriac, Emmanuel; Brix, Kristina; Siems, Katharina; Moeller, Ralf; Kautenburger, Ralf; Mücklich, FrankCopper (Cu) exhibits great potential for application in the design of antimicrobial contact surfaces aiming to reduce pathogenic contamination in public areas as well as clinically critical environments. However, current application perspectives rely purely on the toxic effect of emitted Cu ions, without considering influences on the interaction of pathogenic microorganisms with the surface to enhance antimicrobial efficiency. In this study, it is investigated on how antibacterial properties of Cu surfaces against Escherichia coli can be increased by tailored functionalization of the substrate surface by means of ultrashort pulsed direct laser interference patterning (USP-DLIP). Surface patterns in the scale range of single bacteria cells are fabricated to purposefully increase bacteria/surface contact area, while parallel modification of the surface chemistry allows to involve the aspect of surface wettability into bacterial attachment and the resulting antibacterial effectivity. The results exhibit a delicate interplay between bacterial adhesion and the expression of antibacterial properties, where a reduction of bacterial cell viability of up to 15-fold can be achieved for E. coli on USP-DLIP surfaces in comparison to smooth Cu surfaces. Thereby, it can be shown how the antimicrobial properties of copper surfaces can be additionally enhanced by targeted surface functionalization. © 2020 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH
- ItemFlexible Materials for High-Resolution 3D Printing of Microfluidic Devices with Integrated Droplet Size Regulation(Washington, DC : ACS Publications, 2021) Weigel, Niclas; Männel, Max J.; Thiele, JulianWe develop resins for high-resolution additive manufacturing of flexible micromaterials via projection microstereolithography (PμSL) screening formulations made from monomer 2-phenoxyethyl acrylate, the cross-linkers Ebecryl 8413, tri(propyleneglycol) diacrylate or 1,3,5-triallyl-1,3,5-triazine-2,4,6(1H,3H,5H)-trione, the photoabsorber Sudan 1, and the photoinitiator diphenyl(2,4,6-trimethylbenzoyl)phosphine oxide. PμSL-printed polymer micromaterials made from this resin library are characterized regarding achievable layer thickness depending on UV exposure energy, and for mechanical as well as optical properties. The best-candidate resin from this screening approach allows for 3D-printing transparent microchannels with a minimum cross section of approximately 35 × 46 μm2, which exhibit proper solvent resistance against water, isopropanol, ethanol, n-hexane, and HFE-7500. The mechanical properties are predestined for 3D-printing microfluidic devices with integrated functional units that require high material flexibility. Exemplarily, we design flexible microchannels for on-demand regulation of microdroplet sizes in microemulsion formation. Our two outlines of integrated droplet regulators operate by injecting defined volumes of air, which deform the droplet-forming microchannel cross-junction, and change the droplet size therein. With this study, we expand the library of functional resins for PμSL printing toward flexible materials with micrometer resolution and provide the basis for further exploration of these materials, e.g., as microstructured cell-culturing substrates with defined mechanics. © 2021 American Chemical Society. All rights reserved.
- ItemPolymer Brushes on Graphitic Carbon Nitride for Patterning and as a SERS Active Sensing Layer via Incorporated Nanoparticles(Washington, DC : Soc., 2020) Sheng, Wenbo; Li, Wei; Tan, Deming; Zhang, Panpan; Zhang, En; Sheremet, Evgeniya; Schmidt, Bernhard V.K.J.; Feng, Xinliang; Rodriguez, Raul D.; Jordan, Rainer; Amin, IhsanGraphitic carbon nitride (gCN) has a broad range of promising applications, from energy harvesting and storage to sensing. However, most of the applications are still restricted due to gCN poor dispersibility and limited functional groups. Herein, a direct photografting of gCN using various polymer brushes with tailorable functionalities via UV photopolymerization at ambient conditions is demonstrated. The systematic study of polymer brush-functionalized gCN reveals that the polymerization did not alter the inherent structure of gCN. Compared to the pristine gCN, the gCN-polymer composites show good dispersibility in various solvents such as water, ethanol, and tetrahydrofuran (THF). Patterned polymer brushes on gCN can be realized by employing photomask and microcontact printing technology. The polymer brushes with incorporated silver nanoparticles (AgNPs) on gCN can act as a multifunctional recyclable active sensing layer for surface-enhanced Raman spectroscopy (SERS) detection and photocatalysis. This multifunctionality is shown in consecutive cycles of SERS and photocatalytic degradation processes that can be applied to in situ monitor pollutants, such as dyes or pharmaceutical waste, with high chemical sensitivity as well as to water remediation. This dual functionality provides a significant advantage to our AgNPs/polymer-gCN with regard to state-of-the-art systems reported so far that only allow SERS pollutant detection but not their decomposition. These results may provide a new methodology for the covalent functionalization of gCN and may enable new applications in the field of catalysis, biosensors, and, most interestingly, environmental remediation. Copyright © 2020 American Chemical Society.