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- von Nickisch-Rosenegk, Markus (1)
- von Plessen, Gero (1)
- von Reppert, Alexander (1)
- von Websky, Karoline (1)
- von Zander, Robert Edler (1)
- Öner, Ibrahim Halil (1)
- Özcan, Onur (1)
Year of publication
Document Type
- Article (2394) (remove)
Is part of the Bibliography
- yes (2394) (remove)
Keywords
- Conformational analysis (14)
- biomaterials (13)
- nanoparticles (13)
- fluorescence (12)
- Palladium (11)
- singlet oxygen (11)
- Fluorescence (10)
- SERS (10)
- block copolymers (10)
- conformational analysis (10)
Institute
- Institut für Chemie (2394) (remove)
Neusser, David ; Sun, Bowen ; Tan, Wen Liang ; Thomsen, Lars ; Schultz, Thorsten ; Perdigon-Toro, Lorena ; Koch, Norbert ; Shoaee, Safa ; McNeill, Christopher R. ; Neher, Dieter ; Ludwigs, Sabine
Recent advances in organic solar cell performance have been mainly driven forward by combining high-performance p-type donor-acceptor copolymers (e.g.PM6) and non-fullerene small molecule acceptors (e.g.Y6) as bulk-heterojunction layers. A general observation in such devices is that the device performance, e.g., the open-circuit voltage, is strongly dependent on the processing solvent. While the morphology is a typically named key parameter, the energetics of donor-acceptor blends are equally important, but less straightforward to access in the active multicomponent layer. Here, we propose to use spectral onsets during electrochemical cycling in a systematic spectroelectrochemical study of blend films to access the redox behavior and the frontier orbital energy levels of the individual compounds. Our study reveals that the highest occupied molecular orbital offset (Delta E-HOMO) in PM6:Y6 blends is similar to 0.3 eV, which is comparable to the binding energy of Y6 excitons and therefore implies a nearly zero driving force for the dissociation of Y6 excitons. Switching the PM6 orientation in the blend films from face-on to edge-on in bulk has only a minor influence on the positions of the energy levels, but shows significant differences in the open circuit voltage of the device. We explain this phenomenon by the different interfacial molecular orientations, which are known to affect the non-radiative decay rate of the charge-transfer state. We compare our results to ultraviolet photoelectron spectroscopy data, which shows distinct differences in the HOMO offsets in the PM6:Y6 blend compared to neat films. This highlights the necessity to measure the energy levels of the individual compounds in device-relevant blend films.
Structure, mechanical properties and degradation behavior of electrospun PEEU fiber meshes and films
(2021)
The capability of a degradable implant to provide mechanical support depends on its degradation behavior. Hydrolytic degradation was studied for a polyesteretherurethane (PEEU70), which consists of poly(p-dioxanone) (PPDO) and poly(epsilon-caprolactone) (PCL) segments with a weight ratio of 70:30 linked by diurethane junction units. PEEU70 samples prepared in the form of meshes with average fiber diameters of 1.5 mu m (mesh1.5) and 1.2 mu m (mesh1.2), and films were sterilized and incubated in PBS at 37 degrees C with 5 vol% CO2 supply for 1 to 6 weeks. Degradation features, such as cracks or wrinkles, became apparent from week 4 for all samples. Mass loss was found to be 11 wt%, 6 wt%, and 4 wt% for mesh1.2, mesh1.5, and films at week 6. The elongation at break decreased to under 20% in two weeks for mesh1.2. In case of the other two samples, this level of degradation was achieved after 4 weeks. The weight average molecular weight of both PEEU70 mesh and film samples decreased to below 30 kg/mol when elongation at break dropped below 20%. The time period of sustained mechanical stability of PEEU70-based meshes depends on the fiber diameter and molecular weight.
Stefancu, Andrei ; Nan, Lin ; Zhu, Li ; Chis, Vasile ; Bald, Ilko ; Liu, Min ; Leopold, Nicolae ; Maier, Stefan A. ; Cortes, Emiliano
Plasmon-driven dehalogenation of brominated purines has been recently explored as a model system to understand fundamental aspects of plasmon-assisted chemical reactions. Here, it is shown that divalent Ca2+ ions strongly bridge the adsorption of bromoadenine (Br-Ade) to Ag surfaces.
Such ion-mediated binding increases the molecule's adsorption energy leading to an overlap of the metal energy states and the molecular states, enabling the chemical interface damping (CID) of the plasmon modes of the Ag nanostructures (i.e., direct electron transfer from the metal to Br-Ade).
Consequently, the conversion of Br-Ade to adenine almost doubles following the addition of Ca2+.
These experimental results, supported by theoretical calculations of the local density of states of the Ag/Br-Ade complex, indicate a change of the charge transfer pathway driving the dehalogenation reaction, from Landau damping (in the lack of Ca2+ ions) to CID (after the addition of Ca2+).
The results show that the surface dynamics of chemical species (including water molecules) play an essential role in charge transfer at plasmonic interfaces and cannot be ignored. It is envisioned that these results will help in designing more efficient nanoreactors, harnessing the full potential of plasmon-assisted chemistry.
Informatische Bildung spielt eine immer zentralere Rolle in der Bildung einer Gesellschaft des 21. Jahrhunderts. Für den Chemieunterricht ergeben sich daraus zwei Aspekte: Einerseits können Konzepte der informatischen Bildung dabei helfen, chemie- und naturwissenschaftsspezifische Denk- und Arbeitsweisen zu fördern. Andererseits kann der Chemieunterricht einen Beitrag für die informatische Bildung leisten. Dieser Artikel geht auf beide Aspekte ein und versucht die gegenseitigen Vorteile der informatischen Bildung und der naturwissenschaftlichen Bildung im Chemieunterricht darzustellen.
Zhao, Yuhang ; Opitz, Andreas ; Eljarrat, Alberto ; Kochovski, Zdravko ; Koch, Christoph ; Koch, Norbert ; Lu, Yan
In this study, the kinetics of the adsorption of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F(4)TCNQ) on the surface of Ag nanoparticles (Ag NPs) in chloroform has been intensively investigated, as molecular doping is known to play a crucial role in organic electronic devices. Based on the results obtained from UV-visible (vis)-near-infrared (NIR) absorption spectroscopy, cryogenic transmission electron microscopy, scanning nanobeam electron diffraction, and electron energy loss spectroscopy, a two-step interaction kinetics has been proposed for the Ag NPs and F(4)TCNQ molecules, which includes the first step of electron transfer from Ag NPs to F(4)TCNQ indicated by the ionization of F(4)TCNQ and the second step of the formation of a Ag-F(4)TCNQ complex. The whole process has been followed via UV-vis-NIR absorption spectroscopy, which reveals distinct kinetics at two stages: the instantaneous ionization and the long-term complex formation. The kinetics and the influence of the molar ratio of Ag NPs/F(4)TCNQ molecules on the interaction between Ag NPs and F(4)TCNQ molecules in an organic solution are reported herein for the first time. Furthermore, the control experiment with silica-coated Ag NPs manifests that the charge transfer at the surface between Ag NPs and F(4)TCNQ molecules is prohibited by a silica layer of 18 nm.
Sulfated biomolecules are known to influence numerous biological processes in all living organisms. Particularly, they contribute to prevent and inhibit the hypercoagulation condition. The failure of polymeric implants and blood contacting devices is often related to hypercoagulation and microbial contamination. Here, bioactive sulfated biomacromolecules are mimicked by sulfation of poly(glycerol glycidyl ether) (polyGGE) films. Autoclaving, gamma-ray irradiation and ethylene oxide (EtO) gas sterilization techniques were applied to functionalized materials. The sulfate group density and hydrophilicity of sulfated polymers were decreased while chain mobility and thermal degradation were enhanced post autoclaving when compared to those after EtO sterilization. These results suggest that a quality control after sterilization is mandatory to ensure the amount and functionality of functionalized groups are retained.
Michaelis, Vivien ; Aengenheister, Leonie ; Tuchtenhagen, Max ; Rinklebe, Jörg ; Ebert, Franziska ; Schwerdtle, Tanja ; Buerki-Thurnherr, Tina ; Bornhorst, Julia
Manganese (Mn) as well as iron (Fe) are essential trace elements (TE) important for the maintenance of physiological functions including fetal development. However, in the case of Mn, evidence suggests that excess levels of intrauterine Mn are associated with adverse pregnancy outcomes. Although Mn is known to cross the placenta, the fundamentals of Mn transfer kinetics and mechanisms are largely unknown. Moreover, exposure to combinations of TEs should be considered in mechanistic transfer studies, in particular for TEs expected to share similar transfer pathways. Here, we performed a mechanistic in vitro study on the placental transfer of Mn across a BeWo b30 trophoblast layer. Our data revealed distinct differences in the placental transfer of Mn and Fe. While placental permeability to Fe showed a clear inverse dose-dependency, Mn transfer was largely independent of the applied doses. Concurrent exposure of Mn and Fe revealed transfer interactions of Fe and Mn, indicating that they share common transfer mechanisms. In general, mRNA and protein expression of discussed transporters like DMT1, TfR, or FPN were only marginally altered in BeWo cells despite the different exposure scenarios highlighting that Mn transfer across the trophoblast layer likely involves a combination of active and passive transport processes.
Crovetto, Andrea ; Kojda, Danny ; Yi, Feng ; Heinselman, Karen N. ; LaVan, David A. ; Habicht, Klaus ; Unold, Thomas ; Zakutayev, Andriy
Numerous phosphorus-rich metal phosphides containing both P-P bonds and metal-P bonds are known from the solid-state chemistry literature. A method to grow these materials in thin-film form would be desirable, as thin films are required in many applications and they are an ideal platform for high-throughput studies. In addition, the high density and smooth surfaces achievable in thin films are a significant advantage for characterization of transport and optical properties. Despite these benefits, there is hardly any published work on even the simplest binary phosphorus-rich phosphide films. Here, we demonstrate growth of single-phase CuP2 films by a two-step process involving reactive sputtering of amorphous CuP2+x and rapid annealing in an inert atmosphere. At the crystallization temperature, CuP2 is thermodynamically unstable with respect to Cu3P and P-4. However, CuP2 can be stabilized if the amorphous precursors are mixed on the atomic scale and are sufficiently close to the desired composition (neither too P poor nor too P rich). Fast formation of polycrystalline CuP2, combined with a short annealing time, makes it possible to bypass the diffusion processes responsible for decomposition. We find that thin-film CuP2 is a 1.5 eV band gap semiconductor with interesting properties, such as a high optical absorption coefficient (above 10(5) cm(-1)), low thermal conductivity (1.1 W/(K m)), and composition-insensitive electrical conductivity (around 1 S/cm). We anticipate that our processing route can be extended to other phosphorus-rich phosphides that are still awaiting thin-film synthesis and will lead to a more complete understanding of these materials and of their potential applications.
Tung, Wing Tai ; Maring, Janita A. ; Xu, Xun ; Liu, Yue ; Becker, Matthias ; Somesh, Dipthi Bachamanda ; Klose, Kristin ; Wang, Weiwei ; Sun, Xianlei ; Ullah, Imran ; Kratz, Karl ; Neffe, Axel T. ; Stamm, Christof ; Ma, Nan ; Lendlein, Andreas
Guidance of postinfarct myocardial remodeling processes by an epicardial patch system may alleviate the consequences of ischemic heart disease. As macrophages are highly relevant in balancing immune response and regenerative processes their suitable instruction would ensure therapeutic success. A polymeric mesh capable of attracting and instructing monocytes by purely physical cues and accelerating implant degradation at the cell/implant interface is designed. In a murine model for myocardial infarction the meshes are compared to those either coated with extracellular matrix or loaded with induced cardiomyocyte progenitor cells. All implants promote macrophage infiltration and polarization in the epicardium, which is verified by in vitro experiments. 6 weeks post-MI, especially the implantation of the mesh attenuates left ventricular adverse remodeling processes as shown by reduced infarct size (14.7% vs 28-32%) and increased wall thickness (854 mu m vs 400-600 mu m), enhanced angiogenesis/arteriogenesis (more than 50% increase compared to controls and other groups), and improved heart function (ejection fraction = 36.8% compared to 12.7-31.3%). Upscaling as well as process controls is comprehensively considered in the presented mesh fabrication scheme to warrant further progression from bench to bedside.
Binary III-V nitrides such as AlN, GaN and InN in the wurtzite-type structure have long been considered as potent semiconducting materials because of their optoelectronic properties, amongst others. With rising concerns over the utilization of scarce elements, a replacement of the trivalent cations by others in ternary and multinary nitrides has led to the development of different variants of nitrides and oxide nitrides crystallizing in lower-symmetry variants of wurtzite. This work presents the symmetry relationships between these structural types specific to nitrides and oxide nitrides and updates some prior work on this matter. The non-existence of compounds crystallizing in Pmc2(1), formally the highest subgroup of the wurtzite type fulfilling Pauling's rules for 1:1:2 stoichiometries, has been puzzling scientists for a while; a rationalization is given, from a crystallographic basis, of why this space group is unlikely to be adopted.