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- ItemSynthesis of Modified Poly(vinyl Alcohol)s and Their Degradation Using an Enzymatic Cascade(Weinheim : Wiley-VCH, 2023) von Haugwitz, Gerlis; Donnelly, Kian; Di Filippo, Mara; Breite, Daniel; Phippard, Max; Schulze, Agnes; Wei, Ren; Baumann, Marcus; Bornscheuer, Uwe T.Poly(vinyl alcohol) (PVA) is a water-soluble synthetic vinyl polymer with remarkable physical properties including thermostability and viscosity. Its biodegradability, however, is low even though a large amount of PVA is released into the environment. Established physical-chemical degradation methods for PVA have several disadvantages such as high price, low efficiency, and secondary pollution. Biodegradation of PVA by microorganisms is slow and frequently involves pyrroloquinoline quinone (PQQ)-dependent enzymes, making it expensive due to the costly cofactor and hence unattractive for industrial applications. In this study, we present a modified PVA film with improved properties as well as a PQQ-independent novel enzymatic cascade for the degradation of modified and unmodified PVA. The cascade consists of four steps catalyzed by three enzymes with in situ cofactor recycling technology making this cascade suitable for industrial applications.
- ItemDeveloping a Laser Induced Liquid Beam Ion Desorption Spectral Database as Reference for Spaceborne Mass Spectrometers(Malden, Mass. : American Geophysical Union, 2022) Klenner, Fabian; Umair, Muhammad; Walter, Sebastian H. G.; Khawaja, Nozair; Hillier, Jon; Nölle, Lenz; Zou, Zenghui; Napoleoni, Maryse; Sanderink, Arnaud; Zuschneid, Wilhelm; Abel, Bernd; Postberg, FrankSpaceborne impact ionization mass spectrometers, such as the Cosmic Dust Analyzer on board the past Cassini spacecraft or the SUrface Dust Analyzer being built for NASA's upcoming Europa Clipper mission, are of crucial importance for the exploration of icy moons in the Solar System, such as Saturn's moon Enceladus or Jupiter's moon Europa. For the interpretation of data produced by these instruments, analogue experiments on Earth are essential. To date, thousands of laboratory mass spectra have been recorded with an analogue experiment for impact ionization mass spectrometers. Simulation of mass spectra of ice grains in space is achieved by a Laser Induced Liquid Beam Ion Desorption (LILBID) approach. The desorbed cations or anions are analyzed in a time-of-flight mass spectrometer. The amount of unstructured raw data is increasingly challenging to sort, process, interpret and compare with data from space. Thus far this has been achieved manually for individual mass spectra because no database containing the recorded reference spectra was available. Here we describe the development of a comprehensive, extendable database containing cation and anion mass spectra from the laboratory LILBID facility. The database is based on a Relational Database Management System with a web server interface and enables filtering of the laboratory data using a wide range of parameters. The mass spectra can be compared not only with data from past and future space missions but also mass spectral data generated by other, terrestrial, techniques. The validated and approved subset of the database is available for general public (https://lilbid-db.planet.fu-berlin.de).
- ItemCurvature model for nanoparticle size effects on peptide fibril stability and molecular dynamics simulation data(Amsterdam [u.a.] : Elsevier, 2022) John, Torsten; Martin, Lisandra L.; Risselada, Herre Jelger; Abel, BerndNanostructured surfaces are widespread in nature and are being further developed in materials science. This makes them highly relevant for biomolecules, such as peptides. In this data article, we present a curvature model and molecular dynamics (MD) simulation data on the influence of nanoparticle size on the stability of amyloid peptide fibrils related to our research article entitled “Mechanistic insights into the size-dependent effects of nanoparticles on inhibiting and accelerating amyloid fibril formation” (John et al., 2022) [1]. We provide the code to perform MD simulations in GROMACS 4.5.7 software of arbitrarily chosen biomolecule oligomers adsorbed on a curved surface of chosen nanoparticle size. We also provide the simulation parameters and data for peptide oligomers of Aß40, NNFGAIL, GNNQQNY, and VQIYVK. The data provided allows researchers to further analyze our MD simulations and the curvature model allows for a better understanding of oligomeric structures on surfaces.
- ItemCryo-printed microfluidics enable rapid prototyping for optical-cell analysis(Heidelberg : Springer, 2022) Garmasukis, Rokas; Hackl, Claudia; Dusny, Christian; Elsner, Christian; Charvat, Ales; Schmid, Andreas; Abel, BerndThis paper highlights an innovative, low-cost rapid-prototyping method for generating microfluidic chips with extraordinary short fabrication times of only a few minutes. Microchannels and inlet/outlet ports are created by controlled deposition of aqueous microdroplets on a cooled surface resulting in printed ice microstructures, which are in turn coated with a UV-curable acrylic cover layer. Thawing leaves an inverse imprint as a microchannel structure. For an exemplary case, we applied this technology for creating a microfluidic chip for cell-customized optical-cell analysis. The chip design includes containers for cell cultivation and analysis. Container shape, length, position, and angle relative to the main channel were iteratively optimized to cultivate and analyze different cell types. With the chip, we performed physiological analyses of morphologically distinct prokaryotic Corynebacterium glutamicum DM1919, eukaryotic Hansenula polymorpha RB11 MOX-GFP, and phototrophic Synechocystis sp. PCC 6803 cells via quantitative time-lapse fluorescence microscopy. The technology is not limited to rapid prototyping of complex biocompatible microfluidics. Further exploration may include printing with different materials other than water, printing on other substrates in-situ biofunctionalization, the inclusion of electrodes and many other applications.
- ItemHeterobimetallic conducting polymers based on salophen complexes via electrosynthesis(London [u.a.] : RSC, 2023) Bia, Francesca; Gualandi, Isacco; Griebel, Jan; Rasmussen, Leon; Hallak, Bassam; Tonelli, Domenica; Kersting, BertholdIn this work, we report the first electrochemical synthesis of two copolymeric bimetallic conducting polymers by a simple anodic electropolymerization method. The adopted precursors are electroactive transition metal (M = Ni, Cu and Fe) salophen complexes, which can be easily obtained by direct chemical synthesis. The resulting films, labeled poly-NiCu and poly-CuFe, were characterized by cyclic voltammetry in both organic and aqueous media, attenuated total reflectance Fourier transform infrared spectroscopy, UV-vis spectroscopy, scanning electron microscopy, and coupled energy dispersive X-ray spectroscopy. The films are conductive and exhibit great electrochemical stability in both organic and aqueous media (resistant over 100 cycles without significant loss in current response or changes in electrochemical behavior), which makes them good candidates for an array of potential applications. Electrochemical detection of ascorbic acid was performed using both materials.
- ItemTarget ion and neutral spread in high power impulse magnetron sputtering(New York, NY : Inst., 2022) Hajihoseini, H.; Brenning, N.; Rudolph, M.; Raadu, M.A.; Lundin, D.; Fischer, J.; Minea, T. M.; Gudmundsson, J.T.In magnetron sputtering, only a fraction of the sputtered target material leaving the ionization region is directed toward the substrate. This fraction may be different for ions and neutrals of the target material as the neutrals and ions can exhibit a different spread as they travel from the target surface toward the substrate. This difference can be significant in high power impulse magnetron sputtering (HiPIMS) where a substantial fraction of the sputtered material is known to be ionized. Geometrical factors or transport parameters that account for the loss of produced film-forming species to the chamber walls are needed for experimental characterization and modeling of the magnetron sputtering discharge. Here, we experimentally determine transport parameters for ions and neutral atoms in a HiPIMS discharge with a titanium target for various magnet configurations. Transport parameters are determined to a typical substrate, with the same diameter (100 mm) as the cathode target, and located at a distance 70 mm from the target surface. As the magnet configuration and/or the discharge current are changed, the transport parameter for neutral atoms ζ tn remains roughly the same, while transport parameters for ions ζ ti vary greatly. Furthermore, the relative ion-to-neutral transport factors, ζ ti / ζ tn, that describe the relative deposited fractions of target material ions and neutrals onto the substrate, are determined to be in the range from 0.4 to 1.1.
- ItemLow-temperature atmospheric pressure plasma conversion of polydimethylsiloxane and polysilazane precursor layers to oxide thin films(Weinheim : Wiley VCH, 2023) Rudolph, Martin; Birtel, Peter; Arnold, Thomas; Prager, Andrea; Naumov, Sergej; Helmstedt, Ulrike; Anders, André; With, Patrick C.We study the conversion of two polymeric silicon precursor compound layers (perhydropolysilazane and polydimethylsiloxane) on a silicon wafer and polyethylene terephthalate substrates to silicon oxide thin films using a pulsed atmospheric pressure plasma jet. Varying the scan velocity and the number of treatments results in various film compositions, as determined by X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy. The mechanism suggested for the conversion process includes the decomposition of the precursor triggered by plasma-produced species, the oxidation of the surface, and finally, the diffusion of oxygen into the film, while gases produced during the precursor decomposition diffuse out of the film. The latter process is possibly facilitated by local plasma heating of the surface. The precursor conversion appears to depend sensitively on the balance between the different contributions to the conversion mechanism.
- ItemInfluence of wavelength and accumulated fluence at picosecond laser-induced surface roughening of copper on secondary electron yield(Melville, NY : American Inst. of Physics, 2023) Bez, Elena; Himmerlich, Marcel; Lorenz, Pierre; Ehrhardt, Martin; Gunn, Aidan Graham; Pfeiffer, Stephan; Rimoldi, Martino; Taborelli, Mauro; Zimmer, Klaus; Chiggiato, Paolo; Anders, AndréUltrashort-pulse laser processing of copper is performed in air to reduce the secondary electron yield (SEY). By UV (355 nm), green (532 nm), and IR (1064 nm) laser-light induced surface modification, this study investigates the influence of the most relevant experimental parameters, such as laser power, scanning speed, and scanning line distance (represented as accumulated fluence) on the ablation depth, surface oxidation, topography, and ultimately on the SEY. Increasing the accumulated laser fluence results in a gradual change from a Cu 2 O to a CuO-dominated surface with deeper micrometer trenches, higher density of redeposited surface particles from the plasma phase, and a reduced SEY. While the surface modifications are less pronounced for IR radiation at low accumulated fluence (,1000 J/cm2 ), analogous results are obtained for all wavelengths when reaching the nonlinear absorption regime, for which the SEY maximum converges to 0.7. Furthermore, independent of the extent of the structural transformations, an electron-induced surface conditioning at 250 eV allows a reduction of the SEY maximum below unity at doses of 5×10 -4 C/mm2 . Consequently, optimization of processing parameters for application in particle accelerators can be obtained for a sufficiently low SEY at controlled ablation depth and surface particle density, which are factors that limit the surface impedance and the applicability of the material processing for ultrahigh vacuum systems. The relations between pro- cessing parameters and surface features will provide guidance in treating the surface of vacuum components, especially beam screens of selected magnets of the Large Hadron Collider or of future colliders.
- ItemInvestigating the morphology of bulk heterojunctions by laser photoemission electron microscopy(Amsterdam [u.a.] : Elsevier Science, 2022) Niefind, Falk; Shivhare, Rishi; Mannsfeld, Stefan C.B.; Abel, Bernd; Hambsch, MikeThe nanoscale morphology of bulk heterojunctions is highly important for the charge dissociation and transport in organic solar cells and ultimately defines the performance of the cell. The visualization of this nano-morphology in terms of domain size and polymer orientation in a fast and straightforward way is therefore of great interest to evaluate the suitability of a film for efficient solar cells. Here, we demonstrate that the morphology of different blends of poly(3-hexylthiophene-2,5-diyl) (P3HT) and phenyl-C61-butyric acid methyl ester (PCBM) can be imaged and analyzed by employing photoemission electron microscopy.
- ItemA study on the material properties of novel PEGDA/gelatin hybrid hydrogels polymerized by electron beam irradiation(Lausanne : Frontiers Media, 2023) Şener Raman, Tuğçe; Kuehnert, Mathias; Daikos, Olesya; Scherzer, Tom; Krömmelbein, Catharina; Mayr, Stefan G.; Abel, Bernd; Schulze, AgnesGelatin-based hydrogels are highly desirable biomaterials for use in wound dressing, drug delivery, and extracellular matrix components due to their biocompatibility and biodegradability. However, insufficient and uncontrollable mechanical properties and degradation are the major obstacles to their application in medical materials. Herein, we present a simple but efficient strategy for a novel hydrogel by incorporating the synthetic hydrogel monomer polyethylene glycol diacrylate (PEGDA, offering high mechanical stability) into a biological hydrogel compound (gelatin) to provide stable mechanical properties and biocompatibility at the resulting hybrid hydrogel. In the present work, PEGDA/gelatin hybrid hydrogels were prepared by electron irradiation as a reagent-free crosslinking technology and without using chemical crosslinkers, which carry the risk of releasing toxic byproducts into the material. The viscoelasticity, swelling behavior, thermal stability, and molecular structure of synthesized hybrid hydrogels of different compound ratios and irradiation doses were investigated. Compared with the pure gelatin hydrogel, 21/9 wt./wt. % PEGDA/gelatin hydrogels at 6 kGy exhibited approximately up to 1078% higher storage modulus than a pure gelatin hydrogel, and furthermore, it turned out that the mechanical stability increased with increasing irradiation dose. The chemical structure of the hybrid hydrogels was analyzed by Fourier-transform infrared (FTIR) spectroscopy, and it was confirmed that both compounds, PEGDA and gelatin, were equally present. Scanning electron microscopy images of the samples showed fracture patterns that confirmed the findings of viscoelasticity increasing with gelatin concentration. Infrared microspectroscopy images showed that gelatin and PEGDA polymer fractions were homogeneously mixed and a uniform hybrid material was obtained after electron beam synthesis. In short, this study demonstrates that both the presence of PEGDA improved the material properties of PEGDA/gelatin hybrid hydrogels and the resulting properties are fine-tuned by varying the irradiation dose and PEGDA/gelatin concentration.