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Wolf, Jana ; Flieger, Yannic ; Diewald, Felix ; Langenbach, Kai ; Stephan, Simon ; Hasse, Hans ; Müller, Ralf
Surface wetting can be simulated using a phase field approach which describes the continuous liquid-gas transition with the help of an order parameter. In this publication, wetting of non-planar surfaces is investigated based on a phase field model by Diewald et al. [1, 2]. Different scenarios of droplets on rough surfaces are simulated. The static equilibrium for those scenarios is calculated using an Allen-Cahn evolution equation. The influence of the surface morphology on the resulting contact angle is investigated while the width of the phase transition from liquid to gas is varied as a model parameter.
Meiers, Dominic T. ; Rothammer, Maximilian ; Maier, Maximilian ; Zollfrank, Cordt ; Freymann, Georg von
The great flexibility of direct laser writing (DLW) arises from the possibility to fabricate precise three-dimensional structures on very small scales as well as the broad range of applicable materials. However, there is still a vast number of promising materials, which are currently inaccessible requiring the continuous development of novel photoresists. Herein, a new bio-sourced resist is reported that uses the monomeric unit of chitin, N-acetyl-D-glucosamine, paving the way from existing hydrogel resists based on animal carbohydrates to a new class of non-hydrogel ones. In addition, it is shown that the combined use of two photoinitiators is advantageous over the use of a single one. In this approach, the first photoinitiator is a good two-photon absorber at the applied wavelength, while the second photoinitiator exhibits poor two-photon absorbtion abilities, but is better suited for cross-linking of the monomer. The first photoinitiator absorbs the light acting as a sensitizer and transfers the energy to the second initiator, which subsequently forms a radical and initializes the polymerization. This sensitization effect enables a new route to utilize reactive photointiators with a small two-photon absorption cross section for DLW without changing their chemical structure.
Malchau, Christian ; Fries, Daniela V. ; Mees, Yannick ; Jakobs, Marisa F. ; Sun, Yu ; Becker, Sabine ; Niedner-Schatteburg, Gereon ; Thiel, Werner R.
Starting from [(η5-cyclopentadienyl)(η6-phenyl)iron(II)]imidazole, dicationic imidazolium salts were prepared by N-alkylation. Reaction of these compounds with basic metal precursors such as mesityl copper(I) or palladium(II) acetate led to mono respectively dicationic transition metal NHC complexes (NHC=N-heterocyclic carbene). Transmetalation using the copper(I) complexes opened up the access to NHC gold(I) compounds. PEPPSI-type NHC complexes of palladium(II) and platinum(II) were prepared by offering a neutral pyridine ligand to the transition metal center. A rhodium(I) NHC complex was accessible by deprotonation of the dicationic imidazolium precursor and subsequent treatment with [(COD)Rh(μ2-Cl)]2 (COD=1,5-cyclooctadiene). The new NHC complexes were investigated by means of NMR spectroscopy, mass spectrometry as well as single crystal X-ray structure analysis. Both, the palladium(II) containing PEPPSI-type and the gold(I) complex, were investigated for their catalytic properties in typical model reactions such as cyclization reactions, Suzuki coupling and cyanation. In addition, a selenium adduct was synthesized in order to study the electronic properties of the underlying ligand backbone. Based on the chemical shift in the 77Se NMR spectrum, it is evident that these NHC ligands possess rather poor π-acidity.
Janus materials are anisotropic nano- and microarchitectures with two different faces consisting of distinguishable or opposite physicochemical properties. In parallel with the discovery of new methods for the fabrication of these materials, decisive progress has been made in their application, for example, in biological science, catalysis, pharmaceuticals, and, more recently, in battery technology. This Minireview systematically covers recent and significant achievements in the application of task-specific Janus nanomaterials as heterogeneous catalysts in various types of chemical reactions, including reduction, oxidative desulfurization and dye degradation, asymmetric catalysis, biomass transformation, cascade reactions, oxidation, transition-metal-catalyzed cross-coupling reactions, electro- and photocatalytic reactions, as well as gas-phase reactions. Finally, an outlook on possible future applications is given.
Carius, Yvonne ; Ries, Fabian ; Gries, Karin ; Trentmann, Oliver ; D. Lancaster, C. Roy ; Willmund, Felix
The folding of newly synthesized polypeptides requires the coordinated action of molecular chaperones. Prokaryotic cells and the chloroplasts of plant cells possess the ribosome-associated chaperone trigger factor, which binds nascent polypeptides at their exit stage from the ribosomal tunnel. The structure of bacterial trigger factor has been well characterized and it has a dragon-shaped conformation, with flexible domains responsible for ribosome binding, peptidyl-prolyl cis–trans isomerization (PPIase) activity and substrate protein binding. Chloroplast trigger-factor sequences have diversified from those of their bacterial orthologs and their molecular mechanism in plant organelles has been little investigated to date. Here, the crystal structure of the plastidic trigger factor from the green alga Chlamydomonas reinhardtii is presented at 2.6 Å resolution. Due to the high intramolecular flexibility of the protein, diffraction to this resolution was only achieved using a protein that lacked the N-terminal ribosome-binding domain. The eukaryotic trigger factor from C. reinhardtii exhibits a comparable dragon-shaped conformation to its bacterial counterpart. However, the C-terminal chaperone domain displays distinct charge distributions, with altered positioning of the helical arms and a specifically altered charge distribution along the surface responsible for substrate binding. While the PPIase domain shows a highly conserved structure compared with other PPIases, its rather weak activity and an unusual orientation towards the C-terminal domain points to specific adaptations of eukaryotic trigger factor for function in chloroplasts.
Krieg, Sara-Cathrin ; Grimmer, Jennifer ; Pick, Annika Maria ; Kelm, Harald ; Breugst, Martin ; Manolikakes, Georg
An improved route for the highly stereoselective synthesis of (Z)-2-oxyenamides is reported. The desired products can be accessed in only three steps from aminoacetaldehyde dimethyl acetal as common, readily available building block in a highly modular fashion. The improved procedure has been applied to the synthesis of various acylated and sufonylated oxyenamides. Mechanistic and theoretical studies provide a conclusive rationale for the observed stereoselectivities.
Scaled boundary isogeometric analysis (SB-IGA) describes the computational domain by proper boundary NURBS together with a well-defined scaling center; see [5]. More precisely, we consider star convex domains whose domain boundaries correspond to a sequence of NURBS curves and the interior is determined by a scaling of the boundary segments with respect to a chosen scaling center. However, providing a decomposition into star shaped blocks one can utilize SB-IGA also for more general shapes. Even though several geometries can be described by a single patch, in applications frequently there appear multipatch structures. Whereas a C0 continuous patch coupling can be achieved relatively easily, the situation becomes more complicated if higher regularity is required. Consequently, a suitable coupling method is inevitably needed for analyses that require global C1 continuity.In this contribution we apply the concept of analysis-suitable G1 parametrizations [2] to the framework of SB-IGA for the C1 coupling of planar domains with a special consideration of the scaling center. We obtain globally C1 regular basis functions and this enables us to handle problems such as the Kirchhoff-Love plate and shell, where smooth coupling is an issue. Furthermore, the boundary representation within SB-IGA makes the method suitable for the concept of trimming. In particular, we see the possibility to extend the coupling procedure to study trimmed plates and shells.The approach was implemented using the GeoPDEs package [1] and its performance was tested on several numerical examples. Finally, we discuss the advantages and disadvantages of the proposed method and outline future perspectives.
Print path-dependent contact temperature dependency for 3D printing using fused filament fabrication
(2022)
This paper focuses on the effects of different time spans and thus different contact temperatures when a molten strand contacts an adjacent already solidified strand in a plane during 3D printing with fused filament fabrication. For this purpose, both the manufacturing parameters and the geometry of the component are systematically varied and the effect on morphology and mechanical properties is investigated. The results clearly show that even with identical printing parameters, the transitions between the individual layers are much more visible with long time spans until fusion and lead to low mechanical properties. In contrast, short spans lead to hardly visible welds and high mechanical properties. Transferring the findings to different component sizes ultimately verifies that the average temperature at the time of contact between the already solidified and the currently deposited strand is decisive for component quality. In order to generate high component qualities, this finding must therefore be taken into account in the future in the path generation strategy, i.e., in so-called slicing.
Methods for predicting Henry's law constants Hij are important as experimental data are scarce. We introduce a new machine learning approach for such predictions: matrix completion methods (MCMs) and demonstrate its applicability using a data base that contains experimental Hij values for 101 solutes i and 247 solvents j at 298 K. Data on Hij are only available for 2661 systems i + j. These Hij are stored in a 101 × 247 matrix; the task of the MCM is to predict the missing entries. First, an entirely data-driven MCM is presented. Its predictive performance, evaluated using leave-one-out analysis, is similar to that of the Predictive Soave-Redlich-Kwong equation-of-state (PSRK-EoS), which, however, cannot be applied to all studied systems. Furthermore, a hybrid of MCM and PSRK-EoS is developed in a Bayesian framework, which yields an unprecedented performance for the prediction of Hij of the studied data set.
Based on conservation of resources theory, this paper examines the mediating mechanisms in the relationship between digital affordances and employee corporate entrepreneurship participation likelihood. Findings from an experimental study with 207 employees show a statistically significant and positive indirect effect of digital affordances on employee corporate entrepreneurship participation likelihood through employee-perceived information technology support for innovation and a statistically significant and—contrary to our expectations—positive indirect effect through employee-perceived work overload. Results are corroborated by insights from in-depth interviews with senior managers. They provide support for digital affordances as action potentials that are associated with resource gains that in turn foster employee corporate entrepreneurship participation likelihood.