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General Synthetic Route toward Highly Dispersed Metal Clusters Enabled by Poly(ionic liquid)s
(2017)
The ability to synthesize a broad spectrum of metal clusters (MCs) with their size controllable on a subnanometer scale presents an enticing prospect for exploring nanosize-dependent properties. Here we report an innovative design of a capping agent from a polytriazolium poly(ionic liquid) (PIL) in a vesicular form in solution that allows for crafting a variety of MCs including transition metals, noble metals, and their bimetallic alloy with precisely controlled sizes (similar to 1 nm) and record-high catalytic performance. The ultrastrong stabilization power is a result of an unusual synergy between the conventional binding sites in the heterocyclic cations in PIL and an in situ generated polycarbene structure induced simultaneously to the reduction reaction.
Recently, we proposed a new strategy to construct artificial plant protein assemblies, which were induced by adding a small molecule, based on dual supramolecular interactions. In this paper, we further explored this method by employing Human Galectin-1 (Gal-1) as a building block to form self-assembled microribbons. Two non-covalent interactions, including lactose-lectin binding and dimerization of Rhodamine B (RhB), induced by the small molecule ligand addition, were involved in the crosslinking of the animal protein, resulting in the formation of assemblies. By using transmission electron microscopy (TEM), cryo-electron microscopy (cryo-EM), and three-dimensional (3D) tomographic analysis, we arrived at a possible mechanistic model for the microribbon formation. Furthermore, the morphology of protein assemblies could be fine-timed by varying the incubation time, the protein/ligand ratio, and the chemical structures of ligands. Interestingly, the formation of protein microribbons successfully inhibited Gal-1 induced T-cell agglutination and apoptosis. This is because the multivalent and dynamic interactions in protein assemblies compete with the binding between Gal-1 and the glycans on cell surfaces, which suppresses the function of Gal-1 in promotion of tumor progression and metastasis.
Magnetic fields play important roles in many astrophysical processes. However, there is no universal diagnostic for the magnetic fields in the interstellar medium (ISM) and each magnetic tracer has its limitation. Any new detection method is thus valuable. Theoretical studies have shown that submillimetre fine-structure lines are polarized due to atomic alignment by ultraviolet photon-excitation, which opens up a new avenue to probe interstellar magnetic fields. We will, for the first time, perform synthetic observations on the simulated three-dimensional ISM to demonstrate the measurability of the polarization of submillimetre atomic lines. The maximum polarization for different absorption and emission lines expected from various sources, including star-forming regions are provided. Our results demonstrate that the polarization of submillimetre atomic lines is a powerful magnetic tracer and add great value to the observational studies of the submilimetre astronomy.
Increasing interests in hydrocarbon resources at depths have drawn greater attentions to the deeply-buried carbonate reservoirs in the Tarim Basin in China. In this study, the cyclic dolomite rocks of Upper Cambrian Lower Qiulitag Group from four outcrop sections in northwestern Tarim Basin were selected to investigate and evaluate the petrophysical properties in relation to depositional facies and cyclicity. The Lower Qiulitag Group includes ten lithofacies, which were deposited in intermediate to shallow subtidal, restricted shallow subtidal, intertidal, and supratidal environments on a carbonate ramp system. These lithofacies are vertically stacked into repeated shallowing-upward, meter-scale cycles which are further grouped into six third-order depositional sequences (Sq1 to Sq6). There are variable types of pore spaces in the Lower Qiulitag Group dolomite rocks, including interparticle, intraparticle, and fenestral pores of primary origin, inter crystal, and vuggy pores of late diagenetic modification. The porosity in the dolomites is generally facies-selective as that the microbially-originated thrombolites and stromatolites generally yield a relatively high porosity. In contrast, the high-energy ooidal grainstones generally have very low porosity. In this case, the microbialite-based peritidal cycles and peritidal cycle-dominated highstand (or regressive) successions have relatively high volumes of pore spaces, although highly fluctuating (or vertical inhomogeneous). Accordingly, the grainstone-based subtidal cycles and subtidal cycle-dominated transgressive successions generally yield extremely low porosity. This scenario indicates that porosity development and preservation in the thick dolomite successions are primarily controlled by depositional facies which were influenced by sea-level fluctuations of different orders and later diagenetic overprinting.
This paper studies cosmic-ray (CR) transport in magnetohydrodynamic (MHD) turbulence. CR transport is strongly dependent on the properties of the magnetic turbulence.
We perform test particle simulations to study the interactions of CR with both total MHD turbulence and decomposed MHD modes.
The spatial diffusion coefficients and the pitch angle scattering diffusion coefficients are calculated from the test particle trajectories in turbulence.
Our results confirm that the fast modes dominate the CR propagation, whereas Alfven and slow modes are much less efficient and have shown similar pitch-angle scattering rates.
We investigate the cross field transport on large and small scales. On large/global scales, normal diffusion is observed and the diffusion coefficient is suppressed by M-A(zeta) compared to the parallel diffusion coefficients, with zeta closer to 4 in Alfven modes than that in total turbulence, as theoretically expected.
For the CR transport on scales smaller than the turbulence injection scale, both the local and global magnetic reference frames are adopted. Superdiffusion is observed on such small scales in all the cases. Particularly, CR transport in Alfven modes show clear Richardson diffusion in the local reference frame. The diffusion transitions smoothly from the Richardson's one with index 1.5 to normal diffusion as the particle mean free path decreases from lambda(parallel to) >> L to lambda(parallel to) << L, where L is the injection/coherence length of turbulence.
Our results have broad applications to CRs in various astrophysical environments.
Tailoring the secondary surface morphology of electro-spun nanofibers has been highly desired, as such delicate structures equip nanofibers with distinct functions. Here, we report a simple strategy to directly reconstruct the surface of polyvinyl alcohol/polyvinylpyrrolidone (PVA/PVP) nanofibers by water evaporation. The roughness and diameter of the nanofibers depend on the temperature during vacuum drying. Surface changes of the nanofibers from smooth to rough were observed at 55 degrees C, with a significant drop in nanofiber diameter. We attribute the formation of the secondary surface morphology to the intermolecular forces in the water vapor, including capillary and the compression forces, on the basis of the results from the Fourier-transform infrared (FTIR) and X-ray photoelectron (XPS) spectroscopy. The strategy is universally effective for various electro-spun polymer nanofibers, thus opening up avenues toward more detailed and sophisticated structure design and implementation for nanofibers.
Background/Aims: Angiogenesis plays a key role during embryonic development. The vascular endothelin (ET) system is involved in the regulation of angiogenesis. Lipopolysaccharides (LPS) could induce angiogenesis. The effects of ET blockers on baseline and LPS-stimulated angiogenesis during embryonic development remain unknown so far. Methods: The blood vessel density (BVD) of chorioallantoic membranes (CAMs), which were treated with saline (control), LPS, and/or BQ123 and the ETB blocker BQ788, were quantified and analyzed using an IPP 6.0 image analysis program. Moreover, the expressions of ET-1, ET-2, ET3, ET receptor A (ETRA), ET receptor B (ETRB) and VEGFR2 mRNA during embryogenesis were analyzed by semi-quantitative RT-PCR. Results: All components of the ET system are detectable during chicken embryogenesis. LPS increased angiogenesis substantially. This process was completely blocked by the treatment of a combination of the ETA receptor blockers-BQ123 and the ETB receptor blocker BQ788. This effect was accompanied by a decrease in ETRA, ETRB, and VEGFR2 gene expression. However, the baseline angiogenesis was not affected by combined ETA/ETB receptor blockade. Conclusion: During chicken embryogenesis, the LPS-stimulated angiogenesis, but not baseline angiogenesis, is sensitive to combined ETA/ETB receptor blockade. (C) 2018 The Author(s) Published by S. Karger AG, Basel
Background/Aims: Angiogenesis plays a key role during embryonic development. The vascular endothelin (ET) system is involved in the regulation of angiogenesis. Lipopolysaccharides (LPS) could induce angiogenesis. The effects of ET blockers on baseline and LPS-stimulated angiogenesis during embryonic development remain unknown so far. Methods: The blood vessel density (BVD) of chorioallantoic membranes (CAMs), which were treated with saline (control), LPS, and/or BQ123 and the ETB blocker BQ788, were quantified and analyzed using an IPP 6.0 image analysis program. Moreover, the expressions of ET-1, ET-2, ET3, ET receptor A (ETRA), ET receptor B (ETRB) and VEGFR2 mRNA during embryogenesis were analyzed by semi-quantitative RT-PCR. Results: All components of the ET system are detectable during chicken embryogenesis. LPS increased angiogenesis substantially. This process was completely blocked by the treatment of a combination of the ETA receptor blockers-BQ123 and the ETB receptor blocker BQ788. This effect was accompanied by a decrease in ETRA, ETRB, and VEGFR2 gene expression. However, the baseline angiogenesis was not affected by combined ETA/ETB receptor blockade. Conclusion: During chicken embryogenesis, the LPS-stimulated angiogenesis, but not baseline angiogenesis, is sensitive to combined ETA/ETB receptor blockade.
Human sulfite oxidase (hSO) is a homodimeric two-domain enzyme central in the biological sulfur cycle. A pyranopterin molybdenum cofactor (Moco) is the catalytic site and a heme b(5) group located in the N-terminal domain. The two domains are connected by a flexible linker region. Electrons produced at the Moco in sulfite oxidation, are relayed via heme b(5) to electron acceptors or an electrode surface. Inter-domain conformational changes between an open and a closed enzyme conformation, allowing "gated" electron transfer has been suggested. We first recorded cyclic voltammetry (CV) of hSO on single-crystal Au(111)-electrode surfaces modified by self-assembled monolayers (SAMs) both of a short rigid thiol, cysteamine and of a longer structurally flexible thiol, omega-amino-octanethiol (AOT). hSO on cysteamine SAMs displays a well-defined pair of voltammetric peaks around -0.207 V vs. SCE in the absence of sulfite substrate, but no electrocatalysis. hSO on AOT SAMs displays well-defined electrocatalysis, but only "fair" quality voltammetry in the absence of sulfite. We recorded next in situ scanning tunnelling spectroscopy (STS) of hSO on AOT modified Au(111)-electrodes, disclosing, a 2-5 % surface coverage of strong molecular scale contrasts, assigned to single hSO molecules, notably with no contrast difference in the absence and presence of sulfite. In situ STS corroborated this observation with a sigmoidal tunnelling current/overpotential correlation.
Rapid decline of glomerular filtration rate estimated from creatinine (eGFRcrea) is associated with severe clinical endpoints. In contrast to cross-sectionally assessed eGFRcrea, the genetic basis for rapid eGFRcrea decline is largely unknown. To help define this, we meta-analyzed 42 genome-wide association studies from the Chronic Kidney Diseases Genetics Consortium and United Kingdom Biobank to identify genetic loci for rapid eGFRcrea decline. Two definitions of eGFRcrea decline were used: 3 mL/min/1.73m(2)/year or more ("Rapid3"; encompassing 34,874 cases, 107,090 controls) and eGFRcrea decline 25% or more and eGFRcrea under 60 mL/min/1.73m(2) at follow-up among those with eGFRcrea 60 mL/min/1.73m(2) or more at baseline ("CKDi25"; encompassing 19,901 cases, 175,244 controls). Seven independent variants were identified across six loci for Rapid3 and/or CKDi25: consisting of five variants at four loci with genome-wide significance (near UMOD-PDILT (2), PRKAG2, WDR72, OR2S2) and two variants among 265 known eGFRcrea variants (near GATM, LARP4B). All these loci were novel for Rapid3 and/or CKDi25 and our bioinformatic follow-up prioritized variants and genes underneath these loci. The OR2S2 locus is novel for any eGFRcrea trait including interesting candidates. For the five genome-wide significant lead variants, we found supporting effects for annual change in blood urea nitrogen or cystatin-based eGFR, but not for GATM or (LARP4B). Individuals at high compared to those at low genetic risk (8-14 vs. 0-5 adverse alleles) had a 1.20-fold increased risk of acute kidney injury (95% confidence interval 1.08-1.33). Thus, our identified loci for rapid kidney function decline may help prioritize therapeutic targets and identify mechanisms and individuals at risk for sustained deterioration of kidney function.