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981.
Alexander Dundua Steffen Franzka Mathias Ulbricht 《Macromolecular rapid communications》2016,37(24):2030-2036
Nonspecific adsorption of proteins is a challenging problem for the development of biocompatible materials, as well as for antifouling and fouling‐release coatings, for instance for the marine industry. The concept of preparing amphiphilic systems based on low surface energy hydrophobic materials via their hydrophilic modification is being widely pursued. This work describes a novel two‐step route for the preparation of interpenetrating polymer networks of otherwise incompatible poly(dimethylsiloxane) and zwitterionic polymers. Changes in surface hydrophilicity as well as surface charge at different pH values are investigated. Characterization using atomic force microscopy provides thorough insight into surface changes upon hydrophilic modification. Protein fouling of the materials is assessed using fibrinogen as a model protein.
982.
Steffen?KionkeEmail authorView authors OrcID profile 《Monatshefte für Mathematik》2017,182(4):851-863
We define generalized Collatz mappings on free abelian groups of finite rank and study their iteration trajectories. Using geometric arguments we describe cones of points having a divergent trajectory and we deduce lower bounds for the density of the set of divergent points. As an application we give examples which show that the iteration of generalized Collatz mappings on rings of algebraic integers can behave quite differently from the conjectured behavior in \(\mathbb {Z}\). 相似文献
983.
Marcus Schulze Dr. Andreas Steffen Prof. Dr. Frank Würthner 《Angewandte Chemie (International ed. in English)》2015,54(5):1570-1573
The phosphorescence emission of perylene bisimide derivatives has been rarely reported. Two novel ruthenium(II) and iridium(III) complexes of an azabenz‐annulated perylene bisimide (ab‐PBI), [Ru(bpy)2(ab‐PBI)][PF6]2 1 and [Cp*Ir(ab‐PBI)Cl]PF6 2 are now presented that both show NIR phosphorescence between 750–1000 nm in solution at room temperature. For an NIR emitter, the ruthenium complex 1 displays an unusually high quantum yield (Φp) of 11 % with a lifetime (τp) of 4.2 μs, while iridium complex 2 exhibits Φp<1 % and τp=33 μs. 1 and 2 are the first PBI‐metal complexes in which the spin–orbit coupling is strong enough to facilitate not only the Sn→Tn intersystem crossing of the PBI dye, but also the radiative T1→S0 transition, that is, phosphorescence. 相似文献
984.
Phosphine‐Catalyzed β,γ‐Umpolung Domino Reaction of Allenic Esters: Facile Synthesis of Tetrahydrobenzofuranones Bearing a Chiral Tetrasubstituted Stereogenic Carbon Center 下载免费PDF全文
Dr. Shinobu Takizawa Kenta Kishi Dr. Yasushi Yoshida Steffen Mader Dr. Fernando Arteaga Arteaga Shoukou Lee Dr. Manabu Hoshino Prof. Dr. Magnus Rueping Prof. Dr. Makoto Fujita Prof. Dr. Hiroaki Sasai 《Angewandte Chemie (International ed. in English)》2015,54(51):15511-15515
An enantio‐, diastereo‐, regio‐, and chemoselective phosphine‐catalyzed β,γ‐umpolung domino reaction of allenic esters with dienones has been developed for the first time. The designed sequence, involving oxy‐Michael and Rauhut–Currier reactions, produced highly functionalized tetrahydrobenzofuranones, bearing a chiral tetrasubstituted stereogenic center, in up to 96 % ee. 相似文献
985.
Multi‐frequency (S,X, Q and W‐band) EPR and ENDOR Study of Vanadium(IV) Incorporation in the Aluminium Metal–Organic Framework MIL‐53 下载免费PDF全文
Irena Nevjestić Hannes Depauw Dr. Karen Leus Dr. Vidmantas Kalendra Dr. Ignacio Caretti Prof. Gunnar Jeschke Prof. Sabine Van Doorslaer Prof. Freddy Callens Prof. Pascal Van Der Voort Dr. Henk Vrielinck 《Chemphyschem》2015,16(14):2968-2973
Doping the well‐known metal–organic framework MIL‐53(Al) with vanadium(IV) ions leads to significant changes in the breathing behaviour and might have repercussions on the catalytic behaviour as well. To understand the properties of such a doped framework, it is necessary to determine where dopant ions are actually incorporated. Electron paramagnetic resonance (EPR) and electron–nuclear double resonance (ENDOR) are applied to reveal the nearest environment of the paramagnetic vanadium(IV) dopant ions. EPR spectra of as‐synthesised vanadium‐doped MIL‐53 are recorded at S‐, X‐, Q‐ and W‐band microwave frequencies. The EPR spectra suggest that at low dopant concentrations (1.0–2.6 mol %) the vanadium(IV) ions are well dispersed in the matrix. Varying the vanadium dopant concentration within this range or the dopant salt leads to the same dominant EPR component. In the ENDOR spectra, hyperfine (HF) interactions with 1H, 27Al and 51V nuclei are observed. The HF parameters extracted from simulations strongly suggest that the vanadium(IV) ions substitute Al in the framework. 相似文献
986.
Angel A. Martí Steffen Jockusch Zengmin Li Bindu Raveendra Irina Morozova Daniel L. Akins Nicholas J. Turro 《Tetrahedron》2007,63(17):3591-3600
We report the design, synthesis, and characterization of binary oligonucleotide probes for mRNA detection. The probes were designed to avoid common problems found in standard binary probes such as direct excitation of the acceptor fluorophore and overlap between the donor and acceptor emission spectra. Two different probes were constructed that contained an array of either two or three dyes and were characterized using steady-state fluorescence spectroscopy, time-resolved fluorescence spectroscopy, and fluorescence depolarization measurements. The three-dye binary probe (BP-3d) consists of a Fam fluorophore which acts as a donor, collecting light and transferring it as energy to Tamra, which subsequently transfers energy to Cy5 when the two probes are hybridized to mRNA. This design allows the use of 488 nm excitation, which avoids the direct excitation of Cy5 and at the same time provides a good fluorescence resonance energy transfer (FRET) efficiency. The two-dye binary probe system (BP-2d) was constructed with Alexa488 and Cy5 fluorophores. Although the overlap between the fluorescence of Alexa488 and the absorption of Cy5 is relatively low, FRET still occurs due to their close physical proximity when the probes are hybridized to mRNA. This framework also decreases the direct excitation of Cy5 and reduces the fluorescence overlap between the donor and the acceptor. Picosecond time-resolved spectroscopy showed a reduction in the fluorescence lifetime of donor fluorophores after the formation of the hybrid between the probes and target mRNA. Interestingly, BP-2d in the presence of mRNA shows a slow rise in the fluorescence decay of Cy5 due to a relatively slow FRET rate, which together with the reduction in the Alexa488 lifetime provides a way to improve the signal to background ratio using time-resolved fluorescence spectra (TRES). In addition, fluorescence depolarization measurements showed complete depolarization of the acceptor dyes (Cy5) for both BP-3d (due to sequential FRET steps) and BP-2d (due to the relatively low FRET rate) in the presence of the mRNA target. 相似文献
987.
Yoder NC Kalsani V Schuy S Vogel R Janshoff A Kumar K 《Journal of the American Chemical Society》2007,129(29):9037-9043
A growing body of literature suggests that fluorocarbons can direct self-assembly within hydrocarbon environments. We report here the fabrication and characterization of supported lipid bilayers (SLBs) composed of 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) and a synthetic, fluorocarbon-functionalized analogue, 1. AFM investigation of these model membranes reveals an intricate, composition-dependent domain structure consisting of approximately 50 nm stripes interspersed between approximately 1 microm sized domains. Although DSC of 1 showed a phase transition near room temperature, DSC of DPPC:1 mixtures exhibited complex phase behavior suggesting domain segregation. Finally, temperature-dependent AFM of DPPC:1 bilayers shows that, while the stripe structures can be melted above the Tm of 1, the stripes and domains result from immiscibility of the hydrocarbon and fluorocarbon lipid gel phases. Fluorination appears to be a promising strategy for chemical self-assembly in two dimensions. In particular, because no modification is made to the lipid headgroups, it may be useful for nanopatterning biologically relevant ligands on bilayers in vitro or in living cells. 相似文献
988.
The first disiloxanediolate complexes of cerium(IV) are reported. Starting from the readily available precursor ((t)BuO)(3)Ce(IV)(NO(3))(THF)(2) (1), we prepared the novel heterobimetallic compounds [{(Ph(2)SiO)(2)O}{K(THF)(2)}](2)Ce(O(t)Bu)(2) (2) and [{(Ph(2)SiO)(2)O}(2){(DME)-KO(t)Bu}{(Ph(2)SiO(2))K}Ce](2) (3) and structurally characterized them by X-ray diffraction. 相似文献
989.
990.
Steffen A Thiele C Tietze S Strassnig C Kämper A Lengauer T Wenz G Apostolakis J 《Chemistry (Weinheim an der Bergstrasse, Germany)》2007,13(24):6801-6809
We report the computer-aided optimization of a synthetic receptor for a given guest molecule, based on inverse virtual screening of receptor libraries. As an example, a virtual set of beta-cyclodextrin (beta-CD) derivatives was generated as receptor candidates for the anticancer drug camptothecin. We applied the two docking tools AutoDock and GlamDock to generate camptothecin complexes of every candidate receptor. Scoring functions were used to rank all generated complexes. From the 10 % top-ranking candidates nine were selected for experimental validation. They were synthesized by reaction of heptakis-[6-deoxy-6-iodo]-beta-CD with a thiol compound to form the hepta-substituted beta-CDs. The stabilities of the camptothecin complexes obtained from solubility measurements of five of the nine CD derivatives were significantly higher than for any other CD derivative known from literature. The remaining four CD derivatives were insoluble in water. In addition, corresponding mono-substituted CD derivatives were synthesized that also showed improved binding constants. Among them the 9-H-purine derivative was the best, being comparable to the investigated hepta-substituted beta-CDs. Since the measured binding free energies correlated satisfactorily with the calculated scores, the applied scoring functions appeared to be appropriate for the selection of promising candidates for receptor synthesis. 相似文献