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61.
A convenient three‐step route toward a functionalized pyrrole building block for novel anti‐inflammatory agents is reported. In contrast to previous strategies, the present approach focuses on inexpensive starting materials and application on a multigram scale. A high degree of functional diversity is demonstrated in various derivatives, and the scope and limitations of this route are discussed. Complementary to the described tetrasubstituted pyrroles, a novel ring‐closure protocol based on the Feist–Benary condensation affords trisubstituted analogues. 相似文献
62.
Frank Hörmann Prof. Dr. Andreas Hirsch 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(9):3188-3197
We report here on the facile synthetic access of a new family of bis‐, tetra‐, hexa‐, and heptafullerenes (prototypes I–IV), which can be easily converted into very water soluble polyelectrolytes with up to 60 charges located on their periphery. Their very regioselective formation is based on the use of C2v‐symmetrical pentakisadducts 3 and hexakisadducts 2 as key intermediates. All fullerene moieties incorporated in these macromolecular structures involve a complete or partial octahedral addition pattern. Tripod‐shaped tetrafullerenes 9 a , b (type II), which can accumulate up to thirty positive or negative charges, are very soluble in acidic or basic water, respectively. Hexafullerenes 13 a , b (type III) were synthesized via isoxazolinofullerenes 10 followed by photolytic cleavage of the isoxazoline group. The giant heptafullerene 1 b (type IV) representing the anionic counterpart of the previously synthesized polyelectrolyte 1 a can store up to 60 negative charges on its periphery within a defined three‐dimensional structure. We also discovered a new cyclopropanation reaction of C60 involving dibromomalonates and 1,8‐diazabicyclo[5.4.0]undec‐7‐ene (DBU). This reaction allows even for the highly regioselective formation of hexakisadducts with an octahedral addition pattern without requiring activation with reversibly binding addends such as 9,10‐dimethylanthracene (DMA). 相似文献
63.
Qiuqin Zhou Florian Grundmann Marcel Kaiser Matthias Schiell Dr. Sophie Gaudriault Dr. Andreas Batzer Dr. Michael Kurz Prof. Dr. Helge B. Bode 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(49):16772-16779
During the search for novel natural products from entomopathogenic Xenorhabdus doucetiae DSM17909 and X. mauleonii DSM17908 novel peptides named xenoamicins were identified in addition to the already known antibiotics xenocoumacin and xenorhabdin. Xenoamicins are acylated tridecadepsipeptides consisting of mainly hydrophobic amino acids. The main derivative xenoamicin A ( 1 ) was isolated from X. mauleonii DSM17908, and its structure elucidated by detailed 1 D and 2 D NMR experiments. Detailed MS experiments, also in combination with labeling experiments, confirmed the determined structure and allowed structure elucidation of additional derivatives. Moreover, the xenoamicin biosynthesis gene cluster was identified and analyzed in X. doucetiae DSM17909, and its participation in xenoamicin biosynthesis was confirmed by mutagenesis. Advanced Marfey’s analysis of 1 showed that the absolute configuration of the amino acids is in agreement with the predicted stereochemistry deduced from the nonribosomal peptide synthetase XabABCD. Biological testing revealed activity of 1 against Plasmodium falciparum and other neglected tropical diseases but no antibacterial activity. 相似文献
64.
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66.
Gas thrust bearings are often used in low-load applications, e.g. in air cycle machines, in micro gas turbines or in rotor systems for fuel cell applications, to support a shaft in axial direction. The pressure and temperature distribution in a gas thrust bearing pad are described by the generalized Reynolds equation according to Dowson and the 3D energy equation. In this paper, two different approaches are presented in order to reduce the dimension of the governing nonlinear integro-differential equation system and in order to stabilize the solution process. In the first reduction approach, the temperature in the fluid is averaged across the fluid film according to Lee and Kim. In the second approach, Legendre polynomials are used to approximate temperature, density and fluidity across the fluid film according to Elrod, Brewe and Moraru. The reduction techniques are compared with respect to numerical efficiency, accuracy and convergence behavior. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
67.
Metal sheet forming processes like deep drawing are applied in order to produce carriage parts in mass production. Therefore, forming tools are required that are well protected against wear. For such forming tools, wear resistant surfaces are, e.g., produced by thermal spraying of hard material coatings. The thermal spraying process itself is a highly transient thermo-mechanical process. In order to gain a better understanding of the heat input and transfer during thermal spraying, a simulation framework for thermal spraying processes is presented. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
68.
Andreas Leng Cornelius Weiß Nina Straßner Prof. Dr. Andreas Hirsch 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(53):e202201446
An unprecedented compound class of functional organic hybrids consisting of a photoswitchable norbornadiene building block and a redoxactive chromophore, namely naphthalene diimide, were designed and synthesized. Within these structures the capability of rylene chromophores to function as a redox active catalyst upon their photoexcitation was utilized to initiate the oxidative back-conversion of the in situ formed quadricyclane unit to its norbornadiene analogue. In this way successive photoexcitation at two different wavelengths enabled a controlled photoswitching between the two isomerical states of the hybrids. Beyond this prove of concept, the dependency of the reaction rate to the intramolecular distance of the two functional molecular building blocks as well as the concentration of the photoexcited sample was monitored. The experimental findings and interpretations were furthermore supported by quantum chemical investigations. 相似文献
69.
We address the problem of "nonlocal computation," in which separated parties must compute a function without any individual learning anything about the inputs. Surprisingly, entanglement provides no benefit over local classical strategies for such tasks, yet stronger nonlocal correlations allow perfect success. This provides intriguing insights into the limits of quantum information processing, the nature of quantum nonlocality, and the differences between quantum and stronger-than-quantum nonlocal correlations. 相似文献
70.
Permanently fixed noisily recorded refractive index gratings are discovered in single crystals of LiNbO(3):Fe upon long-term exposure to a single laser beam with high intensities of I=100 kW/m(2) and ambient temperature. The fixing process is explained by considering the effect of laser-induced heating of the sample and the well-known simultaneous thermal fixing procedure. 相似文献