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Divergent Solid‐Phase Synthesis of Natural Product‐Inspired Bipartite Cyclodepsipeptides: Total Synthesis of Seragamide A
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Prof. Dr. Hans‐Dieter Arndt Dr. Stefano Rizzo M. Sc. Christina Nöcker Dr. Vijay N. Wakchaure Dr. Lech‐Gustav Milroy B. Sc. Vanessa Bieker Dr. Abram Calderon Dr. Tuyen T. N. Tran Dr. Silke Brand Dr. Leif Dehmelt Prof. Dr. Herbert Waldmann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(14):5311-5316
Macrocyclic natural products (NPs) and analogues thereof often show high affinity, selectivity, and metabolic stability, and methods for the synthesis of NP‐like macrocycle collections are of major current interest. We report an efficient solid‐phase/cyclorelease method for the synthesis of a collection of macrocyclic depsipeptides with bipartite peptide/polyketide structure inspired by the very potent F‐actin stabilizing depsipeptides of the jasplakinolide/geodiamolide class. The method includes the assembly of an acyclic precursor chain on a polymeric carrier, terminated by olefins that constitute complementary fragments of the polyketide section and cyclization by means of a relay‐ring‐closing metathesis (RRCM). The method was validated in the first total synthesis of the actin‐stabilizing cyclodepsipeptide seragamide A and the synthesis of a collection of structurally diverse bipartite depsipeptides. 相似文献
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Dr. Ralph P. G. Bosmans Jeroen M. Briels Dr. Lech‐Gustav Milroy Dr. Tom F. A. de Greef Prof. Maarten Merkx Prof. Luc Brunsveld 《Angewandte Chemie (International ed. in English)》2016,55(31):8899-8903
Supramolecular split‐enzyme complementation restores enzymatic activity and allows for on–off switching. Split‐luciferase fragment pairs were provided with an N‐terminal FGG sequence and screened for complementation through host‐guest binding to cucurbit[8]uril (Q8). Split‐luciferase heterocomplex formation was induced in a Q8 concentration dependent manner, resulting in a 20‐fold upregulation of luciferase activity. Supramolecular split‐luciferase complementation was fully reversible, as revealed by using two types of Q8 inhibitors. Competition studies with the weak‐binding FGG peptide revealed a 300‐fold enhanced stability for the formation of the ternary heterocomplex compared to binding of two of the same fragments to Q8. Stochiometric binding by the potent inhibitor memantine could be used for repeated cycling of luciferase activation and deactivation in conjunction with Q8, providing a versatile module for in vitro supramolecular signaling networks. 相似文献
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R D Patterson R Milroy R A Lutfi 《The Journal of the Acoustical Society of America》1983,73(3):951-954
Samples of wideband noise 0.05, 0.1, 0.2, or 0.4 s in duration were digitized and then replayed cyclically to produce repeated-noise maskers. The signal was a repeating tone burst (0.4 or 1.6 kHz). It was half the duration of the noise sample, centered in the noise temporally, and it was repeated at the same point in each repetition of the noise. In the antiphasic conditions of the experiment, either the noise sample or the tone burst was inverted in alternate repetitions of the masker; in the homophasic conditions both the tone burst and noise, or neither, were inverted in alternative repetitions. If the auditory system were capable of storing detailed waveforms of sufficient length, alternate repetitions could be added or subtracted and we might expect a release from masking in the antiphasic conditions. The results show a small but significant advantage for the antiphasic conditions when the signal frequency was 0.4 kHz, but no difference with the 1.6-kHz signal. 相似文献
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Interchange modes have been a key limiting instability for many magnetic confinement fusion configurations. In previous studies intended to deal with these ubiquitous instabilities, complex, transport enhancing, minimum-B producing coils were added to the otherwise simple linear mirror plasma. Possible solutions for returning to a simple symmetric mirror configuration, such as ponderomotive fields, are weak and difficult to apply. A new method is demonstrated here for the first time, utilizing rotating magnetic fields that are simple to apply and highly effective. A simple and easily comprehensible theory has also been developed to explain the remarkable stabilizing properties. Although this work has been performed on field reversed configurations, it should have a wide application to other confinement schemes, and could become a cornerstone for high-beta plasma stability. 相似文献
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LANGLEY J. K. 《中国科学 数学(英文版)》2010,(3)
We determine all real meromorphic functions f in the plane such that f has finitely many zeros, the poles of f have bounded multiplicities, and f and F have finitely many non-real zeros, where F is a linear differential polynomial given by F = f (k) +Σk-1j=0ajf(j) , in which k≥2 and the coefficients aj are real numbers with a0≠0. 相似文献
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Dr. Katja Petkau‐Milroy Dr. Michael H. Sonntag Prof. Dr. Luc Brunsveld 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(33):10786-10793
Self‐assembly of discotic molecules into supramolecular polymers offers a flexible approach for the generation of multicomponent one‐dimensional columnar architectures with tuneable biomedical properties. Decoration with ligands induces specific binding of the self‐assembled scaffold to biological targets. The modular design allows the easy co‐assembly of different discotics for the generation of probes for targeted imaging and cellular targeting with adjustable ligand density and composition. 相似文献
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Generation of gas‐phase ions from charged clusters: an important ionization step causing suppression of matrix and analyte ions in matrix‐assisted laser desorption/ionization mass spectrometry
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