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排序方式: 共有261条查询结果,搜索用时 15 毫秒
11.
Emily C. Monkcom Daniël de Bruin Annemiek J. de Vries Dr. Martin Lutz Dr. Shengfa Ye Prof. Dr. Robertus J. M. Klein Gebbink 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(16):5191-5204
We present the synthesis and coordination chemistry of a bulky, tripodal N,N,O ligand, ImPh2NNO t Bu ( L ), designed to model the 2-His-1-carboxylate facial triad (2H1C) by means of two imidazole groups and an anionic 2,4-di-tert-butyl-subtituted phenolate. Reacting K-L with MCl2 (M = Fe, Zn) affords the isostructural, tetrahedral non-heme complexes [Fe(L)(Cl)] ( 1 ) and [Zn(L)(Cl)] ( 2 ) in high yield. The tridentate N,N,O ligand coordination observed in their X-ray crystal structures remains intact and well-defined in MeCN and CH2Cl2 solution. Reacting 2 with NaSPh affords a tetrahedral zinc thiolate complex, [Zn(L)(SPh)] ( 4 ), that is relevant to isopenicillin N synthase (IPNS) biomimicry. Cyclic voltammetry studies demonstrate the ligand's redox non-innocence, where phenolate oxidation is the first electrochemical response observed in K-L , 2 and 4 . However, the first electrochemical oxidation in 1 is iron-centred, the assignment of which is supported by DFT calculations. Overall, ImPh2NNO t Bu provides access to well-defined mononuclear, monoligated, N,N,O-bound metal complexes, enabling more accurate structural modelling of the 2H1C to be achieved. 相似文献
12.
An Efficient Labelling Approach to Harness Backbone and Side‐Chain Protons in 1H‐Detected Solid‐State NMR Spectroscopy 下载免费PDF全文
Deni Mance Dr. Tessa Sinnige Mohammed Kaplan Siddarth Narasimhan Mark Daniëls Dr. Klaartje Houben Prof. Marc Baldus Dr. Markus Weingarth 《Angewandte Chemie (International ed. in English)》2015,54(52):15799-15803
1H‐detection can greatly improve spectral sensitivity in biological solid‐state NMR (ssNMR), thus allowing the study of larger and more complex proteins. However, the general requirement to perdeuterate proteins critically curtails the potential of 1H‐detection by the loss of aliphatic side‐chain protons, which are important probes for protein structure and function. Introduced herein is a labelling scheme for 1H‐detected ssNMR, and it gives high quality spectra for both side‐chain and backbone protons, and allows quantitative assignments and aids in probing interresidual contacts. Excellent 1H resolution in membrane proteins is obtained, the topology and dynamics of an ion channel were studied. This labelling scheme will open new avenues for the study of challenging proteins by ssNMR. 相似文献
13.
Sebastian Milster Tobias Grünbaum Sebastian Bange Simon Kurrmann Hermann Kraus Dani M. Stoltzfus Anna E. Leung Tamim A. Darwish Paul L. Burn Christoph Boehme John M. Lupton 《Angewandte Chemie (International ed. in English)》2020,59(24):9388-9392
The formation of excitons in OLEDs is spin dependent and can be controlled by electron‐paramagnetic resonance, affecting device resistance and electroluminescence yield. We explore electrically detected magnetic resonance in the regime of very low magnetic fields (<1 mT). A pronounced feature emerges at zero field in addition to the conventional spin‐ Zeeman resonance for which the Larmor frequency matches that of the incident radiation. By comparing a conventional π‐conjugated polymer as the active material to a perdeuterated analogue, we demonstrate the interplay between the zero‐field feature and local hyperfine fields. The zero‐field peak results from a quasistatic magnetic‐field effect of the RF radiation for periods comparable to the carrier‐pair lifetime. Zeeman resonances are resolved down to 3.2 MHz, approximately twice the Larmor frequency of an electron in Earth's field. However, since reducing hyperfine fields sharpens the Zeeman peak at the cost of an increased zero‐field peak, we suggest that this result may constitute a fundamental low‐field limit of magnetic resonance in carrier‐pair‐based systems. OLEDs offer an alternative solid‐state platform to investigate the radical‐pair mechanism of magnetic‐field effects in photochemical reactions, allowing models of biological magnetoreception to be tested by measuring spin decoherence directly in the time domain by pulsed experiments. 相似文献
14.
Thirunavukkarasu Annamalai Neil Dani Bokun Cheng Yuk-Ching Tse-Dinh 《BMC biochemistry》2009,10(1):18-8
Background
Mycobacterium tuberculosis DNA topoisomerase I is an attractive target for discovery of novel TB drugs that act by enhancing the accumulation of the topoisomerase-DNA cleavage product. It shares a common transesterification domain with other type IA DNA topoisomerases. There is, however, no homology between the C-terminal DNA binding domains of Escherichia coli and M. tuberculosis DNA topoisomerase I proteins. 相似文献15.
Koole R Liljeroth P de Mello Donega C Vanmaekelbergh D Meijerink A 《Journal of the American Chemical Society》2006,128(32):10436-10441
Stable dispersions of molecularlike aggregates of CdTe quantum dots are prepared by chemical cross-linking. Cryo-TEM images confirm the presence of cross-linked quantum dots and show that the size of the small aggregates can be controlled by the amount of cross-linker added. Optical measurements reveal two types of interdot interactions within these quantum-dot molecules: exciton energy transfer and electronic coupling. Quantitative information on the energy transfer rates in quantum-dot molecules is obtained by photoluminescence lifetime measurements. The degree of electronic coupling is dependent on the size of the quantum dots, which is supported by quantum mechanical calculations. 相似文献
16.
A simple method for determination of polycyclic aromatic hydrocarbons (PAHs) in water using headspace solid-phase microextraction (HS-SPME) with gas chromatography-flame ionisation detector (GC-FID) was developed. In order to obtain the convenient experimental conditions for HS-SPME extraction an experimental design with two steps was accomplished. A 26-2 fractional factorial design and central composite design (CCD) considering three significant factors were used. Naphthalene, anthracene and fluoranthene were chosen as representatives of two, three and four aromatic rings, and the global response of three PAHs was used for the results, evaluation. The chosen extraction conditions were: 85 μm polyacrylate fibre; 50 °C temperature; 60 min time; 20 mL-dissolution volume (in 40 mL glass vial); without salt addition; and 2 min desorption time. The procedure was extended to other seven PAHs (acenaphthylene, acenaphthene, fluorene, phenanthrene, pyrene, chrysene and benzo(a)anthracene) and the analytical characteristics were checked. The limit of detection (LOD) was from 0.08 (anthracene) to 0.20 μg L?1 (naphthalene). The precision expressed as relative standard deviation (RSD in %) using 50 μg L?1 of each analyte ranged from 6.8 to 17 %. The method was applied to the analysis of the surface waters and leaching waters of contaminated soils from Gipuzkoa (North Spain). The PAHs were not detected in surface water samples. Most of the PAHs were found in the leachates from contaminated soils showing a maximum global value of 75.5 μg L?1. 相似文献
17.
18.
Avgoustidis A Copeland EJ Moss A Pogosian L Pourtsidou A Steer DA 《Physical review letters》2011,107(12):121301
We study signatures of cosmic superstring networks containing strings of multiple tensions and Y junctions, on the cosmic microwave background (CMB) temperature and polarization spectra. Focusing on the crucial role of the string coupling constant g(s), we show that the number density and energy density of the scaling network are dominated by different types of string in the g(s) ~ 1 and g(s) ? 1 limits. This can lead to an observable shift in the position of the B-mode peak--a distinct signal leading to a direct constraint on g(s). We forecast the joint bounds on g(s) and the fundamental string tension μ(F) from upcoming and future CMB polarization experiments, as well as the signal to noise in detecting the difference between B-mode signals in the limiting cases of large and small g(s). We show that such a detectable shift is within reach of planned experiments. 相似文献
19.
20.
Fatima El Guezar Hassane Bouzahir Danièle Fournier-Prunaret 《Nonlinear Analysis: Hybrid Systems》2011,5(4):626-638
Many switched circuits are made of linear components switched by a simple logic unit. In this paper, we use a generic planar Piece-wise Affine Hybrid System (PWAHS) to model this kind of circuit. Usually, simulations are run by analytical methods (adapted to a specific simple model) or by numerical simulations that can miss some events’ occurrences. We propose a generic planar method to simulate PWAHSs with periodic and state dependent events. Using analytical expressions, our approach can reach arbitrary accuracy in event detections without any loss. As a result, we have implemented our method in Scilab and Matlab toolboxes. 相似文献