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1.
Dr. Jordan Donat Mr. Patrick Dubourdeaux Dr. Martin Clémancey Dr. Julia Rendon Clara Gervasoni Mr. Morgan Barbier Jessica Barilone Dr. Jacques Pécaut Prof. Dr. Serge Gambarelli Prof. Dr. Pascale Maldivi Prof. Dr. Jean-Marc Latour 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(70):e202201875
Nitrene transfer reactions have emerged as one of the most powerful and versatile ways to insert an amine function to various kinds of hydrocarbon substrates. However, the mechanisms of nitrene generation have not been studied in depth albeit their formation is taken for granted in most cases without definitive evidence of their occurrence. In the present work, we compare the generation of tosylimido iron species and NTs transfer from FeII and FeIII precursors where the metal is embedded in a tetracarbene macrocycle. Catalytic nitrene transfer to reference substrates (thioanisole, styrene, ethylbenzene and cyclohexane) revealed that the same active species was at play, irrespective of the ferrous versus ferric nature of the precursor. Through combination of spectroscopic (UV-visible, Mössbauer), ESI-MS and DFT studies, an FeIV tosylimido species was identified as the catalytically active species and was characterized spectroscopically and computationally. Whereas its formation from the FeII precursor was expected by a two-electron oxidative addition, its formation from an FeIII precursor was unprecedented. Thanks to a combination of spectroscopic (UV-visible, EPR, Hyscore and Mössbauer), ESI-MS and DFT studies, we found that, when starting from the FeIII precursor, an FeIII tosyliodinane adduct was formed and decomposed into an FeV tosylimido species which generated the catalytically active FeIV tosylimide through a comproportionation process with the FeIII precursor. 相似文献
2.
Nonlinear Dynamics - Introduction of stiffness nonlinearities to broaden the frequency bandwidth of vibratory energy harvesters has the adverse influence of complicating the response behavior of... 相似文献
3.
In this paper we study the room temperature ferromagnetism reported on Mn-doped ZnO and ascribed to spin polarization of conduction electrons. We experimentally show that the ferromagnetic behaviour is associated to the coexistence of Mn3+ and Mn+4 in MnO2 grains where diffusion of Zn promotes the Mn4+→Mn3+ reduction. Potential uses of this material in spintronic devices are analysed. 相似文献
4.
Jos A. Gmez-Pedrero Juan A. Quiroga M. Jos Terrn-Lpez Daniel Crespo 《Optics and Lasers in Engineering》2006,44(12):1297-1310
In this paper we present the application of a direct demodulation method for the measurement of surface topography by means of Shadow-Moiré. In our set-up, we use three LEDs (with green, red and blue peak wavelengths) to illuminate the grating. Due to the different position of these light sources, a polychromatic Shadow-Moiré fringe pattern is produced, which can be described as the superposition of three monochromatic (red, green and blue) fringe patterns. Taking the image of this polychromatic fringe pattern with a RGB CCD camera, we get a monochromatic fringe pattern stored at each RGB channel of the CCD. The direct demodulation algorithm employed uses these fringe patterns to calculate the wrapped phase map. After unwrapping the phase map using a standard multi-grid technique, we implemented an automatic procedure to detect the area of interest of the phase map by removing low modulation zones and to calculate the absolute value of the phase. In this way it is possible to determine the topography of a surface with a single RGB snapshot maintaining a simple experimental set-up, which is an important feature, especially for the study of dynamic phenomena such as deformations. We present the experimental results obtained after measuring different objects with both smooth and rough surface textures. 相似文献
5.
M. Froese C. Champagne J. R. Crespo López-Urrutia S. Epp G. Gwinner A. Lapierre J. Pfister G. Sikler J. Ullrich J. Dilling 《Hyperfine Interactions》2006,173(1-3):85-92
The precision of atomic mass measurements in a Penning trap is directly proportional to the charge state q of the ion and,
hence, can be increased by using highly charged ions (HCI). For this reason, charge breeding with an electron beam ion trap
(EBIT) is employed at TRIUMF’s Ion Trap for Atomic and Nuclear science (TITAN) on-line facility in Vancouver, Canada. By bombarding
the injected and trapped singly charged ions with an intense beam of electrons, the charge state of the ions is rapidly increased
inside the EBIT. To be compatible with the on-line requirements of short-lived isotopes, very high electron beam current densities
are needed. The TITAN EBIT includes a 6 Tesla superconducting magnet and is designed to have electron beam currents and energies
of up to 5 A and 60 keV, respectively. Once operational at full capacity, most species can be bred into a He-like configuration
within tens of ms. Subsequently, the HCI are extracted, pass a Wien filter to reduce isobaric contamination, are cooled, and
injected into a precision Penning trap for mass measurement. We will present the first results and current status of the TITAN
EBIT, which has recently been moved to TRIUMF after assembly and commissioning at the Max-Planck-Institute (MPI) for Nuclear
Physics in Heidelberg, Germany. 相似文献
6.
M. T. Crespo J. M. Los Arcos C. E. Granados M. L. Aceña 《Journal of Radioanalytical and Nuclear Chemistry》1989,130(1):99-110
A new method of analysis of the efficiency of four filters of MnO2 in series which takes into account the reactions induced in plutonium by the sorbent is described. The system of differential equations describing the behaviour of plutonium in water as it passes through the filters is solved and the parameters of the filters are determined for a best fitting of the solutions corresponding to the experimental uncertainties. The method is checked by numerical simulation and then applied to water solutions with a known plutonium concentration and to some experimental results given by other authors. In all occassions the results are consistent with the possibility of determining the contents of plutonium in sea and continental waters with uncertainties of the order of 10%. 相似文献
7.
The Castelnuovo-Mumford regularity of a module gives a rough measure of its complexity. We bound the regularity of a module given a system of approximating modules whose regularities are known. Such approximations can arise naturally for modules constructed by inductive combinatorial means. We apply these methods to bound the regularity of ideals constructed as combinations of linear ideals and the module of derivations of a hyperplane arrangement as well as to give degree bounds for invariants of finite groups. 相似文献
8.
Jessica Strömbro Peter Gudmundson 《International Journal of Solids and Structures》2008,45(22-23):5765-5787
In this paper a simplified network model for mechano-sorptive creep is presented, which is a further development of an earlier paper [Strömbro, J., Gudmundson, P., 2008. Mechano-sorptive creep under compressive loading – a micromechanical model. International Journal of Solids and Structures 45 (9), 2420–2450.]. It is assumed that the anisotropic hygroexpansion of the fibres leads to large stresses at the fibre bonds when the moisture content changes. The resulting stress state will accelerate creep if the fibre material obeys a constitutive law that is non-linear. Fibre kinks are included in order to capture experimental observations of larger mechano-sorptive effects in compression than in tension. Moisture dependent material parameters and anisotropy in the fibre distribution have been introduced. Theoretical predictions based on the model are compared to experimental results for an anisotropic paper both under tensile and compressive loading at varying moisture content and it is found that the important features in the experiments are captured by the model. Different kinds of drying conditions have also been examined. 相似文献
9.
This paper introduces a method of combining open and closed microchannels in a single component in a novel way which couples the benefits of both open and closed microfluidic systems and introduces interesting on-chip microfluidic behaviour. Fluid behaviour in such a component, based on continuous pressure driven flow and surface tension, is discussed in terms of cross sectional flow behaviour, robustness, flow-pressure performance, and its application to microfluidic interfacing. The closed-open-closed microchannel possesses the versatility of upstream and downstream closed microfluidics along with open fluidic direct access. The device has the advantage of eliminating gas bubbles present upstream when these enter the open channel section. The unique behaviour of this device opens the door to applications including direct liquid sample interfacing without the need for additional and bulky sample tubing. 相似文献
10.
Merkx M Kopp DA Sazinsky MH Blazyk JL Müller J Lippard SJ 《Angewandte Chemie (International ed. in English)》2001,40(15):2725
The cover picture shows in the background the whole cell of a methanotrophic bacterium on which are superimposed components of methane monooxygenase (the structure of the hydroxylase component (top), one of the two four-helix bundles that house the catalytic diiron centers (left)) and a schematic diagram of the catalytic cycle by which the enzyme converts dioxygen and methane into methanol and water. More about this unusual enzyme system is reported by Lippard et al. on p. 2782 ff. 相似文献