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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.
Synthesis,Electronic Properties and WOLED Devices of Planar Phosphorus‐Containing Polycyclic Aromatic Hydrocarbons
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Dr. François Riobé Rózsa Szűcs Dr. Pierre‐Antoine Bouit Dr. Denis Tondelier Bernard Geffroy Fátima Aparicio Julia Buendía Prof. Luis Sánchez Prof. Régis Réau Prof. László Nyulászi Prof. Muriel Hissler 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(17):6547-6556
We describe the synthesis and the physical properties of polyaromatic hydrocarbons (PAHs) containing a phosphorus atom at the edge. In particular, the impact of the successive addition of aromatic rings on the electronic properties was investigated by experimental (UV/Vis absorption, fluorescence, cyclic voltammetry) and theoretical studies (DFT). The physical properties recorded in solution and in the solid state showed that the P‐containing PAHs exhibit properties expected for an emitter in white organic light‐emitting diodes (WOLEDs). 相似文献
3.
Julia K Pruns Jens-Peter Vietzke Manfred Strassner Claudius Rapp Ulrich Hintze Wilfried A K?nig 《Rapid communications in mass spectrometry : RCM》2002,16(3):208-211
A new solvent-free sample preparation method using silver trifluoroacetate (AgTFA) was developed for the analysis of low molecular weight paraffins and microcrystalline waxes by laser desorption/ionization time-of-flight mass spectrometry (LDI-TOFMS). Experiments show that spectral quality can be enhanced by dispersing AgTFA directly in liquid paraffins without the use of additional solvents. This preparation mixture is applied directly to the MALDI probe. Solid waxes could be examined by melting prior to analysis. The method also provides sufficiently reproducible spectra that peak area ratios between mono- and bicyclic alkane peaks indicated variations in the cycloalkane content of paraffin samples. Dehydrogenation of hydrocarbons observed during the desorption/ionization process was studied by analysis of alkane standards. 相似文献
4.
陈永静 朱胜江 J.H.Hamilton A.V.Ramayya J.K.Hwang Y.X.Luo J.O.Rasmussen 车兴来 丁怀博 李明亮 《中国物理 C》2006,30(8):740-744
通过测量252Cf自发裂变所产生的瞬发γ射线, 对146Ce核的高自旋结构进行了重新研究, 结果更新了以前报道的能级纲图, 把八级形变集体带扩展到更高的自旋, 并且重新构建了可能的准γ带结构. 此外, 用反射不对称壳模型(RASM)对146Ce核的八级形变带进行了计算, 低自旋处的计算结果与实验数据符合得很好. 相似文献
5.
D. Fong J. H. Hamilton A. V. Ramayya J. K. Hwang C. Goodin K. Li J. Kormicki J. O. Rasmussen Y. X. Luo S. C. Wu I. Y. Lee A. V. Daniel G. M. Ter-Akopian G. S. Popeko A. S. Fomichev A. M. Rodin Yu. Ts. Oganessian M. Jandel J. Kliman L. Krupa J. D. Cole M. A. Stoyer R. Donangelo W. C. Ma 《Physics of Atomic Nuclei》2006,69(7):1161-1167
The hot bimodal fission of 252Cf is reexamined with new high-statistics data. We constructed a γ-γ-γ coincidence cube for binary fission and LCP-gated γ-γ matrix for ternary fission. By identifying the secondary fission fragments from their γ-ray transitions, we measured the yields for various fission splits. The normal neutron yield distribution is found to be
Gaussian for Xe-Ru. However, the binary fission split of Ba-Mo is found to exhibit a bimodal neutron distribution with the
“hot mode” corresponding to ≈3.1% of the total yield. In α ternary fission, the first measurements of yields for specific fission splits are presented. The Te-α-Ru and Xe-α-Mo neutron yields fit well with a single mode, but the Ba-α-Zr split shows evidence for an enhanced hot mode with an intensity of ≈13.8% of the normal mode.
The text was submitted by the authors in English. 相似文献
6.
Chris Rasmussen Michelle Zandieh Karen King Anne Teppo 《Mathematical Thinking and Learning》2005,7(1):51-73
The purpose of this article is to contribute to the dialogue about the notion of advanced mathematical thinking by offering an alternative characterization for this idea, namely advancing mathematical activity. We use the term advancing (versus advanced) because we emphasize the progression and evolution of students' reasoning in relation to their previous activity. We also use the term activity, rather than thinking. This shift in language reflects our characterization of progression in mathematical thinking as acts of participation in a variety of different socially or culturally situated mathematical practices. For these practices, we emphasize the changing nature of students' mathematical activity and frame the process of progression in terms of multiple layers of horizontal and vertical mathematizing. 相似文献
7.
We demonstrate that the 3-power torsion points of the Jacobians of the principal modular curves X(3n) are fixed by the kernel of the canonical outer Galois representation of the pro-3 fundamental group of the projective line
minus three points. The proof proceeds by demonstrating the curves in question satisfy a two-part criterion given by Anderson
and Ihara. Two proofs of the second part of the criterion are provided; the first relies on a theorem of Shimura, while the
second uses the moduli interpretation.
Received: 30 September 2005 相似文献
8.
The theory for the calculation of the frequency-dependent hyperpolarizabilities β(?2ω; 0, ω), β(?ω; 0, ω), and β(0; ω, ?ω) is discussed. New relations between these tensors are derived for those wave functions that obey the time-dependent Hellmann–Feynman theorem (e.g., the self-consistent field [SCF] or the exact wave function). Using second-order Møller–Plesset perturbation theory (MP2), expressions are obtained for the hyperpolarizabilities in terms of derivatives of appropriately defined linear polarizability tensors with respect to a static electric field. Results are presented for ammonia and formaldehyde for the optical Kerr effect and for secondharmonic generation. These results indicate that it is desirable to determine the frequency-dependent contribution to the hyperopolarizability at the MP2 rather than the SCF level of theory, in cases where the static hyperpolarizability has a large contribution from electron correlation and/or where the frequency-dependent contribution may be more significant, such as for secondharmonic generation. 相似文献
9.
G. M. Ter-Akopian A. V. Daniel A. S. Fomichev G. S. Popeko A. M. Rodin Yu. Ts. Oganessian J. H. Hamilton A. V. Ramayya J. Kormicki J. K. Hwang D. Fong P. Gore J. D. Cole M. Jandel J. Kliman L. Krupa J. O. Rasmussen I. Y. Lee A. O. Macchiavelli P. Fallon M. A. Stoyer R. Donangelo S. -C. Wu W. Greiner 《Physics of Atomic Nuclei》2004,67(10):1860-1865
Ternary fission of 252Cf was studied at Gammasphere using eight ΔE×E particle telescopes. Helium, beryllium, boron, and carbon light charged particles (LCPs) emitted with kinetic energy more than 9, 21, 26, and 32 MeV, respectively, were identified. The 3368-keV γ transition from the first 2+ excited state in 10Be was found and the population probability ratio N(2+)/N(0+) = 0.160 ± 0.025 was estimated. No evidence was found for 3368-keV γ rays emitted from a triple molecular state. For the first time, charge distributions are obtained for ternary fission fragments emitted with helium, beryllium, and carbon LCPs. 相似文献
10.
Christian Buchgraber Alexander Pogantsch Stefan Kappaun Julia Spanring Wolfgang Kern 《Journal of polymer science. Part A, Polymer chemistry》2006,44(14):4317-4327
Light‐emitting diodes based on organic materials [organic light‐emitting diodes (OLEDs)] have attracted much interest over the past decade. Several different attempts have been made to realize multicolor OLEDs. This article describes a new approach based on energy transfer in a donor/acceptor system. A copolymer containing both donor and acceptor compounds as comonomer units is prepared. The polymer consists of a derivative of a luminescent dye [4‐dicyanmethylene‐2‐methyl‐6‐4H‐pyran (DCM); acceptor compound], which is copolymerized with fluorene (donor compound) to combine the properties of an electroactive polymer with a highly luminescent dye. Photochemical processing is achieved by UV irradiation of this copolymer in the presence of gaseous trialkylsilanes. This reagent selectively saturates the C?C bonds in the DCM comonomer units while leaving the fluorene units essentially unaffected. As a result of the photochemical process, the red electroluminescence of the acceptor compound vanishes, and the blue‐green electroluminescence from the polyfluorene units is recovered. Compared with previous approaches based on polymer blends, this copolymer approach avoids problems associated with phase‐separation phenomena in the active layer of OLEDs. © 2006Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 44: 4317–4327, 2006 相似文献