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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
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We investigate the linear stability of the Bickley jet in the framework of the beta-plane approximation. Because singular inviscid neutral modes exist in the retrograde case , it is necessary to add viscosity to interpret them. One of these modes was found in closed form by Howard and Drazin [1] . However, its critical point is at the center of the jet and it was therefore not possible for these authors to ascertain the relationship of this mode to the stability problem or to discuss how to continue the eigenfunction across the singularity.
The viscous critical layer problem associated with this singularity is considerably more difficult than the usual one (which leads to integrals of the Airy function) because and, consequently, a second-order turning point is involved. Our analysis shows that the Howard–Drazin mode is degenerate in the domain where it is valid as a limit of the viscous problem (wavenumber α2 ≤ 9/2 ), that is, it corresponds to both an odd and an even mode. This conclusion is confirmed by direct numerical solution of the Orr–Sommerfeld equation which shows, in addition, that viscosity is destabilizing along portions of the stability boundary. For a retrograde jet, instability is found to occur beyond the inviscid critical value of β, that is, in the region where the flow would be stable according to the Rayleigh–Kuo condition. 相似文献
The viscous critical layer problem associated with this singularity is considerably more difficult than the usual one (which leads to integrals of the Airy function) because and, consequently, a second-order turning point is involved. Our analysis shows that the Howard–Drazin mode is degenerate in the domain where it is valid as a limit of the viscous problem (wavenumber α
6.
Let
d−1{(x1,…,xd)
d:x21+···+x2d=1} be the unit sphere of the d-dimensional Euclidean space
d. For r>0, we denote by Brp (1p∞) the class of functions f on
d−1 representable in the formwhere dσ(y) denotes the usual Lebesgue measure on
d−1,
and Pλk(t) is the ultraspherical polynomial.For 1p,q∞, the Kolmogorov N-width of Brp in Lq(
d−1) is given bythe left-most infimum being taken over all N-dimensional subspaces XN of Lq(
d−1).The main result in this paper is that for r2(d−1)2,where ANBN means that there exists a positive constant C, independent of N, such that C−1ANBNCAN.This extends the well-known Kashin theorem on the asymptotic order of the Kolmogorov widths of the Sobolev class of the periodic functions. 相似文献
7.
Rebecca L Brown 《Journal of sound and vibration》2003,262(3):591-611
Most structural dynamic systems are of high order; however, they often exhibit phenomena that can be dealt with effectively using low order models. This paper presents a method for describing certain kinds of damage evolution in mechanical systems. The method relies on a simple principle that as damage evolves in a structural dynamic system, the damage indicator (i.e., diagnostic feature) behaves like a stable quasi-stationary equilibrium point in a subsidiary non-linear bifurcating system within the so-called damage center manifold. It is shown that just as linear normal modes govern the behavior of linear structures with idealized damping, so too do non-linear normal forms govern the evolution of damage within structures in many instances. The method is justified with citations from the literature on certain types of mechanical failure and then applied in an experimental case involving reversible damage in a bolted fastener. Off-line experiments on a rotorcraft fuselage show that the evolution of damage is sensitive to both temporal and spatial bifurcation parameters. A diagnostic sensing strategy whereby output-only transmissibility features are used to decrease the order of high order structural dynamic measurements is also described. 相似文献
8.
Richard Brown 《Geometriae Dedicata》2003,97(1):129-150
In this note, we show that given a closed, orientable genus-g surface S
g
, any hyperbolic toral automorphism has a positive power which induces a quadratic, orientable pseudo-Anosov homeomorphism on S
g
. To show this, we lift Anosov toral automorphisms through a ramified topological covering and present the lifted homeomorphism via a standard set of Lickorish twists. This construction provides a general method of producing pseudo-Anosov maps of closed surfaces with predetermined orientable foliations and quadratic dilatation. Since these lifted automorphisms have orientable foliations, this construction is a sort of converse to that of Franks and Rykken [Trans. Amer. Math. Soc. 1999], who established that one can associate to a quadratic pseudo-Anosov homeomorphism with oriented unstable foliation a hyperbolic toral automorphism. 相似文献
9.
Synthetic routes to BEDT-TTF derivatives bearing side chain carboxylic ester and amide groups are reported. Methyl ET-ethanoate was prepared in five steps from vinylacetic acid; amide groups were installed early in the synthesis by mixed anhydride methods before the final coupling reaction. 相似文献
10.