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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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A variational approach is proposed to study some properties of the adiabatic Holstein–Hubbard model which describes an assembly of fermionic charges interacting with a static atomic lattice. The sum of the electronic energy and the lattice elastic energy is proved to have minima with a many-polaron structure in a certain domain of model parameters. Our analytical work consists in expanding these energy minima from the zero electronic transfer limit which remarkably holds for a finite amplitude of the onsite Hubbard repulsion and for an unbounded lattice size. 相似文献
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Ashish Goel Monika R. Henzinger Serge Plotkin Eva Tardos 《Journal of Algorithms in Cognition, Informatics and Logic》2003,48(2):314-332
In this paper we consider the online ftp problem. The goal is to service a sequence of file transfer requests given bandwidth constraints of the underlying communication network. The main result of the paper is a technique that leads to algorithms that optimize several natural metrics, such as max-stretch, total flow time, max flow time, and total completion time. In particular, we show how to achieve optimum total flow time and optimum max-stretch if we increase the capacity of the underlying network by a logarithmic factor. We show that the resource augmentation is necessary by proving polynomial lower bounds on the max-stretch and total flow time for the case where online and offline algorithms are using same-capacity edges. Moreover, we also give polylogarithmic lower bounds on the resource augmentation factor necessary in order to keep the total flow time and max-stretch within a constant factor of optimum. 相似文献
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1.INTRODUCTION[()-227.3()]Endotoxinislipopolysaccharide(LPS)derivedfromthecellmembranesofgram-negativebacteria.Endotoxincancausefebrilereactionsinanimalswithsymptomsofhighfever,vasodilation,diarrheaandfetalshockwheninjectedeveninaverysmallamount[1].Iftheconcentrationofendotoxininpatients?bloodishighenoughitcancauseseveresepsis,whichisamajorcauseofdeathinpatientsandcontinuestohaveahighmortalitydespiteappropriatesurgery,potentantibiotic,andintensivesupportivetherapy[2~5].LipidAisthemaintox… 相似文献
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