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111.
Dr. Jessica Flores Gonzalez Vincent Montigaud Dr. Vincent Dorcet Dr. Kevin Bernot Dr. Boris Le Guennic Dr. Fabrice Pointillart Prof. Olivier Cador 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(39):10160-10168
Single-Molecule Magnet (SMM) property is by essence molecular, while commonly measured in solid crystalline state. Solvent crystallization molecules are usually neglected in the analysis and interpretation of solid-state properties. The solvation/desolvation process in the polyoxometalate(POM)-based Na9[Er(W5O18)2] ⋅ 35 H2O SMM demonstrates that the dehydrated form relaxes more than 1000 times faster than the initial state, while the rehydration process allows the quasi complete recovering of the initial magnetic behaviour. This dehydration process is monitored by thermogravimetric analysis (TGA) and temperature-dependent X-ray powder diffraction, and rationalized by periodic quantum chemical calculations evidencing the tremendous role of the labile water molecules in the stability of the edifice. Ab-initio calculations highlight that sodium ions localization in the structure drive the magnetic responses. Isotopic enrichment with nuclear spin free (166Er, I=0) ErIII ions shows that the relaxation dynamics in the quantum regime depends on the nuclear spin. 相似文献
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Pierre Thesmar Seemon Coomar Dr. Alessandro Prescimone Prof. Dr. Daniel Häussinger Prof. Dr. Dennis Gillingham Prof. Dr. Olivier Baudoin 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(66):15298-15312
This article provides a detailed report of our efforts to synthesize the dithiodiketopiperazine (DTP) natural products (−)-epicoccin G and (−)-rostratin A using a double C(sp3)−H activation strategy. The strategy's viability was first established on a model system lacking the C8/C8’ alcohols. Then, an efficient stereoselective route including an organocatalytic epoxidation was secured to access a key bis-triflate substrate. This bis-triflate served as the functional handles for the key transformation of the synthesis: a double C(sp3)−H activation. The successful double activation opened access to a common intermediate for both natural products in high overall yield and on a multigram scale. After several unsuccessful attempts, this intermediate was efficiently converted to (−)-epicoccin G and to the more challenging (−)-rostratin A via suitable oxidation/reduction and protecting group sequences, and via a final sulfuration that occurred in good yield and high diastereoselectivity. These efforts culminated in the synthesis of (−)-epicoccin G and (−)-rostratin A in high overall yields (19.6 % over 14 steps and 12.7 % over 17 steps, respectively), with the latter being obtained on a 500 mg scale. Toxicity assessments of these natural products and several analogues (including the newly synthesized epicoccin K) in the leukemia cell line K562 confirmed the importance of the disulfide bridge for activity and identified dianhydrorostratin A as a 20x more potent analogue. 相似文献
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We construct planar bi-Sobolev mappings whose local volume distortion is bounded from below by a given function with . More precisely, for any we construct -bi-Sobolev maps with identity boundary conditions; for , we provide bi-Lipschitz maps. The basic building block of our construction are bi-Lipschitz maps which stretch a given compact subset of the unit square by a given factor while preserving the boundary. The construction of these stretching maps relies on a slight strengthening of the celebrated covering result of Alberti, Csörnyei, and Preiss for measurable planar sets in the case of compact sets. We apply our result to a model functional in nonlinear elasticity, the integrand of which features fast blowup as the Jacobian determinant of the deformation becomes small. For such functionals, the derivation of the equilibrium equations for minimizers requires an additional regularization of test functions, which our maps provide. 相似文献
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Access to New Endoperoxide Derivatives by Electrochemical Oxidation of Substituted 3‐Azabicyclo[4.1.0]hept‐4‐enes
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Dr. Frédérick Nuter Dr. Abdou Khadre Djily Dimé Dr. Cheng Chen Dr. Lotfi Bounaadja Dr. Elisabeth Mouray Dr. Isabelle Florent Dr. Yvan Six Dr. Olivier Buriez Dr. Angela Marinetti Dr. Arnaud Voituriez 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(14):5584-5593
A series of substituted 3‐azabicyclo[4.1.0]hept‐4‐ene derivatives were prepared and analysed by cyclic voltammetry. Preparative aerobic electrochemical oxidation reactions were then carried out. Three original endoperoxides were isolated, characterised and subjected to antimalarial and cytotoxicity activity assays. 相似文献
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Wen Chen Olivier Maurel Christian La Borderie Thierry Reess Antoine De Ferron Mohammed Matallah Gilles Pijaudier-Cabot Antoine Jacques Frank Rey-Bethbeder 《Heat and Mass Transfer》2014,50(5):673-684
The objective of this study is to simulate the propagation of the shock wave in water due to an explosion. The study is part of a global research program on the development of an alternative stimulation technique to conventional hydraulic fracturing in tight gas reservoirs aimed at inducing a distributed state of microcracking of rocks instead of localized fracture. We consider the possibility of increasing the permeability of rocks with dynamic blasts. The blast is a shock wave generated in water by pulsed arc electrohydraulic discharges. The amplitude of these shock waves is prescribed by the electrohydraulic discharges which generate high pressures of several kilobars within microseconds. A simplified method has been used to simulate the injected electrical energy as augmentation of enthalpy in water locally. The finite element code EUROPLEXUS is used to perform fluid fast dynamic computation. The predicted pressure is consistent with the experimental results. In addition, shock wave propagation characteristics predicted with simulation can be valuable reference for design of underwater structural elements and engineering of underwater explosion. 相似文献
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Guo Chang Zhuo Xiaoyang Constantinescu Corina Pamen Olivier Menoukeu 《Methodology and Computing in Applied Probability》2018,20(4):1477-1502
Methodology and Computing in Applied Probability - In this paper, we pursue the optimal reinsurance-investment strategy of an insurer who can invest in both domestic and foreign markets. We assume... 相似文献