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91.
Christelle Lemaitre-Guillier Agns Chartier Christelle Dufresne Antonin Douillet Stphanie Cluzet Josep Valls Nicolas Aveline Xavier Daire Marielle Adrian 《Molecules (Basel, Switzerland)》2022,27(18)
The present study is aimed at determining whether leaf volatile organic compounds (VOCs) are good markers of the grapevine response to defence elicitors in the field. It was carried out in two distinct French vineyards (Burgundy and Bordeaux) over 3 years. The commercial elicitor Bastid® (Syngenta, Saint-Sauveur, France) (COS-OGA) was first used to optimise the VOCs’ capture in the field; by bagging stems together with a stir bar sorptive extraction (SBSE) sensor. Three elicitors (Bastid®, copper sulphate and methyl jasmonate) were assessed at three phenological stages of the grapevines by monitoring stilbene phytoalexins and VOCs. Stilbene production was low and variable between treatments and phenological stages. VOCs—particularly terpenes—were induced by all elicitors. However, the response profiles depended on the type of elicitor, the phenological stage and the vineyard, and no sole common VOC was found. The levels of VOC emissions discriminated between weak (Bastid® and copper sulphate) and strong (methyl jasmonate) inducers. Ocimene isomers were constitutively present in the overall blends of the vineyards and increased by the elicitors’ treatments, whilst other VOCs were newly released throughout the growing seasons. Nonetheless, the plant development and climate factors undoubtedly influenced the release and profiles of the leaf VOCs. 相似文献
92.
Eni Kume Nicolas Martin Peter Dunne Patrick Baroni Laurence Noirez 《Molecules (Basel, Switzerland)》2022,27(22)
Mesoscopic shear elasticity has been revealed in ordinary liquids both experimentally by reinforcing the liquid/surface interfacial energy and theoretically by nonextensive models. The elastic effects are here examined in the frame of small molecules with strong electrostatic interactions such as room temperature ionic liquids [emim][Tf2N] and nitrate solutions exhibiting paramagnetic properties. We first show that these charged fluids also exhibit a nonzero low-frequency shear elasticity at the submillimeter scale, highlighting their resistance to shear stress. A neutron scattering study completes the dynamic mechanical analysis of the paramagnetic nitrate solution, evidencing that the magnetic properties do not induce the formation of a structure in the solution. We conclude that the elastic correlations contained in liquids usually considered as viscous away from any phase transition contribute in an effective way to collective effects under external stress whether mechanical or magnetic fields. 相似文献
93.
Gourab Chatterjee Ajay Jha Alejandro Blanco-Gonzalez Vandana Tiwari Madushanka Manathunga Hong-Guang Duan Friedjof Tellkamp Valentyn I. Prokhorenko Nicolas Ferr Jyotishman Dasgupta Massimo Olivucci R. J. Dwayne Miller 《Chemical science》2022,13(32):9392
The concerted interplay between reactive nuclear and electronic motions in molecules actuates chemistry. Here, we demonstrate that out-of-plane torsional deformation and vibrational excitation of stretching motions in the electronic ground state modulate the charge-density distribution in a donor-bridge-acceptor molecule in solution. The vibrationally-induced change, visualised by transient absorption spectroscopy with a mid-infrared pump and a visible probe, is mechanistically resolved by ab initio molecular dynamics simulations. Mapping the potential energy landscape attributes the observed charge-coupled coherent nuclear motions to the population of the initial segment of a double-bond isomerization channel, also seen in biological molecules. Our results illustrate the pivotal role of pre-twisted molecular geometries in enhancing the transfer of vibrational energy to specific molecular modes, prior to thermal redistribution. This motivates the search for synthetic strategies towards achieving potentially new infrared-mediated chemistry.Channelling vibrational excitation energy to achieve ground-state charge-transfer (CT)-assisted isomerization in a donor-bridge-acceptor molecule in solution. 相似文献
94.
Paul Kirren Lucile Barka Saher Rahmani Nicolas Bondon Nicolas Donzel Philippe Trens Aurlie Bessire Laurence Raehm Clarence Charnay Jean-Olivier Durand 《Molecules (Basel, Switzerland)》2022,27(13)
(1) Background: Due to human activities, greenhouse gas (GHG) concentrations in the atmosphere are constantly rising, causing the greenhouse effect. Among GHGs, carbon dioxide (CO2) is responsible for about two-thirds of the total energy imbalance which is the origin of the increase in the Earth’s temperature. (2) Methods: In this field, we describe the development of periodic mesoporous organosilica nanoparticles (PMO NPs) used to capture and store CO2 present in the atmosphere. Several types of PMO NP (bis(triethoxysilyl)ethane (BTEE) as matrix, co-condensed with trialkoxysilylated aminopyridine (py) and trialkoxysilylated bipyridine (Etbipy and iPrbipy)) were synthesized by means of the sol-gel procedure, then characterized with different techniques (DLS, TEM, FTIR, BET). A systematic evaluation of CO2 adsorption was carried out at 298 K and 273 K, at low pressure. (3) Results: The best values of CO2 adsorption were obtained with 6% bipyridine: 1.045 mmol·g−1 at 298 K and 2.26 mmol·g−1 at 273 K. (4) Conclusions: The synthetized BTEE/aminopyridine or bipyridine PMO NPs showed significant results and could be promising for carbon capture and storage (CCS) application. 相似文献
95.
Monoclonal antibodies are emerging as a viable treatment for the coronavirus disease 19 (COVID-19). However, newly evolved variants of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) can reduce the efficacy of currently available antibodies and can diminish vaccine-induced immunity. Here, we demonstrate that the microscopic dynamics of neutralizing monoclonal antibodies can be profoundly modified by the mutations present in the spike proteins of the SARS-COV-2 variants currently circulating in the world population. The dynamical perturbations within the antibody structure, which alter the thermodynamics of antigen recognition, are diverse and can depend both on the nature of the antibody and on the spatial location of the spike mutation. The correlation between the motion of the antibody and that of the spike receptor binding domain (RBD) can also be changed, modulating binding affinity. Using protein-graph-connectivity networks, we delineated the mutant-induced modifications in the information-flow along allosteric pathway throughout the antibody. Changes in the collective dynamics were spatially distributed both locally and across long-range distances within the antibody. On the receptor side, we identified an anchor-like structural element that prevents the detachment of the antibodies; individual mutations there can significantly affect the antibody binding propensity. Our study provides insight into how virus neutralization by monoclonal antibodies can be impacted by local mutations in the epitope via a change in dynamics. This realization adds a new layer of sophistication to the efforts for rational design of monoclonal antibodies against new variants of SARS-CoV2, taking the allostery in the antibody into consideration.Mutations in the new variants of SARS-CoV-2 spike protein modulates the dynamics of the neutralizing antibodies. Capturing such modulations from MD simulations and graph network model identifies the role of mutations in facilitating immune evasion. 相似文献
96.
Quentin Ronzon Dr. Wei Zhang Dr. Nicolas Casaretto Dr. Elisabeth Mouray Prof. Dr. Isabelle Florent Dr. Bastien Nay 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(28):7764-7772
The introduction of substituents on bare heterocyclic scaffolds can selectively be achieved by directed C−H functionalization. However, such methods have only occasionally been used, in an iterative manner, to decorate various positions of a medicinal scaffold to build chemical libraries. We herein report the multiple, site selective, metal-catalyzed C−H functionalization of a “programmed” 4-hydroxyquinoline. This medicinally privileged template indeed possesses multiple reactive sites for diversity-oriented functionalization, of which four were targeted. The C-2 and C-8 decorations were directed by an N-oxide, before taking benefit of an O-carbamoyl protection at C-4 to perform a Fries rearrangement and install a carboxamide at C-3. This also released the carbonyl group of 4-quinolones, the ultimate directing group to functionalize position 5. Our study highlights the power of multiple C−H functionalization to generate diversity in a biologically relevant library, after showing its strong antimalarial potential. 相似文献
97.
Dr. Aurélien Adenot Dr. Lucile Anthore-Dalion Dr. Emmanuel Nicolas Jean-Claude Berthet Dr. Pierre Thuéry Dr. Thibault Cantat 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(72):18047-18053
An air-tolerant Cu-catalyzed sulfonylative Hiyama cross-coupling reaction enabling the formation of diaryl sulfones is described. Starting from aryl silanes, DABSO and aryliodides, the reaction tolerates a large variety of polar functional groups (amines, ketones, esters, aldehydes). Control experiments coupled with DFT calculations shed light on the mechanism, characterized by the formation of a Cu(I)-sulfinate intermediate via fast insertion of a SO2 molecule. 相似文献
98.
Dustin T. Savage Nicolas J. Briot J. Zach Hilt Thomas D. Dziubla 《Journal of polymer science. Part A, Polymer chemistry》2021,59(4):289-299
Per- and polyfluoroalkyl substances (PFAS) have rapidly accumulated in the environment due to their widespread use prior to commercial discussion in the early 21st century, and their slow degradation has magnified concerns of their potential toxicity. Monitoring their distribution is, therefore, necessary to evaluate and control their impact on the health of exposed populations. This investigation evaluates the capability of a simple polymeric detection scheme for PFAS based on crosslinked, thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) hydrogels. Surveying swelling perturbations induced by several hydrotropes and comparable hydrocarbon analogs, tetraethylammonium perfluorooctane sulfonate (TPFOS) showed a significantly higher swelling ratio on a mass basis (65.5 ± 8.8 at 15°C) than any of the other analytes tested. Combining swelling with the fluorimetric response of a solvachromatic dye, nile red, revealed the fluorosurfactant to initiate observable aggregation (i.e., its critical aggregation concentration) at 0.05 mM and reach saturation (i.e., its charge neutralization concentration) at 0.5 mM. The fluorosurfactant was found to homogeneously distribute throughout the polymer matrix with energy dispersive X-ray spectroscopy, marking the swelling response as a peculiar nexus of fluorinated interfacial positioning and delocalized electrostatic repulsion. Results from the current study hold promise for exploiting the physiochemical response of PNIPAM to assess TPFOS's concentration. 相似文献
99.
The interplay among the spectrum, geometry and magnetic field in tubular neighbourhoods of curves in Euclidean spaces is investigated in the limit when the cross section shrinks to a point. Proving a norm resolvent convergence, we derive effective, lower-dimensional models which depend on the intensity of the magnetic field and curvatures. The results are used to establish complete asymptotic expansions for eigenvalues. Spectral stability properties based on Hardy-type inequalities induced by magnetic fields are also analysed. 相似文献
100.
Nicolas P. Cheval Barbara Hoffmann Anna Dikova Fatih Sirindil Philippe Bertus Aurélien Blanc Jean-Marc Weibel Patrick Pale 《Tetrahedron》2018,74(50):7111-7119
Vinyl nosylates, readily obtained from β-dicarbonyl derivatives, could be efficiently engaged in Sonogashira cross-coupling reactions, either cocatalyzed by copper or silver salts. The para-nitrobenzenesulfonate (nosylate) group allows this coupling to be performed under very mild conditions (room temperature). These new leaving group and mild conditions could be applied to the synthesis of acetylenic coumarinyl derivatives and to the total synthesis of an acetylenic monoterpene natural product, named cleviolide. 相似文献