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61.
Dr. Marco Marazzi Dr. Hugo Gattuso Dr. Maria Fumanal Dr. Chantal Daniel Dr. Antonio Monari 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(10):2519-2526
A computational investigation of the triplet excited states of a rhenium complex electronically coupled with a tryptophan side chain and bound to an azurin protein is presented. In particular, by using high-level molecular modeling, evidence is provided for how the electronic properties of the excited-state manifolds strongly depend on coupling with the environment. Indeed, only upon explicitly taking into account the protein environment can two stable triplet states of metal-to-ligand charge transfer or charge-separated nature be recovered. In addition, it is also demonstrated how the rhenium complex plus tryptophan system in an aqueous environment experiences too much flexibility, which prevents the two chromophores from being electronically coupled. This occurrence disables the formation of a charge-separated state. The successful strategy requires a multiscale approach of combining molecular dynamics and quantum chemistry. In this context, the strategy used to parameterize the force fields for the electronic triplet states of the metal complex is also presented. 相似文献
62.
Carlos Camacho‐Camacho Irma Rojas‐Oviedo Ariadna Garza‐Ortiz Rubén Alfredo Toscano Luis Sánchez‐Sánchez Jorge Cardenas Hugo López‐Muñoz 《应用有机金属化学》2016,30(4):199-207
The synthesis in one‐pot reactions and structural characterization of six new tri‐n‐butyltin(IV) derivatives of Schiff bases are reported. The compounds are derived from a condensation reaction between l ‐alanine, l ‐valine, l ‐isoleucine, l ‐methionine, l ‐phenylalanine or l ‐tryptophan and 3,5‐di‐tert‐butyl‐2‐hydroxybenzaldehyde. Characterization was completed using elemental analysis, infrared spectroscopy, mass spectrometry, one‐ and two‐dimensional solution NMR (1H, 13C and 119Sn) as well as solid‐state 119Sn NMR. In addition, the crystal structures of three of the compounds were confirmed using single‐crystal X‐ray diffraction. Although five‐coordinated and polymeric in the solid state, the tin compounds are four‐coordinated and monomeric in solution. The coordination environment around the triorganotin units comprises three carbon atoms and two oxygen atoms from two ligands in a trigonal bipyramidal geometry. The anti‐proliferative effect of these compounds on the cervical carcinoma cell lines HeLa, CaSki and ViBo was screened in vitro, the compounds showing cytotoxic activity against all three strains and null or low cytotoxic activity (necrotic) as well. Copyright © 2016 John Wiley & Sons, Ltd. 相似文献
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Viviana Heguaburu Hugo do Carmo Florencia Parpal María Eugenia Amorós Andrés González 《Tetrahedron letters》2017,58(18):1738-1741
The synthesis of 3-hydroxy-2-hexanone and 2,3-hexanediol, two components of the aggregation pheromone of several cerambycid species, is disclosed in here. Starting from 2-hexanone, through an α-hydroxylation using (diacetoxyiodo)benzene, 3-hydroxy-2-hexanone is obtained in good yield. Further reduction of this compound, gives 2,3-hexanediol in excellent yield. A study of the α-hydroxylation reaction of several alkylketones using an hypervalent iodine reagent is also disclosed in here. The synthesis of optically active compounds (R)- and (S)-3-hydroxy-2-hexanone was achieved starting from 2-hexanone with nitrosobenzene and l- and d-proline respectively, in several reaction media. 相似文献
66.
David Alonso-Gutiérrez Bernardo González Merino C. Hugo Jiménez Rafael Villa 《Journal of Geometric Analysis》2018,28(2):1182-1201
We extend the notion of John’s ellipsoid to the setting of integrable log-concave functions. This will allow us to define the integral ratio of a log-concave function, which will extend the notion of volume ratio, and we will find the log-concave function maximizing the integral ratio. A reverse functional affine isoperimetric inequality will be given, written in terms of this integral ratio. This can be viewed as a stability version of the functional affine isoperimetric inequality. 相似文献
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Francesco Carlà Giulio Campo Claudio Sangregorio Andrea Caneschi César de Julián Fernández Lourdes I. Cabrera 《Journal of nanoparticle research》2013,15(8):1-16
Quantum dots (QDs) have received considerable attention due to their unique optical and electrical properties. Although substantial research has focused on the potential applications and toxicological impacts of QDs, far less effort has been directed toward understanding their fate and transport in the environment. In this work, the effect of four coatings, polyethylene glycol functionalized polymer (PEGP), carboxyl derivatized polymer (COOHP), linoleic acid (LA), and polyacrylic acid-octylamine (PAA-OA), on the transport and retention of QDs in porous media were evaluated under environmentally relevant conditions. Aqueous QD suspensions (ca. 10 nM) were introduced into water-saturated columns packed with 40–50 mesh Ottawa sand at a pore-water velocity of 7.6 m/day. At an ionic strength (IS) of 3 mM and pH of 7, PEGP-coated QDs were completely retained within the column, while more than 60 % of COOHP-coated QDs were transported through a column run under identical conditions. When PAA-OA and LA were used as coatings, effluent QD recoveries increased to more than 65 and 89 % of the injected mass, respectively. Additionally, a decrease in pH from 9.5 to 5.0, or an increase of IS from 0 to 30 mM reduced the eluted mass of PAA-OA-coated QDs by more than 2 and 15 times, respectively. The relative mobility of coated QDs (LA > PAA-OA > COOHP > PEGP) was consistent with total interaction energy profiles between QDs and sand surfaces calculated based on Derjaguin–Landau–Verwey–Overbeek (DLVO) theory. At an IS of 3 mM (NaCl) and pH 7, a linear correlation was obtained between the fraction of eluted QDs and the magnitude of the primary interaction energy barrier. These findings demonstrate the strong dependence of QD transport on coating type and indicate that interaction energies based on DLVO theory can be used to predict the relative mobility of QDs in porous media. 相似文献
69.
Florent Balacheff Hugo Parlier Stéphane Sabourau 《Geometric And Functional Analysis》2012,22(1):37-73
Given a Riemannian surface, we consider a naturally embedded graph which captures part of the topology and geometry of the
surface. By studying this graph, we obtain results in three different directions. 相似文献
70.
One of the most common environmental impacts of road transportation is the traffic noise. Linked to this, Start/Stop is a technology which has demonstrated to save fuel by powering off the engine when the vehicle is stopped, such as in front of a traffic light, and restarting the engine instantly when the driver pushes back the pedal brake to proceed. The technology helps also to reduce the CO2 emission, playing a key role in a way to accomplish stringent emission norms for vehicle manufacturer. However, we are not sure whether it reduces the noise emission and how much? Thus, the main aim of this work is to assess the engine noise emissions of a vehicle incorporating a Start/Stop system in urban traffic, and compare it with those radiated by the mean traffic stream. Experimental results demonstrate that there are no contributions of the Start/Stop system to reduce meaningfully the engine noise in urban traffic. 相似文献