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51.
Prof. Dr. Qianni Guo Qingbin Zeng Weiping Jiang Xiaoxiao Zhang Prof. Dr. Qing Luo Prof. Dr. Xu Zhang Prof. Dr. Louis‐S. Bouchard Prof. Dr. Maili Liu Prof. Dr. Xin Zhou 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(12):3967-3970
Mercury pollution, in the form of mercury ions (Hg2+), is a major health and environmental hazard. Commonly used sensors are invasive and limited to point measurements. Fluorescence‐based sensors do not provide depth resolution needed to image spatial distributions. Herein we report a novel sensor capable of yielding spatial distributions by MRI using hyperpolarized 129Xe. A molecular clamp probe was developed consisting of dipyrrolylquinoxaline (DPQ) derivatives and twocryptophane‐A cages. The DPQ derivatives act as cation receptors whereas cryptophane‐A acts as a suitable host molecule for xenon. When the DPQ moiety interacts with mercury ions, the molecular clamp closes on the ion. Due to overlap of the electron clouds of the two cryptophane‐A cages, the shielding effect on the encapsulated Xe becomes important. This leads to an upfield change of the chemical shift of the encapsulated Xe. This sensor exhibits good selectivity and sensitivity toward the mercury ion. This mercury‐activated hyperpolarized 129Xe‐based chemosensor is a new concept method for monitoring Hg2+ ion distributions by MRI. 相似文献
52.
More Than 12 % Polarization and 20 Minute Lifetime of 15N in a Choline Derivative Utilizing Parahydrogen and a Rhodium Nanocatalyst in Water 下载免费PDF全文
Jeffrey McCormick Dr. Sergey Korchak Dr. Salvatore Mamone Dr. Yavuz N. Ertas Zhiyu Liu Luke Verlinsky Dr. Shawn Wagner Dr. Stefan Glöggler Prof. Louis‐S. Bouchard 《Angewandte Chemie (International ed. in English)》2018,57(33):10692-10696
Hyperpolarization techniques are key to extending the capabilities of MRI for the investigation of structural, functional and metabolic processes in vivo. Recent heterogeneous catalyst development has produced high polarization in water using parahydrogen with biologically relevant contrast agents. A heterogeneous ligand‐stabilized Rh catalyst is introduced that is capable of achieving 15N polarization of 12.2±2.7 % by hydrogenation of neurine into a choline derivative. This is the highest 15N polarization of any parahydrogen method in water to date. Notably, this was performed using a deuterated quaternary amine with an exceptionally long spin‐lattice relaxation time (T1) of 21.0±0.4 min. These results open the door to the possibility of 15N in vivo imaging using nontoxic similar model systems because of the biocompatibility of the production media and the stability of the heterogeneous catalyst using parahydrogen‐induced polarization (PHIP) as the hyperpolarization method. 相似文献
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Ulmeanu SM Josserand J Jensen H Bouchard G Carrupt PA Girault HH 《Journal of chromatography. A》2005,1063(1-2):89-97
A finite element simulation has been used in order to study the partition chromatography process of one species between an aqueous mobile phase and an organic stationary phase located at the bottom of a rectangular microchannel. The transient model incorporates convection--diffusion of the species in the water phase coupled to the diffusion in the stationary organic phase by the way of the partition kinetics at the interface. The time evolution of the injected species concentration is analyzed versus the velocity of the mobile phase, the detecting position and the thickness of the stationary phase. The comparison of simulation results with both experimental data and analytical model confirm its validity. These simulations show that thin channels can be used to measure log P of molecules from their retention time. Finally, we have shown how the sample velocity can be optimized for a given geometry of the channel and diffusion coefficient of the species. 相似文献
55.
[structure: see text] New and facile synthesis of symmetric diindolocarbazoles was developed using the copper-catalyzed Ullmann reaction. The key step is a double-intramolecular cyclization reaction realized on N-alkyl-3,6-dibromo-2,7-bis(2'aminophenyl)carbazole derivatives which offers the desired symmetric ladder oligo(p-aniline)s. Depending upon the nature of the side- and/or end-groups, well-defined thin films and/or semiladder polymers could be obtained. These electroactive ladder oligomers may have great potential in organic electronics. 相似文献
56.
Bouchard G Carrupt PA Testa B Gobry V Girault HH 《Chemistry (Weinheim an der Bergstrasse, Germany)》2002,8(15):3478-3484
This paper first gives a brief review of the main techniques used to measure the lipophilicity of neutral and ionic drugs, namely the shake-flask method, potentiometry, and cyclic voltammetry at liquid-liquid interfaces. The lipophilicity of 28 acidic compounds with various functional groups was studied by potentiometry and cyclic voltammetry in the n-octanol/water and 1,2-dichloroethane/water systems in order to complement our understanding of the lipophilicity of neutral and ionized acids and to clarify the solvation mechanisms responsible for their partition. The parameter diff (log P(N-A)(dce)) (i.e., log P of the neutral acid minus standard log P of the conjugated anion in 1,2-dichloroethane/water) was shown to depend not only on intramolecular interactions and conformational effects in the neutral and anionic forms, but also on the delocalization of the negative charge in the anion, confirming the ability of Born's solvation model to describe qualitatively the effect of the molecular radius on the lipophilicity of ions. 相似文献
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Studies have shown that C(60) fullerene can form stable colloidal suspensions in water that result in C(60) aqueous concentrations many orders of magnitude above C(60)'s aqueous solubility; however, quantitative methods for the analysis of C(60) and other fullerenes in environmental media are scarce. Using a 80/20v/v toluene-acetonitrile mobile phase and a 4.6mmx150mm Cosmosil 5mu PYE column, C(60), C(70), and PCBM ([6,6]-phenyl C(61)-butyric acid methyl ester) were fully resolved. Selectivity factors (alpha) for C(60) relative to PCBM and C(70) relative to C(60) were 3.18 and 2.19, respectively. The best analytical wavelengths for the fullerenes were determined to be 330, 333, and 333nm with log molar absorption coefficients (logvarepsilon) of 4.63, 4.82, and 4.60 for PCBM, C(60), C(70), respectively. Extraction and quantitation of all three fullerenes in aqueous suspensions over a range of pH (4-10) and ionic strengths were very good. Whole-method quantification limits for ground and surface suspensions were 2.87, 2.48, and 6.54mug/L for PCBM, C(60), and C(70), respectively. 相似文献
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Jean Bouchard Myriam Méthot Carole Fraschini Stephanie Beck 《Cellulose (London, England)》2016,23(6):3555-3567
Recent findings indicate there is only a small window of sulfuric acid concentration (60–65 %) and temperature (45–65 °C) which allows efficient extraction of cellulose nanocrystals in significant quantities from bleached chemical pulp. In the present report, we develop a systematic explanation for how hydrolysis temperature, at a specific acid concentration, governs CNC surface properties. We demonstrate that CNCs with different suspension viscosity, stability in electrolyte-containing solutions, and optical properties can be produced, based on the presence or not of a precipitated oligosaccharide layer (OSL) on the surface of the nanocrystals. At hydrolysis temperatures below 65 °C, the degree of polymerization (DP) distribution of cellulose chains in CNC samples exhibits a bimodal distribution, indicating an accumulation of oligosaccharides on the CNC surface which increases as the hydrolysis temperature is decreased. At low hydrolysis temperature (45 °C), the oligosaccharides dissolved in the strong acid phase have a DP between 7 and 20 and precipitate onto CNCs when the reaction is quenched by diluting with water. As the temperature of hydrolysis is increased (50–60 °C), the dissolved oligosaccharides are hydrolyzed faster and their DP decreases such that they remain soluble after quenching. At 65 °C, no precipitated oligosaccharides can be detected on the CNC surface. Based on these results, we propose possible explanations to account for the effects of the OSL on the CNC suspension viscosity and stability and on optical properties of CNC films. 相似文献