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Ghislaine Barouti Dr. Sing Shy Liow Dr. Qingqing Dou Dr. Hongye Ye Clément Orione Prof. Dr. Sophie M. Guillaume Prof. Dr. Xian Jun Loh 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(30):10501-10512
The synthesis of multi‐arm poly([R]‐3‐hydroxybutyrate) (PHB)‐based triblock copolymers (poly([R]‐3‐hydroxybutyrate)‐b‐poly(N‐isopropylacrylamide)‐b‐[[poly(methyl ether methacrylate)‐g‐poly(ethylene glycol)]‐co‐[poly(methacrylate)‐g‐poly(propylene glycol)]], PHB‐b‐PNIPAAM‐b‐(PPEGMEMA‐co‐PPPGMA), and their subsequent self‐assembly into thermo‐responsive hydrogels is described. Atom transfer radical polymerization (ATRP) of N‐isopropylacrylamide (NIPAAM) followed by poly(ethylene glycol) methyl ether methacrylate (PEGMEMA) and poly(propylene glycol) methacrylate (PPGMA) was achieved from bromoesterified multi‐arm PHB macroinitiators. The composition of the resulting copolymers was investigated by 1H and 13C J‐MOD NMR spectroscopy as well as size‐exclusion chromatography (SEC), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC). The copolymers featuring different architectures and distinct hydrophilic/hydrophobic contents were found to self‐assemble into thermo‐responsive gels in aqueous solution. Rheological studies indicated that the linear one‐arm PHB‐based copolymer tend to form a micellar solution, whereas the two‐ and four‐arm PHB‐based copolymers afforded gels with enhanced mechanical properties and solid‐like behavior. These investigations are the first to correlate the gelation properties to the arm number of a PHB‐based copolymer. All copolymers revealed a double thermo‐responsive behavior due to the NIPAAM and PPGMA blocks, thus allowing first the copolymer self‐assembly at room temperature, and then the delivery of a drug at body temperature (37 °C). The non‐significant toxic response of the gels, as assessed by the cell viability of the CCD‐112CoN human fibroblast cell line with different concentrations of the triblock copolymers ranging from 0.03 to 1 mg mL?1, suggest that these PHB‐based thermo‐responsive gels are promising candidate biomaterials for drug‐delivery applications. 相似文献
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Sample Ripening through Nanophase Separation Influences the Performance of Dynamic Nuclear Polarization
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Emmanuelle M. M. Weber Dr. Giuseppe Sicoli Dr. Hervé Vezin Ghislaine Frébourg Dr. Daniel Abergel Prof. Geoffrey Bodenhausen Dr. Dennis Kurzbach 《Angewandte Chemie (International ed. in English)》2018,57(18):5171-5175
Mixtures of water and glycerol provide popular matrices for low‐temperature spectroscopy of vitrified samples. However, they involve counterintuitive physicochemical properties, such as spontaneous nanoscopic phase separations (NPS) in solutions that appear macroscopically homogeneous. We demonstrate that such phenomena can substantially influence the efficiency of dynamic nuclear polarization (DNP) by factors up to 20 % by causing fluctuations in local concentrations of polarization agents (radicals). Thus, a spontaneous NPS of water/glycerol mixtures that takes place on time scales on the order of 30–60 min results in a confinement of polarization agents in nanoscopic water‐rich vesicles, which in return affects the DNP. Such effects were found for three common polarization agents, TEMPOL, AMUPol and Trityl. 相似文献
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Guy Bertrand Antoine Brceiredo Ghislaine Sicard Michel Granier 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1-2):353-356
Abstract Depending on the nature of the diazo-carbon substi tuent, the intermediates generated by photolysis or therrolysis of various α-diazophosphines behave either as “true” carbenes or as phosphorus-carbon multiple-bonded species. 相似文献
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Alexander Acevedo De la Cruz Ghislaine Hilbert Céline Rivière Virginie Mengin Nathalie Ollat Louis Bordenave Stéphane Decroocq Jean-Claude Delaunay Serge Delrot Jean-Michel Mérillon Jean-Pierre Monti Eric Gomès Tristan Richard 《Analytica chimica acta》2012
The composition and concentration of anthocyanins of grape berry skins were analyzed in order to assess phenotypic variation between four grape wine varieties belonging to 4 different species: Vitis vinifera, Vitis amurensis, Vitis cinerea and Vitis X champinii. High-performance liquid chromatography coupled to mass spectrometry (LC–MS) and NMR spectroscopy (LC–NMR) were used to separate and identify the structure of anthocyanins present in these species. Combination of LC–MS and LC–NMR data resulted in the identification of 33 anthocyanins. In particular, newly reported cis isomers of p-coumaric-derivatives were identified (petunidin-, peonidin- and malvidin-3-(6-p-coumaroyl)-5-diglucoside). In V. cinerea and V. vinifera, anthocyanins were monoglucoside derivatives whereas in V. amurensis and V. X champinii, both mono- and diglucoside derivatives were identified. Malvidin-, delphinidin- and petunidin-derivatives were, respectively, the most abundant components in V. cinerea and V. vinifera, V. amurensis and V. X champinii. 相似文献
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Flögel O Okala Amombo MG Reissig HU Zahn G Brüdgam I Hartl H 《Chemistry (Weinheim an der Bergstrasse, Germany)》2003,9(6):1405-1415
Based on our earlier results employing lithiated methoxyallene 2 as C(3) building block and imines 3 for the synthesis of dihydropyrrole derivatives 5, we have investigated chiral imines 6, 10, and 15 as electrophilic components. Combined with lithiated alkoxyallenes, these imines provide the corresponding primary adducts and finally the dihydropyrrole derivatives 8, 12, 17, 20, and 22 in good yields and with high to excellent syn selectivities. This stereochemical outcome is interpreted as a result of alpha-chelate control. Treatment with hydrochloric acid converted syn-8 and syn-12 into bicyclic compounds 9 and 13, whereas under more mildly acidic conditions adduct syn-17 was transformed into diol syn-18. The total synthesis of the uncommon gamma-amino acid (-)-detoxinine could be achieved by starting from (S)-malic acid, which was converted into imine 15 in four steps. Lithiated benzyloxyallene added to imine 15 and efficiently furnished the crucial dihydropyrrole derivative syn-22. The hydrogenolysis of this compound did not directly provide the protected triol 29 as anticipated, but a stepwise protocol made the triol available in a fairly satisfactory manner. A second crucial step of the synthesis was the selective oxidation of 29, which could be achieved by employing platinum dioxide and oxygen. The resulting bicyclic lactone 30 was smoothly transformed into enantiopure (-)-detoxinine. Thus, a fairly short synthesis of this natural product based on a lithiated alkoxyallene could be performed, demonstrating the potential of these intermediates for syntheses of interesting functionalized heterocyclic compounds. 相似文献
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This paper considers the work carried out by online teacher educators and their professional development. We use the theoretical perspective of the documentational approach that focuses, in this case, on the interaction between teacher educators and the resources they use for their online training work. We thus study the following issues: (1) What kinds of resources do online teacher educators need, and how are such resources modified according to the educators?? specific skills and needs? (2) What specific skills are needed for setting up online training for mathematics teachers and how do these skills evolve as teacher education resources are used? We consider both questions simultaneously, while presenting results from a study within a specific teacher training programme in France that proposes ??training paths?? on a national platform. These ??paths?? are resources designed for teacher educators. We follow the appropriation of two training paths by two educator teams. The ways in which these educator teams were able to appropriate the paths give insights into the teacher educators?? skills and, as well, into the resources they need. By looking at their use of resources (as online mathematics teacher educators), we observe and analyse professional geneses, leading to the development of new skills. 相似文献
29.
Anomalous electrophoretic migration of short oligodeoxynucleotides labelled with 5′‐terminal Cy5 dyes
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Tom Killelea Christine Saint‐Pierre Céline Ralec Didier Gasparutto Ghislaine Henneke 《Electrophoresis》2014,35(14):1938-1946
By using a fluorescent exonuclease assay, we reported unusual electrophoretic mobility of 5′‐indocarbo‐cyanine 5 (5′‐Cy5) labelled DNA fragments in denaturing polyacrylamide gels. Incubation time and enzyme concentration were two parameters involved in the formation of 5′‐Cy5‐labelled degradation products, while the structure of the substrate was slightly interfering. Replacement of positively charged 5′‐Cy5‐labelled DNA oligonucleotides (DNA oligos) by electrically neutral 5′‐carboxyfluorescein (5′‐FAM) labelled DNA oligos abolished the anomalous migration pattern of degradation products. MS analysis demonstrated that anomalously migrating products were in fact 5′‐labelled DNA fragments ranging from 1 to 8 nucleotides. Longer 5′‐Cy5‐labelled DNA fragments migrated at the expected position. Altogether, these data highlighted, for the first time, the influence of the mass/charge ratio of 5′‐Cy5‐labelled DNA oligos on their electrophoretic mobility. Although obtained by performing 3′ to 5′ exonuclease assays with the family B DNA polymerase from Pyrococcus abyssi, these observations represent a major concern in DNA technology involving most DNA degrading enzymes. 相似文献
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The 1,4-addition of thio nucleophiles to chiro-inositols containing a cinnamyl Michael acceptor proceeded with excellent diastereochemical induction and good yields. Cleavage of the inositol auxiliary provides beta-thio hydrocinnamic acids in >99% ee's. 相似文献