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71.
72.
Nga H. Nguyen Brad M. Rosen Xuan Jiang Sven Fleischmann Virgil Percec 《Journal of polymer science. Part A, Polymer chemistry》2009,47(21):5577-5590
SET‐LRP is mediated by a combination of solvent and ligand that promotes disproportionation of Cu(I)X into Cu(0) and Cu(II)X2. Therefore, the diversity of solvents suitable for SET‐LRP is limited. SET‐LRP of MA in a library of solvents with different equilibrium constants for disproportionation of Cu(I)X such as DMSO, DMF, DMAC, EC, PC, EtOH, MeOH, methoxyethanol, NMP, acetone and in their binary mixtures with H2O was examined. H2O exhibits the highest equilibrium constant for disproportionation of Cu(I)X. The apparent rate constant of the polymerization exhibits a linear increase with the addition of H2O. This is consistent with higher equilibrium constants for disproportionation generated by addition of H2O to organic solvents. Furthermore, with the exception of alcohols and carbonates, the rate constant of polymerization in binary mixtures could be correlated with the Dimroth‐Reichardt solvent polarity parameter. This is consistent with the single‐electron transfer mechanism proposed for SET‐LRP that involves a polar transition state. These experiments demonstrate that the use of binary mixtures of solvents with H2O provides a new, simple and efficient method for the elaboration of a large diversity of reaction media that are suitable for SET‐LRP even when one of the two solvents does not mediate disproportionation of Cu(I)X. © 2009 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 47: 5577–5590, 2009 相似文献
73.
In several applications, underestimation of functions has proven to be a helpful tool for global optimization. In protein–ligand
docking problems as well as in protein structure prediction, single convex quadratic underestimators have been used to approximate
the location of the global minimum point. While this approach has been successful for basin-shaped functions, it is not suitable
for energy functions with more than one distinct local minimum with a large magnitude. Such functions may contain several
basin-shaped components and, thus, cannot be underfitted by a single convex underestimator. In this paper, we propose using
an underestimator composed of several negative Gaussian functions. Such an underestimator can be computed by solving a nonlinear
programming problem, which minimizes the error between the data points and the underestimator in the L
1 norm. Numerical results for simulated and actual docking energy functions are presented. 相似文献
74.
Self-injection length in La0.7Ca0.3MnO3-YBa2Cu3O7-δ ferromagnet-superconductor multilayer thin films
We have carried out extensive studies on the self-injection problem in barrierless heterojunctions between La0.7Ca0.3MnO3 (LCMO) and YBa2Cu3O7-δ (YBCO) thin films. The heterojunctions were formed in situ by sequentially growing LCMO and YBCO films on 〈100〉 LaAlO3 (LAO) substrate using a pulsed laser deposition (PLD) system. YBCO micro-bridges with 64 μm width were patterned both on
the LAO (control) and LCMO side of the substrate. Critical current, I
c, was measured at 77 K on both the control side as well as the LCMO side for different YBCO film thickness. It was observed
that while the control side showed a J
c of ∼ 2 × 106 A/cm2, the LCMO side showed about half the value for the same thickness (1800 ?). The difference in J
c indicates that a certain thickness of YBCO has become ‘effectively’ normal due to self-injection. From the measurement of
J
c at two different thicknesses (1800 ? and 1500 ?) of YBCO films both on the LAO as well as the LCMO side, the value of self-injection
length (at 77 K) was estimated to be ∼ 900 ?. To the authors’ best knowledge, this is the first time that self-injection length
has been quantified. A control experiment carried out with LaNiO3 deposited by PLD on YBCO did not show any evidence of self-injection. 相似文献
75.
Lone AM Bachovchin DA Westwood DB Speers AE Spicer TP Fernandez-Vega V Chase P Hodder PS Rosen H Cravatt BF Saghatelian A 《Journal of the American Chemical Society》2011,133(30):11665-11674
Peptidases play vital roles in physiology through the biosynthesis, degradation, and regulation of peptides. Prolyl endopeptidase-like (PREPL) is a newly described member of the prolyl peptidase family, with significant homology to mammalian prolyl endopeptidase and the bacterial peptidase oligopeptidase B. The biochemistry and biology of PREPL are of fundamental interest due to this enzyme's homology to the biomedically important prolyl peptidases and its localization in the central nervous system. Furthermore, genetic studies of patients suffering from hypotonia-cystinuria syndrome (HCS) have revealed a deletion of a portion of the genome that includes the PREPL gene. HCS symptoms thought to be caused by lack of PREPL include neuromuscular and mild cognitive deficits. A number of complementary approaches, ranging from biochemistry to genetics, will be required to understand the biochemical, cellular, physiological, and pathological mechanisms regulated by PREPL. We are particularly interested in investigating physiological substrates and pathways controlled by PREPL. Here, we use a fluorescence polarization activity-based protein profiling (fluopol-ABPP) assay to discover selective small-molecule inhibitors of PREPL. Fluopol-ABPP is a substrate-free approach that is ideally suited for studying serine hydrolases for which no substrates are known, such as PREPL. After screening over 300,000 compounds using fluopol-ABPP, we employed a number of secondary assays to confirm assay hits and characterize a group of 3-oxo-1-phenyl-2,3,5,6,7,8-hexahydroisoquinoline-4-carbonitrile and 1-alkyl-3-oxo-3,5,6,7-tetrahydro-2H-cyclopenta[c]pyridine-4-carbonitrile PREPL inhibitors that are able to block PREPL activity in cells. Moreover, when administered to mice, 1-isobutyl-3-oxo-3,5,6,7-tetrahydro-2H-cyclopenta[c]pyridine-4-carbonitrile distributes to the brain, indicating that it may be useful for in vivo studies. The application of fluopol-ABPP has led to the first reported PREPL inhibitors, and these inhibitors will be of great value in studying the biochemistry of PREPL and in eventually understanding the link between PREPL and HCS. 相似文献
76.
Peterca M Imam MR Ahn CH Balagurusamy VS Wilson DA Rosen BM Percec V 《Journal of the American Chemical Society》2011,133(7):2311-2328
The synthesis, structural, and retrostructural analysis of two libraries containing 16 first and second generation C(3)-symmetric self-assembling dendrimers based on dendrons connected at their apex via trisesters and trisamides of 1,3,5-benzenetricarboxylic acid is reported. A combination of X-ray diffraction and CD/UV analysis methods demonstrated that their C(3)-symmetry modulates different degrees of packing on the periphery of supramolecular structures that are responsible for the formation of chiral helical supramolecular columns and spheres self-organizable in a diversity of three-dimensional (3D) columnar, tetragonal, and cubic lattices. Two of these periodic arrays, a 3D columnar hexagonal superlattice and a 3D columnar simple orthorhombic chiral lattice with P222(1) symmetry, are unprecedented for supramolecular dendrimers. A thermal-reversible inversion of chirality was discovered in helical supramolecular columns. This inversion is induced, on heating, by the change in symmetry from a 3D columnar simple orthorhombic chiral lattice to a 3D columnar hexagonal array and, on cooling, by the change in symmetry from a 2D hexagonal to a 2D centered rectangular lattice, both exhibiting intracolumnar order. A first-order transition from coupled columns with long helical pitch, to weakly or uncorrelated columns with short helical pitch that generates a molecular rotator, was also discovered. The torsion angles of the molecular rotator are proportional to the change in temperature, and this effect is amplified in the case of the C(3)-symmetric trisamide supramolecular dendrimers forming H-bonds along their column. The structural changes reported here can be used to design complex functions based on helical supramolecular dendrimers with different degree of packing on their periphery. 相似文献
77.
Garbarine E DePasquale J Gadia V Polikar R Rosen G 《Computational Biology and Chemistry》2011,35(3):199-209
Analysis of DNA sequences isolated directly from the environment, known as metagenomics, produces a large quantity of genome fragments that need to be classified into specific taxa. Most composition-based classification methods use all features instead of a subset of features that may maximize classifier accuracy. We show that feature selection methods can boost performance of taxonomic classifiers. This work proposes three different filter-based feature selection methods that stem from information theory: (1) a technique that combines Kullback-Leibler, Mutual Information, and distance information, (2) a text mining technique, TF-IDF, and (3) minimum redundancy-maximum-relevance (mRMR). The feature selection methods are compared by how well they improve support vector machine classification of genomic reads. Overall, the 6mer mRMR method performs well, especially on the phyla-level. If the number of total features is very large, feature selection becomes difficult because a small subset of features that captures a majority of the data variance is less likely to exist. Therefore, we conclude that there is a trade-off between feature set size and feature selection method to optimize classification performance. For larger feature set sizes, TF-IDF works better for finer-resolutions while mRMR performs the best out of any method for N=6 for all taxonomic levels. 相似文献
78.
A convenient, general, and high yielding Pd-catalyzed cross-coupling of methanesulfonamide with aryl bromides and chlorides is reported. The use of this method eliminates concern over genotoxic impurities that can arise when an aniline is reacted with methanesulfonyl chloride. The application of this method to the synthesis of dofetilide is also reported. 相似文献
79.
80.
Study of magnetoresistance and conductance of bicrystal grain boundary in La0.67Ba0.33MnO3 thin film
La0.67Ba0.33MnO3 (LBMO) thin film is deposited on a 36.7°C SrTiO3 bicrystal substrate using laser ablation technique. A microbridge is created across bicrystal grain boundary and its characteristics
are compared with a microbridge on the LBMO film having no grain boundary. Presence of grain boundary exhibits substantial
magnetoresistance ratio (MRR) in the low field and low temperature region. Bicrystal grain boundary contribution in MRR disappears
at temperature T>175 K. At low temperature, I-V characteristic of the microbridge across bicrystal grain boundary is nonlinear. Analysis of temperature dependence of dynamic
conductance-voltage characteristics of the bicrystal grain boundary indicates that at low temperatures (T<175 K) carrier transport across the grain boundary in LBMO film is dominated by inelastic tunneling via pairs of manganese
atoms and tunneling through disordered oxides. At higher temperatures (T>175 K), magnetic scattering process is dominating. Decrease of bicrystal grain boundary contribution in magnetoresistance
with the increase in temperature is due to enhanced spin-flip scattering process. 相似文献