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231.
Lou Ann Tom Chelsea L. Gerard Colin M. Hutchison Amanda S. Brooker 《Mikrochimica acta》2012,176(3-4):375-380
Several molecularly imprinted polymers (MIPs) for the retention of 4,6-dimethyldibenzothiophene (4,6-DMDBT) were prepared. The first was a polymer prepared non-covalently with methacrylic acid and ethylene glycol dimethacrylate polymerized in the presence of 4,6-DMDBT. After extraction of 4,6-DMDBT, the selectivity of the imprinted polymer was evaluated by HPLC and compared to a non-imprinted control polymer prepared without 4,6-DMDBT. The imprinted polymer retained 4,6-DMDBT slightly longer than the control polymer. The second polymer was prepared using nickel (II)-methacryloylhistidinedihydrate monomer which was combined with 4,6-DMDBT, and polymerized with ethylene glycol dimethacrylate. This is a novel use of this monomer for retention of sulfur-containing organic compounds. Selectivity for 4,6-DMDBT was much greater in this polymer compared to the first, and retention in acetonitrile was more than three times greater on the imprinted polymer compared to a control polymer. Results indicate the potential use of this novel MIP for the removal of organosulfur compounds from fuel. Figure
Chromatograms of a solution of acetone and 10 ppm 4,6-DMDBT in acetonitrile, evaluated on a non-imprinted control (dashed line) and imprinted test (solid line) polymers. Peak at 1.5 min on control column are acetone and 4,6-DMDBT. Peak at 1.5 min on test column is acetone and at 2.5 min is 4,6-DMDBT. 相似文献
232.
Potapenko DI Foster MA Lurie DJ Kirilyuk IA Hutchison JM Grigor'ev IA Bagryanskaya EG Khramtsov VV 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2006,182(1):1-11
New improved pH-sensitive nitroxides were applied for in vivo studies. An increased stability of the probes towards reduction was achieved by the introduction of the bulky ethyl groups in the vicinity of the paramagnetic NO fragment. In addition, the range of pH sensitivity of the approach was extended by the synthesis of probes with two ionizable groups, and, therefore, with two pKa values. Stability towards reduction and spectral characteristics of the three new probes were determined in vitro using 290 MHz radiofrequency (RF)- and X-band electron paramagnetic resonance (EPR), longitudinally detected EPR (LODEPR), and field-cycled dynamic nuclear polarization (FC-DNP) techniques. The newly synthesized probe, 4-[bis(2-hydroxyethyl)amino]-2-pyridine-4-yl-2,5,5-triethyl-2,5-dihydro-1H-imidazol-oxyl, was found to be the most appropriate for the application in the stomach due to both higher stability and convenient pH sensitivity range from pH 1.8 to 6. LODEPR, FC-DNP and proton-electron double resonance imaging (PEDRI) techniques were used to detect the nitroxide localization and acidity in the rat stomach. Improved probe characteristics allowed us to follow in vivo the drug-induced perturbation in the stomach acidity and its normalization afterwards during 1 h or longer period of time. The results show the applicability of the techniques for monitoring drug pharmacology and disease in the living animals. 相似文献
233.
Kiya Y Hutchison GR Henderson JC Sarukawa T Hatozaki O Oyama N Abruña HD 《Langmuir : the ACS journal of surfaces and colloids》2006,22(25):10554-10563
The redox reactions of DMcT at PEDOT-modified glassy carbon electrodes (GCEs) in acetonitrile (AN) have been investigated via cyclic voltammetry (CV) and the electrochemical quartz crystal microbalance (EQCM) in order to elucidate the redox reaction mechanism. A redox couple at -0.29 V versus Ag/Ag+ was assigned to the dimerization process of singly protonated DMcT (DMcT-1H), and a second couple observed at +0.42 V was assigned to the polymerization process of the protonated DMcT dimer. Our investigations revealed further that the anodic current response at +0.55 V (polymerization process) has a shoulder at +0.38 V ascribed to the dimerization process of doubly protonated DMcT (DMcT-2H), indicating that the redox couple at +0.42 V is the overlapping response of the polymerization of the protonated DMcT dimer and the dimerization of the DMcT-2H monomer. It was also confirmed that the dimerization process of DMcT-1H at -0.29 V proceeded not only at the surface of a PEDOT film but also inside the film as previously suggested. Moreover, the thermodynamics of these redox reactions at PEDOT-modified GCEs are dependent on the basicity (or acidity) of the solution, as anticipated and previously shown at unmodified GCEs. The oxidation of DMcT occurs at less positive potentials and the reduction occurs at more negative potentials in the presence of base. On the basis of the results obtained, the full redox reaction scheme for DMcT at a PEDOT-modified GCE is proposed. 相似文献
234.
The Blue Obelisk-interoperability in chemical informatics 总被引:1,自引:0,他引:1
Guha R Howard MT Hutchison GR Murray-Rust P Rzepa H Steinbeck C Wegner J Willighagen EL 《Journal of chemical information and modeling》2006,46(3):991-998
The Blue Obelisk Movement (http://www.blueobelisk.org/) is the name used by a diverse Internet group promoting reusable chemistry via open source software development, consistent and complimentary chemoinformatics research, open data, and open standards. We outline recent examples of cooperation in the Blue Obelisk group: a shared dictionary of algorithms and implementations in chemoinformatics algorithms drawing from our various software projects; a shared repository of chemoinformatics data including elemental properties, atomic radii, isotopes, atom typing rules, and so forth; and Web services for the platform-independent use of chemoinformatics programs. 相似文献
235.
Purification and size-based separation of nanoparticles remain significant challenges in the preparation of well-defined materials for fundamental studies and applications. Diafiltration shows considerable potential for the efficient and convenient purification and size separation of water-soluble nanoparticles, allowing for the removal of small-molecule impurities and for the isolation of small nanoparticles from larger nanostructures in a single process. Herein, we report studies aimed at assessing the suitability of diafiltration for (i) the purification of water-soluble thiol-stabilized 3-nm gold nanoparticles, (ii) the separation of a bimodal distribution of nanoparticles into the corresponding fractions, and (iii) the separation of a polydisperse sample into fractions of differing mean core diameter. NMR, thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS) measurements demonstrate that diafiltration produces nanoparticles with a much higher degree of purity than is possible by dialysis or a combination of solvent washes, chromatography, and ultracentrifugation. UV-visible spectroscopic and transmission electron microscopic (TEM) analyses show that diafiltration offers the ability to separate nanoparticles of disparate core size. These results demonstrate the applicability of diafiltration for the rapid and green preparation of high-purity gold nanoparticle samples and the size separation of heterogeneous nanoparticle samples. They also suggest the development of novel diafiltration membranes specifically suited to high-resolution nanoparticle size separation. 相似文献
236.
Collisions of I2 in the E(0(g)+) electronic state with CF4 molecules induce electronic energy transfer to the nearby D, beta, and D' ion-pair states. Simulations of dispersed fluorescence spectra reveal collision-induced electronic energy transfer rate constants and final vibrational state distributions within each final electronic state. In comparison with earlier reports on I2(upsilon(E)=0-2) collisions with He or Ar atoms, we find markedly different dynamics when I2, excited to the same rovibronic states, collides with CF4. Final vibrational state distributions agree with the associated Franck-Condon factors with the initially prepared state to a greater degree than those found with He or Ar collision partners and suggest that internal degrees of freedom in the CF4 molecule represent a substantial means for accepting the accompanying loss of I2 vibronic energy. Comparison of the E-->D transfer of I2 excited to the J=23 and J=55 levels of the upsilon(E)=0 state reveals the onset of specific, nonstatistical dynamics as the available energy is increased above the threshold for excitation of the low frequency nu2 bending mode of CF4. 相似文献
237.
Parks BW Gilbertson RD Domaille DW Hutchison JE 《The Journal of organic chemistry》2006,71(26):9622-9627
A general synthetic approach was developed for the preparation of a series of 6,6-bicyclic malonamides, a class of ligands that provide a preorganized binding site for f-block ions (particularly trivalent lanthanides). The approach described is convenient to introduce a variety of functional groups at the amide nitrogens to tune the properties of the ligand without altering the preorganized binding. Each of the ten derivatives (that represent a range of functionality, including R = alkyl, hydroxy, phenyl, ester, perfluorocarbon) reported here derives from a single, readily prepared dialdehyde intermediate. This intermediate is converted to the final products via reductive amination with an appropriately functionalized benzylamine, followed by hydrogenolysis and lactam formation. Because derivatization occurs late in the synthesis, the approach is general, requiring only modification of the purification procedures for each new derivative. To aid in the purification of the bicyclic malonamides, we report a novel complexation-based purification method that takes advantage of the high affinity of the ligand for f-block metals. 相似文献
238.
Eric D. Morrison Megan W. Malvey Richard D. Johnson Jeffrey S. Hutchison 《Polymer Degradation and Stability》2010,95(4):656-665
A recently described bottle test method was used to evaluate the dependence of stress crack failure of poly(ethylene terephthalate) (PET) carbonated soft drink bottles on water hardness. Although the industry belief is that water hardness is irrelevant to stress cracking, it was found that hardness ions exert a tremendous positive impact by deactivating water alkalinity through precipitation as harmless carbonate minerals. This mitigating effect of hardness means that no complete understanding of stress cracking as a function of alkalinity is possible without also considering water hardness. A useful concept is that of excess alkalinity, which is defined as alkalinity that is not precipitated during solution evaporation. Limiting excess alkalinity by using water with sufficient hardness is an effective means of stress crack prevention in PET soft drink bottles. Evaluation of compositions which are typical of those used for lubricating PET bottles on production conveyors showed that the role of these compositions in stress cracking was that of spectators, that is, they neither cause failure if water does not otherwise cause it, nor stop failure if water otherwise causes it. 相似文献
239.
Hutchison W. D. Chaplin D. H. Harker S. J. Bowden G. J. 《Hyperfine Interactions》2001,136(3-8):307-312
A NMRON study of magnetically ordered HoF3 using in-situ neutron activated 166m
Ho (I=7) isoelectronic probes in a spherical single crystal is presented. The optimal sensitivity to resonant change in the gamma-ray
anisotropy of the 810 keV daughter gamma-ray emission has been utilised to track the lowest nuclear Zeeman substate resonance
over an applied magnetic field range from 0.300 to 0.524 T, corresponding to the frequency range 1.56 to 1.78 GHz. The 2nd
lowest substate resonance has also been observed at 0.3 T leading to a value P/h=−32.9(14) MHz for the 166m
Ho quadrupolar splitting which is consistent with predictions of a dominant negative pseudo-quadrupole interaction in this
system. The Ho3+ electronic moment, in zero applied magnetic field, is projected to be 16% smaller than measured previously with neutron diffraction.
This revised version was published online in September 2006 with corrections to the Cover Date. 相似文献