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31.
McCullough DH Grygorash R Hsu JT Regen SL 《Journal of the American Chemical Society》2007,129(27):8663-8667
Permeation measurements have been made for He, CO2, and N2 across single Langmuir-Blodgett (LB) bilayers derived from 1,2,4,5-tetrakis[(N-(undecanoamidoethyl)-N,N-dimethyl ammonium) methyl]benzene tetrabromide (2) and 1,2,4,5-tetrakis[(N-(perfluoroundecanoamidoethyl)-N,N-dimethyl ammonium)methyl]benzene tetrabromide (3) in the absence and in the presence of entrapped poly(acrylic acid) (PAA). In the absence of PAA, single LB bilayers of 3 show a higher permeance for He and N2 but a lower permeation rate of CO2, as compared with analogous LB bilayers made from 2. The relatively low permeation rate of CO2 for the former has been attributed to reduced associative interactions with the fluorocarbon-rich bilayer. The same behavior has also been observed for LB bilayers containing PAA, formed under conditions that yield glued bilayers of 2 and 3 having similar diffusional pathways, as judged by He/N2 selectivities. These results, together with the fact that glued bilayers of 2 (having a thinner PAA layer as compared with those made from 3) exhibit lower He and N2 permeances, provide compelling evidence that the main barrier for gas transport is the combination of surfactant plus PAA and not simply a thin PAA layer that is encased within the surfactant bilayer. 相似文献
32.
Zhang R Li B Iovu MC Jeffries-El M Sauvé G Cooper J Jia S Tristram-Nagle S Smilgies DM Lambeth DN McCullough RD Kowalewski T 《Journal of the American Chemical Society》2006,128(11):3480-3481
Low polydispersity regioregular polythiophenes with number average molecular weights ranging from 2 to 13 kDa were cast under the same conditions from solution to form a series of field effect transistors (FETs). Tapping mode AFM and grazing incidence small-angle X-ray scattering revealed that in all cases the polymers formed regular nanofibrillar morphologies with the width of nanofibrils proportional to the weight average contour length of polymer chains, indicating that conjugated backbones were oriented perpendicular to the nanofibril axes. FET charge carrier mobilities exhibited exponential dependence on nanofibril width, pointing to the decisive role of extended conjugated pathways in charge transport. 相似文献
33.
JP Safko JE Kuperstock SM McCullough AM Noviello X Li JP Killarney C Murphy HH Patterson CA Bayse RD Pike 《Dalton transactions (Cambridge, England : 2003)》2012,41(38):11663-11674
The synthesis, X-ray structures and photophysics of ten complexes of CuX (X = I or Br) with bridging N-substituted and N,N'-disubstituted piperazines (Pip) are presented. Depending on the steric demand of the Pip substituents, the complexes fall into four categories: (CuX)(4)(Pip)(2), which are networks of linked Cu(4)X(4) cubane units, (CuX)(2)(Pip), which are chains of linked Cu(2)X(2) rhombs, and (CuX)(2)(Pip)(2) or (CuX)(4)(Pip)(4), which are simple rhomboid dimers and cubane tetramers. A combination of spectroscopic studies and DFT calculations was used to investigate the luminescence of the products. The results suggest that the relatively high energy emission seen in dimers is due to cluster-centred (XMLT/metal-centred) excitations for the aliphatic amines and MLCT (d →π*) for aromatic amines, and low energy emission seen in the tetramers is the result of cluster-centred transitions. The (CuI)(2)(Pip) complexes act as sensor materials, undergoing irreversible reaction with aliphatic and aromatic amines (Nu) in the vapour state, irreversibly producing cubanes (CuI)(4)Nu(4), with corresponding production of long wavelength emission. 相似文献
34.
Jerri HA Adolfsen KJ McCullough LR Velegol D Velegol SB 《Langmuir : the ACS journal of surfaces and colloids》2012,28(4):2262-2268
Moringa oleifera (Moringa) seeds contain a natural cationic protein (MOCP) that can be used as an antimicrobial flocculant for water clarification. Currently, the main barrier to using Moringa seeds for producing potable water is that the seeds release other water-soluble proteins and organic matter, which increase the concentration of dissolved organic matter (DOM) in the water. The presence of this DOM supports the regrowth of pathogens in treated water, preventing its storage and later use. A new strategy has been established for retaining the MOCP protein and its ability to clarify and disinfect water while removing the excess organic matter. The MOCP is first adsorbed and immobilized onto sand granules, followed by a rinsing step wherein the excess organic matter is removed, thereby preventing later growth of bacteria in the purified water. Our hypotheses are that the protein remains adsorbed onto the sand after the functionalization treatment, and that the ability of the antimicrobial functionalized sand (f-sand) to clarify turbidity and kill bacteria, as MOCP does in bulk solution, is maintained. The data support these hypotheses, indicating that the f-sand removes silica microspheres and pathogens from water, renders adhered Escherichia coli bacteria nonviable, and reduces turbidity of a kaolin suspension. The antimicrobial properties of f-sand were assessed using fluorescent (live-dead) staining of bacteria on the surface of the f-sand. The DOM that can contribute to bacterial regrowth was shown to be significantly reduced in solution, by measuring biochemical oxygen demand (BOD). Overall, these results open the possibility that immobilization of the MOCP protein onto sand can provide a simple, locally sustainable process for producing storable drinking water. 相似文献
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36.
This article treats Nevanlinna–Pick interpolation in the setting of a special class of algebraic curves called distinguished varieties. An interpolation theorem, along with additional operator theoretic results, is given using a family of reproducing kernels naturally associated to the variety. The examples of the Neil parabola and doubly connected domains are discussed. 相似文献
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39.
Herr DE Mays MD McCullough RD Bailey AB Cowan DO 《The Journal of organic chemistry》1996,61(20):7006-7011
A systematic synthetic study of the pi-donor tetratellurafulvalene (TTeF, 6) has resulted in an optimized preparation producing repeatable yields of over 20%. The use of a "one-step" Li/Sn metal exchange/Te(0) insertion procedure and freshly prepared microcrystalline Te(0) serve to drive toward products, the equilibria converting (Z)-1,2-bis(trimethylstannyl)ethylene (1) to its corresponding metal-exchanged vinyllithium species and subsequently to lithium ditellurolate 5. Furthermore, the use of LiCl as an additive to enhance the reactivity of n-BuLi in these metal exchange reactions also increases yields and reproducibility. The slow addition of 1 equiv of tetrahaloethylene during the final cyclization step favors intramolecular reactions which produce TTeF vs intermolecular reactions that lead to oligomeric byproducts. The use of tetrabromoethylene in place of tetrachloroethylene in this step also reduces byproduct formation. 相似文献
40.
Zhong-Guo Shi E. A. McCullough Jr. 《Journal of inclusion phenomena and macrocyclic chemistry》1994,18(1):9-26
The complexing properties of macrocyclic ligands have been quantitatively studied by the combined use of molecular mechanics, molecular dynamics, and multiple linear regression. The dependent variables in the regression equations are experimental equilibrium constants for known macrocycle complexes in various solvents. The independent variables are theoretical simulation results on the solvent-free ligand and its complex and additional physically motivated empirical variables to describe solvent and other important effects.The systems studied were: (a) 314 metal ion-macrocycle-solvent (including 3 mixed solvents) combinations; (b) 88 ammonium ion-crown ether-solvent (including 1 mixed solvent) combinations; (c) 24 hydrogen ion-crown ether-H2O combinations; (d) 26 Na+ ion-spherand-CDCl3 combinations; (e) 78 ammonium ion-spherand-CDCl3 combinations; and (f) 73 complicated host-guest-solvent (including 1 mixed solvent) combinations.For each system, we report the best regression equation obtained using the AMBER force field. The standard errors in logK range from 1.42 in the largest system to 0.36 in the smallest. Regression equations were determined for several of the systems using the MMP2 force field as well, and the equations are shown to be relatively insensitive to the force field.The predictive ability of the method was tested by predicting logK for 20% of the cases chosen at random using equations derived from the remaining 80%. The errors in the predicted values are shown to be consistent with the statistical assumptions of the model.Regression equations obtained with this method can be used to predict the equilibrium constants for new complexes involving some combination of new, possibly unknown macrocycle, new host and, in certain cases new solvent. No X-ray or other structural data for the macrocycle is needed. 相似文献