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151.
Pyrazolium-3-carboxylates were examined as relatives of the betainic alkaloid Nigellicine and as new examples of the sparsely populated class 16 of heterocyclic pseudo-cross-conjugated mesomeric betaines (PCCMB). The title compounds were prepared in a 4-step procedure starting from beta-diketo compounds 8 which were cyclized with substituted hydrazines. The resulting isomeric pyrazole esters 9 and 10 were separated and subsequently quaternized with dimethyl sulfate in the presence of nitrobenzene to pyrazolium esters 11 and 12. Saponification was best accomplished in diluted sulfuric acid, which resulted in the formation of the pseudo-cross-conjugated mesomeric betaines 13 and 14 in one step. Protonation to the corresponding carboxylic acids required the treatment of the betaines with tetrafluoroboric acid in dichloromethane. The effect of negative solvatochromism proves the charge separation in the ground state of the molecules. X-ray crystallographic analyses, semiempirical calculations, and ESI mass spectrometric measurements were performed to gain knowledge about the phenomenon of pseudo-cross-conjugation. 相似文献
152.
Coleman BD Swigon D Tobias I 《Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics》2000,61(1):759-770
Configurations of protein-free DNA miniplasmids are calculated with the effects of impenetrability and self-contact forces taken into account by using exact solutions of Kirchhoff's equations of equilibrium for elastic rods of circular cross section. Bifurcation diagrams are presented as graphs of excess link, DeltaL, versus writhe, W, and the stability criteria derived in paper I of this series are employed in a search for regions of such diagrams that correspond to configurations that are stable, in the sense that they give local minima to elastic energy. Primary bifurcation branches that originate at circular configurations are composed of configurations with D(m) symmetry (m=2,3,...). Among the results obtained are the following. (i) There are configurations with C2 symmetry forming secondary bifurcation branches which emerge from the primary branch with m=3, and bifurcation of such secondary branches gives rise to tertiary branches of configurations without symmetry. (ii) Whether or not self-contact occurs, a noncircular configuration in the primary branch with m=2, called branch alpha, is stable when for it the derivative dDeltaL/dW, computed along that branch, is strictly positive. (iii) For configurations not in alpha, the condition dDeltaL/dW>0 is not sufficient for stability; in fact, each nonplanar contact-free configuration that is in a branch other than alpha is unstable. A rule relating the number of points of self-contact and the occurrence of intervals of such contact to the magnitude of DeltaL, which in paper I was found to hold for segments of DNA subject to strong anchoring end conditions, is here observed to hold for computed configurations of protein-free miniplasmids. 相似文献
153.
Tobias I Swigon D Coleman BD 《Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics》2000,61(1):747-758
Results are presented in the theory of the elastic rod model for DNA, among which are criteria enabling one to determine whether a calculated equilibrium configuration of a DNA segment is stable in the sense that it gives a local minimum to the sum of the segment's elastic energy and the potential of forces acting on it. The derived stability criteria are applicable to plasmids and to linear segments subject to strong anchoring end conditions. Their utility is illustrated with an example from the theory of configurations of the extranucleosomal loop of a DNA miniplasmid in a mononucleosome, with emphasis placed on the influence that nicking and ligation on one hand, and changes in the ratio of elastic coefficients on the other, have on the stability of equilibrium configurations. In that example, the configurations studied are calculated using an extension of the method of explicit solutions to cases in which the elastic rod modeling a DNA segment is considered impenetrable, and hence excluded volume effects and forces arising from self-contact are taken into account. 相似文献
154.
Rui M. Novais Frank Simon Petra Pötschke Tobias Villmow José A. Covas Maria C. Paiva 《Journal of polymer science. Part A, Polymer chemistry》2013,51(17):3740-3750
This work reports the study of the effect of chemical functionalization of carbon nanotubes on their dispersion in poly(lactic acid). The nanotubes were functionalized by the 1,3‐dipolar cycloaddition reaction, generating pyrrolidine groups at the nanotube surface. Further reaction of the pyrrolidine groups with poly(lactic acid) was studied in solution and in the polymer melt. The former involved refluxing the nanotubes in a dimethylformamide/polymer solution; the latter was carried out by direct melt mixing in a microcompounder. The carbon nanotubes collected after each process were characterized by thermogravimetry and by X‐ray photoelectron spectroscopy, showing evidence of polymer bonded to the nanotube surface only when the reaction was carried out in the polymer melt. The composites with polymer modified nanotubes present smaller average agglomerate area and a narrower agglomerate area distribution. In addition, they show improved tensile properties at low CNT concentration and present lower electrical resistivity. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2013, 51, 3740–3750 相似文献
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Current models for pressure drop prediction of slug flow pneumatic conveying in a horizontal pipeline system assume some type of steady state conditions for prediction,which limits their capability for increased predictive accuracy relative to experimental data.This is partly because of the nature of slug flow pneumatic conveying system,which,as a dynamic system,never becomes stable.By utilising conservation of mass (airflow),a dynamic pressure analysis model is proposed on the basis of the derivative of the upstream pressure behaviour.The rate of air permeation through slug,one of the important factors in the conservation model,is expressed as a function of a slug permeability factor.Other factors such as slug velocity,slug length and the fraction of stationary layer were also considered.Several test materials were conveyed in single-slug tests to verify the proposed pressure drop model,showing good agreement between the model and experimental results. 相似文献