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91.
92.
Annelation reactions between pentafluorobenzonitrile and N,N-dimethylethylene diamine and 3-methyl picoline gave [6,6]-bicyclic and [6,5,6]-tricyclic ring-fused systems, respectively. Reaction of 4-morpholino tetrafluorobenzonitrile with hydrazine and phenyl hydrazine gave [5,6] ring-fused systems arising from a tandem SNAr and cyclisation process involving annelation onto the pendant cyano group providing an indication of the synthetic possibilities for heterocycle formation using the pentafluorobenzonitrile scaffold. 相似文献
93.
Greszler SN Reichard HA Micalizio GC 《Journal of the American Chemical Society》2012,134(5):2766-2774
A convergent synthesis of highly substituted and stereodefined dihydroindanes is described from alkoxide-directed Ti-mediated cross-coupling of internal alkynes with substituted 4-hydroxy-1,6-enynes (substrates that derive from 2-directional functionalization of readily available epoxy alcohol derivatives). In addition to describing a new and highly stereoselective approach to bimolecular [2 + 2 + 2] annulation that delivers products not available with other methods in this area of chemical reactivity, evidence is provided to support annulation by way of regioselective alkyne-alkyne coupling, followed by metal-centered [4 + 2] rather than stepwise alkene insertion and reductive elimination. Overall, the reaction proceeds with exquisite stereochemical control and defines a convenient, convergent, and enantiospecific entry to fused carbocycles of great potential value in target-oriented synthesis and medicinal chemistry. 相似文献
94.
Andrei L. Ghindilis Maria W. Smith Kevin R. Schwarzkopf Changqing Zhan David R. Evans António M. Baptista Holly M. Simon 《Electroanalysis》2009,21(13):1459-1468
A novel, impedance‐based electronic sensor format was used for label‐free, real‐time detection of microbial DNA on oligonucleotide probe arrays. Detection limits of 5–10 nM were achieved for single‐stranded, PCR‐amplified DNA targets. Hybridization selectivity yielded 9‐ to 12‐fold signal increases for specific targets, and the sensor arrays were re‐used multiple times without significant signal degradation. These and other features of the SHARP Laboratories of America (SLA) sensor array, such as its ability to acquire continuous measurements of DNA as it accumulates on the array surface, make it an attractive biosensor platform for field detection and monitoring of sentinel and/or pathogenic microorganisms. 相似文献
95.
Everest MA Black VM Haehlen AS Haveman GA Kliewer CJ Neill HA 《The journal of physical chemistry. B》2006,110(39):19461-19468
Evanescent-wave cavity ring-down spectroscopy was used to monitor the adsorption of human hemoglobin to a fused-silica surface from aqueous solution. An uncoated dove prism was situated in a ring-down cavity such that the beam entered and exited with a normal-incidence geometry. This afforded ring-down times as high as 5 mus and values of sigma(tau)/tau as low as 0.3%. Normal-incidence geometry permits the detection of both S- and P-polarized light, yielding some information of the orientation of adsorbates. The orientation of the adsorbed hemoglobin molecules is found to change as adsorption progresses, but with a different time profile than adsorption itself. The adsorption kinetics from a quiescent solution is consistent with a reaction-diffusion model that includes both reversible and irreversible adsorption operating in parallel. Systems behaving according to this model also seem to display adsorption isotherms, although the increased adsorption from more concentrated solutions is only a consequence of the system being under kinetic control. In some cases, this may be sufficient to explain the paradox of protein adsorption systems which seem to be both irreversible and consistent with isotherm models as well. 相似文献
96.
Hydrogen-bonding interactions in peptide nucleic acid and deoxyribonucleic acid: a comparative study
Herbert HE Halls MD Hratchian HP Raghavachari K 《The journal of physical chemistry. B》2006,110(7):3336-3343
Peptide nucleic acid (PNA) is a synthetic analogue of deoxyribonucleic acid (DNA) capable of tightly binding to itself and DNA with high specificity. Using hybrid density functional methods, hydrogen-bond (H-bond) strengths have been evaluated for isolated Watson-Crick base pairs, PNA base pairs, and charged as well as neutral DNA base pairs. Heterogeneous base pairs of PNA with charged and neutral DNA have also been investigated. The competing effects of short-range H-bonding and long-range Coulombic repulsions in charged DNA base pairs have been analyzed. Polarizable continuum models have been employed to evaluate solvation effects on the binding energies. 相似文献
97.
Polymerizable ionic liquids and their actuation in an electric field are a combination of material and properties with unique potential to display structural and fluid dynamics above that found in small molecule ionic liquids. In an effort to blend ionic liquid nature with actuation response, we have synthesized a new ionic liquid ammonium sulfonate monomer and polymer. The liquid temperature ranges of both the monomer and polymer ionic liquid systems are quite large extending from their respective glass transitions (Tg) of -57 and -49 degrees C to decomposition at approximately 200 degrees C. Particularly remarkable is the small Tg increment that accompanies the transformation from monomer to polymer. The electrowetting behavior of the polymer and of the monomer presents an interesting contrast. This communication will encompass the polymerization, characterization, and actuation of these new ionic liquids. 相似文献
98.
This paper considers the difficulties associated with a production process that contains a sub-process that is not fully understood and for which data for many parameters are only able to be approximately obtained. The aluminium smelting industry epitomizes such a situation. Here, the critical sub-process that exemplifies these difficulties is the actual heart of the smelter, the electrolytic processing of alumina. This sub-process of aluminium production is at best ‘fuzzy’ and relies on the smelter operators to use their experience and tacit knowledge on a day-to-day basis, that is, the sub-process involves ‘alchemy’. In this paper, this is referred to as the tacit knowledge problem. The impact of such sub-processes on production is significant and the development of a methodology that will lead to a reduced reliance on uncertain alchemy associated with them, highly beneficial. The role of Communities of Practice in finding a solution to the tacit knowledge problem is discussed together with its integration into a mixed-mode model for the determination of best practice production for the smelter. 相似文献
99.
100.
M G Nicholls B J Cargill K S Dhir 《The Journal of the Operational Research Society》2004,55(5):440-452
In this paper, a methodology for the ongoing diagnosis and facilitation (when required) of organizational change management programmes in an Australian University is described. The application of this methodology on an annual basis requires the assessment of research attitudes and behaviour, areas that have assumed considerable importance within universities around the world in the last decade. This increasing importance associated with research stems in part (a significant part) from the linkage of research quantum (output) of universities to their funding from government. The methodology developed in this paper embraces a wide range of OR-type techniques as well as a range of change management tools from human resources management. These two sets of techniques and tools work together as tools in their own right as well as providing the infrastructure to achieve the objectives. The developed methodology is an interesting blend of hard techniques and ‘soft’ approaches implemented through a soft heuristic, indeed this application is an example of mixed-mode modelling. The OR techniques (conventional in both their nature and application) are comprised of social judgement theory (for bench-marking research attitudes) and integer linear programming (for setting research targets). The results of the application of the developed methodology are discussed in terms of the effect on research quantum over a 5-year period. A similar methodology could be developed for a change process covering aspects of an organization other than research output in a number of countries. 相似文献