A high yielding (93%), regiospecific synthesis of cis(4,4')-di(carbomethoxybenzo)-30-crown-10 (1c) is reported. The derived crown ether diol 1d was converted to pyridyl cryptand 12 in 44% yield by reaction with pyridine-2,6-dicarbonyl chloride. Binding of two different 4,4'-bipyridinium (paraquat) species (3) and 2,2'-bipyridinium (diquat) 4 by 12 was explored via (1)H NMR spectroscopy, NOE experiments, mass spectrometry, X-ray crystallographic analyses, and isothermal titration calorimetry. Cryptand 12 exhibits the highest association constant for diquat ever reported (Ka = 1.9 x 10(6) M(-1)) and very high association constants for paraquats (Ka > 10(5) M(-1)) in acetone at 22 degrees C. The binding constant of diquat 4 by cryptand 12 is nearly 6-times higher than any other reported host.
The Empress Judith has been assigned a central role in the reign of Louis the Pious. But the part she has played has been a controversial one. Judith has been stigmatized as a problem, if not the problem, in the reign. In July 817 Louis had made arrangements for the succession in the Ordinatio imperii, which divided the Empire between his three legitimate sons, Lothar, Pippin, and the young Louis: a few months after the death of their mother, Irmengard, in October 818, the forty-year-old Emperor married for a second time. The young Judith gave Louis another son, Charles, born on 13 June 823. A long historiographical tradition has isolated Judith’s political activities on behalf of her son as a cause of strife, provoking, for example, the rebellions against Louis in 830 and 833. And she stands condemned for this as a woman. In the nineteenth century Judith was seen as motivated not by reason but by emotion—blind Mutterliebe—and as having deployed ‘feminine wiles’ to further her ends. In the 1980s the language may have changed, but Judith is still seen in similar terms: Pierre Riche has described her influence over her middle-aged husband as ‘toute-puissante’. This view of Judith is overly dependent upon two sources which are not only hostile to Judith, but also reveal a strong ecclesiastical bias.
Supplementary Appendix A from Association of Insurance and Race/Ethnicity with Disease Severity among Men Diagnosed with Prostate Cancer, National Cancer Database 2004-2006
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