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The first general approach to enantioselective catalysis of the Diels-Alder reaction with simple ketone dienophiles has been accomplished. The use of iminium catalysis has enabled enantioselective access to a fundamental Diels-Alder reaction variant that has previously been unavailable using chiral Lewis acid catalysis. A new chiral amine catalyst has been developed that allows a variety of monodentate cyclic and acyclic ketones to successfully participate in enantioselective [4 + 2] cycloadditions. A wide spectrum of cyclic and acyclic diene substrates can also be accommodated in this new organocatalytic transformation. A computational model is provided that is in accord with the sense of enantioinduction observed for all reactions conducted during the course of this study. 相似文献
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Wijkens P Jastrzebski JT van Der Schaaf PA Kolly R Hafner A van Koten G 《Organic letters》2000,2(11):1621-1624
A general method for the functionalization of Si-Cl terminated carbosilane dendritic molecules via organolithium or organomagnesium reagents is described. Quantitative exchange of the bromine atoms of 4-bromophenyl-functionalized dendrimers affords polylithiated species that are valuable starting materials for further functionalization, e.g., into pyridyl alcohols. The latter were successfully applied as catalyst precursors in a ruthenium-mediated ring-closure metathesis reaction. 相似文献
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Vinyl ketones are prepared by reaction of an aldehyde with a vinyl Grignard reagent followed by a Swern oxidation. β-Phthalimido ketones are then obtained by 1,4-addition of phthalimide. 相似文献
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Voyles PM Chadi DJ Citrin PH Muller DA Grazul JL Northrup PA Gossmann HJ 《Physical review letters》2003,91(12):125505
Electron channeling experiments performed on individually scanned, single columns of atoms show that in highly n-type Si grown at low temperatures the primary electrically deactivating defect cannot belong to either the widely accepted class of donor-vacancy clusters or a recently proposed class of donor pairs. First-principles calculations suggest a new class of defects consisting of two dopant donor atoms near a displaced Si atom, which forms a vacancy-interstitial pair. These complexes are consistent with the present experimental results, the measured open volume of the defects, the observed electrical activity as a function of dopant concentration, and the enhanced diffusion of impurities in the presence of deactivated dopants. 相似文献