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Robin Polt - One of the best experts on this subject based on the ideXlab platform.

  • asymmetric syntheses of 8 epi swainsonine triacetate and 1 2 di epi swainsonine carbonyl addition thwarted by an unprecedented aza pinacol rearrangement
    Journal of Organic Chemistry, 2000
    Co-Authors: Hossein Razavi, Robin Polt
    Abstract:

    Indolizidines (-)-8-epi-swainsonine triacetate and (+)-1, 2-di-epi-swainsonine were synthesized from the O'Donnell Schiff base ester 1 derived from D-serine. Reductive-alkenylation of 1 with (i)()Bu(5)Al(2)H/H(2)C=CHMgBr followed by substrate-directed dihydroxylation of the pendant Allylic Group with OsO(4), reduction of imine, and cyclization with Ph(3)P/CCl(4) gave the polyhydroxylated pyrrolidines 8a and 8b as advanced intermediates. Efficient protecting Group manipulations converted pyrrolidines 8a and 8b to their corresponding partially protected analogues 10a and 10b, which upon Swern oxidation and diastereoselective Keck-type allylation with BF(3).Et(2)O afforded the required three-carbon homologues (10a, >20:1 de; 10b, 3.5:1 de). Use of the chelating Lewis acid MgBr(2) instead of BF(3).Et(2)O with 10a led to a novel aza-pinacol rearrangement and allylation at the alpha-carbon to yield amino alcohol 17, which is similar to a hydride migration in the biosynthetic pathway of indolizidine alkaloids. Subsequent hydroboration, cyclization, and deprotection furnished (-)-8-epi-swainsonine triacetate 15a and (+)-1,2-di-epi-swainsonine 16b in good overall yields (6.3% for 1 --> 15a, 13 steps, and 4.0% for 1 --> 16b, 14 steps).

Koichiro Oshima - One of the best experts on this subject based on the ideXlab platform.

Hossein Razavi - One of the best experts on this subject based on the ideXlab platform.

  • asymmetric syntheses of 8 epi swainsonine triacetate and 1 2 di epi swainsonine carbonyl addition thwarted by an unprecedented aza pinacol rearrangement
    Journal of Organic Chemistry, 2000
    Co-Authors: Hossein Razavi, Robin Polt
    Abstract:

    Indolizidines (-)-8-epi-swainsonine triacetate and (+)-1, 2-di-epi-swainsonine were synthesized from the O'Donnell Schiff base ester 1 derived from D-serine. Reductive-alkenylation of 1 with (i)()Bu(5)Al(2)H/H(2)C=CHMgBr followed by substrate-directed dihydroxylation of the pendant Allylic Group with OsO(4), reduction of imine, and cyclization with Ph(3)P/CCl(4) gave the polyhydroxylated pyrrolidines 8a and 8b as advanced intermediates. Efficient protecting Group manipulations converted pyrrolidines 8a and 8b to their corresponding partially protected analogues 10a and 10b, which upon Swern oxidation and diastereoselective Keck-type allylation with BF(3).Et(2)O afforded the required three-carbon homologues (10a, >20:1 de; 10b, 3.5:1 de). Use of the chelating Lewis acid MgBr(2) instead of BF(3).Et(2)O with 10a led to a novel aza-pinacol rearrangement and allylation at the alpha-carbon to yield amino alcohol 17, which is similar to a hydride migration in the biosynthetic pathway of indolizidine alkaloids. Subsequent hydroboration, cyclization, and deprotection furnished (-)-8-epi-swainsonine triacetate 15a and (+)-1,2-di-epi-swainsonine 16b in good overall yields (6.3% for 1 --> 15a, 13 steps, and 4.0% for 1 --> 16b, 14 steps).

Gareth J Pritchard - One of the best experts on this subject based on the ideXlab platform.

Martin Wills - One of the best experts on this subject based on the ideXlab platform.

  • Palladium-catalyzed Tandem Reactions to Form 1-vinyl-1h-isochromene Derivatives
    Journal of Organic Chemistry, 2001
    Co-Authors: Roger Mutter, Ian B. Campbell, Eva M. Martin De La Nava, And Andy T. Merritt, Martin Wills
    Abstract:

    The palladium-catalyzed reaction of pinacolone with tert-butyldimethyl(3-(2-bromophenyl)allyloxy)silane results in direct formation of 1-vinyl-3-tert-butyl-1H-isochromene. This is the result of a ketone arylation followed by an intramolecular cyclization of the enolate with the Allylic system. The use of a lithium diamide base appears to be essential for success. The tert-butyldimethylsilyl protecting Group is also an essential choice as it furnishes the appropriate reactivity to promote Allylic substitution after the aryl coupling process. The use of more effective leaving Groups, such as acetate, results in reaction of the Allylic Group, and no aryl coupling is observed. Through the appropriate selection of phosphine ligand and solvent, either the cyclized isochromene product or the noncyclized intermediate may be formed selectively. A short combinatorial study of the scope and limitations of the reaction, involving 24 ketones, is described.