The synthesis and structures of arylpyran pseudoacyl derivatives

CHED 508

William D. Robinson, billrobinson78@gmail.com and Edward J. Valente, valente@mc.edu. Department of Chemistry & Biochemistry, Mississippi College, Clinton, MS 39058
Beginning with the dehydration resistant aryl pyran pseudoacid, 4,4-dimethyl-3-hydroxydihydroisobenzopyran-1-one, we have synthesized and determined the structures of several pseudoacyl derivatives. These include the pseudoacyl halide, pseudoesters, pseudoamides with exocyclic and endocyclic nitrogens, and pseudoacyl anhydrides. This series contains a range of exocyclic substituents which are compared and contrasted with the endocyclic pseudoacyl system, which produces considerable variation in the endocyclic C-O bond lengths. At the extremes are the pseudoacyl chloride, 4,4-dimethyl-3-chlorodihydroisobenzopyran-1-one and the tertiaryl pseudoamide, 4,4-dimethyl-3-morpholinodihydroisobenzopyran-1-one. The pseudoacyl chloride crystallizes in the monoclinic system, space group P2(1)/n, with a = 7.8896(2)Å, b = 12.1750(3)Å, c = 10.7140(3)Å, beta = 99.477(3)o, V = 1015.10(9)Å3, and has C-O distance 1.411(2)Å. The tertiaryl pseudoamide crystallizes in the monoclinic system, space group P2(1)/c, with a = 6.2351(4)Å, b = 14.6502(10)Å, c = 15.2232(10)Å, beta = 96.215(6)o, V = 1382.39(16)Å3, and has C-O distance 1.474(2)Å. Consistent with this trend are the locations of the pseudoacyl H resonances, which shifts from 6.1 in the chloride to 4.8 in the amide. This study represents a detailed systematic examination of an arylpyranoid pseudoacyl structures. We acknowledge the support of NSF grant MRI 0618148 and the W. M. Keck Foundation for crystallographic resources.