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Directed metalation of N,N-diethylbenzamides. Silylated benzamides for the synthesis of naturally occurring peri-methylanthraquinones and peri-methyl polycyclic aromatic hydrocarbons

Journal Article · · Journal of Organic Chemistry; (USA)
DOI:https://doi.org/10.1021/jo00279a029· OSTI ID:7071002
;  [1]
  1. Univ. of Waterloo, Ontario (Canada)

Efficient methodologies based on directed ortho metalation, fluoride-induced carbodesilylation, and metal-halogen exchange processes (Scheme I) are reported for the synthesis of peri-methyl-substituted anthraquinone natural products 5 and polycyclic aromatic hydrocarbons 6, 7. Benzamide 8 (Scheme II) is converted in a one-pot sequence into the disilylated derivative 10, which upon metalation, condensation with 3,5-dimethoxybenzaldehyde, CsF desilylation, and TsOH cyclization leads to the key phthalide 11. Compound 11 is transformed into deoxyerythrolaccin tris(methyl ether) 5c, which has been previously converted into the natural product 5a. For the synthesis of erythrolaccin tetrakis(methyl ether) 5d, the silyl and bromo benzamides 14 and 15 (Scheme III) are condensed with 3,5-dimethoxybenzaldehyde by CsF-induced carbodesilylation and metal-halogen exchange expedients, respectively, to give the phthalide 16, which is transformed into the target anthraquinone 55d by methods identical with those used in 5c. Along similar lines, the synthesis of 11-methyl-7,12-benz(a)anthraquinone (6a, Scheme IV), 8-methyl-7,12-benz(a)anthraquinone (6b), and 10-methyl-9,14-dibenz(a,c)anthraquinone (7) is described.

OSTI ID:
7071002
Journal Information:
Journal of Organic Chemistry; (USA), Journal Name: Journal of Organic Chemistry; (USA) Vol. 54:18; ISSN 0022-3263; ISSN JOCEA
Country of Publication:
United States
Language:
English