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Ring Expansion Strategy on the Synthesis of 7-Membered Hetercycles from Azolidinone and haloaryl Ethers
Thesis

Ring Expansion Strategy on the Synthesis of 7-Membered Hetercycles from Azolidinone and haloaryl Ethers

Shu-Yu Lin
Masters, 國立清華大學, 化學系
2004

Abstract

雜環環化反應 鹵素烷基芳香醚 四氫化1,4苯二氮平酮 benzodiazepinone imidazolidinone benzyne sodium bis(trimethylsilyl)amide hetercycles
Tetrahydro-1,4-benzodiazepin-5-ones with an alkoxy group at the C-6 position were synthesized in 76–82% yields from alkyl haloaryl ethers and 1.3-dimethyl-2-imidazolidinone in the presence of sodium bis(trimethylsilyl)amide at reflux. A bigger alkyl group in haloaryl ethers gave a lower yields of the correspondng benzodiazepinone. The same annellation was also accomplished by use of the t-butyldimethylsilyl haloaryl ether to replace an alkyl haloaryl ether. Nevertheless, partial desilylation took place to lead to the desired benzodiazepinone bearing an –OH group. Although the heterocycle fromation was accomplished by use of 1,3-dimethyl-2-imidazolidinone as the starting materials, its replacement with 3-methyl-2-oxazolidinone, 3-methyl-2-thiazolidinone, or 1-methyl-2-pyrrolidinone did not give the corresponding 7-membered heterocycles. Furthermore, ours results indicate that reaction of meta-iodoanisole with 3-methyl-2-oxazolidinone generated 1-(3-methoxyphenyl)-3-methyl-2-imidazolidinone in 25% yield, of which the structure was confirm by X-ray crystallography. Among various bases including lithium 2,2,6,6-tetramethylpiperidide, sodium bis(trimethylsilyl)amide, sodium tert-butoxide, and sodium hydride, choice of sodium bis(trimethylsilyl)amide was essential for the "one-flask" annellation to proceed.

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