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The Formation of Cyclic Ethers by Intramolecular Addition and Substitution Processes in the Reaction of Olefinic Alcohols with Lead Tetraacetate. Part I. Preliminary communication

✍ Scribed by Mihailo Lj. Mihailović; Živorad Čeković; Jezdimir Stanković; Nebojša Pavlović; Stanimir Konstantinović; Silvija Djokić-Mazinjanin


Publisher
John Wiley and Sons
Year
1973
Tongue
German
Weight
261 KB
Volume
56
Category
Article
ISSN
0018-019X

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✦ Synopsis


The lead tetraacetate (LTA) oxidation of saturated alcohols in non-polar solvents affords usually as major products unsubstituted tetrahydrofuran-type ethers, the formation of which involves intramolecular 1,5-hydrogen abstraction by the initially produced alkoxy radicals, followed by internal attack of the hydroxylic oxygen on the electron-deficient &carbon atom [Z]. On the other hand, when treated with LTA in benzene, unsaturated alcohols containing a spatially accessible A4or A5-olefinic linkage undergo intramolecular addition of the hydroxylic oxygen to the double bond, resulting in the formation of acetoxylated or unsaturated five-membered cyclic ethers (from A4-alkenols) and six-membered cyclic ethers (from A4and d5-alkenols)

The mechanistic course of this internal cyclization is not as yet quite clear; several possibilities have been envisaged, such as initial attack of LTA on the hydroxyl group or on the ethylenic grouping, followed by a free-radical or ionic reaction sequence, or a successive combination of homolytic and heterolytic steps [2-41 3).

In this paper we present results of the LTA oxidation of some simple, conformationally mobile unsaturated open-chain alcohols containing an unsubstituted terminal A3-, A4-, A5-, d6-andA7-double bond. Products and yields of these reactions are summarized in the Scheme *).

The following comments about the results obtained can be made.

  1. The absence of cyclic ethers among the reaction products indicates that in A3alkenols, such as 1-octen-4-01 ( l ) , the hydroxyl oxygen does not undergo intramolecular addition to the double bond or intramolecular substitution at the saturated &carbon 1) z j

3)

Commun. 29 on 'Reactions with lead tetraacctate'. For paper 28 see [l].