Pergamon Tetrahedron Letters 41 (2000) 747–749
TETRAHEDRON
LETTERS
Phosphazene bases and the anionic oxy-Cope rearrangement
Hassan T. Mamdani and Richard C. Hartley
*
Department of Chemistry, University of Glasgow, Glasgow, G12 8QQ, UK
Received 18 October 1999; accepted 10 November 1999
Abstract
Compounds containing a 1,5-hexadien-3-ol system undergo anionic oxy-Cope rearrangement when treated with
the phosphazene super-base, P
4
-t-Bu. The [3,3] sigmatropic rearrangement occurs in hexane as well as in THF. The
weaker phosphazene base, P
2
-Et fails to induce rearrangement. This is the first example of the use of a metal-free
base to induce anionic oxy-Cope rearrangement. © 2000 Elsevier Science Ltd. All rights reserved.
Keywords: phosphazenes; rearrangements; alcohols; ketones.
The anionic oxy-Cope (AOC) rearrangement
1
is the [3,3] sigmatropic rearrangement of an alkoxide
1 generated from a 1,5-dien-3-ol 2 to give an enolate 3 (Scheme 1). The alkoxide 1 rearranges 10
10
to 10
17
times faster than alcohol 2 due to weakening of the C(3)–C(4) bond in the ground state by n-
donation from the oxyanion. The n-donation is greatest and the rearrangement fastest when the oxyanion
is completely naked; consequently, potassium salts rearrange faster than sodium salts, which rearrange
faster than lithium salts.
2
Crown ethers and polar aprotic solvents are often used to reduce association
between the oxyanion and the cation. However, metal-free bases have never been used for this reaction.
Scheme 1.
The phosphazene super-bases 4 and 5,
3
developed by Reinhard Schwesinger, are extremely strong,
uncharged, metal-free bases (Fig. 1). We here report that P
4
-t-Bu 4 completely deprotonates alcohol 2 to
give alkoxide 1 and a huge ‘soft’ cation, which is known
3
to have its positive charge delocalised over a
volume of ca. 500 Å
3
, and that this alkoxide is sufficiently naked to undergo AOC rearrangement.
*
Corresponding author.
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