Pergamon Tetrahedron: Asymmetry 10 (1999) 193–206
TETRAHEDRON:
ASYMMETRY
Studies towards the total synthesis of taxoids: a rapid entry into
bicyclo[6.4.0]dodecane ring system. Part 2
Siméon Arseniyadis,
*
Maria del Rosario Rico Ferreira, José Quilez del Moral,
José Ignacio Martin Hernando, Nicolas Birlirakis and Pierre Potier
Institut de Chimie des Substances Naturelles, CNRS, F-91198 Gif-sur-Yvette, France
Received 13 November 1998; accepted 9 December 1998
Abstract
We report a synthetic route that allows access into A-seco taxoid frameworks embodying the entire carbon
skeleton and a large number of oxygen functionalities. The BC-subunit (-)-4 was constructed in five steps from
(+)-3, through a step-efficient and stereocontrolled bond construction. © 1999 Elsevier Science Ltd. All rights
reserved.
1. Introduction
Recently, we have published a synthetic approach of the taxoid BC-subunit, which served the dual
purpose of elucidating the stereochemistry of our aldol–annelation–fragmentation methodology and pro-
viding adequate material for further transformations.
1
We thus described the development of a synthetic
strategy for advanced taxoid substructures such as (+)-3, establishing the feasibility of incorporating all
of the 20 carbons and of essential oxygen functionalities of the taxoid
2
diterpene skeleton I in 12 steps
starting from two achiral aldol partners 1 and 2. With the efficient synthesis of the bicyclo[6.4.0]dodecane
ring system (+)-3 realized, the stage was now set for the completion of the synthesis. So, we went on to
prepare the more advanced intermediates represented by formulas II, III and IV, precursors of taxoid
ABC-tricyclic core of type I, which incorporate ring A in its seco form. An elementary retrosynthetic
analysis (Scheme 1; P stands for ketal protection) of I would suggest two routes to achieve C11–C12
bond formation: samarium iodide
3
induced reductive coupling for precursors of types II and III, and
either samarium iodide coupling or aldol chemistry for precursor IV. Key questions at this stage include
the likelihood of obtaining chemoselectivity in epoxide-ring opening and the nature of functional group
interconversion to be chosen en route towards one of the targeted A-seco taxoid frameworks of type II,
III or IV for final ring closing (C11–C12).
*
Corresponding author. Fax: +33 169-077-247; e-mail: simeon.arseniyadis@icsn.cnrs-gif.fr
0957-4166/99/$ - see front matter © 1999 Elsevier Science Ltd. All rights reserved.
PII: S0957-4166(98)00491-1