Published June 26, 2010 | Version Supplemental Material + Accepted Version
Journal Article Open

A general enantioselective route to the chamigrene natural product family

Abstract

Described in this report is an enantioselective route toward the chamigrene natural product family. The key disconnections in our synthetic approach include sequential enantioselective decarboxylative allylation and ring-closing olefin metathesis to form the all-carbon quaternary stereocenter and spirocyclic core present in all members of this class of compounds. The generality of this strategy is demonstrated by the first total syntheses of elatol and the proposed structure of laurencenone B, as well as the first enantioselective total syntheses of laurencenone C and α-chamigrene. A brief exploration of the substrate scope of the enantioselective decarboxylative allylation/ring-closing metathesis sequence with fully substituted vinyl chlorides is also presented.

Additional Information

© 2010 Elsevier. Received 15 April 2010; revised 28 April 2010; accepted 29 April 2010. Available online 4 May 2010. This publication is based on work supported by Award No. KUS-11-006-02, made by King Abdullah University of Science and Technology (KAUST). Additionally, the authors wish to thank the NIH-NIGMS (R01 GM080269-01, postdoctoral fellowships to D.E.W. and I.C.S.), Abbott, Amgen, Bristol-Myers Squibb, Merck, and Caltech for generous funding; Materia, Inc. for their kind donation of catalyst 49 used in these studies; Professors Mercedes Cueto and Karen L. Erickson for their kind donation of natural samples of elatol (1); Professor Adusumilli Srikrishna for copies of 1H and 13C NMR spectra of synthetic (±)-laurencenone C ((±)-8) and (±)-α-chamigrene ((±)-5); and Professor Peter B. Dervan and David M. Chenoweth for use of their HPLC. Finally, B.M.S. thanks all of his current and former co-workers and colleagues who have made working at Caltech over the past 10 years such an enjoyable experience. As evidenced by the collaborative nature of this project, the spectacular environment at Caltech is one-of-a-kind and second-to-none.

Attached Files

Accepted Version - nihms-203918.pdf

Supplemental Material - f.pdf

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Additional details

Identifiers

PMCID
PMC2925317
Eprint ID
19000
DOI
10.1016/j.tet.2010.04.128
Resolver ID
CaltechAUTHORS:20100712-150605717

Related works

Funding

King Abdullah University of Science and Technology (KAUST)
KUS-11-006-02
NIH
R01GM080269-01
Abbott
Amgen
Bristol-Myers Squibb
Merck
Caltech

Dates

Created
2010-07-14
Created from EPrint's datestamp field
Updated
2021-11-08
Created from EPrint's last_modified field