Literature DB >> 34881491

A Mechanistically Inspired Halenium Ion Initiated Spiroketalization: Entry to Mono- and Dibromospiroketals.

Kumar Dilip Ashtekar1, Hadi Gholami2, Mehdi Moemeni2, Ankush Chakraborty2, Lindsey Kiiskila2, Xinliang Ding2, Edmond Toma2, Christopher Rahn2, Babak Borhan2.   

Abstract

Employing halenium affinity (HalA) as a guiding tool, the weak nucleophilic character of alkyl ketones was modulated by the templating effect of a tethered 2-tetrahydropyranyl(THP)-protected alcohol towards realizing a bromenium ion initiated spiroketalization cascade. Addition of ethanol aided an early termination of the cascade by scavenging the THP group after the halofunctionalization stage, furnishing monobromospiroketals. Alternatively, exclusion of ethanol from the reaction mixture biased the transient oxocarbenium towards α-deprotonation that precedes a second bromofunctionalization event thus, furnishing dibrominated spiroketals. The regio- and stereoselectivity exploited in the current methodology provides a novel and rapid access to the dibrominated spiroketal motifs exhibited by several natural products.
© 2021 Wiley-VCH GmbH.

Entities:  

Keywords:  Halenium affinity; Halocyclization; Reaction mechanisms; Spiroketalization

Mesh:

Substances:

Year:  2022        PMID: 34881491      PMCID: PMC9254888          DOI: 10.1002/anie.202115173

Source DB:  PubMed          Journal:  Angew Chem Int Ed Engl        ISSN: 1433-7851            Impact factor:   16.823


  31 in total

1.  Asymmetric total synthesis of (-)-isolaurallene.

Authors:  M T Crimmins; K A Emmitte
Journal:  J Am Chem Soc       Date:  2001-02-21       Impact factor: 15.419

2.  Diastereoselective synthesis of the C(17)-C(28) fragment (the C-D spiroketal unit) of spongistatin 1 (altohyrtin A) via a kinetically controlled iodo-spiroketalization reaction.

Authors:  Edward B Holson; William R Roush
Journal:  Org Lett       Date:  2002-10-17       Impact factor: 6.005

3.  Theoretical and experimental studies on the Baeyer-Villiger oxidation of ketones and the effect of alpha-halo substituents.

Authors:  Friedrich Grein; Austin C Chen; David Edwards; Cathleen M Crudden
Journal:  J Org Chem       Date:  2006-02-03       Impact factor: 4.354

4.  Enantio- and Diastereoselective Spiroketalization Catalyzed by Chiral Iridium Complex.

Authors:  James Y Hamilton; Simon L Rössler; Erick M Carreira
Journal:  J Am Chem Soc       Date:  2017-06-09       Impact factor: 15.419

5.  Asymmetric spiroacetalization catalysed by confined Brønsted acids.

Authors:  Ilija Čorić; Benjamin List
Journal:  Nature       Date:  2012-03-14       Impact factor: 49.962

6.  Laurene-type sesquiterpenes from the Red Sea red alga Laurencia obtusa as potential antitumor-antimicrobial agents.

Authors:  Walied M Alarif; Sultan S Al-Lihaibi; Seif-Eldin N Ayyad; Mohamed H Abdel-Rhman; Farid A Badria
Journal:  Eur J Med Chem       Date:  2012-07-07       Impact factor: 6.514

7.  Halogenated metabolites from Japanese Laurencia spp.

Authors:  Minoru Suzuki; Tomotake Kawamoto; Charles Santhanaraju Vairappan; Takahiro Ishii; Tsuyoshi Abe; Michio Masuda
Journal:  Phytochemistry       Date:  2005-09-23       Impact factor: 4.072

8.  Development and mechanism of an enantioselective bromocycloetherification reaction via Lewis base/chiral Brønsted acid cooperative catalysis.

Authors:  Scott E Denmark; Matthew T Burk
Journal:  Chirality       Date:  2013-11-07       Impact factor: 2.437

9.  Recent advances in stereoselective bromofunctionalization of alkenes using N-bromoamide reagents.

Authors:  Chong Kiat Tan; Ying-Yeung Yeung
Journal:  Chem Commun (Camb)       Date:  2013-08-01       Impact factor: 6.222

10.  A new tool to guide halofunctionalization reactions: the halenium affinity (HalA) scale.

Authors:  Kumar Dilip Ashtekar; Nastaran Salehi Marzijarani; Arvind Jaganathan; Daniel Holmes; James E Jackson; Babak Borhan
Journal:  J Am Chem Soc       Date:  2014-09-11       Impact factor: 15.419

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