A Photochemical Strategy towards Michael Addition Reactions of Cyclopropenes
The development of Michael addition reactions to conjugated cyclopropenes is a challenge in organic synthesis due to the fleeting and reactive nature of such strained Michael acceptor systems. Herein, the development of a photochemical approach towards such conjugated cyclopropenes is reported that serves as a strategic entry point to densely functionalized cyclopropanes in a diastereoselective fashion. The process involves the light-mediated generation of transient cyclopropenyl α,β-unsaturated esters from vinyl diazo esters, followed by an organic base catalyzed nucleophilic addition of N-heterocycles to directly access β-N-heterocyclic cyclopropanoic esters. With this synergistic approach, various trisubstituted cyclopropanes bearing N-heteroaryl and N-heterocyclic rings such as indole, pyrrole, benzimidazole, isatin, pyridinone, and quinolinone were accessed efficiently in good yield and decent to good diastereoselectivities. Further, β-indolyl cyclopropanoic acids have been synthesized and were successfully evaluated as FABP-4 inhibitors. Theoretical calculations have been performed to elucidate the mechanism, which was further supported by experimental findings.
Authors
- Ewgenij Proschak (ORCID: https://orcid.org/0000-0003-1961-1859)
- Pankaj Chauhan (ORCID: https://orcid.org/0000-0002-8779-0652)
- René M. Koenigs (ORCID: https://orcid.org/0000-0003-0247-4384)
- Yaseen Hussain (ORCID: https://orcid.org/0000-0001-7370-1084)
- Deepak Sharma (ORCID: https://orcid.org/0000-0003-4832-4672)
- Claire Empel (ORCID: https://orcid.org/0000-0002-9362-7755)
- Astrid Kaiser
- Wenyong Zhu (ORCID: https://orcid.org/0000-0003-3907-5782)
- R. Prasanna
- Lilia Weizel (ORCID: https://orcid.org/0000-0002-0373-2114)
- Lennard Kloene (ORCID: https://orcid.org/0000-0002-9587-9219)
Institutions
- Goethe University Frankfurt (DE)
- Fraunhofer Institute for Translational Medicine and Pharmacology (DE)
- Indian Institute of Technology Jammu (IN)
- RWTH Aachen University (DE)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2024-11-07
- DOI
- https://doi.org/10.1002/anie.202416956
- Citations
- 9
- Primary Topic
- Cyclopropane Reaction Mechanisms
- Type
- article
- Field-Weighted Citation Impact
- 2.25