Asymmetric Photoaerobic Lactonization and Aza-Wacker Cyclization of Alkenes Enabled by Ternary Selenium-Sulfur Multicatalysis.
Tao LeiSebastian GrafChristopher SchöllFelix KrätzschmarBernhard GregoriTheresa ApplesonAlexander BrederPublished in: ACS catalysis (2023)
An adaptable, sulfur-accelerated photoaerobic selenium-π-acid ternary catalyst system for the enantioselective allylic redox functionalization of simple, nondirecting alkenes is reported. In contrast to related photoredox catalytic methods, which largely depend on olefinic substrates with heteroatomic directing groups to unfold high degrees of stereoinduction, the current protocol relies on chiral, spirocyclic selenium-π-acids that covalently bind to the alkene moiety. The performance of this ternary catalytic method is demonstrated in the asymmetric, photoaerobic lactonization and cycloamination of enoic acids and unsaturated sulfonamides, respectively, leading to an averaged enantiomeric ratio (er) of 92:8. Notably, this protocol provides for the first time an asymmetric, catalytic entryway to pharmaceutically relevant 3-pyrroline motifs, which was used as a platform to access a 3,4-dihydroxyproline derivative in only seven steps with a 92:8 er.
Keyphrases
- visible light
- reduced graphene oxide
- randomized controlled trial
- solid state
- crystal structure
- estrogen receptor
- ionic liquid
- endoplasmic reticulum
- capillary electrophoresis
- breast cancer cells
- magnetic resonance
- gold nanoparticles
- room temperature
- high throughput
- magnetic resonance imaging
- mass spectrometry
- highly efficient
- computed tomography
- carbon dioxide
- metal organic framework
- tandem mass spectrometry