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Rhodium‐Catalyzed Asymmetric Transfer Hydrogenation of Heterocyclic Diaryl Ketones: Facile Access to Key Intermediate of Baloxavir<sup>†</sup>

Li Wang, Renwei Xiao, Jingyuan Song, Long‐Sheng Zheng, Qiwei Lang, Gen‐Qiang Chen, Xumu Zhang

2023Chinese Journal of Chemistry15 citationsDOIOpen Access PDF

Abstract

Comprehensive Summary Transition metal‐catalyzed asymmetric transfer hydrogenation has been proven to be a powerful approach for the synthesis of chiral alcohols. Herein, a highly efficient and enantioselective transfer hydrogenation of dibenzoheptaheterocyclic ketones catalyzed by an arene‐tethered TsDPEN‐based Rh(III) catalyst has been successfully developed, and a variety of dibenzoheptaheterocyclic ketones were reduced by a 1/1 mixture of formic acid and DBU (1,8‐diazabicyclo[5.4.0]undec‐7‐ene) with high yields and enantioselectivities. With this method, the asymmetric reduction of 7,8‐difluorodibenzo[ b , e ]thiepin‐11(6 H )‐one has been realized, providing the key intermediate of baloxavir marboxil with &gt;99% yield and &gt;99% ee at a substrate/catalyst molar ratio of 1000.

Topics & Concepts

ChemistryTransfer hydrogenationCatalysisEnantioselective synthesisRhodiumYield (engineering)Formic acidNoyori asymmetric hydrogenationAsymmetric hydrogenationCombinatorial chemistryTransition metalMolar ratioOrganic chemistryMedicinal chemistryRutheniumMaterials scienceMetallurgyAsymmetric Hydrogenation and CatalysisCarbon dioxide utilization in catalysisSurface Chemistry and Catalysis
Rhodium‐Catalyzed Asymmetric Transfer Hydrogenation of Heterocyclic Diaryl Ketones: Facile Access to Key Intermediate of Baloxavir<sup>†</sup> | Litcius