Enantioselective Access to Chiral γ-Ketoamides via Photoredox Catalyzed Carbamoyl Radical Addition/Asymmetric Protonation
Herein, we report a method for the enantioselective synthesis of β-chiral amides through photoredox-catalyzed carbamoyl radical addition to α,β-unsaturated ketones, followed by enantioselective protonation. The combination of photoredox catalysis with chiral Brønsted acid catalysis enables the generation of carbamoyl radicals under mild conditions and achieves stereocontrol in the protonation step. This dual catalytic system offers a direct and efficient approach to access synthetically valuable β-chiral γ-ketoamides, delivering products with high enantioselectivities and broad functional group tolerance. Mechanistic investigations support a sequential process involving photoinduced radical conjugate addition, single-electron reduction, and enantioselective protonation. This strategy expands the utility of carbamoyl radicals in asymmetric synthesis and contributes to the development of radical-based enantioselective methodologies.
Authors
- Guo‐Qiang Xu (ORCID: https://orcid.org/0000-0002-9683-4581)
- Xu Ha (ORCID: https://orcid.org/0000-0002-7502-6294)
- Wentao Hou (ORCID: https://orcid.org/0000-0002-0464-6381)
- Peng Zhang (ORCID: https://orcid.org/0000-0003-0606-6855)
- Hongyu Li (ORCID: https://orcid.org/0000-0001-5521-8005)
- Xueying Chen (ORCID: https://orcid.org/0000-0002-3015-791X)
- Jihua Zhang
Institutions
- Resonance Research (United States) (US)
- State Key Laboratory of Applied Organic Chemistry
- Lanzhou University (CN)
Publication Details
- Journal
- ACS Catalysis
- Published
- 2025-06-06
- DOI
- https://doi.org/10.1021/acscatal.4c07743
- Citations
- 3
- Primary Topic
- Radical Photochemical Reactions
- Type
- article
- Field-Weighted Citation Impact
- 2.81
Funders
- National Natural Science Foundation of China
- Natural Science Foundation of Gansu Province
- Higher Education Discipline Innovation Project
- Fundamental Research Funds for the Central Universities