Nickel(II)/BINOL-catalyzed enantioselective C–H activation via desymmetrization and kinetic resolution
The field of nickel catalysis has witnessed remarkable growth in recent years. However, the use of nickel catalysts in enantioselective C-H activation remains a daunting challenge because of their variable oxidation states, intricate coordination chemistry, and unpredictable reactivity patterns. Herein, we report an enantioselective C-H activation reaction catalyzed by commercially available and air-stable nickel(II) catalyst. Readily available and simple (S)-BINOL is used as a chiral ligand. This operationally simple protocol enables the synthesis of planar chiral metallocenes in high yields with excellent enantioselectivity through desymmetrization and kinetic resolution. Air-stable planar chiral nickelacycle intermediates are first synthesized via enantioselective C-H nickelation and shown to be possible intermediates of the reaction. Deuterium-labeling studies, alongside the characterization and transformation of chiral nickel(II) species, suggest that C-H cleavage is the enantio-determining step. Moreover, the large-scale synthesis and diverse synthetic transformations underscore the practicality of this protocol.
Authors
- Fan‐Rui Huang
- Qi‐Jun Yao (ORCID: https://orcid.org/0000-0002-2872-7688)
- Bing‐Feng Shi (ORCID: https://orcid.org/0000-0003-0375-955X)
- Jiahao Chen (ORCID: https://orcid.org/0000-0002-4581-1152)
Institutions
- Zhejiang Lab (CN)
- Zhejiang University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-08-20
- DOI
- https://doi.org/10.1038/s41467-024-51409-3
- Citations
- 18
- Primary Topic
- Catalytic C–H Functionalization Methods
- Type
- article
- Field-Weighted Citation Impact
- 4.50
Funders
- National Natural Science Foundation of China
- Zhejiang University
- Fundamental Research Funds for the Central Universities
- Natural Science Foundation of Zhejiang Province