CO2-promoted photocatalytic aryl migration from nitrogen to carbon for switchable transformation of N-arylpropiolamides
Photocatalytic N-to-C aryl migration allows for quick construction of highly useful amide derivatives from readily available compounds. By developing the reactions of sodium sulfinates with the N-aryl-propiolamides, we herein demonstrate that the CO<sub>2</sub>-promoted visible-light-induced method enables a large variety of aryl groups on nitrogen atoms of the N-arylamides to undergo efficient aryl migration from N atom to C atom to synthesize tetra- and tri-substituted alkenyl amides selectively. 1,4-N-to-C aryl migration is a key step in this transformation which is achieved through photocatalytic radical-polar crossover pathway. The protocol exhibits the remarkably tolerant of the electronic properties of the migrating aryl substituent, as both electron-rich and -poor arenes are compatible with the migration process. As a result, this protocol features with a broad substrate scope, as demonstrated by more than 90 examples including complex bioactive compounds. Notably, abundant, nontoxic and low-cost CO<sub>2</sub> acted as an essential and irreplaceable additive to enable the tetra- and tri-substituted alkenyl amides to be synthesized with excellent selectivity.
Authors
- Fanyuanhang Yang
- Yuzhen Gao (ORCID: https://orcid.org/0000-0002-2690-7407)
- Weiping Su (ORCID: https://orcid.org/0000-0001-5695-6333)
- Denghui Ma
- Ge Liu (ORCID: https://orcid.org/0000-0003-1469-0690)
- Jianchen Zhang
Institutions
- Ningbo University of Technology (CN)
- Chinese Academy of Sciences (CN)
- Fujian Institute of Research on the Structure of Matter (CN)
- Tan Kah Kee Innovation Laboratory (CN)
- University of Chinese Academy of Sciences (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-11-22
- DOI
- https://doi.org/10.1038/s41467-024-54239-5
- Citations
- 17
- Primary Topic
- Sulfur-Based Synthesis Techniques
- Type
- article
- Field-Weighted Citation Impact
- 4.25
Funders
- National Natural Science Foundation of China
- National Key Research and Development Program of China