Photocatalytic Oxyalkynylation of Unactivated Alkenes Enabled by Hypervalent Iodine(III) Reagents
The oxyalkynylation of alkenes offers a valuable strategy for constructing C–C and C–O bonds, generating β-alkynyl alcohols frequently found in bioactive molecules. This work presents a photocatalytic approach for the oxyalkynylation of readily available unactivated alkenes using hypervalent iodine(III) reagents, acetoxylbenziodoxole (BI-OAc) and alkynylbenziodoxole (BI-alkyne), to afford anti-Markovnikov β-alkynyl alcohols. Mechanistic studies reveal a unique energy transfer process between BI-OAc and the photocatalyst, leading to the efficient generation of aryl carboxyl radicals. The aryl carboxyl radicals initiate atom-economical addition reactions with a broad range of commercially available mono-, di-, and trisubstituted alkenes, achieving anti-Markovnikov regioselectivity with BI-alkynes. The reaction can be readily scaled up to the gram scale, demonstrating its potential for late-stage modification of natural products and drug molecules. This method represents a significant advance in leveraging hypervalent iodine(III) reagents for radical generation and opens exciting avenues for future reaction design and development.
Authors
- Yiyun Chen (ORCID: https://orcid.org/0000-0003-0916-0994)
- Hanzhang Qin (ORCID: https://orcid.org/0000-0002-2787-0685)
- Yixin Zhang (ORCID: https://orcid.org/0000-0002-0927-6981)
- Zhengyi Liu (ORCID: https://orcid.org/0009-0007-5313-4159)
Institutions
- ShanghaiTech University (CN)
- Shanghai Institute of Organic Chemistry (CN)
- University of Chinese Academy of Sciences (CN)
Publication Details
- Journal
- ACS Catalysis
- Published
- 2024-08-19
- DOI
- https://doi.org/10.1021/acscatal.4c02977
- Citations
- 8
- Primary Topic
- Oxidative Organic Chemistry Reactions
- Type
- article
- Field-Weighted Citation Impact
- 2.00
Funders
- National Natural Science Foundation of China
- Chinese Academy of Sciences
- Youth Innovation Promotion Association of the Chinese Academy of Sciences
- Program of Shanghai Academic Research Leader