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.

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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

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article

Photocatalytic Oxyalkynylation of Unactivated Alkenes Enabled by Hypervalent Iodine(III) Reagents

Yiyun Chen, Hanzhang Qin, Yixin Zhang, Zhengyi Liu
8 citations
ACS Catalysis
Oxidative Organic Chemistry Reactions
2.00
article

Photocatalytic Oxyalkynylation of Unactivated Alkenes Enabled by Hypervalent Iodine(III) Reagents

Yiyun Chen, Hanzhang Qin, Yixin Zhang, Zhengyi Liu
article en
8 citations

Abstract

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.

ACS CatalysisVol. 14(17)
ShanghaiTech University (CN), Shanghai Institute of Organic Chemistry (CN), University of Chinese Academy of Sciences (CN)
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
Clean water and sanitation
Openalex Percentile: Top 14%
Oxidative Organic Chemistry Reactions
2.00
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