Controlling Selectivity in Shuttle Hetero-difunctionalization Reactions: Electrochemical Transfer Halo-thiolation of Alkynes


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Date

2023-01-09

Publication Type

Journal Article

ETH Bibliography

yes

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Abstract

Shuttle hetero-difunctionalization reaction, in which two chemically distinct functional groups are transferred between two molecules, has long been an unmet goal due to the daunting challenges in controlling the chemo-, regio-, and stereoselectivity. Herein, we disclose an electrochemistry enabled shuttle reaction (e-shuttle) to selectively transfer one RS− and one X− group between β-halosulfides and unsaturated hydrocarbons via a consecutive paired electrolysis mechanism. The preferential anodic oxidation of one anion over the other, which is controlled by their distinct redox potentials, plays pivotal role in controlling the high chemoselectivity of the process. This easily scalable methodology enables the construction of a myriad of densely functionalized β-halo alkenyl sulfides in unprecedented chemo-, regio-, and stereoselectivity using benign surrogates, e.g., 2-bromoethyl sulfide, avoiding the handling of corrosive and oxidative RS–Br reagents. In a broader context, these results open up new strategies for selective shuttle difunctionalization reactions.

Publication status

published

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Book title

Volume

62 (2)

Pages / Article No.

Publisher

Wiley-VCH

Event

Edition / version

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Software

Geographic location

Date collected

Date created

Subject

Bromothiolation; Hetero-Difunctionalization; Paired Electrolysis; Reversible Reactions; Shuttle Catalysis

Organisational unit

09634 - Morandi, Bill / Morandi, Bill check_circle

Notes

Funding

757608 - Shuttle Catalysis for Reversible Molecular Construction (EC)
886102 - Elemental Halogen-Free Reversible Construction and Deconstruction of 1,2- Dihalides via Shuttle Catalysis (EC)

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