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Murugesan, Kathiravan ; Donabauer, Karsten ; Narobe, Rok ; Derdau, Volker ; Bauer, Armin ; König, Burkhard

Photoredox-Catalyzed Site-Selective Generation of Carbanions from C(sp3)–H Bonds in Amines

Murugesan, Kathiravan, Donabauer, Karsten, Narobe, Rok , Derdau, Volker, Bauer, Armin and König, Burkhard (2022) Photoredox-Catalyzed Site-Selective Generation of Carbanions from C(sp3)–H Bonds in Amines. ACS Catalysis 12, pp. 3974-3984.

Date of publication of this fulltext: 18 Mar 2022 11:05
Article
DOI to cite this document: 10.5283/epub.51943


Abstract

The selective activation of sp3 carbon-hydrogen bonds in the presence of multiple C-H bonds is challenging and remains of supreme importance in chemical research. Late-stage modification of complex molecules via sp3 C-H activation is of high prevalence in organic synthesis. Herein, we describe the activation of a C(sp3 )-H bond in the alpha-position to an amine via a carbanion intermediate. In ...

The selective activation of sp3 carbon-hydrogen bonds in the presence of multiple C-H bonds is challenging and remains of supreme importance in chemical research. Late-stage modification of complex molecules via sp3 C-H activation is of high prevalence in organic synthesis. Herein, we describe the activation of a C(sp3 )-H bond in the alpha-position to an amine via a carbanion intermediate. In the presence of several alpha-amine sites, only one specific position is selectively activated. Applying this protocol, the proposed carbanion intermediate was effectively trapped with different electrophiles such as deuterium (D+ ), tritium (T+ ), or carbonyl compounds compiling over 50 examples. Further, this methodology was used to install deuterium or tritium in different drug-derivatives (>10 drugs) at a selected position in a late-stage functionalization. In addition, the protocol is suitable for a gram-scale synthesis, and a detailed mechanistic investigation has been carried out to support our hypothesis.



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Details

Item typeArticle
Journal or Publication TitleACS Catalysis
Publisher:AMER CHEMICAL SOC
Place of Publication:WASHINGTON
Volume:12
Page Range:pp. 3974-3984
Date15 March 2022
InstitutionsChemistry and Pharmacy > Institut für Organische Chemie > Lehrstuhl Prof. Dr. Burkhard König
Identification Number
ValueType
10.1021/acscatal.2c00662DOI
KeywordsC-H; C(SP(3))-H BONDS; ATOM TRANSFER; FUNCTIONALIZATION; DEUTERATION; ALDEHYDES; EQUIVALENTS; ALLYLATION; TRITIATION; ALCOHOLS; photoredox catalysis; carbanion; site-selectivity; isotope labeling; amino alcohols; C-H functionalization
Dewey Decimal Classification500 Science > 540 Chemistry & allied sciences
StatusPublished
RefereedYes, this version has been refereed
Created at the University of RegensburgPartially
URN of the UB Regensburgurn:nbn:de:bvb:355-epub-519437
Item ID51943

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