Direkt zum Inhalt

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

Artikel

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

DOI zum Zitieren dieses Dokuments: 10.5283/epub.51943


Zusammenfassung

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.



Beteiligte Einrichtungen


Details

DokumentenartArtikel
Titel eines Journals oder einer ZeitschriftACS Catalysis
VerlagAMER CHEMICAL SOC
Ort der VeröffentlichungWASHINGTON
Band12
SeitenbereichS. 3974-3984
Datum15 März 2022
Veröffentlichungsdatum18 Mrz 2022 11:05
InstitutionenChemie und Pharmazie > Institut für Organische Chemie > Lehrstuhl Prof. Dr. Burkhard König
Identifikationsnummer
WertTyp
10.1021/acscatal.2c00662DOI
Stichwörter / 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-Dezimal-Klassifikation500 Naturwissenschaften und Mathematik > 540 Chemie
StatusVeröffentlicht
BegutachtetJa, diese Version wurde begutachtet
An der Universität Regensburg entstandenZum Teil
URN der UB Regensburgurn:nbn:de:bvb:355-epub-519437
Dokumenten-ID51943

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