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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 und König, Burkhard (2022) Photoredox-Catalyzed Site-Selective Generation of Carbanions from C(sp3)–H Bonds in Amines. ACS Catalysis 12, S. 3974-3984.

Veröffentlichungsdatum dieses Volltextes: 18 Mrz 2022 11:05
Artikel
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.



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Details

DokumentenartArtikel
Titel eines Journals oder einer ZeitschriftACS Catalysis
Verlag:AMER CHEMICAL SOC
Ort der Veröffentlichung:WASHINGTON
Band:12
Seitenbereich:S. 3974-3984
Datum15 März 2022
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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