Rapid Methylation of Aryl Bromides Using Air‐Stable DABCO‐Bis(Trimethylaluminum) via Nickel Metallaphotoredox Catalysis

J Jonas Djossou (Flow Chemistry Group, van ’t Hoff Institute for Molecular Sciences (HIMS) University of Amsterdam Amsterdam 1098 XH The Netherlands) A Andrea Aloia (Flow Chemistry Group, van ’t Hoff Institute for Molecular Sciences (HIMS) University of Amsterdam Amsterdam 1098 XH The Netherlands) L Luca Capaldo D Demi D. Snabilié (Van ‘t Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands) M Morgan Regnier (Flow Chemistry Group, van ’t Hoff Institute for Molecular Sciences (HIMS) University of Amsterdam Amsterdam 1098 XH The Netherlands) J Jasper H.A. Schuurmans (Flow Chemistry Group, Van’t Hoff Institute for Molecular Sciences (HIMS), University of Amsterdam, Science Park 904, Amsterdam 1098 XH, The Netherlands) A Antonio Monopoli (Chemistry Department University of Bari Aldo Moro Via Orabona 4 Bari 70125 Italy) B Bas de Bruin (Van ‘t Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands) T Timothy Noël (Flow Chemistry Group, Van’t Hoff Institute for Molecular Sciences (HIMS), University of Amsterdam, Science Park 904, Amsterdam 1098 XH, The Netherlands)

Abstract

Abstract We report a metallaphotocatalytic strategy for the selective methylation of (hetero)aryl bromides via nickel‐catalyzed cross‐coupling with bis(trimethylaluminum)‐1,4‐diazabicyclo[2.2.2]octane (DABAl‐Me₃), as a commercially available, air‐stable, and non‐pyrophoric aluminum‐based reagent. The method enables a fast, robust, and scalable methylation protocol that broadly accommodates various functional groups while preventing protodehalogenation. Mechanistic studies confirm the unprecedented generation of methyl radicals from an organo‐aluminum precursor under photoredox conditions, bypassing the limitations of conventional two‐electron pathways. This work expands the toolbox of practical radical precursors and provides a streamlined approach for selective C(sp 2 )─CH 3 bond formation.

Article Details

Volume / Issue Vol. 64, Issue 33
Published August 11, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (9)

J

Jonas Djossou

Flow Chemistry Group, van ’t Hoff Institute for Molecular Sciences (HIMS) University of Amsterdam Amsterdam 1098 XH The Netherlands

A

Andrea Aloia

Flow Chemistry Group, van ’t Hoff Institute for Molecular Sciences (HIMS) University of Amsterdam Amsterdam 1098 XH The Netherlands

L

Luca Capaldo

D

Demi D. Snabilié

Van ‘t Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands

M

Morgan Regnier

Flow Chemistry Group, van ’t Hoff Institute for Molecular Sciences (HIMS) University of Amsterdam Amsterdam 1098 XH The Netherlands

J

Jasper H.A. Schuurmans

Flow Chemistry Group, Van’t Hoff Institute for Molecular Sciences (HIMS), University of Amsterdam, Science Park 904, Amsterdam 1098 XH, The Netherlands

A

Antonio Monopoli

Chemistry Department University of Bari Aldo Moro Via Orabona 4 Bari 70125 Italy

B

Bas de Bruin

Van ‘t Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands

T

Timothy Noël

Flow Chemistry Group, Van’t Hoff Institute for Molecular Sciences (HIMS), University of Amsterdam, Science Park 904, Amsterdam 1098 XH, The Netherlands