An air- and moisture-stable ruthenium precatalyst for diverse reactivity

McArthur, Gillian and Docherty, Jamie H. and Hareram, Mishra Deepak and Simonetti, Marco and Vitorica-Yrezabal, Iñigo J. and Douglas, James J. and Larrosa, Igor (2024) An air- and moisture-stable ruthenium precatalyst for diverse reactivity. Nature Chemistry. ISSN 1755-4330

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Abstract

Versatile, efficient and robust (pre)catalysts are pivotal in accelerating the discovery and optimization of chemical reactions, shaping diverse synthetic fields such as cross-coupling, C–H functionalization and polymer chemistry. Yet, their scarcity in certain domains has hindered the advancement and adoption of new applications. Here we present a highly reactive air- and moisture-stable ruthenium precatalyst [(tBuCN)5Ru(H2O)](BF4)2, featuring a key exchangeable water ligand. This versatile precatalyst drives an array of transformations, including late-stage C(sp2)–H arylation, primary/secondary alkylation, methylation, hydrogen/deuterium exchange, C(sp3)–H oxidation, alkene isomerization and oxidative cleavage, consistently outperforming conventionally used ruthenium (pre)catalysts. The generality and applicability of this precatalyst is exemplified through the potential for rapid screening and optimization of photocatalytic reactions with a suite of in situ generated ruthenium photocatalysts containing hitherto unknown complexes, and through the rapid discovery of reactivities previously unreported for ruthenium. The diverse applicability observed is suggestive of a generic platform for reaction simplification and accelerated synthetic discovery that will enable broader applicability and accessibility to state-of-the-art ruthenium catalysis.

Item Type:
Journal Article
Journal or Publication Title:
Nature Chemistry
Uncontrolled Keywords:
Research Output Funding/yes_externally_funded
Subjects:
?? yes - externally fundedgeneral chemical engineeringgeneral chemistrychemical engineering(all)chemistry(all) ??
ID Code:
217339
Deposited By:
Deposited On:
05 Apr 2024 14:45
Refereed?:
Yes
Published?:
Published
Last Modified:
16 Jul 2024 12:15