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Water co-catalysis in aerobic olefin epoxidation mediated by ruthenium oxo complexes

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journal contribution
posted on 2024-02-27, 14:28 authored by Q Cao, M Diefenbach, C Maguire, V Krewald, MJ Muldoon, U Hintermair
We report the development of a versatile Ru-porphyrin catalyst system which performs the aerobic epoxidation of aromatic and aliphatic (internal) alkenes under mild conditions, with product yields of up to 95% and turnover numbers (TON) up to 300. Water is shown to play a crucial role in the reaction, significantly increasing catalyst efficiency and substrate scope. Detailed mechanistic investigations employing both computational studies and a range of experimental techniques revealed that water activates the RuVI di-oxo complex for alkene epoxidation via hydrogen bonding, stabilises the RuIV mono-oxo intermediate, and is involved in the regeneration of the RuVI di-oxo complex leading to oxygen atom exchange. Distinct kinetics are obtained in the presence of water, and side reactions involved in catalyst deactivation have been identified.

Funding

Hub 'Science' 3: Catalysis for the Circular Economy and Sustainable Manufacturing

Engineering and Physical Sciences Research Council

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An integrated, multi-dimensional in-operando Reaction Monitoring Facility for Homogeneous Catalysis Research

Engineering and Physical Sciences Research Council

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Royal Society (UF160458)

History

Citation

Chem. Sci., 2024, Advance Article

Author affiliation

Chemistry

Version

  • VoR (Version of Record)

Published in

Chemical Science

Publisher

Royal Society of Chemistry (RSC)

issn

2041-6520

eissn

2041-6539

Acceptance date

2024-01-05

Copyright date

2024

Available date

2024-02-27

Language

en

Deposited by

Mr Qun Cao

Deposit date

2024-02-22

Data Access Statement

Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d3sc05516g

Rights Retention Statement

  • No

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