The Origin of Catalytic Benzylic C−H Oxidation over a Redox‐Active Metal–Organic Framework
Authors
Kimberley, LouisSheveleva, Alena M.; orcid: 0000-0001-6190-5944
Li, Jiangnan
Carter, Joseph H.
Kang, Xinchen
Smith, Gemma L.
Han, Xue
Day, Sarah J.
Tang, Chiu C.
Tuna, Floriana; email: Floriana.Tuna@manchester.ac.uk
McInnes, Eric J. L.; email: eric.mcinnes@manchester.ac.uk
Yang, Sihai; email: sihai.yang@manchester.ac.uk
Schröder, Martin; orcid: 0000-0001-6992-0700; email: m.schroder@manchester.ac.uk
Publication Date
2021-06-04Submitted date
2021-02-15
Metadata
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Abstract: Selective oxidation of benzylic C−H compounds to ketones is important for the production of a wide range of fine chemicals, and is often achieved using toxic or precious metal catalysts. Herein, we report the efficient oxidation of benzylic C−H groups in a broad range of substrates under mild conditions over a robust metal–organic framework material, MFM‐170, incorporating redox‐active [Cu2II(O2CR)4] paddlewheel nodes. A comprehensive investigation employing electron paramagnetic resonance (EPR) spectroscopy and synchrotron X‐ray diffraction has identified the critical role of the paddlewheel moiety in activating the oxidant tBuOOH (tert‐butyl hydroperoxide) via partial reduction to [CuIICuI(O2CR)4] species.Citation
Angewandte ChemieType
otherDescription
From Wiley via Jisc Publications RouterHistory: received 2021-02-15, rev-recd 2021-03-27, pub-electronic 2021-06-04
Article version: VoR
Publication status: Published
Funder: Engineering and Physical Sciences Research Council; Id: http://dx.doi.org/10.13039/501100000266; Grant(s): EP/I011870
Funder: H2020 European Research Council; Id: http://dx.doi.org/10.13039/100010663; Grant(s): 742401