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| 001 | 462678 | ||
| 005 | 20250716150527.0 | ||
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| 100 | 1 | _ | |a Jurgeleit, Ramona |0 P:(DE-HGF)0 |b 0 |
| 245 | _ | _ | |a Catalytic Oxygenation of Hydrocarbons by Mono‐μ‐oxo Dicopper(II) Species Resulting from O−O Cleavage of Tetranuclear Cu I /Cu II Peroxo Complexes |
| 260 | _ | _ | |a Weinheim |c 2021 |b Wiley-VCH |
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| 520 | _ | _ | |a One of the challenges of catalysis is the transformation of inert C−H bonds to useful products. Copper-containing monooxygenases play an important role in this regard. Here we show that low-temperature oxygenation of dinuclear copper(I) complexes leads to unusual tetranuclear, mixed-valent $μ_4$-peroxo [Cu$^I$/Cu$^{II}$]$_2$ complexes. These Cu$_4$O$_2$ intermediates promote irreversible and thermally activated O−O bond homolysis, generating Cu$_2$O complexes that catalyze strongly exergonic H-atom abstraction from hydrocarbons, coupled to O-transfer. The Cu$_2$O species can also be produced with N$_2$O, demonstrating their capability for small-molecule activation. The binding and cleavage of O$_2$ leading to the primary Cu$_4$O$_2$ intermediate and the Cu$_2$O complexes, respectively, is elucidated with a range of solution spectroscopic methods and mass spectrometry. The unique reactivities of these species establish an unprecedented, 100 % atom-economic scenario for the catalytic, copper-mediated monooxygenation of organic substrates, employing both O-atoms of O$_2$. |
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| 700 | 1 | _ | |a Grimm-Lebsanft, Benjamin |0 P:(DE-H253)PIP1018557 |b 1 |
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| 700 | 1 | _ | |a Rübhausen, Michael |0 P:(DE-HGF)0 |b 10 |e Corresponding author |
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| 773 | _ | _ | |a 10.1002/anie.202101035 |g Vol. 60, no. 25, p. 14154 - 14162 |0 PERI:(DE-600)2011836-3 |n 25 |p 14154-14162 |t Angewandte Chemie / International edition |v 60 |y 2021 |x 1521-3773 |
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