Dioxygen activation of a trinuclear Cu(I)Cu(I)Cu(I) cluster capable of mediating facile oxidation of organic substrates: competition between O-atom transfer and abortive intercomplex reduction

Chemistry : a European Journal
Suman MajiSunney I Chan

Abstract

The dioxygen activation of a series of Cu(I)Cu(I)Cu(I) complexes based on the ligands (L) 3,3'-(1,4-diazepane- 1,4-diyl)bis(1-{[2-(dimethylamino)ethyl](methyl)amino}propan-2-ol)(7-Me) or 3,3'-(1,4-diazepane-1,4-diyl)bis(1-{[2-(diethylamino)ethyl](ethyl)amino}propan-2-ol)(7-Et) forms an intermediate capable of mediating facile O-atom transfer to simple organic substrates at room temperature. To elucidate the dioxygen chemistry, we have examined the reactions of 7-Me, 7-Et, and 3,3'-(1,4-diazepane-1,4-diyl)bis[1-(4-methylpiperazin-1-yl)propan-2-ol] (7-N-Meppz) with dioxygen at -80, -55, and -35 °C in propionitrile (EtCN) by UV-visible, 77 K EPR, and X-ray absorption spectroscopy, and 7-N-Meppz and 7-Me with dioxygen at room temperature in acetonitrile (MeCN) by diode array spectrophotometry. At both -80 and -55 °C, the mixing of the starting [Cu(I)Cu(I)Cu(I)(L)](1+) complex (1) with O(2)-saturated propionitrile (EtCN) led to a bright green solution consisting of two paramagnetic species: the green dioxygen adduct [Cu(II)Cu(II)(μ-η(2):η(2)-peroxo)Cu(II)(L)](2+) (2) and the blue [Cu(II)Cu(II)(μ-O)Cu(II)(L)](2+) species (3). These observations are consistent with the initial formation of [Cu(II)Cu(II)(μ-O)(2)Cu(III)(L)](1+)(4), foll...Continue Reading

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Citations

Jan 20, 2017·Chemical Reviews·Courtney E ElwellWilliam B Tolman
Feb 17, 2017·Chemical Reviews·Vincent C-C WangSunney I Chan
Mar 15, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Yi-Hsueh HoJwu-Ting Chen
Feb 19, 2013·Angewandte Chemie·Sunney I ChanMichael K Chan
Mar 15, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Sarah E N Brazeau, Linda H Doerrer
Jun 26, 2015·Nature Communications·Sebastian GrundnerJohannes A Lercher
May 1, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Sarah E N BrazeauLinda H Doerrer
Apr 29, 2020·Chemistry, an Asian Journal·Tianxiang ChenTsz Woon Benedict Lo
Mar 13, 2014·Angewandte Chemie·Peter Haack, Christian Limberg

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