Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 138, Issue 16, Pages 5276-5282Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b13311
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Funding
- Ministerio de Economia y Competitividad, Spain [CTQ2011-24016]
- Ministerio de Economia y Competitividad, Spain (FEDER)
- Ministerio de Economia y Competitividad, Spain (FPU grant )
- Fundacion Seneca [19890/GERM/15]
- Universidad de Murcia
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The visible-light driven cyclometalation of arene substrates containing an N-donor heteroaromatic moiety as directing group by monocyclometalated Pt(II) complexes is reported. Precursors of the type [PtMe(C boolean AND N)(N boolean AND CH)], where N boolean AND CH is 2-phenylpyridine (ppyH) or related compunds with diverse electronic properties and CAN is the corresponding cyclometalated ligand, afford homoleptic cis-[Pt(C boolean AND N)(2)] complexes upon irradiation with blue LEDs at room temperature with evolution of methane. Heteroleptic derivatives cis-[Pt(ppy)(C'boolean AND N')] are obtained analogously from [PtMe(ppy)(N'boolean AND C'H)], where N'boolean AND C'H represents an extended set of heteroaromatic compounds. Experimental and computational studies demonstrate an unprecedented C-H oxidative addition, which is initiated by a triplet excited state of metal-to-ligand charge-transfer (MLCT) character and leads to a detectable Pt(IV) methyl hydride intermediate.
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