Abstract
A convenient and general strategy for the synthesis of stable bis(cyclometalated) pentafluorophenyl PtIV complexes fac-[Pt(C^N)2 (C6 F5 )Cl] (3 a-f) and mer-[Pt(C^N)2 (C6 F5 )(CN)] (4 c,d) has been developed. Complexes 3 were selectively generated by low-temperature oxidation of the cyclometalated PtII complexes [Pt(C^N)(HC^N)(C6 F5 )] 2 [prepared from cis-[Pt(C6 F5 )2 (HC^N)2 ] (1) intermediates] with PhICl2 and subsequent metalation of the pendant HC^N ligand. Complexes 3 a,b were also alternatively generated by irradiation (Hg lamp, 400 W) of complexes 2 a,b, respectively, in CH2 Cl2 . This latter reaction proceeds via the hydride PtIV species cis-[Pt(C^N)2 (C6 F5 )H], detected as the only intermediate species. The molecular structures of 1 a,d, 2 a, and 3 a,b,d,e were confirmed by X-ray diffraction. The substitution of Cl- by CN- in fac-[Pt(C^N)2 (C6 F5 )Cl] [C^N=2-phenylbenzothiazole (3 c), 2-(4-bromophenyl)benzothiazole (3 d)] evolved with isomerization to give rise to the isomers (OC-6-42)-[Pt(C^N)2 (C6 F5 )(CN)] (4 c, 4 d) having a mer disposition of the cyclometalated and C6 F5 groups (X-ray, 4 c). All the complexes are luminescent and their electronic spectra have been compared and interpreted with the aid of time-dependent DFT calculations.
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