期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 23, 期 24, 页码 5758-5771出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201605809
关键词
cyclometalating ligands; density functional calculations; luminescence; photochemistry; platinum
资金
- Spanish MINECO/FEDER [CTQ2013-45518-P, CTQ2016-78463-P]
- UR grant
A convenient and general strategy for the synthesis of stable bis(cyclometalated) pentafluorophenyl Pt-IV complexes fac-[Pt((CN)-N-boolean AND)(2)(C6F5)Cl] (3a-f) and mer-[Pt((CN)-N-boolean AND)(2)(C6F5)(CN)] (4c,d) has been developed. Complexes 3 were selectively generated by low-temperature oxidation of the cyclometalated Pt-II complexes [Pt((CN)-N-boolean AND)((HCN)-N-boolean AND)(C6F5)] 2 [prepared from cis-[Pt(C6F5)(2)((HCN)-N-boolean AND)(2)] (1) intermediates] with PhICl2 and subsequent metalation of the pendant (HCN)-N-boolean AND ligand. Complexes 3a,b were also alternatively generated by irradiation (Hg lamp, 400W) of complexes 2a,b, respectively, in CH2Cl2. This latter reaction proceeds via the hydride Pt-IV species cis-[Pt((CN)-N-boolean AND)(2)(C6F5)H], detected as the only intermediate species. The molecular structures of 1a,d, 2a, and 3a,b,d,e were confirmed by X-ray diffraction. The substitution of Cl- by CN- in fac-[Pt((CN)-N-boolean AND)(2)(C6F5)Cl] [(CN)-N-boolean AND=2-phenylbenzothiazole (3c), 2-(4-bromophenyl)benzothiazole (3d)] evolved with isomerization to give rise to the isomers (OC-6-42)-[Pt((CN)-N-boolean AND)(2)(C6F5)(CN)] (4c, 4d) having a mer disposition of the cyclometalated and C6F5 groups (X-ray, 4c). 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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