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Three diplatinum(II) complexes [{PtL} 2 (μ‐thea)] (H 4 thea=2,3,6,7‐tetrahydroxy‐9,10‐dimethyl‐9,10‐dihydro‐9,10‐ethanoanthracene) have been prepared, with diphosphine or bipyridyl “L” co‐ligands. One‐electron oxidation of these complexes gave radical cations containing a mixed‐valent [thea            .] 3−  ligand with discrete catecholate and semiquinonate centers separated by quaternary methylene spacers. The electronic character of these radicals is near the Robin–Day class II/III border determined by UV/Vis/NIR and EPR spectroscopies. Crystal‐structure determinations and a DFT calculation imply that oxidation of the thea 4−  ligand may lead to an increased through‐space interaction between the dioxolene π systems.

Stable Mixed‐Valent Radicals from Platinum(II) Complexes of a Bis(dioxolene) Ligand