Unique 3d–4f\nHeterometallic Networks Based\non a Nitronyl Nitroxide Radical Functionalized with Additional N and\nO Donors

Three 2D heterospin radical-3d–4f networks with\nthe formula\n{[Ln(hfac)<sub>3</sub>]<sub>2</sub>[M(hfac)<sub>2</sub>](NIT-3Py-5-Pyoe)<sub>2</sub>}<sub>n</sub> (M<sup>II</sup> = Co<sup>II</sup> and Ln<sup>III</sup> = Gd <b>1</b>, Dy <b>2</b>; M<sup>II</sup> =\nCu<sup>II</sup> and Ln<sup>III</sup> = Dy <b>3</b>; NIT-3Py-5-Pyoe\n= (2-(5-(4-pyridinone)-3-pyridyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide))\nhave been successfully constructed using a novel multidentate nitronyl\nnitroxide paramagnetic ligand containing mixed N- and O-donor sites.\nIn these 2D structures, the paramagnetic ligand acts as a tridentate\nlinker to bind two Ln<sup>III</sup> ions by means of one aminoxyl\ngroup and one pyridinone unit and one M<sup>II</sup> ion through the\npyridine ring. The magnetic behaviors of <b>1</b>–<b>3</b> are governed by predominant ferromagnetic radical–Ln\ninteractions.