Synthesis, Structure, and Properties of Al((R)bpy)3 Complexes (R = t-Bu, Me): Homoleptic Main-Group Tris-bipyridyl Compounds.
2016
The neutral homoleptic tris-bpy aluminum complexes Al(Rbpy)3, where R = tBu (1) or Me (2), have been synthesized from reactions between AlX precursors (X = Cl, Br) and neutral Rbpy ligands through an aluminum disproportion process. The crystalline compounds have been characterized by single-crystal X-ray diffraction, electrochemical experiments, EPR, magnetic susceptibility, and density functional theory (DFT) studies. The collective data show that 1 and 2 contain Al3+ metal centers coordinated by three bipyridine (bpy•)1– monoanion radicals. Electrochemical studies show that six redox states are accessible from the neutral complexes, three oxidative and three reductive, that involve oxidation or reduction of the coordinated bpy ligands to give neutral Rbpy or Rbpy2– dianions, respectively. Magnetic susceptibility measurements (4–300 K) coupled with DFT studies show strong antiferromagnetic coupling of the three unpaired electrons located on the Rbpy ligands to give S = 1/2 ground states with low lying S ...
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