Ni(II) Complexes of the Redox-Active Bis(2-aminophenyl)dipyrrin: Structural, Spectroscopic, and Theoretical Characterization of Three Members of an Electron Transfer Series

Inorganic Chemistry
Jules MoutetFabrice Thomas

Abstract

The sterically hindered bis(2-aminophenyl)dipyrrin ligand H3NL was prepared. X-ray diffraction discloses a bifurcated hydrogen bonding network involving the dipyrrin and one aniline ring. The reaction of H3NL with one equivalent of nickel(II) in the air produces a paramagnetic neutral complex, which absorbs intensively in the Vis-NIR region. Its electron paramagnetic resonance spectrum displays resonances at g1= 2.033, g2= 2.008, and g3= 1.962 that are reminiscent of an (S = 1/2) system having a predominant organic radical character. Both the structural investigation (X-ray diffraction) and density functional theory calculations on [NiII(NL•)] points to an unprecedented mixed "pyrrolyl-anilinyl" radical character. The neutral complex [NiII(NL•)] exhibits both a reversible oxidation wave at -0.28 V vs Fc+/Fc and a reversible reduction wave at -0.91 V. The anion was found to be highly air-sensitive, but could be prepared by reduction with cobaltocene and structurally characterized. It comprises a Ni(II) ion coordinated to a closed-shell trianionic ligand and hence can be formulated as [NiII(NL)]-. The cation was generated by reacting [NiII(NL•)] with one equivalent of silver hexafluoroantimonate. By X-ray diffraction we establish...Continue Reading

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Citations

Mar 25, 2018·Chemistry : a European Journal·Mu-Chieh ChangJohn S Anderson
Aug 8, 2018·Chemistry : a European Journal·Jarl Ivar van der Vlugt
Jan 24, 2019·Chemical Communications : Chem Comm·Simran S SaundV Sara Thoi
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