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Ladder-Type Cu(II) Coordination Polymer with π-π Stacking of Planar Blatter Radical Ligands: Structural and Magnetic
Hemant K Singh1, Kayla M Smith2, Jeremy M Rawson3
1Centre of Molecular and Macromolecular Studies, Polish Academy of Sciences, 90363 Łódź, Poland.
Abstract:
The synthesis of two C(2)-pyridyl derivatives of the planar Blatter radical was developed by using the tris-(trimethylsilyl)-silane (TTMSS)-assisted cyclization of appropriate iodoarenes. These monodentate paramagnetic ligands were characterized by spectroscopic (UV-vis and electron paramagnetic resonance (EPR)) and electrochemical methods and reacted with (pdc)-Cu-(H2O)3. A complex containing the 3-pyridyl group was characterized structurally, revealing novel polymeric Cu-O-Cu-O ladders separated with slipped stacks of radical ligands. Superconducting quantum interference device (SQUID) magnetometry of this complex demonstrated strong antiferromagnetic interactions between the radicals and largely isolated Cu-(II) ions. Analysis of the magnetic data with the Hatfield model, assuming two isolated one-dimensional (1D) alternating Heisenberg chains, gave J RR/k B = -1200 K and αRR = 0.4 for the paramagnetic ligand stacks, and J CuCu/k B = -3.5 K and αCuCu = 0.9 for the Cu-(II) ion chains. Analysis of the experimental data was augmented with density functional theory (DFT) calculations.
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