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Updated: May 14, 2025
Line Shape Analysis of Dynamic NMR Spectra for Characterizing Coordination Sphere Rearrangements at a Chiral Rhenium Polyhydride Complex
Published on: July 27, 2022
Unusual zig-zag-shaped Ln-radical coordination networks derived from a nitronyl nitroxide with two imidazole groups:
Chao-Yi Jin1, Qiuxue Zhang1, Jinkui Tang2
1Department of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry, College of Chemistry, Nankai University, Tianjin 300071, China. llicun@nankai.edu.cn.
Abstract:
Two unusual two-dimensional coordination networks, namely, {[Gd(hfac)3]3(NIT-Ph-3,5-bIm)2}·2.25C6H14 (1) and {[Dy(hfac)3]3(NIT-Ph-3,5-bIm)2}·2.5C6H14 (2), were obtained using the multidentate nitronyl nitroxide ligand containing two additional imidazole groups, NIT-Ph-3,5-bIm (NIT-Ph-3,5-bIm = 2-[3,5-bis(1-imidazole)phenyl]-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide; hfac = hexafluoroacetylacetonate). In these Ln-radical complexes, the multidentate nitronyl nitroxide radical ligand served as a tridentate linker, binding three LnIII ions via one NO group and two imidazole units, resulting in unique zig-zag-shaped 2D networks with KIa topology. These coordination networks underwent a single-crystal-to-single-crystal transformation from a low-temperature non-centrosymmetric space group (P21) to a room-temperature centrosymmetric space group (P21/c) accompanied by the loss of helicity in chiral chains and an order-disorder transition of the LnIII ions. Direct-current magnetic susceptibility studies of the Gd derivative showed dominant ferromagnetic Gd-NO exchange. Dynamic magnetic studies of the Dy analogue displayed temperature-dependent nonzero out-of-phase signals, indicating slow magnetic relaxation behavior.
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