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  Lanthanide(III) Complexes Based on an 18-Membered Macrocycle Containing Acetamide Pendants. Structural Characterization and paraCEST Properties

Castro, G., Wang, G., Gambino, T., Esteban-Gómez, D., Valencia, L., Angelovski, G., et al. (2021). Lanthanide(III) Complexes Based on an 18-Membered Macrocycle Containing Acetamide Pendants. Structural Characterization and paraCEST Properties. Inorganic Chemistry, 60(3), 1902-1914. doi:10.1021/acs.inorgchem.0c03385.

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Castro, G, Author
Wang, G1, 2, Author              
Gambino, T1, 2, Author              
Esteban-Gómez, D, Author
Valencia, L, Author
Angelovski, G1, 2, Author              
Platas-Iglesias , C, Author
Pérez-Lourido, P, Author
Affiliations:
1Research Group MR Neuroimaging Agents, Max Planck Institute for Biological Cybernetics, Max Planck Society, ou_2528691              
2Max Planck Institute for Biological Cybernetics, Max Planck Society, ou_1497794              

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 Abstract: We report a detailed investigation of the coordination properties of macrocyclic lanthanide complexes containing a 3,6,10,13-tetraaza-1,8(2,6)-dipyridinacyclotetradecaphane scaffold functionalized with four acetamide pendant arms. The X-ray structures of the complexes with the large Ln3+ ions (La and Sm) display 12- and 10-coordinated metal ions, where the coordination sphere is fulfilled by the six N atoms of the macrocycle, the four O atoms of the acetamide pendants, and a bidentate nitrate anion in the La3+ complex. The analogous Yb3+ complex presents, however, a 9-coordinated metal ion because one of the acetamide pendant arms remains uncoordinated. 1H NMR studies indicate that the 10-coordinated form is present in solution throughout the lanthanide series from La to Tb, while the smaller lanthanides form 9-coordinated species. 1H and 89Y NMR studies confirm the presence of this structural change because the two species are present in solution. Analysis of the 1H chemical shifts observed for the Tb3+ complex confirms its D2 symmetry in aqueous solution and evidences a highly rhombic magnetic susceptibility tensor. The acetamide resonances of the Pr3+ and Tb3+ complexes provided sizable paraCEST effects, as demonstrated by the corresponding Z-spectra recorded at different temperatures and studies on tube phantoms recorded at 22 °C.

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 Dates: 2021-012021-02
 Publication Status: Published in print
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 Identifiers: DOI: 10.1021/acs.inorgchem.0c03385
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Title: Inorganic Chemistry
  Abbreviation : Inorg. Chem.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 60 (3) Sequence Number: - Start / End Page: 1902 - 1914 Identifier: ISSN: 0020-1669
CoNE: https://pure.mpg.de/cone/journals/resource/0020-1669