Combining the Best of Two Chelating Titans: A Hydroxypyridinone-Decorated Macrocyclic Ligand for Efficient and Concomitant Complexation and Sensitized Luminescence of f-Elements

Arnedo‐Sanchez, Leticia; Smith, Kurt F.; Deblonde, Gauthier J.‐P.; Carter, Korey P.; Moreau, Liane M.; Rees, Julian A.; Tratnjek, Toni; Booth, Corwin H.; Abergel, Rebecca J.

doi:10.1002/cplu.202100083

Title: Combining the Best of Two Chelating Titans: A Hydroxypyridinone-Decorated Macrocyclic Ligand for Efficient and Concomitant Complexation and Sensitized Luminescence of f-Elements

Journal Article · Wed Mar 17 00:00:00 EDT 2021 · ChemPlusChem

DOI:https://doi.org/10.1002/cplu.202100083· OSTI ID:1811790

^[1]; Smith, Kurt F. ^[1];

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^[1]; Tratnjek, Toni ^[1];

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Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Abstract An ideal chelator for f‐elements features rapid kinetics of complexation, high thermodynamic stability, and slow kinetics of dissociation. Here we present the facile synthesis of a macrocyclic ligand bearing four 1‐hydroxy‐2‐pyridinone units linked to a cyclen scaffold that rapidly forms thermodynamically stable complexes with lanthanides (Sm ³⁺ , Eu ³⁺ , Tb ³⁺ , Dy ³⁺ ) and a representative late actinide (Cm ³⁺ ) in aqueous media and concurrently sensitizes them. Extended X‐ray absorption fine structure (EXAFS) spectroscopy revealed an increase in the Ln/An−O bond lengths following the trend Cm>Eu>Tb and EXAFS data were compatible with time‐resolved luminescence studies, which indicated one to two water molecules in the inner metal coordination sphere of Eu(III) and two water molecules for the Cm(III) complex. Spectrofluorimetric ligand competition titrations against DTPA confirmed the high thermodynamic stability of DOTHOPO complexes, with pM values between 19.9(1) and 21.9(2).

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1811790

Alternate ID(s):: OSTI ID: 1786480

Report Number(s):: LLNL-JRNL-823793; 1036148

Journal Information:: ChemPlusChem, Vol. 86, Issue 3; ISSN 2192-6506

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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