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Spectroscopic and computational investigation of actinium coordination chemistry #MMPMID27531582
Ferrier MG; Batista ER; Berg JM; Birnbaum ER; Cross JN; Engle JW; La Pierre HS; Kozimor SA; Lezama Pacheco JS; Stein BW; Stieber SCE; Wilson JJ
Nat Commun 2016[]; 7 (ä): ä PMID27531582show ga
Actinium-225 is a promising isotope for targeted-? therapy. Unfortunately, progress in developing chelators for medicinal applications has been hindered by a limited understanding of actinium chemistry. This knowledge gap is primarily associated with handling actinium, as it is highly radioactive and in short supply. Hence, AcIII reactivity is often inferred from the lanthanides and minor actinides (that is, Am, Cm), with limited success. Here we overcome these challenges and characterize actinium in HCl solutions using X-ray absorption spectroscopy and molecular dynamics density functional theory. The Ac?Cl and Ac?OH2O distances are measured to be 2.95(3) and 2.59(3) Å, respectively. The X-ray absorption spectroscopy comparisons between AcIII and AmIII in HCl solutions indicate AcIII coordinates more inner-sphere Cl1? ligands (3.2±1.1) than AmIII (0.8±0.3). These results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique AcIII chemical behaviour.