Spectroscopic and computational investigation of actinium coordination chemistry

被引：78

作者：

Ferrier, Maryline G. ^{[1
]}

Batista, Enrique R. ^{[1
]}

Berg, John M. ^{[1
]}

Birnbaum, Eva R. ^{[1
]}

Cross, Justin N. ^{[1
]}

Engle, Jonathan W. ^{[1
]}

La Pierre, Henry S. ^{[1
]}

Kozimor, Stosh A. ^{[1
]}

Pacheco, Juan S. Lezama ^{[2
]}

Stein, Benjamin W. ^{[1
]}

Stieber, S. Chantal E. ^{[1
,3
]}

Wilson, Justin J. ^{[1
,4
]}

机构：

[1] Los Alamos Natl Lab, Los Alamos, NM 87545 USA

[2] Stanford Univ, Stanford, CA 94305 USA

[3] Calif State Polytech Univ Pomona, Pomona, CA 91768 USA

[4] Cornell Univ, Ithaca, NY 14853 USA

来源：

NATURE COMMUNICATIONS | 2016年 / 7卷

基金：

美国能源部; 美国国家卫生研究院;

关键词：

MOLECULAR-DYNAMICS; IONIC-RADII; SOLID-STATE; TRIVALENT; SORPTION; METAL; HYDROLYSIS; EXTRACTION; 5F-SERIES; ELEMENTS;

D O I：

10.1038/ncomms12312

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Actinium-225 is a promising isotope for targeted-a 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, Ac-III 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)angstrom, respectively. The X-ray absorption spectroscopy comparisons between Ac-III and Am-III in HCl solutions indicate Ac-III coordinates more inner-sphere Cl1-ligands (3.2 +/- 1.1) than Am-III (0.8 +/- 0.3). These results imply diverse reactivity for the +3 actinides and highlight the unexpected and unique Ac-III chemical behaviour.

引用

页数：8

共 60 条

[1] Coordination chemistry of trivalent lanthanide and actinide ions in dilute and concentrated chloride solutions [J].