Spectroscopic and Computational Characterization of Diethylenetriaminepentaacetic Acid/Transplutonium Chelates: Evidencing Heterogeneity in the Heavy Actinide(III) Series

Angewandte Chemie
Gauthier J-P DeblondeRebecca J Abergel

Abstract

The chemistry of trivalent transplutonium ions (Am3+ , Cm3+ , Bk3+ , Cf3+ , Es3+ …) is usually perceived as monotonic and paralleling that of the trivalent lanthanide series. Herein, we present the first extended X-ray absorption fine structure (EXAFS) study performed on a series of aqueous heavy actinide chelates, extending past Cm. The results obtained on diethylenetriaminepentaacetic acid (DTPA) complexes of trivalent Am, Cm, Bk, and Cf show a break to much shorter metal-oxygen nearest-neighbor bond lengths in the case of Cf3+ . Corroborating those results, density functional theory calculations, extended to Es3+ , suggest that the shorter Cf-O and Es-O bonds could arise from the departure of the coordinated water molecule and contraction of the ligand around the metal relative to the other [MIII DTPA(H2 O)]2- (M=Am, Cm, Bk) complexes. Taken together, these experimental and theoretical results demonstrate inhomogeneity within the trivalent transplutonium series that has been insinuated and debated in recent years, and that may also be leveraged for future nuclear waste reprocessing technologies.

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Aug 25, 2017·Nature Chemistry·Gauthier J-P DeblondeRebecca J Abergel

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Citations

Sep 4, 2018·Chemical Communications : Chem Comm·Morgan P KelleyJenifer C Shafer
Sep 7, 2018·Chemical Communications : Chem Comm·Korey P CarterJohn K Gibson
Mar 26, 2019·Chemistry : a European Journal·Frankie D WhiteThomas E Albrecht-Schmitt
Aug 9, 2019·Chemical Science·Abel RicanoRebecca J Abergel
Jun 6, 2019·Nature Communications·Gauthier J-P DeblondeRebecca J Abergel
Mar 12, 2021·Environmental Science & Technology·Margaux MolinasRizlan Bernier-Latmani
Apr 29, 2021·Inorganic Chemistry·Yang GaoGeorg Schreckenbach
Jun 26, 2021·Chemical Science·Zachary R JonesDavid H Woen
Feb 5, 2019·Inorganic Chemistry·Thomas E Albrecht-Schmitt
Dec 4, 2019·Journal of the American Chemical Society·Benjamin W SteinPing Yang
Mar 2, 2019·Inorganic Chemistry·Aditi Chandrasekar, Tapan K Ghanty
Jul 11, 2019·Inorganic Chemistry·Matthew L MarshThomas E Albrecht-Schmitt

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