In situ beam reduction of Pu(IV) and Bk(IV) as a route to trivalent transuranic coordination complexes with hydroxypyridinone chelators

open access.

Bibliographische Detailangaben
Veröffentlicht in:Journal of synchrotron radiation. - 1994. - 29(2022), Pt 2 vom: 01. März, Seite 315-322
1. Verfasser: Carter, Korey P (VerfasserIn)
Weitere Verfasser: Wacker, Jennifer N, Smith, Kurt F, Deblonde, Gauthier J P, Moreau, Liane M, Rees, Julian A, Booth, Corwin H, Abergel, Rebecca J
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2022
Zugriff auf das übergeordnete Werk:Journal of synchrotron radiation
Schlagworte:Journal Article X-ray absorption spectroscopy berkelium coordination complexes periodicity plutonium Chelating Agents Coordination Complexes Berkelium 2YQA718KUU mehr... Plutonium 53023GN24M
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520 |a The solution-state interactions of plutonium and berkelium with the octadentate chelator 3,4,3-LI(1,2-HOPO) (343-HOPO) were investigated and characterized by X-ray absorption spectroscopy, which revealed in situ reductive decomposition of the tetravalent species of both actinide metals to yield Pu(III) and Bk(III) coordination complexes. X-ray absorption near-edge structure (XANES) measurements were the first indication of in situ synchrotron redox chemistry as the Pu threshold and white-line position energies for Pu-343-HOPO were in good agreement with known diagnostic Pu(III) species, whereas Bk-343-HOPO results were found to mirror the XANES behavior of Bk(III)-DTPA. Extended X-ray absorption fine structure results revealed An-OHOPO bond distances of 2.498 (5) and 2.415 (2) Å for Pu and Bk, respectively, which match well with bond distances obtained for trivalent actinides and 343-HOPO via density functional theory calculations. Pu(III)- and Bk(III)-343-HOPO data also provide initial insight into actinide periodicity as they can be compared with previous results with Am(III)-, Cm(III)-, Cf(III)-, and Es(III)-343-HOPO, which indicate there is likely an increase in 5f covalency and heterogeneity across the actinide series 
650 4 |a Journal Article 
650 4 |a X-ray absorption spectroscopy 
650 4 |a berkelium 
650 4 |a coordination complexes 
650 4 |a periodicity 
650 4 |a plutonium 
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650 7 |a Coordination Complexes  |2 NLM 
650 7 |a Berkelium  |2 NLM 
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700 1 |a Wacker, Jennifer N  |e verfasserin  |4 aut 
700 1 |a Smith, Kurt F  |e verfasserin  |4 aut 
700 1 |a Deblonde, Gauthier J P  |e verfasserin  |4 aut 
700 1 |a Moreau, Liane M  |e verfasserin  |4 aut 
700 1 |a Rees, Julian A  |e verfasserin  |4 aut 
700 1 |a Booth, Corwin H  |e verfasserin  |4 aut 
700 1 |a Abergel, Rebecca J  |e verfasserin  |4 aut 
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