Chelation and stabilization of berkelium in oxidation state +IV

Deblonde, Gauthier J. -P.; Sturzbecher-Hoehne, Manuel; Rupert, Peter B.; An, Dahlia D.; Illy, Marie-Claire; Ralston, Corie Y.; Brabec, Jiri; de Jong, Wibe A.; Strong, Roland K.; Abergel, Rebecca J.

doi:10.1038/nchem.2759

Chelation and stabilization of berkelium in oxidation state +IV

Journal Article · Mon Apr 10 00:00:00 EDT 2017 · Nature Chemistry

DOI:https://doi.org/10.1038/nchem.2759· OSTI ID:1436161

Deblonde, Gauthier J. -P. ^[1]; Sturzbecher-Hoehne, Manuel ^[1]; Rupert, Peter B. ^[2]; An, Dahlia D. ^[1]; Illy, Marie-Claire ^[1]; Ralston, Corie Y. ^[3]; Brabec, Jiri ^[4]; de Jong, Wibe A. ^[5]; Strong, Roland K. ^[2]; Abergel, Rebecca J. ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Fred Hutchinson Cancer Research Center, Seattle, WA (United States). Division of Basic Science
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Berkeley Center for Structural Biology
Academy of Sciences of the Czech Republic, Prague (Czech Republic). J. Heyrovsky Institute of Physical Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Computational Research Division

Berkelium (Bk) has been predicted to be the only transplutonium element able to exhibit both +III and +IV oxidation states in solution, but evidence of a stable oxidized Bk chelate has so far remained elusive. Here, in this work, we describe the stabilization of the heaviest 4+ ion of the periodic table, under mild aqueous conditions, using a siderophore derivative. The resulting Bk(IV) complex exhibits luminescence via sensitization through an intramolecular antenna effect. This neutral Bk(IV) coordination compound is not sequestered by the protein siderocalin - a mammalian metal transporter - in contrast to the negatively charged species obtained with neighbouring trivalent actinides americium, curium and californium (Cf). The corresponding Cf(III)-ligand-protein ternary adduct was characterized by X-ray diffraction analysis. Finally, combined with theoretical predictions, these data add significant insight to the field of transplutonium chemistry, and may lead to innovative Bk separation and purification processes.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1436161

Journal Information:: Nature Chemistry, Journal Name: Nature Chemistry Journal Issue: 9 Vol. 9; ISSN 1755-4330

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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