Journal Article

FZJ-2021-02976

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Gamma and pulsed electron radiolysis studies of CyMe4BTBP and CyMe4BTPhen: Identification of radiolysis products and effects on the hydrometallurgical separation of trivalent actinides and lanthanides

Schmidt, H. ; Wilden, A. (Corresponding author)FZJ* ; Modolo, G.FZJ* ; Bosbach, D.FZJ* ; Santiago-Schübel, B.FZJ* ; Hupert, M.FZJ* ; Mincher, B. J. ; Mezyk, S. P. ; Švehla, J. ; Grüner, B. ; Ekberg, C.

2021
Pergamon Press Frankfurt, M.

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Please use a persistent id in citations: http://hdl.handle.net/2128/28365  doi:10.1016/j.radphyschem.2021.109696

Abstract: The radiolytic stability of the highly selective ligands CyMe4BTBP and CyMe4BTPhen against ionizing gamma radiationwas studied in 1-octanol solution. CyMe4BTBP and CyMe4BTPhen are important extractants for a potentialtreatment of used nuclear fuel. They were studied under identical experimental conditions to directly comparethe effects of gamma and pulsed electron radiolysis on the ligands and systematically study the influence ofstructural changes in the ligand backbone. Distribution ratios of Am3+, Cm3+ and Eu3+, the residual concentrationof CyMe4BTBP and CyMe4BTPhen in solution, and the formation of radiolysis products were studied as afunction of absorbed gamma dose and presence of an acidic aqueous phase during irradiation. Quantitative andsemi-quantitative analyses were used to elucidate the radiolysis mechanism for both ligands. Addition productsof alpha-hydroxyoctyl radicals formed through radiolysis of the 1-octanol diluent to the ligand molecules wereidentified as the predominant radiolysis products. These addition products also extract trivalent metal ions, asdistribution ratios remained high although the parent molecule concentrations decreased. Therefore, the utilizationtime of a solvent using these extractants under the harsh conditions of used nuclear fuel treatment could beconsiderably longer than expected. Understanding the radiolysis mechanism is crucial for designing more radiationresistant extractants.

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Contributing Institute(s):

1. Nukleare Entsorgung und Reaktorsicherheit (IEK-6)
2. Analytik (ZEA-3)

Research Program(s):

1. 1412 - Predisposal (POF4-141) (POF4-141)
2. SACSESS - Safety of ACtinide Separation proceSSes (323282) (323282)
3. GENIORS - GEN IV Integrated Oxide fuels recycling strategies (755171) (755171)
4. BMBF-02NUK059D - Spektroskopische Charakterisierung von f-Element-Komplexen mit soft donor-Liganden (f-Char) (BMBF-02NUK059D) (BMBF-02NUK059D)

Appears in the scientific report 2021

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; Essential Science Indicators ; Nationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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