Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling

H. Galan, C.A. Zarzana, A. Wilden, A. Nunez, Holger Schmidt, Richard J.M. Egberink, Andrea Leoncini, J. Cobos, Willem Verboom, G. Modolo, G.S. Groenewold, B.J. Mincher

Research output: Contribution to journalArticleAcademicpeer-review

19 Citations (Scopus)

Abstract

The stability against gamma radiation of MeTODGA (methyl tetraoctyldiglycolamide) and Me2TODGA (dimethyl tetraoctyldiglycolamide), derivatives from the well-known extractant TODGA (N,N,N′,N′-tetraoctyldiglycolamide), were studied and compared. Solutions of MeTODGA and Me2TODGA in alkane diluents were subjected to 60Co γ-irradiation in the presence and absence of nitric acid and analyzed using LC-MS to determine their rates of radiolytic concentration decrease, as well as to identify radiolysis products. The results of product identification from three different laboratories are compared and found to be in good agreement. The diglycolamide (DGA) concentrations decreased exponentially with increasing absorbed dose. The MeTODGA degradation rate constants (dose constants) were uninfluenced by the presence of nitric acid, but the acid increased the rate of degradation for Me2TODGA. The degradation products formed by irradiation are also initially produced in greater amounts in acid-contacted solution, but products may also be degraded by continued radiolysis. The identified radiolysis products suggest that the weakest bonds are those in the diglycolamide center of these molecules.
Original languageEnglish
Pages (from-to)18049-18056
Number of pages8
JournalDalton transactions
Volume44
Issue number41
DOIs
Publication statusPublished - 2015

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Actinoid Series Elements
Radiolysis
Recycling
Nitric Acid
Derivatives
Degradation
Irradiation
Alkanes
Acids
Gamma rays
Rate constants
Molecules

Keywords

  • METIS-314667
  • IR-99895

Cite this

Galan, H., Zarzana, C. A., Wilden, A., Nunez, A., Schmidt, H., Egberink, R. J. M., ... Mincher, B. J. (2015). Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling. Dalton transactions, 44(41), 18049-18056. https://doi.org/10.1039/C5DT02484F
Galan, H. ; Zarzana, C.A. ; Wilden, A. ; Nunez, A. ; Schmidt, Holger ; Egberink, Richard J.M. ; Leoncini, Andrea ; Cobos, J. ; Verboom, Willem ; Modolo, G. ; Groenewold, G.S. ; Mincher, B.J. / Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling. In: Dalton transactions. 2015 ; Vol. 44, No. 41. pp. 18049-18056.
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abstract = "The stability against gamma radiation of MeTODGA (methyl tetraoctyldiglycolamide) and Me2TODGA (dimethyl tetraoctyldiglycolamide), derivatives from the well-known extractant TODGA (N,N,N′,N′-tetraoctyldiglycolamide), were studied and compared. Solutions of MeTODGA and Me2TODGA in alkane diluents were subjected to 60Co γ-irradiation in the presence and absence of nitric acid and analyzed using LC-MS to determine their rates of radiolytic concentration decrease, as well as to identify radiolysis products. The results of product identification from three different laboratories are compared and found to be in good agreement. The diglycolamide (DGA) concentrations decreased exponentially with increasing absorbed dose. The MeTODGA degradation rate constants (dose constants) were uninfluenced by the presence of nitric acid, but the acid increased the rate of degradation for Me2TODGA. The degradation products formed by irradiation are also initially produced in greater amounts in acid-contacted solution, but products may also be degraded by continued radiolysis. The identified radiolysis products suggest that the weakest bonds are those in the diglycolamide center of these molecules.",
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author = "H. Galan and C.A. Zarzana and A. Wilden and A. Nunez and Holger Schmidt and Egberink, {Richard J.M.} and Andrea Leoncini and J. Cobos and Willem Verboom and G. Modolo and G.S. Groenewold and B.J. Mincher",
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Galan, H, Zarzana, CA, Wilden, A, Nunez, A, Schmidt, H, Egberink, RJM, Leoncini, A, Cobos, J, Verboom, W, Modolo, G, Groenewold, GS & Mincher, BJ 2015, 'Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling' Dalton transactions, vol. 44, no. 41, pp. 18049-18056. https://doi.org/10.1039/C5DT02484F

Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling. / Galan, H.; Zarzana, C.A.; Wilden, A.; Nunez, A.; Schmidt, Holger; Egberink, Richard J.M.; Leoncini, Andrea; Cobos, J.; Verboom, Willem; Modolo, G.; Groenewold, G.S.; Mincher, B.J.

In: Dalton transactions, Vol. 44, No. 41, 2015, p. 18049-18056.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling

AU - Galan, H.

AU - Zarzana, C.A.

AU - Wilden, A.

AU - Nunez, A.

AU - Schmidt, Holger

AU - Egberink, Richard J.M.

AU - Leoncini, Andrea

AU - Cobos, J.

AU - Verboom, Willem

AU - Modolo, G.

AU - Groenewold, G.S.

AU - Mincher, B.J.

PY - 2015

Y1 - 2015

N2 - The stability against gamma radiation of MeTODGA (methyl tetraoctyldiglycolamide) and Me2TODGA (dimethyl tetraoctyldiglycolamide), derivatives from the well-known extractant TODGA (N,N,N′,N′-tetraoctyldiglycolamide), were studied and compared. Solutions of MeTODGA and Me2TODGA in alkane diluents were subjected to 60Co γ-irradiation in the presence and absence of nitric acid and analyzed using LC-MS to determine their rates of radiolytic concentration decrease, as well as to identify radiolysis products. The results of product identification from three different laboratories are compared and found to be in good agreement. The diglycolamide (DGA) concentrations decreased exponentially with increasing absorbed dose. The MeTODGA degradation rate constants (dose constants) were uninfluenced by the presence of nitric acid, but the acid increased the rate of degradation for Me2TODGA. The degradation products formed by irradiation are also initially produced in greater amounts in acid-contacted solution, but products may also be degraded by continued radiolysis. The identified radiolysis products suggest that the weakest bonds are those in the diglycolamide center of these molecules.

AB - The stability against gamma radiation of MeTODGA (methyl tetraoctyldiglycolamide) and Me2TODGA (dimethyl tetraoctyldiglycolamide), derivatives from the well-known extractant TODGA (N,N,N′,N′-tetraoctyldiglycolamide), were studied and compared. Solutions of MeTODGA and Me2TODGA in alkane diluents were subjected to 60Co γ-irradiation in the presence and absence of nitric acid and analyzed using LC-MS to determine their rates of radiolytic concentration decrease, as well as to identify radiolysis products. The results of product identification from three different laboratories are compared and found to be in good agreement. The diglycolamide (DGA) concentrations decreased exponentially with increasing absorbed dose. The MeTODGA degradation rate constants (dose constants) were uninfluenced by the presence of nitric acid, but the acid increased the rate of degradation for Me2TODGA. The degradation products formed by irradiation are also initially produced in greater amounts in acid-contacted solution, but products may also be degraded by continued radiolysis. The identified radiolysis products suggest that the weakest bonds are those in the diglycolamide center of these molecules.

KW - METIS-314667

KW - IR-99895

U2 - 10.1039/C5DT02484F

DO - 10.1039/C5DT02484F

M3 - Article

VL - 44

SP - 18049

EP - 18056

JO - Dalton transactions

JF - Dalton transactions

SN - 1477-9226

IS - 41

ER -