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Title: A Comparison of the ?-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis

Abstract

Solutions of TODGA and T(EH)DGA in n-dodecane were subjected to ?-irradiation in the presence and absence of an aqueous nitric acid phase and analyzed using UHPLC-ESI-MS to determine the rates of radiolytic decay of the two extractants, as well as to identify radiolysis products. The DGA concentrations decreased exponentially with increasing dose, and the measured degradation rate constants were uninfluenced by the presence or absence of an acidic aqueous phase, or by chemical variations in the alkyl side-chains. The DGA degradation was attributed to reactions of the dodecane radical cation, whose kinetics were measured for TODGA using picosecond electron pulse radiolysis to be k2 = (9.72 ± 1.10) × 109 M-1 s-1. The identified radiolysis products suggest that the bonds most vulnerable to radiolytic attack are those in the diglycolamide center of these molecules and not on the side-chains.

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
DOE - NE
OSTI Identifier:
1186739
Report Number(s):
INL/JOU-14-32985
Journal ID: ISSN 0736-6299
DOE Contract Number:
DE-AC07-05ID14517
Resource Type:
Journal Article
Resource Relation:
Journal Name: Solvent Extraction and Ion Exchange; Journal Volume: 33; Journal Issue: 5
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Radiolysis; TEHDGA; TODGA; UHPLC-MS

Citation Formats

Zarzana, Chris A., Groenewold, Gary S., Mincher, Bruce J., Mezyk, Stephen P., Modolo, Giuseppe, Wildens, Andreas, Schmidt, Holgar, Wishart, James F., and Cook, Andrew R. A Comparison of the ?-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis. United States: N. p., 2015. Web. doi:10.1080/07366299.2015.1012885.
Zarzana, Chris A., Groenewold, Gary S., Mincher, Bruce J., Mezyk, Stephen P., Modolo, Giuseppe, Wildens, Andreas, Schmidt, Holgar, Wishart, James F., & Cook, Andrew R. A Comparison of the ?-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis. United States. doi:10.1080/07366299.2015.1012885.
Zarzana, Chris A., Groenewold, Gary S., Mincher, Bruce J., Mezyk, Stephen P., Modolo, Giuseppe, Wildens, Andreas, Schmidt, Holgar, Wishart, James F., and Cook, Andrew R. Sun . "A Comparison of the ?-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis". United States. doi:10.1080/07366299.2015.1012885.
@article{osti_1186739,
title = {A Comparison of the ?-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis},
author = {Zarzana, Chris A. and Groenewold, Gary S. and Mincher, Bruce J. and Mezyk, Stephen P. and Modolo, Giuseppe and Wildens, Andreas and Schmidt, Holgar and Wishart, James F. and Cook, Andrew R.},
abstractNote = {Solutions of TODGA and T(EH)DGA in n-dodecane were subjected to ?-irradiation in the presence and absence of an aqueous nitric acid phase and analyzed using UHPLC-ESI-MS to determine the rates of radiolytic decay of the two extractants, as well as to identify radiolysis products. The DGA concentrations decreased exponentially with increasing dose, and the measured degradation rate constants were uninfluenced by the presence or absence of an acidic aqueous phase, or by chemical variations in the alkyl side-chains. The DGA degradation was attributed to reactions of the dodecane radical cation, whose kinetics were measured for TODGA using picosecond electron pulse radiolysis to be k2 = (9.72 ± 1.10) × 109 M-1 s-1. The identified radiolysis products suggest that the bonds most vulnerable to radiolytic attack are those in the diglycolamide center of these molecules and not on the side-chains.},
doi = {10.1080/07366299.2015.1012885},
journal = {Solvent Extraction and Ion Exchange},
number = 5,
volume = 33,
place = {United States},
year = {Sun Mar 01 00:00:00 EST 2015},
month = {Sun Mar 01 00:00:00 EST 2015}
}