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

Zarzana, Chris A.; Groenewold, Gary S.; Mincher, Bruce J.; Mezyk, Stephen P.; Modolo, Giuseppe; Wildens, Andreas; Schmidt, Holgar; Wishart, James F.; Cook, Andrew R.

doi:10.1080/07366299.2015.1012885

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

Journal Article · Sat Feb 28 23:00:00 EST 2015 · Solvent Extraction and Ion Exchange

DOI:https://doi.org/10.1080/07366299.2015.1012885· OSTI ID:1186739

Zarzana, Chris A.; Groenewold, Gary S.; Mincher, Bruce J.; Mezyk, Stephen P.; Modolo, Giuseppe; Wildens, Andreas; Schmidt, Holgar; Wishart, James F.; Cook, Andrew R.

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.

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: DOE - NE

DOE Contract Number:: AC07-05ID14517

OSTI ID:: 1186739

Report Number(s):: INL/JOU-14-32985

Journal Information:: Solvent Extraction and Ion Exchange, Journal Name: Solvent Extraction and Ion Exchange Journal Issue: 5 Vol. 33; ISSN 0736-6299

Publisher:: Taylor and Francis

Country of Publication:: United States

Language:: English

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