A comparison of the y-Radiolysis of TODGA and T(EH)DGA using UHPLC-ESI-MS analysis
Abstract
Solutions of the diglycolamide extractants TODGA and T(EH)DGA in n-dodecane were subjected to γ- irradiation in the presence and absence of an acidic aqueous phase. These solutions were then analyzed using UHPLC-ESI-MS to determine the rates of radiolytic decay of the two extractants neat and in contact with respect to the acidity of the contacted aqueous phase, as well as to identify radiolysis products. The presence or absence of an acidic aqueous phase was shown to have no influence on the measured decay rates, nor did the side-chain have an influence. A number of radiolysis products were identified, consistent with those previously identified for these two compounds using GC-MS. The identity of these radiolysis products suggests that the bonds most vulnerable to radiolytic attack are those in the dyglycolamide center of these molecules, and not on the side-chains. The agreement of these results with previous work using GC-MS indicates supports the further use of UHPLC-ESI-MS as a tool for studying diglycolamide extractant systems.
- Authors:
-
- Idaho National Lab. (INL), Idaho Falls, ID (United States)
- California State Uni
- Forschungszentrum Jülich GmbH, Institut für Energie- und Klimaforschung-Nukleare Entsorgung und Reaktorsicherheit (IEK-6), Jülich (Germany)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Idaho National Lab. (INL), Idaho Falls, ID (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1184759
- Alternate Identifier(s):
- OSTI ID: 1240715
- Report Number(s):
- INL/JOU-14-32985; BNL-111893-2016-JA
Journal ID: ISSN 0736-6299
- Grant/Contract Number:
- AC07-05ID14517; SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Solvent Extraction and Ion Exchange
- Additional Journal Information:
- Journal Name: Solvent Extraction and Ion Exchange; Journal ID: ISSN 0736-6299
- Publisher:
- Taylor and Francis
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zarzana, Christopher A., Groenewold, Gary S., Mincher, Bruce J., Mezyk, Stephen P., Wilden, Andreas, Schmidt, Holger, Modolo, Giuseppe, Wishart, James F., and Cook, Andrew R. A comparison of the y-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, Christopher A., Groenewold, Gary S., Mincher, Bruce J., Mezyk, Stephen P., Wilden, Andreas, Schmidt, Holger, Modolo, Giuseppe, Wishart, James F., & Cook, Andrew R. A comparison of the y-Radiolysis of TODGA and T(EH)DGA using UHPLC-ESI-MS analysis. United States. https://doi.org/10.1080/07366299.2015.1012885
Zarzana, Christopher A., Groenewold, Gary S., Mincher, Bruce J., Mezyk, Stephen P., Wilden, Andreas, Schmidt, Holger, Modolo, Giuseppe, Wishart, James F., and Cook, Andrew R. Mon .
"A comparison of the y-Radiolysis of TODGA and T(EH)DGA using UHPLC-ESI-MS analysis". United States. https://doi.org/10.1080/07366299.2015.1012885. https://www.osti.gov/servlets/purl/1184759.
@article{osti_1184759,
title = {A comparison of the y-Radiolysis of TODGA and T(EH)DGA using UHPLC-ESI-MS analysis},
author = {Zarzana, Christopher A. and Groenewold, Gary S. and Mincher, Bruce J. and Mezyk, Stephen P. and Wilden, Andreas and Schmidt, Holger and Modolo, Giuseppe and Wishart, James F. and Cook, Andrew R.},
abstractNote = {Solutions of the diglycolamide extractants TODGA and T(EH)DGA in n-dodecane were subjected to γ- irradiation in the presence and absence of an acidic aqueous phase. These solutions were then analyzed using UHPLC-ESI-MS to determine the rates of radiolytic decay of the two extractants neat and in contact with respect to the acidity of the contacted aqueous phase, as well as to identify radiolysis products. The presence or absence of an acidic aqueous phase was shown to have no influence on the measured decay rates, nor did the side-chain have an influence. A number of radiolysis products were identified, consistent with those previously identified for these two compounds using GC-MS. The identity of these radiolysis products suggests that the bonds most vulnerable to radiolytic attack are those in the dyglycolamide center of these molecules, and not on the side-chains. The agreement of these results with previous work using GC-MS indicates supports the further use of UHPLC-ESI-MS as a tool for studying diglycolamide extractant systems.},
doi = {10.1080/07366299.2015.1012885},
journal = {Solvent Extraction and Ion Exchange},
number = ,
volume = ,
place = {United States},
year = {Mon Apr 27 00:00:00 EDT 2015},
month = {Mon Apr 27 00:00:00 EDT 2015}
}
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Figures / Tables:
Figure 1: Structures of the two diglycolamides studied here: a. N,N,N’,N’‐tetraoctyldiglycolamide (TODGA) and b. N,N,N’,N’‐tetra‐2‐ethylhexyldiglycolamide (T(EH)DGA).
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Works referencing / citing this record:
Evaluation of the impacts of gamma radiolysis on an ALSEP process solvent
journal, February 2018
- Peterman, Dean R.; Zarzana, Christopher A.; Tillotson, Richard D.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 316, Issue 2
Radiolytic degradation of hydrophilic PyTri ligands for minor actinide recycling
journal, September 2019
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- Journal of Radioanalytical and Nuclear Chemistry, Vol. 322, Issue 3
A Study of the γ-Radiolysis of N,N -Didodecyl- N′,N′ -Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis
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Radiation chemistry of the branched-chain monoamide di-2-ethylhexyl-isobutyramide
journal, September 2017
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- Solvent Extraction and Ion Exchange, Vol. 35, Issue 7
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides
journal, June 2018
- Wilden, Andreas; Mincher, Bruce J.; Mezyk, Stephen P.
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Gamma Radiolysis of TODGA and CyMe 4 BTPhen in the Ionic Liquid Tri- n -Octylmethylammonium Nitrate
journal, January 2020
- Zsabka, Peter; Van Hecke, Karen; Wilden, Andreas
- Solvent Extraction and Ion Exchange, Vol. 38, Issue 2
Radiation chemistry of the branched-chain monoamide di-2-ethylhexyl-isobutyramide
text, January 2017
- Drader, J.; Saint-Louis, G.; Muller, J. M.
- Taylor & Francis
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides
text, January 2018
- Wilden, Andreas; Mincher, Bruce J.; Mezyk, Stephen P.
- Taylor & Francis
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides
text, January 2018
- Wilden, Andreas; Mincher, Bruce J.; Mezyk, Stephen P.
- Taylor & Francis
Radiation chemistry of the branched-chain monoamide di-2-ethylhexyl-isobutyramide
text, January 2017
- Drader, J.; Saint-Louis, G.; Muller, J. M.
- Taylor & Francis
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides
text, January 2018
- Wilden, Andreas; Mincher, Bruce J.; Mezyk, Stephen P.
- Taylor & Francis
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