A Study of the γ-Radiolysis of N,N-Didodecyl-N',N'-Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis
Abstract
In this paper, solutions of N,N-didodecyl-N',N'-dioctyldiglycolamide in n-dodecane were subjected to γ-irradiation in the presence and absence of both an aqueous nitric acid phase and air sparging. The solutions were analyzed using ultra-high-performance liquid chromatography-electrospray ionization-mass spectrometry (UHPLC-ESI-MS) to determine the rates of radiolytic decay of the extractant as well as to identify radiolysis products. The DGA concentration decreased exponentially with increasing dose, and the measured degradation rate constants were uninfluenced by the presence or absence of acidic aqueous phase, or by air sparging. Finally, the identified radiolysis products suggest that the bonds most vulnerable to radiolytic attack are those in the diglycolamide center of these molecules and not in the side chains.
- Authors:
-
- Idaho National Lab. (INL), Idaho Falls, ID (United States)
- Forschungszentrum Julich (Germany)
- Publication Date:
- Research Org.:
- Idaho National Lab. (INL), Idaho Falls, ID (United States); Forschungszentrum Juelich (Germany)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5); European Commission (EC)
- OSTI Identifier:
- 1367875
- Report Number(s):
- INL/JOU-15-37316
Journal ID: ISSN 0736-6299
- Grant/Contract Number:
- AC07-05ID14517; FP7-Fission-2012-323-282
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Solvent Extraction and Ion Exchange
- Additional Journal Information:
- Journal Volume: 34; Journal Issue: 5; Journal ID: ISSN 0736-6299
- Publisher:
- Taylor and Francis
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; diglycolamide; UHPLC-MS; radiolysis; D3DODGA; radiation chemistry
Citation Formats
Roscioli-Johnson, Kristyn M., Zarzana, Christopher A., Groenewold, Gary S., Mincher, Bruce J., Wilden, Andreas, Schmidt, Holger, Modolo, Giuseppe, and Santiago-Schübel, Beatrix. A Study of the γ-Radiolysis of N,N-Didodecyl-N',N'-Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis. United States: N. p., 2016.
Web. doi:10.1080/07366299.2016.1212540.
Roscioli-Johnson, Kristyn M., Zarzana, Christopher A., Groenewold, Gary S., Mincher, Bruce J., Wilden, Andreas, Schmidt, Holger, Modolo, Giuseppe, & Santiago-Schübel, Beatrix. A Study of the γ-Radiolysis of N,N-Didodecyl-N',N'-Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis. United States. https://doi.org/10.1080/07366299.2016.1212540
Roscioli-Johnson, Kristyn M., Zarzana, Christopher A., Groenewold, Gary S., Mincher, Bruce J., Wilden, Andreas, Schmidt, Holger, Modolo, Giuseppe, and Santiago-Schübel, Beatrix. Tue .
"A Study of the γ-Radiolysis of N,N-Didodecyl-N',N'-Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis". United States. https://doi.org/10.1080/07366299.2016.1212540. https://www.osti.gov/servlets/purl/1367875.
@article{osti_1367875,
title = {A Study of the γ-Radiolysis of N,N-Didodecyl-N',N'-Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis},
author = {Roscioli-Johnson, Kristyn M. and Zarzana, Christopher A. and Groenewold, Gary S. and Mincher, Bruce J. and Wilden, Andreas and Schmidt, Holger and Modolo, Giuseppe and Santiago-Schübel, Beatrix},
abstractNote = {In this paper, solutions of N,N-didodecyl-N',N'-dioctyldiglycolamide in n-dodecane were subjected to γ-irradiation in the presence and absence of both an aqueous nitric acid phase and air sparging. The solutions were analyzed using ultra-high-performance liquid chromatography-electrospray ionization-mass spectrometry (UHPLC-ESI-MS) to determine the rates of radiolytic decay of the extractant as well as to identify radiolysis products. The DGA concentration decreased exponentially with increasing dose, and the measured degradation rate constants were uninfluenced by the presence or absence of acidic aqueous phase, or by air sparging. Finally, the identified radiolysis products suggest that the bonds most vulnerable to radiolytic attack are those in the diglycolamide center of these molecules and not in the side chains.},
doi = {10.1080/07366299.2016.1212540},
journal = {Solvent Extraction and Ion Exchange},
number = 5,
volume = 34,
place = {United States},
year = {Tue Jul 12 00:00:00 EDT 2016},
month = {Tue Jul 12 00:00:00 EDT 2016}
}
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Works referenced in this record:
Influence of diluent on radiolysis of amides in organic solution
journal, May 2007
- Sugo, Yumi; Izumi, Yoshinobu; Yoshida, Yoichi
- Radiation Physics and Chemistry, Vol. 76, Issue 5
Studies on hydrolysis and radiolysis of N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide
journal, January 2002
- Sugo, Y.; Sasaki, Y.; Tachimori, S.
- Radiochimica Acta, Vol. 90, Issue 3
Feasibility of Using Di-Dodecyl-Di-Octyl Diglycolamide for Partitioning of Minor Actinides from Fast Reactor High-Level Liquid Waste
journal, May 2014
- Ravi, Jammu; Venkatesan, K. A.; Antony, M. P.
- Solvent Extraction and Ion Exchange, Vol. 32, Issue 4
MODIFICATION OF TODGA- n -DODECANE SOLVENT WITH A MONOAMIDE FOR HIGH LOADING OF LANTHANIDES(III) AND ACTINIDES(III)
journal, January 2002
- Tachimori, Shoichi; Sasaki, Yuji; Suzuki, Shin-ichi
- Solvent Extraction and Ion Exchange, Vol. 20, Issue 6
Aqueous Partitioning of Minor Actinides by Different Processes
journal, February 2011
- Ansari, Seraj A.; Pathak, Priyanath; Mohapatra, Prashanta K.
- Separation & Purification Reviews, Vol. 40, Issue 1
Demonstration of trivalent actinide partitioning from simulated high-level liquid waste using modifier-free unsymmetrical diglycolamide in n-dodecane
journal, January 2015
- Nayak, P. K.; Kumaresan, R.; Chaurasia, Shivkumar
- Radiochimica Acta, Vol. 103, Issue 5
Impact limits of partitioning and transmutation scenarios on the radiotoxicity of actinides in radioactive waste
journal, October 2003
- Magill, J.; Berthou, V.; Haas, D.
- Nuclear Energy, Vol. 42, Issue 5
Tuning the diglycolamides for modifier-free minor actinide partitioning
journal, July 2012
- Ravi, Jammu; Venkatesan, K. A.; Antony, M. P.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 295, Issue 2
Review Article: The Effects of Radiation Chemistry on Solvent Extraction 3: A Review of Actinide and Lanthanide Extraction
journal, December 2009
- Mincher, Bruce J.; Modolo, Giuseppe; Mezyk, Stephen P.
- Solvent Extraction and Ion Exchange, Vol. 27, Issue 5-6
Chemistry of Diglycolamides: Promising Extractants for Actinide Partitioning
journal, November 2011
- Ansari, Seraj A.; Pathak, Priyanath; Mohapatra, Prasanta K.
- Chemical Reviews, Vol. 112, Issue 3
A Comparison of the γ -Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis
journal, March 2015
- Zarzana, Christopher A.; Groenewold, Gary S.; Mincher, Bruce J.
- Solvent Extraction and Ion Exchange, Vol. 33, Issue 5
Demonstration of a TODGA‐Based Continuous Counter‐Current Extraction Process for the Partitioning of Actinides from a Simulated PUREX Raffinate, Part II: Centrifugal Contactor Runs
journal, January 2008
- Modolo, Giuseppe; Asp, Hanna; Vijgen, Hendrik
- Solvent Extraction and Ion Exchange, Vol. 26, Issue 1
Synthesis of some N,N,N′,N′‐Tetraalkyl‐3‐Oxa‐Pentane‐1,5‐Diamide and their Applications in Solvent Extraction
journal, February 2007
- Mowafy, E. A.; Aly, H. F.
- Solvent Extraction and Ion Exchange, Vol. 25, Issue 2
Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling
journal, January 2015
- Galán, Hitos; Zarzana, Christopher A.; Wilden, Andreas
- Dalton Transactions, Vol. 44, Issue 41
Radiolytic Stability of TODGA: Characterization of Degraded Samples under Different Experimental Conditions
journal, January 2012
- Galán, Hitos; Núñez, Ana; Espartero, Amparo G.
- Procedia Chemistry, Vol. 7
Extraction Capacity of Diglycolamide Derivatives for Ca(II), Nd(III) and Zr(IV) from Nitric Acid to n-Dodecane Containing a Solvent Modifier
journal, January 2005
- Sasaki, Yuji; Zhu, Zhi-Xuan; Sugo, Yumi
- Analytical Sciences, Vol. 21, Issue 10
Extraction Behavior of Some Actinides and Fission Products from Nitric Acid Medium by a New Unsymmetrical Diglycolamide
journal, January 2011
- Ravi, Jammu; Suneesh, A. S.; Prathibha, T.
- Solvent Extraction and Ion Exchange, Vol. 29, Issue 1
Use of Soft Heterocyclic N-Donor Ligands To Separate Actinides and Lanthanides
journal, June 2012
- Hudson, Michael J.; Harwood, Laurence M.; Laventine, Dominic M.
- Inorganic Chemistry, Vol. 52, Issue 7
Hydrolysis and Radiation Stability of m-Xylylene Bis-diglycolamide: Synthesis and Quantitative Study of Degradation Products by HPLC-APCI+
journal, June 2011
- Galán, Hitos; Murillo, María Teresa; Sedano, Rosa
- European Journal of Organic Chemistry, Vol. 2011, Issue 20-21
The Radiation Chemistry of CMPO: Part 1. Gamma Radiolysis
journal, September 2013
- Mincher, Bruce J.; Mezyk, Stephen P.; Elias, Gracy
- Solvent Extraction and Ion Exchange, Vol. 31, Issue 7
Use of Polyaminocarboxylic Acids as Hydrophilic Masking Agents for Fission Products in Actinide Partitioning Processes
journal, November 2012
- Sypula, Michal; Wilden, Andreas; Schreinemachers, Christian
- Solvent Extraction and Ion Exchange, Vol. 30, Issue 7
Demonstration of a TODGA based Extraction Process for the Partitioning of Minor Actinides from a PUREX Raffinate: Part III: Centrifugal Contactor Run using Genuine Fuel Solution
journal, January 2009
- Magnusson, Daniel; Christiansen, Birgit; Glatz, Jean‐Paul
- Solvent Extraction and Ion Exchange, Vol. 27, Issue 1
Hydrolytic and Radiolytic Degradation of Oφd(iB)Cmpo: Continuing Studies
journal, October 1988
- Nash, K. L.; Gatrone, R. C.; Clark, G. A.
- Separation Science and Technology, Vol. 23, Issue 12-13
THE NOVEL EXTRACTANTS, DIGLYCOLAMIDES, FOR THE EXTRACTION OF LANTHANIDES AND ACTINIDES IN HNO 3 – n -DODECANE SYSTEM
journal, January 2001
- Sasaki, Yuji; Sugo, Yumi; Suzuki, Shinichi
- Solvent Extraction and Ion Exchange, Vol. 19, Issue 1
Radiolytic Stability of N,N,N ′ ,N ′-Tetraoctyl Diglycolamide (TODGA) in the Presence of Phase Modifiers Dissolved in n -Dodecane
journal, May 2012
- Gujar, R. B.; Ansari, S. A.; Bhattacharyya, A.
- Solvent Extraction and Ion Exchange, Vol. 30, Issue 3
A method for the determination of extraction capacity and its application to N,N,N′,N′-tetraalkylderivatives of diglycolamide-monoamide/n-dodecane media
journal, July 2005
- Sasaki, Yuji; Sugo, Yumi; Suzuki, Shinichi
- Analytica Chimica Acta, Vol. 543, Issue 1-2
Development of a TODGA based Process for Partitioning of Actinides from a PUREX Raffinate Part I: Batch Extraction Optimization Studies and Stability Tests
journal, October 2007
- Modolo, Giuseppe; Asp, Hanna; Schreinemachers, Christian
- Solvent Extraction and Ion Exchange, Vol. 25, Issue 6
Evaluation of radiation stability of N,N-didodecyl N′,N′-di-octyl diglycolamide: a promising reagent for actinide partitioning
journal, October 2013
- Ravi, Jammu; Robert Selvan, B.; Venkatesan, K. A.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 299, Issue 1
A Comparison of the γ-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis
text, January 2015
- Zarzana, Christopher A.; Groenewold, Gary S.; Mincher, Bruce J.
- Taylor & Francis
A Comparison of the γ-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis
text, January 2015
- Zarzana, Christopher A.; Groenewold, Gary S.; Mincher, Bruce J.
- Taylor & Francis
Works referencing / citing this record:
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journal, February 2018
- Peterman, Dean R.; Zarzana, Christopher A.; Tillotson, Richard D.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 316, Issue 2
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journal, September 2017
- Drader, J.; Saint-Louis, G.; Muller, J. M.
- 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.
- Solvent Extraction and Ion Exchange, Vol. 36, Issue 4
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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