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

Journal Article · · Solvent Extraction and Ion Exchange

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 Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Organization:
DOE - NE
DOE Contract Number:
DE-AC07-05ID14517
OSTI ID:
1186739
Report Number(s):
INL/JOU-14-32985
Journal Information:
Solvent Extraction and Ion Exchange, Vol. 33, Issue 5; ISSN 0736-6299
Publisher:
Taylor and Francis
Country of Publication:
United States
Language:
English

References (26)

Chemistry of Diglycolamides: Promising Extractants for Actinide Partitioning journal November 2011
THE NOVEL EXTRACTANTS, DIGLYCOLAMIDES, FOR THE EXTRACTION OF LANTHANIDES AND ACTINIDES IN HNO 3n -DODECANE SYSTEM journal January 2001
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
Studies on the use of N,N,N′,N′ -Tetra(2-Ethylhexyl) Diglycolamide (TEHDGA) for Actinide Partitioning II: Investigation on Radiolytic Stability journal March 2011
The Actinide-Lanthanide Separation Concept journal May 2014
Actinide Lanthanide Separation Process—ALSEP journal January 2014
ACSEPT—Partitioning technologies and actinide science: Towards pilot facilities in Europe journal September 2011
Modified Diglycolamides for the An(III) + Ln(III) Co-separation: Evaluation by Solvent Extraction and Time-Resolved Laser Fluorescence Spectroscopy journal January 2014
Synthesis and Am/Eu extraction of novel TODGA derivatives journal August 2010
The Partitioning of Americium and the Lanthanides Using Tetrabutyldiglycolamide (TBDGA) in Octanol and in Ionic Liquid Solution journal November 2012
Complexation and Back Extraction of Various Metals by Water-soluble Diglycolamide journal January 2007
Development and Validation of the EXAm Separation Process for Single Am Recycling journal January 2012
Studies on hydrolysis and radiolysis of N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide journal January 2002
Studies on hydrolysis and radiolysis of tetra(2-ethylhexyl)diglycolamide (TEHDGA)/isodecyl alcohol/n-dodecane solvent system journal January 2010
Influence of diluent on radiolysis of amides in organic solution journal May 2007
Comparative evaluation of two substituted diglycolamide extractants for ‘actinide partitioning’ journal February 2010
Evaluation of radiation stability of N,N-didodecyl N′,N′-di-octyl diglycolamide: a promising reagent for actinide partitioning journal October 2013
Feasibility of Using Di-Dodecyl-Di-Octyl Diglycolamide for Partitioning of Minor Actinides from Fast Reactor High-Level Liquid Waste journal May 2014
Review Article: The Effects of Radiation Chemistry on Solvent Extraction 3: A Review of Actinide and Lanthanide Extraction journal December 2009
The LEAF picosecond pulse radiolysis facility at Brookhaven National Laboratory journal November 2004
Considerations for choice of a kinetic fig. of merit in process radiation chemistry for waste treatment journal February 2000
Radiolytic Stability of TODGA: Characterization of Degraded Samples under Different Experimental Conditions journal January 2012
Radiolytic Stability of N,N,N,N ′-Tetraoctyl Diglycolamide (TODGA) in the Presence of Phase Modifiers Dissolved in n -Dodecane journal May 2012
Diamex Process for Minor Actinide Partitioning: Hydrolytic and Radiolytic Degradations of Malonamide Extractants journal June 2001
The Radiation Chemistry of CMPO: Part 1. Gamma Radiolysis journal September 2013
Femtosecond pulse radiolysis study on geminate ion recombination in n-dodecane journal February 2011

Cited By (13)

Evaluation of the impacts of gamma radiolysis on an ALSEP process solvent journal February 2018
Radiolytic degradation of hydrophilic PyTri ligands for minor actinide recycling journal September 2019
31 P NMR study of the activated radioprotection mechanism of octylphenyl- N , N -diisobutylcarbamoylmethyl phosphine oxide (CMPO) and analogues journal January 2019
Gamma radiolysis of hydrophilic diglycolamide ligands in concentrated aqueous nitrate solution journal January 2019
A Study of the γ-Radiolysis of N,N -Didodecyl- N′,N′ -Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis journal June 2016
Radiation chemistry of the branched-chain monoamide di-2-ethylhexyl-isobutyramide journal September 2017
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides journal June 2018
Gamma Radiolysis of TODGA and CyMe 4 BTPhen in the Ionic Liquid Tri- n -Octylmethylammonium Nitrate journal January 2020
Radiation chemistry of the branched-chain monoamide di-2-ethylhexyl-isobutyramide text January 2017
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides text January 2018
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides text January 2018
Radiation chemistry of the branched-chain monoamide di-2-ethylhexyl-isobutyramide text January 2017
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides text January 2018


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