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Title: Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling

Journal Article · · Dalton Transactions
DOI:https://doi.org/10.1039/C5DT02484F· OSTI ID:1294500
 [1];  [2];  [3];  [1];  [3];  [4];  [4];  [1];  [4];  [3];  [2];  [2]
  1. Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas (CIEMAT), Madrid (Spain)
  2. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  3. Forschungszentrum Julich GmbH, Institut fur Energie-und Klimaforschung -Nukleare Entsorgung und Reaktorsicherheit (IEK), Julich (Germany)
  4. Univ. of Twente, Enschede (The Netherlands)

The stability against gamma radiation of MeTODGA (methyl tetraoctyldiglycolamide) and Me2TODGA (dimethyl tetraoctyldiglycolamide), derivatives from the well-known extractant TODGA (N,N,N',N';-tetraoctyldiglycolamide), were studied and compared. Solutions of MeTODGA and Me2TODGA in alkane diluents were subjected to 60Co γ-irradiation in the presence and absence of nitric acid and analyzed using LC-MS to determine their rates of radiolytic concentration decrease, as well as to identify radiolysis products. The results of product identification from three different laboratories are compared and found to be in good agreement. The diglycolamide (DGA) concentrations decreased exponentially with increasing absorbed dose. The MeTODGA degradation rate constants (dose constants) were uninfluenced by the presence of nitric acid, but the acid increased the rate of degradation for Me2TODGA. The degradation products formed by irradiation are also initially produced in greater amounts in acid-contacted solution, but products may also be degraded by continued radiolysis. As a result, the identified radiolysis products suggest that the weakest bonds are those in the diglycolamide center of these molecules.

Research Organization:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC07-05ID14517
OSTI ID:
1294500
Report Number(s):
INL/JOU-15-35577; ICHBD9
Journal Information:
Dalton Transactions, Vol. 44, Issue 41; ISSN 1477-9226
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 36 works
Citation information provided by
Web of Science

References (29)

Assessment of the environmental footprint of nuclear energy systems. Comparison between closed and open fuel cycles journal May 2014
A review of the demonstration of innovative solvent extraction processes for the recovery of trivalent minor actinides from PUREX raffinate journal August 2012
Direct Selective Extraction of Actinides (III) from PUREX Raffinate using a Mixture of CyMe 4 BTBP and TODGA as 1-cycle SANEX Solvent Part III: Demonstration of a Laboratory-Scale Counter-Current Centrifugal Contactor Process journal March 2013
Laboratory-Scale Counter-Current Centrifugal Contactor Demonstration of an Innovative-SANEX Process Using a Water Soluble BTP journal October 2014
The Actinide-Lanthanide Separation Concept journal May 2014
Implementation of Americium Separation from a PUREX Raffinate journal January 2012
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
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
Plutonium Loading of Prospective Grouped Actinide Extraction (GANEX) Solvent Systems based on Diglycolamide Extractants journal March 2012
Development of a New Flowsheet for Co-Separating the Transuranic Actinides: The “EURO-GANEX” Process journal June 2014
ACSEPT—Partitioning technologies and actinide science: Towards pilot facilities in Europe journal September 2011
Synthesis and Am/Eu extraction of novel TODGA derivatives journal August 2010
Modified Diglycolamides for the An(III) + Ln(III) Co-separation: Evaluation by Solvent Extraction and Time-Resolved Laser Fluorescence Spectroscopy journal January 2014
Influence of diluent on radiolysis of amides in organic solution journal May 2007
Radiolytic Stability of TODGA: Characterization of Degraded Samples under Different Experimental Conditions journal January 2012
A Comparison of the γ -Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis journal March 2015
Review: The Effects of Radiation Chemistry on Solvent Extraction 4: Separation of the Trivalent Actinides and Considerations for Radiation-Resistant Solvent Systems journal June 2010
Comparative evaluation of two substituted diglycolamide extractants for ‘actinide partitioning’ journal February 2010
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 hydrolysis and radiolysis of N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide journal January 2002
Hydrolysis and Radiation Stability of m-Xylylene Bis-diglycolamide: Synthesis and Quantitative Study of Degradation Products by HPLC-APCI+ journal June 2011
Studies on hydrolytic and radiolytic stability of N , N , N ´, N ´-tetra-(2-ethylhexyl) thiodiglycolamide T(2EH)TDGA 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
Considerations for choice of a kinetic fig. of merit in process radiation chemistry for waste treatment journal February 2000
Extraction of Nitric Acid into Alcohol: Kerosene Mixtures journal August 2010
The Radiation Chemistry of CMPO: Part 1. Gamma Radiolysis journal September 2013
Diamex Process for Minor Actinide Partitioning: Hydrolytic and Radiolytic Degradations of Malonamide Extractants journal June 2001
Development and use of quantum mechanical molecular models. 76. AM1: a new general purpose quantum mechanical molecular model journal June 1985

Cited By (15)

Unprecedented Inversion of Selectivity and Extraordinary Difference in the Complexation of Trivalent f  Elements by Diastereomers of a Methylated Diglycolamide journal March 2019
Application of quantum mechanical simulations for studying the radiolytic stability of prospective extractants in the nuclear fuel cycle journal October 2018
Radiolytic degradation of hydrophilic PyTri ligands for minor actinide recycling journal September 2019
Ligands for f-element extraction used in the nuclear fuel cycle journal January 2017
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
Actinide–lanthanide co-extraction by rigidified diglycolamides journal December 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
Actinide–lanthanide co-extraction by rigidified diglycolamides text January 2017
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides text January 2018

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