Review Article: The Effects of Radiation Chemistry on Solvent Extraction: 1. Conditions in Acidic Solution and a Review of TBP Radiolysis

Mincher, Bruce J.; Modolo, Giuseppe; Mezyk, Strephen P.

doi:10.1080/07366290802544767

Cited by 196 publications

(104 citation statements)

References 78 publications

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“…6 Assuming that HDBP is the only radiolysis product formed, the value of -G TBP = -0.119 PmolJ -1 determined in this work agrees well with reported G-values for the production of HDBP which fall in the range of 0.07 -0.12 PmolJ -1 . Since it is known that HMBP is also a degradation product formed via gamma radiolysis of TBP, this assumption is not strictly valid.…”

Section: Discussionsupporting

confidence: 89%

“…The radiation chemistry of the TBP was recently reviewed by Mincher et al. 6 A TBP/n-dodecane flowsheet was modeled as a reference point for the initial test in the radiolysis/hydrolysis loop. The basis for the model was taken from a typical PUREX flowsheet for the recycle of spent light water reactor fuel.…”

Section: Radiolysis Testing Of Tbp/n-dodecane Solvent Systemmentioning

confidence: 99%

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Summary Report on Gamma Radiolysis of TBP/n-dodecane in the Presence of Nitric Acid Using the Radiolysis/Hydrolysis Test Loop

Peterman¹,

Mincher²,

Riddle³

et al. 2010

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Section: Discussionsupporting

confidence: 89%

Section: Radiolysis Testing Of Tbp/n-dodecane Solvent Systemmentioning

confidence: 99%

Summary Report on Gamma Radiolysis of TBP/n-dodecane in the Presence of Nitric Acid Using the Radiolysis/Hydrolysis Test Loop

Peterman¹,

Mincher²,

Riddle³

et al. 2010

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“…The main products of TBP radiolysis are hydrogen, methane and dibutylphosphoric acid (HDBP) with monobutylphosphoric acid (H 2 MBP) and phosphoric acid produced in lesser amount [1], which usually can be removed through alkali washing. The principal impurities of the diluents comprise aliphatic nitro compounds, aliphatic carboxylic acids, aliphatic nitroso compounds, aromatic compounds and ketones and aldehydes [2], some of them are metal complexing agents and are diffi cult to remove from the solvent with alkaline solutions.…”

Section: Introductionmentioning

confidence: 99%

“…The work by Mincher et al [1] as well as the TBP book by Navratil [3] have described most of the processes. Most of the research performed on the degradation of TBP solvents has focused on the identifi cation and measurement of degradation products [4][5][6][7], the degradation mechanisms [8][9][10] and the degradation impact factors, such as diluent [11][12][13], water [14, Infl uence of alpha and gamma radiolysis on Pu retention in the solvent TBP/kerosene 15], nitric acid [16][17][18][19], metal ion [20], atmosphere [21], etc.…”

Section: Introductionmentioning

confidence: 99%

Influence of alpha and gamma radiolysis on Pu retention in the solvent TBP/kerosene

et al. 2014

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Abstract. In light of the issue of radiolysis of the solvent system in PUREX process, alpha and gamma radiation stability of tributyl phosphate (TBP)/kerosene (OK) have been studied in this paper, in which 238 Pu dissolved in the organic phase and 60 Co are selected as alpha and gamma irradiation sources, respectively. The amount of the degradation products not easily removed after the washing process has been measured by the plutonium retention. The effects of the absorbed dose, the TBP volume fraction, the cumulative absorbed dose and the presence of UO 2 2+ and Zr 4+ on the radiolysis of the solvents have been investigated. The results have indicated that the Pu retention increases with the increase of the absorbed dose after alpha or gamma irradiation, and is larger for the solvent containing less TBP. There is competition between UO 2 2+ and Pu 4+ to complex with the degradation products, and Zr 4+ accelerates the radiolysis of the system.

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“…One of the disadvantages of this approach is the process complexity. For example, in the -UREX+1a‖ concept for irradiated fuel recycling, a series of four solvent extraction processes are proposed to partition the fuel into useful products and fission product waste (Mincher et al 2009). The Minor Actinide Separation Sigma Team was established within the Fuel Cycle Research and Development (FCR&D) Program to discover and develop new more efficient methods for separating the TRU elements from the lanthanide elements and for separating americium from curium.…”

Section: Introductionmentioning

confidence: 99%

Sigma Team for Minor Actinide Separation: PNNL FY 2010 Status Report

Lumetta¹,

Sinkov²,

Neiner³

et al. 2010

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SUMMARYWork conducted at Pacific Northwest National Laboratory (PNNL) in FY 2010 addressed two lines of inquiry. The two hypotheses put forth were:1. The extractants from the TRUEX (a) process (CMPO) (b) and from the TALSPEAK (c) process (HDEHP) (d) can be combined into a single process solvent to separate 1) the lanthanides and actinides from acidic high-level waste and 2) the actinides from the lanthanides in a single solvent extraction process. (Note: This combined process will hereafter be referred to as the TRUSPEAK process.) A series of empirical measurements performed (both at PNNL and Argonne National Laboratory) in FY 2009 supported this hypothesis, but also indicated some nuances to the chemistry. Lanthanide/americium separation factors of 12 and higher were obtained with a prototypic TRUSPEAK solvent when extracting the lanthanides from a citrate-buffered DTPA (e) solution. Although the observed separation factors are sufficiently high to design an actinide/lanthanide separation process, a better understanding of the chemistry is expected to lead to improved solvent formulations and improved process performance. Work in FY 2010 focused on understanding the synergistic extraction behavior observed for Nd(III) and Am(III) when extracted into mixtures of CMPO and HDEHP. The interaction between CMPO and HDEHP in dodecane was investigated by 31 P NMR spectroscopy, and an adduct of the type CMPO·HDEHP was found to form. The formation of this adduct will reduce the effective extractant concentrations and must be taken into account when modeling metal ion extraction data in this system. Studies were also initiated to determine the Pitzer parameters for Nd(III) in lactate media.2. Higher oxidation states (e.g., +5 and +6) of Am can be stabilized in solution by complexation with uranophilic ligands, and this chemistry can be exploited to separate Am from Cm. To test this hypothesis, the previously reported stereognostic uranophilic ligands NPB (f) and EETAC (e) were investigated. To assess the potential of these ligands to stabilize pentavalent and hexavalent actinides, stability constants were measured for complexation of these ligands to Nd(III), Np(V), and Pu(VI) in a solvent mixture consisting of 80% methanol/20% water. For comparison, an analogous non-stereognostic ligand, NTA, (f) was also examined. The ligand EETAC showed greater binding affinity for hexavalent Pu versus trivalent Nd by two orders-of-magnitude. Such selectivity was not observed for either NTA or NPB.

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Review Article: The Effects of Radiation Chemistry on Solvent Extraction: 1. Conditions in Acidic Solution and a Review of TBP Radiolysis

Cited by 196 publications

References 78 publications

Summary Report on Gamma Radiolysis of TBP/n-dodecane in the Presence of Nitric Acid Using the Radiolysis/Hydrolysis Test Loop

Summary Report on Gamma Radiolysis of TBP/n-dodecane in the Presence of Nitric Acid Using the Radiolysis/Hydrolysis Test Loop

Influence of alpha and gamma radiolysis on Pu retention in the solvent TBP/kerosene

Sigma Team for Minor Actinide Separation: PNNL FY 2010 Status Report

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