Experimental and modelling study of ruthenium extraction with tri-n-butylphosphate in the purex process

Moeyaert, P.; Miguirditchian, Manuel; Masson, M.; Dinh, Binh; Hérès, Xavier; Sio, S. de; Sorel, C.

doi:10.1016/j.ces.2016.10.035

Cited by 26 publications

(20 citation statements)

References 14 publications

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“…Hence, the fractions of Zr, Pd and Ag which were extracted in the extraction section were not backextracted in the scrubbing section. Ruthenium is known to have a very complex behaviour with a range of species present in nitric acid and is difficult to decontaminate in the PUREX process [43]. Similar behaviour was observed in other processes using TODGA [44][45] or DMDOHEMA [46][47] and hence is suspected in the EURO-GANEX solvent system.…”

Section: Part 1 Preparation Of the Loaded Solventsupporting

confidence: 52%

Homogenous recycling of transuranium elements from irradiated fast reactor fuel by the EURO-GANEX solvent extraction process

et al. 2019

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The EURO-GANEX process was developed for co-separating transuranium elements from irradiated nuclear fuels. A hot flow-sheet trial was performed in a counter-current centrifugal contactor setup, using a genuine high active feed solution. Irradiated mixed (carbide, nitride) U80Pu20 fast reactor fuel containing 20 % Pu was thermally treated to oxidise it to the oxide form which was then dissolved in HNO3. From this solution uranium was separated to >99.9 % in a primary solvent extraction cycle using 1.0 mol/L DEHiBA (N,N-di(2-ethylhexyl)isobutyramide in TPH (hydrogenated tetrapropene) as the organic phase. The raffinate solution from this process, containing 10 g/L Pu, was further processed in a second cycle of solvent extraction. In this EURO-GANEX flow-sheet, TRU and fission product lanthanides were firstly co-extracted into a solvent composed of 0.2 mol/L TODGA (N,N,N′,N′-tetra-n-octyl diglycolamide) and 0.5 mol/L DMDOHEMA (N,N′-dimethyl-N,N′-dioctyl-2-(2-hexyloxy-ethyl) malonamide) dissolved in Exxsol D80, separating them from most other fission and corrosion products. Subsequently, the TRU were selectively stripped from the collected loaded solvent using a solution containing 0.055 mol/L SO3-Ph-BTP (2,6-bis(5,6-di(3-sulphophenyl)-1,2,4-triazin-3-yl)pyridine tetrasodium salt) and 1 mol/L AHA (acetohydroxamic acid) in 0.5 mol/L HNO3; lanthanides were finally stripped using 0.01 mol/L HNO3. Approximately 99.9 % of the TRU and less than 0.1 % of the lanthanides were found in the product solution, which also contained the major fractions of Zr and Mo.

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Section: Part 1 Preparation Of the Loaded Solventsupporting

confidence: 52%

Homogenous recycling of transuranium elements from irradiated fast reactor fuel by the EURO-GANEX solvent extraction process

et al. 2019

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“…One major contributor to radiolysis is the fission product ruthenium, particularly the β and γ radiation in the decay chain of the isotope 106 Ru ( T 1/2 = 374 d). , Some species of the fission product ruthenium can be coextracted in solvent extraction processes. Co-extracted ruthenium challenges solvent purification cycles, which are designed to ensure a high purity of recovered uranium and plutonium/or neptunium, americium, and curium. , …”

Section: Introductionmentioning

confidence: 99%

Ruthenium Nitrosyl Structure in Solvent Extraction Systems: A Comparison of Tributyl Phosphate, Tetrabutyl Urea, N-Methyl, N-Octyl Ethylhexanamide, and N,N,N′,N′-Tetraoctyl Diglycolamide

Dirks

Dumas

Solari

et al. 2019

Ind. Eng. Chem. Res.

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In the course of nuclear fuel treatment, solvent extraction cycles separate uranium and plutonium from fission products and minor actinides. During these steps, small amounts of the fission product ruthenium may follow the uranium and plutonium products. Herein, we show by Raman spectroscopy how ruthenium complexes in the aqueous phase differ as a function of the nitric acid concentration. Furthermore, we compare ruthenium extraction by the industrially used solvent tri-n-butylphosphate to other extractants such as tetrabutyl urea, N-methyl, N-octyl ethylhexanamide, and N,N,N′,N′-tetraoctyl diglycolamide. Analysis by inductively coupled plasma atomic emission spectroscopy demonstrates that all of these solvents have different ruthenium distribution ratios. In contrast, similar ruthenium complexes were identified by Fourier transform infrared and extended X-ray absorption fine structure spectroscopy in all extractions from 4 M nitric acid. Hence, different distribution ratios of ruthenium are not due to different ruthenium complexes. By comparing ruthenium extraction with nitric acid and water extraction, we show a linear correlation between ruthenium and water concentration in the organic phase. This suggests an interaction between the solvent and water ligands during ruthenium extraction. To limit the ruthenium coextraction in nuclear fuel treatments, we suggest further investigation of solvents with low water coextraction.

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“…Alkyl‐phosphate has been widely used for many years in industrial processes such as solvent extraction, heavy metal ion reagent, plasticizer, lubricant, surfactant, corrosion inhibitor, etc . Tri‐n‐butyl phosphate (TBP) is one of the alkyl‐phosphates and has been used as an extractant in the PUREX process for the separation of uranium and plutonium from irradiated nuclear fuel over the last six decades . At present, TBP is also used to extract important raw materials zirconium and hafnium in the atomic energy industry .…”

Section: Introductionmentioning

confidence: 99%

“…[1][2][3][4][5][6][7] Tri-n-butyl phosphate (TBP) is one of the alkyl-phosphates and has been used as an extractant in the PUREX process for the separation of uranium and plutonium from irradiated nuclear fuel over the last six decades. 8,9 At present, TBP is also used to extract important raw materials zirconium and hafnium in the atomic energy industry. 10 In addition, TBP has also been widely used as an extractant for the extraction of various acids.…”

Section: Introductionmentioning

confidence: 99%

Intensification of esterification process in TBP synthesis by in situ vapor stripping

Zhang

Jin

et al. 2019

J of Chemical Tech & Biotech

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BACKGROUND Over the past few decades, tri‐n‐butyl phosphate (TBP) has been a widely used and irreplaceable extractant that can extract a variety of heavy metal ions and inorganic acids. The conventional process of tri‐n‐butyl phosphate synthesis has the problem of low yield. The in situ vapor stripping method was developed to intensify the tri‐n‐butyl phosphate synthesis reaction. RESULTS In this work, the coupling process of in situ vapor stripping and reaction was proposed for the first time in the process of synthesis of TBP. It was found that the reaction of high concentration hydrogen chloride and 1‐butanol would produce water, which resulted in increasing the possibility of side reactions, especially when the temperature was higher than 55 °C. In the lower temperature range, n‐pentane was selected as the stripping medium, which effectively removed hydrogen chloride from the reaction system by in situ vapor stripping. The FT‐IR analysis confirmed that TBP can be synthesized successfully by the vapor stripping process. In addition, the effects of n‐pentane volume, temperature and stripping time on the yield of TBP and the amount of hydrogen chloride stripped were investigated. By applying the optimum reaction conditions, the yield of TBP was increased to 94%, larger than that of the current industrial process whose yield is only 80%. CONCLUSION The in situ vapor stripping process is demonstrated to be an effective method for intensification of the esterification process in TBP synthesis. It can be used for other reactions which generate volatile gases as the byproduct. © 2018 Society of Chemical Industry

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Experimental and modelling study of ruthenium extraction with tri-n-butylphosphate in the purex process

Cited by 26 publications

References 14 publications

Homogenous recycling of transuranium elements from irradiated fast reactor fuel by the EURO-GANEX solvent extraction process

Homogenous recycling of transuranium elements from irradiated fast reactor fuel by the EURO-GANEX solvent extraction process

Ruthenium Nitrosyl Structure in Solvent Extraction Systems: A Comparison of Tributyl Phosphate, Tetrabutyl Urea, N-Methyl, N-Octyl Ethylhexanamide, and N,N,N′,N′-Tetraoctyl Diglycolamide

Intensification of esterification process in TBP synthesis by in situ vapor stripping

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