Influence of radiation effect on extractability of an isobutyl-BTP/ionic liquid system: quantitative analysis and identification of radiolytic products

Yuan, Wei; Ao, Yinyong; Zhao, L.; Zhai, Maolin; Peng, Jing; Li, Jiuqiang; Wei, Yuezhou

doi:10.1039/c4ra08308c

Cited by 14 publications

(4 citation statements)

References 30 publications

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“…13 Moreover, it has been, recently, reported that the R-BTP based extraction system is more radiation resistant in RTIL medium as compared to that in molecular solvents. 14 It is, therefore, important to explore the use of RTILs for process applications using radioactive elements with better recycling possibilities. Cocalia et al 15 have observed similar extraction and complexation behaviour of various actinide and lanthanide ions with dialkyl phosphoric and phosphinic acids in RTIL and molecular diluents.…”

Section: Introductionmentioning

confidence: 99%

A remarkable enhancement in Am³⁺/Eu³⁺selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

et al. 2015

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Mutual separation of trivalent actinide (An(3+)) and lanthanide (Ln(3+)) using several soft (N) donor ligands (bis(5,6-dialkyl-1,2,4-triazinyl)pyridine (R-BTP)) is attempted for the first time in room temperature ionic liquid (RTIL) medium. The results indicate a spectacular enhancement in the selectivity as compared to that in molecular diluents with a separation factor (S.F.) of >3000 for Am(3+) over Eu(3+) using the methyl derivative (Me-BTP) in RTIL medium using [C(n)mim]·[NTf2] as the diluents (where n = 2, 3, 4, 6 or 8). Such a high S.F. value has never been reported before with any of the R-BTP derivatives in molecular diluents. An opposite trend in the distribution ratio values of both Am(3+) and Eu(3+) with the increasing size of the alkyl (R) group is observed in RTIL medium when compared with that in molecular diluents. The differences in the extraction behaviour of R-BTPs in RTILs vis-à-vis molecular diluents are explained on the basis of the difference in the nature of complexes extracted in these two distinctly different media as supported by the time resolved fluorescence (TRFS) study. An unusually high extractability and selectivity for Am(3+) over Eu(3+) with Me-BTP was attributed to the formation of a 1 : 4 complex for Am(3+), which was never reported earlier with any of the R-BTP derivatives in molecular diluents. DFT studies indicated higher metal 'd' and 'f' orbital participation (covalence) in the bonding with R-BTP in the case of Am(3+) complexes as compared to that in the case of Eu(3+) complexes, which resulted in the selectivity of these classes of ligands. The observed results may have a great significance in the radioactive waste management involving the partitioning and transmutation strategy.

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Section: Introductionmentioning

confidence: 99%

A remarkable enhancement in Am³⁺/Eu³⁺selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

et al. 2015

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“…In the case of liquid–liquid extraction using BTP derivatives, radiation-induced degradation of the extractant is mainly facilitated by the diluents . The degradation of i Bu-BTP was found to be much higher in the 1-octanol medium than in the room-temperature ionic-liquid (RTIL) medium, as 1-octanol produced free radicals more easily under gamma irradiation .…”

Section: Resultsmentioning

confidence: 99%

“…In the case of liquid−liquid extraction using BTP derivatives, radiation-induced degradation of the extractant is mainly facilitated by the diluents. 49 The degradation of iBu-BTP was found to be much higher in the 1-octanol medium than in the room-temperature ionic-liquid (RTIL) medium, as 1-octanol produced free radicals more easily under gamma irradiation. 47 Even with the hydrophilic BTP derivative (SO 3 PhBTP), the separation behavior deteriorated significantly at a radiation dose of 300 kGy beyond which the extraction of americium was found to have increased by an order of 2.…”

Section: Stability Of the Materialmentioning

confidence: 99%

First Report on a 1-Cycle Solid-Phase Extraction Method for Selective Separation of Am³⁺ and Eu³⁺: Use of BTP-Grafted Silica Decorated on Activated Carbon

Ansari,

Gujar,

Bhattacharyya

et al. 2024

Ind. Eng. Chem. Res.

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A new composite sorbent material was prepared by grafting bistriazinylpyridine (BTP) onto silica and then blending it with activated charcoal (AC− Si−BTP) for the selective separation of Am 3+ over Eu 3+ using a 1-cycle solid-phase extraction for the direct separation of lanthanides from actinides. BTP was attached to silica via a sulfonamide bond between R−BTP and amino silane, and the resulting Si− BTP was covalently bonded to activated carbon (AC) with a favorable orientation of the ligand coordination sites. The material exhibited a significantly large distribution coefficient for Am 3+ over Eu 3+ at lower acidities (<0.5 M HNO 3 ), and the separation factor between the two metal ions was found to be maximum in 0.2 M HNO 3 with a value of 110. The loading capacity of the material was 4.05 ± 0.12 mg of Eu per gram of the composite when investigated at pH 3. The radiation stability of the material was excellent when studied up to an absorbed dose of 1000 kGy. The material was tested for the separation of Am 3+ and Eu 3+ in a column mode, which gave selective loading of Am 3+ over Eu 3+ . The reusability studies indicated slow leaching of the BTP fraction from the solid, with a resultant decrease of the K d values with time. To address this issue, the material was embedded in polysulfone beads for a separate set of studies, but the separation efficiencies were found to be comparable.

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“…The results showed that [C 2 mim][NTf 2 ] provided radioprotection for isobutyl-BTP comparing 1-octanolas a conjugated system was formed between isobutyl-BTP and imidazoliumcation. 28,29 However, as far as our best knowledge is concerned, few work focused on the radiation effect on the extractability of TODGA in RTILs.…”

Section: Introductionmentioning

confidence: 99%

γ-Radiation effect on Th⁴⁺ extraction behaviour of TODGA/[C₂mim][NTf₂]: identification and extractability study of radiolytic products

Yuan

Wang

et al. 2016

RSC Adv.

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Influence of radiation effect on extractability of an isobutyl-BTP/ionic liquid system: quantitative analysis and identification of radiolytic products

Abstract: Approaches were established for assessing the influence of radiation effect on the extractability of the 2,6-di(5,6-diisobutyl-1,2,4-triazin-3-yl)pyridine (isobutyl-BTP)/1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide ([C2mim][NTf2]) extraction system.

Cited by 14 publications

References 30 publications

A remarkable enhancement in Am³⁺/Eu³⁺selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

A remarkable enhancement in Am³⁺/Eu³⁺selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

First Report on a 1-Cycle Solid-Phase Extraction Method for Selective Separation of Am³⁺ and Eu³⁺: Use of BTP-Grafted Silica Decorated on Activated Carbon

γ-Radiation effect on Th⁴⁺ extraction behaviour of TODGA/[C₂mim][NTf₂]: identification and extractability study of radiolytic products

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Influence of radiation effect on extractability of an isobutyl-BTP/ionic liquid system: quantitative analysis and identification of radiolytic products

Abstract: Approaches were established for assessing the influence of radiation effect on the extractability of the 2,6-di(5,6-diisobutyl-1,2,4-triazin-3-yl)pyridine (isobutyl-BTP)/1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) imide ([C2mim][NTf2]) extraction system.

Cited by 14 publications

References 30 publications

A remarkable enhancement in Am3+/Eu3+selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

A remarkable enhancement in Am3+/Eu3+selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

First Report on a 1-Cycle Solid-Phase Extraction Method for Selective Separation of Am3+ and Eu3+: Use of BTP-Grafted Silica Decorated on Activated Carbon

γ-Radiation effect on Th4+ extraction behaviour of TODGA/[C2mim][NTf2]: identification and extractability study of radiolytic products

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A remarkable enhancement in Am³⁺/Eu³⁺selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

A remarkable enhancement in Am³⁺/Eu³⁺selectivity by an ionic liquid based solvent containing bis-1,2,4-triazinyl pyridine derivatives: DFT validation of experimental results

First Report on a 1-Cycle Solid-Phase Extraction Method for Selective Separation of Am³⁺ and Eu³⁺: Use of BTP-Grafted Silica Decorated on Activated Carbon

γ-Radiation effect on Th⁴⁺ extraction behaviour of TODGA/[C₂mim][NTf₂]: identification and extractability study of radiolytic products