Carrier mediated transport of actinides using hexa–n-hexylnitrilotriacetamide (HHNTA)

Mahanty, Bholanath; Karak, Ananda; Mohapatra, Prasanta K.; Egberink, Richard J.M.; Valsala, T.P.; Sathe, Darshan B.; Bhatt, Ranu; Huskens, Jurriaan; Verboom, Willem

doi:10.1016/j.cep.2021.108323

Cited by 5 publications

(3 citation statements)

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“…Nitrilotriacetamide (NTAmide) ligands, with soft N -donor atoms, have been studied by several authors for the extraction of lanthanide (Ln)/actinide (An) ions for their potential application toward An 3+ /Ln 3+ separation. − However, higher extraction of tetravalent actinide compared to the trivalent or hexavalent actinides by NTAmide was also reported by others. − The involvement of the central nitrogen of the NTAmide in the extraction of softer trivalent actinides was suggested by Bhattacharyya et al, , whereas interaction of amidic oxygen of lignad for tetravalent ion extraction was shown by Huang et al The long alkyl chain derivatives of NTAmide , such as the one with n -octyl groups (HONTA( L II ), Figure ), show high extraction ability and selectivity for Th(IV) compared to trivalent Ln ions from pH 1 to 10.0 M HNO 3 with separation factors ( SF Th – Ln = D Th / D Ln ) ranging from 2.5 × 10 2 to 10 3 . The high relative extraction of Pu 4+ compared to U(VI) and Am(III) from 3 M HNO 3 solution was also suggested by others. ,,,− The separation factor of Pu 4+ was found to be greater than10 3 and 5 × 10 3 for UO 2 2+ and Am 3+ , respectively, at 3 M HNO 3 for HONTA dissolved in n -dodecane +10% isodecanol. The distribution ratio of Pu(IV) ( D Pu ) in the presence of phase modifiers, for example, isodecanol (IDA), shows a significant decrease from ca.…”

Section: Introductionmentioning

confidence: 99%

Aggregation Behavior of Nitrilotriacetamide (NTAmide) Ligands in Thorium(IV) Extraction from Acidic Medium: Small-Angle Neutron Scattering, Fourier Transform Infrared, and Theoretical Studies

et al. 2022

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Two tripodal amides obtained from nitrilotriacetic acid with n-butyl and n-octyl alkyl chains (HBNTA(L I ) and HONTA(L II ), respectively) were studied for the extraction of Th(IV) ions from nitric acid medium. The effect of the diluent medium, i.e., n-dodecane alone and a mixture of n-dodecane and 1-decanol, onto aggregate formation were investigated using small angle neutron scattering (SANS) studies. In addition, the influence of the ligand structure, nitric acid, and Th(IV) loading onto ligand aggregation and third-phase formation tendency was discussed.The L I /L II exist as monomers (aggregarte radius for L I : 6.0 Å; L II :7.4 Å) in the presence of 1-decanol, whereas L II forms dimers (aggregarte radius for L II :9.3 Å; L I does not dissolve in n-dodecane) in the absence of 1-decanol. The aggregation number increases for both the ligands after HNO 3 and Th(IV) loading. The maximum organic concentration (0.050 ± 0.004 M) of Th(IV) was reached without third-phase formation for 0.1 M L I /L II dissolved in 20% isodecanol +80% ndodecane. The interaction of 1-decanol with L II and HNO 3 /Th(IV) with amidic oxygens of L I /L II results in shift of carbonyl stretching frequency, as shown by attenuated total reflectance-Fourier transform infrared (ATR-FTIR) studies. The structural and bonding information of the Th-L I /L II complex were derived from the density functional theoretical (DFT) studies. The molecular dynamics (MD) simulations suggested that the aggregation behavior of the ligand in the present system is governed by the population of hydrogen bonds by phase modifier around the ligand molecules. Although the theoretical studies suggested higher Gibbs free energy of complexation for Th 4+ ions with L I than L II, the extraction was found to be higher with the latter, possibly due to the higher lipophilicity and solubility of the Th-L II aggregate in the nonpolar media.

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Section: Introductionmentioning

confidence: 99%

Aggregation Behavior of Nitrilotriacetamide (NTAmide) Ligands in Thorium(IV) Extraction from Acidic Medium: Small-Angle Neutron Scattering, Fourier Transform Infrared, and Theoretical Studies

et al. 2022

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“…They display promising results for the extraction of Pu(IV) ions as compared to that of UO 2 2+ and Am(III) ions from nitric acid feed solutions. [12][13][14][15] Out of the different alkyl NTA ligands (alkyl: n-butyl, n-hexyl, n-octyl and n-dodecyl) studied by us, the hexa-n-octyl nitrilotriacetamide (HONTA) ligand was found to be superior for the extraction of tetravalent metal ions from nitric acid medium. However, the spacer length effect of the HRNTA ligands is unexplored.…”

Section: Introductionmentioning

confidence: 99%

Role of ligand spacer length of a tripodal amide on uranium(vi) and plutonium(iv) complexation: synthesis, solvent extraction, liquid membrane transport and theoretical studies

et al. 2022

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“…In fact, supported liquid membrane technologies have been proposed for the treatment of strategic and toxic metals. Some of their uses have recently been reviewed [6,7] and specifically published in the case of heavy metals [8][9][10], germanium [11], rare earth metals [12,13], scandium [14], europium [15], and tungsten [16].…”

Section: Introductionmentioning

confidence: 99%

Separation Iron(III)-Manganese(II) via Supported Liquid Membrane Technology in the Treatment of Spent Alkaline Batteries

López

2021

Membranes

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In this paper, the transport of iron(III) from iron(III)-manganese(II)-hydrochloric acid mixed solutions, coming from the treatment of spent alkaline batteries through a flat-sheet supported liquid membrane, is investigated (the carrier phase being of Cyanex 923 (commercially available phosphine oxide extractant) dissolved in Solvesso 100 (commercially available diluent)). Iron(III) transport is studied as a function of hydrodynamic conditions, the concentration of manganese and HCl in the feed phase, and the carrier concentration in the membrane phase. A transport model is derived that describes the transport mechanism, consisting of diffusion through a feed aqueous diffusion layer, a fast interfacial chemical reaction, and diffusion of the iron(III) species-Cyanex 923 complex across the membrane phase. The membrane diffusional resistance (Δm) and feed diffusional resistance (Δf) are calculated from the model, and their values are 145 s/cm and 361 s/cm, respectively. It is apparent that the transport of iron(III) is mainly controlled by diffusion through the aqueous feed boundary layer, this being the thickness of this layer calculated as 2.9 × 10−3 cm. Since manganese(II) is not transported through the membrane phase, the present system allows the purification of these manganese-bearing solutions.

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Carrier mediated transport of actinides using hexa–n-hexylnitrilotriacetamide (HHNTA)

Cited by 5 publications

References 41 publications

Aggregation Behavior of Nitrilotriacetamide (NTAmide) Ligands in Thorium(IV) Extraction from Acidic Medium: Small-Angle Neutron Scattering, Fourier Transform Infrared, and Theoretical Studies

Aggregation Behavior of Nitrilotriacetamide (NTAmide) Ligands in Thorium(IV) Extraction from Acidic Medium: Small-Angle Neutron Scattering, Fourier Transform Infrared, and Theoretical Studies

Role of ligand spacer length of a tripodal amide on uranium(vi) and plutonium(iv) complexation: synthesis, solvent extraction, liquid membrane transport and theoretical studies

Separation Iron(III)-Manganese(II) via Supported Liquid Membrane Technology in the Treatment of Spent Alkaline Batteries

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