Solid-phase extraction technology for actinide and lanthanide separations in nuclear fuel reprocessing

Tranter, T. J.

doi:10.1533/9780857092274.3.377

Cited by 9 publications

(15 citation statements)

References 76 publications

(72 reference statements)

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“…An alternative approach—solid-phase extraction—has been pursued by impregnating the pores of macroporous polymer substrates with extractant solutions. 14 Such methods have received considerable attention because they eliminate the agitated contactors demanded by solvent extraction, while maintaining the binding selectivity of conventional ligand sets. In addition, nanoparticles and mesoporous materials have been tested for the encapsulation of early actinides.…”

Section: Introductionmentioning

confidence: 99%

“…In addition, the equipment required for multistage extraction and stripping, such as mixer-settlers and centrifugal contactors, greatly increases capital costs. An alternative approachsolid-phase extractionhas been pursued by impregnating the pores of macroporous polymer substrates with extractant solutions . Such methods have received considerable attention because they eliminate the agitated contactors demanded by solvent extraction, while maintaining the binding selectivity of conventional ligand sets.…”

Section: Introductionmentioning

confidence: 99%

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Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework

Demir¹,

Brune²,

Humbeck³

et al. 2016

ACS Cent. Sci.

110

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Porous aromatic frameworks (PAFs) incorporating a high concentration of acid functional groups possess characteristics that are promising for use in separating lanthanide and actinide metal ions, as required in the treatment of radioactive waste. These materials have been shown to be indefinitely stable to concentrated acids and bases, potentially allowing for multiple adsorption/stripping cycles. Additionally, the PAFs combine exceptional features from MOFs and inorganic/activated carbons giving rise to tunable pore surfaces and maximum chemical stability. Herein, we present a study of the adsorption of selected metal ions, Sr2+, Fe3+, Nd3+, and Am3+, from aqueous solutions employing a carbon-based porous aromatic framework, BPP-7 (Berkeley Porous Polymer-7). This material displays high metal loading capacities together with excellent adsorption selectivity for neodymium over strontium based on Langmuir adsorption isotherms and ideal adsorbed solution theory (IAST) calculations. Based in part upon X-ray absorption spectroscopy studies, the stronger adsorption of neodymium is attributed to multiple metal ion and binding site interactions resulting from the densely functionalized and highly interpenetrated structure of BPP-7. Recyclability and combustibility experiments demonstrate that multiple adsorption/stripping cycles can be completed with minimal degradation of the polymer adsorption capacity.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework

Demir¹,

Brune²,

Humbeck³

et al. 2016

ACS Cent. Sci.

110

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“…The optical band gaps of both Mg-NMS, Na-NMS, and all their derivatives are presented in Figure 8a,b, respectively, and summarized in Tables 4 and 5. The band gaps of each parent material are almost identical at 2.40 (5) eV for Mg-NMS and 2.42 (5) eV for Na-NMS. This result is similar to the values for other reported layered metal sulfides based on SnS 2 16,39−41 and is identical to the bandgap of K 2 MgSn 2 S 6 (KMS-2).…”

Section: Inorganic Chemistrymentioning

confidence: 91%

“…When the Na-HMS and Mg-HMS react with selected amines, the band gaps relative to the pristine materials are similarly redshifted between 0.13 and 0.58 (5) eV for (R− NH 3 ) 2x Mg 2y−x Sn 4−y S 8 and 0.18−0.54 (5) eV for (R− NH 3 ) y−1 Na y ) 4 [Na 1.33 Sn 2.67 ]S 8 . Of the amines tested, aniline and ethylenediamine produced the smallest gaps for both materials tested, with band gaps within the range of 1.82(5) − 1.98(5) eV.…”

Section: T H I S C O N T E N T Imentioning

confidence: 99%

Metal Sulfide Ion Exchangers: High Acid Stability of Na_2xMg_2y–xSn_4–yS₈ (NMS) and Topotactic Conversion to 2D Solid Acids with Semiconducting Character

Quintero,

Pournara,

Godsel

et al. 2023

Inorg. Chem.

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Metal sulfide ion exchange materials (MSIEs) are of interest for nuclear waste remediation applications. We report the high stability of two structurally related metal sulfide ion exchange materials, Na2x Mg2y–x Sn4–y S8 (Mg-NMS) and Na2SnS3 (Na-NMS), in strongly acid media, in addition to the preparation of Na2x Ni2y–x Sn4–y S8 (Ni-NMS). Their formation progress during synthesis is studied with in-situ methods, with the target phases appearing in <15 min, reaction completion in <12 h, and high yields (75–80%). Upon contact with nitric or hydrochloric acid, these materials topotactically exchange Na+ for H+, proceeding in a stepwise protonation pathway for Na5.33Sn2.67S8. Na-NMS is stable in 2 M HNO3 and Mg-NMS is stable in 4 M HNO3 for up to 4 h, while both NMS materials are stable in 6 M HCl for up to 4 days. However, the treatment of Mg-NMS and Na-NMS with 2–6 M H2SO4 reveals a much slower protonation process since after 4 h of contact both NMS and HMS are present in the solution. The resultant protonated materials, H2x Mg2y–x Sn4–y S8 and H4x [(H y Na y–1)1.33x Sn4––1.33x ]S8, are themselves solid acids and readily react with and intercalate a variety of organic amines, where the band gap of the resultant adduct is influenced by amine choice and can be tuned within the range of 1.88(5)–2.27(5) eV. The work function energy values for all materials were extracted from photoemission yield spectroscopy in air (PYSA) measurements and range from 5.47 (2) to 5.76 (2) eV, and the relative band alignments of the materials are discussed. DFT calculations suggest that the electronic structure of Na2MgSn3S8 and H2MgSn3S8 makes them indirect gap semiconductors with multi-valley band edges, with carriers confined to the [MgSn3S8]2– layers. Light electron effective masses indicate high electron mobilities.

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“…The selective complexation of lanthanide ions in coordination chemistry is important for many different areas, including the design of metal complexes for diagnostic and imaging , applications, therapeutic agents, , and the preparation of selective metal extractants for hydrometallurgy and nuclear waste management. − However, the selective complexation of Ln 3+ cations is challenging because of their similar physical and chemical properties. According to the classification by Pearson, they behave as hard Lewis acids of similar radii with contraction of the ionic radius from La 3+ to Lu 3+ by 16%.…”

mentioning

confidence: 99%

Employing Lewis Acidity to Generate Bimetallic Lanthanide Complexes

et al. 2020

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With the advent of lanthanide-based technologies, there is a clear need to advance the fundamental understanding of 4f-element chelation chemistry. Herein, we contribute to a growing body of lanthanide chelation chemistry and report the synthesis of bimetallic 4f-element complexes within an imine/hemiacetalate framework, Ln 2 TPT OMe [Ln = lanthanide; TPT OMe = tris(pyridineimine)(Tren)tris(methoxyhemiacetalate); Tren = tris(2-aminoethylamine)]. These products are generated from hydrolysis and methanolysis of the cage ligand tris(pyridinediimine)bis(Tren) (TPT; Tadanobu et al. Chem. Lett. 1993, 22 (5), 859−862) likely facilitated by inductive effects stemming from the Lewis acidic lanthanide cations. These complexes are interesting because they result from imine cleavage to generate two metal binding sites: one pocketed site within the macrocycle and the other terminal site capping a hemiacetalate moiety. A clear demarcation in reactivity is observed between samarium and europium, where the lighter and larger lanthanides generate a mixture of products, Ln 2 TPT OMe and LnTPT. Meanwhile, the heavier and smaller lanthanides generate exclusively bimetallic Ln 2 TPT OMe . The cleavage reactivity to form Ln 2 TPT OMe was extended beyond methanol to include other primary alcohols.

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Solid-phase extraction technology for actinide and lanthanide separations in nuclear fuel reprocessing

Cited by 9 publications

References 76 publications

Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework

Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework

Metal Sulfide Ion Exchangers: High Acid Stability of Na_2xMg_2y–xSn_4–yS₈ (NMS) and Topotactic Conversion to 2D Solid Acids with Semiconducting Character

Employing Lewis Acidity to Generate Bimetallic Lanthanide Complexes

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Solid-phase extraction technology for actinide and lanthanide separations in nuclear fuel reprocessing

Cited by 9 publications

References 76 publications

Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework

Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework

Metal Sulfide Ion Exchangers: High Acid Stability of Na2xMg2y–xSn4–yS8 (NMS) and Topotactic Conversion to 2D Solid Acids with Semiconducting Character

Employing Lewis Acidity to Generate Bimetallic Lanthanide Complexes

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Resources

About

Metal Sulfide Ion Exchangers: High Acid Stability of Na_2xMg_2y–xSn_4–yS₈ (NMS) and Topotactic Conversion to 2D Solid Acids with Semiconducting Character