Selective Crystallization of a Highly Radiation-Resistant Isonicotinic Acid-Based Metal–Organic Framework as a Primary Actinide Waste Form

Lv, Kai; Patzschke, Michael; März, Juliane; Bazarkina, Elena F.; Kvashnina, Kristina O.; Schmidt, Moritz

doi:10.1021/acsmaterialslett.2c01087

Cited by 6 publications

(4 citation statements)

References 80 publications

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“…Utilizing Th-based multi-functional materials for monitoring and sequestrating more radioactive radionuclides represents a promising strategy to overcome the aforementioned challenge. − As a subgroup of MOFs, Th-MOFs inherit the combinatorial benefits of high porosity, a large surface, and structural modularity, which offer the potential of capturing specific radionuclides in their voids. − Moreover, integrating luminescent organic linkers in a framework matrix allows for the spatial distribution of the fluorophores, which eliminates aggregation-induced quenching (AIQ) and enhances the sensing efficacy via increasing the photoluminescence quantum yield. − Indeed, actinide-based MOFs have stood out as a unique and efficient platform for capturing radionuclides, including 85 Kr, 99 Tc, 129/131 I, and 137 Cs in ionic or molecular forms. − However, the sector of radionuclide sensing based on actinide MOFs is much less explored, despite the fact that they feature unique photoswitch properties such as photoluminescence, photochromism, and fluorochromism. , …”

Section: Introductionmentioning

confidence: 99%

Adsorption and Detection of Iodine Species by a Thorium-Based Metal–Organic Framework

Qiu

et al. 2023

Inorg. Chem.

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Actinide-bearing metal−organic frameworks (MOFs) encompass intriguing structures and properties, but the radioactivity of actinide cripples their applications. Herein, we have constructed a new thorium-based MOF (Th-BDAT) as a bifunctional platform for the adsorption and detection of radioiodine, a more radioactive fission product that can readily spread through the atmosphere in its molecular form or via solution as anionic species. The iodine capture within the framework of Th-BDAT from both the vapor phase and the cyclohexane solution has been verified, showing that Th-BDAT features maximum I 2 adsorption capacities (Q max ) of 959 and 1046 mg/g, respectively. Notably, the Q max of Th-BDAT toward I 2 from cyclohexane solution ranks among the highest value for Th-MOFs reported to date. Furthermore, incorporating highly extended and π-electronrich BDAT 4− ligands renders Th-BDAT as a luminescent chemosensor whose emission can be selectively quenched by iodate with a detection limit of 1.367 μM. Our findings thus foreshadow promising directions that might unlock the full potential of actinide-based MOFs from the point of view of practical application.

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Section: Introductionmentioning

confidence: 99%

Adsorption and Detection of Iodine Species by a Thorium-Based Metal–Organic Framework

Qiu

et al. 2023

Inorg. Chem.

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“…Metal–organic frameworks (MOFs), crystalline hybrid materials having the rigidity of inorganic and flexibility of organic materials, exhibited high potential in the extraction of metal ions including actinides. − Since their invention, MOFs − have been designed with task of performing a great variety of applications , thanks to their high surface area, porosity, structural tailorability, and ease of synthesis. Recently, Lillerud et al first reported synthesis of Zr 4+ containing a porous organic framework made of dicarboxylic acid termed as UiO-66.…”

Section: Introductionmentioning

confidence: 99%

Diglycolic Acid Monoamide-Functionalized UiO-66-Based Metal Organic Framework (MOFDGAMA) for Selective Removal of UO₂²⁺ and Th⁴⁺

Khan,

Pahan,

Sengupta

et al. 2024

Ind. Eng. Chem. Res.

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U and Th have attracted a great deal of attention due to their potential application as nuclear fuel materials. For the first time, we report here the synthesis and sorption of diglycolamic acid monoamidefunctionalized metal organic framework (MOF), UiO-66-NH-CODGAMA (MOFDGAMA), as a robust sorbent for the efficient removal of UO 2 2+ and Th 4+ . Introduction of the DGAMA group remarkably enhances the sorption capacity for both UO 2 2+ (193 mg g −1 ) and Th 4+ (227 mg g −1 ) compared to pristine UiO-66-NH 2 . MOFDGAMA was found to exhibit high radiolytic stability and good recyclability over multiple cycles for the efficient extraction of hexavalent uranium (UO 2 2+ ) and tetravalent thorium (Th 4+ ) from aqueous acidic streams. The findings of this work demonstrate the potential application of the materials to remove radionuclides from nuclear effluents.

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“…Therefore, this Perspective provides a conceptual framework that guides the design of innovative thorium-based materials and outlines potential solutions for addressing urgent needs in the nuclear energy − and waste remediation ,, sectors from the lens of Zr- and U- chemistry.…”

Section: Introductionmentioning

confidence: 99%

Mining for Metal–Organic Systems: Chemistry Frontiers of Th-, U-, and Zr-Materials

Park,

Lim,

Thaggard

et al. 2024

J. Am. Chem. Soc.

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The conceptual framework presented in this Perspective overviews the design principles of innovative thorium-based materials that could address urgent needs of the medicinal, nuclear energy, and waste remediation sectors from the lens of zirconium and uranium analogs. We survey the intersections of Zr, Th, and U chemistry with a focus on how the intrinsic behavior of each metal translates to broader material properties, including, but not limited to, structural and topological diversity, preferential metal− ligand binding, and reactivity. On the example of several classes of materials, including organometallic complexes, polyoxometalates, and the primary focus of this Perspective, metal−organic frameworks (MOFs), the design principles that govern the preparation of Zr-, Th-, and U-compounds, including oxophilicity, variation in oxidation states, and stable coordination environments have been considered. Further, we highlight how the impact of the mentioned variables may shift throughout the progression from discrete molecular systems to extended structures. We discuss the common assumption that zirconium-organic materials are typically considered a close analog of thorium-based congeners in areas such as material design and preparation. Through consideration of fundamental chemistry principles, we shed light on the relationships between Zr-, Th-, and U-based materials and highlight how a critical analysis of their distinct properties can be used to target a desired material performance. As a result, we provide a detailed understanding of Th-based materials chemistry by anchoring their fundamental properties between two well-studied reference points, zirconium-and uranium-containing analogs.

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Selective Crystallization of a Highly Radiation-Resistant Isonicotinic Acid-Based Metal–Organic Framework as a Primary Actinide Waste Form

Abstract: Isonicotinic acid (INA), as a prototypical N,O-donor bifunctional ligand, has demonstrated its ability to differentiate Th 4+ from representative ions for products in spent nuclear fuels

Cited by 6 publications

References 80 publications

Adsorption and Detection of Iodine Species by a Thorium-Based Metal–Organic Framework

Adsorption and Detection of Iodine Species by a Thorium-Based Metal–Organic Framework

Diglycolic Acid Monoamide-Functionalized UiO-66-Based Metal Organic Framework (MOFDGAMA) for Selective Removal of UO₂²⁺ and Th⁴⁺

Mining for Metal–Organic Systems: Chemistry Frontiers of Th-, U-, and Zr-Materials

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Selective Crystallization of a Highly Radiation-Resistant Isonicotinic Acid-Based Metal–Organic Framework as a Primary Actinide Waste Form

Abstract: Isonicotinic acid (INA), as a prototypical N,O-donor bifunctional ligand, has demonstrated its ability to differentiate Th 4+ from representative ions for products in spent nuclear fuels

Cited by 6 publications

References 80 publications

Adsorption and Detection of Iodine Species by a Thorium-Based Metal–Organic Framework

Adsorption and Detection of Iodine Species by a Thorium-Based Metal–Organic Framework

Diglycolic Acid Monoamide-Functionalized UiO-66-Based Metal Organic Framework (MOFDGAMA) for Selective Removal of UO22+ and Th4+

Mining for Metal–Organic Systems: Chemistry Frontiers of Th-, U-, and Zr-Materials

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About

Diglycolic Acid Monoamide-Functionalized UiO-66-Based Metal Organic Framework (MOFDGAMA) for Selective Removal of UO₂²⁺ and Th⁴⁺