Ultrafiltration separation of Am(VI)-polyoxometalate from lanthanides

• Published in: Nature (London) Vol. 616; no. 7957; pp. 482 - 487
• Main Authors: Zhang, Hailong, Li, Ao, Li, Kai, Wang, Zhipeng, Xu, Xiaocheng, Wang, Yaxing, Sheridan, Matthew V., Hu, Han-Shi, Xu, Chao, Alekseev, Evgeny V., Zhang, Zhenyi, Yan, Pu, Cao, Kecheng, Chai, Zhifang, Albrecht-Schönzart, Thomas E., Wang, Shuao
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 20.04.2023; Nature Publishing Group
• Subjects: 639/4077/4091/4094; 639/638/903; Acids; Actinides; Americium; Aqueous solutions; Chemistry; Clusters; Coordination; Humanities and Social Sciences; Ions; Lanthanides; MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; multidisciplinary; Nitric acid; Nuclear chemistry; Nuclear fuels; Nuclear waste; Oxidation; Polyoxometallates; Radiolysis; Reagents; Science; Science (multidisciplinary); Separation; Spent nuclear fuels; Sustainable development; Ultrafiltration
• ISSN: 0028-0836; 1476-4687
• DOI: 10.1038/s41586-023-05840-z

Partitioning of americium from lanthanides (Ln) present in used nuclear fuel plays a key role in the sustainable development of nuclear energy 1 – 3 . This task is extremely challenging because thermodynamically stable Am(III) and Ln(III) ions have nearly identical ionic radii and coordination chemistry. Oxidization of Am(III) to Am(VI) produces AmO 2 2+ ions distinct with Ln(III) ions, which has the potential to facilitate separations in principle. However, the rapid reduction of Am(VI) back to Am(III) by radiolysis products and organic reagents required for the traditional separation protocols including solvent and solid extractions hampers practical redox-based separations. Herein, we report a nanoscale polyoxometalate (POM) cluster with a vacancy site compatible with the selective coordination of hexavalent actinides ( 238 U, 237 Np, 242 Pu and 243 Am) over trivalent lanthanides in nitric acid media. To our knowledge, this cluster is the most stable Am(VI) species in aqueous media observed so far. Ultrafiltration-based separation of nanoscale Am(VI)-POM clusters from hydrated lanthanide ions by commercially available, fine-pored membranes enables the development of a once-through americium/lanthanide separation strategy that is highly efficient and rapid, does not involve any organic components and requires minimal energy input. A new strategy to separate radioactive americium from lanthanides based on complexation with polyoxometalates and ultrafiltration technique is highly efficient and rapid, does not involve any organic components and requires minimal energy input.