Ultrafiltration separation of Am(VI)-polyoxometalate from lanthanides

Hailong Zhang, Ao Li, Kai Li, Zhipeng Wang, Xiaocheng Xu, Yaxing Wang (), Matthew V. Sheridan, Han-Shi Hu, Chao Xu (), Evgeny V. Alekseev, Zhenyi Zhang, Pu Yan, Kecheng Cao, Zhifang Chai, Thomas E. Albrecht-Schönzart () and Shuao Wang ()
Additional contact information
Hailong Zhang: Soochow University
Ao Li: Soochow University
Kai Li: Soochow University
Zhipeng Wang: Tsinghua University
Xiaocheng Xu: Tsinghua University
Yaxing Wang: Soochow University
Matthew V. Sheridan: Soochow University
Han-Shi Hu: Tsinghua University
Chao Xu: Tsinghua University
Evgeny V. Alekseev: IEK-9, Forschungszentrum Jülich
Zhenyi Zhang: Bruker (Beijing) Scientific Technology Co., Ltd
Pu Yan: ShanghaiTech University
Kecheng Cao: ShanghaiTech University
Zhifang Chai: Soochow University
Thomas E. Albrecht-Schönzart: Colorado School of Mines
Shuao Wang: Soochow University

Nature, 2023, vol. 616, issue 7957, 482-487

Abstract: Abstract Partitioning of americium from lanthanides (Ln) present in used nuclear fuel plays a key role in the sustainable development of nuclear energy1–3. 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 AmO22+ 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 (238U, 237Np, 242Pu and 243Am) 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.

Date: 2023
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DOI: 10.1038/s41586-023-05840-z

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