Separation of ²⁴¹Am³⁺ from ¹⁵⁴Eu³⁺ Using 3,3’-Butyloxy-Bis-1,2,4-Triazinyl-2,6-Pyridine as a Potent Receptor

ABSTRACT

The effective partitioning and transmutation of the minor An from the Ln in spent nuclear fuel in a non-proliferative manner is critical to lowering potential impact to the environment, moderating concern over the increase of nuclear power as a green alternative to fossil fuels, and solving a grand challenge in separation science. Although present in less than .1 wt.%, Am and Cm represent half-lives of over 400 years and significantly contribute to heat load through radioactive decay. Separation of the minor An from the neutron-poisoning Ln can advance the nuclear fuel cycle further toward closure and decrease the volume and radiotoxicity of daughter nuclides stored in a geologic repository. Similar physical properties and metal-complexant binding phenomena render this separation difficult. In this work, a comprehensive liquid-liquid separations study using the recently discovered 3,3’-butyloxy-bis-1,2,4-triazinyl-2,6-pyridine in the polar aprotic solvent trifluoromethylphenyl sulfone is presented. Unlike contemporary bis-1,2,4-triazinyl-2,6-pyridine complexants, the current system is stable and performs well in highly acidic systems. Separation of ²⁴¹Am³⁺ from ¹⁵⁴Eu³⁺, acid range tolerance, complexant concentration, and decomplexation studies are presented herein.

Graphical abstract

KEYWORDS:

• Alkoxy-BTP
• minor An separations
• liquid-liquid
• complexant
• heterocycle

Acknowledgments

Financial support for this work was provided by an award from the U.S. Department of Energy, Basic Energy Sciences, Separations Program, Award: DE-SC0018033. The Camille and Henry Dreyfus Foundation is gratefully acknowledged for a Henry Dreyfus Teacher-Scholar Award to J.D.C. An award from the National Science Foundation Major Research Instrumentation (MRI) Program (1531870) supported the acquisition of TN Tech’s 500 MHz multinuclear NMR spectrometer. The authors would like to thank Prof. David Dan, TN Tech, for helpful discussions on radiochemistry experimental technique.

Disclosure statement

No potential conflict of interest was reported by the author(s).

Supplementary data

Supplemental data for this article can be accessed online at https://doi.org/10.1080/07366299.2024.2320094

Data availability statement

The data underlying this study are available in the online supplementary material.

Additional information

Funding

This work was supported by the Camille and Henry Dreyfus Foundation [Henry Dreyfus Teacher-Scholar Award 2022]; United States Department of Energy, Basic Energy Sciences, Separations Program [DE-SC0018033].