Abstract

Expanded low-carbon baseload power production through the use of nuclear fission can be enabled by recycling long-lived actinide isotopes within the nuclear fuel cycle. This approach provides the benefits of (a) more completely utilizing the energy potential of mined uranium, (b) reducing the footprint of nuclear geological repositories, and (c) reducing the time required for the radiotoxicity of the disposed waste to decrease to the level of uranium ore from one hundred thousand years to a few hundred years. A key step in achieving this goal is the separation of long-lived isotopes of americium (Am) and curium (Cm) for recycle into fast reactors. To achieve this goal, a novel process was successfully demonstrated on a laboratory scale using a bank of 1.25-cm centrifugal contactors, fabricated by additive manufacturing, and a simulant containing the major fission product elements. Americium and Cm were separated from the lanthanides with over 99.9% completion. The sum of the impurities of the Am/Cm product stream using the simulated raffinate was found to be 3.2 × 10−3 g/L. The process performance was validated using a genuine high burnup used nuclear fuel raffinate in a batch regime. Separation factors of nearly 100 for 154Eu over 241Am were achieved. All these results indicate the process scalability to an engineering scale.

Highlights

  • Expanded low-carbon baseload power production through the use of nuclear fission can be enabled by recycling long-lived actinide isotopes within the nuclear fuel cycle

  • Americium and Cm were separated from the lanthanides with over 99.9% completion

  • Owing to the larger 5-f electron orbitals, there is an increased covalent bonding nature within the actinides compared to the lanthanide 4-f series[26,34]

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Summary

Introduction

Expanded low-carbon baseload power production through the use of nuclear fission can be enabled by recycling long-lived actinide isotopes within the nuclear fuel cycle This approach provides the benefits of (a) more completely utilizing the energy potential of mined uranium, (b) reducing the footprint of nuclear geological repositories, and (c) reducing the time required for the radiotoxicity of the disposed waste to decrease to the level of uranium ore from one hundred thousand years to a few hundred years. The transmutation option offers benefits to geological disposition of UNF by increasing the loading capacity of the repository (by reducing the heat load), and by reducing the long-term radiotoxicity of the disposed material[3] To enable this advanced nuclear fuel cycle, cost-effective, high throughput, and reliable separation schemes are needed. We have focused our efforts on liquid-liquid extraction methods since this technology is the only industrially proven technique suitable for reprocessing of vast quantities of nuclear materials in a timely manner, and is compatible with current industrial practices[9,10]

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