<p>Efficient recovery of uranium from spent nuclear fuel (SNF) reprocessing in ultra-acidic and radiation-intensive environments is critical for sustainable uranium resources management. However, traditional extractants exhibit instability and reduced uranium adsorption capacity under such harsh conditions. Here, we present a metal-free pyrophosphate-incorporated g-C₃N₄ polymer (PCN<sub>x</sub>) featuring unsaturated nitrogen sites and pyrophosphate groups for robust uranyl ion coordination. The inherent stability of g-C<sub>3</sub>N<sub>4</sub> endows PCN<sub>x</sub> with high resistance to concentrated 12 M HNO<sub>3</sub> and 500 kGy radiation. The optimal PCN<sub>1/3</sub> achieves an uranium adsorption capacity of 75.3 mg g<sup>−1</sup> in 12 M HNO<sub>3</sub> and a high removal efficiency of 79.1% in a mixed ion solution, with a high distribution coefficient (<i>K</i><sub><i>d</i></sub>) of 18,964 mL g<sup>−1</sup>. This study demonstrates a promising proof-of-concept for designing functional polymers that efficiently recovers uranium from ultra-acidic and radiation-intensive conditions during SNF reprocessing.</p>

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Synergy of pyrophosphate and unsaturated nitrogen sites for efficient uranium recovery from concentrated nitric acid

  • Yaping Jian,
  • Jiacheng Zhang,
  • Xuewen Cao,
  • Qin Peng,
  • Jun Zhang,
  • Xuefeng Tian,
  • Jianfei Du,
  • Yan Li,
  • Yihui Yuan,
  • Ning Wang

摘要

Efficient recovery of uranium from spent nuclear fuel (SNF) reprocessing in ultra-acidic and radiation-intensive environments is critical for sustainable uranium resources management. However, traditional extractants exhibit instability and reduced uranium adsorption capacity under such harsh conditions. Here, we present a metal-free pyrophosphate-incorporated g-C₃N₄ polymer (PCNx) featuring unsaturated nitrogen sites and pyrophosphate groups for robust uranyl ion coordination. The inherent stability of g-C3N4 endows PCNx with high resistance to concentrated 12 M HNO3 and 500 kGy radiation. The optimal PCN1/3 achieves an uranium adsorption capacity of 75.3 mg g−1 in 12 M HNO3 and a high removal efficiency of 79.1% in a mixed ion solution, with a high distribution coefficient (Kd) of 18,964 mL g−1. This study demonstrates a promising proof-of-concept for designing functional polymers that efficiently recovers uranium from ultra-acidic and radiation-intensive conditions during SNF reprocessing.