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

Jian, Yaping; Zhang, Jiacheng; Cao, Xuewen; Peng, Qin; Zhang, Jun; Tian, Xuefeng; Du, Jianfei; Li, Yan et al. · Nat Commun · 2025

basic_science · Level V

Where this comes from

Abstract

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 (K<sub>d</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.