Nuclear Engineering and Technology

Korean Nuclear Society (한국원자력학회)
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Radiation stability and radiolysis mechanism of hydroxyurea in HNO3 solution: Alpha, beta, and gamma irradiations

  • Yilin Qin (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Wei Liao (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Tu Lan (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Fengzhen Li (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Feize Li (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Jijun Yang (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Jiali Liao (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Yuanyou Yang (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University) ;
  • Ning Liu (Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University)
  • Received : 2022.05.26
  • Accepted : 2022.07.30
  • Published : 2022.12.25
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Abstract

Hydroxyurea (HU) is a novel salt-free reductant used potentially for the separation of U/Pu in the advanced PUREX process. In this work, the radiation stability of HU were systematically investigated in solution by examining the effects of the type of rays (α, β, and γ irradiations), the absorbed dose (10-50 kGy), and the HNO3 concentration (0-3 mol L-1). The influence degree on HU radiolysis rates followed the order of the absorbed dose > the ray type > the HNO3 concentration, but the latter two had moderate effects on HU radiolysis products where NH4+ and NO2- were found to be the most abundant ones, suggesting that the differences of α, β, and γ rays should be considered in the study of irradiation effects. The radiolysis mechanism was explored using density functional theory (DFT) calculations, and it proposed the dominant radiolysis paths of HU, indicating that the radiolysis of HU was mainly a free radical reaction among ·H, eaq-, H2O, intermediates, and the radiolytic free radical fragments of HU. The results reported here provide valuable insights into the mechanistic understanding of HU radiolysis under α, β, and γ irradiations and reliable data support for the application of HU in the reprocessing of spent fuel.

Keywords

Acknowledgement

Financial support from the National Natural Science Foundation of China (Grant No. 21876122), the State Administration of Science, Technology, and Industry for National Defense (PRC) for the Spent Fuel Reprocessing Project, and the Fundamental Research Funds for the Central Universities is gratefully acknowledged.

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