<p>To assess the effect of external <i>γ</i>-radiation on the dissolution of the spent UO<sub>2</sub> fuel matrix, dynamic dissolution experiments were performed with UO<sub>2</sub> pellets using well-controlled flow-through reactor at different low flowrates under oxic conditions. Firstly, the setup was validated without radiation at different leachant compositions (<i>I</i> = 0.02&#xa0;mol·L<sup>−1</sup> of ionic strength and pH from 5.4 to 12.2), flowrates (from ~ 4.5&#xa0;mL·d<sup>−1</sup> to 120&#xa0;mL·d<sup>−1</sup>), and residence times (11.3–383&#xa0;h) at room conditions. A good agreement of data trends (U concentration <i>vs</i> flowrates) is obtained. The results show the impact of the flowrates and carbonates on the dissolution rate of U, <i>i.e.,</i> the concentration of dissolved U(VI) increased with increasing [HCO<sub>3</sub><sup>−</sup>]. For the experiment under external <i>γ</i>-radiation (0.014 kGy·h<sup>−1</sup>) with UO<sub>2</sub> in 20-mmol·L<sup>−1</sup> NaClO<sub>4</sub>, the presence of studtite was confirmed and consistent with the measured H<sub>2</sub>O<sub>2</sub> concentrations (~ 10<sup>–5</sup>&#xa0;mol L<sup>−1</sup>).</p> Graphical abstract <p></p>

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Impact of in situ gamma irradiation simulates on UO2: Set-up flow-through corrosion experiments

  • Nieves Rodríguez-Villagra,
  • Laura J. Bonales,
  • Joaquín Cobos,
  • Hitos Galán

摘要

To assess the effect of external γ-radiation on the dissolution of the spent UO2 fuel matrix, dynamic dissolution experiments were performed with UO2 pellets using well-controlled flow-through reactor at different low flowrates under oxic conditions. Firstly, the setup was validated without radiation at different leachant compositions (I = 0.02 mol·L−1 of ionic strength and pH from 5.4 to 12.2), flowrates (from ~ 4.5 mL·d−1 to 120 mL·d−1), and residence times (11.3–383 h) at room conditions. A good agreement of data trends (U concentration vs flowrates) is obtained. The results show the impact of the flowrates and carbonates on the dissolution rate of U, i.e., the concentration of dissolved U(VI) increased with increasing [HCO3]. For the experiment under external γ-radiation (0.014 kGy·h−1) with UO2 in 20-mmol·L−1 NaClO4, the presence of studtite was confirmed and consistent with the measured H2O2 concentrations (~ 10–5 mol L−1).

Graphical abstract