Treatment method for volume reduction of spent uranium catalyst

• US 10,643,758 B2
• Filed: 04/23/2018
• Issued: 05/05/2020
• Est. Priority Date: 07/14/2017
• Status: Active Grant

• Current Assignee: Korea Atomic Energy Research Institute (Government of The Republic of Korea)
• Original Assignee: Korea Atomic Energy Research Institute (Government of The Republic of Korea)
• Inventors: Kim, Kwang-Wook, Lee, Keun-Young, Ahn, Byung-Gil, Chung, Dong Yong, Seo, Bum Kyoung
• Primary Examiner(s): Johnson, Edward M
• Application Number:
  US15/960,166
• Publication Number:
  US 20190019590A1
• Time in Patent Office: 743 Days
• Field of Search: 588 2
• CPC Class Codes: C22B 60/0234 sulfurated ion as active agent
• CPC Class Codes: C22B 60/0247 using basic solutions or liquors
• CPC Class Codes: C22B 60/0278 by chemical methods C22B60/0256, C22B60/026, C22B60/0265 take precedence
• CPC Class Codes: G21F 9/12 by absorption; by adsorption; by ion-exchange
• CPC Class Codes: G21F 9/305 Glass or glass like matrix C03B5/005 takes precedence; compositional aspects C03C
• CPC Class Codes: Y02P 10/20 Recycling

Abstract

A volume reduction treatment method able to reduce the volume of the final disposal waste of a spent uranium catalyst. As a result, the disposal cost of the spent uranium catalyst is able to be reduced and the utilization of waste repositories are able to be improved.

Claims

1. A treatment method of a spent uranium catalyst, wherein said spent uranium catalyst comprises a support component, said method comprising the following steps:

selectively dissolving the support component by immersing the spent uranium catalyst in an alkali solution (step

     1), thereby generating a dissolution solution and undissolved solid materials;

separating the dissolution solution and the undissolved solid materials in the step 1 by solid-liquid separation (step

     2);

selectively precipitating the silicon ions in the dissolution solution as silicon dioxide (step

     3);

separating the silicon dioxide generated in step 3 by solid-liquid separation and purification (step

     4), thereby generating a residual solution;

precipitating uranium ions as uranium phosphate by adding phosphate to the residual solution separated in step 4 (step

     5);

separating the uranium phosphate generated in step 5 by solid-liquid separation (step

     6);

mixing the undissolved solid materials separated in step 2 with the precipitate of uranium phosphate separated in step 6 and then adding a glassification agent thereto thereby generating a mixture, followed by heat-treatment to fix the mixture in the form of a glass-ceramic composite medium (step

     7).

2. The treatment method of a spent uranium catalyst according to claim 1, wherein the spent uranium catalyst of step 1 has a form in which U_wSb_xM_yO_z is supported on a silicon dioxide support, wherein M is one or more materials selected from the group consisting of Fe, Al, Mo, V, and Bi;

and w, x, y, and z indicate the molar ratio of the elements constituting the oxide.

3. The treatment method of a spent uranium catalyst according to claim 1, wherein the alkali solution of step 1 is one or more solutions selected from the group consisting of sodium hydroxide solution, potassium hydroxide solution, lithium hydroxide solution, and ammonium hydroxide solution.

4. The treatment method of a spent uranium catalyst according to claim 1, wherein the molar concentration of hydroxide ions in the alkali solution of step 1 is 2 to 4 M.

5. The treatment method of a spent uranium catalyst according to claim 1, wherein the dissolution of step 1 is induced at the boiling point of the solution.

6. The treatment method of a spent uranium catalyst according to claim 1, further comprising an additional step of heat-treating the spent uranium catalyst at 550 to 750°

C. before the dissolution process is accomplished in step 1.

7. The treatment method of a spent uranium catalyst according to claim 1, wherein when the spent uranium catalyst is dissolved in the alkali solution in step 1, the ratio of the volume (mL) of the alkali solution to the weight (g) of the spent uranium catalyst is 0.125 to 0.25 g/mL.

8. The treatment method of a spent uranium catalyst according to claim 1, wherein the solid-liquid separation in step 2 is performed by using a separation membrane coated with diatomite powder.

9. The treatment method of a spent uranium catalyst according to claim 8, wherein the separation membrane is coated with diatomite powder at the thickness of 1 to 2 mm.

10. The treatment method of a spent uranium catalyst according to claim 8, wherein the separation membrane is appropriate for filtering the particles in the mean diameter of 0.5 to 1 μ

m.

11. The treatment method of a spent uranium catalyst according to claim 8, wherein the diatomite has an average diameter of 30 to 38 μ

m.

12. The treatment method of a spent uranium catalyst according to claim 1, further comprising an additional step of converting uranium into complex ions by adding hydrogen peroxide and phosphate to the dissolution solution separated by solid-liquid separation before the selective precipitation of the silicon ions remaining in the dissolution solution in step 3.

13. The treatment method of a spent uranium catalyst according to claim 12, wherein the uranium complex ions are in the form of UO₂(O₂)(CO₃)₂⁴⁻

.

14. The treatment method of a spent uranium catalyst according to claim 1, wherein the selective precipitation of silicon ions in step 3 is accomplished by adjusting the pH of the dissolution solution separated by solid-liquid separation to 9 to 10.

15. The treatment method of a spent uranium catalyst according to claim 1, wherein the solid-liquid separation is performed by using a media filtration method.

16. The treatment method of a spent uranium catalyst according to claim 1, wherein the phosphate of step 5 is NaH₂PO₄, KH₂PO₄, or NH₄H₂PO₄.

17. The treatment method of a spent uranium catalyst according to claim 1, wherein the precipitation of uranium ions in the form of uranium phosphate in step 5 is performed after adding phosphate to the solution remaining after the solid-liquid separation in the step 4 at the concentration of 0.1 to 6 mM, during which the pH is adjusted to 5 to 7.

18. The treatment method of a spent uranium catalyst according to claim 1, wherein the glassification agent of step 7 is NaO₂ or B₂O₃.

19. The treatment method of a spent uranium catalyst according to claim 1, wherein the glassification agent of step 7 is added at the concentration of 5 to 15 weight % by the total silicon oxide weight of mixture of the undissolved solid separated in step 2 and the uranium phosphate precipitate separated in step 6.

20. The treatment method of a spent uranium catalyst according to claim 1, wherein the temperature for the heat-treatment of step 7 is 700 to 1200°

C.

21. The treatment method of a spent uranium catalyst according to claim 1, further comprising an additional step of washing the precipitate separated in step 4 by passing acid and water through the precipitate.