IP Library Granted Patent US 9,842,664
Granted Patent B2
US 9,842,664 · App. 14/038,424 · Granted Dec 12, 2017

Recovering and recycling uranium used for production of molybdenum-99

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Quick Facts
Patent No.
US 9,842,664
App. No.
14/038,424
Granted
Dec 12, 2017
Kind
B2
Abstract

A processes for recycling uranium that has been used for the production of molybdenum-99 involves irradiating a solution of uranium suitable for forming fission products including molybdenum-99, conditioning the irradiated solution to one suitable for inducing the formation of crystals of uranyl nitrate hydrates, then forming the crystals and a supernatant and then separating the crystals from the supernatant, thus using the crystals as a source of uranium for recycle. Molybdenum-99 is recovered from the supernatant using an adsorbent such as alumina. Another process involves irradiation of a solid target comprising uranium, forming an acidic solution from the irradiated target suitable for inducing the formation of crystals of uranyl nitrate hydrates, then forming the crystals and a supernatant and then separating the crystals from the supernatant, thus using the crystals as a source of uranium for recycle. Molybdenum-99 is recovered from the supernatant using an adsorbent such as alumina.

Claims (43)

1. A process for recycling uranium that has been used for the production of molybdenum-99 (Mo-99), comprising:

providing an aqueous solution comprising a first nitric acid concentration and a first uranium concentration;

irradiating the aqueous solution to produce soluble fission products comprising Mo-99;

adjusting the first uranium concentration to a second uranium concentration suitable for formation of uranyl nitrate hydrate crystals;

adding an inorganic oxidant to the aqueous solution to ensure that the Mo-99 is in a +VI oxidation state;

inducing the formation of uranyl nitrate hydrate crystals and a supernatant; and

separating the uranyl nitrate hydrate crystals from the supernatant.

2. The process of claim 1 , wherein the uranium is low enriched uranium.

3. The process of claim 1 , wherein the inducing the formation of uranyl nitrate hydrate crystals comprises cooling the aqueous solution to a temperature effective for the formation of the uranyl nitrate hydrate crystals.

4. The process of claim 1 , wherein the inducing formation of uranyl nitrate hydrate crystals comprises evaporating the aqueous solution under reduced pressure.

5. The process of claim 1 , further comprising separating the Mo-99 from the supernatant after separating the uranyl nitrate hydrate crystals from the supernatant.

6. The process of claim 1 , further comprising purifying the uranyl nitrate hydrate crystals after separating the uranyl nitrate hydrate crystals from the supernatant.

7. A process for recycling uranium that has been used for the production of Mo-99, comprising:

providing an aqueous solution comprising a nitric acid concentration of about 0.01 M to about 0.5 M, and a uranium concentration of about 80 to 310 gU/L;

irradiating the aqueous solution to produce soluble fission products comprising Mo-99;

adjusting the nitric acid concentration to about 4 M to about 8 M and the uranium concentration to about 350 to 650 gU/L;

adding an inorganic oxidant to the aqueous solution to ensure that the Mo-99 is in a +VI oxidation state;

inducing formation of uranyl nitrate hydrate crystals and a supernatant; and

separating the uranyl nitrate hydrate crystals from the supernatant, the supernatant comprising the soluble fission products.

8. The process of claim 7 , wherein the uranium is low enriched uranium.

9. The process of claim 7 , wherein the inducing the formation of uranyl nitrate hydrate crystals comprises cooling the aqueous solution to a temperature effective for the formation of the uranyl nitrate hydrate crystals.

10. The process of claim 7 , wherein the inducing formation of uranyl nitrate hydrate crystals comprises evaporating the aqueous solution under reduced pressure.

11. The process of claim 7 , further comprising separating the Mo-99 from the supernatant after separating the uranyl nitrate hydrate crystals from the supernatant.

12. The process of claim 7 , further comprising purifying the uranyl nitrate hydrate crystals after separating the uranyl nitrate hydrate crystals from the supernatant.

13. The process of claim 7 , further comprising:

preparing a second aqueous solution from the uranyl nitrate hydrate crystals, the second aqueous solution comprising a second nitric acid concentration of about 0.01 M to about 0.5 M, and a second uranium concentration of about 80 to 310 gU/L;

irradiating the second aqueous solution to produce soluble fission products comprising Mo-99;

adjusting the second nitric acid concentration to about 4 M to about 8 M, and the second uranium concentration to about 350 to 650 gU/L;

inducing formation of a second batch of uranyl nitrate hydrate crystals and a second supernatant from the second aqueous solution, the second supernatant comprising soluble fission products comprising Mo-99; and

separating the second batch of uranyl nitrate hydrate crystals from the second supernatant.

14. The process of claim 13 , further comprising separating Mo-99 from the second supernatant.

15. A process for recycling uranium that has been used for the production of Mo-99, comprising:

irradiating a solid target comprising uranium to produce fission products comprising Mo-99;

forming an aqueous acidic solution from the solid target, the aqueous acidic solution comprising a uranium concentration and a nitric acid concentration;

adjusting the nitric acid concentration to about 4 M to about 8 M, and the uranium concentration to about 350 to 650 gU/L;

inducing formation of uranyl nitrate hydrate crystals and a supernatant;

adding an inorganic oxidant to the supernatant to ensure that the Mo-99 is in a +VI oxidation state; and

separating the uranyl nitrate hydrate crystals from the supernatant.

16. The process of claim 15 , wherein the uranium is low enriched uranium.

17. The process of claim 15 , wherein the inducing formation of uranyl nitrate hydrate crystals comprises cooling the aqueous acidic solution to a temperature effective for formation of the uranyl nitrate hydrate crystals.

18. The process of claim 15 , wherein the inducing formation of uranyl nitrate hydrate crystals comprises evaporating the aqueous acidic solution under reduced pressure.

19. The process of claim 15 , further comprising separating Mo-99 from the supernatant after separating the uranyl nitrate hydrate crystals from the supernatant.

20. The process of claim 15 , further comprising purifying the uranyl nitrate hydrate crystals after separating the uranyl nitrate hydrate crystals from the supernatant.

Assignments (3)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 1, 2018
From: LOS ALAMOS NATIONAL SECURITY, LLC
To: TRIAD NATIONAL SECURITY, LLC
Reel/Frame 047401/0957 →
CONFIRMATORY LICENSE Recorded Nov 27, 2015
From: LOS ALAMOS NATIONAL SECURITY
To: U.S. DEPARTMENT OF ENERGY
Reel/Frame 037149/0445 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 30, 2013
From: REILLY, SEAN DOUGLAS; MAY, IAIN; COPPING, ROY; DALE, GREGORY EDWARD
To: LOS ALAMOS NATIONAL SECURITY, LLC
Reel/Frame 031308/0410 →