Apparatus and process for the electrolytic reduction of uranium and plutonium oxides

• US 4,995,948 A
• Filed: 07/24/1989
• Issued: 02/26/1991
• Est. Priority Date: 07/24/1989
• Status: Expired due to Fees

• Current Assignee: United States Department Of Health And Human Services
• Original Assignee: United States Department of Energy
• Inventors: Tomczuk, Zygmunt, Burris, Leslie, Steunenberg, Robert K., Poa, David S.
• Primary Examiner(s): Valentine, Donald R.
• Application Number:
  US07/384,195
• Time in Patent Office: 582 Days
• Field of Search: 204/1.5, 204/64 R, 204/240, 204/245, 204/246, 204/273, 204/292, 204/243 R, 204/247, 204/294, 204/241
• US Class Current: 205/47
• CPC Class Codes: C25C 3/34 of metals not provided for in groups C25C3/02 - C25C3/32
• CPC Class Codes: C25C 7/005 of cells for the electrolysis of melts C25C7/02 - C25C7/06 take precedence

Abstract

An apparatus and process for reducing uranium and/or plutonium oxides to produce a solid, high-purity metal. The apparatus is an electrolyte cell consisting of a first container, and a smaller second container within the first container. An electrolyte fills both containers, the level of the electrolyte in the first container being above the top of the second container so that the electrolyte can be circulated between the containers. The anode is positioned in the first container while the cathode is located in the second container. Means are provided for passing an inert gas into the electrolyte near the lower end of the anode to sparge the electrolyte and to remove gases which form on the anode during the reduction operation. Means are also provided for mixing and stirring the electrolyte in the first container to solubilize the metal oxide in the electrolyte and to transport the electrolyte containing dissolved oxide into contact with the cathode in the second container. The cell is operated at a temperature below the melting temperature of the metal product so that the metal forms as a solid on the cathode.

Claims

1. An apparatus for electrolytically reducing metal oxides selected from the group consisting of uranium and plutonium to solid, high-purity metal comprising:

an electrolytic cell having a first container for receiving an electrolyte,

a relatively smaller second container, having an open top, located within the first container,

an electrolyte in the first and second containers for receiving and solubilizing the oxides to be reduced, the level of the electrolyte in the first container being above the top of the second container,

a rod-shaped carbon anode having a lower end extending into the electrolyte in the first container,

gas delivery means for delivering a supply of inert gas into the electrolyte near the lower end of the anode to sparge the electrolyte and sweep gases from the surface of the anode,

an outer concentric, tubular-shaped shield enclosing the anode, the shield having a lower end extending into the electrolyte in the first container, said tube being spaced from the anode to form an annular space therebetween for removing gases which form on the anode from the cell,

a cathode having a lower end extending into the electrolyte in the second container,

heating means for melting the electrolyte,

means for passing a current between the anode and cathode, and

mixing means in the first container for mixing and stirring the electrolyte to dissolve the oxides and for moving the electrolyte containing the dissolved oxides into contact with the cathode in the second container, whereby the oxides in the electrolyte are reduced to high-purity metal which forms as a solid on the cathode within the second chamber.

2. The apparatus of claim 1 wherein the gas delivery means is a tube extending down the annular space between the shielding tube and the anode.

3. The apparatus of claim 2 wherein the electrolyte consists of one or more members selected from the group consisting of LiF, KF, NaF, CaF₂, BaF₂, and MgF₂, and also contains UF₄.

4. The apparatus of claim 3 wherein the cathode is constructed of a material selected from the group consisting of molybdenum and uranium.

5. The apparatus of claim 2 wherein the mixing means in the first container is a paddle stirrer having blades extending from a control rotatable shaft and includes means for rotating the shaft.

6. The apparatus of claim 5 wherein the electrolyte is about 45.6 mole % LiF, 41.2 mole % KF 11.7 mole % NaF and 1.5 mole % CaF₂, and contains about 6 to 8 mole % UF₄.

7. A process for electrolytically reducing metal oxides selected from the group consisting of uranium and plutonium to high-purity solid metal comprising:

providing an electrolytic cell having a first container, a relatively smaller second container within the first container, an electrolyte in the cell filling both containers, the level of the electrolyte in the first container being above the top of the second container, an anode in the electrolyte in the first container, means in the electrolyte for passing a sparging gas over the anode, a cathode in the electrolyte in the second container, stirring means in the first container for stirring and mixing the electrolyte and for circulating the electrolyte between the two chambers,

heating the electrolyte to a temperature between 900 degrees C and the melting temperature of the metal to be produced,

adding the metal oxide to the heated electrolyte in the first chamber,

electrolytically reducing the metal oxide to metal while stirring and mixing the electrolyte in the first container and circulating the electrolyte containing the dissolved oxides between the chambers, whereby high-purity metal forms as a solid on the cathode within the second chamber.

8. The method of claim 7 wherein the electrolyte consists of one or more members selected from the group consisting of LiF, KF, NaF, CaF₂, BaF₂, and MgF₂, and also contains UF₄.

9. The method of claim 8 wherein the electrolyte is about 45.6 mole % LiF, 41.2 mole % KF 11.7 mole % NaF and 1.5 mole % CaF₂, and contains about 6 to 8 mole % UF₄.

10. The method of claim 9 wherein the metal oxides are uranium oxides and the electrolyte is heated to between 900°

C. and 1130°

C.

11. The method of claim 10 wherein the electrolyte is heated to between 950°

C. and 1000°

C.