Process and composition for the immobilization of radioactive and hazardous wastes in borosilicate glass

• US 7,550,645 B2
• Filed: 01/18/2006
• Issued: 06/23/2009
• Est. Priority Date: 02/23/2004
• Status: Expired due to Fees

• Current Assignee: Geomatrix Solutions, Inc.
• Original Assignee: Geomatrix Solutions, Inc.
• Inventors: Chekhmir, Anatoly, Gribetz, Arthur
• Primary Examiner(s): Mayes; Melvin C
• Assistant Examiner(s): Gregorio; Guinever S
• Application Number:
  US11/333,236
• Publication Number:
  US 20060189471A1
• Time in Patent Office: 1,252 Days
• Field of Search: None
• US Class Current: 588/11
• CPC Class Codes: C03C 1/002 Use of waste materials, e.g. slags
• CPC Class Codes: C03C 3/072 containing boron
• CPC Class Codes: C03C 3/074 containing zinc

Abstract

The present invention provides processes to immobilize radioactive and/or hazardous waste in a borosilicate glass, the waste containing one or more of radionuclides, hazardous elements, hazardous compounds, and/or other compounds. The invention also provides borosilicate glass compositions for use in immobilizing radioactive and/or hazardous waste.

Claims

1. A process for immobilizing wastes in glass which achieves a high concentration of waste constituents (waste loading) comprising:

combining a waste stream having one or more of radionuclides, hazardous elements, and hazardous components with fluorine and glass-forming components in proportion to achieve a mixture capable of forming a highly polymerized borosilicate glass consisting essentially of about 1 to about 1.3 mole parts of a combination of monovalent cation oxides (R₂O) and divalent cation oxides (RO), about 1 to about 1.4 mole parts trivalent cation oxides (R₂O₃), and about 1.2 to about 4.2 mole parts of a combination of tetravalent cation oxides (RO₂) and pentavalent cation oxides (R₂O₅), wherein SiO₂ is present in an amount greater than 30 weight percent, B₂O₃ is present in an amount between 8.7 and 15.3 weight percent, Al₂O₃ present in an amount between 7 and 15.1 weight percent, CaO is present in an amount between 0.2 and 2.3 weight percent, and fluorine is present in an amount between about 1 to about 3 weight percent;

melting the mixture to form a melted glass with integrated waste; and

solidifying the melted glass with integrated waste by cooling to form said highly polymerized borosilicate glass.

3. The process of claim 1 or claim 2, wherein said melting step is performed at temperatures up to about 1200 degrees Celsius.

4. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass is peraluminous.

5. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass has a viscosity of 2 to 10 Pascal second at a temperature of about 1150 to about 1200 degrees Celsius.

6. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass has a calculated degree of polymerization (K) less than about 15.

7. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass has a calculated degree of polymerization (K) less than about 7.

8. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass has crystallinity of less than 1 volume percent at about 1150 degrees Celsius, and crystallinity of up to 2 volume percent after three days at about 950 degrees Celsius.

9. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass has specific electrical resistivity ranging between about 1.4 Ω

cm to about 10 Ω

cm at about 1150 degrees Celsius, that is acceptable for processing in vitrification melters.

10. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass meets the leaching requirements of less than about 1.19 grams per square meter per day for boron, less than about 0.69 grams per square meter per day for lithium, and less than about 0.95 grams per square meter per day for sodium, for acceptance in U.S. high-level waste repositories.

11. The borosilicate glass produced by the process of claim 1 or claim 2, wherein the borosilicate glass contains fluorine in an amount between about 1.2 and about 2.5 weight percent.

2. A process for immobilizing wastes comprising:

combining a waste stream having one or more of radionuclides, hazardous elements, and hazardous components with fluorine and glass-forming components in proportion to achieve a mixture capable of forming a highly polymerized borosilicate glass consisting essentially of about 1 to about 1.3 mole parts of a combination of monovalent cation oxides (R₂O) and divalent cation oxides (RO), including alkaline oxides and alkaline earth oxides, about 1 to about 1.4 mole parts trivalent cation oxides (R₂O₃), including alumina, boric oxide, and ferric oxide, and about 1.2 to about 4.2 mole parts of a combination of tetravalent cation oxides (RO₂) and pentavalent cation oxides (R₂O₅), including silica, zirconia, titania, and phosphoric oxide, wherein SiO₂ is present in an amount greater than 30 weight percent, B₂O₃ is present in an amount between 8.7 and 15.3 weight percent, Al₂O₃ is present in an amount between 7 and 15.1 weight percent, CaO is present in an amount between 0.2 and 2.3 weight percent, and fluorine is present in an amount between about 1 to about 3 weight percent;

melting the mixture to form a melted glass with integrated waste; and

solidifying the melted glass with integrated waste by cooling to form said highly polymerized borosilicate glass.