IP Library Granted Patent US 11,433,353
Granted Patent B2
US 11,433,353 · App. 16/433,500 · Granted Sep 6, 2022

Hydrogen isotope separation methods and systems

Inventors: Dale A. Hitchcock (Aiken, SC); Steven M. Serkiz (Aiken, SC); Timothy M. Krentz (Aiken, SC); Josef A. Velten (Dallas, TX); Kyle S. Brinkman (Clemson, SC); Eric M. Vogel (Marietta, GA); Katherine T. Young (Atlanta, GA)
Assignees: Savannah River Nuclear Solutions, LLC; Clemson University Research Foundation; Georgia Tech Research Corporation
B01D59/42B01D59/14B01D71/02B01D71/021B01D71/022B01D71/024B01D71/025B01D71/027C01B4/00
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Quick Facts
Patent No.
US 11,433,353
App. No.
16/433,500
Granted
Sep 6, 2022
Kind
B2
Abstract

Methods and systems for the separation of hydrogen isotopes from one another are described. Methods include utilization of a hydrogen isotope selective separation membrane that includes a hydrogen isotope selective layer (e.g., graphene) and a hydrogen ion conductive supporting layer. An electronic driving force encourages passage of isotopes selectively across the membrane at an elevated separation temperature to enrich the product in a selected hydrogen isotope.

Claims (21)

1. A method for separating hydrogen isotopes from one another comprising:

contacting a first side of a separation membrane with a sample, the sample comprising water in an amount of about 0.03 kg/m 3 or less, the sample including a first hydrogen isotope and a second hydrogen isotope, the separation membrane comprising a first layer and a second layer, the first layer comprising a crystalline material of from one to about 5 atomic or molecular layers and a metal selected from Groups 8 to 10 of the periodic table, wherein the metal reduces a thermal conduction barrier of the separation membrane, wherein the metal is present in a discontinuous fashion on a surface of the first layer, the second layer comprising a hydrogen ion conductive ceramic;

heating the separation membrane to a separation temperature of about 200° C. or greater; and

applying a voltage across the heated separation membrane from the first side of the separation membrane to the second side of the separation membrane, the voltage providing a driving force to selectively conduct the first hydrogen isotope across the separation membrane from the first side to the second side, thereby forming a product on the second side of the separation membrane that is enriched in the first hydrogen isotope, a remaining sample on the first side of the separation membrane being enriched in the second hydrogen isotope.

2. The method of claim 1 , the sample further comprising a third hydrogen isotope, wherein the remaining sample on the first side of the separation membrane is enriched in the second hydrogen isotope and the third hydrogen isotope.

3. The method of claim 1 , wherein the first hydrogen isotope comprises protium and the second hydrogen isotope comprises deuterium.

4. The method of claim 1 , wherein the first hydrogen isotope comprises protium and the second hydrogen isotope comprises tritium.

5. The method of claim 1 , wherein the voltage is about 20 Volts or less.

6. The method of claim 1 , wherein the separation temperature is from about 200° C. to about 800° C.

7. The method of claim 1 , further comprising contacting a first side of a second separation membrane with the product and applying a voltage across the second separation membrane.

8. The method of claim 7 , further comprising repeating the process with one or more additional separation membranes.

9. The method of claim 1 , the crystalline material comprising graphene, hexagonal boron nitride, or a transition metal chalcogenide.

10. The method of claim 1 , the hydrogen ion conductive ceramic comprising a perovskite type ceramic.

11. The method of claim 1 , wherein the sample comprises water in an amount of about 0.02 kg/m 3 or less.

12. The method of claim 1 , wherein the sample is a dry sample.

13. The method of claim 1 , wherein at least one layer of the crystalline material includes atoms in a hexagonal pattern.

14. The method of claim 10 , wherein the perovskite type ceramic comprises BaZrO 3 , BaCeO 3 , SrCeO 3 , CaZrO 3 , SrZRO 3 , or BaCe 0.7 Zr 0.1 Y 0.1 Yb 0.1 O 3-δ .

15. The method of claim 3 , wherein the method separates the protium from the deuterium with a single step separation factor of about 3.3 or greater.

16. The method of claim 4 , wherein the method separates the protium form the tritium with a single step separation factor of from about 10 to about 30.

17. The method of claim 1 , wherein the voltage is about 5 Volts or less.

18. The method of claim 1 , the crystalline material comprising graphene, wherein the graphene further functions as an electrode in application of the voltage across the heated separation membrane.

Assignments (9)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Dec 14, 2022
From: SAVANNAH RIVER NUCLEAR SOLUTIONS, LLC
To: BATTELLE SAVANNAH RIVER ALLIANCE, LLC
Reel/Frame 062083/0187 →
CONFIRMATORY LICENSE Recorded Feb 16, 2022
From: CLEMSON UNIVERSITY
To: UNITED STATES DEPARTMENT OF ENERGY
Reel/Frame 059168/0279 →
CONFIRMATORY LICENSE Recorded Aug 20, 2019
From: SAVANNAH RIVER NUCLEAR SOLUTIONS, LLC
To: U.S. DEPARTMENT OF ENERGY
Reel/Frame 050098/0451 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 25, 2019
From: CLEMSON UNIVERSITY
To: CLEMSON UNIVERSITY RESEARCH FOUNDATION
Reel/Frame 049572/0956 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 10, 2019
From: OAK RIDGE ASSOCIATED UNIVERSITIES, INC.
To: SAVANNAH RIVER NUCLEAR SOLUTIONS, LLC
Reel/Frame 049417/0241 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 6, 2019
From: VELTEN, JOSEF
To: OAK RIDGE ASSOCIATED UNIVERSITIES, INC.
Reel/Frame 049395/0668 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 6, 2019
From: HITCHCOCK, DALE A.; SERKIZ, STEVEN M.; KRENTZ, TIMOTHY M.
To: SAVANNAH RIVER NUCLEAR SOLUTIONS, LLC
Reel/Frame 049395/0785 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 6, 2019
From: BRINKMAN, KYLE S.
To: CLEMSON UNIVERSITY
Reel/Frame 049403/0223 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 6, 2019
From: VOGEL, ERIC M.; YOUNG, KATHERINE T.
To: GEORGIA TECH RESEARCH CORPORATION
Reel/Frame 049395/0422 →
Continuity (1)
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