IP Library Granted Patent US 12,421,115
Granted Patent B1
US 12,421,115 · App. 17/854,307 · Granted Sep 23, 2025

Separation of krypton gas from xenon gas using natural clinoptilolite

Inventors: Guangping Xu (Albuquerque, NM); Matthew J. Paul (Albuquerque, NM); Jeffery A. Greathouse (Albuquerque, NM)
Assignee: National Technology & Engineering Solutions of Sandia, LLC
C01B23/0068B01D53/0462B01D53/0476B01J20/165B01J20/3408B01J20/3483B01J20/3491C01B23/0078B01D53/047B01D2253/108B01D2256/18B01D2257/11C01B2210/0018C01B2210/0035C01B2210/0037
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Quick Facts
Patent No.
US 12,421,115
App. No.
17/854,307
Granted
Sep 23, 2025
Kind
B1
Abstract

A system and method for separating Kr gas from Xe gas utilizing natural clinoptilolite. The method includes separating Kr gas from Xe gas by selectively adsorbing Kr gas. The method includes providing a vessel comprising a Kr adsorbent bed comprising a natural clinoptilolite adsorbent. A feed gas comprising Kr gas and Xe gas is exposed to the Kr adsorbent bed for a residence time to selectively adsorb sufficient Kr gas from the feed gas to form a Xe enriched gas raffinate product. The Xe enriched gas raffinate product is removed from the vessel. Thereafter, the Kr adsorbent bed is regenerated to release a Kr enriched gas extract product.

Claims (32)

1. A method for separating Kr gas from Xe gas by selectively adsorbing Kr gas, the method comprising:

providing a vessel comprising a Kr adsorbent bed comprising a natural clinoptilolite adsorbent;

exposing a feed gas comprising Kr gas and Xe gas to the adsorbent bed for a residence time to selectively adsorb sufficient Kr gas from the feed gas to form a Xe enriched gas raffinate product;

removing the Xe enriched gas raffinate product from the vessel; and

thereafter regenerating the Kr adsorbent bed to form a Kr enriched gas extract product.

2. The method of claim 1 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the Kr adsorbent bed is for a time sufficient to maintain a greater Kr uptake amount than Xe uptake amount for the Kr adsorbent bed.

3. The method of claim 1 , wherein the residence time to selectively adsorb the Kr gas is less than or equal to 70% of the total time to equilibrium of Kr gas within the Kr adsorbent bed.

4. The method of claim 1 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the Kr adsorbent bed is for a time equal to or less than 1 hour.

5. The method of claim 1 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the Kr adsorbent bed is for a time equal to or less than 30 minutes.

6. The method of claim 1 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the Kr adsorbent bed is for a time equal to or less than 15 minutes.

7. The method of claim 1 , wherein the regenerating includes drawing a vacuum on the vessel.

8. The method of claim 1 , wherein the regenerating includes heating the Kr adsorbent bed to a temperature sufficient to release adsorbed Kr gas.

9. A method for purifying Kr gas and Xe gas comprising:

providing a vessel comprising a first Kr adsorbent bed comprising a natural clinoptilolite adsorbent;

exposing a feed gas comprising Kr gas and Xe gas to the first Kr adsorbent bed for a residence time to selectively adsorb sufficient Kr gas from the feed gas to form a Xe enriched gas raffinate product;

removing the Xe enriched gas raffinate product from the vessel and providing the Xe enriched gas raffinate product to an Xe adsorbent bed and exposing the Xe enriched gas raffinate product to the Xe adsorbent bed for a residence time to selectively adsorb sufficient Xe gas from the feed gas-Xe enriched gas raffinate product to form a purified Xe stream; and

thereafter regenerating the Kr adsorbent bed to form a Kr enriched gas extract product and providing the Kr enriched gas extract product to a second Kr adsorbent bed for a residence time to selectively adsorb sufficient Kr gas from the feed gas to form a purified Kr stream.

10. The method of claim 9 , further comprising providing the purified Xe stream to a second Xe adsorbent bed to further purify the purified Xe stream.

11. The method of claim 9 , further comprising providing the purified Kr stream to a third Kr adsorbent bed to further purify the purified Kr stream.

12. The method of claim 9 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the first Kr adsorbent bed is for a time sufficient to maintain a greater Kr uptake amount than Xe uptake amount for the first Kr adsorbent bed.

13. The method of claim 9 , wherein the residence time to selectively adsorb the Kr gas is less than or equal to 70% of the total time to equilibrium of Kr gas within the first Kr adsorbent bed.

14. The method of claim 9 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the first Kr adsorbent bed is for a time equal to or less than 1 hour.

15. The method of claim 9 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the first Kr adsorbent bed is for a time equal to or less than 30 minutes.

16. The method of claim 9 , wherein the residence time for exposing the feed gas comprising Kr gas and Xe gas to the first Kr adsorbent bed is for a time equal to or less than 15 minutes.

17. The method of claim 9 , wherein the Xe adsorbent bed comprises mordenite.

18. A system for separating Kr gas from Xe gas comprising:

a vessel containing a Kr adsorbent bed comprising natural clinoptilolite adsorbent;

a first valve arrangement arranged and disposed to remove a Xe enriched gas raffinate product stream from the vessel after a feed gas exposure to the Kr adsorbent bed; and

a second valve arrangement and a regenerator arranged and disposed to regenerate the Kr adsorbent bed and release a Kr enriched gas extract product stream;

wherein is configured such that the feed gas can be exposed to the Kr adsorbent bed for a residence time to selectively adsorb sufficient Kr gas so the Xe enriched gas raffinate product can be removed; and

thereafter the Kr adsorbent bed can be regenerated to form a Kr enriched gas extract product.

19. The system of claim 18 , wherein the regenerator is a vacuum pump.

Assignments (3)
CONFIRMATORY LICENSE Recorded Dec 11, 2025
From: NATIONAL TECHNOLOGY & ENGINEERING SOLUTIONS OF SANDIA, LLC
To: NNSA
Reel/Frame 073194/0070 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jul 27, 2022
From: XU, GUANGPING; PAUL, MATTHEW J.; GREATHOUSE, JEFFERY A.
To: NATIONAL TECHNOLOGY & ENGINEERING SOLUTIONS OF SANDIA, LLC
Reel/Frame 060637/0460 →
CONFIRMATORY LICENSE Recorded Jul 19, 2022
From: NATIONAL TECHNOLOGY & ENGINEERING SOLUTIONS OF SANDIA, LLC
To: U.S. DEPARTMENT OF ENERGY
Reel/Frame 060548/0445 →
References Cited (14)
US 5587003A · Bulow et al. · 1996 [cited by applicant]
US 5938819A · Seery · 1999 [cited by applicant]
US 20240100470A1 · Dasappa · 2024 [cited by examiner]
JP 2000171589A · 2020 [cited by examiner]
JP2000171589A_ENG (Espacenet machine translation of Munakata) (Year: 2000). [cited by examiner]
Z. Niu et al., “Self-Adjusting Metal-Organic Framework for Efficient Capture of Trace Xenon and Krypton”, Angew. Chem. Int. Ed. (2022) 61, e202117807, pp. 1-5. [cited by applicant]
J. Feldman et al., “Effects of Natural Zeolites on Field-Scale Geologic Noble Gas Transport”, Journal of Environmental Radioactivity (2020), 220-221, 106279, 10 pages. [cited by applicant]
S.K. Elsaidi et al., “Radiation-Resistant Metal-Organic Framework Enables Efficient Separation of Krypton Fission Gas From Spent Nuclear Fuel”, Nature Communications (2020) 11:3103, pp. 1-8, https://doi.org/10.1038/s414… [cited by applicant]
T. Wu et al., “Microporous Crystalline Membranes for KR/XE Separation: Comparison Between AIPO-18, SAPO-34, and ZIF-8”, ACS Applied Nano Materials (2018) 1:463-470. [cited by applicant]
S. Bhadra et al., “Ideal Cascade Theory Applied to Carbon Monoxide Isotope Separation by Pressure Swing Adsorption”, Adsorption (2015) 21:467-478. [cited by applicant]
J. Liu et al., “A Two-Column Method for the Separation of KR and XE From Process Off-Gases”, Industrial & Engineering Chemistry Research (2014) 53:12893-12899. [cited by applicant]
P. Ryan et al., “Computational Screening of Metal-Organic Frameworks for Xenon/Krypton Separation”, AIChE Journal (2011) 57(7):1759-1766. [cited by applicant]
F. Pechar et al., “Thermal Decomposition of Natural Mordenite”, Chem. Papers (1987) 41(3):351-362. [cited by applicant]
G. Aguilar-Armenta et al. “Adsorption Kinetic Behaviour of Pure CO2, N2 and CH4 in Natural Clinoptilolite at Different Temperatures”, Adsorption Science-Technology (2003) 21(1):81-91, https://doi.org/10.1260/02636170360… [cited by applicant]