CA2344671A1 - Hyperpolarized noble gas extraction methods, masking methods, and associated transport containers - Google Patents
Hyperpolarized noble gas extraction methods, masking methods, and associated transport containers Download PDFInfo
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- CA2344671A1 CA2344671A1 CA002344671A CA2344671A CA2344671A1 CA 2344671 A1 CA2344671 A1 CA 2344671A1 CA 002344671 A CA002344671 A CA 002344671A CA 2344671 A CA2344671 A CA 2344671A CA 2344671 A1 CA2344671 A1 CA 2344671A1
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- container
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
- G01R33/00—Arrangements or instruments for measuring magnetic variables
- G01R33/20—Arrangements or instruments for measuring magnetic variables involving magnetic resonance
- G01R33/28—Details of apparatus provided for in groups G01R33/44 - G01R33/64
- G01R33/282—Means specially adapted for hyperpolarisation or for hyperpolarised contrast agents, e.g. for the generation of hyperpolarised gases using optical pumping cells, for storing hyperpolarised contrast agents or for the determination of the polarisation of a hyperpolarised contrast agent
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K49/00—Preparations for testing in vivo
- A61K49/06—Nuclear magnetic resonance [NMR] contrast preparations; Magnetic resonance imaging [MRI] contrast preparations
- A61K49/18—Nuclear magnetic resonance [NMR] contrast preparations; Magnetic resonance imaging [MRI] contrast preparations characterised by a special physical form, e.g. emulsions, microcapsules, liposomes
- A61K49/1806—Suspensions, emulsions, colloids, dispersions
- A61K49/1815—Suspensions, emulsions, colloids, dispersions compo-inhalant, e.g. breath tests
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T436/00—Chemistry: analytical and immunological testing
- Y10T436/11—Automated chemical analysis
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T436/00—Chemistry: analytical and immunological testing
- Y10T436/24—Nuclear magnetic resonance, electron spin resonance or other spin effects or mass spectrometry
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T436/00—Chemistry: analytical and immunological testing
- Y10T436/25—Chemistry: analytical and immunological testing including sample preparation
Abstract
Methods of extracting and removing hyperpolarized gas from a container inclu de introducing an extraction fluid into the container to force the hyperpolariz ed gas out of an exit port. The hyperpolarized gas is forced out of the contain er separate and apart from the extraction fluid. Alternatively, if the fluid is a gas, a portion of the gas is mixed with the hyperpolarized gas to form a sterile mixed fluid product suitable for introduction to a patient. An additional method includes engaging a gas transfer source such as a syringe to a transport container and pulling a quantity of the hyperpolarized gas out o f the container in a controlled manner. Another method includes introducing a quantity of liquid into a container and covering at least one predetermined internal surface or component with the liquid to mask the surfaces and keep the hyperpolarized gas away from the predetermined internal surface, thereby inhibiting any depolarizing affect from same. Examples of surfaces or components suitable for masking include valves, seals, and the like. Yet another extraction method includes expanding a resilient member inside the container to force the hyperpolarized gas to exit therefrom. Containers include a resilient member positioned in fluid communication with the hyperpolarized gas in the container. An additional container includes inlet and outlet ports in fluid communication with the chamber and positioned on opposing sides or end portions of the container. Another container includes a port configured to receive a portion of a syringe therein. An additional aspect of the disclosure relates to calibration methods and apparatus for identifying the hyperpolarization status of the gas.
Claims (67)
1. A method of extracting hyperpolarized noble gas from a container, comprising the steps of:
introducing liquid into a container holding a quantity of hyperpolarized noble gas;
contacting the hyperpolarized gas in the container with the liquid; and removing the hyperpolarized gas from the container separate from the liquid.
introducing liquid into a container holding a quantity of hyperpolarized noble gas;
contacting the hyperpolarized gas in the container with the liquid; and removing the hyperpolarized gas from the container separate from the liquid.
2. A method according to Claim 1, wherein the liquid is substantially de-oxygenated prior to said introducing step.
3. A method according to Claim 1, wherein the liquid is at least partially de-oxygenated and de-ionized prior to said introducing step.
4. A method according to Claim 3, wherein the liquid comprises water.
5. A method according to Claim 1, wherein the liquid is sterile and non-toxic.
6. A method according to Claim 4, wherein the liquid is substantially non-depolarizing to the hyperpolarized noble gas such that the gas retains sufficient hyperpolarization after extraction to produce clinically useful magnetic resonance images.
7. A method according to Claim 5, wherein the hyperpolarized noble gas has an associated hyperpolarized life, and wherein said removing step is minimally depolarizing to the hyperpolarized gas such that the hyperpolarized gas retains at least 90% of the initial polarization, the initial polarization measured immediately prior to extraction.
8. A method according to Claim 1, wherein said introducing step is performed by injecting a quantity of liquid into the container with a syringe.
9. A method according to Claim 1, wherein said introducing step comprises gravimetrically introducing a liquid source in fluid communication with the container.
10. A method according to Claim 1, wherein the hyperpolarized gas is resistant to dissolution in the liquid.
11. A method according to Claim 1, wherein the hyperpolarized gas is non-toxic and directed to a medical delivery system far introduction into a patient via inhalation.
12. A method according to Claim 1, wherein the hyperpolarized noble gas is one of 3He and 129Xe.
13. A method according to Claim 1, wherein the liquid comprises at least partially de-oxygenated and de-ionized water, and wherein the hyperpolarized noble gas is 3He.
14. A method according to Claim 1, wherein the liquid is sterile, and wherein the hyperpolarized gas is substantially insoluble in the liquid.
15. A method according to Claim 1, wherein the container includes an liquid entry port and a gas exit port, the gas exit port is in fluid communication with the exit path, and the exit port is positioned on the container such that it is on the opposing side of the container from and above the entry port.
16. A method for removing hyperpolarized noble gas from a container, comprising the steps of:
introducing fluid into a container holding a quantity of hyperpolarized noble gas;
contacting the hyperpolarized gas in the container with the fluid; and removing at least a portion of the hyperpolarized gas from the container by forcing the hyperpolarized gas to flowably exit the container responsive to said step of introducing fluid into the container.
introducing fluid into a container holding a quantity of hyperpolarized noble gas;
contacting the hyperpolarized gas in the container with the fluid; and removing at least a portion of the hyperpolarized gas from the container by forcing the hyperpolarized gas to flowably exit the container responsive to said step of introducing fluid into the container.
17. A method according to Claim 16, wherein the fluid is a non-toxic gas.
18. A method according to Claim 16, wherein the fluid is a non-toxic liquid, and wherein the hyperpolarized noble gas exits the container substantially separate and apart from the liquid.
19. A method according to Claim 17, wherein the hyperpolarized noble gas exits the container substantially separate and apart from the extraction gas, and wherein the extraction gas has a density which is substantially different from the hyperpolarized gas to minimize mixing of the hyperpolarized gas and the extraction gas.
20. A method according to Claim 17, wherein the hyperpolarized gas is 129Xe which has a first density associated therewith and the extraction gas has a second density associated therewith, wherein said first density is greater than said second density.
21. A method according to Claim 17, wherein the hyperpolarized gas is 3He which has a first density associated therewith and the extraction gas has a second density associated therewith, wherein said first density is less than said second density.
22. A method according to Claim 17, wherein at least some of the extraction gas exits the container with the hyperpolarized gas to form a gas mixture suitable for patient inhalation.
23. A method of extracting a quantity of hyperpolarized noble gas from a container configured to hold a quantity of hyperpolarized gas therein, comprising the steps of:
engaging a hyperpolarized gas transfer source to the container having a quantity of hyperpolarized noble gas in a gaseous state releasably held therein;
extracting a first quantity of hyperpolarized noble gas held in the container in a gaseous state into an exit path comprising the gas transfer source sealably connected to the container such that the hyperpolarized noble gas is directed out of the container and into the gas transfer source, wherein the gas transfer source extracts the first quantity of hyperpolarized noble gas in the gaseous state such that the first quantity of hyperpolarized gas is substantially isolated from contact with liquid during said extracting step; and capturing, after said extracting step, a second quantity of hyperpolarized gas within the container, the second quantity being a portion of the first quantity.
engaging a hyperpolarized gas transfer source to the container having a quantity of hyperpolarized noble gas in a gaseous state releasably held therein;
extracting a first quantity of hyperpolarized noble gas held in the container in a gaseous state into an exit path comprising the gas transfer source sealably connected to the container such that the hyperpolarized noble gas is directed out of the container and into the gas transfer source, wherein the gas transfer source extracts the first quantity of hyperpolarized noble gas in the gaseous state such that the first quantity of hyperpolarized gas is substantially isolated from contact with liquid during said extracting step; and capturing, after said extracting step, a second quantity of hyperpolarized gas within the container, the second quantity being a portion of the first quantity.
24. A method according to Claim 23, wherein the gas transfer source is a syringe having an internally disposed plunger, wherein said engaging step is performed by inserting the syringe into the container, and wherein said extracting step is performed by refracting the syringe plunger to draw a quantity of the hypeipolarized noble gas in the container into the syringe in a substantially gaseous state.
25. A method according to Claim 23, wherein the gas transfer source is one of a piston, vacuum pump, and syringe.
26. A method according to Claim 24, wherein the container includes a primary body portion and a gas flow path with an access port and a valve positioned between the body of the container and the access port such that it is in fluid communication with the hyperpolarized gas held in the container, and wherein the access port is configured to sealably receive the end of the syringe therein.
27. A method according to Claim 23, wherein the gas transfer source has gas contact surfaces which are formed of materials which are friendly to polarization, thereby reducing the loss of polarization attributed to contact-induced relaxation.
28. A method according to Claim 24, wherein the method further comprises the steps of:
obtaining a collapsible patient delivery bag or inhalation mask;
sealably connecting a coupling member onto the collapsible patient delivery bag or inhalation mask such that the coupling member is intermediate the syringe and the patient delivery bag or inhalation mask;
holding the extracted hyperpolarized gas in the syringe; and expelling the extracted hyperpolarized gas out of the [chamber] syringe into the coupling member such that it then enters the patient delivery bag or inhalation mask.
obtaining a collapsible patient delivery bag or inhalation mask;
sealably connecting a coupling member onto the collapsible patient delivery bag or inhalation mask such that the coupling member is intermediate the syringe and the patient delivery bag or inhalation mask;
holding the extracted hyperpolarized gas in the syringe; and expelling the extracted hyperpolarized gas out of the [chamber] syringe into the coupling member such that it then enters the patient delivery bag or inhalation mask.
29. A method according to Claim 24, wherein the method further comprises expelling the extracted hyperpolarized gas out of the syringe into a patient delivery bag or inhalation mask.
30. A method according to Claim 29, wherein the patient delivery bag has an intake path adapted to receive a portion of the syringe therein, and wherein the method further comprises the step of collapsing the exterior of the patient delivery bag to direct the hyperpolarized gas to be delivered to a subject.
31. A method of masking exposed surfaces to inhibit the depolarizing contact induced relaxation relative to hyperpolarized gases, comprising the steps of:
introducing a quantity of fluid into a container holding hyperpolarized gas therein; and covering at least one predetermined exposed internal surface of the container with the fluid to inhibit direct contact between the predetermined internal surface and the hyperpolarized gas, thereby masking the exposed surface with polarization friendly liquid.
introducing a quantity of fluid into a container holding hyperpolarized gas therein; and covering at least one predetermined exposed internal surface of the container with the fluid to inhibit direct contact between the predetermined internal surface and the hyperpolarized gas, thereby masking the exposed surface with polarization friendly liquid.
32. A method according to Claim 31, wherein the fluid is a liquid, and further comprising the step of orienting the container such that the liquid is directed to the predetermined exposed area.
33. A method according to Claim 31, wherein the predetermined area includes at least one of a seal and a valve.
34. A method according to Claim 32, wherein the liquid comprises de-ionized and de-oxygenated water.
35. A method of decreasing the residual amount of hyperpolarized noble gas in a container, comprising the steps of:
sizing a container to have a volume of less than about 500 cubic centimeters;
introducing a quantity of hyperpolarized noble gas into the container;
increasing the pressure in the container to at least about 3 atm;
sealing the container;
transporting the container from a polarization site to a site remote from the polarization site; and opening the sealed vessel to release the hyperpolarized gas from the container to a patient delivery unit through the equalization of container pressure between the container and the patient delivery unit.
sizing a container to have a volume of less than about 500 cubic centimeters;
introducing a quantity of hyperpolarized noble gas into the container;
increasing the pressure in the container to at least about 3 atm;
sealing the container;
transporting the container from a polarization site to a site remote from the polarization site; and opening the sealed vessel to release the hyperpolarized gas from the container to a patient delivery unit through the equalization of container pressure between the container and the patient delivery unit.
36. A method of removing hyperpolarized gas from a vessel, comprising the steps of:
positioning a resilient member in fluid communication with the internal chamber of a container holding hyperpolarized gas;
expanding the resilient member to extend into the container to contact the hyperpolarized gas; and forcing the hyperpolarized gas to exit the container away from the expanded resilient member.
positioning a resilient member in fluid communication with the internal chamber of a container holding hyperpolarized gas;
expanding the resilient member to extend into the container to contact the hyperpolarized gas; and forcing the hyperpolarized gas to exit the container away from the expanded resilient member.
37. A method according to Claim 36, wherein the container includes an inlet port and exit port positioned on opposing sides of the container, and wherein the resilient member is securely attached to the inlet port such that fluid introduced therein acts to inflate the resilient member and the hyperpolarized gas exits the container through the exit port.
38. A method according to Claim 37, wherein the resilient member includes a surface which is coated with or formed from a material which inhibits depolarization of the hyperpolarized gas.
39. A method according to Claim 38, wherein the method further comprises the step of deflating the resilient member.
40 40. A vessel for holding a quantity of hyperpolarized noble gas, comprising:
a chamber;
a quantity of hyperpolarized noble gas disposed in said chamber; and a resilient member in communication with said hyperpolarized gas in said chamber, said resilient member having a first collapsed position and a second expanded position, wherein when in said second position said resilient member extends into said chamber a further distance than when in said first position.
a chamber;
a quantity of hyperpolarized noble gas disposed in said chamber; and a resilient member in communication with said hyperpolarized gas in said chamber, said resilient member having a first collapsed position and a second expanded position, wherein when in said second position said resilient member extends into said chamber a further distance than when in said first position.
41. A vessel according to Claim 40, wherein said vessel further comprises a fluid inlet port and an exit port in fluid communication with said chamber.
42. A vessel according to Claim 41, wherein said resilient member translates to said second position responsive to fluid introduced into said inlet port.
43. A vessel according to Claim 42, wherein said resilient member is sealed to a portion of said chamber such that said resilient member is positioned intermediate of said inlet port and said hyperpolarized gas and wherein said resilient member prevents said hyperpolarized gas from contacting said fluid inlet port.
44. A container for transporting hyperpolarized noble gas, comprising:
a gas holding chamber;
a quantity of hyperpolarized gas disposed in said chamber; and an access port in fluid communication with said holding chamber, wherein said access port is resiliently configured to receive a portion of a syringe therein.
a gas holding chamber;
a quantity of hyperpolarized gas disposed in said chamber; and an access port in fluid communication with said holding chamber, wherein said access port is resiliently configured to receive a portion of a syringe therein.
45. A container according to Claim 44, wherein said access port comprises a valve and an externally accessible connector in fluid communication with said container.
46. A container according to Claim 44, wherein said access port includes a seal which is configured with material which is friendly to polarization of said hyperpolarized gas in said chamber.
47. A container according to Claim 44, wherein said container further comprises a quantity of liquid positioned adjacent said access port, thereby providing a polarization friendly mask to inhibit loss of polarization of said hyperpolarized gas in said container.
48. A container according to Claim 47, wherein said liquid comprises substantially de-oxygenated water.
49. A container for transporting a quantity of hyperpolarized noble gas from a polarization site to a use site remote from the polarization site, comprising:
a gas holding chamber having opposing ends;
a quantity of hyperpolarized noble gas disposed in said chamber;
an inlet port in fluid communication with said chamber; and an outlet port in fluid communication with said chamber, wherein said inlet port and said outlet port are positioned spaced apart on different sides of sand chamber, and wherein when dispensing hyperpolarized gas from the container, said outlet port is positioned at a higher level than said inlet port.
a gas holding chamber having opposing ends;
a quantity of hyperpolarized noble gas disposed in said chamber;
an inlet port in fluid communication with said chamber; and an outlet port in fluid communication with said chamber, wherein said inlet port and said outlet port are positioned spaced apart on different sides of sand chamber, and wherein when dispensing hyperpolarized gas from the container, said outlet port is positioned at a higher level than said inlet port.
50. A container according to Claim 49, wherein said inlet and outlet ports are offset relative to the other and positioned on opposing sides of a centerline of the container defined by a line extending through the center of the container between said opposing ends.
51. A container according to Claim 49, wherein said container further comprises a quantity of liquid positioned adjacent at least one of said inlet and outlet port to inhibit direct contact between said gas and said at least one port, thereby providing a depolarization mask to inhibit loss of polarization of said hyperpolarized gas in said container.
52. A container according to Claim 51, wherein said liquid comprises substantially de-oxygenated water.
53. A method for dispensing hyperpolarized gas from a polarization cell, comprising the steps of:
positioning a chamber in fluid communication with a polarization cell;
directing a quantity of hyperpolarized gas out of the polarization cell and into the chamber;
cooling at least a portion of the chamber, thereby increasing the gas volumes and pressures in the chamber and improving the quantity of hyperpolarized gas transferred from the polarization cell.
positioning a chamber in fluid communication with a polarization cell;
directing a quantity of hyperpolarized gas out of the polarization cell and into the chamber;
cooling at least a portion of the chamber, thereby increasing the gas volumes and pressures in the chamber and improving the quantity of hyperpolarized gas transferred from the polarization cell.
54. A method according to Claim 53, wherein said hyperpolarized gas is 3He, and wherein said cooling step includes exposing the chamber to liquid nitrogen temperatures during said directing step.
55. A method according to Claim 53, wherein said container is a closed container configured to capture all the gas exiting the polarization cell.
56. A method of identifying the hyperpolarization state of a quantity of hyperpolarized gas, comprising the steps of:
positioning a container having a quantity of hyperpolarized substance in a magnetic field, determining the polarization level of the hyperpolarized substance in the container;
affixing externally visible indicia of shelf life associated with a desired level of polarization of the hyperpolarized substance; and protecting the identified container from depolarizing levels of magnetic gradients.
positioning a container having a quantity of hyperpolarized substance in a magnetic field, determining the polarization level of the hyperpolarized substance in the container;
affixing externally visible indicia of shelf life associated with a desired level of polarization of the hyperpolarized substance; and protecting the identified container from depolarizing levels of magnetic gradients.
57. A method according to Claim 56, wherein said determining step comprises transmitting a signal to the hyperpolarized substance in the container and receiving a signal back therefrom, the signal back corresponding to the hyperpolarization level of the substance in the container.
58. A method according to Claim 57, further comprising the step of polarizing a quantity of noble gas at a production site, wherein said determining step is carried out at a use site remote from a production site.
59. A method according to Claim 56, further comprising the steps of hyperpolarizing a quantity of noble gas via spin exchange at a production site;
transporting a first container having a first quantity of hyperpolarized gas from a production site to a second site remote from the production site; dispensing a portion of said first quantity into a second container at the second site; and wherein said determining step is carried out on the second container proximate to an end use site.
transporting a first container having a first quantity of hyperpolarized gas from a production site to a second site remote from the production site; dispensing a portion of said first quantity into a second container at the second site; and wherein said determining step is carried out on the second container proximate to an end use site.
60. A method according to Claim 59, wherein said first quantity is sufficiently large to provide multiple doses, and wherein said dispensing step dispenses a single dose quantity into the second container.
61. A method according to Claim 57, wherein said determining step is carried out in the presence of a low magnetic field.
62. A method according to Claim 59, wherein the second site is an end use clinical site, and wherein said dispensing step is repeatedly performed at the second site to thereby provide single sized doses of the hyperpolarized gas in a plurality of second vessels suitable for in vivo human administration in order to obtain Magnetic Resonance Images or NMR signal analysis therefrom.
63. A method according to Claim 59, further comprising the step of measuring the level of polarization associated with the hyperpolarized gas in the second vessel prior to administration to a desired subject.
64. A method of extracting a quantity of hyperpolarized noble gas from a vessel, comprising the steps of:
holding a quantity of hyperpolarized noble gas in a first vessel;
withdrawing at least a portion of the hyperpolarized noble gas in the gaseous state in isolation of liquid from the first vessel into a syringe- releasably engaged with and in fluid communication with the first vessel; and subsequently expelling the hyperpolarized noble gas from the syringe.
holding a quantity of hyperpolarized noble gas in a first vessel;
withdrawing at least a portion of the hyperpolarized noble gas in the gaseous state in isolation of liquid from the first vessel into a syringe- releasably engaged with and in fluid communication with the first vessel; and subsequently expelling the hyperpolarized noble gas from the syringe.
65. A method according to Claim 64, further comprising the step of transporting the first vessel from a production site to a second site remote from the production site, and wherein said withdrawing step is carried out at the second site.
66. A method according to Claim 64, wherein said first vessel is configured to hold a multi-dose quantity of the hyperpolarized gas, and wherein said withdrawing and expelling steps are repeated to provide single dose quantities of the hyperpolarized gas.
67. A method according to Claim 64, further comprising the step of measuring the level of polarization associated with the hyperpolarized gas in the second vessel prior to administration to a human subject.
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
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US09/163,721 | 1998-09-30 | ||
US09/163,721 US6237363B1 (en) | 1998-09-30 | 1998-09-30 | Hyperpolarized noble gas extraction methods masking methods and associated transport containers |
PCT/US1999/022990 WO2000020042A2 (en) | 1998-09-30 | 1999-09-30 | Hyperpolarized noble gas extraction methods, masking methods, and associated transport containers |
Publications (2)
Publication Number | Publication Date |
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CA2344671A1 true CA2344671A1 (en) | 2000-04-13 |
CA2344671C CA2344671C (en) | 2010-04-27 |
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ID=22591288
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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CA2344671A Expired - Fee Related CA2344671C (en) | 1998-09-30 | 1999-09-30 | Hyperpolarized noble gas extraction methods, masking methods, and associated transport containers |
Country Status (16)
Country | Link |
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US (5) | US6237363B1 (en) |
EP (1) | EP1123117B1 (en) |
JP (1) | JP2002526168A (en) |
CN (1) | CN1328472A (en) |
AT (1) | ATE324120T1 (en) |
AU (2) | AU764801B2 (en) |
BR (1) | BR9914172A (en) |
CA (1) | CA2344671C (en) |
DE (1) | DE69931060T2 (en) |
DK (1) | DK1123117T3 (en) |
ES (1) | ES2263295T3 (en) |
HU (1) | HUP0203653A2 (en) |
MX (1) | MXPA01003291A (en) |
NO (1) | NO20011596L (en) |
NZ (1) | NZ510684A (en) |
WO (1) | WO2000020042A2 (en) |
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1999
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