A wide variety of radioactive isotopes are used for medical, industrial, research, and commercial applications. In general, radioisotopes may be produced by irradiating target isotope materials with nuclear particles. The target atoms either transmute directly into the desired isotope, or a radioisotope is produced through a chain of absorption and decay that subsequently generates the desired radioactive product.
The latter is the case, for example, in the production of the important medical imaging isotope Technetium-99m, which represents about 90% of the isotopes used in today's nuclear medicine. Tc-99m produces high-energy gamma rays, which makes detection easy, and its short half-life of 6 hours minimizes the radiation dose delivered to the patient. Nuclear medical imaging is unique in its ability to analyze organ structure and functioning. It allows the gathering of diagnostic information that would otherwise require surgery, or not be available at all. It also promotes early detection and treatment of cancers and other problems.
Two different technologies are used to provide the source of radiation for radioisotope production: nuclear reactors, which produce a flux of neutrons, and particle accelerators or cyclotrons, which produce a flux of charged particles, usually protons, but sometimes electrons or other particles. As an example, Tc-99m is the decay daughter product of Mo-99, an isotope with a half-life of 66 hours that is produced in nuclear reactors as a fission product of the neutron bombardment of a uranium target material. This is the source of all of the Tc-99m used in the world today. After irradiation, Mo-99 is recovered from the target, and packed into a production device from which technetium may be eluted in substantially pure form as needed for preparing radiopharmaceuticals for nuclear medical procedures
Other exemplary radioisotopes used for medical, industrial, research and commercial applications include thallium-201, which is used for medical cardiac imaging; calcium-44, which is used in bone growth studies; iridium-192, which is used for nondestructive testing of construction and other materials; cobalt-60, which is used to destroy cancer cells, to disinfect surgical equipment and medications, and the sterilization of food supplies; thulium-170, which is used for portable blood irradiations for leukemia, lymphoma treatment, and power source; gadolinium-153, which is used for osteoporosis detection and SPECT imaging; nickel-63, which can be used for the creation of long-life batteries; and americium-241, which is used in smoke detectors. In addition, rapid advances in nuclear medicine and other fields are focusing attention on a number of isotopes that have not previously been considered commercially important.
As an example of a conventional reactor used in radioisotope production, medical and industrial radioisotopes have been produced since 1957 by Canada's National Research Universal (NRU) reactor at the Atomic Energy of Canada's (AECL's) Chalk River Laboratories in Ontario, Canada. The NRU is a CANDU reactor designed for neutron beam research, materials research and medical/industrial isotope production. In general, CANDU plants are designed to use heavy water (deuterium oxide, or D2O) as the moderator and coolant. The use of heavy water, combined with other features of its design, allows the CANDU reactor to use natural uranium (NU) fuel, which is relatively inexpensive and abundant worldwide.
The NRU produces a high percentage of the world's medical and industrial radioisotopes, including molybdenum-99, a critical isotope used for medical diagnoses. In general, specimen rods containing an isotope target are inserted through penetrations in the NRU in a continuous process and subject to irradiation therein, so as to produce isotopes at a desired specific activity for use in nuclear medicine and/or industrial applications.
Two specialty reactors, the MAPLE 1 and MAPLE 2, are under construction at Chalk River Laboratories. These reactors are intended to replace the NRU. The MAPLE 1 and MAPLE 2 are dedicated exclusively for the production of medical radioisotopes. These research reactors are not intended nor designed for commercial power generation, since they are being designed for power levels of about 10 MWt. The MAPLE is a low-pressure, low-temperature, open-tank-in-pool type research reactor that uses low-enriched uranium (LEU) fuel. The core is compact, and is cooled and moderated by light water. Surrounding the light water core is a heavy water reflector tank, which maximizes the available neutron fluxes needed for radioisotope generation.
Exemplary embodiments of the present invention, in general, may be directed to a method of producing isotopes in a light water power reactor, in which at least one or more targets within the reactor is irradiated under a neutron flux to produce at least one or more isotopes. The targets may be assembled into one or more fuel bundles that are to be loaded in a core of the reactor at a given outage. Power operations in the reactor irradiate the fuel bundles so as to generate desired isotopes, such as one or more radioisotopes at a desired specific activity or stable isotopes at a desired concentration.
The present invention will become more apparent by describing, in detail, exemplary embodiments thereof with reference to the attached drawings, wherein like elements are represented by like reference numerals, which are given by way of illustration only and thus do not limit the exemplary embodiments of the present invention.
As to be described in further detail below, the exemplary embodiments may be directed to using power light water reactors designed for commercial power generation to produce medical and industrial isotopes, in addition to generating thermal and electrical power for residential, commercial and/or industrial use. Unlike research reactors dedicated only to the production of radioisotopes, these light water power reactors may be existing boiling water reactors (BWRs) and/or pressurized water reactors (PWRs) that are configured to generate at least 100 megawatts thermal (MWt) and in example on the order of several hundred or thousand MWt. These power LWRs generally have a bundle average enrichment of less than 10%.
Once the fuel bundle(s) are assembled with one or more target rods, the fuel bundle(s), which may be occasionally referred to as “bulk isotope generation bundles (BIGs)” may be assembled in the core during the outage period. Thereafter, power operations for a next energy cycle in the reactor may be commenced to irradiate the target material therein (S200). The energy cycle represents a period of time (an exposure period as measured in megawatt-days per short time (MWD/st)) in which the reactor is operated for generating power between planned outages. Exemplary energy cycles for BWRs and/or PWRs may be 12 months, 18 months, 2 years, etc., for example.
During power operations, those fuel bundles containing targets are irradiated under a neutron flux in order to produce desired isotopes. The produced isotope may be understood as a radioisotope produced from the target isotope material at a desired specific activity, or a stable isotope that is produced from the target isotope material at a desired concentration, as the target absorbs one or more neutrons during the energy cycle.
The produced isotopes may be removed at a pre-planned outage at end of cycle (S300) so that isotope product removal coincides with the pre-planned outage, so as to minimize the impact on the expect energy production of the light water power reactor, for example. Accordingly, at end of cycle, the reactor may be shutdown and those bundles with produced isotopes (BIG bundles) may be removed or discharged from the reactor during the planned outage following shutdown.
The rods 18a-c and at least a pair of water rods 22 and 24 may be maintained in spaced relation to each other in the fuel bundle 10 by a plurality of spacers 20 provided at different axial locations in the fuel bundle 10 so as to define passages for reactor coolant flow between the rods 18a-c in the fuel bundle 10. In
In an exemplary embodiment of the present invention, various ones of the rods 18a-c may include a container assembly therein.
Referring to
Containment structure 310 may house one or more irradiation targets (i.e., isotope targets) 320 therein. Target 320 shown in
Optionally, an interior of the containment structure 310 may include a spring 340 to provide a counter force against target 320 when sealed by end plug 330. The end plug 330 may be attached to the containment structure 310 by suitable attachment means, i.e., weld, threaded engagement, friction connection, etc. The containment structure 310 may include a pilot hole 303 at end 311 for removing the target(s) 320 after irradiation (which include isotope material therein). End 311 may include exterior threads 301 and an O-ring 302 that is used for sealing container assembly 300 when inserted into a piece of equipment. Pilot hole 303 may include interior threads to aid in the removal of container assembly 300 from a rod 18a-c. Further details of suitable container assemblies are described in the issued patent entitled “Rod Assembly for Nuclear Reactors”, U.S. Pat. No. 7,526,058, the entire contents of which are incorporated by reference herein.
One or more tubing portions 180 of a given rod 18a-c may thus include container assemblies 300 with the same target 320, different targets or multiple targets that produce different isotopes at a desired specific activity (radioisotopes) and/or different stable isotopes at desired concentration, for example. In other words, a given target rod 18a-c can include a plurality of the same or different targets 320 spaced axially at different locations along the target rod 18a-c.
In one exemplary aspect of the invention, at least one target rod includes one or more container assemblies 300 but includes no nuclear fuel (i.e., “nuclear fuel” may be understood as desired enrichments of uranium of UO2 pellets and/or gadolinium). In an aspect, the target 320 may be coated with a magnetic material to improve solubility and prevent release of target material therein into the reactor coolant.
In another aspect, one or more of the target rods 18a-c (full-length, part-length and/or segmented rods) may also include desired enrichments of uranium and/or gadolinium. A given fuel bundle 10 may include various combinations of rods 18a-c that include nuclear fuel, rods 18a-c that include no nuclear fuel but include targets 320, and rods 18a-c which have enriched uranium and/or gadolinium zoned at certain axial locations with targets 320 placed at other axial locations within the target rod 18a-c along the length thereof. The axial and/or radial locations and concentrations of fuel and poisons may be based on the desired characteristics of the bundle 10 for a planned energy cycle in the light water power reactor, for example. In an example, a rod segment of the segmented rod 18a-c that includes a container assembly 300 could also include nuclear fuel, although adjacent rod segments could include nuclear fuel therein.
The target 320 may be a target selected from a group of isotopes having an atomic number greater than 3. In an example, the target 320 may be selected from isotopes comprising one or more of cadmium, cobalt, iridium, molybdenum, nickel, thallium, and/or thulium isotope. Desirably, a given tubing portion 180 and/or container assembly 300 may include indicia or indicators thereon to indicate what target 320 is loaded therein, for example, and/or what isotope is to be produced from that target. As discussed above, the target 320 may be embodied in solid, liquid or gas form and placed inside a tubing portion 180 of a target rod 18a-c.
It may be desirable to place the target 320 in the reactor at a location that maximizes the specific activity of the produced radioisotope/concentration of the produced stable isotope at end of cycle. The properties of the target isotope and produced radioisotopes or stable isotopes may factor in this determination. Accordingly, the target 320 may be placed at a location in the reactor that may be determined as a function of the absorption cross-section of the target isotope itself, and also as a function of the half-life of the produced isotope and the absorption cross-section of the produced isotope. These factors influence the axial and radial zoning of target material within the fuel bundle and more specifically within individual target rods 18a-c of a BIG bundle such as the fuel bundle 10, for example. The absorption cross section of the containment structure 310 housing the target 320 may also be a factor. For some isotopes (such as IR-192), higher neutron fluxes are not necessarily desirable due to the fact that the target may prematurely burn out. By using a containment structure 310 with a material such as stainless steel instead of zircaloy, the desired reduced neutron flux on the target may be achieved, resulting in a high specific activity isotope at the end of cycle without premature burnout of the produced isotope.
The axial and radial locations within the core may be substantially strong independent variables that affect the amount and spectral characteristics of neutron flux that a target will observe. For example, if the absorption/decay characteristics indicate that a larger flux is desired to maximize specific activity, placement of the bundle away from the core boundaries (towards center of core) in both radial and axial directions may be desired. Similarly, if the absorption/decay characteristics indicate that a lower flux is desired to prevent burnout of the target isotope, then the target bundle should be placed towards the perimeter of the core and/or at the extreme top or bottom of the bundle.
Also, selection of the location of the target rod within a given target BIG bundle can greatly influence the final specific activity. As shown in the bundle 10 example of
Although the container assembly 300 with target 320 has been described as being located in a tubing portion 180 of a given rod 18a-c where there is no nuclear fuel, for some isotope targets it may be desirable to surround the container assembly 300 with additional enrichment. For example, a tubing portion 180 containing the containment structure 310 may be packed with additional enrichment in the area between the containment structure 310 outer surface and the inside of the tubing portion 180 during rod manufacture. By packing additional uranium in proximity to the target 320 within the containment structure 310, additional neutron flux may be obtained for the target 320. Consequently, the specific activity of the produced radioisotope may be higher and more valuable to the customer. In addition to adding enrichment, another factor which may affect the neutron fluxes surrounding the containment structure 310 may be the moderator. Packing a tubing portion 180 with additional or alternative moderator (such as graphite) in the space between the containment structure 310 and the inside of the tubing portion of a given rod 18a-c during rod manufacture may enable additional neutron flux to be obtained for the target 320 during power operations in the reactor. Done prior to reactor operation, providing additional moderator in closer proximity to a desired target location in the reactor may thus influence the energy spectrum of the neutron flux through the target during power operations.
Heretofore, the exemplary embodiments have been described loading an isotope target 320 within a containment structure 310 to be provided in one or more of the rods 18a-c of the exemplary bundle 10. However, depending upon the properties of the target isotopes and that of the produced radioisotope or stable isotope (i.e., absorption cross section, half life, etc.), it may be desirable to place the target in an axial location within the fuel bundle 10 that typically receives less neutron flux during an energy cycle. For example, each of rods 18a-c (and water rods 22, 24) include an upper end plug and a lower end plug that are connected to upper and lower end tie plate 14 and 16 in the bundle 10. One or more container assemblies 300 may be placed within interior portions of one of the upper or lower end plugs during the rod manufacturing process, for insertion into the fuel bundle 10 at a planned outage.
Alternatively, a containment structure housing one or more targets 320 therein may be placed within a control blade during a control blade manufacturing process. For example, a control blade which is used for reactor control between fuel bundles may have its neutron absorbers (i.e., B4C, Hf, etc.) replaced with a container assembly 300. Such control blades would not be used for reactor control and could be used as radioisotope target vehicles into and out of the core. This may allow for insertion and removal of targets 320 at times other than reloads at a planned outage, for example. This may also provide flexibility in axial elevation selection for neutron flux tuning within the core.
A core of a light water power reactor includes several penetrations for insertion of instrumentation tubes during the energy cycle to take measurements, readings, etc. Accordingly, a containment structure 310 with radioisotope target 320 may be inserted into BWR instrumentation tubes through the use of a traversing and core probe machine, for example. This may also allow for insertion and removal of targets, to perhaps produce isotope material for those isotope having shorter half-lives or which do not need as much neutron flux to be removed at a time other than a planned reload at a planned outage.
In another alternative, isotope targets may be placed outside the core but within the pressure vessel. A typical light water power reactor such as a BWR includes a core shroud which connects the core to the reactor pressure vessel. A containment structure 310 with isotope target 320 therein may be attached to the core shroud during a planned outage and subsequently irradiated during a next energy cycle for irradiating the target 320 to produce a desired isotope therein. Placing the target 320 outside the core may facilitate licensing since it does not include core internals such as fuel, control blades, etc. Targets 320 which produce isotopes that require low flux may be desirable candidates for placing on the core shroud and may withstand an entire cycle of the radiation, for example.
Additionally, carrier bundle uranium and components for the bulk isotope generation bundle may be procured (S420) and the bulk isotope generation (BIG) may be assembled from the target rods, procured uranium and associated components (S430). Standard reload bundle procurement and manufacture of the reload bundles (S440) may also be performed, as is known, to be loaded at next planned outage. The reload bundles and BIG bundles may be shipped to the reactor site for loading into the core of a desired light water power reactor such as a BWR. Reload licensing for the reload bundles would be done prior to shipping or prior to loading the bundles in the core. The same is expected for the BIG bundles. The BIG and reload bundles are loaded into the reactor core (S450). Up on completion of the outage, the reactor may commence power operations for a given energy cycle to irradiate the BIG bundles (S460).
At end of cycle, the reactor is shut down and the BIG bundles may be discharged (S470) during the subsequent outage period to a staging area in the spent fuel pool. The staging area may be an enclosed work area or “safe chamber” within the spent fuel pool. The same chamber may be at a sufficient size to hold the BIG bundles and necessary tools, casks/shielded shipping containers and surveillance equipment. The safe chamber would allow for accidental dropping of target rods and prevent a potential radiation exposure accident and may provide a convenient way to secure and obtain quick access to surveillance equipment and disassembly tools.
In the staging area, the target rods may be harvested (S480) from the BIG bundle using suitable tooling and loaded into shielded shipping containers or casks for transport to an off-site facility. Those harvested BIG bundles are then returned to the spent fuel pool. Alternatively, if the plant site includes a hot cell facility, the hot cell facility may be joined to the reactor by a suitable corridor through which the materials irradiated in the reactor may be brought to the hot cells (shielded work areas) where the isotopes may be extracted and packaged for shipment. Thus, the target rods are disassembled (S490) in the hot cell to retrieve the desired isotope materials for final processing and transport (S495) to the customer.
Heretofore, the exemplary embodiments have been described in which the produced isotope is removed at a point in time to coincide with an end of cycle of a given energy cycle. However, there are occasions where an unplanned outage occurs at a point during the energy cycle, sometimes referred to as a mid-cycle outage. Accordingly, target isotopes may be loaded in the reactor that produce isotopes at a desired specific activity or stable isotope at a desired concentration at such a mid-cycle outage point. These radioisotopes or stable isotopes may then be removed at the mid-cycle outage point to provide a revenue stream that may potentially offset the costs associated with the unplanned outage period.
Accordingly, the exemplary methodology may illustrate the advantages of assembling bulk isotope generation bundles for a core of an existing light water power reactor that is designed for commercial power operations. A BIG bundle may include one or more target rods, and each target rod may include one or more of the same or different target isotopes that, upon irradiation under a neutron flux during an energy cycle, produce radioisotopes at a desired specific activity or stable isotopes at a desired concentration for medical and/or industrial isotope applications.
Since the core of the exemplary light water power reactor may include in upwards of several hundred fuel bundles, the potential to generate (bulk produce) medical and/or industrial isotopes to satisfy the world demand may be realized. As an example, a core loaded with no more than about 8 to 16 BIG bundles (out of a total of several hundred fuel bundles) could potentially produce sufficient isotope product to satisfy the current world demand for those applications that require medical and/or industrial isotopes.
The exemplary embodiments of the present invention being thus described, it will be obvious that the same may be varied in many ways. Such variations are not to be regarded as departure from the spirit and scope of the exemplary embodiments of the present invention, and all such modifications as would be obvious to one skilled in the art are intended to be included within the scope of the following claims.
This application is a divisional application of and claims priority under 35 U.S.C. §§120, 121 to co-pending application Ser. No. 11/002,680 “Method of producing isotopes in power nuclear reactors,” filed Dec. 13, 2004, the entirety of which is incorporated by reference.
Number | Name | Date | Kind |
---|---|---|---|
3015616 | Sturtz et al. | Jan 1962 | A |
3072549 | Compton et al. | Jan 1963 | A |
3120471 | Duffield et al. | Feb 1964 | A |
3158546 | Cordova | Nov 1964 | A |
3229096 | Bonilla et al. | Jan 1966 | A |
3269915 | Ransohoff et al. | Aug 1966 | A |
3282655 | Case et al. | Nov 1966 | A |
3324540 | Lotts et al. | Jun 1967 | A |
3549492 | Ricci et al. | Dec 1970 | A |
3594275 | Ransohoff et al. | Jul 1971 | A |
3745069 | Sofer et al. | Jul 1973 | A |
3955093 | Quinby | May 1976 | A |
3998691 | Shikata et al. | Dec 1976 | A |
4196047 | Mitchem et al. | Apr 1980 | A |
4284472 | Pomares et al. | Aug 1981 | A |
4393510 | Lang et al. | Jul 1983 | A |
4462956 | Boiron et al. | Jul 1984 | A |
4475948 | Cawley et al. | Oct 1984 | A |
4493813 | Loriot et al. | Jan 1985 | A |
4526741 | Cawley et al. | Jul 1985 | A |
4532102 | Cawley | Jul 1985 | A |
4597936 | Kaae | Jul 1986 | A |
4617985 | Triggs et al. | Oct 1986 | A |
4650635 | Le Rat et al. | Mar 1987 | A |
4663111 | Kim et al. | May 1987 | A |
4729903 | McGovern et al. | Mar 1988 | A |
4782231 | Svoboda et al. | Nov 1988 | A |
4818468 | Jungerman et al. | Apr 1989 | A |
4859431 | Ehrhardt | Aug 1989 | A |
4908515 | McLeod | Mar 1990 | A |
5009837 | Nguyen et al. | Apr 1991 | A |
5053186 | Vanderheyden et al. | Oct 1991 | A |
5145636 | Vanderhevden et al. | Sep 1992 | A |
5291533 | Orr | Mar 1994 | A |
5309489 | Tate et al. | May 1994 | A |
5347550 | Tanabe et al. | Sep 1994 | A |
5349619 | Mochida et al. | Sep 1994 | A |
5355394 | Van Geel et al. | Oct 1994 | A |
5377247 | Yoshioka et al. | Dec 1994 | A |
5394275 | Iketani et al. | Feb 1995 | A |
5400375 | Suzuki et al. | Mar 1995 | A |
5513226 | Baxter et al. | Apr 1996 | A |
5596611 | Ball | Jan 1997 | A |
5633900 | Hassal | May 1997 | A |
5682409 | Caine | Oct 1997 | A |
5758254 | Kawamura et al. | May 1998 | A |
5867546 | Hassal | Feb 1999 | A |
5871708 | Park et al. | Feb 1999 | A |
5910971 | Ponomarev-Stepnoy et al. | Jun 1999 | A |
5987087 | Zhuikov et al. | Nov 1999 | A |
6011825 | Welch et al. | Jan 2000 | A |
6056929 | Hassal | May 2000 | A |
6160862 | Wiencek et al. | Dec 2000 | A |
6233299 | Wakabayashi | May 2001 | B1 |
6299666 | Apostolidis et al. | Oct 2001 | B1 |
6347130 | Nylund | Feb 2002 | B1 |
6456680 | Abalin et al. | Sep 2002 | B1 |
6516043 | Chaki et al. | Feb 2003 | B1 |
6678344 | O'Leary et al. | Jan 2004 | B2 |
6697446 | Kang et al. | Feb 2004 | B2 |
6751280 | Mirzadeh et al. | Jun 2004 | B2 |
6804319 | Mirzadeh et al. | Oct 2004 | B1 |
6895064 | Ritter | May 2005 | B2 |
6896716 | Jones, Jr. | May 2005 | B1 |
7139360 | Lahoda | Nov 2006 | B2 |
7157061 | Meikrantz et al. | Jan 2007 | B2 |
7235216 | Kiselev et al. | Jun 2007 | B2 |
20020034275 | Abalin et al. | Mar 2002 | A1 |
20030012325 | Kernert et al. | Jan 2003 | A1 |
20030016775 | Jamriska, Sr. et al. | Jan 2003 | A1 |
20030103896 | Smith | Jun 2003 | A1 |
20030179844 | Filippone | Sep 2003 | A1 |
20040064010 | Wagner | Apr 2004 | A1 |
20040091421 | Aston et al. | May 2004 | A1 |
20040105520 | Carter | Jun 2004 | A1 |
20040196942 | Mirzadeh et al. | Oct 2004 | A1 |
20040196943 | Di Caprio | Oct 2004 | A1 |
20050105666 | Mirzadeh et al. | May 2005 | A1 |
20050118098 | Vincent et al. | Jun 2005 | A1 |
20060062342 | Gonzalez Lepera et al. | Mar 2006 | A1 |
20060126774 | Kim et al. | Jun 2006 | A1 |
20070133731 | Fawcett et al. | Jun 2007 | A1 |
20070297554 | Lavie et al. | Dec 2007 | A1 |
20080031811 | Ryu et al. | Feb 2008 | A1 |
20080076957 | Adelman | Mar 2008 | A1 |
Number | Date | Country |
---|---|---|
2 172 953 | Apr 1995 | CA |
2647945 | Dec 1990 | FR |
2065955 | Jul 1981 | GB |
Entry |
---|
Mirzadeh et al., “Production Capabilities in U.S. Nuclear Reactors for Medical Radioisotopes”, Nov. 1992. |
Paas, A. and Sullivan, R., “Measurement of Neutron Activated Short-lived Nuclides using a Pneumatic Transfer System”, 1962. |
Manual for reactor produced radioisotopes, Jan. 2003, IAEA, pp. i-45. |
Garland, M.A., “Medical Isotope Production in the Fast Flux Test Facility and the High Flux Isotope Reactor and Isotope Production Software Users Guides”, Aug. 2000, DOE, pp. 1-72. |
Flanagan, G. F.; “Description of High Flux Isotope Reactor and Future Upgrades”, specific date unknown, pp. 49-57 (evidentiary reference). |
Borschev et al., “Possibilities for producing radionuclides in nuclear power plants,” Atomic Energy, vol. 95, No. 6, 2003 . |
European Office Action dated Jul. 1, 2009. |
Office Action for corresponding U.S. Appl. No. 11/002,680 dated May 11, 2011. |
Office Action dated Apr. 4, 2012 issued in corresponding Canadian Application No. 2,527,682. |
Japanese Notice of Allowance dated Sep. 25, 2012 for corresponding Japanese Application No. 2005-344804 (full translation provided). |
Number | Date | Country | |
---|---|---|---|
20150348663 A1 | Dec 2015 | US |
Number | Date | Country | |
---|---|---|---|
Parent | 11002680 | Dec 2004 | US |
Child | 12890845 | US |