This invention relates generally to the production of radioisotopes, and, more particularly, to a target system for irradiating a sample material by an accelerated particle beam.
A radioisotope, also called radionuclide, is an unstable element that releases excess energy in the form of radiation (particles or electromagnetic waves), while it is converted into a different element (stable or unstable). The radioisotope is said to undergo radioactive decay. The rate of decay is constant. The time taken for the activity of a given amount of a radioactive substance to decay to half of its initial value is called half-life (t1/2). The range of half-lives of radioactive atoms spans over many orders of magnitude.
Radioisotopes may be used in several different applications. Medical applications of radioisotopes may include, for example, imaging and measuring of physiological processes or the treatment of cancer.
Radioisotopes may be created by several processes, including subjecting a material to bombardment with accelerated particles. The collision between the accelerated particles, e.g., a stream of protons generated by a cyclotron, and the material, can cause the atomic structure of the material to be altered. The altered atomic structure can be unstable, resulting in discharges of further particles or electromagnetic radiation from the atomic structure over time. This process is called a nuclear reaction. The product created, as a result of the nuclear reaction, will be recognized as a radioactive material. A radioactive material can contain a mixture of radioisotopes.
Many substances may be subjected to this bombardment of accelerated particles. This bombardment is commonly termed irradiation. These substances are termed “targets.” The targets can be in a solid, liquid or gas phase.
The existing technology transforms stable substances into radioactive material. Handling of the now radioactive material requires care and specialized facilities or tooling.
It will be appreciated that the particle accelerator produces a substantially linear particle beam. One function of the target structure is to position the target within the beam. The target structure therefore may have a linear orientation parallel to the longitudinal axis of the particle beam.
The transformation of target substances by irradiation, i.e., bombardment of solids, liquids, or gases, generates heat. This phenomenon therefore necessitates heat abatement or cooling mechanisms to be employed. Streams of cold helium gas, as well as jacketing the target holding and positioning structure for conveying cold water or other fluids, have been used for cooling both the target substance and the holding and positioning structure.
As indicated above, the target substance can be a gas. Gases provide a target of limited density, thereby limiting the radioactivity that can be produced via the irradiation process.
In the irradiation of liquids, a target of greater density is provided, increasing the radioactivity that can be produced. The heat of the irradiation process transforms at least a portion of the liquid into a gas phase. The expanding gas creates pressure upon a closed container, i.e., target chamber. Expanding gas can damage or cause a breach of the target structure, resulting in the dispersal of hazardous radioactive material. Prior methods of irradiating liquids have employed a target structure having an enlarged chamber that can capture the vapor.
In the irradiation of solids, the target structure must be adapted to handle the heat generated and to prevent or minimize undesired alterations of the target material.
Attempts have been made to dissolve solids and irradiate liquid solutions. An amount of solids, in a solution is limited, thereby limiting the radioactivity that can be produced via this irradiation process.
The now radioactive product must be removed from the target structure for further processing. It will be appreciated that radioactive materials pose a danger and health hazard to living organisms, obviously this includes workers. Prior methods of irradiating targets have had the challenge of removing the now radioactive product with minimized workers exposure to radiation.
In the process of irradiating gases and liquids, ports connected to the interior of the chamber of the target structure have been used to remotely remove the irradiated target material by pumping gas through one port into the chamber and forcing the target material out through a second port. It will be appreciated that the second port may be connected to a radiation shielded cell, also called a “Hot Cell.”
In the process of irradiating solids, the prior art required mechanical disassembly of the target structure to allow removal of the solid target (now radioactive) and transportation to a separate location for further processing.
Attempts have been made for mechanically opening the solid target structure and deposit the target material manually or automatically into a shielded container, thereby making it safe for further handling by workers.
Attempts also have been made for remotely operated mechanical opening the solid target structure and automatic transport of the solid target to a processing cell.
Attempts also have been made for remotely operated mechanical opening the solid target structure, transfer the target into a dissolution apparatus and pumping the dissolved material in liquid form to a processing cell.
However, in the prior art, there have been limited to no available options to add solid target technology with safe mechanism for removal of the irradiated target into existing facilities. The prior art requires mechanical disassembly of the target structure to allow removal and transfer of the solid target after irradiation. It will be appreciated that the solid target (now radioactive) poses a great hazard in as much as the selected target product emits a great amount of radioactivity, typically with long half-life.
As will be understood, irradiation of substances is useful in the production of radioisotopes. Radioisotopes are a tool used in various applications including biology, wherein the radioisotopes of carbon can serve as radioactive tracers because they are chemically very similar to the nonradioactive nuclides, so most chemical, biological, and ecological processes treat them in a nearly identical way. One can then examine the results with a radiation detector, such as a Geiger counter, to determine where the provided atoms were incorporated. For example, one might culture plants in an environment in which the carbon dioxide contained radioactive carbon; then the parts of the plant that incorporated atmospheric carbon would be radioactive. Radioisotopes can be used to monitor processes such an DNA replication or amino acid transport.
Radioisotopes may also be used in nuclear medicine, being used for diagnosis, treatment, and research. Radioactive chemical tracers emitting gamma rays or positrons can provide diagnostic information about internal anatomy and the functioning of specific organs, including the human brain. This is used in some forms of tomography: single photon emission computed tomography and positron emission tomography (PET) scanning and Cherenkov luminescence imaging. Radioisotopes are also a method treatment in hemopoietic forms of tumors; the success for treatment of solid tumors has been limited. More powerful gamma sources sterilize syringes and other medical equipment.
Further radioisotopes are used for food preservation, radiation is used to stop the sprouting of root crops after harvesting, to kill parasites and pests, and to control the ripening of stored fruit and vegetables.
Radioisotopes are also used in industry and in mining. Radioisotopes are used to examine welds, to detect leaks, to study the rate of wear, erosion, and corrosion of metals, and for on-stream analysis of a various minerals and fuels.
In spacecraft and elsewhere, radioisotopes are used to provide power and heat, notably through radioisotope thermoelectric generators (RTGs). Also, in astronomy and cosmology, radioisotopes play a role in understanding stellar and planetary processes. In particle physics, radioisotopes help by measuring the energy and momentum of their beta decay products.
In ecology, radioisotopes are used to trace and analyze pollutants, to study the movement of surface water, and to measure water runoffs from rain and snow, as well as the flow rates of streams and rivers. Radioisotopes are used in geology, archaeology, and paleontology to measure ages of rocks, minerals, and fossil materials.
Radioisotopes are produced through the nuclear reactions in reactors or from charged particle bombardment in accelerators. In accelerators, the typical charged particle reactions utilize protons although deuterons and helium nuclei (3 He++ and alpha particles) also play a role. One clear advantage that accelerators possess is the fact that, in general, the target and product are different chemical elements.
The production of radioisotopes in a charged particle accelerator such as a cyclotron or in a linear accelerator is achieved through a nuclear reaction wherein the accelerator bombards a directed stream of particles, e.g., protons, at high energy into a chemical element, e.g., zinc or calcium, thereby causing one or more particles to be ejected from the nucleus of the element. The ejection of a particle from the nucleus transforms the original element into a separate element. This separate element is typically unstable and will decay, resulting in the emission of radiation.
This disclosure includes illustration and description of a target and target structure that achieves safe removal of solid irradiated substances from the target structure at the conclusion of irradiation without the requirement of mechanical operations. The disclosure teaches irradiation of a solid target. The disclosure further teaches a novel process causing the target to change in-situ from a solid to a liquid phase to facilitate safe removal of the radioactive material from the target structure. This process is termed hybridization of the structure during and after the irradiation process.
The disclosure also includes a novel method to remove heat from the solid target material during irradiation. The solid target material is positioned in a closed chamber within the target structure to receive the bombardment of particles from the cyclotron. It is within this closed chamber that a substance, initially in liquid form, will be utilized to remove the heat produced during the irradiation process by means of multiple liquid/vapor phase changes.
The disclosure also includes novel configuration of the substrate with the solid target material. Such substrates, also called backing materials, may be used to allow passage of the irradiating particles into the solid material. In some embodiments, the solid material may be contained on an inert metal plate or foil upon which the solid has been attached, e.g., electro-plating. In another embodiment, the foil may be modified to form a receptacle to retain solid material in powdered or metallic form. In yet another embodiment, the solid material maybe positioned between two foil pieces. In yet a further embodiment, multiple foils may be used. After irradiation, the outer most foil (as determined by proximity to the particle beam interface with the target structure) and the target material may be dissolved by acid, e.g., dilute HCl, and then pumped to a processing unit.
The disclosure also describes a solid wall split chamber that is positioned within the target structure and proximate to the foil surface containing the target. The chamber component is open to the surface containing the target. Part of the chamber may hold water or other liquid. The second part of the chamber, configured to be in communication of the first portion of the chamber, can be used to contain vapor formed by the heat of the irradiation process. The solid walls of the second chamber segment may be used as a lower temperature surface to facilitate the condensation of the vapor.
The target component may contain a cooling jacket through which liquid may flow.
The accompanying drawings, which are incorporated in and constitute a part of the specification, illustrate preferred embodiments of the disclosure. These drawings, together with the general description of the disclosure given above and the detailed description of the preferred embodiments, given below, serve to explain the principles of the disclosure.
The invention may be best understood by reference to the following description taken in conjunction with the accompanying drawings, in which like reference numerals identify like elements, and in which:
Note the elongated opening suited for the split target oriented at an oblique angle to the particle beam.
Illustrative embodiments of the invention are described below. In the interest of clarity, not all features of an actual implementation are described in this specification. It will of course be appreciated that in the development of any such actual embodiment, numerous implementation-specific decisions must be made to achieve the developers' specific goals, such as compliance with system-related and business-related constraints, which will vary from one implementation to another. Moreover, it will be appreciated that such a development effort while complex and time-consuming, would nevertheless be a routine undertaking for those of ordinary skill in the art having the benefit of this disclosure.
The novel elements taught by this disclosure may be utilized in either a cyclotron or linear accelerator. These devices may be referred to collectively as particle accelerators.
The chemical element subjected to this bombardment is referred to herein as the “target.” The target is held within the orientation of the stream of particles by means of a target structure. The target structure is assembled from multiple components. In some embodiments, many of the components are made of Aluminum. These components can be assembled and attached using various subcomponents such as threaded screws bolts fitting into threaded holes. The assembled target structure can also be structured and described as forming a rigid but quickly detachable structure. Other attachment fixtures could be used including snaps, latches and “lock-and-twist” fittings. The fittings may incorporate detent mechanisms with complementary protrusions and indentions to mate adjoining components of the target structure. It will be appreciated that such devices, e.g., as snaps and latches can facilitate prompt and quick assembly and disassembly of the target structure (or the target handle to the target structure). This can be advantageous when manually removing the now radioactive target material or target structure from the particle accelerator. This is one of the novel features of this disclosure.
In another novel embodiment, portions of the target structure may comprise radioactive insulating or shielding material to enhance safe transfer of irradiated materials required for additional processing. In one embodiment, this shielding material could be used in the target structure component containing the split chamber discussed below.
In yet another embodiment, a tool with an elongated shaft may be used to attach to and remove the portion of the target structure housing that contains a split chamber as described more completely below. The tool may be dimensioned to fit into portals of the target structure used to convey cooling fluids. The fluid conveying tubing or conduit would need to be removed prior to the attachment of the tool.
In still another embodiment of this disclosure, the target is positioned into the target structure as part of the assembly of the target structure components.
The target elements can be in a liquid or solid phase. In the liquid phase, the chemical element can be a solution with a solvent or in a liquid phase of a pure element.
It will be appreciated that the target is positioned within the target structure perpendicular to the stream of particles. Alternatively, the target material can be positioned at an angle to the particle stream.
A principal constraint in the manufacturing of radioisotopes utilizing a cyclotron accelerator is the production of heat. It is necessary to abate this heat within the target structure. This can be achieved in various ways, including but not limited to maintaining a flow of chilled helium gas or chilled liquid, such as water, through the structure.
It will also be appreciated that the cyclotron conducts the accelerated particles through a vacuum. It is convenient to separate the vacuum from the atmosphere within the target structure. The target is isolated and separated from the cyclotron. This is important not to contaminate the cyclotron structure. This separation is typically achieved by an isolation window, i.e., a thin strip or foil of metal or other substance such as Aluminum or HAVAR alloy. A chemically inert foil may be inserted between the window and the target material to protect the particle accelerator from contamination. It will be appreciated that Niobium and Tantalum are suitable metals for this purpose due to their inertness, resistance to acids and low residual radioactivity. The thin strip has an inner surface, i.e., proximate to the cyclotron and distal to the target. The foil window prevents gas or other material from entering the cyclotron. It does not however significantly impede the particle beam. The outer surface of the foil is proximal to the target within the target structure.
As discussed in greater detail below, it is important that the energy of the particle beam be within a specified range corresponding to the desired nuclear reaction, to control the alteration of the nuclei of the target material. When the minimum energy of the beam provided by the particle accelerator cannot be reduced to the required energy for the desired nuclear reaction, an energy degrader is used. As the name implies, the energy degrader can serve to dampen the energy of the particle beam irradiating the target. The energy degrader will be of a solid plate that intersects the particle beam path prior to the beam irradiating the target. Typically, an energy degrader is placed after the isolation foil. In an embodiment, the foil may be optional if an energy degrader is utilized. In another embodiment, the isolation foil may be needed if the degrader is subjected to cooling with Helium gas. In such a configuration, the isolation foil separates the particle accelerator from the front side of the degrader (proximal to the accelerator). It will be appreciated that the target will be on the opposite side of the degrader. Alternatively, the isolation foil can also be used as an energy degrader.
It will also be appreciated that the energy degrader functions to normalize the energy of the particle beam. The strength of the particle beam can vary with the manufacture of the cyclotron. For example, the respective proton energy varies among several cyclotron models as follows: IBA Cyclone and Kiube 18 MeV; ACSI 19 or 24 MeV; and GE PETtrace 16.5 MeV.
It will also be appreciated that the particle beam energy may need to be dampened to avoid production of unwanted isotopes.
This disclosure teaches the use of Aluminum, Niobium, Tantalum or other metals for energy degraders for the production of radioactive metals, also called radiometals, such as 68Ga from 68Zn, 64Cu from 64Ni, 89Sr from 89Y, 123I from 123Te, etc.
When Aluminum, or another metal chemically incompatible with the target material, is used as an energy degrader, a second foil may be required to isolate the target material from the Aluminum, e.g., Niobium. Continuing into the interior of the target structure, (distal to the particle accelerator) the second foil will be proximal to the above energy degrader. For a solid target, the target material will be placed on the outer surface of the second foil or directly on the energy degrader. If the solid target is a powder, the powder may be contained in an indenture or cavity of a component positioned across the particle beam path (similar to the positioning of a foil). Again, for orientation purposes, the inner surface of this second foil is opposite the outer surface (proximal to the particle accelerator) of the isolation foil discussed in the preceding paragraph. In one embodiment, helium gas may flow between the isolation foil and the degrader or second foil. It will be understood that the path of the flowing gas may be orthogonal to the particle beam path.
Continuing with the discussion of the irradiation of powder target material, in one embodiment the powder is contained in an indenture of a first solid plate or degrader. The plate may be circular or oval. The plate intersects the particle beam path. There can be a second solid plate have a protrusion of a complementary dimension to the first plate indenture. The protrusion may fit into the indenture, thereby compressing the powder. Behind the second plate may be a cavity for holding water or other liquid or gas for cooling. This cavity may be in communication with an inlet and outlet to allow liquid to flow through the cavity. This cavity may be termed a combination of a liquid reservoir and vapor capture enclosure. It may be referred to as a split chamber.
This disclosure teaches a novel target structure for irradiating solid target material. In one embodiment, the target structure contains a split chamber. The chamber is placed in contact with the outer surface of an internal foil. The foil can be plated with the solid target or similarly affixed to the outer foil surface. The split chamber has an aperture of a complementary size and shape of the solid target material positioned on the internal foil. The split chamber may be made of acid resistant material.
The split chamber is positioned within a housing component of the target structure. One portion of the split chamber forms a reservoir for placement of a liquid, e.g., sterile water. The portion of the split chamber may be termed “reservoir.” Connected to and above the reservoir is a second portion of the split chamber that may receive vapor from the liquid in the event the liquid temperature increases. This second portion may be termed “expansion chamber” or “vapor capture enclosure.” The end of the expansion chamber may have an aperture for receipt of pressurized gas or liquid, i.e., fluid. It will be appreciated that the expansion chamber or vapor capture enclosure may be dimensioned to hold a volume of fluid vapor with minimal resulting pressure. This is another novel feature of the disclosure.
As indicated above, the solid target material fits adjacent and in communication with the opening of the split chamber. The opening of the split chamber may be attached to a flange wherein the flange contacts the internal foil, but not the portion of the foil with the solid target. This communication allows the liquid within the liquid reservoir to contact the surface of the target material.
In an embodiment the lower portion of the reservoir, the split chamber also has controllable orifices or portals for closeable input and outlet for fluid. These portals can allow filing of the reservoir as well as purging the split chamber of liquids or gases.
It will be appreciated that unlike the prior art, the target material is positioned on the outer portion of a foil or degrader and accessible to the interior of the split chamber. The target material may be in contact with the liquid. The split chamber can be purged of the liquid or gas, including particles of radioactive isotopes created by the irradiation of the target with the particle beam.
Further, the split chamber is surrounded by a jacket having a space allowing for the circulation of cooling fluid such as helium or water. As will be discussed below, this can cool the outer surface of the split chamber, particularly the expansion chamber. This cooling jacket comprises part of the target structure. This can also alleviate the build of vapor pressure which may damage the foil or target.
As noted, heat is a significant by-product of the irradiation activity. This factor illustrates another novel aspect of the disclosure. As the beam irradiates the target, the target and/or degrader are heated. This heat is absorbed into the liquid contained in the reservoir. Additionally, after passing through the target, the dampened particle beam deposits energy into the liquid contained in the reservoir producing more heat. The liquid temperature is raised, thereby causing some of the liquid to evaporate and enter the gas phase.
The vapor rises above the liquid surface and contacts the cooled surface of the expansion chamber. This may result in condensation of the vapor into liquid. This second phase change also requires the absorption of heat energy into the chamber walls and the liquid circulating in the cooling jacket, thereby removing the heat from the chamber.
It will be appreciated that the radioisotopes produced by the irradiation of the target may leach or otherwise transfer into solution with the liquid. This phenomenon also teaches another novel aspect of this disclosure. After completion of the irradiation, much, if not all, of the radioisotopes may have migrated into the solution by thermal diffusion or other means. The liquid in the chamber can contain an acid, including a weak or diluted acid, to facilitate the thermal diffusion process. The controllable portal within the expansion chamber and the controllable portal at the bottom of the reservoir may be opened and the radioisotopes may be drained from the target structure for further processing.
Also, the isotopes formed from the irradiated target material may be concentrated on the outer surface of the target. This outer surface is proximate to and in contact with the liquid. Exposure of this surface to a weak acid may “etch” the target surface of the radioisotope, leaving much of the target material in its original nuclear state. The “etching” facilitates removal of the isotopes from the target surface. It will be appreciated that a weak acid is an acid that is partially dissociated into its ions in an aqueous solution of water. At the same concentrations, weak acids have a higher pH value than strong acids. The properties of a weak acid may facilitate the removal of the outer surface of the target material without alteration of the substrate. It will be further appreciated that this liquid, e.g., acid rinse, may be a suitable for radionucleotide diagnostic purposes.
Moreover, the above steps, i.e., thermal diffusion facilitated by a weak acid to leach the radioisotope into the liquid, may preserve much of the original target material, e.g., zinc, such that the target material can be reused. Dissolution of the target foil is therefore not required.
Furthermore, another novel aspect of this disclosure is that the split chamber, in conjunction with the controllable opening and closing of the portals may be filled with a liquid that will remove remaining product, i.e., the radioactive radioisotopes, from the outer surface of the foil. In one embodiment, this target product removal step may be accomplished by introducing dilute acid, such as HCl, through the upper or lower portal of the expansion chamber. The particle beam could be used to increase the temperature of the acid, to optimize the dissolution process. The dilute acid may then be drained through the lower portal of the reservoir. This process may be enhanced by then introducing pressurized gas through the expansion chamber portal and out from the reservoir portal. The introduced gas may be inert gas such as Argon, He, etc. This process can also be used to recover the target material.
The radioactive radioisotopes, now in fluid solution, may be safely conveyed from the target structure to a processing station, i.e., “hot cell.”
It will be appreciated that this transfer of the radioactive and harmful radioisotopes can be performed without worker activity in proximity to this now radioactive material. This is unlike the prior art wherein removal of the radioisotopes required workers to disassemble the target housing or rely upon remote mechanical, motor or pneumatic driven opening of the target housing. In such prior art, workers were required to accomplish the removal of the radioisotopes by activity in close proximity to the radioactive product. Alternatively, automated mechanical or pneumatic transfer systems were used in the prior art. These automated systems are complex and expensive. Additionally, these systems require large passages through the accelerator or target shielding. Those, passages are difficult to add to existing installations.
This disclosure also teaches the production of radioisotopes where the target material is in powder form, e.g., 44gSc radioisotope from 44Ca powder. Note add that the solid powder may be placed on an energy degrader. Another novel aspect of the teaching of this disclosure is covering the pressed powder (which may be positioned on an energy degrader or foil) with a metal foil such as Zinc to contain the powder and/or protect it from reaction with water, e.g., 44Ca reacts violently with water. After completion of irradiation, the foil and the target material containing the radioactive product may be dissolved with acid, e.g., dilute HCl. The now dissolved target material, product and foil material will have to be separated during subsequent processing, e.g., separating 44Ca, 44gSc and Zn.
It will be appreciated that the teachings of this disclosure include, but are not limited to, creation of the following radioisotopes: 18F from 18O and 13N from 16O. In this case the target material will be the liquid contained inside the chamber, instead of solid form.
It will be appreciated that the teachings of this disclosure include simultaneous production of multiple radioisotopes, i.e., production 44gSc from 44Ca powder, 68Ga from 68Zn foil covering the powder and 18F or 13N from liquid contained in the chamber. The radioisotopes produced can be separated during post processing.
Turning now to the drawings,
The split chamber 6 is cooled by the liquid flowing through the jacket 7 and ports 3A and 3B. The vapor 11 may condense on the surface of the vapor reservoir 6B. This will further facilitate the cooling of the target, i.e., the heat absorbed in the phase change from liquid to gas and the heat energy absorbed in the second phase change of vapor returning to liquid via condensation.
The evaporation chamber includes a closeable port 8 through which gas or liquid may be conveyed. The bottom of the liquid reservoir of the split chamber also contains a closeable port 9. It will be appreciated that the liquid or gas may be drained through this port. It will further be appreciated that due to the heat of the irradiation process, the solid target may melt, thereby mixing with the liquid 10. The solid target may also otherwise degrade causing particles to break from the surface, and also mix with the liquid. As discussed above, the produced radioisotopes may be concentrated on the outer surface of the target, and leach into the liquid.
In some embodiments, the solid target illustrated in
In another embodiment, after the liquid and vapor has been removed from the split chamber as described above, the lower port 9 can be closed and an agent such as diluted acid may be pumped into the split chamber 6 through port 8. The acid may be allowed contact with the target material (similar as to the liquid 10 and target 1 contact). The acid may dissolve the target material, thereby allowing the lower port 9 to be opened and the solution removed from the split chamber. Another novel feature of this disclosure is the option to use the particle beam to heat the acid to facilitate the dissolution of the solid target material. Also, the diluted acid may facilitate the leaching of the radioisotope product from the target. It will be appreciated that a diluted acid is an acid in which the concentration of water mixed in the acid is higher than the concentration of the acid itself.
It will be yet further appreciated that the disclosure is not limited to the shape or configuration of the structure that has been termed “split chamber.” Other configurations may be utilized. See for example
This specification is to be construed as illustrative only and is for the purpose of teaching those skilled in the art the manner of carrying out the disclosure. It is to be understood that the forms of the disclosure herein shown and described are to be taken as the presently preferred embodiments. As already stated, various changes may be made in the shape, size and arrangement of components or adjustments made in the steps of the method without departing from the scope of this disclosure. For example, equivalent elements may be substituted for those illustrated and described herein and certain features of the disclosure maybe utilized independently of the use of other features, all as would be apparent to one skilled in the art after having the benefit of this description of the disclosure.
While specific embodiments have been illustrated and described, numerous modifications are possible without departing from the spirit of the disclosure, and the scope of protection is only limited by the scope of the accompanying claims.
This Patent Application is a Divisional Application of U.S. patent application Ser. No. 16/777,271 filed Jan. 30, 2020, which claims priority to U.S. Provisional Patent Application Ser. No. 62/845,693 filed May 9, 2019, both of which applications are hereby incorporated by reference in their entirety.
Number | Date | Country | |
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Parent | 16777271 | Jan 2020 | US |
Child | 17660621 | US |