CN114242299A - Cyclotron metal composite target material for preparing targeted nuclide medicine - Google Patents

Cyclotron metal composite target material for preparing targeted nuclide medicine Download PDF

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CN114242299A
CN114242299A CN202111329308.7A CN202111329308A CN114242299A CN 114242299 A CN114242299 A CN 114242299A CN 202111329308 A CN202111329308 A CN 202111329308A CN 114242299 A CN114242299 A CN 114242299A
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target material
cyclotron
aluminum substrate
metal composite
composite target
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冯钰天
迈克尔·扎鲁茨基
马博然
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Astatine Fanukele Ningbo Medical Technology Co ltd
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Astatine Fanukele Ningbo Medical Technology Co ltd
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • G21G2001/0094—Other isotopes not provided for in the groups listed above

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  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Particle Accelerators (AREA)

Abstract

The invention discloses a cyclotron metal composite target material for preparing a targeted nuclide drug, which comprises an aluminum substrate with the shape matched with the shape of a target position of an accelerator, wherein a bismuth layer is attached or embedded on the surface of the aluminum substrate, and the thickness of the bismuth layer is 10-20 mu m. The invention provides a cyclotron metal composite target material for preparing targeted nuclide drugs, which reduces or even avoids melting of the target material, improves the heat conduction efficiency of the target material, and avoids pollution of equipment and products thereof.

Description

Cyclotron metal composite target material for preparing targeted nuclide medicine
Technical Field
The invention belongs to the field of targeted drug preparation, relates to a cyclotron target material, and particularly relates to a cyclotron metal composite target material.
Background
In recent years, radionuclide-containing targeted nuclides have been remarkably developed for diagnostic and therapeutic applications of diseases, and have gradually become one of the mainstream pharmaceutical means for cancer diagnosis and treatment. The targeted nuclide drug can deliver the radionuclide to the focus (including cancer cells and the like) through the targeted molecules, the diagnostic nuclide can release gamma rays with strong penetrating power to provide focus information, and the therapeutic nuclide can accurately release the radiation dose enough to kill cancer tissues so as to achieve the therapeutic effect. Among the numerous species, the alpha species astatine-211 (211At) has good physical properties and is very suitable forIs suitable for treating cancer.
The most critical factor limiting the development and popularization of nuclide drugs is the production source of the nuclide drugs. At present, only limited astatine-211 production and research application are reported by atomic science and technology institute of Sichuan university in China, but no cases are reported for large-scale production of astatine-211 enough for clinical use.
The mainstream astatine-211 production method uses high-energy alpha particle beams generated by a cyclotron to bombard a metallic bismuth target material, and the metallic bismuth target material is obtained by209Bi(α，2n)211At nuclear reaction produces astatine-211, but only 272 ℃ due to the low melting point of metallic bismuth, and poor thermal conductivity, only 7.97W/(Kxm). Therefore, in the case of high-energy particle beam bombardment, a phenomenon in which the target material is melted easily occurs, resulting in a reduction in production efficiency or a contamination damage of production equipment.
Disclosure of Invention
The technical problem to be solved by the invention is to provide a cyclotron metal composite target material for preparing targeted nuclide drugs, which reduces or even avoids the melting of the target material, improves the heat conduction efficiency of the target material, and avoids the pollution of equipment and products thereof, aiming at the defects of the prior art.
The technical scheme adopted by the invention for solving the technical problems is as follows: a cyclotron metal composite target material for preparing targeted nuclide drugs comprises an aluminum substrate of which the shape is matched with that of a target position of an accelerator, wherein a bismuth layer is attached or embedded on the surface of the aluminum substrate, and the thickness of the bismuth layer is 10-20 mu m.
Further, in the cyclotron metal composite target material for preparing a targeted nuclide drug, preferably, the aluminum substrate includes edge portions arranged at two sides of the aluminum substrate and a central portion arranged between the edge portions, and the top surface of the edge portions is higher than that of the central portion; the bismuth layer is provided in the center.
Further, in the cyclotron metal composite target material for preparing the targeted nuclide drug, preferably, the central part is provided with an inwards concave base groove along the axial direction, the bismuth layer is filled and embedded in the base groove, and the bismuth layer is flush with the surface of the central part.
Further, in the cyclotron metal composite target material for preparing targeted nuclide drugs, the base groove is preferably a through groove which penetrates through both ends of the center of the aluminum substrate; or the base groove is an end sealing groove with two closed ends, and the central parts of two axial sides of the end sealing groove are heat absorption areas.
Further, in the cyclotron metal composite target material for preparing the targeted nuclide drug, the bismuth layer is preferably in a dense and non-porous state.
Further, in the cyclotron metal composite target material for preparing the targeted nuclide drug, the bismuth layer preferably has a width of 1cm and a length of 7.5-8.5 cm.
Furthermore, in the cyclotron metal composite target material for preparing targeted nuclide drugs, the bottom surface of the base groove is preferably an arc surface which is axially symmetrical with respect to the aluminum substrate, and the lowest point of the arc surface is on the axial line of the aluminum substrate; or the lowest point of the bottom surface of the base groove is positioned in the center of the aluminum base, and the periphery of the base groove is smoothly transited from the top surface of the center part to the lowest point of the base groove.
Furthermore, in the cyclotron metal composite target material for preparing targeted nuclide drugs, an inwards concave cooling groove is preferably arranged on the back surface of the aluminum substrate.
Furthermore, in the cyclotron metal composite target material for preparing targeted nuclide drugs, preferably, a plurality of cooling grooves are arranged at intervals, and the shape of each cooling groove is a polygon, a curved surface or a combination of the polygon and the curved surface.
The target material is a composite target material with an aluminum substrate matched with a bismuth layer, wherein the aluminum substrate has good heat-conducting property, and the melting point of aluminum metal is 660.4 ℃, so that the temperature of the metal bismuth layer is reduced, the possibility of melting the target material is reduced, and the limit of maximum beam intensity is improved. Meanwhile, the thickness of the metal bismuth target is reduced to 10-20 μm, so that the utilization degree of the metal bismuth target is increased, the temperature rise of the target is reduced, the melting of the bismuth target is reduced, and the limit of the maximum beam intensity is improved; furthermore, reducing the thickness of the target material accelerates the release of astatine-211 during the distillation process, and reduces the requirement for distillation temperature, increasing the average production yield of astatine-211 from 10.6 ± 1.2 million beckers per microampere to 41 ± 7 million beckers per microampere, and increasing the maximum production capacity to ninety hundred million beckers.
Drawings
The invention will be further described with reference to the accompanying drawings and examples, in which:
FIG. 1 is a perspective view of a first embodiment of an example of the present invention;
FIG. 2 is a schematic structural diagram of the front side of an aluminum substrate according to a first embodiment of the present invention;
FIG. 3 is a schematic view of the backside structure of an aluminum substrate according to a first embodiment of the present invention;
FIG. 4 is a perspective view of a second embodiment of an example of the present invention;
FIG. 5 is a schematic front view of an aluminum substrate according to a second embodiment of the present invention.
Detailed Description
For a more clear understanding of the technical features, objects and effects of the present invention, embodiments of the present invention will now be described in detail with reference to the accompanying drawings.
An element is said to be "secured to" or "disposed on" another element, either directly or indirectly on the other element. When an element is referred to as being "connected to" another element, it can be directly or indirectly connected to the other element.
The terms "upper," "lower," "left," "right," "front," "back," "vertical," "horizontal," "top," "bottom," "inner," "outer," and the like refer to an orientation or position based on the orientation or position shown in the drawings.
The terms "axial," radial, "and" transverse "refer to the length of the entire device or component as" axial, "and the direction perpendicular to the axial direction as" radial "or" transverse.
The terms "first", "second", etc. are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features. The meaning of "plurality" is two or more unless specifically limited otherwise.
The above terms are for convenience of description only and are not to be construed as limiting the present technical solution.
The metal composite target material is used in a cyclotron for preparing targeted nuclide medicines, and has different target material size requirements and consistent structure requirements according to different cyclotrons.
The following is a detailed description taking a CS-30 type cyclotron as an example:
as shown in fig. 1-5, the cyclotron metal composite target material for preparing targeted nuclide drugs comprises an aluminum substrate 100 with a shape matched with the shape of a target site of an accelerator, wherein a bismuth layer 200 is attached to or embedded in the surface of the aluminum substrate 100, and the thickness of the bismuth layer 200 is 10-20 μm. The thickness range of the bismuth layer 200 is that the thickness of the metal bismuth layer 200 is reduced to 10 to 20 mu m on the basis of the prior art, so that the utilization degree of the metal bismuth target material is increased, namely the product At-211 produced by unit volume or unit mass is improved. Moreover, as the bismuth layer 200 is thinned, the heat conduction of the aluminum substrate 100 is increased, the temperature rise of the target material is reduced, the melting of the bismuth target material is reduced or even avoided, and the limit of the maximum beam intensity is improved; meanwhile, the release of astatine-211 in the distillation process can be accelerated by reducing the thickness of the target material, and the requirement of the distillation temperature is reduced.
When the cyclotron is operated, the energy of an incident high-energy alpha particle beam is 29 MeV, the energy of the particle beam is reduced along with the action of the particle beam and the target, when the particle beam is incident at an angle of 4.7 degrees, the energy of the alpha particle beam is reduced to be below 20 MeV at the thickness of the target which is below 10 mu m, the energy of the particle beam is already lower than the energy range for generating the astatine-211, so the astatine-211 is not generated any more, and therefore, the thickness of the target adopted by the invention is not lower than 10 mu m. The thicker the target material is more likely to melt leading to production failure, as determined by the heat generation of the bismuth target material, the thickness of the target material of the present invention is selected to be at most 20 μm. Thus, the bismuth layer 200 of the present invention is between 10 and 20 μm thick.
The composite target material comprises two parts, namely an aluminum substrate 100 and a bismuth layer 200. The shape of the aluminum substrate 100 is consistent with the shape of the target site of the built-in target of the cyclotron, and the aluminum substrate 100 of the invention has a strip-shaped axial concave structure and a one-step forming integral structure, and the size of the aluminum substrate is preferably 9.5cm in length, 2.1cm in width and 0.6cm in thickness. Specifically, the aluminum substrate 100 comprises edge portions 110 arranged at two sides of the aluminum substrate and a central portion 120 arranged between the edge portions 110, wherein the top surfaces of the edge portions 110 at two sides are flush and are planar, the top surface of the edge portion 110 is higher than that of the central portion 120, and the shape structure is consistent with the shape of a target position in the cyclotron; the width of the central portion 120 is preferably 1cm, and the bismuth layer 200 is provided in the central portion 120.
The central part 120 is provided with an inwards concave base groove along the axial direction, the bismuth layer 200 is filled and embedded in the base groove, the bismuth layer 200 can be made of metal bismuth material attached to the base groove of the central part 120 by adopting a magnetron sputtering method, and the wall surface of the base groove can be a smooth plane or a rough plane without affecting the attachment of the bismuth material. The cross-sectional shape of the base groove is not limited, and may be any structure from the width of the groove opening to the edge portion 110, such as a square, trapezoid, U-shaped, arc-shaped, other curved or straight line combination, etc., preferably a symmetrical structure, more preferably the cross-sectional shape of the base groove is U-shaped, i.e., two side wall surfaces are perpendicular to the bottom surface or the top surface of the aluminum base 100, still more preferably the cross-sectional shape of the base groove is arc-shaped, the bottom surface of the base groove is an arc surface, the arc surface is axially symmetrical with respect to the aluminum base 100, and the lowest point is on the axial line of the aluminum base 100; or alternatively, the lowest point of the base groove bottom surface is located at the center of the aluminum substrate 100 and the periphery thereof smoothly transitions from the top surface of the central portion 120 to the lowest point of the base groove, and the base groove is symmetrical about the axial centerline and the transverse centerline of the aluminum substrate 100.
The depth of the basal groove is 10-20 μm, which can mean the average depth of the basal groove, and the depth of the lowest point is 10-20 μm, preferably the depth of the lowest point is 20 μm at most. Specifically, the depth of the trench may be arbitrarily selected within this range, and preferably the depth is 10, 12, 15, 17, 18, 20 μm, the bismuth layer 200 is flush with the surface of the central portion 120, and the thickness of the bismuth layer 200 is also arbitrarily selected between 10 and 20 μm, and preferably the thickness is 10, 12, 15, 17, 18, 20 μm.
The base groove is divided into two embodiments according to the structure:
as shown in fig. 1 to 3, the first embodiment is: the base groove is an end seal groove with two closed ends, and the central part 120 of the two axial sides of the end seal groove is a heat absorption area 300. In the embodiment, the base groove is only positioned in the middle, the axial length of the base groove is relatively reduced, the two ends of the base groove are both aluminum substrates 100, and as the two ends of the aluminum substrates 100 are high-temperature areas, bismuth materials are not arranged at the high-temperature areas, so that the bismuth materials are prevented from being melted, the overall temperature of the bismuth layer 200 is reduced, the limit of the maximum beam intensity can be improved, and the production yield of astatine-211 is further improved.
According to the temperature distribution, the high-temperature region exists at the two ends of the target material, and the bismuth layer 200 is preferably 1cm wide and 7.5-8.5cm long. Within the size range, on one hand, the requirements of the cyclotron on the target material are met, and meanwhile, aluminum metal with higher melting point and better heat conductivity is arranged in a high-temperature area, so that the target material is prevented from melting, and meanwhile, optimal conditions are passed for producing astatine-211. The length of the bismuth layer 200 may be selected from any of the above ranges.
As shown in fig. 4-5, the second embodiment is: the through grooves extending through the center portion 120 of the aluminum substrate 100 to both ends thereof, i.e., the length of the through grooves is equal to the length of the aluminum substrate 100; the bismuth layer 200 is filled in the base groove and extends from one end of the aluminum substrate 100 to the other end. In this structure, the bismuth layer 200 has a reduced thickness, the utilization of the bismuth layer 200 is improved, heat is conducted through the aluminum substrate 100, the overall temperature of the target is reduced through the overall target heat-conducting property, and the problem of pollution caused by target melting is avoided.
The bismuth layer 200 is formed by attaching a metal bismuth material to the aluminum substrate 100 by a magnetron sputtering method, which may be performed by a conventional magnetron sputtering method and is not described herein again. The bismuth layer 200 is completely adhered to the base groove of the aluminum substrate 100, and has a dense non-porous structure, wherein the bismuth metal density in the bismuth layer 200 formed by sputtering reaches 9.8g/cm3Has a dense structure without abnormal pores.
As shown in FIG. 3, to further reduce the target temperature, the backside of the aluminum substrate 100 is provided with a concave cooling groove 500. The cooling grooves 500 are provided at intervals, and the shape of the cooling grooves 500 is polygonal, curved, or a combination thereof. The cooling bath 500 is used for water cooling and is cooled by increasing the heat dissipation area of the aluminum substrate 100.
The following is described in detail by way of specific examples:
embodiment 1, a cyclotron metal composite target material for preparing targeted nuclide drugs, comprising an aluminum substrate 100 with a shape matched with the shape of a target site of an accelerator, wherein the surface of the aluminum substrate 100 is attached or embedded with a bismuth layer 200, and the aluminum substrate 100 has a length of 9.5cm, a width of 2.1cm and a thickness of 0.6 cm. The base groove penetrates through the two ends of the aluminum substrate 100, and has a length of 9.5cm and a width of 1 cm. Specifically, the cross section of the base groove is concave with a radius of 71cm, the deepest point is at the center (axial center line) of the aluminum substrate 100, and the depth is 0.2 cm. The bismuth layer 200 has a thickness of 20 μm, a length of 9.5cm and a width of 1cm, and the aluminum substrate 100 has 7 cooling grooves 500 on its back surface, which are 0.2cm deep, 0.2cm wide and 7cm long, and can be cooled by cooling water. The cooling channel 500 is square in cross-section.
Embodiment 2, a cyclotron metal composite target material for preparing targeted nuclide drugs, comprising an aluminum substrate 100 with a shape matched with the shape of a target site of an accelerator, wherein the surface of the aluminum substrate 100 is attached or embedded with a bismuth layer 200, and the aluminum substrate 100 has a length of 9.5cm, a width of 2.1cm and a thickness of 0.6 cm. The base groove is an end sealing groove, the length of the end sealing groove is 8cm, and the width of the end sealing groove is 1 cm. The heat absorbing regions 300 at both ends are 0.75cm in length, respectively. The cross section of the base groove is square, the thickness of the bismuth layer 200 is 10 μm, the length is 8cm, the width is 1cm, 5 cooling grooves 500 with the depth of 0.3cm, the width of 0.15cm and the length of 8cm are arranged on the back surface of the aluminum substrate 100 and can be cooled by cooling water. The cooling channel 500 is arcuate in cross-section.
Embodiment 3, a cyclotron metal composite target material for preparing targeted nuclide drugs, comprising an aluminum substrate 100 with a shape matched with the shape of the target site of an accelerator, wherein the surface of the aluminum substrate 100 is attached or embedded with a bismuth layer 200, and the aluminum substrate 100 has a length of 9.5cm, a width of 2.1cm and a thickness of 0.6 cm. The base groove is a closed end groove, and has a length of 7.5cm and a width of 1 cm. Specifically, the lowest point of the base groove bottom surface is located at the center of the aluminum substrate 100 and the periphery thereof smoothly transitions from the top surface of the center portion 120 to the lowest point of the base groove, and the base groove is symmetrical about the axial centerline and the lateral centerline of the aluminum substrate 100. The groove depth at the lowest point is 20 μm, the bismuth layer 200 has a thickness of 10 μm-20 μm, a length of 7.5cm and a width of 1cm, and 4 cooling grooves 500 with a depth of 0.2cm, a width of 0.3cm and a length of 7cm are arranged on the back surface of the aluminum substrate 100 and can be cooled by cooling water. The cooling channel 500 is U-shaped in cross-section.
Embodiment 4, a cyclotron metal composite target material for preparing targeted nuclide drugs, comprising an aluminum substrate 100 with a shape matched with the shape of the target site of an accelerator, wherein the surface of the aluminum substrate 100 is attached or embedded with a bismuth layer 200, and the aluminum substrate 100 has a length of 9.5cm, a width of 2.1cm, and a thickness of 0.6 cm. The base groove is a closed end groove, the length of the base groove is 8.2cm, and the width of the base groove is 1 cm. Specifically, the cross section of the base groove is square, the bismuth layer 200 has a thickness of 15 μm, a length of 8.2cm and a width of 1cm, and 6 cooling grooves 500 with a depth of 0.2cm, a width of 0.2cm and a length of 8cm are formed on the back surface of the aluminum substrate 100 and can be cooled by cooling water. The cooling channel 500 is V-shaped in cross-section.
And (3) experimental test: the target materials of the embodiments 1-3 of the invention are respectively used for preparing astatine-211, and the preparation process and astatine-211 products are detected, wherein the parameters of the cyclotron are as follows: 1500W heating power
The following results were obtained:
Figure BDA0003348114490000091
as seen from the above table: the maximum temperature of the target material is 189.3 ℃, and the maximum temperature is lower than the melting temperature of the metal bismuth. Under the condition of the same power, the highest temperature of the target material in the prior art is 284.3 ℃, so the target material effectively avoids the problem that the target material is melted to pollute the product. Through the half-life period test, the astatine-211 half-life period produced by the target material of the invention is consistent with the literature report. The purity of the product astatine-211 is detected, the impurity content is below 2.3ppm, and compared with the prior art, the impurity content is greatly reduced. The production yield of astatine-211 is increased to greater than 41 megabeckers per microampere.

Claims (9)

1. A cyclotron metal composite target material for preparing targeted nuclide drugs is characterized by comprising an aluminum substrate, the shape of which is matched with that of a target position of an accelerator, wherein a bismuth layer is attached or embedded on the surface of the aluminum substrate, and the thickness of the bismuth layer is 10-20 microns.
2. The cyclotron metal composite target material for preparing a targeted nuclide drug of claim 1, wherein the aluminum substrate comprises edge portions arranged at two sides of the aluminum substrate and a central portion arranged between the edge portions, and the top surface of the edge portions is higher than that of the central portion; the bismuth layer is provided in the center.
3. The cyclotron metal composite target material for preparing targeted nuclide drugs as claimed in claim 1, wherein the central portion is provided with an inward concave base groove along the axial direction, the bismuth layer is embedded and embedded in the base groove, and the bismuth layer is flush with the surface of the central portion.
4. The cyclotron metal composite target material for preparing targeted nuclide drugs as claimed in claim 3, wherein the base groove is a through groove that penetrates to both ends of the center portion of the aluminum substrate; or the base groove is an end sealing groove with two closed ends, and the central parts of two axial sides of the end sealing groove are heat absorption areas.
5. The cyclotron metal composite target material for preparing targeted nuclide drugs as claimed in claim 1, wherein the bismuth layer is in a dense non-porous state.
6. The cyclotron metal composite target material for preparing targeted nuclide drugs as claimed in claim 1, wherein the bismuth layer has a width of 1cm and a length of 7.5-8.5 cm.
7. The cyclotron metal composite target material for preparing targeted nuclide drugs as claimed in claim 1, wherein the bottom surface of the base groove is an arc surface, the arc surface is axially symmetric with respect to the aluminum substrate, and the lowest point is on the axial line of the aluminum substrate; or the lowest point of the bottom surface of the base groove is positioned in the center of the aluminum base, and the periphery of the base groove is smoothly transited from the top surface of the center part to the lowest point of the base groove.
8. The cyclotron metal composite target material for preparing targeted nuclide drugs as claimed in claim 1, wherein the back surface of the aluminum substrate is provided with an inward-concave cooling groove.
9. The cyclotron metal composite target material for preparing targeted nuclide drugs as claimed in claim 8, wherein a plurality of cooling grooves are provided at intervals, and the cooling grooves have polygonal shapes, curved shapes, or a combination thereof.
CN202111329308.7A 2021-11-10 2021-11-10 Cyclotron metal composite target material for preparing targeted nuclide medicine Pending CN114242299A (en)

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