Method for producing and preparing 67Cu through irradiation of medium-high energy proton accelerator

Abstract

The invention discloses a method for producing and preparing 67Cu through irradiation of a medium-high energy proton accelerator. Comprising the following steps: determining that a target nuclide in a radiopharmaceutical to be produced is 67Cu, and determining a composite target material which can continuously produce the target nuclide 67Cu in the whole energy range of an accelerator comprising a medium-high energy section and a low energy section, the half-life period of the target nuclide 67Cu generated after each target material of the composite target material reacts with the protons is longer than the half-life period of the impurity nuclide generated along with the target material, and the radioactive nuclear purity of the target nuclide 67Cu is required to reach 99% or above through certain irradiation time and cooling time; a composite target material with relatively high target nuclide yield and relatively low impurity nuclide yield from a high-energy section to a low-energy section is selected, and the target material not only can control the ratio of the impurity nuclide / target nuclide, but also can consider the yield of 67Cu; according to the method, the target material in the medium-high energy section is combined with the target material in the low-energy section, and the target material in the low-specific-energy section is combined with the appropriate irradiation time, so that the yield is increased.

Description

Technical Field

[0001] The present invention belongs to the technical field of cyclotron radioisotope production, and specifically provides a medium- and high-energy proton accelerator irradiation production and preparation method. 67 Cu's method. Background Art

[0002] 67Cu has a half-life of 61.83 hours. Its emitted beta rays (average energy 141 keV) have short- to medium-range therapeutic effects on target cells. In addition to the therapeutic 141 keV beta particles, 67Cu also emits gamma rays of 185 keV (49%) and 93 keV (16%), which are suitable for SPECT imaging. Therefore, 67Cu is an ideal choice for radionuclide therapy and imaging. The future development of 67Cu is promising.

[0003] During the production of 67Cu, the impurity nuclide 64Cu is generally produced simultaneously. The half-life of 64Cu is 12.7h, and the half-life of 67Cu is 61.83h. Since they cannot be removed by chemical separation, they can only be reduced by natural decay. The lower the ratio of 64Cu / 67Cu, the more conducive it is to the production of 67Cu.

[0004] One of the reasons why the yield of 67Cu produced by existing cyclotrons is not high is that only one target material is generally used, and the energy range of a target material is limited, which is not conducive to improving the yield.

[0005] A second reason for the low yield of 67Cu produced by existing cyclotron accelerators is the lack of comprehensive planning for irradiation time. This lack of planning refers to the failure to consider the relationship between the proportion of impurity nuclides and irradiation time when designing the irradiation time, as well as the failure to consider the ratio between the yield growth rate and the nuclide decay rate. Because existing technologies fail to consider that a lower proportion of impurity nuclides is more conducive to higher yields, and that an appropriate irradiation time is required to ensure that the yield growth rate exceeds the decay rate of the target nuclides within that time, the yield improvement is unsatisfactory. Summary of the Invention

[0006] In response to the problems existing in the prior art, the present invention proposes a method for producing 67Cu by irradiation using a medium- to high-energy proton accelerator. The purpose is to solve the problems that the prior art generally uses only one target material, and the effective energy range of one target material that can be used to produce the target nuclide is limited, which is not conducive to improving the yield. In addition, the prior art does not have a comprehensive plan for the irradiation time, resulting in unsatisfactory yield improvement.

[0007] The present invention proposes the following technical solutions to solve the technical problems:

[0008] A medium- and high-energy proton accelerator irradiation production and preparation 67Cu method, the method comprising the following steps:

[0009] Step 1: Determine the target nuclide in the radiopharmaceutical to be produced. 67 Cu and used to produce target nuclides 67 Cu composite target material, which can continuously produce the target nuclide within the accelerator energy range 67 Cu composite target material, the accelerator energy range is the entire energy range including the medium and high energy segments and the low energy segment;

[0010] Step 2: Determine the target nuclide produced after each target material of the composite target reacts with protons 67 The half-life of Cu is greater than the half-life of the impurity nuclide; and it is determined that after each target material of the composite target reacts with protons, the target nuclide yield is relatively high and the impurity nuclide yield is relatively low; and it is determined that the composite target material undergoes a certain irradiation time and cooling time to make the target nuclide 67 The radioactive nuclear purity of Cu is required to reach more than 99%. The thickness of each target material of the composite target material is calculated by theory and Monte Carlo simulation software, so that the proton beam can still have appropriate energy to be incident on the target material behind after passing through the front target material. 67 Cu nuclide.

[0011] Furthermore, the composite target material of step 1 is: the first target material is arranged in sequence along the proton incident direction. 70 Zn, second target 68 Zn, third target 71 Ga, fourth target 70 Zn, fifth target 67 Zn; the impurity nuclides generated after the composite target reacts with protons are 64 Cu, 65 Cu, and impurity nuclides 64 The half-life of Cu is lower than that of the target nuclide 67 The half-life of Cu, 65 Cu is a stable isotope and does not decay.

[0012] Furthermore, the step 2 of determining that after each target material of the composite target material reacts with the proton, the target nuclide yield is relatively high and the impurity nuclide yield is relatively low is specifically as follows:

[0013] In the energy range of 58-75 MeV, 67 Cu has high yield, 64 The yield of Cu is relatively low. 70 Zn(p,x) 67 Cu reaction production 67 Cu;

[0014] In the energy range of 34-58 MeV, 67 Cu has high yield, 64 The yield of Cu is relatively low. 68 Zn(p,x) 67 Cu reaction production 67 Cu;

[0015] In the energy range of 25-34 MeV, 67 Cu has high yield, 65 The yield of Cu is relatively low. 71 Zn(p,x) 67 Cu reaction production 67 Cu;

[0016] In the energy range of 7-25MeV, 67 Cu has high yield, 65 The yield of Cu is relatively low. 70 Zn(p,x) 67 Cu reaction production 67 Cu;

[0017] In the residual energy range below 7MeV, the fifth target is used 67 Zn ensures that the remaining beam energy is completely deposited in the target, and at the same time, the neutrons generated by the proton beam in the cascade target composed of the first four targets are used to 67 Zn(n,p) 67 Cu reaction production 67 Cu.

[0018] Furthermore, the target nuclides produced after each target material of the composite target material reacts with the protons in step 2 are determined. 67 The half-life of Cu is greater than that of the impurity nuclide, specifically:

[0019] Using the first target 70 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 64 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life;

[0020] Using the second target 68 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 64 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life;

[0021] Using the third target 71 Zn(p,x) 67Cu reaction production 67 Cu, impurity nuclide 65 Cu is a stable isotope;

[0022] Using the fourth target 70 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 65 Cu is a stable isotope.

[0023] Furthermore, the thickness of each target material of the composite target material in step 2 is calculated by theoretical and Monte Carlo simulation software, so that the proton beam still has appropriate energy to be incident on the target material behind after passing through the front target material to produce 67 Cu nuclide, specifically: the first target material for the 58-75 MeV energy range 70 The thickness of Zn is 3.88mm; the second target material used in the energy range of 34-58MeV 68 The thickness of Zn is 4.03mm; the third target material used in the energy range of 25-34MeV 71 The thickness of Zn is 1.32mm; the fourth target material used in the energy range of 7-25MeV 70 The thickness of Zn is 1.3 mm; the fifth target used in the remaining energy range 67 The thickness of Zn is 125 mm.

[0024] Furthermore, the step 2 of determining that the composite target material undergoes a certain irradiation time and cooling time to make the target nuclide 67 The radioactive nuclide purity of Cu is required to reach more than 99%. Specifically, when the irradiation time is the irradiation time when the growth rate of the ratio of the target nuclide to the impurity nuclide reaches a relatively stable saturation point, the cooling days of the first target, the second target, the third target, the fourth target, and the fifth target corresponding to the saturation point irradiation time.

[0025] Furthermore, the irradiation time is the irradiation time during which the growth rate of the ratio of the target nuclide to the impurity nuclide reaches a relatively stable level, and the irradiation time is 8 days.

[0026] Furthermore, the cooling days corresponding to the saturation point irradiation time are 4 days for the first target, 6 days for the second target, 0 day for the third target, 0 day for the fourth target, and 0 day for the fifth target.

[0027] Advantages and effects of the present invention

[0028] 1. The present invention combines the selection of target materials in the medium and high energy segments with the selection of target materials in the low energy segment to improve the yield: the target materials in the medium and high energy segments are selected because protons first enter the target materials in the medium and high energy segments, and consume a certain amount of energy to penetrate the target materials in the medium and high energy segments before entering the target materials in the low energy segment; the target materials in the low energy segment are selected because the proportion of impurity nuclides after the reaction between the target materials in the low energy segment and protons is lower, and no cooling time is required. If no cooling time is required, the target nuclides in the low energy segment will not decay during the cooling time, thereby improving the yield.

[0029] 2. The present invention combines the selection of target materials with low energy percentages and the selection of appropriate irradiation time to improve the yield: the selection of target materials with low energy percentages is to reduce the excessive cooling time caused by excessive impurities. If the cooling time is too long, the decay of the target nuclide will increase with the cooling time; the selection of appropriate irradiation time is because once the irradiation time exceeds the saturation point, the rate of production capacity growth cannot keep up with the rate of target nuclide decay during the irradiation process (both the target nuclide and the impurity nuclide will decay). In order to increase the yield, the irradiation is terminated when the irradiation time has reached 68.94% of the target nuclide 67Cu. However, the irradiation time is not the less the better, from Figure 8 It can be seen that the production capacity increases with the increase of the number of irradiation days after 1 day of irradiation and after 8 days of irradiation. In this embodiment, in order to improve the production capacity, 8 days should be selected as the appropriate irradiation time. BRIEF DESCRIPTION OF THE DRAWINGS

[0030] Figure 1 The proton beam of the present invention is incident on 70 Zn target, 68 Zn target, 71 Ga target, 70 Zn and 67 Schematic diagram of Zn target;

[0031] Figure 2 For the present invention 68 Zn target and 70 Zn target and proton reaction production 67 Reaction cross sections of Cu and 64Cu;

[0032] Figure 3 for Figure 2 middle 68 Further description of Zn target: 68 Zn target and proton reaction production 67 Reaction cross sections of Cu and 64Cu;

[0033] Figure 4 for Figure 2 middle 70 Further description of Zn target: 70 Zn target and proton reaction production 67 Cu,64 Cu and 65 Reaction cross section of Cu;

[0034] Figure 5 For the present invention 71 Ga target and proton reaction production 67 Cu and 65 Reaction cross section of Cu;

[0035] Figure 6 For the present invention 67 Timeline of Cu proportion changes with irradiation days;

[0036] Figure 7 Table 1: Target thickness corresponding to target materials in different energy ranges of the present invention;

[0037] Figure 8 Table 2 of the present invention: 70 Zn target under different irradiation times in the range of 58-75 MeV 67 Cu proportion;

[0038] Figure 9 Table 3: The results of different targets under proton irradiation for 8 days 67 Cooling days required for Cu content to be greater than 99%;

[0039] Figure 10 This invention is a kind of medium and high energy proton accelerator irradiation production preparation 67 Flowchart of the method for Cu. DETAILED DESCRIPTION

[0040] Design principle of the present invention

[0041] 1. The innovation lies in: combining the selection of medium and high energy target materials with the selection of low energy target materials, and combining the selection of low energy target materials with the selection of appropriate irradiation time. The ultimate goal of this combination is to improve 67 The yield of Cu. The target material in the low energy range is selected because the proportion of impurity nuclides after the reaction between the target material in the low energy range and the protons is lower, and no cooling time is required. Without cooling time, the target nuclides in the low energy range will not decay during the cooling time, thereby increasing the yield; the appropriate irradiation time is selected because once the irradiation time exceeds the saturation point, the rate of production capacity growth cannot keep up with the rate of target nuclides decay during the irradiation process (both the target nuclides and the impurity nuclides will decay). In order to increase the yield, the irradiation is terminated when the irradiation time has reached 68.94% of the target nuclide 67Cu. However, the irradiation time is not the less the better, from Figure 8 It can be seen that the production capacity increases with the increase of the number of irradiation days after 1 day of irradiation and after 8 days of irradiation. In this embodiment, in order to improve the production capacity, 8 days should be selected as the appropriate irradiation time.

[0042] 2. Design Principle of the Invention

[0043] 1. Combination of high energy segment and low energy segment: Conventional methods for producing nuclides generally do not occupy the entire accelerator energy segment, but only select one energy segment in the accelerator. The present invention fully utilizes the medium-high energy segment and the low energy segment, and selects the first, second, third, and fourth target materials from the medium-high energy segment to the low energy segment of the accelerator (the fifth target material is used to collect the remaining energy). The reason why the present invention selects the target material of the low energy segment is that after the target material of the low energy segment reacts with protons, the proportion of impurity nuclides produced (impurity nuclides / (impurity nuclides + target nuclides)) is relatively low (such as Figure 4 In the 7-25MeV range shown, the 65Cu / 67Cu ratio is low. Figure 5 The 65Cu / 67Cu ratio is low in the 25-34MeV range, while the proportion of impurity nuclides after the reaction between the target material and protons in the medium and high energy segments is high. Since the proportion of impurity nuclides in the low energy segment is very low, and the half-life of the impurity nuclides is shorter than the half-life of the target nuclides (if the half-life is small, it will decay first, and the remaining is the target nuclides, so the purity of the target nuclides can reach the required 99% or more), the impurity nuclides produced in the low energy segment with a small proportion almost do not require cooling time. Since both the target nuclides and the impurity nuclides decay during the cooling time, no cooling time is required and no target nuclides decay. Therefore, in order to improve the yield of 67Cu, the present invention not only uses target materials in the medium and high energy segments, but also selects a low energy segment with a high yield of target nuclides.

[0044] 2. Combination of low energy segment and irradiation time; the low energy segment refers to the first four targets 70 Zn, 68 Zn, 71 Zn, 70 The energy ranges selected for Zn are 58-75MeV, 34-58MeV, 25-34MeV, and 7-25MeV, which have the lowest proportion of impurity nuclides compared to other energy ranges. The combination of the low-proportion energy range and the irradiation time means that on the one hand, the proportion of impurity nuclides is as low as possible (the lower the proportion of impurity nuclides, the shorter the cooling time, and the less the decay of the target nuclides during the cooling time), and on the other hand, the irradiation time is controlled at a saturation point. The saturation point refers to the point where the yield of the target nuclides tends to increase slowly when the irradiation time exceeds this saturation point. Figure 6 As shown in the figure, after the irradiation time exceeds 8 days, the yield increase is not obvious. The purpose of controlling the irradiation time is to improve the yield. As the irradiation time increases, the target nuclide also decays. Although the yield increase is not obvious when the saturation point is reached, the decay rate of the target nuclide remains unchanged as the irradiation time increases. Therefore, controlling the irradiation time is also one aspect of improving the 67Cu yield.

[0045] Based on the above principles, the present invention designs a medium and high energy proton accelerator irradiation production preparation method. 67 Cu's method Figure 10 As shown, the method includes the following steps:

[0046] Step 1: Determine the target nuclide in the radiopharmaceutical to be produced. 67 Cu and used to produce target nuclides 67 Cu composite target material, which can continuously produce the target nuclide within the accelerator energy range 67 Cu composite target material, the accelerator energy range is the entire energy range including the medium and high energy segments and the low energy segment;

[0047] Step 2: Determine the target nuclide produced after each target material of the composite target reacts with protons 67 The half-life of Cu is greater than the half-life of the impurity nuclide; and it is determined that after each target material of the composite target reacts with protons, the target nuclide yield is relatively high and the impurity nuclide yield is relatively low; and it is determined that the composite target material undergoes a certain irradiation time and cooling time to make the target nuclide 67 The radioactive nuclear purity of Cu is required to reach more than 99%. The thickness of each target material of the composite target material is calculated by theory and Monte Carlo simulation software, so that the proton beam can still have appropriate energy to be incident on the target material behind after passing through the front target material. 67 Cu nuclide.

[0048] like Figure 1 As shown, the composite target material of step 1 is: arranged in sequence along the proton incident direction, the first target material 70 Zn, second target 68 Zn, third target 71 Ga, fourth target 70 Zn, fifth target 67 Zn; the impurity nuclides generated after the composite target reacts with protons are 64 Cu, 65 Cu, and impurity nuclides 64 The half-life of Cu is lower than that of the target nuclide 67 The half-life of Cu, 65 Cu is a stable isotope and does not decay.

[0049] like Figure 2-5 The step 2 of determining that after each target material of the composite target material reacts with the proton, the target nuclide yield is relatively high and the impurity nuclide yield is relatively low is specifically as follows:

[0050] In the energy range of 58-75 MeV, 67 Cu has high yield,64 The yield of Cu is relatively low. 70 Zn(p,x) 67 Cu reaction production 67 Cu;

[0051] In the energy range of 34-58 MeV, 67 Cu has high yield, 64 The yield of Cu is relatively low. 68 Zn(p,x) 67 Cu reaction production 67 Cu;

[0052] In the energy range of 25-34 MeV, 67 Cu has high yield, 65 The yield of Cu is relatively low. 71 Zn(p,x) 67 Cu reaction production 67 Cu;

[0053] In the energy range of 7-25MeV, 67 Cu has high yield, 65 The yield of Cu is relatively low. 70 Zn(p,x) 67 Cu reaction production 67 Cu;

[0054] In the residual energy range below 7MeV, the fifth target is used 67 Zn ensures that the remaining beam energy is completely deposited in the target, and at the same time, the neutrons generated by the proton beam in the cascade target composed of the first four targets are used to 67 Zn(n,p) 67 Cu reaction production 67 Cu.

[0055] The step 2 is to determine the target nuclides produced after each target material of the composite target material reacts with the protons. 67 The half-life of Cu is greater than that of the impurity nuclide, specifically:

[0056] Using the first target 70 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 4 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life;

[0057] Using the second target 68 Zn(p,x) 67 Cu reaction production 67 Cu, the half-life of the impurity nuclide 4Cu is shorter than that of the target nuclide67 Half-life of Cu; impurity nuclides 65 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life;

[0058] Using the third target 71 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 65 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life;

[0059] Utilize the fourth target 70 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 65 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life;

[0060] like Figure 1 As shown, the thickness of each target material of the composite target material in step 2 is calculated by theory and Monte Carlo simulation software, so that the proton beam still has appropriate energy to be incident on the target material behind after passing through the front target material. 67 Cu nuclide, specifically: the first target material for the 58-75 MeV energy range 70 The thickness of Zn is 3.88mm; the second target material used in the energy range of 34-58MeV 68 The thickness of Zn is 4.03mm; the third target material used in the energy range of 25-34MeV 71 The thickness of Zn is 1.32mm; the fourth target material used in the energy range of 7-25MeV 70 The thickness of Zn is 1.3 mm; the fifth target used in the remaining energy range 67 The thickness of Zn is 125 mm.

[0061] like Figure 6 、 Figure 8 、 Figure 9 As shown in the step 2, the composite target material is determined to have a target nuclide through a certain irradiation time and cooling time. 67 The radioactive nuclide purity of Cu is required to reach more than 99%. Specifically, when the irradiation time is the irradiation time when the growth rate of the ratio of the target nuclide to the impurity nuclide reaches a relatively stable saturation point, the cooling days of the first target, the second target, the third target, the fourth target, and the fifth target corresponding to the saturation point irradiation time.

[0062] like Figure 6 、 Figure 8 、 Figure 9As shown, the irradiation time is the irradiation time when the growth rate of the ratio of the target nuclide to the impurity nuclide reaches a relatively stable level, and the irradiation time is 8 days.

[0063] like Figure 6 、 Figure 8 、 Figure 9 As shown, the cooling days corresponding to the saturation point irradiation time are 4 days for the first target, 6 days for the second target, 0 day for the third target, 0 day for the fourth target, and 0 day for the fifth target.

[0064] Example 1

[0065] Taking the 75MeV high-current proton cyclotron as an example, the current intensity during production is 200μA, and the proton beam irradiates the target for 8 days. Figure 2 yes 68 Zn target and 70 Zn target and proton reaction production 67 Cu and 64 The reaction cross section of Cu is simulated by Monte Carlo software. The 75MeV proton beam generated by the accelerator is first incident on the 3.88mm thick 70 On the Zn target,

[0066] First, as Figure 2 As shown, in the energy range of 58-78MeV, 67 Cu has high yield, 64 The yield of Cu is relatively low, so the use of 70 Zn(p,x) 67 Cu reaction production 67 Cu,

[0067] Second, if Figure 2 As shown, wear out 70 After the Zn target, the proton energy is 58MeV, in the energy range of 34-58MeV, 67 Cu has high yield, 64 The yield of Cu is relatively low, and the beam is incident on a 4.03mm thick 68 On the Zn target, 68 Zn(p,x) 67 Cu reaction production 67 Cu; in the energy range of 34-58MeV 68 Zn target production 67 Although Cu is less than 58-78 MeV, 70 Zn target production 67 Cu, but this time it is 70 Zn target production 64 The peak range of Cu is used 68 Zn production 64 Cu / 67The Cu ratio is lower, so choose the one with lower cost. 68 Zn target is the most cost-effective method.

[0068] Third, if Figure 5 As shown, wear out 68 After the Zn target, the proton energy is 34MeV, in the energy range of 25-34MeV, in order to ensure 65 Cu / 67 The Cu ratio is low while taking into account 67 Cu yield, select 71 Ga target, target thickness 1.32mm, through 71 Ga(p,x) 67 Cu reaction production 67 Cu.

[0069] Fourth, if Figure 4 As shown, wear out 71 Ga target, the proton energy is 25MeV, in the energy range of 7-25MeV, in order to ensure 65 Cu / 67 The Cu ratio is low while taking into account 67 Cu yield, select 70 Zn target, through 70 Zn(p,x) 67 Cu reaction production 67 Cu. Pierce 70 After the Zn target, the proton energy is 7MeV. 70 The thickness of the Zn target was 1.3 mm.

[0070] Fifth, in order to block the remaining energy of the beam, the neutrons generated by the proton beam in the cascade target (the neutrons are generated by the previous four targets) are placed at the position of the fifth target. 67 Zn target, through neutrons and 67 Zn reaction ( 67 Zn(n,p) 67 Cu) production 67 Cu. 67 The thickness of the Zn target is 95 mm.

[0071] Summary Figure 7 、 Figure 8 、 Figure 9 As shown in Table 1, Table 2 and Table 3.

[0072] The present invention produces by multi-stage cascade target 67 Cu, fully utilize the energy of the accelerator and reduce the main impurity nuclides by optimizing the irradiation time and cooling time. 64 Cu ratio, increase 67 Cu production to meet future market product demand.

[0073] It should be emphasized that the above specific embodiments are merely explanations of the present invention and are not limitations of the present invention. After reading this specification, those skilled in the art may make non-creative modifications to the above embodiments as needed, but as long as they are within the scope of the claims of the present invention, they are protected by patent law.

Claims

1. A medium- and high-energy proton accelerator irradiation production and preparation 67 Cu method, the method comprising the following steps: Step 1: Determine the target nuclide in the radiopharmaceutical to be produced. 67 Cu and used to produce target nuclides 67 Cu composite target material, which can continuously produce the target nuclide within the accelerator energy range 67 Cu composite target material, the accelerator energy range is the entire energy range including the medium and high energy segments and the low energy segment; Step 2: Determine the target nuclide produced after each target material of the composite target reacts with protons 67 The half-life of Cu is greater than the half-life of the impurity nuclide; and it is determined that after each target material of the composite target reacts with protons, the target nuclide yield is relatively high and the impurity nuclide yield is relatively low; and it is determined that the composite target material undergoes a certain irradiation time and cooling time to make the target nuclide 67 The radioactive nuclear purity of Cu is required to reach more than 99%. The thickness of each target material of the composite target material is calculated by theory and Monte Carlo simulation software, so that the proton beam can still have appropriate energy to be incident on the target material behind after passing through the front target material. 67 Cu nuclide.

2. A medium- and high-energy proton accelerator irradiation production and preparation according to claim 1 67 Cu's method, characterized in that: The composite target material of step 1 is: arranged in sequence along the proton incident direction, the first target material 70 Zn, second target 68 Zn, third target 71 Ga, fourth target 70 Zn, fifth target 67 Zn; the impurity nuclides generated after the composite target reacts with protons are 64 Cu, 65 Cu, and impurity nuclides 64 The half-life of Cu is lower than that of the target nuclide 67 The half-life of Cu, 65 Cu is a stable isotope and does not decay.

3. A medium-high energy proton accelerator irradiation production preparation according to claim 2 67 Cu's method, characterized in that: The step 2 of determining that after each target material of the composite target material reacts with the proton, the target nuclide yield is relatively high and the impurity nuclide yield is relatively low is specifically as follows: In the energy range of 58-75 MeV, 67 Cu has high yield, 64 The yield of Cu is relatively low. 70 Zn(p,x) 67 Cu reaction production 67 Cu; In the energy range of 34-58 MeV, 67 Cu has high yield, 64 The yield of Cu is relatively low. 68 Zn(p,x) 67 Cu reaction production 67 Cu; In the energy range of 25-34 MeV, 67 Cu has high yield, 65 The yield of Cu is relatively low. 71 Zn(p,x) 67 Cu reaction production 67 Cu; In the energy range of 7-25MeV, 67 Cu has high yield, 65 The yield of Cu is relatively low. 70 Zn(p,x) 67 Cu reaction production 67 Cu; In the residual energy range below 7MeV, the fifth target is used 67 Zn ensures that the remaining beam energy is completely deposited in the target, and at the same time, the neutrons generated by the proton beam in the cascade target composed of the first four targets are used to 67 Zn(n,p) 67 Cu reaction production 67 Cu.

4. A medium- and high-energy proton accelerator irradiation production method according to claim 3 67 Cu's method, characterized in that: The step 2 is to determine the target nuclides produced after each target material of the composite target material reacts with the protons. 67 The half-life of Cu is greater than that of the impurity nuclide, specifically: Using the first target 70 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 64 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life; Using the second target 68 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 64 The half-life of Cu is shorter than that of the target nuclide 67 Cu half-life; Using the third target 71 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 65 Cu is a stable isotope; Using the fourth target 70 Zn(p,x) 67 Cu reaction production 67 Cu, impurity nuclide 65 Cu is a stable isotope.

5. The method for producing 67Cu by irradiation with a medium- to high-energy proton accelerator according to claim 3, characterized in that: The thickness of each target material of the composite target material in step 2 is calculated by theoretical and Monte Carlo simulation software, so that the proton beam still has appropriate energy to be incident on the target material behind after passing through the front target material. 67 Cu nuclide, specifically: the first target material for the 58-75 MeV energy range 70 The thickness of Zn is 3.88mm; the second target material used in the energy range of 34-58MeV 68 The thickness of Zn is 4.03mm; the third target material used in the energy range of 25-34MeV 71 The thickness of Zn is 1.32mm; the fourth target material used in the energy range of 7-25MeV 70 The thickness of Zn is 1.3 mm; the fifth target used in the remaining energy range 67 The thickness of Zn is 125mm.

6. The method of producing by irradiation of a medium- and high-energy proton accelerator according to claim 1 67 Cu's method, characterized in that: The step 2 determines that the composite target material has a target nuclide after a certain irradiation time and cooling time. 67 The radioactive nuclide purity of Cu is required to reach more than 99%. Specifically, when the irradiation time is the irradiation time when the growth rate of the ratio of the target nuclide to the impurity nuclide reaches a relatively stable saturation point, the cooling days of the first target, the second target, the third target, the fourth target, and the fifth target corresponding to the saturation point irradiation time.

7. A medium- and high-energy proton accelerator irradiation production method according to claim 6 67 Cu's method, characterized in that: The irradiation time is the irradiation time during which the growth rate of the ratio of the target nuclide to the impurity nuclide reaches a relatively stable state, and the irradiation time is 8 days.

8. A medium- and high-energy proton accelerator irradiation production method according to claim 7 67 Cu's method, characterized in that: The cooling days corresponding to the saturation point irradiation time are 4 days for the first target, 6 days for the second target, 0 day for the third target, 0 day for the fourth target, and 0 day for the fifth target.

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