(5) Influence of Different Adsorption Times

In this example, yttrium-loaded CMSs prepared through the following adsorption times were tested: 1 min, 2 min, 5 min, 10 min, 20 min, 30 min, 40 min, 60 min, and 120 min, and test results are shown in FIG. 5.

It can be seen from FIG. 5 that the adsorption of the CMS to the yttrium is a fast kinetic process, and when the adsorption time is greater than or equal to 2 min, the load rate is greater than 99%.

(6) Influence of Different Added Yttrium Amounts

In this example, yttrium-loaded CMSs prepared at the following added yttrium amounts were tested: 0.2, 0.5, 1, 2, 4, and 8 mg/0.25 g, and test results are shown in FIG. 6.

It can be seen from FIG. 6 that the added yttrium amount has an influence on the adsorption rate to some extent. When the added yttrium amount increases to 32 mg/g, the yttrium load rate of the CMS is 90.7%, indicating that a saturated yttrium load per gram of the CMS can be greater than 32 mg.

It should be noted that adsorption behaviors of the CMS to other rare earth elements are very similar to the adsorption behavior of the CMS to yttrium without a significant difference. Detailed data of research on the influencing factors will not be provided in the subsequent examples.

Example 12

Preparation of a Medical Yttrium-90-Loaded CMS

A yttrium-90 ion, a small organic molecule, and water were mixed to allow a reaction to obtain a complex as follows: 1 mL of a 1.0 g/L yttrium trichloride aqueous solution was added to a reaction flask. A radioactive yttrium-90 solution with an activity of 2 Ci was added. Then a specified volume of a 1.0 g/L 5-SSA solution was added, such that the molar amount of the 5-SSA was 5 times a molar amount of the yttrium, and water was added to 50 mL. The pH value of the resulting solution was adjusted to 4.5, water with a pH value of 4.5 was added to 100 mL, and the resulting solution was thoroughly shaken to obtain the complex for later use.

A CMS was allowed to adsorb the complex as follows: 1.0 g of the CMS with a particle size of 20 μm to 60 μm was weighed and added to the above complex solution, and the resulting mixture was stirred for 20 min to complete the adsorption.

The CMS adsorbing the complex was subjected to a first treatment as follows: The supernatant was taken and tested for yttrium-90 radioactivity, and an adsorption rate for the radionuclide was calculated to be 99.2%. 150 mL of a 0.1 mol/L sodium phosphate solution was added to the solution of the CMS adsorbing the complex, and the resulting mixture was stirred for 5 min.

Cleaning and dispensing the yttrium-90-loaded CMS: The yttrium-90-loaded CMS product was washed twice with water for injection (WFI), and the resulting mixture was subjected to solid-liquid separation (SLS) to obtain a yttrium-90-loaded CMS solid. 10 mL of WFI was added to the solid to obtain a suspension, which was equally dispensed into 10 bottles with 1 mL in each bottle. Each bottle had a radioactivity of about 195 mCi and included about 100 mg of the yttrium-90-loaded CMS; the suspension was sterilized at 121° C. for 15 min to obtain a yttrium-90-loaded CMS product for injection.

A dissolution rate of the yttrium-90 nuclide in the yttrium-90-loaded CMS was detected as follows: About 20 mg of the above yttrium-90-loaded CMS was added to a hydrothermal reactor, 20 mL of WFI or a 0.9% sodium chloride solution was added, and the hydrothermal reactor was sealed and placed in a constant-temperature oven with heating and incubation procedures set and run. The resulting system was cooled to room temperature and centrifuged, and a specified volume of the resulting supernatant was taken and tested for activity, and a dissolution rate was calculated. The product was incubated at each temperature of 40° C. (1.0 MPa), 80° C. (1.0 MPa), 100° C. (1.0 MPa), 120° C. (2.0 MPa), 140° C. (3.6 MPa), 160° C. (6.1 MPa), and 180° C. (10.0 MPa) for 2 h, and then a release rate of the yttrium-90 nuclide was tested. Test results are shown in Table 1 below.

Table 1 Yttrium-90 dissolution rates of the yttrium-90-loaded CMS in aqueous solutions at different temperatures and pressures

Experimental
Yttrium-90

conditions
dissolution rate
Yttrium-90

(temperature;
(0.9% sodium
dissolution rate

No.
pressure; time)
chloride solution)
(WFI)

1
40° C.; 1.0 Mpa; 2 h
0.0732%
0.0094%

2
80° C.; 1.0 Mpa; 2 h
0.0718%
0.0334%

3
100° C.; 1.0 Mpa; 2 h
0.0429%
0.0383%

4
120° C.; 2.0 Mpa; 2 h
0.0216%
0.0323%

5
140° C.; 3.6 Mpa; 2 h
0.0782%
0.0158%

6
160° C.; 6.1 Mpa; 2 h
0.0656%
0.0718%

7
180° C.; 10.0 Mpa; 2 h
0.0753%
0.0824%

The results in Table 1 show that dissolution rates of the yttrium-90 nuclide of the yttrium-90-loaded CMS product in the WFI and 0.9% sodium chloride solution at 40° C. to 180° C. (pressure: 1.0 MPa to 10.0 MPa) are each lower than 0.1%.

Example 13

Preparation of a Yttrium-90-Loaded CMS

Yttrium-90, a small organic molecule, and water were mixed to allow a reaction to obtain a complex as follows: 1 mL of a 1.0 g/L yttrium trichloride aqueous solution was added to a reaction flask, radioactive yttrium-90 solution with an activity of 10 mCi was added, then a specified volume of a 1.0 g/L 5-NSA solution was added such that a molar amount of the 5-NSA was 6 times a molar amount of the yttrium, and water was added to 50 mL. The pH value of the resulting solution was adjusted to 5.5, water with a pH value of 5.5 was added to 100 mL, and the resulting solution was thoroughly shaken to obtain the complex for later use.

A CMS was allowed to adsorb the complex as follows: 1.0 g of the CMS with a particle size of 20 μm to 60 μm was weighed and added to the above complex solution, and the resulting mixture was stirred for 20 min to complete the adsorption.

The CMS adsorbing the complex was subjected to a first treatment as follows: The supernatant was taken and tested for yttrium-90 radioactivity. The adsorption rate for the radionuclide was calculated to be 98.1%. 150 mL of a 0.1 mol/L sodium phosphate solution was added to the solution of the CMS adsorbing the complex, and the resulting mixture was stirred for 5 min.

Cleaning, sterilizing, and dispensing of the yttrium-90-loaded CMS: The yttrium-90-loaded CMS product was washed twice with WFI. The resulting mixture was subjected to SLS to obtain a yttrium-90-loaded CMS solid, and 10 mL of WFI was added to the solid to obtain a suspension, which was equally dispensed into 10 bottles with 1 mL in each bottle. Each bottle had a radioactivity of about 0.96 mCi and included about 100 mg of the yttrium-90-loaded CMS, and the suspension was sterilized at 121° C. for 15 min.

A yttrium-90 dissolution rate of the yttrium-90-loaded CMS was detected as follows: A bottle of the above product was taken and centrifuged, the resulting supernatant was collected and tested for activity, and a yttrium-90 dissolution rate was calculated to be 0.0435%.

Example 14

Preparation of a Medical Lutetium-177-Loaded CMS

Lutetium-177, a small organic molecule, and water were mixed to allow a reaction to obtain a complex as follows: 0.2 mL of a 1.0 g/L lutetium trichloride aqueous solution was added to a reaction flask, a radioactive lutetium-177 solution with an activity of 0.8 Ci was added, then a specified volume of a 1.0 g/L 5-SSA solution was added such that a molar amount of the 5-SSA was 4 times a molar amount of the lutetium, and water was added to 20 mL. The pH value of the resulting solution was adjusted to 5.0, water with a pH value of 5.0 was added to 30 mL, and the resulting solution was thoroughly shaken to obtain the complex for later use.

A CMS was allowed to adsorb the complex as follows: 0.3 g of the CMS with a particle size of 20 μm to 60 μm was weighed and added to the above complex solution, and the resulting mixture was stirred for 20 min to complete the adsorption.

The CMS adsorbing the complex was subjected to a first treatment as follows: The supernatant was taken and tested for lutetium-177 radioactivity, and the adsorption rate for the radionuclide was calculated to be 99.3%; 150 mL of a 0.1 mol/L sodium phosphate solution was added to the solution of the CMS adsorbing the complex, and the resulting mixture was stirred for 5 min.

Cleaning and dispensing of the lutetium-177-loaded CMS: The lutetium-177-loaded CMS product was washed twice with WFI, the resulting mixture was subjected to SLS to obtain a lutetium-177-loaded CMS solid, and 6 mL of WFI was added to the solid to obtain a suspension, which was equally dispensed into 3 bottles with 2 mL in each bottle. Each bottle had a radioactivity of about 250 mCi and included about 100 mg of the lutetium-177-loaded CMS. The suspension was sterilized at 121° C. for 15 min to obtain a lutetium-177-loaded CMS product for injection.

A dissolution rate of the lutetium-177 nuclide in the lutetium-177-loaded CMS was detected as follows: 20 mg of the above lutetium-177-loaded CMS was added to a hydrothermal reactor, 20 mL of WFI or a 0.9% sodium chloride solution was added, and the hydrothermal reactor was sealed and incubated at 120° C. for 2 h in a constant-temperature oven. The resulting system was cooled to room temperature and centrifuged, a specified volume of the resulting supernatant was tested for activity, and the dissolution rate was calculated. The results show that the lutetium-177-loaded CMS has a dissolution rate of 0.0788% in the 0.9% sodium chloride solution and a dissolution rate of 0.0548% in the WFI.

Example 15

Preparation of a Medical Holmium-166/Holmium-165-Loaded CMS

Holmium-166/holmium-165, a small organic molecule, and water were mixed to allow a reaction to obtain a complex as follows: 0.5 mL of a 0.5 g/L holmium chloride (holmium-165) aqueous solution was added to a reaction flask, a radioactive holmium-166 solution with an activity of 0.5 Ci was added, then a specified volume of a 1.0 g/L 5-SSA solution was added such that a molar amount of the 5-SSA was 4.5 times a molar amount of the holmium, and water was added to 30 mL. The pH value of the resulting solution was adjusted to 4.2, and the resulting solution was thoroughly shaken to obtain the complex for later use.

A CMS was allowed to adsorb the complex as follows: 0.3 g of the CMS with a particle size of 20 μm to 60 μm was weighed and added to the above complex solution, and the resulting mixture was stirred for 10 min to complete the adsorption.

The CMS adsorbing the complex was subjected to a first treatment as follows: The supernatant was tested for holmium-166 radioactivity, and the adsorption rate for the radionuclide was calculated to be 98.6%. 150 mL of a 0.1 mol/L sodium phosphate solution was added to the solution of the CMS adsorbing the complex, and the resulting mixture was stirred for 5 min.

Cleaning and dispensing of the holmium-loaded CMS: The holmium-loaded CMS product was washed twice with 30 mL of WFI, the resulting mixture was subjected to SLS to obtain a holmium-loaded CMS solid, and 6 mL of WFI was added to the solid to obtain a suspension, which was equally dispensed into 3 bottles with 2 mL in each bottle. Each bottle had a radioactivity of about 120 mCi and included about 100 mg of the holmium-loaded CMS. The suspension was sterilized at 121° C. for 15 min to obtain a holmium-166/holmium-165-loaded CMS product for injection.

The dissolution rate of the holmium-166 nuclide in the holmium-166/holmium-165-loaded CMS was detected as follows: 10 mg of the above holmium-166/holmium-165-loaded CMS was added to a hydrothermal reactor, 10 mL of WFI or a 0.9% sodium chloride solution was added, and the hydrothermal reactor was sealed and incubated at 120° C. for 2 h in a constant-temperature oven. The resulting system was cooled to room temperature and centrifuged, a specified volume of a resulting supernatant was tested for activity, and the dissolution rate was calculated. The results show that the holmium-166-loaded CMS has a dissolution rate of 0.0188% in the 0.9% sodium chloride solution and a dissolution rate of 0.0245% in the WFI.

Example 16

Preparation of a Medical Samarium-153-Loaded CMS

Samarium-153, a small organic molecule, and water were mixed to allow a reaction to obtain a complex as follows: 1 mL of a 0.5 g/L samarium chloride aqueous solution was added to a reaction flask, a radioactive samarium-153 solution with an activity of 0.82 Ci was added, then a specified volume of a 1.0 g/L 5-SSA solution was added such that a molar amount of the 5-SSA was 4 times a molar amount of the samarium, and water was added to 30 mL. The pH value of the resulting solution was adjusted to 5.6, water with a pH value of 5.6 was added to 50 mL, and the resulting solution was thoroughly shaken to obtain the complex for later use.

A CMS was allowed to adsorb the complex as follows: 0.5 g of the CMS with a particle size of 20 μm to 60 μm was weighed and added to the above complex solution, and the resulting mixture was stirred for 10 min to complete the adsorption.

The CMS adsorbing the complex was subjected to a first treatment as follows: The supernatant was taken and tested for samarium-153 radioactivity, and the adsorption rate for the radionuclide was calculated to be 99.3%. 50 mL of a 0.1 mol/L sodium phosphate solution was added to the solution of the CMS adsorbing the complex, and the resulting mixture was stirred for 5 min.

Cleaning and dispensing of the samarium-153-loaded CMS: The samarium-153-loaded CMS product was washed twice with 50 mL of WFI, the resulting mixture was subjected to SLS to obtain a samarium-153-loaded CMS solid, and 10 mL of WFI was added to the solid to obtain a suspension, which was equally dispensed into 5 bottles with 1 mL in each bottle. Each bottle had a radioactivity of about 150 mCi and included about 100 mg of the samarium-153-loaded CMS; the suspension was sterilized at 121° C. for 15 min to obtain a samarium-153-loaded CMS product for injection.

A dissolution rate of the samarium-153 nuclide in the samarium-153-loaded CMS was detected as follows: 10 mg of the above samarium-153-loaded CMS was added to a hydrothermal reactor, 10 mL of WFI or a 0.9% sodium chloride solution was added, and the hydrothermal reactor was sealed and incubated at 120° C. for 2 h in a constant-temperature oven. The resulting system was cooled to room temperature and centrifuged. A specified volume of the resulting supernatant was tested for activity, and the dissolution rate was calculated. The results show that the samarium-153-loaded CMS has a dissolution rate of 0.0326% in the 0.9% sodium chloride solution and a dissolution rate of 0.0137% in the WFI.

Example 17

Preparation of a CMS Loaded with Light Rare Earth Metals (Lanthanum, Cerium, Praseodymium, Neodymium, Promethium, Samarium, and Europium)

Light rare earth ions, a small organic molecule, and water were mixed to allow a reaction to obtain a complex as follows: 3 mL of a 0.5 g/L aqueous solution of lanthanum chloride, cerium chloride, praseodymium chloride, neodymium chloride, promethium chloride, samarium chloride, and europium chloride was taken and added to a reaction flask, which was thoroughly shaken. Then a specified volume of a 1.0 g/L 5-SSA solution was added such that a molar amount of the 5-SSA was 8 times a molar amount of the rare earth ions. The pH value of the resulting solution was adjusted to 4.8, and the solution was thoroughly shaken to obtain the complex for later use.

A CMS was allowed to adsorb the complex as follows: 3.0 g of the CMS was weighed and added to the above complex solution, and the resulting mixture was stirred for 10 min to complete the adsorption.

The CMS adsorbing the complex was subjected to a first treatment as follows: The supernatant was tested through inductively coupled plasma atomic emission spectroscopy (ICP-AES) to determine the content of the supernatant (lanthanum, cerium, praseodymium, neodymium, promethium, samarium, and europium). An average load rate of the lanthanum, cerium, praseodymium, neodymium, promethium, samarium, and europium was calculated to be 98.3%, and then the first treatment was conducted according to one of the following methods:

Method 1: 200 mg of the above CMS loaded with the light rare earth nuclides was added to 50 mL of a 0.1 mol/L sodium carbonate aqueous solution. The resulting mixture was thoroughly shaken, subjected to a reaction for 10 min, and subjected to SLS, and the resulting solid was dried. The rare earth nuclides in the rare earth-doped CMS obtained by this method mainly existed in the form of a carbonate.

Method 2: 200 mg of the above CMS loaded with the light rare earth nuclides was added to 50 mL of a 0.1 mol/L sodium phosphate solution, and the resulting mixture was stirred for 5 min. The rare earth nuclides in the rare earth-doped CMS obtained by this method mainly existed in the form of a phosphate.

Method 3: 200 mg of the above CMS loaded with the light rare earth nuclides was added to 50 mL of a 0.1 mol/L tannic acid solution, and the resulting mixture was stirred for 5 min.

Method 4: 200 mg of the above CMS loaded with the light rare earth nuclides was treated at 800° C. for 2 h in a high-temperature furnace, cooled, and washed with water until neutral. In the product obtained by this method, the rare earth nuclides were mainly loaded on the CMS in the form of a rare earth oxide (REO).

Method 5: 200 mg of the above CMS loaded with the light rare earth nuclides was treated at 800° C. for 2 h in a high-temperature furnace under a hydrogen atmosphere, cooled, and washed with water until neutral. In the product obtained by this method, the rare earth nuclides were mainly loaded on the CMS in the form of a rare earth metal.

Method 6: 200 mg of the above CMS loaded with the light rare earth nuclides was treated at 900° C. for 3 h in a high-temperature furnace under a hydrogen sulfide and carbon disulfide atmosphere, cooled, and washed with water until neutral. In the product obtained by this method, the rare earth nuclides were mainly loaded on the CMS in the form of a rare earth sulfide.

Since many, if not all, rare earth nuclide ions (whether light rare earth or heavy rare earth) have similar chemical behaviors, the above 6 curing methods are also suitable for the curing of other rare earth nuclides on the CMS.

The dissolution rate of the light rare earth nuclides in the light rare earth-loaded CMS was detected as follows: About 50 mg of each of the CMS products obtained by the methods 1 to 6 was added to a hydrothermal reactor, 10 mL of purified water was added, and the hydrothermal reactor was sealed and incubated at 120° C. for 2 h in a constant-temperature oven. The resulting system was cooled to room temperature and centrifuged, and a specified volume of a resulting supernatant was tested to determine the content of the light rare earth nuclide ions. The results show that the total dissolution rates of the light rare earth nuclides of the products obtained by methods 1 to 6 in water are 0.065%, 0.096%, 0.071%, 0.068%, 0.091%, and 0.077%, respectively.

Example 18

Preparation of a CMS Loaded with Heavy Rare Earths (Gadolinium, Terbium, Dysprosium, Holmium, Erbium, Thulium, Ytterbium, Lutetium, and Yttrium)

Heavy rare earth ions, a small organic molecule, and water were mixed to allow a reaction to obtain a complex as follows: 2 mL of a 0.5 g/L aqueous solution of gadolinium chloride, terbium chloride, dysprosium chloride, holmium chloride, erbium chloride, thulium chloride, ytterbium chloride, lutetium chloride, and yttrium chloride was added to a reaction flask, which was thoroughly shaken. Then a specified volume of a 1.0 g/L 5-SSA solution was added such that a molar amount of the 5-SSA was 10 times a molar amount of the rare earth ions. The pH value of the resulting solution was adjusted to 4.9, water with a pH value of 4.9 was added to 200 mL, and the resulting solution was thoroughly shaken to obtain the complex for later use.

A CMS was allowed to adsorb the complex as follows: 5.0 g of the CMS was weighed and added to the above solution, and the resulting mixture was stirred for 10 min to complete the adsorption.

The CMS adsorbing the complex was subjected to a first treatment as follows: The supernatant was tested through ICP-AES to determine the content of the CMS (gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, and yttrium). The average load rate was calculated to be 98.8%. 150 mL of a 0.1 mol/L sodium phosphate solution was added to the CMS loaded with heavy rare earth nuclides. The resulting mixture was shaken for 5 min, and the CMS was washed twice with purified water and then separated out through SLS.