RADIOACTIVE MICROSPHERE, PREPARATION METHOD THEREOF AND RADIOACTIVE FILLER COMPOSITION

Abstract

Provided is a radioactive microsphere including glass having a structure represented by a formula Ca.sub.3Si.sub.2O.sub.7 and yttrium oxide contained in the glass. The radioactive microsphere has sphericity of from 0.71 to 1, and is radioactive after being activated by neutron irradiation. A method for preparing a radioactive microsphere and a radioactive filler composition is further provided. The present disclosure can be used to treat tumor by delivering radioactive microspheres to the target tissue, and then radioactive microspheres are activated by neutrons to generate radiation. The radioactivity of microspheres disappears over time, and the microspheres were dissolved and absorbed by the bone tissue in the end.

Claims

1. A radioactive microsphere, comprising glass represented by a chemical formula of Ca.sub.3Si.sub.2O.sub.7 and yttrium oxide contained in the glass, and having sphericity from 0.71 to 1, wherein the radioactive microsphere is radioactive after being activated by neutron irradiation.

2. The radioactive microsphere of claim 1, further comprising an imaging nuclide oxide.

3. The radioactive microsphere of claim 2, wherein the imaging nuclide oxide has an imaging nuclide that is at least one selected from the group consisting of phosphorus, calcium, sodium, rhenium, scandium, lanthanum, cerium, praseodymium, neodymium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, actinium-225, antimony-127, arsenic-74, barium-140, bismuth-210, californium-246, calcium-46, calcium-47, carbon-11, carbon-14, cesium-131, cesium-137, chromium-51, cobalt-57, cobalt-58, cobalt-60, dysprosium-165, erbium-169, fluorine-18, gallium-67, gallium-68, gold-198, holmium-166, hydrogen-3, indium-111, indium-113m, iodine-123, iodine-125, iodine-131, iridium-192, iron-59, iron-82, krypton-81m, lanthanum-140, lutetium-177, molybdenum-99, nitrogen-13, oxygen-15, palladium-103, phosphorus-32, radon-222, radium-224, rhenium-186, rhenium-188, rhodium-82, samarium-153, selenium-75, sodium-22, sodium-24, strontium-89, technetium-99m, thallium-201, xenon-127, xenon-133 and yttrium-90.

4. The radioactive microsphere of claim 1, wherein the radioactive microsphere has a particle diameter of 20 m to 100 m.

5. The radioactive microsphere of claim 1, wherein a molar ratio of the glass to the yttrium oxide is from 80:20 to 70:30.

6. The radioactive microsphere of claim 1, further comprising a coating layer formed on a surface of the glass.

7. The radioactive microsphere of claim 6, wherein the coating layer comprises one of an organic material, an inorganic material, or a combination thereof.

8. The radioactive microsphere of claim 7, wherein the organic material comprises a biodegradable material and/or a residue comprising an acid group, a hydroxyl group, an amine group or a carboxyl group, and the inorganic material comprises a phosphate compound, a sulfate compound, a chloride salt compound, a nitrate compound or a borate compound.

9. The radioactive microsphere of claim 7, wherein the coating layer is poly-vinyl-pyrrolidone, poly-vinyl-alcohol, carboxymethyl cellulose, poly-ethylene glycol (PEG6000), methylcellulose, hydroxyl-propyl methyl cellulose, hydroxyl-propyl cellulose, gum arabic, poly-L-lactic acid/poly(lactic-co-glycolic acid) (PLLA/PLGA) or Ca.sub.3(PO.sub.4).sub.2.

10. A radioactive filler composition comprising the radioactive microsphere of claim 1 and an absorbable artificial bone filling material.

11. The radioactive filler composition of claim 10, wherein the absorbable artificial bone filling material is at least one selected from the group consisting of calcium sulfate, calcium phosphate, calcium carbonate and poly-lactic acid.

12. A method of preparing a radioactive microsphere, comprising: melting a mixture comprising glass powder represented by a chemical formula Ca.sub.3Si.sub.2O.sub.7 and yttrium oxide powder to form glass; cooling the glass; grinding the glass to obtain glass fine grains; and flame spraying the glass fine grains to form a radioactive microsphere having sphericity of from 0.71 to 1, wherein the radioactive microsphere is radioactive after being activated by neutron irradiation.

13. The method of claim 12, further comprising adding imaging nuclide oxide powder to the mixture prior to melting the mixture.

14. The method of claim 13, wherein the imaging nuclide oxide has an imaging nuclide that is at least one selected from the group consisting of phosphorus, calcium, sodium, rhenium, scandium, lanthanum, cerium, praseodymium, neodymium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, actinium-225, antimony-127, arsenic-74, barium-140, bismuth-210, californium-246, calcium-46, calcium-47, carbon-11, carbon-14, cesium-131, cesium-137, chromium-51, cobalt-57, cobalt-58, cobalt-60, dysprosium-165, erbium-169, fluorine-18, gallium-67, gallium-68, gold-198, holmium-166, hydrogen-3, indium-111, indium-113m, iodine-123, iodine-125, iodine-131, iridium-192, iron-59, iron-82, krypton-81m, lanthanum-140, lutetium-177, molybdenum-99, nitrogen-13, oxygen-15, palladium-103, phosphorus-32, radon-222, radium-224, rhenium-186, rhenium-188, rhodium-82, samarium-153, selenium-75, sodium-22, sodium-24, strontium-89, technetium-99m, thallium-201, xenon-127, xenon-133 and yttrium-90.

15. The method of claim 12, wherein the radioactive microsphere has a particle diameter of 20 m to 100 m.

16. The method of claim 12, wherein a molar ratio of the glass powder to the yttrium oxide represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 is from 80:20 to 70:30.

17. The method of claim 12, further comprising forming a coating layer on a surface of the radioactive microsphere.

18. The method of claim 17, wherein the coating layer comprises one of an organic material, an inorganic material, or a combination thereof.

19. The method of claim 18, wherein the organic material comprises a bio-degradable material and/or a residue comprising an acid group, a hydroxyl group, an amine group or a carboxyl group, and the inorganic material comprises a phosphate compound, a sulfate compound, a chloride salt compound, a nitrate compound or a borate compound.

20. The method of claim 18, wherein the coating layer is poly-vinyl-pyrrolidone, poly-vinyl-alcohol, carboxymethyl cellulose, poly-ethylene glycol (PEG6000), methylcellulose, hydroxyl-propyl methyl cellulose, hydroxyl-propyl cellulose, gum arabic, poly-L-lactic acid/poly(lactic-co-glycolic acid) (PLLA/PLGA) or Ca.sub.3(PO.sub.4).sub.2.

Description

BRIEF DESCRIPTION OF THE DRAWINGS

[0012] FIG. 1 is a scanning electron microscope (SEM) photograph of radioactive microspheres; and

[0013] FIG. 2 is a scanning electron microscope (SEM) photograph of the radioactive microspheres.

DETAILED DESCRIPTION OF THE EMBODIMENTS

[0014] The following embodiments are intended to illustrate the disclosure of the present disclosure. After reading the disclosure of the specification, those skilled in the art can easily understand the advantages and functions thereof.

[0015] It shall be understood that the structure, the proportions, the dimensions, and the like of the present disclosure are intended to enhance the understanding and perusal by those skilled in the art, and are not intended to limit the present disclosure with the specific conditions. Accordingly, they do not have technical significance. Any changes in the structure, changes in the proportional relationship, or adjustments in the dimensions are intended to be included in the scope of the present disclosure, without affecting the effects and the achievable objectives of the present specification. Without substantially altering the technical contents, changes or adjustments in relative relationships are considered as fallen within the implementable scope of the present disclosure.

[0016] The present disclosure provides radioactive microspheres including glass represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and yttrium oxide contained in the glass, and the sphericity of the radioactive microspheres is from 0.71 to 1.

[0017] Ca.sub.3Si.sub.2O.sub.7 is mainly formed by mixing CaO with SiO.sub.2 and melting at a high temperature, and a molar ratio of CaO to SiO.sub.2 is 4:6, and the temperature is at least 1400 degrees.

[0018] CaSiO.sub.3 (wollastonite) is a typical calcium-based biomaterial capable of forming a calcium phosphate layer and an yttrium-rich layer in SBF (simulated body fluid), produces hydroxyapatite (HA) with osteo-conductive and osteo-inductive biological activity, and has better biological activity and degradability than HA. The types of CaSiO.sub.3 include -wollastonite (Ca.sub.2SiO.sub.4), -wollastonite (Ca.sub.2SiO.sub.4), -wollastonite (pseudo wollastonite; Ca.sub.3Si.sub.3O.sub.9), hatrurite (Ca.sub.3SiO.sub.5), and rankinite (Ca.sub.3Si.sub.2O.sub.7), wherein Ca.sub.3Si.sub.2O.sub.7 exhibits glass phase.

[0019] The sphericity () used in the present disclosure is calculated by Wadell sphericity, and the formula thereof is:

[00001]$\begin{array}{cc}=\frac{A_s}{A_p}=\frac{{{}^{1/3}\left(6.Math..Math.V_p\right)}^{2/3}}{A_p}=\frac{\sqrt[3]{36.Math..Math..Math..Math.V_p^2}}{A_p}& \left(\mathrm{Formula}.Math..Math.I\right)\end{array}$

[0020] Wherein A.sub.s is the equivalent spherical surface area (an equivalent sphere, that is, the sphere whose volume is the same as the object to be tested), A.sub.p is the surface area of the object to be tested, and V.sub.p is the volume of the object to be tested.

[0021] In an embodiment, the glass sphere further includes an imaging nuclide oxide. Before neutron activation, the imaging nuclide oxide is at least selected from the group consisting of phosphorus, calcium, sodium, rhenium, scandium, lanthanum, cerium, praseodymium, neodymium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, actinium-225, antimony-127, arsenic-74, barium-140, bismuth-210, californium-246, calcium-46, calcium-47, carbon-11, carbon-14, cesium-131, cesium-137, chromium-51, cobalt-57, cobalt-58, cobalt-60, dysprosium-165, erbium-169, fluorine-18, gallium-67, gallium-68, gold-198, holmium-166, hydrogen-3, indium-111, indium-113m, iodine-123, iodine-125, iodine-131, iridium-192, iron-59, iron-82, krypton-81m, lanthanum-140, lutetium-177, molybdenum-99, nitrogen-13, oxygen-15, palladium-103, phosphorus-32, radon-222, radium-224, rhenium-186, rhenium-188, rhodium-82, samarium-153, selenium-75, sodium-22, sodium-24, strontium-89, technetium-99m, thallium-201, xenon-127, xenon-133 and yttrium-90. The imaging nuclide oxide is then activated by neutron activation and decays into an element represented in the brackets: phosphorus (.sup.32P->.sup.32S), calcium (.sup.47Ca->.sup.47Sc; .sup.49Ca->.sup.49Sc), sodium (.sup.22Na->.sup.22Ne), rhenium (.sup.188Re->.sup.188Os), scandium (.sup.44Sc->.sup.44Ca; .sup.48Sc->.sup.48Ti; .sup.46Sc->.sup.46Ti; .sup.47Sc->.sup.47Y), lanthanum (.sup.140La->.sup.140Ce; .sup.142La->.sup.142Ce), cerium, praseodymium, neodymium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, actinium-225(.sup.225Ac->.sup.221Fr, .sup.211Bi,.sup.14C), antimony-127(.sup.127Sb->.sup.127Te), arsenic-74(.sup.74As->.sup.74Ge), barium-140(.sup.140Ba->.sup.140La), bismuth-210(.sup.210Bi->.sup.210Po), californium-246(.sup.246Cf->.sup.246Cm), calcium-46(.sup.46Ca->.sup.46Sc), calcium-47(.sup.47Ca->.sup.47Sc), carbon-11(.sup.11C->.sup.11B), carbon-14(.sup.14C->.sup.14N), cesium-131(.sup.131Cs->.sup.131Xe;.sup.131Cs->.sup.131Ba), cesium-137(.sup.137Cs->.sup.137Ba), chromium-51(.sup.51Cr->.sup.51V), cobalt-57(.sup.57Co->.sup.57Fe), cobalt-58(.sup.58Co->.sup.58Fe), cobalt-60(.sup.60Co->.sup.60Ni), dysprosium-165(.sup.165Dy->.sup.165Ho), erbium-169(.sup.169Er->.sup.169Tm), fluorine-18(.sup.18F->.sup.18O), gallium-67(.sup.67Ga->.sup.67Zn), gallium-68(.sup.68Ga->.sup.68Zn), gold-198(.sup.198Au->.sup.198Hg), holmium-166(.sup.166Ho->.sup.166Er), hydrogen-3(.sup.3H->.sup.3He), indium-111(.sup.111In->.sup.111Cd), indium-113m (.sup.113mIn->.sup.113Sn), iodine-123(.sub.123I->.sup.123Te), iodine-125(.sub.125I->.sub.125Te), iodine-131(.sup.131I->.sup.131Xe), iridium-192 (.sup.192Ir->.sup.192Os,.sup.192Pt), iron-59(.sup.59Fe->.sup.59Co), krypton-81m (.sup.81mKr->.sup.81Br), lanthanum-140(.sup.140La->.sup.140Ce), lutetium-177(.sup.177Lu->.sup.177Hf), molybdenum-99(.sup.99Mo->.sup.99Tc,.sup.99Ru), nitrogen-13(.sup.13N->.sup.13C), oxygen-15(.sup.15O->.sup.15N), palladium-103(.sup.103Pd->.sup.103Rh), Phosphorus-32(.sup.32P->.sup.32S), radon-222(.sup.222Rn->.sup.218Po), radium-224(.sup.224Ra->.sup.220Rn,.sup.210Pb,.sup.14C), rhenium-186(.sup.186Re->.sup.186Os,.sup.186W), rhenium-188(.sup.188Re->.sup.188Os), samarium-153(.sup.153Sm->.sup.153Eu), selenium-75 (.sup.75Se->.sup.75As), sodium-22(.sup.22Na->.sup.22Ne), sodium-24(.sup.24Na->.sup.24Mg), strontium-89(.sup.89Sr->.sup.89Y), technetium-99m (.sup.99Tc->.sup.99Ru), thallium-201(.sup.201Tl->.sup.201Hg), xenon-127(.sup.127Xe->.sup.127Cs), xenon-133(.sup.133Xe->.sup.133Cs) and yttrium-90(.sup.90Y->.sup.90Zr).

[0022] In an embodiment, the imaging nuclide oxide is in an amount of from 0 to 10% by weight, more preferably, from 3 to 8% by weight, in the radioactive microspheres.

[0023] The imaging nuclide oxide used in the present disclosure emits y-rays after being activated by neutron irradiation, and can be detected and distributed in vivo through special photographic equipment such as y camera or positron tomography. The integration of these photographic devices with computers can display images and can be calculated and analyzed for more information. Since most diseases have physiological, biochemical and metabolic changes in the early stages of the disease, and then structural changes, X-ray inspection and computerized tomography are those commonly used to detect the body structure changes. In addition, the nuclear angiography can detect abnormalities before the onset of the disease and the presence of symptoms in other examination methods, because it can show the physiological changes of the organ tissues. This ability to diagnose early often allows the disease to be treated before the disease progresses rapidly.

[0024] In an embodiment, the particle size of the radioactive microspheres is preferably from 20 to 100 m.

[0025] In an embodiment, the molar ratio of glass to yttrium oxide in the radioactive microspheres is preferably from 80:20 to 70:30, within which Ca.sub.3Si.sub.2O.sub.7 maintains a good glass phase and has a sufficient radiation dose.

[0026] In an embodiment, the radioactive microspheres further include a coating layer formed on a surface of the glass, the coating layer comprising one of an organic material and an inorganic material, or a combination thereof.

[0027] In an embodiment, the organic material includes an acid group, a hydroxyl group, an amine group, or a carboxyl group.

[0028] In an embodiment, the organic material includes a biodegradable material.

[0029] In an embodiment, the inorganic material includes a phosphate compound, a sulfate compound, a chloride salt compound, a nitrate compound, or a borate compound.

[0030] In an embodiment, the coating layer is poly-vinyl-pyrrolidone, poly-vinyl-alcohol, carboxymethyl cellulose, polyethylene glycol (PEG6000), methylcellulose, hydroxyl-propyl methyl cellulose, hydroxyl-propyl cellulose, gum arabic, poly-L-lactic acid/poly(lactic-co-glycolic acid) (PLLA/PLGA) or Ca.sub.3(PO.sub.4).sub.2.

[0031] When the radioactive microsphere of the present disclosure remains radioactive in time and remains in the body, it does not affect the degradation of the absorbable artificial bone filling material. Also, the radioactive microsphere can become a stable structure with the absorbable artificial bone filling material before the new bone is formed, and provides an environment for bone growth. It is suitable for use as an additive to artificial bone filling materials.

[0032] The present disclosure also provides a radioactive filling composition, comprising the radioactive microsphere and an absorbable artificial bone filling material, wherein the absorbable artificial bone filling material is at least one selected from the group consisting of calcium sulfate, calcium phosphate, calcium carbonate and poly-lactic acid.

[0033] The calcium sulfate salt is one or more selected from the group consisting of calcium sulfate anhydrate, calcium sulfate hemihydrate, calcium sulfate di-hydrate, or a mixture, composition or adduct of anhydrous calcium sulfate/calcium sulfate hemihydrate, anhydrous calcium sulfate/calcium sulfate di-hydrate, calcium sulfate hemihydrate/calcium sulfate di-hydrate, or anhydrous calcium sulfate/calcium sulfate hemihydrate/calcium sulfate di-hydrate.

[0034] The calcium phosphate salt is one or more selected from the group consisting of calcium phosphate, di-calcium phosphate (DCP), tri-calcium phosphate (TCP), calcium hydrogen phosphate, tetra-calcium phosphate (TTCP), hydroxyapatite (HA), strontium hydroxyapatite, magnesium hydroxyapatite, and silver hydroxyapatite, or a mixture, composition or adduct of DCP/TCP, DCP/TTCP, DCP/HA, TCP/TTCP, TCP/HA, TTCP/HA, DCP/TCP/TTCP, DCP/TCP/HA, DCP/TTCP/HA, TCP/TTCP/HA, and DCP/TCP/TTCP/HA.

[0035] The radioactive microsphere and the absorbable artificial bone filling material are mixed with an additive and a liquid, and can be implanted and solidified after being implanted into the bone defect site after the tumor resection, providing a scaffold for stress and cell growth and locally killing the residual cancer. Distribution may be observed using imaging nuclide.

[0036] The additive is one or more selected from polyethylene glycol, sodium alginate, polyvinyl alcohol, cellulose, chitosan, hyaluronic acid, sodium stearate, magnesium stearate, gelatin, preferably one or more of polyethylene glycol, sodium alginate, hyaluronic acid, chitosan, and cellulose.

[0037] The liquid is, for example, pure water, physiological saline, phosphate solution, graphene oxide solution, chitosan solution, sodium alginate solution, sodium citrate solution, sodium hyaluronate solution, polyvinyl alcohol solution, polyethylene glycol solution, cellulose solution, silver nitrate solution, cellulose solution, artificial body fluid or human blood. Preferably, it is 0.05 to 3% by weight of a sodium hyaluronate solution, 0.05 to 3% by weight of a chitosan solution, 0.05 to 3% by weight of a sodium alginate solution, water or blood.

[0038] The present disclosure also provides a method for preparing a radioactive microsphere, including steps of melting a mixture comprising glass powder represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and yttrium oxide powder to form glass; cooling the glass; grinding the glass to obtain glass fine grains; and flame-spraying the glass fine grains to form a radioactive microsphere, wherein the radioactive microsphere has sphericity of from 0.71 to 1.

[0039] In an embodiment, the glass fine grains are flame-sprayed to form a radioactive microsphere, and then collected in a cooling collection zone.

[0040] The cooling collection zone may be a solid or liquid interface, the solid may be ice or dry ice, and the liquid may be a liquid that can excite for a nuclide component (an organic/inorganic acid) or water.

[0041] In an embodiment, the method of preparing the radioactive microspheres further comprises adding an imaging nuclide oxide powder to the mixture prior to melting the mixture.

[0042] In an embodiment, the method for preparing the radioactive microspheres further comprises forming a coating layer on the surface of the radioactive microspheres.

[0043] Specifically, the mixed powder is pre-ball milled and uniformly mixed, and then melted to form glass; after grinding the glass, the glass fine grains are obtained. Said glass fine grains are heated and sprayed by high-speed gas flame. Specifically, the glass fine grains are heated by the high-temperature combustion flame, with the high-speed combustion gas spraying away from the flame core, to cause the surface melting, and under the influence of surface tension interaction, high-temperature molten droplets are formed. During the rotating flight, the high-temperature molten droplets gradually form a spherical shape due to the influence of air temperature gradient, gravity and droplet rotation, and eventually contact the cooling collection zone when the distance from the flame center is increased. The temperature gradient of the cooling collection zone is sharply reduced to form a radioactive microsphere. On the other hand, under different processing conditions of different flight distances and different nature flames, the resulting shape would form a solid sphere, a hollow sphere or a mesoporous sphere as the distance of the radioactive microspheres from the flame center is different. Moreover, the composition of the flame depends on the mixing ratio of the combustion gas and the oxygen. In particular, when the mixing ratio of oxygen and acetylene in the oxidizing flame (Nm.sup.3/hr) is greater than 1.2, it is an oxygen-excess flame, which is with oxidizing property. When the mixing ratio of oxygen and acetylene in the neutral flame is 1.1 to 1.2, oxygen and acetylene are fully burned, and there is no problem of excess oxygen and acetylene; and the inner flame has a certain reducing property, so that the CO.sub.2 and CO generated during combustion have a protective effect. When in the carbonized flame the mixing ratio of oxygen to acetylene is less than 1.1, the acetylene is excessive and has strong reducing property; and the flame has free carbon and excessive hydrogen.

[0044] The present disclosure illustrates the details by way of examples of the embodiments. However, the interpretation of the present disclosure should not be limited to the description of the following examples.

Example (1)

[0045] The glass powder represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and the yttrium oxide powder were uniformly ball-milled at a molar ratio of 80:20, and melted to form glass; after powder grinding, flame spraying was performed by a high-speed gas mixed with acetylene and oxygen (gas ratio of 1.1 to 1.2) for heating and spraying. The radioactive microspheres were formed at a flame temperature range of from 1200 C. to 2000 C., with a spray distance of 50 cm, and a flight time of 15 seconds. The radioactive microspheres were as shown in FIG. 1. The radioactive microspheres were subject to Wadell sphericity analysis (as shown in FIG. 2 and Table 1), and the spherical microspheres had sphericity between 0.7276 and 1.

[0046] The radioactive microspheres were taken by 10 mg for neutron activation irradiation; and after neutron activation element analysis, Ca signal was observed, as shown in Table 2.

Example (2)

[0047] The glass powder represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and the yttrium oxide powder were uniformly ball-milled at a molar ratio of 80:20, and then imaging nuclide oxide powders such as 5% by weight of ReO, 5% by weight of CuO, and 5% by weight of TeO were separately added. After being melted to form glass, powder grinding was performed, and then flame spraying was performed by a high-speed gas (gas ratio of 1.1 to 1.2) mixed with acetylene and oxygen. The flame was sprayed at a flame temperature range of from 1200 C. to 2000 C., with a spraying distance of 50 cm and a flight time of 15 seconds, to form radioactive microspheres. The radioactive microspheres comprising ReO, CuO or TeO were taken by 10 mg and irradiated for neutron activation. After neutron activation element analysis, the signals of Re, Cu and Te (I-131) were observed, as shown in Table 3.

Example (3)

[0048] The glass powder represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and the yttrium oxide powder were uniformly ball-milled at a molar ratio of 80:20, and then imaging nuclide oxide powders such as 5% by weight of ReO, 5% by weight of CuO, and 5% by weight of TeO were separately added. After being melted to form glass, powder grinding was performed, and then flame spraying was performed by a high-speed gas (gas ratio of 1.1 to 1.2) mixed with acetylene and oxygen. The flame was sprayed at a flame temperature range of from 1200 C. to 2000 C., with a spraying distance of 50 cm and flight time of 15 seconds, to form radioactive microspheres. The radioactive microspheres were mixed with 10 g of calcium sulfate hemihydrate and 0.5 g of magnesium stearate at room temperature, and then were stirred with 3 g of pure water as a mixed liquid. The results were all moldable and curable.

Example (4)

[0049] The glass powder represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and the yttrium oxide powder were uniformly ball-milled at a molar ratio of 80:20, and then imaging nuclide oxide powders such as 5% by weight of ReO, 5% by weight of CuO, and 5% by weight of TeO were separately added. After being melted to form glass, powder grinding was performed, and then flame spraying was performed by a high-speed gas (gas ratio of 1.1 to 1.2) mixed with acetylene and oxygen, and the flame was sprayed at a flame temperature range of from 1200 C. to 2000 C., with a spraying distance of 50 cm and a flight time of 15 seconds, to form radioactive microspheres. The radioactive microspheres were mixed with 10 g of mono-calcium phosphate glass and 0.5 g of magnesium stearate additive at room temperature, and then were stirred with 3 g of PBS artificial body fluid as a mixed liquid. The results were all moldable and curable.

Example (5)

[0050] The glass powder represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and the yttrium oxide powder were uniformly ball-milled at a molar ratio of 80:20, and then imaging nuclide oxide powders such as 5% by weight of ReO, 5% by weight of CuO, and 5% by weight of TeO were separately added. After being melted to form glass, powder grinding was performed, and then flame spraying was performed by a high-speed gas (gas ratio of 1.1 to 1.2) mixed with acetylene and oxygen, and the flame was sprayed at a flame temperature range of from 1200 C. to 2000 C., with a spraying distance of 50 cm and a flight time of 15 seconds, to form radioactive microspheres. The radioactive microspheres were respectively mixed with 10 g of a mixture mono-calcium phosphate glass and calcium sulfate hemihydrate at room temperature, where the two powders were blended at a ratio of 1:4, 1:1 and 4:1, and then the mixture was stirred with 3 g of PBS artificial body fluid. The results were all moldable and curable.

Example (6)

[0051] The glass powder represented by the chemical formula Ca.sub.3Si.sub.2O.sub.7 and the yttrium oxide powder were uniformly ball-milled at a molar ratio of 80:20, and then imaging nuclide oxide powders such as 5% by weight of ReO, 5% by weight of CuO, and 5% by weight of TeO were separately added. After being melted to form glass, powder grinding was performed, and then flame spraying was performed by a high-speed gas (gas ratio of 1.1 to 1.2) mixed with acetylene and oxygen, and the flame was sprayed at a flame temperature range of from 1200 C. to 2000 C., with a spraying distance of 50 cm and a flight time of 15 seconds, to form radioactive microspheres. The radioactive microspheres were coated with an organic or inorganic material layer (as shown in Table 4) on the outer surface of the glass microspheres by a spray granulation method at room temperature. The results show that the radioactive microspheres can be over molded.

TABLE-US-00001 TABLE 1 Sphericity analysis A.sub.s being Elliptical Elliptical equivalent A.sub.p being long short spherical surface area axis axis surface of the object Sphericity (m) (m) area to be tested () (1) 50 50 7853.98 7853.30 1.000 (2) 35 31.25 3067.9615 3256.964 0.942 (3) 47.5 40 5026.548 5517.946 0.911 (4) 48.75 41.25 5345.616 5851.2905 0.9135 (5) 62.5 37.5 4417.86467 6071.2508 0.7276 (6) 51.25 50 7853.98 7952.0769 0.9876 (7) 41.25 40 5026.548 5162.959 0.9735

TABLE-US-00002 TABLE 2 Neutron irradiation activation element analysis -ray energy spectrum main Test peak Specific product Radio- energy AUC activity Compound weight isotope (keV) (cnts) Bq (uCi/mg) 1 Y, Ca 10 mg Y-90m 202 keV 393 74.1 0.00022

TABLE-US-00003 TABLE 3 Neutron irradiation activation element analysis -ray energy spectrum main Specific Test peak activity product Radio- energy AUC (uCi/ Compound weight isotope (keV) (cnts) Bq mg) 1 Y, Cu 10 mg Y-90m 202 keV 410 66.9 0.00018 2 Y, Cu 10 mg Y-90m 202 keV 393 64.1 0.00017 3 Y, Te 10 mg I-131 364.5 keV 20 3.9 0.00001 4 Y, Te 10 mg Y-90m 202 keV 288 47.0 0.00013 5 Y, Re 10 mg Re-188 155.1 keV 1524 1612.7 0.00435

TABLE-US-00004 TABLE 4 Microsphere coated with organic and inorganic materials Outlet Over- Test coatingmaterial wt % Flow rate temperature molding Poly-vinyl-pyrrolidone 0.1-10 357 L/h 180-245 C. Yes (PVP) Poly-vinyl alcohol (PVA) 0.1-10 357 L/h 180-245 C. Yes Carboxymethylcellulose 0.1-10 357 L/h 180-245 C. Yes (CMC) Poly-ethyleneglycol 0.1-10 357 L/h 180-245 C. Yes (PEG 6000) Methylcellulose(MC) 0.1-10 357 L/h 180-245 C. Yes Hydroxy-propyl methyl 0.1-10 357 L/h 180-245 C. Yes cellulose(HPMC) Hydroxy-propyl cellulose 0.1-10 357 L/h 180-245 C. Yes (HPC) Gum arabic 0.1-10 357 L/h 180-245 C. Yes Poly L-lactic acid/poly- 0.1-10 357 L/h 180-245 C. Yes lactic acid-glycolic acid copolymer (PLLA/ PLGA) Ca.sub.3(PO.sub.4).sub.2 0.1-10 357 L/h 180-245 C. Yes