Metal molybdates and methods of making the same

Abstract

A method for producing a titanium molybdate material.SOLUTION: The method of the present invention comprises reacting a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition, combining the Mo composition with a metal source to obtain a metal-Mo composition, pH adjusting the metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates, controlling the temperature of the aqueous medium by heating the aqueous medium, removing heat from the aqueous medium, or both, and agitating the metallic Mo-99 material and the aqueous medium during at least a portion of the reaction. The metal source comprises a metal, metallate, or metal salt, wherein the metal, metallate, or metal salt forms a bond with another metal, metallate, metal salt, or molybdate, wherein the bond comprises a cyano, nitro, sulfide, amide nitride, acetate, carbonate, phosphate, carbonyl, or a combination thereof.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] This application claims priority to U.S. Nonprovisional Patent Application No. 15 / 902,140, ​​filed in the U.S. Patent and Trademark Office on February 22, 2018, and to U.S. Provisional Patent Application No. 62 / 463,020, filed in the U.S. Patent and Trademark Office on February 24, 2017, and to U.S. Provisional Patent Application No. 62 / 592,737, filed in the U.S. Patent and Trademark Office on November 30, 2017, the disclosures of which are incorporated herein by reference in their entireties.

[0002] The invention disclosed herein generally relates to metal molybdate materials suitable for use in technetium-99m generators (Mo-99 / Tc-99m generators) and methods for making same. [Background technology]

[0003] Technetium-99m (Tc-99m) is the most commonly used radioisotope in nuclear medicine (e.g., medical imaging). Tc-99m (m is metastable) is typically injected into patients, and when used in certain facilities, it is used to image the patient's internal organs. However, Tc-99m has a half-life of only six hours. Therefore, readily available sources of Tc-99m are of particular interest and / or need, at least in the field of nuclear medicine.

[0004] Given the short half-life of Tc-99m, Tc-99m is typically obtained where and / or when needed (e.g., at pharmacies, hospitals, etc.) through Mo-99 / Tc-99m generators. Mo-99 / Tc-99m generators are devices used to extract a metastable isotope of technetium (i.e., Tc-99m) from a decaying source of molybdenum-99 (Mo-99) by passing saline solution through the Mo-99 material. Mo-99 is unstable and decays to Tc-99m with a half-life of 66 hours. Mo-99 is typically produced in a high-neutron flux reactor from the irradiation of a highly enriched uranium target (93% uranium-235) and transported to the manufacturing site of the Mo-99 / Tc-99m generator. The Mo-99 / Tc-99m generators are then distributed from these central locations to hospitals and pharmacies nationwide. Because there are a limited number of production sites and it is compounded in a limited number of available high-flux reactors, the supply of Mo-99 is subject to frequent interruptions and shortages, causing delays in nuclear medicine procedures. Summary of the Invention [Problem to be solved by the invention]

[0005] Therefore, there remains a need for at least a method for producing materials suitable for use in technetium-99m generators (Mo-99 / Tc-99m generators). [Means for solving the problem]

[0006] One or more embodiments of the present invention may address one or more of the aforementioned problems. Certain embodiments of the present invention provide methods for producing metal molybdates (also referred to herein as metal-Mo) suitable for use in technetium-99m generators, e.g., metal-Mo materials. As used herein, the term "metal molybdate" generally refers to metal molybdates, metal-molybdenum, molybdenum-metallates, or any form of Mo-metal or metal-Mo species. Methods according to certain embodiments of the present invention may include reacting a metal molybdenum (Mo) material in a liquid medium (e.g., an aqueous medium) with a first acid (e.g., a mineral acid) to obtain a Mo composition, and combining the Mo composition with a metal source to obtain the metal-Mo composition. Methods according to certain embodiments of the present invention may further include pH-adjusting the metal-Mo composition with a base (e.g., ammonium hydroxide) to precipitate a plurality of metal-Mo particulates (interchangeably referred to herein as particles). According to certain embodiments of the present invention, the metal-Mo particulates may be isolated or separated from the liquid medium. According to certain embodiments of the present invention, the isolated metal-Mo particles may be in the form of a slurry containing the remaining liquid medium. The isolated metal-Mo particles may be subjected to thermal energy to at least partially dry the metal-Mo particles. The metal-Mo particles may be crushed and washed. According to certain embodiments of the present invention, the method may include irradiating a metallic molybdenum target to obtain the Mo material discussed herein. That is, irradiating a metallic molybdenum target to obtain the Mo material may be performed before combining the metallic Mo material with the first acid in the liquid medium. The metallic molybdenum target may include, for example, a tubular capsule containing metallic molybdenum and a plurality of metallic molybdenum internal components (e.g., balls, rods, wires, disks) housed in the tubular capsule. Alternatively, for example, the metallic molybdenum target may be one or more metallic molybdenum components (e.g., balls, rods, wires, disks), used alone or in combination, for example, a rod and a series of disks. In this regard, certain embodiments of the present invention include metal-Mo materials produced according to the methods disclosed herein.

[0007] In some embodiments of the present invention, intermediate products may be present for further processing, if desired.

[0008] In yet another aspect, the present invention provides a metal-Mo material comprising a plurality of metal-Mo particulates.

[0009] According to certain embodiments of the present invention, the method may include irradiating the resulting metal-Mo material comprising a plurality of metal-Mo particles. For example, irradiation may be performed prior to loading the metal-Mo particles into the elution vessel.

[0010] According to certain embodiments of the present invention, the metal-Mo material has an elution efficiency of 30% or greater, 80% or greater, 90% or greater, or 95% or greater. According to certain embodiments of the present invention, the metal-Mo material can be placed in an elution column (e.g., a technetium-99m generator) and at least 90% (e.g., at least 95% or at least 99%) of the total technetium content is released from the metal-Mo material by passing an aqueous liquid (e.g., water, saline, dilute acid) through the metal-Mo material.

[0011] Other embodiments of the invention are described herein.

[0012] The present invention now will be described more fully hereinafter with reference to the accompanying drawings, in which some, but not all, embodiments of the invention are shown. Indeed, this invention may be embodied in many different forms and should not be construed as limited to the embodiments set forth herein; rather, these embodiments are presented so that this disclosure will satisfy applicable legal requirements. Like numbers refer to like elements throughout. [Brief explanation of the drawings]

[0013] [Figure 1] FIG. 1 is a block diagram of a method for producing a metal molybdate material according to an embodiment of the present invention. [Figure 2]FIG. 1 is a block diagram of a method for producing a metal molybdate material, after optional irradiation, according to an embodiment of the present invention. [Figure 3] FIG. 1 is a block diagram of a method for producing a metal molybdate material according to an embodiment of the present invention. [Figure 4] FIG. 1 is a block diagram of a method for producing a metal molybdate material, after optional irradiation, according to an embodiment of the present invention. [Figure 5] FIG. 1 illustrates a cask transfer case according to one embodiment of the present invention. [Figure 6] FIG. 6 illustrates a cross-sectional view of the cask transfer case illustrated in FIG. 5. DETAILED DESCRIPTION OF THE INVENTION

[0014] The present invention will now be described more fully hereinafter with reference to the accompanying drawings, in which some, but not all, embodiments of the invention are shown. Indeed, the invention may be embodied in many different forms and should not be construed as limited to the embodiments set forth herein; rather, these embodiments are presented so that this disclosure will satisfy applicable legal requirements. As used in this specification and the appended claims, the singular forms "a," "an," and "the" include plural referents unless the context clearly dictates otherwise.

[0015] The present invention, according to certain embodiments, provides a method for producing metal molybdates (also referred to herein as metal-Mo), such as porous Ti—Mo materials suitable for use in technetium-99m generators. As used herein, the term “metal molybdate” generally refers to metal molybdates, metal-molybdenum, molybdenum-metallates, or any form of Mo-metal or metal-Mo species.

[0016] According to certain embodiments, the method may include reacting a metallic molybdenum (Mo) material (e.g., solid molybdenum metal in various forms, including powders and bulk solids of various particle sizes and shapes) with an acid(s) (e.g., a mineral acid) in a liquid medium to obtain a Mo composition (e.g., a Mo solution), and combining the Mo composition with a metal source to obtain a metal-Mo composition. Metallic molybdenum is typically produced by powder metallurgy techniques, for example, in which Mo powder is hydrostatically compacted and sintered. According to certain embodiments of the present invention, the metallic molybdenum material may comprise, consist essentially of, or consist of Mo atoms. Non-limiting examples of metallic molybdenum materials include, but are not limited to, natural Mo, enriched Mo (including, but not limited to, Mo-98 enriched Mo), and Mo alloys (including, but not limited to, any material with a Mo content greater than 50% where the other alloying component(s) are easily separated chemically from the Mo).

[0017] Methods according to certain embodiments of the present invention may further include adjusting the pH of the metal-Mo composition with a base (e.g., ammonium hydroxide) to precipitate a plurality of metal-Mo particulates. According to certain embodiments of the present invention, methods for producing solid metal-Mo may include a single-pot method in which the metal-Mo material is converted to solid metal-Mo particulates in a single pot (i.e., in the same tank or pot).

[0018] According to certain embodiments, the acid(s) utilized may include one or more mineral acids or hydrogen peroxide. In this regard, mineral acids suitable for combination with metallic Mo may include hydrochloric acid, nitric acid, sulfuric acid, phosphoric acid, hydrofluoric acid, boric acid, hydrobromic acid, perchloric acid, hydroiodic acid, halogen acids (e.g., HAt, where At is astatine), or any combination thereof. According to certain embodiments, the mineral acid may include hydrochloric acid, nitric acid, or a combination thereof. In this regard, metallic Mo may be immersed and stirred in a liquid medium while one or more of the aforementioned acids are added to lower the pH of the liquid medium. According to certain embodiments, reacting the metallic molybdenum (Mo) material in the liquid medium with the first acid may subject the metallic Mo material, and / or any metal oxides formed thereby, to a process including, but not limited to, oxidation, dissolution, other reaction processes, or combinations thereof.

[0019] According to certain embodiments of the present invention, the liquid medium may comprise an aqueous medium. In this regard, the liquid medium may comprise water. According to certain embodiments of the present invention, the liquid medium consists of water to which metallic Mo and one or more of the aforementioned acids are added.

[0020] According to certain embodiments of the present invention, the step of reacting the metallic molybdenum (Mo) material with a first acid in a liquid medium may be carried out at a molar ratio of Mo to acid (Mo:acid) ranging from about 0.1:1 to about 10:1.

[0021] The step of reacting metallic Mo may further include controlling the temperature of a liquid medium (e.g., an aqueous medium) in which the metallic Mo is immersed at any time during the reaction. In this regard, controlling the temperature of the liquid medium (e.g., an aqueous medium) may include heating the liquid medium, removing heat from the liquid medium, not heating the liquid medium, or a combination thereof. Heating and / or heat removal may be achieved by a variety of known heat transfer methods (e.g., internal tank coils, heat exchangers, jacketed tanks, etc.). According to certain embodiments of the present invention, for example, the temperature of the liquid medium can be desirably controlled by heating and / or removing heat from the liquid medium throughout the reaction. According to certain embodiments of the present invention, for example, heat may be added to the liquid medium in which the metallic Mo is immersed sufficient to raise the temperature of the liquid medium to about 25°C or more, about 35°C or more, about 45°C or more, about 55°C or more, etc. The temperature of the liquid medium may begin to rise. In this regard, controlling the temperature of the liquid medium by removing released heat may be desirable, for example, at least regarding safety concerns. If the liquid medium includes any co-chemicals, the boiling points of such chemicals may at least partially determine the desired maximum temperature reached by the liquid medium. According to certain embodiments of the present invention, the temperature of the liquid medium may be controlled by maintaining the temperature of the liquid medium at or below about 80°C, for example, by removing heat from the liquid medium. According to certain embodiments of the present invention, the temperature of the liquid medium may be controlled by maintaining the temperature of the liquid medium at or below about 100°C, at or below about 80°C, at or below about 70°C, at or below about 60°C, at or below about 50°C, or at or below about 40°C.

[0022] The reacting step may further include agitating the metallic Mo material and the liquid medium during at least a portion of the step. In this regard, agitating the metallic Mo material and the liquid medium may improve the interaction between the metallic Mo material and the liquid medium, such as by lowering the pH of the liquid medium with the addition of an acid (i.e., one or more mineral acids). For example, agitation may improve the contact of the metallic Mo material with the acid in the liquid medium, thereby increasing the rate of any reaction process that occurs, including, but not limited to, oxidation, dissolution, or a combination thereof. According to certain embodiments of the present invention, for example, agitation may include mechanically mixing the metallic Mo material and the liquid medium. According to certain embodiments of the present invention, agitation may be improved by utilizing baffles in the internal tank to promote vertical mixing of the metallic Mo and the liquid medium.

[0023] According to certain embodiments of the present invention, the step of combining the metallic Mo material may include simultaneously adding one or more acids to a liquid medium in which the metallic Mo material is immersed, controlling the temperature of the liquid medium, and agitating the metallic Mo material and the liquid medium during at least a portion of the step. The resulting Mo composition (e.g., a solution of Mo) may then be subjected to further processing.

[0024] According to certain embodiments of the present invention, there is provided a method for producing metal molybdate (Ti—Mo), the method comprising the steps of: fully or partially oxidizing a metallic molybdenum (Mo) material with a first acid in a liquid medium to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and pH adjusting the metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates.

[0025] According to certain embodiments of the present invention, a method for producing metal molybdate (Ti—Mo) is provided, the method including the steps of: dissolving a metallic molybdenum (Mo) material in whole or in part with a first acid in a liquid medium to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates.

[0026] In the foregoing examples, the process parameters and / or conditions for oxidizing and / or dissolving may be the same as those discussed herein with respect to the reacting step.

[0027] According to certain embodiments of the present invention, after forming the Mo composition, the method may include combining the Mo composition with a metal source to obtain a metal-Mo composition.

[0028] According to embodiments of the present invention, the metal source may include elements from the p-block, d-block, or f-block of the periodic table. The p-block of the periodic table includes elements from the six groups excluding helium, starting with Group 3A and ending with Group 8A. p-block metals generally have high melting points and readily react with nonmetals to form ionic compounds. Metalloids, which possess both metallic and nonmetallic properties, also exist in the p-block. The d-block of the periodic table includes elements from Groups 3, 4, 5, 6, 7, 8, 9, 10, 11, and 12 of the periodic table. These elements are known as transition metals. Transition metals (also called transition elements) may also be defined by the IUPAC definition, which states that transition metals are "elements whose atoms have an incomplete d subshell or can give rise to cations with an incomplete d subshell." The f-block of the periodic table includes the lanthanide and actinide series. An f-block element has one or more outermost electrons in an f-orbital, but not in a d- or p-orbital. An f-orbital can contain up to seven pairs of electrons.

[0029] Non-limiting examples of metal sources are one or more metals, metalates, or metal salts, including, but not limited to, elemental or non-oxidized metals, metal oxides, metal hydroxides, metal halides, nitrates, phosphates, tetrafluoroborides, phosphorus hexafluoride, tosylates, acetates, formates, or any other counter anion capable of forming a soluble salt. The metals, metalates, or metal salts can be M in various oxidation states. n+, n=1, 2, 3, 4, 5, 6, which may allow for the formation of oxo or hydroxo bridges with another metal, metalate, metal salt, or molybdate. An oxo bridge typically refers to an oxygen ion covalently bonded to a metal, as in MOM.

[0030] According to an embodiment of the present invention, the metal source is a metal, metalate, or metal salt that: (1) forms individual units or composite units of tetrahedral, octahedral, or more complex structures; (2) Mo x O y (3) remains unchanged under ionizing radiation and Mo x O y The bonds formed with the seeds remain, and / or (4) if the material is synthesized before Mo irradiation, it does not produce any daughter products from neutron bombardment, which may be undesirable in the final eluate.

[0031] In the case of titanium, the titanium source may include titanium chloride (e.g., TiCl). According to certain embodiments of the present invention, the titanium chloride may include titanium(III) chloride (TiCl), titanium(II) chloride (TiCl), titanium tetrachloride (TiCl), or any combination thereof.

[0032] In addition to the titanium salts mentioned above, + , 3 + or 4 + Titanium salts present in the oxidized state have counterions, e.g., nitrate NO3 - , or other halides F - , Br - , At - Or I - The additional titanium source may include, but is not limited to, unoxidized titanium metal or metal carbonyls, or may be combined with metal oxides, metal hydroxides, phosphates, tetrafluoroborides, phosphorus hexafluoride, tosylates, acetates, formates, or any other counteranions capable of forming soluble salts in various oxidation states.

[0033] In addition to titanium, other metals capable of forming elutable structures with Mo may also be added in various ratios. These metals may be in the form of the non-oxidized metal or in the form of the aforementioned salts that are incorporated into titanium. Furthermore, these titanium metal substitutes may be present in various oxidation states of M. n+ , n=1, 2, 3, 4, 5, 6. Substitutions for titanium come from the selection of p-block, d-block (transition metals), and / or f-block metals. Some of these metals are aluminum (Al) (p-block), silicon (Si) (p-block), tin (Sn) (p-block), germanium (Ge) (p-block), zirconium (Zr) (d-block), hafnium (Hf) (d-block), vanadium (V) (d-block), chromium (Cr) (d-block), manganese (Mn) (d-block), cobalt (Co) (d-block), nickel (N) (d-block), and tungsten (Tg) (p-block). The elements may include, but are not limited to, iron (Fe) (d-block), copper (Cu) (d-block), niobium (Nb) (d-block), rhodium (Rh) (d-block), gadolinium (Gd) (f-block), thorium (Th) (f-block), cerium (f-block), uranium (U) (f-block), praseodymium (Pr) (f-block), or terbium (Tb) (f-block).

[0034] The metals mentioned above can be bound to the Mo unit in a variety of ways. When selecting a metal for the elutable structure, the metal preferably forms a direct covalent bond with the Mo unit. Bonding can occur via any method, but the bond will typically be an oxo or hydroxo bridge. Bonding forms include, but are not limited to, cyano, nitro, sulfide, amide-nitride, acetate, carbonate, phosphate, and carbonyl bonding schemes, or any combination thereof, as well as others typically found in inorganic compounds. The metal may be bound to the Mo unit without precipitating or forming an oxide or salt, which would result in a homogeneous or heterogeneous mixture of its individual units, e.g., molybdate and metalate units. Preferably, the metal does not act as a binder for Mo or Tc decay products.

[0035] The step of combining the Mo composition and the metal source to obtain the metal-Mo composition may, according to certain embodiments of the present invention, include adding the metal source to the Mo composition, which, according to certain embodiments of the present invention, is stirred or mixed during the addition of the metal source.

[0036] Adding the titanium source to the Mo composition may include, for example, dropwise addition of the metal source to the Mo composition. In this regard, adding the metal source to the Mo composition may include administering the metal source one drop (e.g., 0.05 mL) at a time to the stirring Mo composition. According to certain embodiments of the present invention, the number of drops of metal source added to the Mo composition per minute may be varied. Combining the Mo composition and the metal source to obtain the metal-Mo composition may also include adding an acid (e.g., a second mineral acid) to the Mo composition. According to certain embodiments of the present invention, the temperature may be preferably lowered to a range of about 25°C to about 35°C when the metal source is added with the acid. The acid may include a mineral acid disclosed above. For example, the mineral acid added to the Mo composition during combination of the metal source and the Mo composition may include hydrochloric acid. According to certain embodiments of the present invention, the metal source and the acid (e.g., hydrochloric acid) may be added to the Mo composition simultaneously. For example, the metal source may comprise a liquid composition including, by way of example, one or more metal-containing compounds (e.g., TiCl) and an acid (e.g., hydrochloric acid) disclosed herein. In this regard, adding the metal source may include simultaneous addition of the metal-containing compound(s) and the acid. According to certain embodiments of the present invention, the resulting metal-Mo composition may comprise a final pH of about 3 or less (e.g., about 2 or less, or about 1 or less) at the end of the step of combining the Mo composition and the metal source. According to certain embodiments of the present invention, in the case of titanium, combining the Mo composition and the metal source (e.g., TiCl) to obtain the metal-Mo composition may be performed until a molar ratio of titanium to Mo (metal:Mo) of about 0.1:1 to about 10:1 is reached.

[0037] Methods according to certain embodiments of the present invention may further include adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo fine particles. Suitable bases for neutralizing the acid-decomposed salt or soluble salt include, but are not limited to, metal hydroxide(s), such as alkali and alkaline earth metal hydroxides, ammonium hydroxide, sodium hydroxide, quaternary alkylamine hydroxide, or combinations thereof. According to certain embodiments of the present invention, the pH of the metal-Mo composition is adjusted with a base to a pH in the range of about 4 to about 9. Thus, in certain embodiments of the present invention, the pH of the metal-Mo composition may be adjusted to a minimum of any of the following: about 4, 4.5, 5, 5.5, 6, 6.5, and 7, and / or a maximum of about 9, 8.5, 8, 7.5, 7, 6.5, and 6. While adjusting the pH of the metal-Mo composition, the metal-Mo composition may be subjected to agitation, such as mechanical agitation.

[0038] According to certain embodiments of the present invention, adjusting the pH of the metal-Mo composition may include adding a base dropwise. In this regard, adding a base to the metal-Mo composition may include administering one drop (e.g., 0.05 mL) of base simultaneously with stirring of the Ti-Mo composition. According to certain embodiments of the present invention, the number of drops of base added per minute to the metal-Mo composition may be varied. Other administration forms of the metal source that may be used include, but are not limited to, a mist, a spray, or a combination thereof.

[0039] The metal-Mo composition after the step of adjusting the pH includes a plurality of precipitated metal-Mo fine particles from the pH adjustment and may be subjected to a cooling or chilling step during and / or after adjusting the pH. According to certain embodiments of the present invention, the step of cooling the metal-Mo composition may include lowering the temperature of the metal-Mo composition to about 0°C to about 20°C (e.g., about 3°C ​​to about 10°C). Thus, in certain embodiments of the present invention, the step of cooling the metal-Mo composition may include lowering the temperature of the metal-Mo composition to a minimum of any of the following: about 3°C, 5°C, 8°C, 10°C, and 12°C, and / or to a maximum of about 20°C, 15°C, 12°C, and 10°C.

[0040] After the plurality of metal-Mo particles have precipitated in the metal-Mo composition, the metal-Mo composition may be subjected to a separation operation (e.g., solid-liquid separation), with or without the cooling step discussed above. In this regard, methods according to certain embodiments of the present invention may include a step of separating the plurality of metal-Mo particles from a liquid medium (e.g., an undesired bulk liquid medium). In this regard, the metal-Mo particles may be isolated or separated from the undesired liquid medium. According to certain embodiments of the present invention, the isolated metal-Mo particles may be in the form of a slurry containing a residual amount of the liquid medium therein. According to certain embodiments of the present invention, the step of separating the plurality of metal-Mo particles from the liquid medium may include filtering (e.g., vacuum filtering) or centrifuging the metal-Mo composition to retain at least a majority of the plurality of metal-Mo particles. Filtration media may include, but are not limited to, paper, calcined metal, metal mesh, or combinations thereof. First and / or second filtration media may be used. The separating step can include utilizing a metal filtration surface, with at least a majority of the plurality of metal-Mo particulates being retained on the metal filtration surface. As noted above, the isolated or retained metal-Mo particulates can be in the form of a slurry containing a residual amount of liquid medium therein.

[0041] According to certain embodiments of the present invention, isolated or retained metal-Mo particulates (e.g., in the form of a slurry) can be subjected to thermal energy to at least partially dry the metal-Mo particulates. During exposure to thermal energy, the residual liquid medium entraining the metal-Mo particulates begins to evaporate. However, the metal molybdate molecules remain in a somewhat amorphous solid state rather than in a strongly crystalline state.

[0042] The step of subjecting the plurality of metal-Mo particulates to thermal energy, according to certain embodiments of the present invention, can include exposing the plurality of metal-Mo particulates to infrared radiation. According to certain embodiments of the present invention, the infrared radiation has a wavelength of about 700 nm to about 1400 nm. Thus, in certain embodiments of the present invention, the infrared radiation can have a wavelength of at least any of the following: about 700, 750, 800, 850, 900, 920, 940, 960, 980, and 1000 nm, and / or at most about 1400, 1300, 1200, 1150, 1100, 1080, 1060, 1040, 1020, and 1000 nm.

[0043] According to certain embodiments of the present invention, the thermal energy source may include one or more of convection heat, freeze drying, infrared heaters such as light emitting diodes (LEDs), quartz crystals, quartz infrared heating elements, and incandescent bulbs emitting infrared light. According to certain embodiments of the present invention, the operating temperature may be controlled to be from about 20° C. to about 80° C. In this regard, the operating temperature may include a minimum of any of the following: about 20° C., 30° C., 40° C., 45° C., 50° C., 55° C., and 60° C., and / or a maximum of about 80° C., 75° C., 70° C., 65° C., and 60° C.

[0044] After subjecting the metal-Mo particulate to thermal energy, the metal-Mo particulate may optionally be subjected to a crushing or grinding operation. According to certain embodiments of the present invention, the metal-Mo particulate may be crushed by a number of commercially available mills, such as ball mills, hammer mills, high-pressure grinding rolls, tower mills, and wet mills (e.g., conical wet mills).

[0045] According to certain embodiments of the present invention, after the milling step, the plurality of metal-Mo particulates may have an average size of about 10 microns to about 1275 microns (e.g., about 100 microns to about 200 microns, about 630 microns to about 1015 microns). According to certain embodiments of the present invention, for example, after the milling step, the average size of the plurality of metal-Mo particulates may include a minimum of any of the following: about 10, 50, 75, 125, 150, 175, 200, 225, 250, 275, 300, 350, 400, 450, 500, 550, 600, 650, 700, 750, 800, 850, 900, 925, and 950 microns, and / or a maximum of about 1275, 1250, 1225, 1200, 1175, 1150, 1125, 1100, 1050, 1000, and 950 microns.

[0046] According to certain embodiments of the present invention, the selected particle size can be selected by mechanical filtering, chemical filtering, or a combination thereof.

[0047] Metal-Mo particulates milled according to certain embodiments of the present invention may be subjected to a washing step.

[0048] According to certain embodiments of the present invention, the washed metal-Mo particles can be collected and dried to remove most of the washing solution. The drying operation is not particularly limited. After drying the washed metal-Mo particles, the metal-Mo particles may tend to agglomerate together. Therefore, the metal-Mo particles may be subjected to a second grinding process, including a dry grinding process, and after the second grinding step, the plurality of metal-Mo particles may comprise particles of about 10 microns to about 1275 microns (e.g., about 100 microns to about 200 microns, about 630 microns to about 1015 microns). According to certain embodiments of the present invention, for example, after the second milling step, the average size of the plurality of metal-Mo particulates may include a minimum of any of the following: about 10, 50, 75, 125, 150, 175, 200, 225, 250, 275, 300, 350, 400, 450, 500, 550, 600, 650, 700, 750, 800, 850, 900, 925, and 950 microns, and / or a maximum of about 1275, 1250, 1225, 1200, 1175, 1150, 1125, 1100, 1050, 1000, and 950 microns.

[0049] According to certain embodiments of the present invention, a method may include irradiating a metallic molybdenum target to obtain the Mo material discussed herein. The metallic molybdenum target may include, for example, a tubular capsule including metallic molybdenum and a plurality of metallic molybdenum internal components (e.g., balls, rods, wires, disks) housed within the tubular capsule. For example, the tubular capsule may include a first end, a second end, and a wall connecting the first end and the second end to define a cavity therein. In this regard, a plurality of metallic molybdenum internal components (e.g., balls, rods, wires, disks) may be packed into the cavity within the tubular capsule. According to certain embodiments of the present invention, at least the first end may be configured to be accessible to the cavity for receiving, and optionally not receiving, a plurality of metallic molybdenum internal components (e.g., balls, rods, wires, disks). In this regard, at least the first end (or a portion thereof) may be configured to be removable from the tubular capsule for access to the cavity. According to certain embodiments of the present invention, the metallic Mo material in the reacting step includes a plurality of metallic molybdenum internal components, a tubular capsule, or both.

[0050] The molybdenum metal target may include a plurality of molybdenum metal disks (e.g., circular disks) each having a length, width, and thickness in the z-direction. In this regard, the thickness may be less than both the length and the width. According to certain embodiments of the present invention, the thickness may be from about 2 microns to about 260 microns (e.g., from about 10 microns to about 150 microns). According to certain embodiments of the present invention, for example, the thickness may be at least about 2, 10, 20, 30, 40, 50, 60, 70, 80, 90, and 100 microns, and / or at most about 275, 260, 250, 225, 200, 175, 150, 140, 130, 120, 110, and 100 microns. According to certain embodiments of the present invention, the molybdenum metal disks are packed side-by-side in the z-direction inside a tubular capsule. According to certain embodiments of the present invention, the molybdenum metal disks may be used without a capsule. According to certain embodiments of the present invention, the molybdenum metal disks may be formed from a molybdenum metal sheet, for example, by stamping. According to certain embodiments of the present invention, the Mo metal material in the reacting step includes a plurality of molybdenum metal disks, tubular capsule components, or both.

[0051] Figure 1 illustrates an exemplary embodiment according to the present invention. Specifically, Figure 1 illustrates a method that includes, in operation 10, the optional step (indicated by a dashed line) of irradiating a metallic molybdenum target to obtain a metallic Mo material, followed by combining the metallic Mo material (e.g., obtained from operation 10 or obtained from a third party) with at least a first acid in a liquid medium to obtain a Mo composition in operation 20. As illustrated in Figure 1, the method includes, in operation 30, combining a Mo composition with a metal source to obtain a metal-Mo composition, and, in operation 40, adjusting the pH of the metal-Mo composition to about 4 to about 9 with a base to precipitate a plurality of metal-Mo particles. As illustrated in the exemplary embodiment of Figure 1, the metal-Mo composition may optionally be subjected to a step of cooling the metal-Mo composition in operation 50 prior to separating the plurality of metal-Mo particles from the liquid medium in operation 60. The metal-Mo particulate isolated after operation 60 may be subjected to a step of exposing the plurality of metal-Mo particulates to thermal energy in operation 70, followed by a step of milling the plurality of metal-Mo particulates in operation 80. As illustrated by the detailed illustrative example of Figure 1, the method may then include an optional step of washing the plurality of metal-Mo particulates in operation 90, followed by a second drying step in operation 100. As shown in Figure 1, the method may include an optional step 110 of re-milling (e.g., dry-milling) the dried metal-Mo particulates.

[0052] As noted above, the molybdenum metal target that can be irradiated to obtain Mo material can include a tubular capsule and / or multiple molybdenum metal parts (eg, balls, rods, wires, disks).

[0053] The metallic molybdenum target, according to certain embodiments of the present invention, may be irradiated by, for example, neutron capture in a nuclear fission reactor. According to certain embodiments of the present invention, the Mo materials disclosed herein may be obtained by a variety of Mo production techniques, including, for example, nuclear fission reactors (e.g., recovered uranium, low-enriched uranium, and highly enriched uranium), particle accelerators, and neutron capture. According to certain embodiments of the present invention, the metallic molybdenum target may be irradiated by any type of nuclear reactor into which a Mo target can be inserted. Non-limiting examples of nuclear reactors include, but are not limited to, high-flux isotope reactors (HFIRs), CANDU reactors (e.g., CANDU reactors, CANDU 6 reactors, CANDU 9 reactors, Advanced CANDU Reactors (ACRs), etc.). Other non-limiting examples of nuclear reactors are power and research reactors, including, but not limited to, the University of Missouri Research Reactor (MURR), the National Institute of Standards and Technology (NIST) reactor, the MIT Nuclear Research Reactor (MITR), and the Advanced Test Reactor (ATR).

[0054] In this regard, according to certain embodiments of the present invention, the source of the Mo materials disclosed herein is not particularly limited.

[0055] According to certain embodiments of the present invention, for example, the average size of the plurality of metal-Mo particulates may include a minimum of any of the following: about 10, 50, 75, 100, 125, 150, 175, 200, 225, 250, 275, 300, 350, 400, 450, 500, 550, 600, 650, 700, 750, 800, 850, 900, 925, and 950 microns, and / or a maximum of about 1275, 1250, 1225, 1200, 1175, 1150, 1125, 1100, 1050, 1000, and 950 microns.

[0056] According to certain embodiments of the present invention, the metal-Mo material has an elution efficiency of 30% or greater, 80% or greater, 90% or greater, or 95% or greater. According to certain embodiments of the present invention, the metal-Mo material can be placed in an elution column and equipped with a technetium-99m generator, and at least 90% (e.g., at least 95% or at least 99%) of the total technetium content can be released from the metal-Mo material by passing an aqueous liquid (e.g., water, saline, dilute acid) through the metal-Mo material. In this regard, certain embodiments of the present invention enable the use of larger elution columns (e.g., technetium-99m generators). For example, elution with a standard 20 milliliter saline solution can extract technetium from a much larger elution column than a standard 3 milliliter-sized elution column. Therefore, certain embodiments of the present invention enable the achievement of a target Tc-99m activity from a smaller than expected Mo activity. As a result, lower neutron flux reactors can be used to provide commercially viable products to the industry, and a larger number of reactors can be involved in suitable Mo production.

[0057] In this regard, certain embodiments of the present invention enable the use of elution columns (e.g., technetium-99m generators) larger than the standard 3 milliliter size (e.g., 5 mL, 10 mL, 12 mL, 15 mL, 20 mL, 25 mL, 30 mL, 60 mL, or 100 mL), such that the use of low neutron flux reactors to produce the desired target activity of technetium is now feasible. For example, low neutron flux reactors that were previously unavailable to generate sufficiently high specific activities of technetium for commercial purposes may now be feasibly utilized in accordance with certain embodiments of the present invention. In this regard, a variety of nuclear reactors may be used to provide Mo for processing in accordance with certain embodiments of the present invention.

[0058] As noted above, metal-Mo materials according to certain embodiments of the present invention allow for the use of elution columns larger than the standard 3 milliliter size (e.g., 5 mL, 10 mL, 12 mL, 15 mL, 20 mL, 25 mL, 30 mL, 60 mL, or 100 mL), so that the use of low neutron flux reactors to produce the desired target activity of technetium is now feasible.

[0059] Therefore, the present invention also provides an elution pig configured to accept elution columns of various sizes, allowing a variety of nuclear reactors (e.g., high and / or low flux reactors) to be integrated into a supply chain for producing Tc-99m. According to certain embodiments of the present invention, the elution pig can be configured to accept a variety of elution columns of different sizes, including 3 mL, 5 mL, 10 mL, 12 mL, 15 mL, 20 mL, 25 mL, 30 mL, 60 mL, 100 mL, or any combination thereof.

[0060] According to certain embodiments of the present invention, the metal-Mo particles may be irradiated prior to loading into the cask transfer case or elution column. This step can eliminate the optional step of irradiating the metal molybdenum target earlier in the process. Of such post-irradiation process steps, conducting chemical processes without radiation control can be particularly advantageous as it reduces or eliminates the generation of radioactive waste and shortens the processing time leading to higher initial activity of the metal-Mo particles.

[0061] Figure 2 illustrates this embodiment after irradiation in accordance with the present invention. As illustrated in Figure 2, the method includes step 210 of reacting a metal-Mo material in a liquid medium with at least a first acid to obtain a Mo composition. The method includes combining the Mo composition with a metal source to obtain a metal-Mo composition in step 215, and adjusting the pH of the metal-Mo composition with a base to a pH of about 4 to about 9 to precipitate a plurality of metal-Mo particles / particulates in step 220. As illustrated in the exemplary embodiment of Figure 2, prior to step 230 of separating the plurality of metal-Mo particles from the liquid medium, the metal-Mo composition may optionally be subjected to step 225 of cooling the metal-Mo composition. After step 230, the isolated metal-Mo particles may be subjected to step 235 of exposing the plurality of metal-Mo particles to thermal energy, followed by step 240 of milling the plurality of metal-Mo particles. As illustrated by the detailed illustrative example of Figure 2, the method may then include an optional step 245 of washing the plurality of metal-Mo particles, followed by a second drying step 250. As shown in Figure 2, the method may then include an optional step 255 of re-grinding (e.g., dry-grinding) the dried metal-Mo particles. As illustrated by the detailed illustrative example of Figure 2, the method may then include an optional step 260 of irradiating the resulting metal-Mo particles prior to loading into the elution column.

[0062] According to certain embodiments of the present invention, another method for producing a metal molybdate material is provided. As illustrated in FIG. 3 , the method optionally includes step 310 of irradiating a metallic molybdenum target to obtain a metallic Mo material. The method also includes step 315 of reacting the metallic Mo material in a liquid medium with at least a first acid to obtain a Mo composition. The method includes combining the Mo composition with a metal source to obtain a metal-Mo composition in step 320, and pH-adjusting the metal-Mo composition to about pH 4 to about pH 9 with a base in step 325 to precipitate a plurality of metal-Mo particles or particulates. As illustrated in the exemplary embodiment of FIG. 3 , the metal-Mo composition may optionally be subjected to step 330 of cooling the metal-Mo composition before step 335 of separating the plurality of metal-Mo particles from the liquid medium. As illustrated by the detailed exemplary embodiment of FIG. 3 , the method may then include optional step 340 of washing the plurality of metal-Mo particles, preferably with deionized water. As shown in Figure 3, the method may include an optional step 345 of optionally loading the metal-Mo particles, either wet or in slurry form, into a cask transfer case or elution column. If step 345 is not performed, the method includes a step 350 of drying the metal-Mo particles and a step 355 of crushing the metal-Mo particles. The crushed metal-Mo particles may be loaded into a cask transfer case or elution column, as shown in step 360 of Figure 3.

[0063] Certain embodiments of the present invention provide methods for producing metal molybdate materials, with optional post-irradiation steps. FIG. 4 illustrates an example of another embodiment according to the present invention. As illustrated in FIG. 4, the method includes step 415 of reacting a metal-Mo material in a liquid medium with at least a first acid to obtain a Mo composition. The method includes combining the Mo composition with a metal source to obtain a metal-Mo composition in step 420, and then adjusting the pH of the metal-Mo composition with a base to about 4 to about 9 to precipitate a plurality of metal-Mo particles or particulates in step 425. As illustrated in the exemplary embodiment of FIG. 4, the metal-Mo composition may optionally be subjected to step 430 of cooling the metal-Mo composition prior to step 435 of separating the plurality of metal-Mo particles from the liquid medium. As illustrated by the detailed exemplary embodiment of FIG. 4, the method may then include an optional step 440 of washing the plurality of metal-Mo particles, preferably with deionized water. As shown in Figure 4, the method may include an optional step 445 of optionally loading the metal-Mo particles, either wet or in slurry form, into a cask transfer case or an elution column. If step 445 is not performed, the method may include a step 450 of drying the metal-Mo particles and a step 455 of crushing the metal-Mo particles. As illustrated by the detailed illustrative example of Figure 4, the method may then include an optional step 460 of irradiating the resulting metal-Mo particles. The crushed and optionally irradiated metal-Mo particles may be loaded into a cask transfer case or an elution column, as shown in step 465 of Figure 4.

[0064] 3 and 4 may operate with a variety of process parameters and still fall within the scope of the present invention, however, some illustrative process parameters are provided below for illustrative purposes only.

[0065] In step 315 of Figure 3 and step 415 of Figure 4, a minimum concentration of 2 to 15 molar nitric acid can be used, diluted with water as needed to achieve the required concentration. In a drying step, such as step 350 of Figure 3 or step 450 of Figure 4, the drying temperature can range from 70°C to 200°C, for example. In the methods of Figures 3 and 4, the initial loading of molybdenum can be low, for example, 20 grams. Similarly, the volume of the metal source can be low, for example, 134 mL for a 20 gram loading of Mo. The amount of ammonium hydroxide can be varied as a result of reducing the amount of metal source. The particle size can be varied, preferably from 10 microns (µm) to 250 microns (µm) in diameter.

[0066] In yet another aspect, the present invention provides a cask transfer case and process. For transporting highly radioactive Mo material from a nuclear reactor to a site for chemical processing (e.g., addition to a metal source) or for transporting irradiated metal-Mo particles, certain embodiments of the present invention provide a cask transfer case that can protect personnel from unwanted doses of radioactivity. The cask transfer case can safely load and transport Mo material, as well as unloaded Mo material. FIG. 5 illustrates an exemplary embodiment of a cask transfer case 1000, including, for example, a housing (e.g., comprising lead) 1110 and a dial 1120 connected to a rotating shaft 1130 that protrudes at least partially through the body of the housing. As shown in FIG. 5, the dial 1120 can be rotated to indicate the operating status of the cask transfer case 1000. As shown in FIG. 5, for example, "L1" indicates that the cask transfer case is in an operational state with radioactive material loaded into a first location via material inlet port 1140, as discussed in more detail below. As shown in FIG. 6, cask transfer case 1000 includes multiple loading locations (e.g., "L1," "L2," and "L3"). For example, FIG. 6 is a cross-sectional view of FIG. 5 illustrating the internal structure of cask transfer case 1000 according to certain embodiments of the present invention. As shown in FIG. 6, material inlet port 1140 is operably connected to inlet conduit 1150. FIG. 6 illustrates inlet port 1140 for, for example, radioactive Mo material 600 being inserted into and via inlet conduit 1150. As shown in FIG. 6, 11. The rotational axis 1130 is connected to an internal conduit housing 1160, which defines one or more internal conduits 1170 defined by the internal conduit housing 1160. In this regard, the one or more internal conduits 1170 extend the entire length of the internal conduit housing 1160. In this regard, the length of the one or more internal conduits 1170 exceeds the length of the material (e.g., radioactive Mo material 600) loaded therein, such that the internal conduit housing can freely rotate about the rotational axis 1130.According to certain embodiments of the present invention, one of the internal conduits 1170 can be aligned with the inlet conduit 1150 when the dial 1120 is positioned to indicate material loading. Thus, material (e.g., radioactive Mo material 600) to be loaded into the cask transfer case 1000 can be inserted through the inlet port 1140, moved through the inlet conduit 1150, and placed inside the aligned internal conduit 1170 (e.g., the bottom surface of the loaded material can be placed inside the bottom of the housing 1110 and confined by the internal conduit 1170). As shown in FIG. 6, the housing 1110 also includes an outlet conduit 1180 located below the internal conduit housing 1160 so that material loaded into the cask transfer case can drop into and be released from the internal conduit 1170 when the dial is positioned to indicate a dropping material operating state (e.g., "D1," "D2," and "D3" in FIG. 5). In such an operating state, internal conduits 1170 may be aligned with outlet conduits 1180 such that loaded material falls from the internal conduits, passes through the outlet conduits, and exits cask transfer case 100 via outlet ports 1190. As illustrated by FIG. 5 , cask transfer case may include an operating state (e.g., “XFER” in FIG. 5 ) that indicates that the cask transfer case is ready to be transferred or that any loaded material therein may be repositioned without risk of exiting via inlet port 1140 or outlet port 1190. For example, when cask transfer case 1000 is in an operating state for transfer according to certain embodiments of the present invention, none of internal conduits 1170 are aligned with inlet conduits 1150 or outlet conduits 1180. That is, inlet conduit 1150 is not aligned with any of internal conduits 1170, and / or outlet conduit 1180 is not aligned with any of internal conduits 1170. In this regard, cask transfer case 1000 is considered safe to be repositioned to transport radioactive material disposed therein.

[0067] Additionally or alternatively, the present invention may have the following configurations. [Article 1] 1. A method for producing metal molybdate (metal-Mo), comprising: reacting a metallic molybdenum (Mo) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and 1. A method comprising: adjusting the pH of a metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates. [Clause 2] 10. The method of claim 1, wherein the first acid comprises a mineral acid. [Article 3] 3. The method of claim 2, wherein the mineral acid is selected from the group consisting of hydrochloric acid, nitric acid, sulfuric acid, phosphoric acid, hydrofluoric acid, boric acid, hydrobromic acid, perchloric acid, hydroiodic acid, halogen acids, and combinations thereof. [Article 4] 4. The method of claim 3, wherein the mineral acid is selected from the group consisting of hydrochloric acid, nitric acid, sulfuric acid, and combinations thereof. [Article 5] 10. The method of claim 1, wherein the liquid medium comprises an aqueous medium. [Article 6] 10. The method of claim 1, wherein the step of reacting the metallic Mo material in a liquid medium with a first acid is carried out at a molar ratio of Mo material to first acid ranging from about 0.1:1 to about 10:1. [Article 7] 10. The method of claim 1, wherein the step of reacting the metallic Mo material in the liquid medium with the first acid subjects the metallic Mo material to oxidation, dissolution, or a combination of oxidation and dissolution. [Article 8] 10. The method of claim 1, wherein the step of reacting the metallic Mo material in a liquid medium with a first acid subjects the metal oxide formed from the combination to oxidation, dissolution, or a combination of oxidation and dissolution. [Article 9] 6. The method of clause 5, further comprising controlling the temperature of the aqueous medium by heating the aqueous medium, removing heat from the aqueous medium, or both. [Article 10] 10. The method of clause 9, wherein controlling the temperature of the aqueous medium comprises heating the aqueous medium to above 25°C. [Article 11] 10. The method of clause 9, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below about 80°C. [Article 12] 10. The method of clause 9, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below about 70°C. [Article 13] 10. The method of clause 9, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below about 60°C. [Article 14] 10. The method of clause 9, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below about 50°C. [Article 15] 10. The method of clause 9, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below about 40°C. [Article 16] 10. The process of clause 9, further comprising agitating the metallic Mo material and the aqueous medium during at least a portion of the reaction. [Article 17] 17. The method of claim 16, wherein the agitating comprises mechanically mixing the metallic Mo material and the aqueous medium. [Article 18] 10. The method of claim 1, wherein the metal source comprises an element from the p-block, d-block, or f-block of the periodic table. [Article 19] 17. The method of clause 16, wherein the metal source comprises a metal, metalate, or metal salt. [Article 20] 10. The method of claim 1, wherein the metal source is selected from the group consisting of elemental or non-oxidized metals, metal oxides, metal hydroxides, metal halides, nitrates, phosphates, tetrafluoroborides, phosphorus hexafluoride, tosylates, acetates, formates, any other counter anions capable of forming a soluble salt, and combinations thereof. [Article 21] The metal, metalate or metal salt may be in various oxidation states of M n+ 20. The method of claim 19, wherein n=1, 2, 3, 4, 5 or 6. [Article 22] 20. The method of claim 19, wherein the metal, metalate, or metal salt forms a bond with another metal, metalate, metal salt, or molybdate. [Article 23] 23. The method of clause 22, wherein the linkage comprises an oxo bridge, a hydroxo bridge, or a combination thereof. [Article 24] 23. The method of clause 22, wherein the linkage comprises cyano, nitro, sulfide, amide nitride, acetate, carbonate, phosphate, carbonyl, or a combination thereof. [Article 25] 20. The method of claim 19, wherein the metal, metalate, or metal salt forms an individual structural unit or a composite structural unit. [Article 26] The metal, metalate or metal salt is Mo x O y is linked to the individual structural units present, x is the number of Mo atoms, and y is the number of O atoms. [Article 27] The metal, metalate, or metal salt remains unchanged under ionizing radiation and is x O y and x is the number of Mo atoms and y is the number of O atoms. [Article 28] 20. The method of clause 19, wherein the metal, metalate or metal salt does not give rise to any unwanted daughter products from neutron bombardment in the final eluate. [Article 29] 2. The method of claim 1, wherein the metal source is selected from the group consisting of aluminum, silicon, tin, germanium, zirconium, titanium, hafnium, vanadium, chromium, manganese, cobalt, nickel, iron, copper, niobium, rhodium, gadolinium, thorium, cerium, uranium, praseodymium, terbium, and combinations thereof. [Article 30] 30. The method of claim 29, wherein the titanium is a titanium salt selected from the group consisting of titanium (III) chloride (TiCl), titanium (II) chloride (TiCl), titanium tetrachloride (TiCl), and combinations thereof. [Article 31] 31. The method of clause 30, wherein the titanium salt comprises a counterion selected from the group consisting of nitrate, halide, and combinations thereof. [Article 32] 30. The method of claim 29, wherein the titanium comprises unoxidized titanium metal or a metal carbonyl. [Article 33] 30. The method of claim 29, wherein titanium is combined with a metal oxide, metal hydroxide, phosphate, tetrafluoroborate, phosphorus hexafluoride, tosylate, acetate, formate, or any other counteranion capable of forming a soluble salt. [Article 34] 10. The method of claim 1, wherein combining the Mo composition and the metal source to obtain the metal-Mo composition comprises adding the metal source to the Mo composition. [Article 35] 10. The method of claim 1, wherein the step of combining the Mo composition and the metal source is carried out until a molar ratio of titanium to Mo of about 0.1:1 to about 10:1 is reached. [Article 36] 35. The method of claim 34, wherein adding the metal source to the Mo composition comprises adding the metal source to the Mo composition in a form selected from the group consisting of droplets, a spray, a mist, and combinations thereof. [Article 37] 10. The method of claim 1, wherein the step of combining the Mo composition and the metal source to obtain the metal-Mo composition further comprises adding a second acid to the Mo composition. [Article 38] 38. The method of clause 37, wherein the second acid comprises a mineral acid. [Article 39] 38. The method of clause 37, wherein the second acid comprises hydrochloric acid. [Article 40] 38. The method of claim 37, wherein adding the second acid occurs simultaneously with adding the metal source to the Mo composition. [Article 41] 10. The method of claim 1, wherein at the end of the step of combining the Mo composition and the metal source, the metal-Mo composition has a final pH of about 3 or less. [Article 42] 10. The method of claim 1, wherein adjusting the pH of the metal-Mo composition comprises adding a base to bring the pH to a range of about 4 to about 9. [Article 43] 10. The method of claim 1, wherein the base for adjusting the pH of the metal-Mo composition comprises ammonium hydroxide. [Article 44] 10. The method of claim 1, wherein adjusting the pH of the metal-Mo composition comprises adding a base to the metal-Mo composition dropwise. [Article 45] 10. The method of claim 1, further comprising cooling the metal-Mo composition during the step of pH adjusting the metal-Mo composition, after the step of pH adjusting the metal-Mo composition, or both. [Article 46] 46. ​​The method of clause 45, wherein the step of cooling the metal-Mo composition comprises lowering the temperature of the metal-Mo composition to between about 0°C and about 20°C. [Article 47] 46. ​​The method of clause 45, wherein the step of cooling the metal-Mo-99 composition comprises reducing the temperature of the metal-Mo composition to between about 3°C ​​and about 10°C. [Article 48] 10. The method of claim 1, further comprising separating the plurality of metal particulates from the liquid medium. [Article 49] 49. The method of claim 48, wherein the step of separating the plurality of metal-Mo particulates from the liquid medium comprises filtering the metal-Mo composition to retain at least a majority of the plurality of metal-Mo particulates. [Article 50] 50. The method of claim 49, wherein filtering the metal-Mo composition comprises utilizing a metal filtering surface. [Article 51] 51. The method of clause 50, wherein at least a majority of the plurality of metal-Mo particulates are retained on the metal filtering surface. [Article 52] 49. The method of claim 48, wherein the metal-Mo composition has a temperature of about 0° C. to about 20° C. during the step of separating the plurality of metal-Mo particulates from the liquid medium. [Article 53] 10. The method of claim 1, further comprising milling the plurality of metal-Mo particulates. [Article 54] 54. The method of claim 53, wherein the milling step comprises wet milling. [Article 55] 54. The method of claim 53, wherein the plurality of metal-Mo particulates have an average size after milling ranging from about 10 microns to about 1275 microns. [Article 56] 54. The method of claim 53, wherein the plurality of metal-Mo particulates have an average size after milling in the range of about 10 microns to about 1015 microns. [Article 57] 10. The method of claim 1, further comprising washing the plurality of metal-Mo particulates with water. [Article 58] 10. The method of claim 1, further comprising drying the plurality of metal-Mo particulates. [Article 59] 10. The method of claim 1, further comprising irradiating the plurality of metal-Mo particulates. [Article 60] 10. The method of claim 1, further comprising irradiating a metallic molybdenum target to obtain a metallic Mo material. [Article 61] 61. The method of clause 60, wherein the molybdenum metal target comprises a plurality of molybdenum metal disks. [Article 62] 61. The method of clause 60, wherein the metallic Mo material comprises a plurality of metallic molybdenum disks, tubular capsule components, or both. [Article 63] 2. A metal molybdate prepared by the method described in clause 1. [Article 64] 1. A method for producing metal molybdate (metal-Mo), comprising: wholly or partially oxidizing a metallic molybdenum (Mo) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and A method comprising: adjusting the pH of a metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates. [Article 65] 65. A metal molybdate prepared by the method described in clause 64. [Article 66] 1. A method for producing metal molybdate (metal-Mo), comprising: wholly or partially dissolving a metallic molybdenum (Mo) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and A method comprising: adjusting the pH of a metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates. [Article 67] 1. A method for producing metal molybdate (metal-Mo), comprising: combining a metallic molybdenum (Mo) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and A method comprising: adjusting the pH of a metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates. [Article 68] A metal molybdate (metal-Mo) material, wherein the plurality of metal-Mo particulates comprises at least one bond between the metal, metalate or metal salt, and the molybdate of the metal-Mo particulate, wherein the bond is in the form of an oxo-bridge, a hydroxo-bridge, or a combination thereof. [Article 69] 69. The material of clause 68, wherein the plurality of metal-Mo particulates have an average size ranging from about 10 microns to about 1275 microns. [Article 70] 69. The material of clause 68, wherein the plurality of metal-Mo particulates have an average size ranging from about 10 microns to about 1015 microns. [Article 71] 69. The material of clause 68, wherein the metal-Mo material has an elution efficiency of 30% or greater. [Article 72] 69. The material of clause 68, wherein the metal-Mo material has an elution efficiency of 70% or greater. [Article 73] 69. The material of clause 68, wherein the metal-Mo material has an elution efficiency of 80% or greater. [Article 74] 69. The material of clause 68, wherein the metal-Mo material is placed in an elution column and at least 90% of the total technetium content is released from the metal-Mo material by passing an aqueous liquid through the metal-Mo material. [Article 75] 75. The material of clause 74, wherein the aqueous liquid is selected from the group consisting of water, saline, dilute acid and combinations thereof. [Article 76] A cask transfer case containing metal-Mo material as described in Article 68. [Article 77] 69. A system for producing technetium comprising an elution column having a volume of at least 3 mL and a metal-Mo material as described in clause 68. [Article 78] 78. The system of clause 77, wherein the elution column has a volume of greater than 3 mL.

[0068] The present invention may additionally or alternatively have the following configurations. [Article 1] 1. A method for producing metal molybdate (metal-Mo), comprising: reacting a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition, wherein the liquid medium comprises an aqueous medium; combining the Mo composition with a metal source to obtain a metal-Mo composition; adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates; controlling the temperature of the aqueous medium by heating the aqueous medium, removing heat from the aqueous medium, or both; and agitating the metallic Mo-99 material and the aqueous medium during at least a portion of the reaction; the metal source comprises a metal, metalate, or metal salt; a metal, metalate, or metal salt forms a bond with another metal, metalate, metal salt, or molybdate; The method wherein the linkage comprises a cyano, nitro, sulfide, amide nitride, acetate, carbonate, phosphate, carbonyl, or combinations thereof. [Clause 2] 10. The method of claim 1, wherein the first acid comprises a mineral acid. [Article 3] 3. The method of clause 2, wherein the mineral acid is a halogen acid. [Article 4] 4. The method of claim 3, wherein the mineral acid is selected from the group consisting of hydrochloric acid, nitric acid, sulfuric acid, and combinations thereof. [Article 5] 10. The method of claim 1, wherein the step of reacting the metallic Mo-99 material in a liquid medium with a first acid is carried out at a molar ratio of Mo-99 material to first acid in the range of 0.1:1 to 10:1. [Article 6] 10. The method of claim 1, wherein the step of reacting the metallic Mo-99 material in the liquid medium with the first acid subjects the metallic Mo-99 material to oxidation, dissolution, or a combination of oxidation and dissolution. [Article 7] 10. The method of claim 1, wherein the step of reacting the metallic Mo-99 material in a liquid medium with a first acid subjects the metal oxide formed from the combination to oxidation, dissolution, or a combination of oxidation and dissolution. [Article 8] 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises heating the aqueous medium to above 25°C. [Article 9] 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 80°C. [Article 10] 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 70°C. [Article 11] 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 60°C. [Article 12] 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 50°C. [Article 13] 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 40°C. [Article 14] 10. The method of claim 1, wherein the agitating comprises mechanically mixing the metallic Mo-99 material and the aqueous medium. [Article 15] 10. The method of claim 1, wherein the metal source comprises an element from the p-block, d-block, or f-block of the periodic table. [Article 16] 10. The method of claim 1, wherein the metal source is selected from the group consisting of elemental or non-oxidized metals, metal oxides, metal hydroxides, metal halides, nitrates, phosphates, tetrafluoroborides, phosphorus hexafluoride, tosylates, acetates, formates, any other counter anions capable of forming a soluble salt, and combinations thereof. [Article 17] The metal, metalate or metal salt may be in various oxidation states of M n+ 2. The method of clause 1, wherein n=1, 2, 3, 4, 5 or 6. [Article 18] 10. The method of claim 1, wherein the linkage comprises an oxo bridge, a hydroxo bridge, or a combination thereof. [Article 19] 10. The method of claim 1, wherein the metal, metalate, or metal salt forms an individual structural unit or a composite structural unit. [Article 20] The metal, metalate or metal salt is Mo x O y is linked to the individual structural units present, x is the number of Mo atoms, and y is the number of O atoms. [Article 21] The metal, metalate, or metal salt remains unchanged under ionizing radiation and is x O y and the bond formed by x is the number of Mo atoms and y is the number of O atoms. [Article 22] 10. The method of claim 1, wherein the metal, metalate, or metal salt does not produce any unwanted daughter products from neutron bombardment in the final eluate. [Article 23] 2. The method of claim 1, wherein the metal source is selected from the group consisting of aluminum, silicon, tin, germanium, zirconium, hafnium, vanadium, chromium, manganese, cobalt, nickel, iron, copper, niobium, rhodium, gadolinium, thorium, cerium, uranium, praseodymium, terbium, and combinations thereof. [Article 24] 10. The method of claim 1, wherein combining the Mo composition and the metal source to obtain the metal-Mo composition comprises adding the metal source to the Mo composition. [Article 25] 25. The method of claim 24, wherein adding the metal source to the Mo composition comprises adding the metal source to the Mo composition in a form selected from the group consisting of droplets, a spray, a mist, and combinations thereof. [Article 26] 10. The method of claim 1, wherein the step of combining the Mo composition and the metal source to obtain the metal-Mo composition further comprises adding a second acid to the Mo composition. [Article 27] 27. The method of clause 26, wherein the second acid comprises a mineral acid. [Article 28] 27. The method of clause 26, wherein the second acid comprises hydrochloric acid. [Article 29] 27. The method of claim 26, wherein adding the second acid occurs simultaneously with adding the metal source to the Mo composition. [Article 30] 10. The method of claim 1, wherein at the end of the step of combining the Mo composition and the metal source, the metal-Mo composition has a final pH of 3 or less. [Article 31] 10. The method of claim 1, wherein adjusting the pH of the metal-Mo composition comprises adding a base to achieve a pH in the range of 4 to 9. [Article 32] 10. The method of claim 1, wherein the base for adjusting the pH of the metal-Mo composition comprises ammonium hydroxide. [Article 33] 10. The method of claim 1, wherein adjusting the pH of the metal-Mo composition comprises adding a base to the metal-Mo composition dropwise. [Article 34] 10. The method of claim 1, further comprising cooling the metal-Mo composition during the step of pH adjusting the metal-Mo composition, after the step of pH adjusting the metal-Mo composition, or both. [Article 35] 35. The method of claim 34, wherein the step of cooling the metal-Mo composition comprises lowering the temperature of the metal-Mo composition to between 0°C and 20°C. [Article 36] 35. The method of claim 34, wherein the step of cooling the metal-Mo composition comprises reducing the temperature of the metal-Mo composition to between 3°C and 10°C. [Article 37] 10. The method of claim 1, further comprising separating the plurality of metal particulates from the liquid medium. [Article 38] 38. The method of claim 37, wherein separating the plurality of metal-Mo particulates from the liquid medium comprises filtering the metal-Mo composition to retain at least a majority of the plurality of metal-Mo particulates. [Article 39] 39. The method of claim 38, wherein filtering the metal-Mo composition comprises utilizing a metal filtering surface. [Article 40] 40. The method of claim 39, wherein at least a majority of the plurality of metal-Mo particulates are retained on the metal filtering surface. [Article 41] 38. The method of claim 37, wherein the metal-Mo composition has a temperature of 0° C. to 20° C. during the step of separating the plurality of metal-Mo particulates from the liquid medium. [Article 42] 10. The method of claim 1, further comprising milling the plurality of metal-Mo particulates. [Article 43] 43. The method of claim 42, wherein the milling step comprises wet milling. [Article 44] 43. The method of claim 42, wherein the plurality of metal-Mo particulates have an average size after milling in the range of 10 microns to 1275 microns. [Article 45] 43. The method of claim 42, wherein the plurality of metal-Mo particulates have an average size after milling in the range of 10 microns to 1015 microns. [Article 46] 10. The method of claim 1, further comprising washing the plurality of metal-Mo particulates with water. [Article 47] 10. The method of claim 1, further comprising drying the plurality of metal-Mo particulates. [Article 48] 10. The method of claim 1, further comprising irradiating the plurality of metal-Mo particulates. [Article 49] 10. The method of claim 1, further comprising irradiating a metallic molybdenum target to obtain metallic Mo-99 material. [Article 50] 50. The method of clause 49, wherein the molybdenum metal target comprises a plurality of molybdenum metal disks. [Article 51] 50. The method of claim 49, wherein the metallic Mo-99 material comprises a plurality of metallic molybdenum disks, tubular capsule components, or both. [Article 52] 1. A method for producing metal molybdate (metal-Mo), comprising: wholly or partially oxidizing a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates; The method wherein the metal source is titanium, the titanium comprising unoxidized titanium metal or a metal carbonyl. [Article 53] 1. A method for producing metal molybdate (metal-Mo), comprising: dissolving metallic molybdenum-99 (Mo-99) material in a liquid medium, either wholly or partially, with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates; The method wherein the metal source is titanium, the titanium comprising unoxidized titanium metal or a metal carbonyl. [Article 54] 1. A method for producing metal molybdate (metal-Mo), comprising: combining a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo particulates; The method wherein the metal source is titanium, the titanium comprising unoxidized titanium metal or a metal carbonyl.

[0069] These and other modifications and variations to the present invention can be practiced by those skilled in the art without departing from the spirit and scope of the present invention, which is more particularly set forth in the appended claims. Furthermore, it should be understood that aspects of the various embodiments may be interchangeable in whole or in part. Furthermore, those skilled in the art will recognize that the foregoing description is merely exemplary and is not intended to limit the invention as further set forth in such appended claims. Accordingly, the spirit and scope of the appended claims should not be limited to the illustrative descriptions contained herein.

Claims

1. 1. A method for producing metal molybdate (metal-Mo), comprising: reacting a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition, wherein the liquid medium comprises an aqueous medium; combining the Mo composition with a metal source to obtain a metal-Mo composition; adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo fine particles; controlling the temperature of the aqueous medium by heating the aqueous medium, removing heat from the aqueous medium, or both; and agitating the metallic Mo-99 material and the aqueous medium during at least a portion of the reaction; the metal source comprises a metal, metalate, or metal salt; the metal, metalate, or metal salt forms a bond with another metal, metalate, metal salt, or molybdate; The method, wherein the linkage comprises a cyano, nitro, sulfide, amide nitride, acetate, carbonate, phosphate, carbonyl, or a combination thereof.

2. The method of claim 1 , wherein the first acid comprises a mineral acid.

3. 3. The method of claim 2, wherein the mineral acid is a halogen acid.

4. 4. The method of claim 3, wherein the mineral acid is selected from the group consisting of hydrochloric acid, nitric acid, sulfuric acid, and combinations thereof.

5. 2. The method of claim 1, wherein the step of reacting the metallic Mo-99 material in the liquid medium with the first acid is carried out at a molar ratio of the Mo-99 material to the first acid in the range of 0.1:1 to 10:

1.

6. 10. The method of claim 1, wherein reacting the metallic Mo-99 material in the liquid medium with the first acid subjects the metallic Mo-99 material to oxidation, dissolution, or a combination of oxidation and dissolution.

7. 10. The method of claim 1, wherein reacting the metallic Mo-99 material in the liquid medium with the first acid oxidizes, dissolves, or a combination of oxidizes and dissolves the metal oxide formed from the combination.

8. 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises heating the aqueous medium to above 25°C.

9. 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 80°C.

10. 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 70°C.

11. 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 60°C.

12. 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 50°C.

13. 10. The method of claim 1, wherein controlling the temperature of the aqueous medium comprises maintaining the temperature of the aqueous medium below 40°C.

14. The method of claim 1 , wherein agitating comprises mechanically mixing the metallic Mo-99 material and the aqueous medium.

15. The method of claim 1 , wherein the metal source comprises an element from the p-block, d-block, or f-block of the periodic table.

16. 2. The method of claim 1, wherein the metal source is selected from the group consisting of elemental or non-oxidized metals, metal oxides, metal hydroxides, metal halides, nitrates, phosphates, tetrafluoroborides, phosphorus hexafluoride, tosylates, acetates, formates, any other counter anions capable of forming a soluble salt, and combinations thereof.

17. The metal, metalate or metal salt may be in various oxidation states of M ｎ＋ 2. The method of claim 1 , wherein n=1, 2, 3, 4, 5, or 6.

18. The method of claim 1 , wherein the linkage comprises an oxo bridge, a hydroxo bridge, or a combination thereof.

19. The method of claim 1 , wherein the metal, metalate, or metal salt forms a discrete structural unit or a composite structural unit.

20. The metal, metalate or metal salt is Mo ｘ O ｙ The method of claim 1, wherein x is the number of Mo atoms and y is the number of O atoms.

21. The metal, metalate or metal salt remains unchanged under ionizing radiation and Mo ｘ O ｙ 2. The method of claim 1, wherein x is the number of Mo atoms and y is the number of O atoms.

22. 10. The method of claim 1, wherein the metal, metalate, or metal salt does not produce any daughter products from neutron bombardment that are undesirable in the final eluate.

23. 2. The method of claim 1, wherein the metal source is selected from the group consisting of aluminum, silicon, tin, germanium, zirconium, hafnium, vanadium, chromium, manganese, cobalt, nickel, iron, copper, niobium, rhodium, gadolinium, thorium, cerium, uranium, praseodymium, terbium, and combinations thereof.

24. 2. The method of claim 1, wherein combining the Mo composition and the metal source to obtain the metal-Mo composition comprises adding the metal source to the Mo composition.

25. 25. The method of claim 24, wherein adding the metal source to the Mo composition comprises adding the metal source to the Mo composition in a form selected from the group consisting of droplets, a spray, a mist, and combinations thereof.

26. 10. The method of claim 1, wherein combining the Mo composition and the metal source to obtain the metal-Mo composition further comprises adding a second acid to the Mo composition.

27. 27. The method of claim 26, wherein the second acid comprises a mineral acid.

28. 27. The method of claim 26, wherein the second acid comprises hydrochloric acid.

29. 27. The method of claim 26, wherein adding the second acid occurs simultaneously with adding the metal source to the Mo composition.

30. 10. The method of claim 1, wherein at the end of the step of combining the Mo composition and the metal source, the metal-Mo composition has a final pH of 3 or less.

31. 2. The method of claim 1, wherein the step of adjusting the pH of the metal-Mo composition comprises adding the base to bring the pH to a range of 4 to 9.

32. 10. The method of claim 1, wherein the base for adjusting the pH of the metal-Mo composition comprises ammonium hydroxide.

33. 2. The method of claim 1, wherein the step of adjusting the pH of the metal-Mo composition comprises adding the base dropwise to the metal-Mo composition.

34. 10. The method of claim 1, further comprising the step of cooling the metal-Mo composition during the step of pH adjusting the metal-Mo composition, after the step of pH adjusting the metal-Mo composition, or both.

35. 35. The method of claim 34, wherein the step of cooling the metal-Mo composition comprises lowering the temperature of the metal-Mo composition to between 0°C and 20°C.

36. 35. The method of claim 34, wherein the step of cooling the metal-Mo composition comprises reducing the temperature of the metal-Mo composition to between 3°C and 10°C.

37. The method of claim 1 , further comprising separating the plurality of metal particulates from the liquid medium.

38. 38. The method of claim 37, wherein separating the plurality of said metal-Mo particulates from the liquid medium comprises filtering the metal-Mo composition to retain at least a majority of the plurality of said metal-Mo particulates.

39. 39. The method of claim 38, wherein filtering the metal-Mo composition comprises utilizing a metal filtering surface.

40. 40. The method of claim 39, wherein at least a majority of the plurality of metal-Mo particulates are retained on the metal filtering surface.

41. 38. The method of claim 37, wherein the metal-Mo composition has a temperature of from 0° C. to 20° C. during the step of separating the plurality of metal-Mo particulates from the liquid medium.

42. The method of claim 1 further comprising the step of milling the plurality of metal-Mo particulates.

43. 43. The method of claim 42, wherein the milling step comprises wet milling.

44. 43. The method of claim 42, wherein the plurality of metal-Mo particulates have an average size after milling ranging from 10 microns to 1275 microns.

45. 43. The method of claim 42, wherein the plurality of metal-Mo particulates have an average size after milling ranging from 10 microns to 1015 microns.

46. The method of claim 1 further comprising washing the plurality of metal-Mo particulates with water.

47. The method of claim 1 further comprising the step of drying the plurality of metal-Mo particulates.

48. The method of claim 1 further comprising the step of irradiating the plurality of metal-Mo particulates.

49. 10. The method of claim 1, further comprising irradiating a metallic molybdenum target to obtain said metallic Mo-99 material.

50. 50. The method of claim 49, wherein the molybdenum metal target comprises a plurality of molybdenum metal disks.

51. 50. The method of claim 49, wherein metallic Mo-99 material comprises a plurality of said metallic molybdenum disks, tubular capsule components, or both.

52. 1. A method for producing metal molybdate (metal-Mo), comprising: wholly or partially oxidizing a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo fine particles; The method wherein the metal source is titanium, and the titanium comprises unoxidized titanium metal or a metal carbonyl.

53. 1. A method for producing metal molybdate (metal-Mo), comprising: wholly or partially dissolving a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo fine particles; The method wherein the metal source is titanium, and the titanium comprises unoxidized titanium metal or a metal carbonyl.

54. 1. A method for producing metal molybdate (metal-Mo), comprising: combining a metallic molybdenum-99 (Mo-99) material in a liquid medium with a first acid to obtain a Mo composition; combining the Mo composition with a metal source to obtain a metal-Mo composition; and adjusting the pH of the metal-Mo composition with a base to precipitate a plurality of metal-Mo fine particles; The method wherein the metal source is titanium, and the titanium comprises unoxidized titanium metal or a metal carbonyl.

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