Manufacturing of a fissionable element metal alloy target.
Technical field
The present invention relates to a method for manufacturing a fissionable metal alloy target comprising a core and an enclosure, a use of a tungsten electrode in the manufacturing of such a target and a tungsten electrode.
Prior art
The most common technique for the production of the fission product 99Mo (molybdenum 99) is the neutron irradiation of metallic targets (e.g. UA1X-A1), sometimes embodied as fuel plates, in a nuclear reactor. After the neutron irradiation the targets are dissolved within approximately 24 hours, after which the "Mo is removed and purified from the dissolved material. 99Mo has a half-life of 66 hours. The "Mo is a source that decays to 99Tc (Technetium 99), which is mainly used for medical applications, must be sufficiently pure in order to have an appropriate quality for medical injection. One of the chemical elements that is rather difficult to be removed from the "Mo is tungsten. Tungsten is not a fission product but typically can be induced as impurity in the 99Mo, since tungsten impurity can be present in the target already at the start of the irradiation. Tungsten has several stable isotopes. The isotope W can absorb a neutron and becomes W, which has a half-life of 24 hours. W has a rather high abundance in natural tungsten (about 28 atomic%) and a rather high neutron absorption cross section for thermal neutrons (about 37 barn). This makes that natural tungsten impurities induce a significant amount of 187W during neutron irradiation. Also other radioactive tungsten radioisotopes can be formed due to neutron absorption of natural tungsten impurities, but these radioisotopes have a much smaller abundance and thereby a smaller radiological impact.
It is therefore an object of the present invention to provide a method that overcomes one or more of the disadvantages from the prior art.
Summary of the invention
The object is achieved by a method as defined in claim 1, for manufacturing a fissionable element metal alloy target comprising a core and an enclosure, wherein the core is enveloped by the enclosure; the core material being a composite comprising an alloy of a fissionable element and at least one second element, and a further element; the method comprising: collecting the material of the fissionable element and the material of the second element in a volume; melting the collected materials by applying heat supplied by an electric arc from a tungsten electrode to form and solidify an alloy of the fissionable element and the at least one second element, wherein the tungsten electrode consists of W depleted tungsten, the depletion being relative to the natural abundance of 186W in tungsten.
The tungsten in the metal alloy in the target originates from either impurities present in the fissionable and second element material from which the metal alloy target is formed or from impurities that enter into the metal alloy target from the manufacturing process. The material batches that are used for the fissionable and second element material are chosen such as to have a low amount of impurities, especially tungsten impurities. In this respect the melting and alloying of the fissionable and second element materials by exposing to a material that contains tungsten results in contamination of the materials by tungsten.
In particular, supplying heat from an electron arc created by a tungsten electrode, e.g. a tungsten inert gas electrode (TIG), to the metallic materials is a source for tungsten impurities in the alloy. The exposure of the tungsten electrode to the electric field, the electron arc and the associated discharge plasma causes a release of tungsten particles or vapor that can enter into the metal alloy target during the melting of the constituent materials. Typically, the release of tungsten is substantially independent on the isotope, which has the result that impurities in the metal alloy will have substantially the same isotope composition as the isotope composition of the tungsten electrode.
By reducing the relative abundance of the detrimental 186W in the tungsten electrode, the amount of the 186W in the tungsten impurity in the metal alloy and the metal alloy fuel plate will accordingly be reduced. As an advantage, during neutron irradiation, the creation of 187W as impurity will be less due to the reduction of the relative abundance of 186W in the tungsten impurity in the metal alloy target as caused by the TIG melting process.
Also, exposure of the materials to other tungsten-based tools for example in the form of a tungsten crucible during the manufacturing process can add tungsten impurities. According to the invention, such tungsten-based tools can also be made of 186W depleted tungsten, the depletion being relative to the natural abundance of 186W in tungsten.
The method can be used for uranium or any other fissionable element when the method involves melting of the collected materials by a tungsten based electrode.
According to an aspect, the present invention provides a method as described above that further comprises the step of forming an alloy powder from the solidified alloy of the fissionable element and the second element; mixing the alloy powder with powder of the further element to form to a powder mixture of the alloy and the further element; and pressing the powder mixture to form the core.
According to an aspect, the present invention provides a method as described above that further comprises: providing a first and a second plate of enclosure material; creating a layered stack of the first plate, the second plate and the core, with the core being arranged between the first and second plates; rolling the layered stack to form a fissionable element metal alloy target.
According to an aspect, the present invention provides a method as described above wherein the second element is one selected from aluminum and silicon, the further element is aluminum, and the enclosure material is one selected from a group comprising aluminum, aluminum alloy, zirconium and Zr alloy.
Thus, in case the fissionable element is uranium, the alloy of the fissionable element and the second element maybe an uranium -aluminium compound (denoted UA1X) or an uranium-silicon alloy (denoted here as USi). Such an alloy is manufactured by a melting process that involves a tungsten inert gas electric arc heating and possibly exposure to other tungsten based tools such as a crucible. Said alloy is then mixed with pure A1 as further element to form an alloy compound - A1 material (for example UA1X-A1 or USi-Al).
The enclosure material can be a pure aluminum but alternatively an aluminum alloy with low content of alloying elements as for instance Mg and/or Si can be used. Alternatively, the enclosure material can be zirconium or a zirconium alloy.
According to an aspect, the present invention provides a method as described above, wherein the compound material comprises a trace amount of tungsten, the trace amount of tungsten originating from the tungsten electrode being depleted in 186W relative to the natural abundance of 186W in tungsten.
According to an aspect, the present invention provides a method as described above, comprising: the step of creating 186W depleted tungsten by means of an isotope enrichment process that reduces the amount of 186W relative to its natural abundance in tungsten.
According to an aspect, the present invention provides a method as described above, wherein the solid tungsten material of the electrode depleted in 186W isotope has an abundance of elemental 186W in tungsten being less than 20% at%.
According to an aspect, the present invention provides a method as described above, wherein the solid tungsten material of the electrode depleted in 186W isotope has an abundance of elemental 186W in tungsten being less than 10% at%.
According to an aspect, the present invention provides a method as described above, wherein the solid tungsten material of the electrode depleted in 186W isotope has an abundance of elemental W in tungsten being less than 5% at%.
According to an aspect, the present invention provides a method as described above, wherein the trace amount of tungsten in the compound material has an abundance of elemental 186W in tungsten being less than 20 at%, preferably less than 10 at%, more preferably less than 5% at%.
According to an aspect, the present invention provides a method as described above, that further comprises creating a tungsten electrode depleted in 186W from the 186W depleted tungsten solid material.
According to an aspect, the present invention provides a method as described above, that further comprises the step of adding one or more high temperature oxides to the 186W depleted tungsten before creating the tungsten electrode.
Additionally, the present invention relates to a use of a tungsten electrode in the manufacturing of a fissionable element metal alloy target as described above, with the tungsten electrode being arranged for melting the fissionable element and a second element to form an alloy of the fissionable element and the second element by tungsten inert gas electric arc heating, wherein the tungsten electrode consists of 186W depleted tungsten, the depletion being relative to the natural abundance of 186W in tungsten.
Also, the present invention relates to a fissionable element-based metal (uranium or other fissionable element) target comprising a layered stack of a first layer of a enclosure material, a second layer of the enclosure material, and a fissionable element-based core compound of an alloy of the fissionable element and at least one second element with a further element, the fissionable element-based core compound material being arranged between the first and second layers of the enclosure material, wherein the core material comprises a trace amount of tungsten, the trace amount of tungsten being depleted in 186W relative to the natural abundance of 186W in tungsten.
Moreover, the present invention relates to a tungsten electrode for an electric arc heating device, the electrode material comprising 186W depleted tungsten, the depletion being relative to the natural abundance of 186W in tungsten.
Furthermore, the present invention relates to a tungsten based tool for use in the manufacturing of a fissionable element-based core compound of an alloy of the fissionable element and a second element with a further element, wherein the tungsten-based tool comprises 186W depleted tungsten, the depletion being relative to the natural abundance of 186W in tungsten.
The tool can be selected from a group comprising an electric arc electrode and a crucible.
Advantageous embodiments are further defined by the dependent claims.
Brief description of drawings
The invention will be explained in more detail below with reference to drawings in which illustrative embodiments of the invention are shown.
The drawings are intended for illustration purposes only without limitation of the scope of protection, which is defined by the subject matter of the appended claims.
Figure 1 shows a process flow for manufacturing a fissionable element metal alloy target according to an embodiment of the invention.
Description of embodiments
Figure 1 shows a process flow for manufacturing a fissionable element metal alloy target according to an embodiment of the invention. A fissionable element metal alloy target is typically used in nuclear reactors to form fission products by irradiation with neutrons.
Such fission products are radio-isotopes of which some can be useful, i.e., radioactive isotopes that decay to stable isotopes and that can be used for radiation based applications, such as radiography (imaging), radiotherapy and radiopharmaceuti cal appli cations.
An example of a radiopharmaceutical application is the creation of "Mo that decays to 99mTc for application in a living being. The 99Mo isotope is created as a fission product by irradiating a fissionable element (e.g. uranium) metal alloy target (e.g., UA1X-A1) by neutrons.
As mentioned in the introductory part, if the uranium target contains tungsten then also radioisotopes of tungsten will be created. Chemically separating molybdenum from tungsten is known to be difficult. Separating tungsten from molybdenum may require an additional processing step in the "Mo production process, causing additional costs and delay. As a result, when "Mo is chemically released from the metal alloy fuel plate, the obtained "Mo product will contain also tungsten impurities that may be radioactive isotopes. In particular, W may have a detrimental impact on radiological application of "Mo and it’s daughter products.
In the process flow 100 of figure 1, the preparation of a metal alloy fuel target is described in which the contamination of the 99Mo product by 187W is significantly reduced.
Process flow 100 comprises after some initial steps a first step 102 of preparation of a mixture of a fissionable element and a second element. In an embodiment the fissionable element is uranium or an other fissionable element, the second element is aluminum or silicon. As mentioned above, silicon can be chosen as the second element. Optionally, the second element could be a mixture of A1 and Si.
The fissionable element and the second element(s) are collected in a volume, such as a crucible.
Next in step 104, the mixture of the fissionable element and the second element(s) is melted using a tungsten electrode as heat source in a tungsten inert gas electric arc. Between the tungsten electrode and the mixture of the metals a high electric potential is generated, which creates an electric discharge (electric arc) between the electrode and the mixture of the metals. The tungsten electrode is surrounded by flowing inert gas. The electric discharge is accompanied by a release of heat that causes the mixture of metals to melt and form a compound material or alloy of the fissionable element and the second element(s).
In case of uranium as fissionable element and aluminum as second element a UA1X alloy is formed.
An alternative compound may comprise uranium and silicon for forming an USi alloy.
Subsequently the alloy material is then solidified. The alloy material is thereafter crushed, ground and sieved, thereby obtaining UA1X powder. The powder is inspected and thereafter mixed with aluminium powder. This mixture is homogenized and inspected. Thereafter core pressing or rolling of the UA1X -A1 mixture takes place to create the fuel core.
In subsequent step 106, the core material is then machined into a shape of a plate.
In next step 108, the core material plate is arranged into an metallic enclosure by e.g. sandwiching between two plates of a third element for example, aluminum or A1 alloy or zirconium or zirconium alloy. The stack of the plates is rolled (hot rolled) to form a uranium metal alloy target e.g., a target comprising a core of UA1X-A1 enclosed within two A1 (alloy) plates or Zr (alloy) plates.
In case of uranium as first metal, aluminum as second metal and aluminium as a further metal, the metal alloy target comprises a stack of a first outer layer of aluminum, an intermediate layer of UA1X-A1 core and a second outer layer of aluminum, if aluminum is used as enclosing material.
If zirconium (alloy) is used as layer material, the metal alloy fuel plate comprises a stack of a first outer layer of zirconium (alloy), an intermediate layer of UA1X-A1 and a second outer layer of zirconium (alloy).
The metal alloy target can be further processed as will be described in more detail below.
With reference to the step 104 of melting the mixture of first and second metals it is noted that the tungsten electrode comprises tungsten that is depleted in 186W relative to the natural abundance of 186W in tungsten.
During the tungsten inert gas electric arc heating, some tungsten particles or tungsten vapor will be released from the tungsten electrode and enter the melted compound material as an impurity or trace amount. Thus the compound material will comprise a trace amount of tungsten. Since the release of tungsten during operation of the tungsten electrode is substantially independent of the isotope number, the trace amount of tungsten that is added to the uranium compound material during the tungsten inert gas heating will have a substantially same isotope composition as the tungsten electrode. Thus, if the electrode comprises tungsten that is 186W depleted relative to the natural abundance of 186W in tungsten, then the trace amount of W originating from the tungsten electrode in the compound material will show a 186W depleted isotope composition.
The 186W depleted tungsten electrode can be manufactured according to the steps 200 - 206.
In step 200, a tungsten source material is provided with a given abundance of 186W. Typically, the tungsten source material will be a tungsten source with natural abundance of 186W.
In step 202, the tungsten source material is converted in an isotopic enrichment process into a raw 186W depleted tungsten material. The isotopic enrichment process could be based on an isotopic separation process for a gaseous tungsten compound such as tungsten-hexafluoride WF6.
In step 204, from the raw 186W depleted tungsten material a 186W depleted tungsten electrode is fabricated using a method known in the art.
As known to a person skilled in the art, the 186W depleted tungsten electrode may comprise one or more additives such as a high temperature oxide (e.g., a rare-earth oxide such as Lanthanum oxide) that improves the mechanical stability of the 186W depleted tungsten electrode during high temperature operation.
The natural abundance of 186W in tungsten is about 28.4 at.%. According to the invention, the abundance of 186W in tungsten of the 186W depleted tungsten electrode is about 20 at% or less, preferably about 10 at.% or less, more preferably the abundance of 186W in tungsten of the 186W depleted tungsten electrode is about 5 at.% or less.
The metal alloy target manufactured according to the invention, and that comprises the trace amount of tungsten depleted in 186W can be used in a nuclear reactor (not shown) for creation of fission product from uranium by neutron irradiation.
The tungsten impurity in the metal alloy can form tungsten radioisotopes during the neutron irradiation. However, due to the 186W depletion in comparison to the natural abundance, the amount of 187W in the irradiated uranium metal alloy will be proportionally reduced.
After irradiation, the metal alloy target can be dissolved and radioisotopes such as 99Mo can be isolated chemically. Since separation of Mo from W is difficult, the problem of contamination of "Mo by 187W is reduced if the tungsten impurity in the metal alloy was depleted in 186W.
In particular for radiopharmaceutical applications of "Mo, the use of 186W depleted tungsten as electrode in the melting process of the fissionable element and the second element(s) is beneficial.
The skilled in the art will appreciate that the release of tungsten into the uranium-metal alloy may also originate from other tungsten-based tools such as a crucible. In accordance with an embodiment of the invention, such tungsten based tools can be manufactured from 186W depleted tungsten material in similar manner as described above for a 186W depleted tungsten electrode.
The invention has been described with reference to the preferred embodiment. Obvious modifications and alterations will occur to others upon reading and understanding the preceding detailed description. It is intended that the invention be construed as including all such modifications and alterations insofar as they come within the scope of the appended claims.