The disclosure pertains to improvements in a gamma radiation source (including radiological and radiographic sources), typically containing low-density alloys or compounds or composites of iridium in mechanically deformable and compressible configurations, for use within a sealed encapsulation, and methods of manufacture thereof.
Improvements in iridium sources have been described in PCT/US2017/033508 entitled “Low Density Spherical Iridium”; PCT/US2017/050425 entitled “Low Density Porous Iridium”; and PCT/US2015/029806 entitled “Device and Method for Enhanced Iridium Gamma Irradiation Sources.” The disclosures of these applications are well-suited to their intended purposes. However, further improvements and refinements are sought.
It is therefore an object of this application to provide improvements and refinement with respect to the above-identified prior art.
Objects of this disclosure include:
1. developing a deformable and/or compressible low density iridium alloy containing 30-85% (volume percentage) Iridium, preferably in the range of 30-70%, more preferably in the range of 40-60%.
2. the alloying constituents ideally or typically should not irradiate to produce other radionuclides that generate interfering gamma rays.
3. the alloying constituents ideally or typically should not have excessively high density or high neutron activation cross-section, which could decrease the activation yield or decrease the source-output yield of Iridium-192.
4. the alloying constituents ideally or typically should produce an alloy that is workable in that the alloy needs to be sufficiently ductile/deformable/compressible whereas pure iridium and most of its alloys are brittle and unworkable; the alloy ideally or typically should preferably have a lower melting point than pure iridium (a melting point less than 2000 degrees Centigrade would be desirable to lower processing costs and simplify thermal technologies); and the alloy ideally or typically should be substantially physicochemically inert (i.e., it does not oxidize/corrode/decompose under conditions of manufacture or use).
The general class of compounds that are predicted to have suitable mechanical and density properties are called L21 Heusler structures. Specifically, these comprise Ir2M1N1, where M and N represent two different metals. Ir2MnAl is described above. Ir2CrAl Is a potential alternative. There may be others, e.g., Ir2Al and Ir2Al11B.
With regard to the L21 Heusler compounds and structures, a range of compounds and structures should be taken into account. It is known that after irradiation of a L21 Heusler compound like Ir2MnAl, it would transmute to Ir2−(x+y)PtxOsyMnAl where “x+y” is the proportion of iridium that transmutes to platinum and osmium. There is typically approximately 10-20% conversion, depending on neutron flux, enrichment, irradiation time and decay lime (burn-up/transmutation) in an irradiation. Iridium-191 (37.3% in natural iridium, approximately 80% in enriched iridium) activates to Iridium-192 of which approximately 95% decays to Platinum-192 and 5% decays to Osmium-192 over the life of the source. Iridium-193 (62.7% in natural iridium, ˜20% in enriched iridium) activates to Iridium-194, which all decays to Platinum-194 in the reactor. In summary, an irradiated disk may contain roughly 5-20% platinum and 0.25-1% osmium after activation, depending on the flux, time and enrichment. It is the post-irradiated alloy that is desired to be ductile, deformable or compressible. The addition of platinum to iridium is likely to increase ductility.
Even if pre-irradiated alloy disks do not have optimum mechanical properties for source manufacture, post-irradiated disks may. Quaternary alloys that contain small amounts of other ingredients, such as, but not limited to, platinum or osmium, or other purposeful additions included before irradiation (such as, but not limited to, chromium) may improve the physicochemical and mechanical properties without activating adversely. Ternary and quaternary alloys are synthesized to account for the conversion of 10-20 atom % of the Iridium to its daughters platinum and osmium in the nuclear reactor. Representative alloys in this regard include Ir1.8 Pt0.2MnAl and Ir1.6 Pt0.4MnAl, also including a very small percentage of osmium. A further representative alloy is Ir3Zr0.25 V0.75.
Similarly, yttrium alloyed with iridium has increased ductility. Stable, natural 89Yttrium activates with very low cross section to form a very small amount of radioactive 90Yttrium, a pure beta emitter with a 64 hour half-life. It is therefore an acceptable metal to co-irradiate with Iridium. It does not produce long term interfering gamma rays. Moreover, 90Y decays to stable zirconium. Yttrium is therefore one of the preferred alloying additives. The most likely composition is IrY (i.e. 50/50-atomic percent alloy), but other ratios of IrxYy may also have increased ductility. Further representative alloys include IrY, Ir0.9 Pt0.1Y, and Ir0.8 Pt0.2Y.
The density of Ir2MnAl is reported or calculated to be 13.89 g/cc vs. 22.56 g/cc for pure iridium (i.e., 61.5%). Further studies may confirm or refine this number. This is slightly higher than optimum for many applications, therefore this alloy may be used for porous or 3-D printed shapes that contain empty spaces, so that the net density may be reduced to the optimum range of 30-85% (preferably in the range of 30-70%, more preferably 40-60%), as illustrated in the various figures of this application. It is also expected that these compounds may have anti-ferromagnetic properties.
These alloys may be formed by mixing powdered elements in molar proportions, e.g. Ir2+Mn+Al and heating—e.g. arc melting or using a high temperature vacuum furnace. As a variant of this basic method, it is expected, under some circumstances, to advantageously first pre-alloy Mn+Al and then mix/process this with pure iridium. MnAl melts at approximately 1500 degrees Centigrade.
Other approaches may include pre-alloying iridium and aluminum and then adding Mn or Mn+Al later. The alloy composition Al7Ir3 (i.e. 30 mol % Iridium) is reported to have a eutectic at approximately 1930 degrees Kelvin (1657 degrees Centigrade).
Reference is made to the article “Antiferromagnetism in γ-Phase Mn—Ir Alloys,” as reported in the Journal of the Physical Society of Japan in 1974, pages 445-450 (Online ISSN: 1347-4073, Print ISSN 0031-9015). This article indicates that antiferromagnetic disordered γ-phase Mn(1−x)Irx (0.05<x<0.35) alloys exists. Mixing an Ir+Mn alloy in this composition range, e.g. Mn7Ir11 powder or granules with Al7Ir3 powder or granules in equimolecular proportions followed by thermal processing (arc melting or furnace) is expected to produce an alloy with a composition of Ir14Mn7Al7 (═Ir2MnAl).
Further objects and advantages of the disclosure will become apparent from the following description and from the accompanying drawings, wherein:
In accordance with the above, the alloy Ir2MnAl forms an embodiment of the present disclosure of a gamma radiation source (including radiological and radiographic sources). It is believed to have ductile properties similar to steel. Additionally, manganese and aluminum are not expected to generate interfering gamma rays after activation by neutron irradiation. Platinum, osmium, chromium or mixtures thereof may likewise be found within the alloy.
This alloy or similar alloys (such as with ternary additions of other non-activating elements) is expected have suitable mechanical properties to make deformable/compressible radiation sources. Although the addition of manganese slightly increases the density with respect to iridium plus aluminum or iridium plus aluminum plus Boron-11, it is expected that the metallurgical properties of Ir2MnAl may offer significant processing advantages.
Iridium manganese copper alloys are also applicable to the present disclosure. These alloys are expected to be ductile and have a melting point significantly below 2000 degrees Centigrade and potentially as low as 1300 degrees Centigrade, depending upon the alloy composition after irradiation. These alloys are disclosed in U.S. Pat. No. 4,406,693 entitled “Method for Refining Contaminated Iridium,” issued on Sep. 27, 1983. However, it is expected that aluminum will be preferable over copper as a tertiary alloying element in most applications.
Yttrium alloyed with indium is likewise a relevant material for the present disclosure.
Furthermore, reduced density may be achieved in some embodiments by the use of porous, microporous or macroporous (i.e., metal foam) forms of the alloy of choice.
All radiation sources are typically designed and expected to be inserted into a sealed encapsulation.
Referring now to
Thus the several aforementioned objects and advantages are most effectively attained. Although preferred embodiments of the invention have been disclosed and described in detail herein, it should be understood that this invention is in no sense limited thereby.
This application claims priority under 35 U.S.C. 119(e) of U.S. provisional application Ser. No. 62/686,748, filed on Jun. 19, 2018, the contents of which is hereby incorporated by reference in its entirety and for all purposes.
Number | Name | Date | Kind |
---|---|---|---|
4406693 | Heshmatpour et al. | Sep 1983 | A |
5840008 | Klein | Nov 1998 | A |
6099458 | Robertson | Aug 2000 | A |
6132359 | Bolenbaugh | Oct 2000 | A |
6248057 | Mavity | Jun 2001 | B1 |
6547816 | O'Foghludha | Apr 2003 | B1 |
6554756 | Schaart | Apr 2003 | B1 |
6689043 | McIntire | Feb 2004 | B1 |
6716156 | Menuhr | Apr 2004 | B2 |
7311655 | Schaart | Dec 2007 | B2 |
8357316 | Munro, III | Jan 2013 | B2 |
9165692 | Finger | Oct 2015 | B2 |
10141080 | Vose | Nov 2018 | B2 |
10607743 | Vose | Mar 2020 | B2 |
10714226 | Vose | Jul 2020 | B2 |
10811156 | Shilton | Oct 2020 | B2 |
20030149329 | O'Foghludha | Aug 2003 | A1 |
20150102238 | Finger et al. | Apr 2015 | A1 |
Number | Date | Country |
---|---|---|
PCTUS2015029806 | May 2015 | WO |
2015105539 | Jul 2015 | WO |
PCTUS201703350 | May 2017 | WO |
PCTUS2017050425 | Sep 2017 | WO |
2019246073 | Dec 2019 | WO |
Entry |
---|
Takashi Yamaoka, “Antiferromagnetism in γ-Phase Mn—Ir Alloys” Journal of the Physical Society of Japan, 1974, pp. 445-450. |
International Search Report issued in PCT/US2020/017601 dated Jul. 17, 2020. |
International Search Report issued in PCT/US2019/037697 dated Sep. 26, 2019. |
V. Raghavan, “Al—B—Ir (Aluminum-Boron-Iridum)”, Journal of Phase Equilibria and Diffusion, vol. 29, No. 1, 2008, p. 42. |
V. Raghavan, “Al—Ir—V (Aluminum-Iridium-Vanadium)”, Journal of Phase Equilibria and Diffusion, vol. 29, No. 4, 2008, p. 372. |
H. Ipser and P. Rogl, “Constitution Diagrams of the Binary Systems Pd—B and Ir—B”, Elsevier Sequoia/Printed in The Netherlands, Metall. Trans. A., 1981, p. 363. |
G. B. Ulrich, “The Metallurgical Integrity of the Frit Vent Assembly Diffusion Bond”, Process Metallurgy Department Development Organization, Jun. 1994, pp. 1-22. |
himikatus.ru, http://www.himikatus.ru/art/phase-diagr1/Al-Ir.php, pp. 1-5. |
Number | Date | Country | |
---|---|---|---|
20200027621 A1 | Jan 2020 | US |
Number | Date | Country | |
---|---|---|---|
62686748 | Jun 2018 | US |