CN117616145A - Uranium-based cermet alloy - Google Patents
Uranium-based cermet alloy Download PDFInfo
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- CN117616145A CN117616145A CN202280032945.4A CN202280032945A CN117616145A CN 117616145 A CN117616145 A CN 117616145A CN 202280032945 A CN202280032945 A CN 202280032945A CN 117616145 A CN117616145 A CN 117616145A
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- 239000000956 alloy Substances 0.000 title claims abstract description 136
- 229910045601 alloy Inorganic materials 0.000 title claims abstract description 135
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 title claims abstract description 59
- 229910052770 Uranium Inorganic materials 0.000 title claims abstract description 58
- 239000011195 cermet Substances 0.000 title claims abstract description 21
- 229910052750 molybdenum Inorganic materials 0.000 claims abstract description 54
- 239000011733 molybdenum Substances 0.000 claims abstract description 52
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims abstract description 46
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 23
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 22
- 239000010703 silicon Substances 0.000 claims abstract description 21
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims abstract description 20
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 20
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 20
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 13
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 12
- 239000011651 chromium Substances 0.000 claims abstract description 12
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 12
- 239000001301 oxygen Substances 0.000 claims abstract description 12
- 229910052726 zirconium Inorganic materials 0.000 claims abstract description 12
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims abstract description 11
- 229910052804 chromium Inorganic materials 0.000 claims abstract description 11
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims abstract description 10
- 229910052758 niobium Inorganic materials 0.000 claims abstract description 10
- 239000010955 niobium Substances 0.000 claims abstract description 10
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims abstract description 10
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000011135 tin Substances 0.000 claims abstract description 8
- 229910052718 tin Inorganic materials 0.000 claims abstract description 8
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052719 titanium Inorganic materials 0.000 claims abstract description 7
- 239000010936 titanium Substances 0.000 claims abstract description 7
- 238000003723 Smelting Methods 0.000 claims description 21
- 238000000265 homogenisation Methods 0.000 claims description 13
- 229910052751 metal Inorganic materials 0.000 claims description 11
- 239000002184 metal Substances 0.000 claims description 11
- 229910001182 Mo alloy Inorganic materials 0.000 claims description 10
- 239000000446 fuel Substances 0.000 abstract description 31
- 239000000919 ceramic Substances 0.000 abstract description 13
- 239000002131 composite material Substances 0.000 abstract description 10
- 239000011159 matrix material Substances 0.000 abstract description 10
- 238000004519 manufacturing process Methods 0.000 abstract description 7
- 239000000463 material Substances 0.000 abstract description 7
- 239000003758 nuclear fuel Substances 0.000 abstract description 6
- 238000011160 research Methods 0.000 abstract description 6
- 229910000831 Steel Inorganic materials 0.000 abstract description 5
- 239000010959 steel Substances 0.000 abstract description 5
- 238000005253 cladding Methods 0.000 abstract description 4
- 239000004411 aluminium Substances 0.000 abstract description 2
- 239000003381 stabilizer Substances 0.000 abstract description 2
- 229910008894 U—Mo Inorganic materials 0.000 abstract 1
- 230000009257 reactivity Effects 0.000 abstract 1
- 238000002844 melting Methods 0.000 description 31
- 230000008018 melting Effects 0.000 description 31
- 239000000203 mixture Substances 0.000 description 17
- 230000005855 radiation Effects 0.000 description 14
- 238000000137 annealing Methods 0.000 description 13
- 239000006104 solid solution Substances 0.000 description 13
- KTEXACXVPZFITO-UHFFFAOYSA-N molybdenum uranium Chemical compound [Mo].[U] KTEXACXVPZFITO-UHFFFAOYSA-N 0.000 description 12
- OOAWCECZEHPMBX-UHFFFAOYSA-N oxygen(2-);uranium(4+) Chemical compound [O-2].[O-2].[U+4] OOAWCECZEHPMBX-UHFFFAOYSA-N 0.000 description 8
- FCTBKIHDJGHPPO-UHFFFAOYSA-N uranium dioxide Inorganic materials O=[U]=O FCTBKIHDJGHPPO-UHFFFAOYSA-N 0.000 description 8
- 238000011835 investigation Methods 0.000 description 7
- 239000010935 stainless steel Substances 0.000 description 7
- 229910001220 stainless steel Inorganic materials 0.000 description 7
- 230000015572 biosynthetic process Effects 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 238000010587 phase diagram Methods 0.000 description 6
- 229910000711 U alloy Inorganic materials 0.000 description 5
- 150000001875 compounds Chemical class 0.000 description 5
- 239000000155 melt Substances 0.000 description 5
- XJAORWFICNKZCM-UHFFFAOYSA-N [U].[C]=O Chemical compound [U].[C]=O XJAORWFICNKZCM-UHFFFAOYSA-N 0.000 description 4
- 238000004458 analytical method Methods 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- 230000006698 induction Effects 0.000 description 4
- 229910000765 intermetallic Inorganic materials 0.000 description 4
- 229910001092 metal group alloy Inorganic materials 0.000 description 4
- 150000002739 metals Chemical class 0.000 description 4
- 230000006641 stabilisation Effects 0.000 description 4
- 238000011105 stabilization Methods 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 229910000476 molybdenum oxide Inorganic materials 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 239000011257 shell material Substances 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- 229910017263 Mo—C Inorganic materials 0.000 description 2
- 229910017305 Mo—Si Inorganic materials 0.000 description 2
- 229910017339 Mo—Sn Inorganic materials 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 238000005266 casting Methods 0.000 description 2
- 239000002826 coolant Substances 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 230000000779 depleting effect Effects 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 239000002019 doping agent Substances 0.000 description 2
- 230000005496 eutectics Effects 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 238000012932 thermodynamic analysis Methods 0.000 description 2
- -1 uranium nitrogen oxides Chemical class 0.000 description 2
- 229910000838 Al alloy Inorganic materials 0.000 description 1
- 229910001295 No alloy Inorganic materials 0.000 description 1
- 229910002796 Si–Al Inorganic materials 0.000 description 1
- PIZYHTQSHRQOBI-UHFFFAOYSA-N [C].O=[N] Chemical compound [C].O=[N] PIZYHTQSHRQOBI-UHFFFAOYSA-N 0.000 description 1
- 238000005275 alloying Methods 0.000 description 1
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical group [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- MVXWAZXVYXTENN-UHFFFAOYSA-N azanylidyneuranium Chemical compound [U]#N MVXWAZXVYXTENN-UHFFFAOYSA-N 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 238000009690 centrifugal atomisation Methods 0.000 description 1
- 230000001427 coherent effect Effects 0.000 description 1
- 230000000295 complement effect Effects 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- PTVDYARBVCBHSL-UHFFFAOYSA-N copper;hydrate Chemical compound O.[Cu] PTVDYARBVCBHSL-UHFFFAOYSA-N 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000004455 differential thermal analysis Methods 0.000 description 1
- 238000010891 electric arc Methods 0.000 description 1
- 238000001493 electron microscopy Methods 0.000 description 1
- JEGUKCSWCFPDGT-UHFFFAOYSA-N h2o hydrate Chemical compound O.O JEGUKCSWCFPDGT-UHFFFAOYSA-N 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 238000003754 machining Methods 0.000 description 1
- 229910002109 metal ceramic alloy Inorganic materials 0.000 description 1
- 239000000078 metal ceramic alloy Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 239000011824 nuclear material Substances 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 238000000399 optical microscopy Methods 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- DECCZIUVGMLHKQ-UHFFFAOYSA-N rhenium tungsten Chemical compound [W].[Re] DECCZIUVGMLHKQ-UHFFFAOYSA-N 0.000 description 1
- 229910021332 silicide Inorganic materials 0.000 description 1
- FVBUAEGBCNSCDD-UHFFFAOYSA-N silicide(4-) Chemical compound [Si-4] FVBUAEGBCNSCDD-UHFFFAOYSA-N 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 238000005728 strengthening Methods 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 230000000699 topical effect Effects 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- JFALSRSLKYAFGM-OIOBTWANSA-N uranium-235 Chemical compound [235U] JFALSRSLKYAFGM-OIOBTWANSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
- G21C3/42—Selection of substances for use as reactor fuel
- G21C3/58—Solid reactor fuel Pellets made of fissile material
- G21C3/60—Metallic fuel; Intermetallic dispersions
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C43/00—Alloys containing radioactive materials
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
- G21C3/42—Selection of substances for use as reactor fuel
- G21C3/58—Solid reactor fuel Pellets made of fissile material
- G21C3/62—Ceramic fuel
- G21C3/64—Ceramic dispersion fuel, e.g. cermet
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Ceramic Engineering (AREA)
- General Engineering & Computer Science (AREA)
- Plasma & Fusion (AREA)
- Dispersion Chemistry (AREA)
- High Energy & Nuclear Physics (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Manufacture Of Alloys Or Alloy Compounds (AREA)
- Manufacture And Refinement Of Metals (AREA)
Abstract
The present invention relates to nuclear engineering, and more particularly to uranium-based cermet alloys and is suitable for use in the manufacture of nuclear fuels for fuel elements of thermal and fast neutron reactors and in the creation of reactors for research. Uranium-based alloys contain 2.5-12wt% molybdenum and a main ceramic phase containing oxygen, carbon or nitrogen in an amount of 0.1-3.0wt% and may be doped with other elements in the form of silicon, tin, chromium or aluminium forming intermetallic phases, and elements as gamma stabilizers, in particular niobium, titanium or zirconium. The claimed uranium-based cermet alloy containing molybdenum and having a composite cermet alloy structure consists of a y- (U-Mo) matrix phase and a ceramic and/or one or more intermetallic phases. The alloy has a low thermal neutron capture cross section and a high liquidus temperature and is compatible with structural materials including steel or aluminum cladding. The thermodynamic stability and reactivity resistance of the alloy are also increased.
Description
Technical Field
The present invention relates to nuclear engineering and can be used as fault tolerant fuel for commercial thermal neutron water-water high energy reactors (VVERs) as well as fast neutron reactors and research reactors in the manufacture of nuclear fuel elements (fuel rods).
Background
Worldwide, international fault tolerant fuel (ATF) development programs are developing metal fuels (cold fuels), in particular uranium disilicide and uranium-molybdenum alloys, which have a higher thermal conductivity than uranium dioxide, which enables the fuel operating temperature to be reduced to 500-600 ℃ [ H.J.Chichester, R.D.Mariani, S.L.Hayes, J.R.Kennedy, A.E.Wright, Y.S.Kim, "Advanced metallic fuel for ultra-high burn-up: irradiation tests in ATR", embedded Topical on Nuclear Fuel and Structural Material, american Nuclear Society, (2012), pp.1349-1351].
The higher uranium content (40-50% higher than uranium dioxide) of metallic (uranium-molybdenum) nuclear fuels also allows to increase the conversion coefficient of the nuclear fuel, reduce its enrichment, extend the fuel rod life and increase the plant capacity utilization coefficient (ICUF), which will ultimately have a positive impact on the fuel recycling economy.
Furthermore, the ATF program assumed the use of stainless steel cladding, which is more resistant to zirconium vapor reaction than zirconium, and has significantly higher capture capacity for thermal neutrons [ S.J.Zinkle, K.A.Terrani, J.C.Gehin, L.J.Ott, L.L.Snead, "Accident tolerant fuels for LWRs: A coherent", journal of Nuclear Materials,448 (2014), pp.374-379]. In order to meet the standard limits of 5% uranium-235 enrichment in manufacturing plants, it is also necessary in this case to use fuels with a higher uranium content. Uranium-molybdenum fuel (OM-9) has been known for VVER type reactors such as the belobino nuclear power plant (Bilibino NPP), AM, the Beloyarsk nuclear power plant (Beloyarsk NPP), but in the form of dispersion fuel [ A.G.Samoilov, A.I.Kashtanov, V.S.Volkov, "Dispersion fuel elements of nuclear reactors", volume 1, mosow: energoizdat,1982, p.295].
However, the use of uranium-molybdenum fuels in VVER reactors is hampered by drawbacks such as: relatively large expansion (which is characteristic of all uranium-based metal alloys), low liquidus temperatures, and high capture of thermal neutrons in U-Mo alloys. In addition, when such fuels are used as fault tolerant fuels (ATF) with stainless steel enclosures, the enclosure may "burn through" in a coolant loss accident (LOCA) because pure uranium forms a low melting eutectic with iron, nickel and chromium.
One known uranium alloy [ patent GB809597, IPC C22C43/00, published in 1959 at 02/25 ] contains 5-15wt% molybdenum and 15-25wt% niobium.
The higher content of molybdenum and niobium in the alloy also stabilizes the gamma-phase structure of uranium, improves the thermodynamic stability of the structure, and increases the liquidus temperature of the alloy to about 1400 ℃.
However, the content of elements absorbing thermal neutrons (molybdenum and niobium) is higher, and the lower uranium content of alloys with such high content of doping elements is significantly reduced (from 15.9g/cm of U-9Mo 3 Down to 8.0-12.4g/cm of the alloy 3 ) Making it unacceptable for use in thermal neutron reactors and not exceeding on average 9.6g/cm uranium content of uranium dioxide 3 。
One known uranium alloy [ patent GB766061, IPC C22C43/00, published on 16/01 in 1957 ] contains 0.1-5wt% molybdenum and 0.1-5wt% silicon.
The alloy has a relatively small thermal neutron capture cross section and has increased radiation resistance due to precipitation of U-Mo-Si intermetallic phases having a lower coefficient of expansion.
However, it has the following drawbacks. At a given amount of molybdenum, the silicon content in the alloy results in the formation of intermetallic phases having a composition of U-9.3Mo-2Si, with a higher molybdenum content than the uranium-based solid gamma-phase solution. Therefore, even at a maximum molybdenum content of 5%, its transformation to intermetallic phases leads to decomposition of the gamma solid solution. The lower molybdenum content results in the formation of an alpha phase with low radiation properties.
At a given molybdenum content, silicon content up to 1.5% lowers the liquidus temperature of the alloy to 1000-1100 ℃ and promotes the formation of co-crystals.
The increase in silicon content reduced the uranium content of the alloy (at 5% Mo and 5% Si, the uranium content of the alloy was 12.9g/cm 3 This is significantly lower than the uranium content (15.9 g/cm 3 )。
Known uranium alloys [ patent GB766060, IPC C22C43/00, published 16 in 01 month 1957 ] contain 6-10wt% molybdenum.
The higher molybdenum content in the alloy further stabilizes the gamma-phase structure of uranium and helps to improve the thermal power of the structureStability in science. The uranium content is not less than 15.0g/cm 3 This makes it promising for use in fuel elements of thermal and fast neutron reactors.
However, it has the following drawbacks.
This alloy with a gamma phase structure has a low liquidus temperature (1250 ℃) which does not meet the requirement of at least 1400 ℃ to exceed the vapor-zirconium reaction temperature of fault tolerant nuclear fuel (ATF). The steam-zirconium reaction starts at about 861℃ and then proceeds very quickly and becomes self-sustaining at 1200℃ [ O.B.Samoilov, G.B.Usynin, A.M.Bakhmetiev, "Safety of nuclear power plants", moscow: energuotomizdat, 1989,280pages ].
It exhibits a significant expansion under irradiation (which is characteristic of all uranium metal alloys), a low thermodynamic stability (6-8% for the lower composition limit), and a relatively large thermal neutron capture (8-10% for the upper composition limit)
As with all similar single-phase gamma solid solution type alloys, the alloy interacts positively with the structural shell and the matrix material (stainless steel and aluminum), which does not allow to improve the compatibility of the materials during reactor operation and in emergency situations.
The closest prior art to the claimed invention is a uranium alloy comprising 2-6wt% molybdenum, 0.1-1.0% aluminium and 0.1-1.0% silicon [ patent DE1151389, IPC C22C43/00; G21C3/60, published in 1963, publication No. 07, month 11 ].
Such alloys have a relatively small thermal neutron capture cross section. The uranium content is not less than 14.9g/cm 3 This makes it promising for use in fuel elements of thermal and fast neutron reactors. It has a high strength and thus a high radiation resistance.
At the same time, its structure comprises a complex combined intermetallic phase U-Mo-Si-Al, which has a higher molybdenum content and reduces the stability of the gamma-phase solid solution, which leads to the formation of the alpha-phase of the radiation-unstable uranium and counteracts the radiation-resistant effect. In order to maintain gamma phase stability at a given aluminum and silicon content, it is necessary to increase the molybdenum content to 10-12%, which leads to an increase in thermal neutron capture.
The alloy has a low liquidus temperature 970-1120 ℃ and promotes the formation of co-crystals.
Although intermetallic phases improve the radiation resistance of metal alloys in part, they are insufficient for use in VVER type reactors in place of ceramic fuels from uranium dioxide, since ceramics are significantly better than intermetallic compounds in terms of radiation resistance. Furthermore, the volume fraction of intermetallic phases in the alloy is low (1-10%).
The low structural content of intermetallic phases comprising aluminum and silicon, which interact positively with the structural materials (steel and aluminum), does not improve the compatibility of the alloy.
Uranium-molybdenum alloys can generally be divided into two groups. The first group of alloys has a low molybdenum content (0.4-4.0%) and an unstable structure, consisting of alpha, alpha' and alpha "phases, and a small amount of gamma phase, which increases at higher molybdenum contents, depending on the molybdenum concentration. They expand strongly under irradiation, deform easily, interact more strongly with the shell material (steel) and the matrix (aluminum alloy), and have a lower corrosion resistance in water. For these reasons, their applicability is limited. Therefore, the alloys commonly used belong to the second group, having a cubic gamma-phase structure and a high molybdenum content (5-10%), which stabilizes these alloys. It should be noted that the stability of the gamma phase can also be achieved by a number of other doping elements: niobium, zirconium and titanium. However, they are less effective than molybdenum and also reduce the uranium content of the alloy to a greater extent.
However, only the upper limit of molybdenum content (9-10%) ensures the relative stability of the gamma phase during fuel manufacture and operation, although this may not be sufficient for complete and balanced stabilization of the gamma phase. Lowering the molybdenum content of the fuel to a lower limit to improve certain properties thereof, such as reducing thermal neutron capture, can result in a loss of structural stability thereof, decay to the alpha phase, and loss of its fundamental radiation properties.
Thus, analysis of known uranium gamma phase alloys used in nuclear reactors has shown that no alloy is currently available that has thermodynamic stability while maintaining low thermal neutron capture, high radiation resistance (low expansion), high liquidus temperature, and compatibility with structural cladding (stainless steel) and matrix materials (aluminum).
Disclosure of Invention
The invention aims to provide a uranium-based alloy with a composite cermet structure composed of a matrix gamma- (U-Mo) phase, a ceramic phase and an intermetallic phase.
The technical effect of the present invention is to provide a gamma-phase cermet uranium-molybdenum alloy which is thermodynamically stable while maintaining low thermal neutron capture, has a higher liquidus temperature and higher radiation resistance (less propensity to expand), and is compatible with structural materials such as steel shells in LOCA-type emergency (VVER-type reactors) and with aluminum matrices (research reactors).
The technical effect is achieved by the following facts: uranium-based cermet alloys contain molybdenum U-Mo-X and additionally contain at least one element X selected from the group consisting of oxygen, carbon and nitrogen, the proportions of the components being as follows (wt%):
2.5 to 12.0 portions of molybdenum;
x is at least one element selected from the group consisting of:
oxygen-0.1-3.0;
carbon-0.1-2.0;
nitrogen-0.1-3.0; and
the balance of uranium.
In a particular embodiment, the uranium-based cermet alloy is characterized in that it further comprises at least one metal Y selected from the group consisting of silicon, tin, chromium, aluminum, niobium, zirconium and titanium, wherein Y is at least one metal (wt%) selected from the group consisting of:
silicon-0.1-3.5;
tin-0.1-3.0;
chromium-0.1-2.0;
0.1 to 1.0 percent of aluminum;
niobium-0.1-5.0;
zirconium-0.1-5.0; and
titanium-0.1-5.0.
The uranium-based cermet alloy is obtained by smelting and then homogenizing annealing.
In order to solve this problem, a completely new alloying method of U-Mo alloy is proposed, which comprises obtaining a composite cermet structure. Which consists of a matrix gamma- (U-Mo) phase and a ceramic and/or intermetallic phase(s) with high radiation resistance and high melting point. These phases have a maximum uranium content and good compatibility with aluminum and do not contain molybdenum, which remains in the structure of the gamma phase to stabilize it.
The main difficulty in doping gamma-U phase alloys, such as U-Mo fuels, is the reduction of the molybdenum content in the gamma- (U-Mo) phase by adding doping elements, especially aluminum, resulting in a reduced stability of the gamma- (U-Mo) phase. The molybdenum fraction from the gamma uranium phase enters the intermetallic phase, depleting the solid solution of gamma phase in terms of molybdenum. This should reduce its stability. To prevent this, thermodynamic analysis using phase diagrams is applied.
Fig. 1 shows a phase diagram pattern of a U-Mo alloy forming a ternary intermetallic compound (U-Mo-Al).
FIG. 2 shows the phase diagram pattern (U-Mo-C isothermal cross section at 1500 ℃) of a U-Mo alloy forming a binary compound.
FIG. 3 shows the appearance of a U-4.2Mo-1.5C alloy ingot according to example 1.
FIG. 4 shows the microstructure of the U-4.2Mo-1.5C alloy after smelting according to example 1.
FIG. 5 shows the microstructure of the U-4.2Mo-1.5C alloy after a homogenization anneal at 1100 ℃ for 4 hours according to example 1.
FIG. 6 shows the microstructure of the U-6Mo-0.5O alloy after smelting according to example 2.
FIG. 7 shows the microstructure of the U-6Mo-0.5O alloy after a homogenization anneal at 800℃for 4 hours according to example 2.
FIG. 8 shows the microstructure of the U-6Mo-0.1C-0.5O-0.1N-0.7Si alloy after melting according to example 4.
FIG. 9 shows the microstructure of the U-10Mo-0.3C-0.1O-0.1Si-0.1Cr alloy after smelting according to example 5.
FIG. 10 shows the microstructure of the U-10Mo-0.3C-0.1O-0.1Si-0.1Cr alloy after a homogenization anneal at 1000℃for 3 hours according to example 5.
FIG. 11 shows the microstructure-3 of the U-3Mo-3.0C-3.0O-1.0Si-3.1Nb-0.3Ti alloy after smelting according to example 6.
FIG. 12 shows the microstructure of the U-3Mo-3.0C-3.0O-1.0Si-3.1Nb-0.3Ti alloy after a homogenization anneal at 1050 ℃ for 2 hours in accordance with example 6.
FIG. 13 shows the microstructure of the U-7Mo-0.1O-2.0Si-0.3Cr-0.5Zr alloy after melting according to example 7.
FIG. 14 shows the microstructure of the U-4.5Mo-0.4O-0.4Si-0.4Al-0.5Sn alloy after melting according to example 8.
When doping a U-Mo alloy with elements that form intermetallic compounds with uranium, the method in fig. 1 shows an undesirable phase diagram pattern, as molybdenum enters the resulting ternary intermetallic phase, depleting the U-Mo gamma solid solution and causing its partial decomposition. Such results are observed, for example, in ternary systems of U-Mo-Al, U-Mo-Sn.
In order to prevent molybdenum from entering the intermetallic phase and to remain in solid solution with uranium, it is necessary to implement the phase diagram pattern shown in fig. 2.
In FIG. 2, the phase triangle is formed by three phases U-U 2 Mo-U.psi, wherein U.psi is a binary intermetallic compound of uranium and the doping element psi. Such an embodiment is possible in U-Mo-C systems, wherein, theoretically, no ternary compounds should be formed near the uranium angle of the phase diagram. A similar effect should occur when the following elements are added to a U-Mo system: nitrogen and oxygen, which may also be added in combination, because they form complex uranium nitrogen oxides, wherein the thermodynamic presence of molybdenum is unlikely. With sufficient amounts of these phases, the thermodynamic equilibrium is not affected by the addition of small amounts of silicon.
The uranium-based ceramic-metal alloy containing molybdenum of the present invention is characterized by the fact that when the alloy is doped with at least one doping element X selected from the group consisting of oxygen, carbon and nitrogen, they do not enter into a solid solution of uranium gamma phase, but form a ceramic phase in the matrix separated from the U-Mo gamma solid solution, thereby forming a composite structure having improved properties compared to the matrix solid solution, as with all composite materials. But most importantly, the proposed dopants do not form undesirable ternary compounds such as U-Mo-Al, U-Mo-Sn, U-Mo-Si, U-Mo-Cr, etc. Such compounds, alone, are formed from common uranium dopants such as aluminum, tin, silicon, chromium, and the like. Thus, by introducing oxygen, carbon, nitrogen, we can maintain thermodynamic stability of the gamma phase at much lower molybdenum content by increasing the liquidus temperature of the alloy, and further improve the neutron properties of such reactors by reducing the thermal neutron capture cross section of the doping element.
The ceramic phase in the gamma solid solution structure of uranium has significantly better radiation resistance and less expansion due to stronger interatomic bonds [ A.S.Zaimovskiy, V.V.Kalashnikov, I.S.Golovnin, "Fuel elements of nuclear reactors", moscow: atom izdat,1966]. Which in turn determines the melting point value. Table 1 shows the main phases formed in the proposed cermet alloys and their melting points.
TABLE 1 ceramic and intermetallic phases formed in multicomponent doped U-Mo alloys and some properties thereof
The presence of refractory compounds in the alloy structure significantly increases the liquidus temperature of the alloy, which determines the thermodynamic stability of the fuel in the event of a LOCA type emergency in a VVER type reactor. For cermet alloys, the liquidus temperature of undoped uranium-molybdenum alloys increases from 1230-1270deg.C to 1400-1800 deg.C (see Table 2). Table 2 shows the liquidus temperatures of the U-Mo alloys and sintered alloys with various doping elements.
TABLE 2 liquidus temperatures of U-Mo alloys and sintered alloys with various doping elements
| Alloy and phase | Liquidus temperature, DEG C |
| U-Mo alloy (7-10% Mo) | 1230-1270 |
| Second phase: | |
| UO 2 | 1480-1800 |
| UO (stabilized with C, N or O) | 1430-1700 |
| UC | 1400-1730 |
| UN | 1430-1800 |
| U(C、N、O、Si) | 1420-1750 |
| UO 2 +U 3 Si 2 | 1400-1670 |
| UO 2 +UAl 2 | 1400-1690 |
Uranium alloys having a ceramic phase but no molybdenum (UO) compared to uranium-molybdenum alloys not having a ceramic phase 2 UC, UN, etc.) exhibit particular properties with respect to structural materialsIs highly compatible with stainless steel housings and with aluminum substrates. U-Mo alloys are known to have "burned through" stainless steel fuel cladding [ A.S.Zaimovskiy, V.V.Kalashnikov, I.S.Golovnin, "Fuel elements of nuclear reactors," Moscow: atomizdat,1966, at 850 ℃ due to the formation of low melting eutectic with uranium]。
At the same time, this limits the operating temperature of the fuel elements of a fast neutron reactor with metal fuel. In the claimed alloy, the initial temperature of the alloy to stainless steel interaction is raised to 1030-1300 c (see table 3) due to the presence of chemically inert phases in the structure and strengthening of the interatomic bonds.
Metals such as niobium, titanium, zirconium that stabilize U-Mo gamma solid solutions may also be added to the U-Mo cermet alloys of the present invention to further stabilize the gamma phase.
As a complement to the main doping element, small amounts of other doping metals (silicon, tin, chromium, aluminum) form further intermetallic phases, which improve the radiation resistance.
Molybdenum contents below 2.5% can lead to thermodynamic instability of the alloy structure and initiate decay of the gamma uranium phase. Molybdenum contents exceeding 12% increase undesirable thermal neutron capture and reduce the uranium content of the alloy.
The content of the elements carbon, oxygen, nitrogen forming the ceramic phase of less than 0.1% is slightly effective in improving the above properties.
Oxygen and nitrogen contents exceeding 3% and carbon contents exceeding 2% reduce the uranium content of the alloy and further lead to reduced ductility due to a reduced volume fraction of plastic γuranium phase in the alloy structure. This results in difficulties in the process of manufacturing alloys by casting, in the machining of alloys and in the manufacture of sheets, and in the manufacture of particles from alloys by centrifugal atomization.
Metals such as niobium, titanium, zirconium that stabilize U-Mo gamma solid solutions have a content below 0.1% do not practically affect the stabilization of the gamma phase, whereas their content exceeding 5% reduces the uranium content of the alloy.
Metals such as silicon, aluminum, tin, chromium, which form additional intermetallic phases in the alloy, have little effect below 0.1%.
The silicon content is over 3.5%, the tin content is over 3%, the chromium content is over 2%, and the aluminum content is over 1%, which reduces the uranium content of the alloy.
The alloy is smelted in an induction vacuum furnace or an arc furnace. Homogenizing and annealing at 800-1150 deg.c for 0.5-4 hr. The homogenizing annealing contributes to further stabilization of the gamma phase, achieving an equilibrium state of the alloy and a higher density of the alloy.
The study of microstructure, differential Thermodynamic Analysis (DTA) and phase analysis was performed both after melting and after homogenization annealing.
Detailed Description
Example 1.Alloy composition U-4.2Mo-1.5C was produced by arc melting.
Smelting was performed in a small electric arc furnace MIFI-9 under argon in a copper water cooled mold using multiple (4 or 5 weight) smelting with non-consumable tungsten electrodes.
The charge used consisted of a U-2Mo alloy billet, molybdenum in plate form and graphite powder.
Fig. 3 shows the appearance of the ingot. After smelting, the ingot was cut for metallographic investigation.
After smelting, at 10 in a CYD furnace -5 A further homogenization anneal was performed at 1100℃for 4 hours under a vacuum of mmHg.
Research is carried out on fuel uranium-molybdenum alloy materials. The microstructure of the as-cast and homogenized annealed alloy was studied using optical and electron microscopy. The alloy microstructure after melting is shown in fig. 4, and the alloy microstructure after annealing is shown in fig. 5.
The liquidus temperature of the alloy was determined by Differential Thermal Analysis (DTA) at a heating and cooling rate of 20 degrees/min.
X-ray phase analysis was performed on a DRON-3 universal diffractometer using monochromatic CuK beta radiation at a wavelength of 0.1393nm by continuous scanning at a rate of 1 degree/min.
After the homogenization annealing, further stabilization of the alloy structure occurs, as indicated by an increase in alloy density of 0.5-1.5%.
Phase analysis shows that the structure of the alloy only comprises two main components of uranium-based gamma solid solution and uranium carbide, which confirms our thermodynamic calculation. Oxide inclusions are also present. It should be noted that although a small amount of molybdenum (4.2%) was used as the gamma stabilizer, no trace of gamma-phase decomposition was found in the alloy structure. The liquidus temperature of the alloy was 1470 ℃. Whereas in the U-4.2Mo alloy (undoped 1.5% C), the main phases are alpha 'and alpha', and only a small amount of gamma phase is present.
Table 3 shows the properties of the U-4.2Mo-1.5C alloy.
Example 2.Alloy composition U-6Mo-0.5O (see example 1) was produced by arc melting. Oxygen in the form of uranium dioxide particles and molybdenum oxide (MoO) having a low melting point 3 ) Is introduced in the form of (c).
After smelting, the ingot was cut for metallographic investigation. Fig. 6 shows the microstructure of the alloy after melting, and fig. 7 shows the microstructure of the alloy after homogenizing annealing at 800 ℃ for 4 hours.
The study was performed as described in example 1.
The structure of the alloy consists of two phases: uranium-molybdenum gamma phase and uranium dioxide. The liquidus temperature of the alloy was 1470 ℃. Table 3 shows other properties of the alloy.
Example 3.Alloy composition U-3.5Mo-2.0N (see example 1) was produced by arc melting. Nitrogen is introduced into the atmosphere of the furnace and absorbed by the melt. After smelting, the ingot was cut for metallographic investigation. The study was performed as described in example 1.
After melting, a homogenization anneal was performed at 1150 ℃ for 0.5 hours.
The alloy structure is composed of three phases: gamma-uranium-molybdenum phase, gamma 0 -uranium-molybdenum phase and uranium nitride. Table 3 shows other properties of the alloy.
Example 4.The alloy compositions U-6Mo-0.1C-0.5O-0.1N-0.7Si (see example 1) were produced by arc melting. Oxygen is oxidized with molybdenum (MoO) 3 ) Is introduced into the mixture. Carbon is introduced into the mixture in the form of graphite powder. Silicon is added to the mixture in the form of a chunk. Nitrogen is introduced into the atmosphere of the furnace and absorbed by the melt. After smelting, cutting the cast ingot for metallographic research. Fig. 8 shows the microstructure of the alloy after melting.
The study was performed as described in example 1.
After melting, homogenization annealing was performed at 950 ℃ for 2.5 hours.
The structure of the alloy consists of a composite phase of a gamma-uranium-molybdenum phase and a carbon-nitrogen oxide of uranium, the composite phase also comprising silicon. Small amounts of uranium silicide were also found. No trace of gamma-phase decay was found. Table 3 shows other properties of the alloy.
Example 5.Alloy compositions U-10Mo-0.3C-0.1O-0.1Si-0.1Cr (see example 1) were produced by arc melting. Molybdenum, oxygen, carbon and silicon were added to the mixture as in example 4. Chromium is added to the mixture in the form of a block.
After smelting, the ingot was cut for metallographic investigation. The study was performed as described in example 1.
After melting, homogenizing annealing was performed at 1000℃for 3 hours.
The microstructure of the alloy after melting is shown in fig. 9 and the microstructure of the alloy after homogenizing annealing is shown in fig. 10.
The structure of the alloy consists of a gamma-uranium-molybdenum phase and a composite phase of uranium carbon oxide, and the composite phase also comprises silicon. No trace of gamma-phase decay was found. Table 3 shows other properties of the alloy.
Example 6.The alloy composition U-3Mo-3.0C-3.0O-1.0Si-3.1Nb-0.3Ti was produced by arc melting.
After smelting, the ingot was cut for metallographic investigation. The study was performed as described in example 1.
After melting, homogenization annealing was performed at 1050 ℃ for 2 hours.
The microstructure of the alloy after melting is shown in fig. 11, and the microstructure of the alloy after homogenizing annealing is shown in fig. 12.
The alloy has a very complex structure and mainly consists of uranium carbon oxide, uranium carbide, uranium dioxide and gamma-uranium-molybdenum phases. No trace of gamma-phase decay was found. Table 3 shows other properties of the alloy.
Example 7.Alloy compositions U-7Mo-0.1O-0.3C-2.0Si-0.3Cr-0.5Zr were produced by induction melting.
Induction melting at 1.10 -3 Performed under vacuum at mmHg. High density graphite grade ARVs are used as materials for smelting and casting tool operations. The starting materials for the charge are uranium, molybdenum and silicon, uranium dioxide particles, chromium and zirconium. Molybdenum in plate form and other alloy components in block form are placed at the bottom of the melting crucible. During smelting, the temperature of the melt is controlled by an immersed thermocouple.
The melt temperature was 1550 ℃ when the metal was poured into the mold. Temperature control was performed using a tungsten rhenium thermocouple. The melt was poured into a graphite mold. The finished alloy ingot is a bar with a diameter of 31 to 32mm and a length of 200 to 250 mm. The weight of the ingot was about 2kg.
The study was performed as described in example 1. After smelting, the ingot was cut for metallographic investigation. Fig. 13 shows the alloy microstructure after smelting.
After melting, a homogenization anneal was performed at 900 ℃ for 3.5 hours.
The alloy structure mainly comprises gamma-uranium-molybdenum phase, uranium carbon oxide and uranium disilicide distributed along grain boundary. No trace of gamma-phase decay was found. Table 3 shows other properties of the alloy.
Example 8.Alloy compositions U-4.5Mo-0.4O-0.4Si-0.4Al-0.5Sn were produced by induction melting (see example 7).
The study was performed as described in example 1. After smelting, the ingot was cut for metallographic investigation. Fig. 14 shows the alloy microstructure after smelting.
After melting, homogenization annealing was performed at 850 ℃ for 4 hours.
The alloy structure mainly comprises gamma-uranium-molybdenum phase, uranium carbon oxide and metastable gamma 0 Phase composition. A small amount of UAl is also detected 2 And U 5 Sn 4 Phase precipitates. Table 3 shows other properties of the alloy.
Industrial applicability
Table 3 shows the main properties of the alloyed uranium-molybdenum alloys as claimed in examples 1-8 compared to metallic uranium-molybdenum simulated alloys.
TABLE 3 Properties of the Metal-ceramic alloys according to examples 1-8
Thus, the claimed uranium-based cermet alloy comprising molybdenum has unique characteristics in terms of the form of the composite cermet structure of the alloy compared to the prior art alloys, consisting of a matrix gamma- (U-Mo) phase and a ceramic and/or one or more intermetallic phases, ensuring the following technical effects are achieved: providing an alloy that maintains low thermal neutron capture, higher liquidus temperature, higher radiation resistance (lower propensity to expand), and compatibility with the following structural materials while having thermodynamic stability: steel shell and aluminum matrix (research reactor) in the event of loss of coolant.
Claims (3)
1. Uranium-based cermet molybdenum alloy U-Mo-X, characterized in that it additionally comprises at least one element X selected from the group consisting of oxygen, carbon and nitrogen, the proportions of the components being as follows (wt%):
2.5 to 12.0 portions of molybdenum;
x is at least one element selected from the group consisting of:
oxygen 0.1-3.0;
0.1 to 2.0 carbon;
nitrogen 0.1-3.0; and
the balance of uranium.
2. Uranium-based cermet alloy according to claim 1, characterized in that the uranium-based cermet molybdenum alloy additionally comprises at least one Y metal selected from the group consisting of silicon, tin, chromium, aluminum, niobium, zirconium, titanium, wherein Y is at least one metal (wt%) selected from the group consisting of:
0.1 to 3.5 percent of silicon;
0.1 to 3.0 portions of tin;
0.1 to 2.0 portions of chromium;
0.1 to 1.0 percent of aluminum;
niobium 0.1-5.0;
zirconium 0.1-5.0; and
titanium 0.1-5.0.
3. Uranium-based cermet alloy according to any of claims 1 and 2, characterized in that the uranium-based cermet molybdenum alloy is obtained by smelting followed by a homogenization anneal.
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| NL207549A (en) * | 1955-06-14 | |||
| BE589678A (en) * | 1959-04-14 | 1960-08-01 | Atomic Energy Commission | Uranium-based alloy that can be used in a nuclear reactor. |
| RU2154312C1 (en) * | 1999-02-16 | 2000-08-10 | Государственный научный центр Российской Федерации Всероссийский научно-исследовательский институт неорганических материалов им. академика А.А. Бочвара | Nuclear reactor fuel element |
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