US3188202A - Aluminum-plutonium alloys - Google Patents

Aluminum-plutonium alloys Download PDF

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US3188202A
US3188202A US104183A US10418361A US3188202A US 3188202 A US3188202 A US 3188202A US 104183 A US104183 A US 104183A US 10418361 A US10418361 A US 10418361A US 3188202 A US3188202 A US 3188202A
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percent
alloy
alloys
aluminum
plutonium
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US104183A
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Jones Thomas Ivor
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Atomic Energy of Canada Ltd AECL
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Atomic Energy of Canada Ltd AECL
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Priority to US104183A priority patent/US3188202A/en
Priority to GB10697/62A priority patent/GB934544A/en
Priority to DEA39942A priority patent/DE1252905B/en
Priority to FR894581A priority patent/FR1319838A/en
Priority to NL6503035A priority patent/NL6503035A/xx
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C21/00—Alloys based on aluminium
    • C22C21/02—Alloys based on aluminium with silicon as the next major constituent
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C21/00—Alloys based on aluminium
    • 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
    • G21C3/60—Metallic fuel; Intermetallic dispersions
    • 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

Definitions

  • ALUMINUM-PLUTONIUM ALLOYS Figure 1 A1 S wt.% Pu Alloy-- Control Light phase: A1 dendrites Dark phase: Al/PuAlh eutectc Wilma un Figure 3. A1+Swt.%Pu+ 1S Win55 Si Alloy Figure l1. A1 S :913.55 Pu Figure 5. A1 2O wt.% Pu Alloy 1S wh!
  • This invention relates to alloys of aluminum and plutonium, and to methods for their preparation.
  • the invention includes ternary alloys of aluminum, plutonium and one element selected from the group consisting of uranium, silicon and nickel.
  • Binary Al-Pu alloys have been found suitable for use as fuel in research reactors operating with low temperature water.
  • the corrosion resistance to high temperature water of Al alloys containing about 13-20 wt. percent Pu and of hyper-eutectic structure has been found to be good.
  • Al alloys containing less than 13 percent Pu and of hypo-eutectic structure undergo rapid corrosion attack by high temperature water.
  • Rod-type fuel elements in water-cooled power reactors would normally be enriched with less than 13 wt. percent Pu.
  • Al-Pu alloys of up to 13 Wt. percent Pu would be of value as fuel elements if they were resistant to corrosion by water at up to about 350 C.
  • An object of this invention is to prepare a corrosionresistant aluminum-plutonium alloy of less than 13 wt. percent Pu. Another object is to provide such an alloy which does not absorb neutrons to a significant degree.
  • the proportion of Pu in the alloys may range from about 2 ⁇ to about 8 wt. percent. Four to six wt. percent Pu is presently preferred.
  • the nickel has a relatively large neutron-capture cross-section and its proportion is desirably kept low. From 1 to 2 wt. percent Ni is suitable.
  • the proportions of silicon and uranium fall within the range 13-17 wt. percent, with the total Pu-l-Si or total Pu-i-U preferably being within the range 19-21 wt. percent.
  • the hyper-eutectic structure and the absence of any signicant free Al phase is ensured at these proportions.
  • Zirconium was found to be unsuitable as a ternary additive since the ⁇ corrosion resistance to high temperature water was decreased from that of the hypo-eutectic binary alloy.
  • the alloys are preferably prepared by reducing plutonium dioxide with excess aluminum metal in the presence of cryolite (3NaF.AlF3) at about l100-1200 C., to produce billets of the desired composition. These billets are remelted and the temperature raised to about (a) 775 C. before making the Ni addition, (b) 850 C. before making the Si addition, or (c) 950 C. before mak-ing the U addition,
  • the Ni, Si, and U are preferably added in their elemental form.
  • the above preferred tempera- 3,188,202 Patented June 8, 1965 tures of the ternary addition are not critical and may be increased or decreased by about 10 C. to 20 C. or more. However, if the temperatures are much outside these limits non-uniform dispersion, lack of dissolution, presence oct dissolved gases, etc. may be the result.
  • the ternary alloys are then cast into moulds preheated to about C. (c g., graph-ite moulds).
  • Other methods may be used for preparing the initial binary alloy such as reducing plutonium trifluoride with excess aluminum or adding Pu metal to Al metal in the melt. (See Runnalls, Progress in Nuclear Energy, Series V, 2, 98 to 118, Pergamon Press, 1959.)
  • Binary alloy of Al and 5 wt. percent Pu was prepared by the reduction of Pu02 with excess Al, in the presence of cryolite, at 1l50 C. Ternary additions of 1 wt. percent Ni, 15 wt. percent Si and 15 wt. percent U were then made as described above to separate portions of the binary alloy.
  • Corrosion tests were carried out on the alloys using static de-ionized Water at 340 C. This would be a typical temperature of the fuel exterior for a power reactor element cooled by water at 270-280o C. and having a 60- 70 C. temperature gradient across Zircaloy-Z sheathing.
  • Zircaloy-2I is an alloy typically consisting of 1.5% Sn, 0.1% Fe, 0.1% Cr, 0.05% Cr, 0.05% Ni and the ballance Zr.
  • Corrosion test specimens were machined from cast rods, degreased in acetone, etched for one minute in 5% NaOH solution and thoroughly washed in deionized water. The time of exposure to the high temperature water was 20 hours. 'Ihe corrosion ⁇ test results are summarized in the following Table.
  • FIGURES 1 to 5 illustrate the 'as-cast structures of the alloys listed in the above table.
  • Tlhe Al-i-S wt. percent Pu alloy is typical of an alloy having a hypo-eutectic structure with considerable free Al phase -being present-as shown in FIGURE l. This binary alloy is rapidly corroded.
  • the nickel alloy structure includes a hypo-eutectic structure with very small equiaxed grains off oc-Al distributed as shown in FIGURE 2. It will be observed in FIGURES 3-5 that the structures of the 20 wt. percent Pu alloy, the Si alloy and the U alloy, are all qui-te similar Ibeing highly relined and hypereutectic.
  • the corrosion resistance of the three ternary alloys is similar to that of the 20 wt. percent Pu alloy.
  • the corrosion resistance of the ternary alloys is signicantly improved relative to the 5 wt. percent plutonium ⁇ binary alloy-such that the ternary alloys are suitable from a corrosion standpoint :for fuel applications using high temperature water coolant.
  • An alloy consisting of from 2 to 8 Wt. percent plu- Y tonium, uranium from 13 to 17 Wt. percent, and Ythe balance aluminum.
  • An alloy consisting of about 5 wt. percent plu-v tonium, alnout 1 Wt. percent nickel, and the bal-ance aluminum.
  • An alloy consisting of about 5 Wt. percent plutonium, about 15 wt. percent uranium, and the balance aluminum.
  • An ⁇ alloy consisting of from 2 to 8 Wt. percent plutonium, nickel in from 1 to 2 Wt. percent, and the balance aluminum.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Dispersion Chemistry (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Manufacture Of Alloys Or Alloy Compounds (AREA)
  • Structure Of Emergency Protection For Nuclear Reactors (AREA)
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Description

June s, 1965 T. 1. JONES 3,188,202
ALUMINUM-PLUTONIUM ALLOYS Figure 1. A1 S wt.% Pu Alloy-- Control Light phase: A1 dendrites Dark phase: Al/PuAlh eutectc Wilma un Figure 3. A1+Swt.%Pu+ 1S Win55 Si Alloy Figure l1. A1 S :913.55 Pu Figure 5. A1 2O wt.% Pu Alloy 1S wh! U Alloy X i420 X h2o Lghb phase: PuAl Dark phase: eutectic 3,183,202 ALUMINUM-PLUTONIUM ALLOYS Thomas Ivor .i ones, Deep River, Ontario, Canada, assigner to Atomic Energy of Canada Limited, Ontario, Canada, a corporation n Filed Apr. 19, 1961, Ser. No. 104,183 7 Claims. (Cl. 75-122.5)
This invention relates to alloys of aluminum and plutonium, and to methods for their preparation. In particular, the invention includes ternary alloys of aluminum, plutonium and one element selected from the group consisting of uranium, silicon and nickel.
Considerable attention is being devoted to the development of nuclear .power reactors which W-ill produce e-lectrical power competitively With the other conventional energy sources. One type of power reactor which is being investigated is water-cooled, in which pressurized water or steam at elevated temperatures (e.g., 250-400 C) is circulated around the fuel rods. The fuel rods are sheathed in a suitable strong, corrosion-resistant alloy (e.g., Zircaloy-Z). It is important that, in the event of sheath failure, the coolant :system should not become ex- Y cessively contaminated by the corrosion of the nuclear fuel.
Binary Al-Pu alloys have been found suitable for use as fuel in research reactors operating with low temperature water. The corrosion resistance to high temperature water of Al alloys containing about 13-20 wt. percent Pu and of hyper-eutectic structure, has been found to be good. However, Al alloys containing less than 13 percent Pu and of hypo-eutectic structure, undergo rapid corrosion attack by high temperature water. (T. I. Jones, Second International Conference Plutoniurn Metallurgy, Grenoble, France, April 1960, IV Session, Paper 1.)
Rod-type fuel elements in water-cooled power reactors, would normally be enriched with less than 13 wt. percent Pu. Al-Pu alloys of up to 13 Wt. percent Pu would be of value as fuel elements if they were resistant to corrosion by water at up to about 350 C.
An object of this invention is to prepare a corrosionresistant aluminum-plutonium alloy of less than 13 wt. percent Pu. Another object is to provide such an alloy which does not absorb neutrons to a significant degree.
I have now found that Al alloys with up to about 8 percent Pu will form ternary alloys with one of the group consisting of nickel, silicon and uranium, which ternary alloys have good corrosion-resistance to high temperature water.
'The proportion of Pu in the alloys, Agiving 1a suitable enriclrment, lmay range from about 2 `to about 8 wt. percent. Four to six wt. percent Pu is presently preferred. The nickel has a relatively large neutron-capture cross-section and its proportion is desirably kept low. From 1 to 2 wt. percent Ni is suitable. The proportions of silicon and uranium fall within the range 13-17 wt. percent, with the total Pu-l-Si or total Pu-i-U preferably being within the range 19-21 wt. percent. The hyper-eutectic structure and the absence of any signicant free Al phase is ensured at these proportions. Zirconium was found to be unsuitable as a ternary additive since the `corrosion resistance to high temperature water was decreased from that of the hypo-eutectic binary alloy.
The alloys are preferably prepared by reducing plutonium dioxide with excess aluminum metal in the presence of cryolite (3NaF.AlF3) at about l100-1200 C., to produce billets of the desired composition. These billets are remelted and the temperature raised to about (a) 775 C. before making the Ni addition, (b) 850 C. before making the Si addition, or (c) 950 C. before mak-ing the U addition, The Ni, Si, and U are preferably added in their elemental form. The above preferred tempera- 3,188,202 Patented June 8, 1965 tures of the ternary addition are not critical and may be increased or decreased by about 10 C. to 20 C. or more. However, if the temperatures are much outside these limits non-uniform dispersion, lack of dissolution, presence oct dissolved gases, etc. may be the result.
The ternary alloys are then cast into moulds preheated to about C. (c g., graph-ite moulds). Other methods may be used for preparing the initial binary alloy such as reducing plutonium trifluoride with excess aluminum or adding Pu metal to Al metal in the melt. (See Runnalls, Progress in Nuclear Energy, Series V, 2, 98 to 118, Pergamon Press, 1959.)
The following examples will illustrate the invention. Binary alloy of Al and 5 wt. percent Pu was prepared by the reduction of Pu02 with excess Al, in the presence of cryolite, at 1l50 C. Ternary additions of 1 wt. percent Ni, 15 wt. percent Si and 15 wt. percent U were then made as described above to separate portions of the binary alloy.
Corrosion tests were carried out on the alloys using static de-ionized Water at 340 C. This would be a typical temperature of the fuel exterior for a power reactor element cooled by water at 270-280o C. and having a 60- 70 C. temperature gradient across Zircaloy-Z sheathing. [Zircaloy-2I is an alloy typically consisting of 1.5% Sn, 0.1% Fe, 0.1% Cr, 0.05% Cr, 0.05% Ni and the ballance Zr.] Corrosion test specimens were machined from cast rods, degreased in acetone, etched for one minute in 5% NaOH solution and thoroughly washed in deionized water. The time of exposure to the high temperature water was 20 hours. 'Ihe corrosion `test results are summarized in the following Table.
Corrosion of Al-Pu alloys FIGURES 1 to 5 illustrate the 'as-cast structures of the alloys listed in the above table.
Tlhe Al-i-S wt. percent Pu alloy is typical of an alloy having a hypo-eutectic structure with considerable free Al phase -being present-as shown in FIGURE l. This binary alloy is rapidly corroded. The nickel alloy structure includes a hypo-eutectic structure with very small equiaxed grains off oc-Al distributed as shown in FIGURE 2. It will be observed in FIGURES 3-5 that the structures of the 20 wt. percent Pu alloy, the Si alloy and the U alloy, are all qui-te similar Ibeing highly relined and hypereutectic. The corrosion resistance of the three ternary alloys is similar to that of the 20 wt. percent Pu alloy.
The corrosion resistance of the ternary alloys is signicantly improved relative to the 5 wt. percent plutonium `binary alloy-such that the ternary alloys are suitable from a corrosion standpoint :for fuel applications using high temperature water coolant.
The above examples are not intended to be limiting. The proportions may be varied as indicated afbove. Other methods of preparing the initial binary Al-P-u alloy may be used. The uranium in the example was the naturallyoccurring mixture of isotopes, but other isotope mixtures may be used. In the above illustrative alloys, super-purity yaluminum Was used. Spectrographic analyses of the ternary alloys revealed the following impurities:
Weight percent Na 0.03 B, Cr, Fe, K', Pxb, Ca, Ti, Zn 0.02
However, it is not necessary `to use such rsu'peppurity aluminum.
I claim:
1. An alloy consisting of from 2 to 8 Wt. percent plu- Y tonium, uranium from 13 to 17 Wt. percent, and Ythe balance aluminum.
2. The alloy of claim 1 wherein the plutonium is pres- Vent in from 4 to 6 Wt. percent.
3. The alloy of claim 1 wherein the total'pl-utonium plus uranium concentration is from 19 to 21 wt. percent.
4. An alloy consisting of about 5 wt. percent plu-v tonium, alnout 1 Wt. percent nickel, and the bal-ance aluminum.
5. An alloy consisting of about 5 Wt. percent plutonium, about 15 wt. percent uranium, and the balance aluminum.
6. An `alloy consisting of from 2 to 8 Wt. percent plutonium, nickel in from 1 to 2 Wt. percent, and the balance aluminum.
7. The `alloy of claim 6 wherein the plutonium is present in from 4 to 6 Wt. percent.
References Cited by the Examiner UNTED STATES PATENTS 2,885,283 5/59 Sohonlfeld' et al. 75-122.5 r2,919,186 12/59 Colbeck 75-l22.7 2,929,706 3/60 Cramer et al. 75-122.7 y2,934,424 4/60 MacKenzie 75-84.1 2,992,915 7/61 Nelson 75-84.1
CARL D. QUARFORTH, Primary Examiner. OSCAR R. VERTIZ, Examiner.

Claims (2)

1. AN ALLOY CONSISTING OF FROM 2 TO 8 WT. PERCENT PLUTONIUM, URANIUM FROM 13 TO 17 WT. PERCENT, AND THE BALANCE ALUMINUM.
6. AN ALLOY CONSISTING OF FROM 2 TO 8 WT.. PERCENT PLUTONIUM, NICKEL IN FROM 1 TO 2 WT. PERCENT, AND THE BALANCE ALUMINUM.
US104183A 1961-04-19 1961-04-19 Aluminum-plutonium alloys Expired - Lifetime US3188202A (en)

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Application Number Priority Date Filing Date Title
NL277379D NL277379A (en) 1961-04-19
US104183A US3188202A (en) 1961-04-19 1961-04-19 Aluminum-plutonium alloys
GB10697/62A GB934544A (en) 1961-04-19 1962-03-20 Aluminum alloys
DEA39942A DE1252905B (en) 1961-04-19 1962-04-13 Aluminum-plutonium alloys and processes for their manufacture
FR894581A FR1319838A (en) 1961-04-19 1962-04-16 New aluminum and plutonium alloys and preparation process
NL6503035A NL6503035A (en) 1961-04-19 1965-03-10

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4509978A (en) * 1982-12-07 1985-04-09 The United States Of America As Represented By The United States Department Of Energy Recoverable immobilization of transuranic elements in sulfate ash

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2885283A (en) * 1957-08-29 1959-05-05 Fred W Schonfeld Plutonium-aluminum alloys
US2919186A (en) * 1946-07-02 1959-12-29 Colbeck Eric Winearls Uranium alloys
US2929706A (en) * 1959-04-21 1960-03-22 Eugene M Cramer Delta phase plutonium alloys
US2934424A (en) * 1956-05-02 1960-04-26 Ca Atomic Energy Ltd Decontamination of plutoniumaluminum alloy material
US2992915A (en) * 1959-09-29 1961-07-18 Paul A Nelson Pyrometallurgical method

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2919186A (en) * 1946-07-02 1959-12-29 Colbeck Eric Winearls Uranium alloys
US2934424A (en) * 1956-05-02 1960-04-26 Ca Atomic Energy Ltd Decontamination of plutoniumaluminum alloy material
US2885283A (en) * 1957-08-29 1959-05-05 Fred W Schonfeld Plutonium-aluminum alloys
US2929706A (en) * 1959-04-21 1960-03-22 Eugene M Cramer Delta phase plutonium alloys
US2992915A (en) * 1959-09-29 1961-07-18 Paul A Nelson Pyrometallurgical method

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4509978A (en) * 1982-12-07 1985-04-09 The United States Of America As Represented By The United States Department Of Energy Recoverable immobilization of transuranic elements in sulfate ash

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DE1252905B (en) 1967-10-26
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GB934544A (en) 1963-08-21

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