CN109652628A - A kind of used by nuclear fuel jacketing FeCrAl alloy and its preparation and crystallite dimension control method - Google Patents
A kind of used by nuclear fuel jacketing FeCrAl alloy and its preparation and crystallite dimension control method Download PDFInfo
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- CN109652628A CN109652628A CN201910126790.0A CN201910126790A CN109652628A CN 109652628 A CN109652628 A CN 109652628A CN 201910126790 A CN201910126790 A CN 201910126790A CN 109652628 A CN109652628 A CN 109652628A
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- C—CHEMISTRY; METALLURGY
- C21—METALLURGY OF IRON
- C21D—MODIFYING THE PHYSICAL STRUCTURE OF FERROUS METALS; GENERAL DEVICES FOR HEAT TREATMENT OF FERROUS OR NON-FERROUS METALS OR ALLOYS; MAKING METAL MALLEABLE, e.g. BY DECARBURISATION OR TEMPERING
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- C21D1/26—Methods of annealing
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- C21D—MODIFYING THE PHYSICAL STRUCTURE OF FERROUS METALS; GENERAL DEVICES FOR HEAT TREATMENT OF FERROUS OR NON-FERROUS METALS OR ALLOYS; MAKING METAL MALLEABLE, e.g. BY DECARBURISATION OR TEMPERING
- C21D6/00—Heat treatment of ferrous alloys
- C21D6/002—Heat treatment of ferrous alloys containing Cr
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- C—CHEMISTRY; METALLURGY
- C21—METALLURGY OF IRON
- C21D—MODIFYING THE PHYSICAL STRUCTURE OF FERROUS METALS; GENERAL DEVICES FOR HEAT TREATMENT OF FERROUS OR NON-FERROUS METALS OR ALLOYS; MAKING METAL MALLEABLE, e.g. BY DECARBURISATION OR TEMPERING
- C21D8/00—Modifying the physical properties by deformation combined with, or followed by, heat treatment
- C21D8/02—Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of plates or strips
- C21D8/0221—Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of plates or strips characterised by the working steps
- C21D8/0226—Hot rolling
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- C21—METALLURGY OF IRON
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- C21D9/00—Heat treatment, e.g. annealing, hardening, quenching or tempering, adapted for particular articles; Furnaces therefor
- C21D9/0081—Heat treatment, e.g. annealing, hardening, quenching or tempering, adapted for particular articles; Furnaces therefor for slabs; for billets
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- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
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- C22C38/00—Ferrous alloys, e.g. steel alloys
- C22C38/001—Ferrous alloys, e.g. steel alloys containing N
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
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- C22C38/004—Very low carbon steels, i.e. having a carbon content of less than 0,01%
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
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- C22C38/00—Ferrous alloys, e.g. steel alloys
- C22C38/06—Ferrous alloys, e.g. steel alloys containing aluminium
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- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C38/00—Ferrous alloys, e.g. steel alloys
- C22C38/18—Ferrous alloys, e.g. steel alloys containing chromium
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- 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
- G21C3/02—Fuel elements
- G21C3/04—Constructional details
- G21C3/06—Casings; Jackets
- G21C3/07—Casings; Jackets characterised by their material, e.g. alloys
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention belongs to cladding nuclear fuels technical fields, and in particular to a kind of used by nuclear fuel jacketing FeCrAl alloy and its preparation and crystallite dimension control method.FeCrAl alloy material of the present invention for nuclear-power reactor fuel element cladding, following components composition: Cr, Al, Fe, impurity, wherein, the total weight percent content of Cr alloying element is 11.00wt%~14.00wt%, and the total weight percent content of Al alloying element is 5.50wt%-6.50wt%.The FeCrAl alloy of this method preparation has preferable high temperature oxidation resistance and corrosion resistance.By the control to alloying element content, processing technology, so that the crystallite dimension of FeCrAl alloy can satisfy design needs.The present invention is in the method for preparing FeCrAl alloy material using techniques such as Low Temperature Hot Rolling, high temperature re-crystallization heat treatments simultaneously, make alloy material that there is very excellent high temperature oxidation resistance under 1200 DEG C of vapor, pyrogenic steam oxidation rate is well below current commercial nuclear power cladding materials Zr-4.
Description
Technical field
The invention belongs to cladding nuclear fuels technical fields, and in particular to a kind of used by nuclear fuel jacketing FeCrAl alloy and its system
Standby and crystallite dimension control method.
Background technique
In March, 2011, nuclear leakage accident occurs for Fukushima nuclear power station, main reason is that zirconium alloy cladding is in accident conditions
Lower and high temperature coolant water vigorous reaction, releases big calorimetric and explosion gas hydrogen, and cladding materials mechanical property is caused to deteriorate, and produces
The nuclear catastrophes consequences such as life reactor hydrogen is quick-fried and a large amount of radioactive products leak.The same year, the fault-tolerant nuclear fuel of nuclear reactor accident
(ATF) involucrum concept is suggested, it is the fuel system of new generation resisting major accident ability for raising fuel element and developing,
It can prevent fission product loss and fuel is avoided to be corroded and effectively exported thermal energy by coolant.This proposes cladding materials
Higher requirement.
Crash-proof cladding materials requires it can be in 800~1200 DEG C or so steam ambients in several hours.Nuclear reactor
The fault-tolerant nuclear fuel of accident (ATF) cladding materials developing direction mainly has SiC ceramic matrix composite material, stainless steel (ferrite, austenite, Ni-
Cr steel) and surface denatured fuel involucrum etc..SiC material has good mechanical behavior under high temperature and inoxidizability as ceramic material
Can, but itself has certain brittleness, and differs larger with metal material thermal expansion coefficient, is easy in fast fast-growing cooling repeatedly
It cracks in the process, and its long preparation period, poor processability etc. keeps its application more difficult.Coating technology is zircaloy
To the Transition Technology of cladding materials of new generation, it can be obviously improved the high temperature oxidation resistance of zircaloy, but if its film layer material
Material is inconsistent with the thermal expansion coefficient of basis material, and film layer has the risk to fall off, and coating alloy during long service
It is often different with matrix alloy electrochemical potential, it is possible to create electrochemical corrosion.And stainless steel-like cladding materials had both had higher than zirconium
The mechanical property and high temperature oxidation resistance of alloy, and there is the toughness higher than SiC ceramic material, and in ferritic stainless steel
Fe-Cr-Al alloy has outstanding water oxidation susceptibility resistant to high temperatures, heat-mechanical property and radiation-resistant property, by countries in the world
Pay attention to, is the prior development direction of the fault-tolerant nuclear fuel of next-generation nuclear reactor accident (ATF) cladding materials.
Existing commercialization FeCrAl alloy is greatly improved on the basis of Aludirome by adding various microelements
The mechanical property of Aludirome, but the content of Cr, Al element of matrix alloy and proportion be there is still a need for carrying out necessary optimization,
To further increase the mechanical behavior under high temperature and thermal stability of FeCrAl alloy.Due to cladding materials face be high temperature, high pressure,
The adverse circumstances of the various factors comprehensive functions such as irradiation, corrosion and oxidation, it is therefore desirable to which its performance is comprehensively considered and commented
Valence, wherein the regulation of grain size is a wherein important ring.If crystallite dimension is excessive, alloy mechanical property decline, easily
Stress is generated to concentrate；And crystal grain is too small when alloy preparation, then being also easy to produce crystal grain in the high temperature environment grows up, and leads to alloy physics
Crystal grain that can be unstable and too small is more vulnerable to intercrystalline corrosion since grain boundary area increases.So it is brilliant to grasp FeCrAl alloy
The control technology of particle size can design the good FeCrAl conjunction of comprehensive performance that preparation meets cladding materials requirement of new generation
Gold.
Summary of the invention
The purpose of the present invention is to provide a kind of nuclear fuel with preferable high temperature oxidation resistance and corrosion resistance
Involucrum FeCrAl alloy.
A kind of used by nuclear fuel jacketing FeCrAl alloy, FeCrAl alloy material, weight percentage, by following
Group is grouped as, Cr 11wt%~14wt%；Al 5.5wt%~6.5wt%；C≦1000ppm；N≦l000ppm；Surplus is Fe
With inevitable microelement, and FeCrAl alloy material need to carry out it is each to equal deflections forging.
A kind of used by nuclear fuel jacketing FeCrAl alloy, FeCrAl alloy material consist of the following compositions: Cr
13.0wt%；Al 6.0wt%；C≦1000ppm；N≦1000ppm；Surplus is Fe and inevitable microelement.
A kind of used by nuclear fuel jacketing FeCrAl alloy, FeCrAl alloy material consist of the following compositions: Cr
11.0wt%；Al 6.0wt%；C≦1000ppm；N≦1000ppm；Surplus is Fe and inevitable microelement.
The purpose of the present invention is to provide a kind of used by nuclear fuel jacketing FeCrAl alloys that pyrogenic steam oxidation rate is low
Preparation and crystallite dimension control method.
A kind of preparation and crystallite dimension control method of used by nuclear fuel jacketing FeCrAl alloy, specifically comprise the following steps:
Step 1, the high purity alloys with ingot iron and purity greater than 99.9wt% are mixed according to FeCrAl alloy material ratio
It closes, using vacuum induction melting furnace melting and pours to cast from and prepare ingot casting in square dies, be slowly cooled to room temperature with furnace；
Step 2, ingot casting homo genizing annelaing at 1150 DEG C~1200 DEG C, and keep the temperature 3h；
Step 3, rectangular ingot casting is carried out at 1200 DEG C three different directions etc. deflections pull out forging, the forging forged every time
Than being greater than 3；
Step 4 carries out high temperature, short time dynamic recrystallization treatment, heat treatment temperature 950 to the FeCrAl alloy after forging
DEG C -1050 DEG C, soaking time about 20min；
The surface scale of plate after step 5, removal forging, by surface cleaning, treated that plate is heated to 400-1200
DEG C and keep the temperature 2h, hot rolled plate after heat treatment, the initial temperature of hot rolling is 400 DEG C -1200 DEG C, material deflection >=50wt%；
Plate after hot rolling is carried out recrystallization annealing processing by step 6, and recrystallization annealing temperature is 800 DEG C~1000 DEG C,
Soaking time is 50min~70min, and the type of cooling is air-cooled.
The beneficial effects of the present invention are:
FeCrAl alloy material of the present invention for nuclear-power reactor fuel element cladding, Cr:11wt%~
14wt%, Al:5.5wt%~6.5wt% have preferable high temperature oxidation resistance and corrosion resistance.By to alloying element
The control of content, processing technology, so that the crystallite dimension of FeCrAl alloy can satisfy design needs.Simultaneously prepared by the present invention
Using techniques such as Low Temperature Hot Rolling, high temperature re-crystallization heat treatments in the method for FeCrAl alloy material, make alloy material at 1200 DEG C
There is very excellent high temperature oxidation resistance, pyrogenic steam oxidation rate is well below current commercial nuclear power involucrum under vapor
Material Zr-4.
Detailed description of the invention
Fig. 1 is that Fe11Cr6Al is rolled at 400 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 800 DEG C；
Fig. 2 is that Fe11Cr6Al is rolled at 400 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 900 DEG C；
Fig. 3 is that Fe11Cr6Al is rolled at 400 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 1000 DEG C；
Fig. 4 is that Fe11Cr6Al is rolled at 400 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 1100 DEG C；
Fig. 5 is that Fe11Cr6Al is rolled at 600 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 800 DEG C；
Fig. 6 is that Fe11Cr6Al is rolled at 600 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 900 DEG C；
Fig. 7 is that Fe11Cr6Al is rolled at 600 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 1000 DEG C；
Fig. 8 is that Fe11Cr6Al is rolled at 600 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 1100 DEG C；
Fig. 9 is that Fe11Cr6Al is rolled at 800 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 800 DEG C；
Figure 10 is that Fe11Cr6Al is rolled at 800 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 900 DEG C；
Figure 11 is that Fe11Cr6Al is rolled at 800 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 1000 DEG C；
Figure 12 is that Fe11Cr6Al is rolled at 800 DEG C, keeps the temperature 10min air-cooled metallographic microscope again after then air-cooled at 1100 DEG C；
Figure 13 is FeCrAl based alloy component list.
Specific embodiment
The invention will be further described below in conjunction with the accompanying drawings.
A kind of nuclear reactor fuel element involucrum FeCrAl alloy material, weight percentage, by following components
Composition, Cr 11wt%~14wt%；Al 5.5wt%~6.5wt%；C≦1000ppm；N≦l000ppm；Surplus is for Fe and not
Evitable microelement.Then regulate and control rolling deformation amount, rolling temperature and recrystallization annealing to equal deformations forging by each,
The last gained alloy size of control is controllable in 30 μm -400 μm.
FeCrAl is alloy hardening in order to prevent and the aggravation of brittle tendency, causes alloy in reactor operation and processing preparation
It is broken in the process, it should have compared with strict control on highly resistance pyrogenic steam oxidation capability foundation discussion and reduce in guarantee FeCrAl alloy
Cr, Al content.Meanwhile containing Cr appropriate, the FeCrAl alloy of Al content makes as reactor crash-proof fuel canning material
With other than with above-mentioned performance requirement, also alloy high-temp tissue should be made more stable, improve the recrystallization of alloy as far as possible
Temperature is grown up so that alloy has stronger thermal structure stability at 800 DEG C or more and postpones alloy grain size, only stable
Organizing ability bring the enough reliabilities of alloy.
Impurity content of the present invention meets the standard of current commercial industrial pure iron and ferritic stainless steel.
FeCrAl alloy formula of the present invention is the service demand according to nuclear reactor cladding materials to existing FeCrAl
The improvement of alloy has advanced optimized the composition range of Cr content and Al content on the basis of existing components, while to Cr, Al
Content controlled, reduce Cr, the content of Al, to avoid alloy hardening and brittle tendency.
Applicant pass through study for a long period of time test discovery: FeCrAl alloy Al content in 5.5wt%~6.5wt%,
Its steam oxidation performance resistant to high temperatures is excellent, and good mechanical properties, therefore can advanced optimize out that have both crystallite dimension full
The FeCrAl alloy of sufficient design requirement.Alloy of the present invention is moved back by Reasonable Regulation And Control rolling deformation amount, rolling temperature, recrystallization
Fiery temperature, recrystallization annealing soaking time regulate and control the grain size of FeCrAl alloy, can meet design
It needs.And reference is provided to be used as the design of the material of the core structures body such as fuel element cladding, screen work in power producer.
The technical program advanced optimizes the high temperature oxidation resistance of FeCrAl alloy, the function directly and Cr, Al's
Content is related, by Cr, the total weight percent of Al alloying element and when being set as 17wt%~19wt%, room-temperature mechanical property,
Elevated temperature strength is optimal；In FeCrAl alloy the total weight percent of Al alloying element and are as follows: when 5.5-6.5wt%, entire alloy
High temperature oxidation resistance with superior alloy.
Further, the alloying element content in FeCrAl alloy is carried out preferably, the total weight percentage of Cr alloying element
Than for 12.5wt%~13.5wt%, the total weight percent of C alloy element is less than or equal to 0.01wt%, N alloying element it is total
Weight percent is less than or equal to 0.01wt%.
Further, nuclear reactor fuel element involucrum FeCrAl alloy material, weight percentage, by following
Group is grouped as: Cr:11~14, Al:5.5~6.5, C :≤0.01, N :≤0.01, surplus is Fe and impurity.
Further, nuclear reactor fuel element involucrum FeCrAl alloy material, weight percentage, by following
Group is grouped as, Cr:13.0wt%, Al:6.0wt%, C :≤0.01, N :≤0.01, surplus is Fe and impurity.
Further, nuclear reactor fuel element involucrum FeCrAl alloy material, weight percentage, by following
Group is grouped as, Cr:11.0wt%, Al:6.0wt%, C :≤0.01, N :≤0.01, surplus is Fe and impurity.
Embodiment 1: a kind of crash-proof nuclear power fuel element FeCrAl alloy, concrete composition are as shown in figure 13.1~5
Alloy is prepared with following methods using the composition in above-mentioned Figure 13 for specific proportion of the invention, it is specific the preparation method comprises the following steps:
1. the high purity alloys with ingot iron and purity greater than 99.9wt% are formulated ingredient by Figure 13, vacuum induction melting is used
Furnace melting prepares 9-11 kilograms of ingot casting；
| Embodiment | Cr wt% | Al wt% | C wt% | N wt% | F wt% |
| 1 | 10.82 | 6.20 | ≦0.01 | ≦0.01 | 82.98 |
| 2 | 12.89 | 5.91 | ≦0.01 | ≦0.01 | 80.97 |
Figure 13 FeCrAl based alloy component list
2. above-mentioned ingot casting is carried out high temperature homogenizing annealing temperature.Annealing temperature: it is not less than 1150 DEG C, soaking time: no
Lower than 3h；
3. the equal deflections that rectangular ingot casting is carried out at 1200 DEG C to three different directions pull out forging, the forging ratio forged every time is big
In 3；
4. pair forging after FeCrAl alloy carry out high temperature, short time dynamic recrystallization treatment, heat treatment temperature be 950 DEG C-
1050 DEG C, soaking time about 20min.
5. the rolling of rolling deformation amount control plate after 55% or so, forging-recrystallization temperature control variable and correspondence
Number is as shown in table 1:
1 rolling of table-recrystallization temperature control variable and reference numeral table
6. the plate after hot rolling is carried out recrystallization annealing processing, soaking time is recrystallized are as follows: 10min, the type of cooling are
It is air-cooled.
The present invention is detected to above-mentioned by manufactured FeCrAl alloy in Figure 13, table 1, detects each alloy in final crystalline substance
Particle size size (μm), and corresponding control parameter-crystallite dimension figure is drawn out, as shown in table 2.
By table 2: rolling-recrystallization annealing technological parameter by regulating and controlling FeCrAl alloy, we can obtain
The FeCrAl alloy that a series of crystallite dimensions wanted to design determine.
Rolling-recrystallization annealing-crystallite dimension table of 2 FeCrAl alloy of table
The testing result of 3 FeCrAl alloy property of table
In summary, the selection of elemental constituent and the optimization of proportion and the optimization of preparation method through the invention, is having
While effect guarantees significant high temperature oxidation resistance, and it can obtain what a series of crystallite dimensions that design is wanted determined
FeCrAl alloy.Thus, alloy design technology of the invention can be used as fuel element cladding, screen work etc. in power producer
Reference is provided when the design of material preparation of core structure body.
Above-described specific embodiment has carried out further the purpose of the present invention, technical scheme and beneficial effects
It is described in detail, it should be understood that being not intended to limit the present invention the foregoing is merely a specific embodiment of the invention
Protection scope, all within the spirits and principles of the present invention, any modification, equivalent substitution, improvement and etc. done should all include
Within protection scope of the present invention.
Claims (4)
1. a kind of used by nuclear fuel jacketing FeCrAl alloy, it is characterised in that: the FeCrAl alloy material, by weight percentage composition
Meter, composed of the following components, Cr 11wt%~14wt%；Al 5.5wt%~6.5wt%；C≦1000ppm；N≦
l000ppm；Surplus is Fe and unavoidable microelement, and FeCrAl alloy material need to carry out it is each to equal deflections forging
It makes.
2. a kind of used by nuclear fuel jacketing FeCrAl alloy according to claim 1, it is characterised in that: the FeCrAl alloy material
Material consists of the following compositions: Cr 13.0wt%；Al 6.0wt%；C≦1000ppm；N≦1000ppm；Surplus is Fe and can not
The microelement avoided.
3. a kind of used by nuclear fuel jacketing FeCrAl alloy according to claim 1, it is characterised in that: the FeCrAl alloy material
Material consists of the following compositions: Cr 11.0wt%；Al 6.0wt%；C≦1000ppm；N≦1000ppm；Surplus is Fe and can not
The microelement avoided.
4. the preparation and crystallite dimension control method of a kind of used by nuclear fuel jacketing FeCrAl alloy, which is characterized in that specifically include
Following steps:
Step 1, the high purity alloys with ingot iron and purity greater than 99.9wt% are mixed according to FeCrAl alloy material ratio, are made
It with vacuum induction melting furnace melting and pours to cast from and prepares ingot casting in square dies, be slowly cooled to room temperature with furnace；
Step 2, ingot casting homo genizing annelaing at 1150 DEG C~1200 DEG C, and keep the temperature 3h；
Step 3, rectangular ingot casting is carried out at 1200 DEG C three different directions etc. deflections pull out forging, the forging ratio forged every time is big
In 3；
Step 4, to after forging FeCrAl alloy carry out high temperature, short time dynamic recrystallization treatment, heat treatment temperature be 950 DEG C-
1050 DEG C, soaking time 20min；
The surface scale of plate after step 5, removal forging, by surface cleaning, treated that plate is heated to 400-1200 DEG C simultaneously
2h is kept the temperature, hot rolled plate after heat treatment, the initial temperature of hot rolling is 400 DEG C -1200 DEG C, material deflection >=50wt%；
Plate after hot rolling is carried out recrystallization annealing processing by step 6, and recrystallization annealing temperature is 800 DEG C~1000 DEG C, heat preservation
Time is 50min~70min, and the type of cooling is air-cooled.
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| CN110629128A (en) * | 2019-10-15 | 2019-12-31 | 哈尔滨工程大学 | FeCrAlZr cladding material and preparation method thereof |
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| CN113736966A (en) * | 2021-08-27 | 2021-12-03 | 西安交通大学 | FeCrAl-based alloy with dual heterostructure and preparation method thereof |
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