CN1890758B - Fuel element for a fast neutron reactor (variants) and a cladding for the production thereof - Google Patents

Fuel element for a fast neutron reactor (variants) and a cladding for the production thereof Download PDF

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CN1890758B
CN1890758B CN2004800361451A CN200480036145A CN1890758B CN 1890758 B CN1890758 B CN 1890758B CN 2004800361451 A CN2004800361451 A CN 2004800361451A CN 200480036145 A CN200480036145 A CN 200480036145A CN 1890758 B CN1890758 B CN 1890758B
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steel
clad
carbonide
ferrite
mass
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CN1890758A (en
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A·G·约图科夫斯基
M·V·列昂季耶娃-斯米尔诺娃
A·V·瓦图林
V·N·戈洛瓦诺夫
V·K·沙马丁
T·M·布拉诺娃
V·V·茨韦伊莱夫
I·A·什卡布拉
J·A·伊瓦诺夫
V·A·福斯特曼
M·I·索洛宁
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Fed State Unitarian Enterprise Aa Borgval All-Russia Inorganic Material Research Institute
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Fed State Unitarian Enterprise Aa Borgval All-Russia Inorganic Material Research Institute
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    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/22Ferrous alloys, e.g. steel alloys containing chromium with molybdenum or tungsten
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D6/00Heat treatment of ferrous alloys
    • C21D6/002Heat treatment of ferrous alloys containing Cr
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/001Ferrous alloys, e.g. steel alloys containing N
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/005Ferrous alloys, e.g. steel alloys containing rare earths, i.e. Sc, Y, Lanthanides
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/12Ferrous alloys, e.g. steel alloys containing tungsten, tantalum, molybdenum, vanadium, or niobium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/24Ferrous alloys, e.g. steel alloys containing chromium with vanadium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/28Ferrous alloys, e.g. steel alloys containing chromium with titanium or zirconium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/32Ferrous alloys, e.g. steel alloys containing chromium with boron
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D2211/00Microstructure comprising significant phases
    • C21D2211/005Ferrite
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D2211/00Microstructure comprising significant phases
    • C21D2211/008Martensite

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  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
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  • Crystallography & Structural Chemistry (AREA)
  • Heat Treatment Of Steel (AREA)
  • Powder Metallurgy (AREA)
  • Materials For Medical Uses (AREA)

Abstract

The invention relates to nuclear engineering. The inventive fuel element for a fast neutron reactor is characterised in that the cladding thereof is made of a martensite-ferrite steel. The structure of said steel consists of at least two areas through the height of the cladding, i.e. the steel structure provides a high heat resistance in the upper area and a high low-temperature radiation embrittlement resistance in the lower area of said cladding. Said steel has the following component ratio: 0.10-0.21 mass % C, 0.1-0.8 mass % Si, 0.5-2.0 mass % Mn, 10.0-13.5 mass % Cr 0.8-2.5 mass % W, 0.05-0.4 mass % V, 0.05-0.4 mass % Ti, 0.001-008 mass % B, 0.001-0.01 mass % Ce and/or Yt in total, 0.05-0.2 mass % Zr, 0.05-0.2 mass % Ta, and 0.02-0.15 mass % N the rest, being Fe at a ratio between a total V, Ti, Zr and Ta content and a total C and N content ranging from 2 to 9. Said invention makes it possible to develop a fuel element and a cladding for the production thereof made of the steel which exhibits a low level of induced radioactivity and the rapid loss thereof after a neutron exposure, a high embrittlement resistance at a temperature ranging from 270 to 400 DEG C at a neutron irradiation and a high heat resistance at temperatures up to 700 DEG C.

Description

The clad of the fuel element of rapid neutron reactor (variant) and the described element of preparation
Technical field
The present invention relates to the nuclear engineering field, particularly, relate to the material that is used for nuclear engineering, and the present invention can be used to make the fuel element and the parts of fast reaction heap reactor core (below be referred to as the BN reactor).
The steel that is used to make BN reactor fuel element clad and other parts must satisfy a series of strict demands to performance, and these performances comprise that thermotolerance, low-temp radiating cause the embrittlement drag, the room causes expansion drag, processibility, weldability etc.Recently, it is highly important that also to require steel after the neutron field that leaves the BN reactor core that its radioactivity of being brought out can decay fast, in other words, promptly designs so-called low activity steel.One of potential material that is used for fuel-cladding is a chromium steel, and the feature of this steel is to have favourable performance, particularly has the performance that radiation-actuate expands obviously not occur.
Background technology
Known low activity radioresistance steel (referring to RU patent N2135623) contains carbon, silicon, manganese, chromium, nickel, vanadium, copper, molybdenum, cobalt, tungsten, yttrium, niobium, aluminium and iron, and the content range of above-mentioned each element (by weight percentage) is: carbon-0.13-0.18; Silicon-0.20-0.35; Manganese-0.30-0.60; Chromium-2.0-3.5; Tungsten-1.0-2.0; Vanadium-0.10-0.35; Molybdenum-0.01-0.05; Nickel-0.01-0.05; Cobalt-0.01-0.05; Copper-0.01-0.10; Aluminium-0.01-0.10; Niobium-0.01-0.05; Yttrium-0.05-0.15; Surplus is an iron.
Here, the total content of nickel, cobalt, molybdenum, niobium and copper is not higher than 0.2% (weight), and ratio (V+0.3W)/C is 3-6.
This steel has the low activity of bringing out, but is surpassing under 500 ℃ the temperature thermo-labile (referring to the article .Heat resistant Alloys of M.V.Zakha rov and A.M.Zakharov, M.:Metallurgy, 1972).
Also known a kind of low activity heat-resisting (up to 550 ℃) steel (according to RU patent N2033461), this steel contains carbon, silicon, manganese, chromium, tungsten, vanadium, boron, titanium, cerium and iron, and the content range of above-mentioned each element (in mass percent) is: carbon-0.10-0.20; Silicon-0.02-1.00; Manganese-0.50-2.0; Chromium-10.0-13.9; Tungsten-0.8-2.9; Vanadium-0.05-0.45; Titanium-0.01-0.10; Boron-0.0005-0.008; Cerium-0.001-0.100; Surplus is an iron.
In described invention, do not provide the radiance of this steel.But, research work (A.G.Ioltukhovsky, M.V.Leonteva-Smirnova, the article of V.S.Ageev etc. " Influence of Original Structure State on Propensity of 12%Chromium Steels for Irradiation Effected Embrittlement ", referring to 1994 the 51st page of the 3rd Interbranch Conference onReactor Materials Science proceeding first volume that Dimitrovgrad holds) show: a kind of steel with described composition is owing to exist the delta ferrite of 40-50% in its tissue, low-temp radiating embrittlement (being lower than LTIE) will inevitably take place for it.Therefore, the major defect with the very approaching this steel of the steel of being claimed is lower in the thermotolerance deficiency and the LTIE drag that are higher than under 550 ℃.
Become to be grouped into the very approaching a kind of steel of function and the steel of being claimed be the EP823 steel, M.I.Solonin, F.G.Reshetnicov, A.G.Ioltukhovsky etc. have introduced the composition and the performance of this steel at paper " Novel Structural Materials for Cores of Nuclear PowerInstallations " (referring to the magazine Physics and Chemistryof Materials Processing of the 4th phase of calendar year 2001,17-27 page or leaf).
Described steel contains (by weight percentage): carbon-0.14-0.18; Silicon-1.1-1.3; Manganese-0.5-0.8; Chromium-10.0-12.0; Nickel-0.5-0.8; Vanadium-0.2-0.4; Molybdenum-0.6-0.9; Tungsten-0.5-0.8; Niobium-0.2-0.4; Boron-0.006 (calculated value); Cerium-be not higher than 0.1; Nitrogen-be not higher than 0.05; Sulphur-be not higher than 0.010; Phosphorus-be not higher than 0.015; Surplus is an iron.
The major defect of this steel is to have a high activation capacity, its under neutron irradiation by neutron to Ni, Mo, Nb, Cu, the effect of Co and other elements forms long-life radioactive isotope.In addition, described steel is in that to be not less than 650 ℃ of thermotolerances under the temperature low, but also has the tendency that LTIE takes place at 270-400 ℃.
Summary of the invention
Technical goal of the present invention is to create the BN reactor fuel element with clad, and described clad has following performance: bring out active low and to be exposed to rate of decay height, the embrittlement drag under 270-400 ℃ of temperature neutron irradiation after the neutron high and be up to 700 ℃ of thermotolerance height under the temperature.
Technical result is to create the fuel element that has clad, and described clad has the high embrittlement drag under 270-400 ℃ of temperature and is being up to 700 ℃ of contour performances of the high-fire resistance under the temperature.
The target relevant with realizing first kind of form of BN reactor fuel element that is proposed is achieved in the following way: adopt ferrite-martensite level steel to form its clad, this steel has heterogene structure along the clad length direction, it comprises at least two zones, structure of steel in the fuel element top area makes element have higher thermotolerance, then improves its low-temp radiating embrittlement drag organizing of bottom section.
The target relevant with realizing second kind of form of BN reactor fuel element that is proposed is achieved in the following way: adopt the low activity steel to form its clad, this steel contains carbon, silicon, manganese, chromium, vanadium, tungsten, boron, cerium and/or yttrium, titanium, tantalum, zirconium, nitrogen, iron and unavoidable impurities, and the content range of above-mentioned each element (by weight percentage) is:
Carbon 0.10-0.21
Silicon 0.1-0.8
Manganese 0.5-2.0
Chromium 10.0-13.5
Tungsten 0.8-2.5
Vanadium 0.05-0.4
Titanium 0.03-0.3
Boron 0.001-0.008
The total amount 0.001-0.10 of cerium and/or yttrium
Zirconium 0.05-0.2
Tantalum 0.05-0.2
Nitrogen 0.02-0.15
Iron surplus
The total content of vanadium, titanium, zirconium and tantalum is 2-9 with the ratio of the total content of carbon and nitrogen, structure of steel along the clad length direction comprises at least two zones, structure of steel in the fuel element top area makes element have higher thermotolerance, and it comprises the carbonide M of alpha ferrite, δ-ferrite, sorbite, chromium 23C 6And M 6The carbonide of C, steel constituent element (V, Ta, Ti, Zr, W etc.) and carbonitride, Fe 2(W) type intermetallic compound, in the low-temp radiating embrittlement drag that organizing of bottom section then improved element, it comprises the carbonide and the carbonitride of sorbite, δ-ferrite, alpha ferrite, retained austenite, steel constituent element (Cr, V, Ta, W etc.).In this case, high-angle boundary is carbonide M 23C 6And M 6C is occupied, and has the carbonide and the carbonitride VC of disperse distribution (individual) in sorbite and δ-ferritic crystal grain, V (CN), and the precipitated phase of Ti (CN) and Ta (CN), other elements (Fe, Mn, Mo, W, Si etc.) then enter complicated carbide M 23C 6And M 6In the composition of C or enter in the FeCr solid solution.
The target that is proposed also can be achieved in the following way: adopt the low activity steel to form clad on rapid reaction heap fuel element, this steel contains carbon, silicon, manganese, chromium, vanadium, tungsten, boron, cerium and/or yttrium, titanium, tantalum, zirconium, nitrogen, iron and unavoidable impurities, and the content range of above-mentioned each element (by weight percentage) is:
Carbon 0.10-0.21
Silicon 0.1-0.8
Manganese 0.5-2.0
Chromium 10.0-13.5
Tungsten 0.8-2.5
Vanadium 0.05-0.4
Titanium 0.03-0.3
Boron 0.001-0.008
The total amount 0.001-0.10 of cerium and/or yttrium
Zirconium 0.05-0.2
Tantalum 0.05-0.2
Nitrogen 0.02-0.15
Iron surplus
The total content of vanadium, titanium, zirconium and tantalum is 2-9 with the ratio of the total content of carbon and nitrogen, structure of steel along the clad length direction comprises at least two zones, structure of steel in the fuel element top area makes element have higher thermotolerance, and it comprises the carbonide M of alpha ferrite, sorbite, chromium 23C 6And M 6The carbonide of C, steel constituent element (V, Ta, Ti, Zr, W etc.) and carbonitride, Fe 2(W) type intermetallic compound, in the low-temp radiating embrittlement drag that organizing of bottom section then improved element, it comprises the carbonide and the carbonitride of sorbite, δ-ferrite, alpha ferrite, retained austenite, steel constituent element (Cr, V, Ta, W etc.).In this case, high-angle boundary is carbonide M 23C 6And M 6C is occupied, and the carbonide and the carbonitride VC that exist disperse to distribute in sorbite and δ-ferritic crystal grain, V (CN), the precipitated phase of Ti (CN) and Ta (CN), other elements (Fe, Mn, Mo, W, Si etc.) then enter complicated carbide M 23C 6And M 6In the composition of C or enter in the FeCr solid solution.
The various variants of particular of the present invention
In the particular condition of realizing fuel element the-kind of form, comprise three zones along the structure of steel of clad length direction, wherein, to compare with top area with the bottom, the tissue of central region has moderate thermotolerance and low-temp radiating embrittlement drag.
In one of particular condition of making second kind of forms of fuels clad, unavoidable impurities content is done following restriction:
Nickel is not higher than 0.1;
Niobium is not higher than 0.01;
Molybdenum is not higher than 0.01;
Copper is not higher than 0.1;
Cobalt is not higher than 0.01;
Sulphur is not higher than 0.008;
Phosphorus is not higher than 0.008;
Oxygen is not higher than 0.005
In the another kind of particular condition of making clad, high activity metal impurity, promptly the total content of molybdenum, niobium, nickel, copper and cobalt is no more than 0.1% (quality).Its objective is in order to reduce the activity that neutron irradiation brings out and to quicken steel and bring out the active rate of decay.
In another particular condition of making clad, low-melting-point metal impurity, promptly the total content of lead, bismuth, tin, antimony and arsenic is no more than 0.05% (quality).Its objective is in order to improve the low-temp radiating embrittlement drag of steel under neutron irradiation.
Main points of the present invention are: the structure of steel along the clad length direction is inhomogeneous, and, this tissue with fall consistent along BN reactor core length direction up to the actual temperature of several Baidu.Desired the invention process that Here it is has the different reasons that require this new principle to the performance of fuel-cladding with tissue along its length.
Structure of steel in zone, fuel-cladding bottom (temperature is low) comprises the carbonide of strong carbide formation constituent element (Cr, V, Ti, Ta, W etc.) possible in sorbite, alpha ferrite, retained austenite, the steel, the nitride and the carbonitride of above-mentioned each element.There is not carbonide M basically in the wide-angle grain boundary 23C 6And M 6The precipitated phase of C, but have the coalescent carbonide phase of a kind of intracrystalline.Owing to formed this tissue, the chromium in the solid solution is consumed, thus can not radiation-actuate separate out fragility phase (υ) phase, α equates), thereby improved clad in the drag of its low temperature bottom section to the LTIE process.
In order to form this tissue, to the low-temperature region of fuel element circulate (being up to 10 circulations) handle, this circulation comprises that the temperature that is heated to Ac1+20 ℃ is cooled to room temperature then; In this case, after tempering, in cyclic process and after the loop ends in the air during cooling cooling velocity of product must be not less than 50 ℃/minute.
As previously mentioned, have best tissue and make clad have low active and good thermotolerance and radiation drag at high temperature and low-temperature region, adopt the element of the active decay fast of radiation-actuate that steel is carried out complicated Alloying Treatment in order to ensure fuel-cladding, make γ phase stable element (C, N is Mn) with α stable element (Cr mutually, W, V, Ta, Ti, Zr, Mo, Nb, etc.) between satisfy specific proportionate relationship.
Be not less than 600 ℃ fuel element high-temperature area in the clad working temperature, organize and obtain high-fire resistance by making clad form stable martensite-ferrite, described clad tissue has contained the interstitial element (C of solution strengthening effect, N, B) and substitutional element (W, V, Cr), play the carbonide (MC of invigoration effect, M2C, M 23C 6Deng), nitride (MN, M 2N) with carbonitride (MCN) mutually and the laves phase of Fe (W) type.
This tissue of fuel-cladding high-temperature region by also forming 680-760 ℃ of following tempering at 1050-1150 ℃ of following chilling in 40 minutes subsequently.
Increase W content, replace molybdenum according to equivalent proportionate relationship roughly with tungsten, can reduce the activity of clad, and can make it that decay fast takes place after neutron irradiation, reason is the half life period that has reduced the cross section of neutron and the effect of tungsten nuclear and shortened the tungsten isotoppe of radiation generation.Increasing W content also helps to make the long-term and short term strength of steel to remain on high level.
By adding zirconium, tantalum and nitrogen, can make the short-term of steel and long-term strength remain on fully high level.
By adding nitrogen, and the ratio of the total content of titanium, tantalum, zirconium and vanadium and the total content of carbon and nitrogen is defined as 2-9, then can improves the drag that the low-temp radiating of steel under neutron irradiation causes embrittlement.
Adding content is cerium and/or the yttrium of 0.001-0.10% (quality), can promote the refinement and the fragmentation of crystalline grain of steel.In this case, the activity of bringing out that can not increase steel of the present invention as the cerium and the yttrium of low activity element.
The lower limit correspondence of cerium and/or yttrium content described element, and refinement has the least concentration of obvious favourable influence to steel.The upper limit of cerium and/or yttrium content should be able to help steel and keep sufficient processibility in the hot-working stage.
The lower limit basis of zirconium content makes part nitrogen be attached to tiny dispersion and thermodynamically stable these needs of zirconium nitride particle are determined.
Whether zirconium upper content limit basis can form the low melting point ferrozirconium eutectic phase of the processibility that may reduce steel is determined.
The lower limit basis of Ti content makes part carbon be attached to tiny dispersion and these needs of thermodynamically stable titanium carbide are determined.
Whether the upper limit of Ti content can redistribute to determine between zirconium and titanium according to nitrogen.This redistribution is not wished to take place, and reason is to reduce the long-term strength of steel.
The lower limit of tantalum content is according to making part carbon be attached to thermodynamically stable tantalum carbide and guaranteeing that its content in solid solution these needs of solubleness that reach capacity determine.
The globular carbide whether upper limit basis of tantalum content can form the processibility that reduces steel is mingled with to determine.
The lower limit of nitrogen content is determined according to these needs of zirconium nitride particle that make zirconium be attached to tiny dispersion.Require the upper limit of restriction nitrogen, so that steel has processibility at weld period: the activity of bringing out that can not increase steel of the present invention as the zirconium and the tantalum of low activity element.
Nitrogen under neutron irradiation as isotope 14N (99% content) activation that becomes forms long-life isotope 14C, isotope 14(half life period is 5.7 * 10 to C in decay 3Year) produces α particle (stable isotope the time 6He), and can not cause the γ radiation, that is: this utilizability of nitrogen can not influence the decay by the steel radiation activity of γ radiation decision.
The silicone content scope is 0.1-0.8, to guarantee the deoxidation of steel.
For processibility that steel is provided and the amount that reduces delta ferrite, manganese content is remained 0.5-2.0% (weight).
In order to provide heat-resisting and radiation resistance, the chromium content of steel of the present invention is remained on 10-13.5% (weight).
The carbon content scope of steel of the present invention is 0.10-0.21% (weight), so that make steel have high structure stability and thermotolerance by the martensite transfor mation process.
In vaccum sensitive stove, prepare two steel ingots of each heavy 25kg and two ingot castings of each heavy 500kg, as the clad of fuel element of the present invention.With quality is the steel billet that the steel ingot of 25kg forges into diameter 35mm, forges into the bar of thick sheet material of 10mm and diameter 12mm subsequently again.With quality is the steel billet that the ingot of 500kg forges into diameter 90mm, rerolls subsequently and makes the bar of thick thin plate of 6mm and diameter 12mm.Described bar, thin plate and sheet material are heat-treated under standard conditions, i.e. normalizing and tempering.Adopt heat treated metal to be to process effective portion size
Figure 048361451_0
The cylindric sample of 5 * 25mm is so that according to GOST (Γ OCT) 10145-81 and GOST (Γ OCT) 3248-81 test long-term strength and creep.Also use standard sample to measure radiation tensile property afterwards according to GOST (Γ OCT) 10446-80.Described sample must the analog operation temperature be not less than the residing condition of metal in 600 ℃ the fuel-cladding high-temperature part.
Simultaneously, prepare similar small size Gagarin (gagarin) sample, this sample is used for simulating in working temperature and is not higher than the residing condition of metal in 400 ℃ the fuel-cladding low temperature part, promptly is used for testing the tendency that LTIE takes place for they.
In order in the metal of said sample, to form the higher tissue of LTIE drag, sample is carried out circular treatment, that is, be heated to Ac1+20 ℃, be incubated 10 minutes, and between 600 ℃ and 20 ℃ of temperature, be cooled to room temperature with the speed that is not less than 50 ℃/minute.Carry out 10 circulations altogether.After circular treatment, sample afterwards, quickens cooling (cooling rate is not less than 50 ℃/minute) to room temperature 720 ℃ of following temper 2 hours.
Steel of the present invention carries out neutron irradiation under 345-365 ℃ in research property rapid neutron reactor BOR-60, reach (1.14-2.0) 10 in the destruction dosage down-off of 5.8-8.0dpa 22N/cm2 (E>0.1MeV).Tension test adopts remote-operated rupture test machine 1794-Y5 to carry out in air with the strain rate of about 1mm/min.Shown under the condition, sample of having heat-treated under standard conditions and the sample that carries out cycle heat treatment are carried out radiation.
Table 1 has provided as the steel of fuel element clad of the present invention and the chemical composition of known steel, and table 2 shows described steel and bring out the dynamic (dynamical) result of calculation of decay of activity, and table 3 and table 4 item are stretch test results.
Steel is supposed radiation 560 hours and is kept subsequently reaching most 500 years in rapid neutron reactor BN-600 after, it brings out decay of activity dynamics (promptly, γ radiation dose ratio) computational data has confirmed the advantage of steel of the present invention, after the retention time surpasses 10 years (referring to table 2), described advantage is especially remarkable.After keeping 50 years, steel of the present invention can continue to be on active service does not need special protection, and in addition remelting utilizes again.
The similar calculating that the neutron spectra of fusion reactor DEMO is carried out confirms to bring out active quick decay can make material safety still after keeping 50 years.
Industrial applicability
Stretching The performance test results (seeing Table 3) confirms that the tolerance limit of steel anti-power of LTIE after circular treatment that fuel package coating of the present invention is used significantly improves. As a result, when adopting the BN-600 pileradiation under the 345-365 that LTIE the occurring ℃ temperature, the value of the percentage elongation percentage of steel sample of the present invention is lower, is 2.6-6.1% under 20 ℃, is 1.3-1.7% under radiation temperature; And after carrying out circular treatment, above-mentioned percentage elongation result all improves 1.5-2 doubly.
The result who carries out long-term strength and creep test according to GOST (Γ OCT) 10145-81 and GOST (Γ OCT) 3248-81 confirms that (referring to table 4) fuel element of the present invention clad descends heat-resisting at 650-750 ℃ after heat-treating under selected condition with steel, and, even also like this when nitrogen in steel content reduces. For example, steel of the present invention is at 650 ℃, 8kgf/mm2Effect of stress under creep speed be (0.9-7) * 10-4%/hour. When stress is 10 and 12kgf/mm2The time also can be observed similar results.
Therefore, fuel element clad of the present invention can be used for the reactor core of quick neutron reactor. Use the fuel element that has the clad with performance of the present invention faster owing to bringing out active decay, its cost efficiency index will be very high, and described element also has high heat resistance and the anti-power of low-temp radiating embrittlement. In the effect that reduces environmental pollution and will show this kind cost-efficient at the structure material aspect can reusing by moving nuclear power station facility of new generation.
The chemistry of table 1 the present invention and known steel forms
Steel The steel ingot Notional Number Constituent content (weight percent number)
Carbon Silicon Manganese Chromium Tungsten Vanadium Titanium Boron Cerium (and/or yttrium, total amount) Zirconium Tantalum Nitrogen
The present invention   1   0.21   0.8   2.0   13.5   1.5   0.05   0.03   0.001  0.001   0.1   0.05   0.15
  2   0.12   0.5   0.8   12.0   1.2   0.2   0.1   0.007  0.05   0.1   0.18   0.02
  3   0.10   0.1   0.8   11.5   0.8   0.4   0.3   0.008  0.10   0.05   0.1   0.04
  4   0.16   0.5   0.5   10.0   2.5   0.10   0.03   0.006  0.002   0.07   0.2   0.04
Known   5   0.16   0.3   0.59   3.1   1.6   0.25   A1-0.06   -  0.07   -   -   -
Steel The steel ingot Notional Number Constituent content (weight percent number)
Oxygen Nickel Niobium Molybdenum Copper Cobalt Sulphur Phosphorus   ∑ Ti,V,  Zr, Ta,  Nb/∑C,N   ∑  Ni,  Nb,Mo,  Cu. Co   ∑  Pb.  Bi.  Sb.  As.Sn Iron
The present invention   1   0.007   0.07   0.005   0.010   0.01   0.002   0.007   0.007   6   0.097   0.004 Surplus
  2   0.005   0.035   0.005   0.010   0.01   0.002   0.006   0.007   4   0.052   0.005 Surplus
  3   0.006   0.040   0.004   0.005   0.02   0.003   0.006   0.006   9   0.054   0.004 Surplus
  4   0.005   0.030   0.004   0.006   0.02   0.003   0.005   0.007   2.0   0.063   0.003 Surplus
Known   5   -   0.040   0.04   0.035   0.06   0.03   -   -   -   -   - Surplus
(the neutron amount of accumulating on first wall is 12.5MW/m to the decaying kinetics of the γ dose of radiation ratio (Sv/h) that table 2 steel of the present invention absorbs when adopting nuclear fusion reactor DEMO radiation2, radiated time-10 year, E=14MeV)
The steel ingot Notional Number γ dose of radiation (Sv/h) after radiation finishes
1 hour 1 month 1 year 10 years 50 years 100 years 500 years
  1   5·10 2   2.9·10 2  16   1   1·10 -2**   1·10 -3**   5·10 -4
  2   4·10 2   1.5·10 2  20   1   1·10 -2**   1·10 -3**   5·10 -4
  3   6·10 2   2.5·10 2  17   1   1·10 -2**   1·10 -3**   5·10 -4
  4   1·10 2   4·10 2  30   1   1·10 -2**   1·10 -3**   5·10 -4
Remarks: the transmuting of * element and bring out active employing program FISPACT-30 (referring to R.A.Forrest, " the FISPACT-30 user's handbook " that J.-CH.Sublet writes, reportAEA/FUS/227,1993) calculate, the gamma-radiation dose ratio is the spike of element cooling, and being calculated as from radioactive material surface lies quality is the γ radiation of the distance of 1 kilogram of sample 1cm.
* follows 1 * 10-2The γ dose of radiation of the radioactivity decay of Sv/h is a kind of γ radiation of safe level, and according to the principle of IAEA, under this dosage, material can be reused.
Table 3 is by the stretching performance of the steel 16X12B2 Φ TaP of reactor BOR-60 radiation
The steel ingot numbering The heat treatment condition Radiation Temperature T during the definition performanceDefinition,℃   σ B  MPa   σ 1,2  MPa Uniform elongation, % Breaking elongation, %
  T Radiation,  ℃ Dosage, d.p.a
  1 Normalizing (1070 ℃, 30min)+tempering (720 ℃, 3h)   -   0   20   764   653   5.3   19.2
  -   0   350   594   503   3.5   14.2
  -   0   650   355   330   -   22.5
  325   6-8   20   1196   1161   0.7   6.1
  325   6-8   350   973   785   1.7   1.7
  325   6-8   650   250   170   3.6   22.2
Circular treatment+tempering (720 ℃, 3h)   -   0   20   750   645   7.3   21.4
  -   0   350   581   492   6.3   16.5
  -   0   650   339   319   8.1   24.1
  325   5.8   20   969   924   1.3   9.9
  <<-<<   5.8   350   801   787   0.7   9.4
  <<-<<   5.8   650   230   170   3.9   25.3
The steel ingot numbering The heat treatment condition Radiation Temperature T during the definition performanceDefinition,℃   σ B  MPa   σ 1,2  MPa Uniform elongation, % Breaking elongation, %
  2 Normalizing (1070 ℃, 30min)+tempering (720 ℃, 3h)   -   0   20   829   728   4.6   19.8
  0   350   651   565   3.1   13.8
  -   0   650   241   172   4.1   20.3
  335-345   6-8   20   1098   933   2.6   2.6
  <<-<<   6-8   350   770   760   0.3   1.3
  <<-<<   6-8   650   295   200   5.2   21.2
Circular treatment+tempering (720 ℃, 3h)   -   0   20   750   645   7.3   21.4
  -   0   350   581   492   6.3   16.5
  -   0   650   339   319   8.1   24.1
  335-345   6-8   20   1072   908   4.3   6.1
  6-8   350   753   340   1.2   4.3
  6-8   650   271   187   7.4   24.5
Table 4 carries out long-term strength and the creep experiments of the steel sample of the present invention of standard heat treatment (normalizing+tempering)
Steel The steel ingot numbering Test temperature, ℃ Stress, Kgf/mm2 Rupture time Secondary creep speed, %/h Remarks
The present invention   1   650   8   >4500   2.5·10 -4 Protracted test
  10   >4500   2.6·10 -4 Protracted test
  12   250   1.1·10 -3   6=22.3%
  2   650   8   >4500   9.4·10 -5 Protracted test
  10   >4500   2.1·10 -4 Protracted test
  12   2935   3.3·10 -4   δ=22.6%
  3   650   8   >4500   4.8·10 -4 Protracted test
  10   2384   5.0·10 -4   δ=24%
  12   980   3.3·10 -3   δ=21.1%
  4   650   8   >4500   7.0·10 -4 Protracted test
  10   >4500   7.5·10 -4 Protracted test
  12   505   1.1·10 -3   δ=16%
Known   5   650   8   5009   8·10 -4   δ=10%
  10   1710   4·10 -3   δ=16%
  12   103   8·10 -3   δ=21%

Claims (6)

1. the fuel element of a rapid neutron reactor, it is included in the tubulose clad of end with top and the sealing of bottom embolism, be positioned at the granular nuclear fuel and the necessary structural detail of clad, it is characterized in that: its clad is formed by ferrite-martensite steel manufacturing, and the tissue of this steel comprises at least two zones along the clad length direction: top area and bottom section; Structure of steel in the clad top area provides higher thermotolerance, and provides higher low-temp radiating embrittlement drag at the structure of steel of bottom section.
2. according to the fuel element of claim 1, it is characterized in that: the structure of steel along the clad length direction comprises three zones: top area, bottom section and central region, wherein, compare with top area with the bottom, have the intermediate value of thermotolerance and low-temp radiating embrittlement drag at the structure of steel of central region.
3. the fuel element of a rapid neutron reactor, be included in the tubulose clad of end with top and the sealing of bottom embolism, be positioned at the granular nuclear fuel and the necessary structural detail of clad, it is characterized in that: its clad is made by the low activity steel and is formed, described steel contains carbon, silicon, manganese, chromium, vanadium, tungsten, boron, cerium and/or yttrium, titanium, tantalum, zirconium, nitrogen, iron and unavoidable impurities, the content range of above-mentioned each element is, by weight percentage:
Carbon 0.10-0.21
Silicon 0.1-0.8
Manganese 0.5-2.0
Chromium 10.0-13.5
Tungsten 0.8-2.5
Vanadium 0.05-0.4
Titanium 0.03-0.3
Boron 0.001-0.008
The total amount 0.001-0.10 of cerium and/or yttrium
Zirconium 0.05-0.2
Tantalum 0.05-0.2
Nitrogen 0.02-0.15
Iron surplus
The total content of vanadium, titanium, zirconium and tantalum is 2-9 with the ratio of the total content of carbon and nitrogen, comprises at least two zones along the described structure of steel of clad length direction: top area and bottom section; Structure of steel in the fuel-cladding top area makes element have higher thermotolerance, comprises the carbonide M of alpha ferrite, δ-ferrite, sorbite, chromium 23C 6And M 6C, steel constituent element V, Ta, Ti, the carbonide of Zr and W and carbonitride, Fe 2(W) type intermetallic compound in the low-temp radiating embrittlement drag that organizing of bottom section then provides higher, comprises sorbite, δ-ferrite, alpha ferrite, retained austenite, steel constituent element Cr, V, the carbonide of Ta and W and carbonitride; High-angle boundary is carbonide M 23C 6And M 6C is occupied, and the carbonide and the carbonitride VC that exist disperse to distribute in sorbite and the δ-ferrite crystal grain, V (CN), the precipitated phase of Ti (CN) and Ta (CN), and other element of Fe, Mn, Mo, W and Si enter complicated carbide M 23C 6And M 6In the composition of C or enter in the FeCr solid solution.
4. fuel-cladding of making the rapid neutron reactor that forms by the low activity steel, described steel contains carbon, silicon, manganese, chromium, vanadium, tungsten, boron, cerium and/or yttrium, titanium, tantalum, zirconium, nitrogen, iron and unavoidable impurities, the content range of above-mentioned each element is, by weight percentage:
Carbon 0.10-0.21
Silicon 0.1-0.8
Manganese 0.5-2.0
Chromium 10.0-13.5
Tungsten 0.8-2.5
Vanadium 0.05-0.4
Titanium 0.03-0.3
Boron 0.001-0.008
The total amount 0.001-0.10 of cerium and/or yttrium
Zirconium 0.05-0.2
Tantalum 0.05-0.2
Nitrogen 0.02-0.15
Iron surplus
The total content of vanadium, titanium, zirconium and tantalum is 2-9 with the ratio of the total content of carbon and nitrogen, comprises at least two zones along the structure of steel of clad length direction: top area and bottom section; Structure of steel in the fuel element top area makes element have higher thermotolerance, comprises the carbonide M of alpha ferrite, δ-ferrite, sorbite, chromium 23C 6And M 6C, steel constituent element V, Ta, Ti, the carbonide of Zr and W and carbonitride, Fe 2(W) type intermetallic compound in the low-temp radiating embrittlement drag that organizing of bottom section then provides higher, comprises sorbite, δ-ferrite, alpha ferrite, retained austenite, steel constituent element Cr, V, the carbonide of Ta and W and carbonitride; High-angle boundary is carbonide M 23C 6And M 6C is occupied, and the carbonide and the carbonitride VC that exist disperse to distribute in sorbite and the δ-ferrite crystal grain, V (CN), the precipitated phase of Ti (CN) and Ta (CN), other element of Fe, Mn, Mo, W and Si enter complicated carbide M 23C 6And M 6In the composition of C or enter in the FeCr solid solution.
5. according to the fuel-cladding of claim 4, it is characterized in that: unavoidable impurities content in the steel is done following restriction, by weight percentage:
Nickel is not higher than 0.1;
Niobium is not higher than 0.01;
Molybdenum is not higher than 0.01;
Copper is not higher than 0.1;
Cobalt is not higher than 0.01;
Sulphur is not higher than 0.008;
Phosphorus is not higher than 0.008;
Oxygen is not higher than 0.005
High activity metal impurity, promptly the total content of molybdenum, niobium, nickel, copper and cobalt is no more than 0.1 weight %.
6. according to the fuel-cladding of claim 4, it is characterized in that: described low activity steel also comprises low-melting-point metal impurity, i.e. lead, bismuth, tin, antimony and arsenic, and the total content of these impurity is no more than 0.05 weight %.
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