CN109972048B - FeCrAl alloy and ferrite/martensite heat-resistant steel composite tube for nuclear fuel cladding of nuclear reactor and preparation method thereof - Google Patents
FeCrAl alloy and ferrite/martensite heat-resistant steel composite tube for nuclear fuel cladding of nuclear reactor and preparation method thereof Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B21—MECHANICAL METAL-WORKING WITHOUT ESSENTIALLY REMOVING MATERIAL; PUNCHING METAL
- B21C—MANUFACTURE OF METAL SHEETS, WIRE, RODS, TUBES OR PROFILES, OTHERWISE THAN BY ROLLING; AUXILIARY OPERATIONS USED IN CONNECTION WITH METAL-WORKING WITHOUT ESSENTIALLY REMOVING MATERIAL
- B21C37/00—Manufacture of metal sheets, bars, wire, tubes or like semi-manufactured products, not otherwise provided for; Manufacture of tubes of special shape
- B21C37/06—Manufacture of metal sheets, bars, wire, tubes or like semi-manufactured products, not otherwise provided for; Manufacture of tubes of special shape of tubes or metal hoses; Combined procedures for making tubes, e.g. for making multi-wall tubes
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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
- C21D1/00—General methods or devices for heat treatment, e.g. annealing, hardening, quenching or tempering
- C21D1/18—Hardening; Quenching with or without subsequent tempering
- C21D1/25—Hardening, combined with annealing between 300 degrees Celsius and 600 degrees Celsius, i.e. heat refining ("Vergüten")
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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
- C21D1/00—General methods or devices for heat treatment, e.g. annealing, hardening, quenching or tempering
- C21D1/26—Methods of annealing
- C21D1/30—Stress-relieving
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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
- C21D8/10—Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of tubular bodies
- C21D8/105—Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of tubular bodies of ferrous alloys
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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
- C21D9/00—Heat treatment, e.g. annealing, hardening, quenching or tempering, adapted for particular articles; Furnaces therefor
- C21D9/08—Heat treatment, e.g. annealing, hardening, quenching or tempering, adapted for particular articles; Furnaces therefor for tubular bodies or pipes
- C21D9/085—Cooling or quenching
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C38/00—Ferrous alloys, e.g. steel alloys
- C22C38/02—Ferrous alloys, e.g. steel alloys containing silicon
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C38/00—Ferrous alloys, e.g. steel alloys
- C22C38/04—Ferrous alloys, e.g. steel alloys containing manganese
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C38/00—Ferrous alloys, e.g. steel alloys
- C22C38/06—Ferrous alloys, e.g. steel alloys containing aluminium
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- C—CHEMISTRY; METALLURGY
- 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
- C22C38/24—Ferrous alloys, e.g. steel alloys containing chromium with vanadium
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- C—CHEMISTRY; METALLURGY
- 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
- C22C38/26—Ferrous alloys, e.g. steel alloys containing chromium with niobium or tantalum
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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
- C21D2211/00—Microstructure comprising significant phases
- C21D2211/005—Ferrite
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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
- C21D2211/00—Microstructure comprising significant phases
- C21D2211/008—Martensite
Abstract
The invention relates to the field of fuel cladding tubes with high neutron irradiation resistance, corrosion resistance and high temperature resistance in nuclear reactors, in particular to a FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for nuclear fuel cladding of nuclear reactors and a preparation method thereof. The inner layer is made of ferrite/martensite heat-resistant steel material, the outer layer is made of FeCrAl alloy material, and an iron-based material auxiliary layer is arranged between the ferrite/martensite heat-resistant steel material and the FeCrAl alloy material, and the preparation method comprises the following steps: the method comprises the steps of assembling an outer layer, an intermediate transition layer and an inner layer pipe, then assembling and packaging the seamless composite pipe blank after exhausting, welding an end head for sealing, heating, forming a metallurgical composite seamless composite pipe blank by adopting thermal deformation processing, and finally processing the seamless composite pipe blank into a finished pipe with required specification by cold deformation.
Description
Technical Field
The invention relates to the field of fuel cladding tubes with high neutron irradiation resistance and corrosion resistance in a water-cooled nuclear reactor, in particular to a FeCrAl alloy and T91 ferrite/martensite heat-resistant steel metal seamless composite tube structure for a nuclear fuel cladding of a nuclear reactor and a preparation method thereof.
Background
Zr alloy is an important nuclear reactor structural material in the past and at present, has good corrosion resistance and neutron irradiation resistance in high-pressure water and steam at the temperature of 300-400 ℃, and some newly developed Zr alloys (such as ZIRLO, M5, E635 and the like) are used as cladding and structural components of high-fuel-consumption fuel assemblies of pressurized water reactors and boiling water reactors. The research content of the advanced zirconium alloy comprises: corrosion resistance, mechanical properties, water corrosion resistance, radiation growth resistance, PCI (pellet-cladding interaction) crack propagation resistance, and improved fuel burn-up.
Austenitic stainless steels were the first generation fast reactor cladding material due to their good corrosion and hot creep resistance, but these austenitic steels have severe radiation swell problems. It was found that the degree of swelling can be reduced by the addition of stabilizing elements (e.g., Ti, etc.) and moderate cold deformation, and that fuel cladding materials such as 15-15Ti, 316Ti, etc. were developed. However, when the irradiation dose is high, significant radiation swelling occurs, and thus it cannot be used in advanced high irradiation reactors.
Ferritic/martensitic heat resistant steels are considered as the primary candidate for cladding for fast reactor design in fourth generation reactors, having high thermal conductivity and low coefficient of thermal expansion, superior resistance to swelling and small and stable swelling rates than austenitic steels. Experiments show that ferrite/martensite heat-resistant steel containing 8-9% of Cr by mass shows the highest anti-swelling capacity, and low swelling is the common performance of the ferrite alloy. Therefore, the alloy becomes an ideal candidate material for the fast breeder reactor, but the strength of the material is reduced above 550 ℃, so that the application of the material as a key material of an advanced reactor is limited.
Oxide dispersion strengthened steel (ODS steel) including ferritic steel, martensitic steel and ferrite/martensite dual phase heat resistant steel. Researches show that the microstructure of the nanostructured ODS steel enables the ODS steel to have excellent radiation resistance, can meet the radiation resistance requirement (particularly the He expansion resistance under the condition of high He) of an advanced reactor core material, can meet or nearly meet the strength requirement of 650 ℃ service temperature, and becomes an alternative material of the advanced reactor core component. However, the material has high processing cost and difficult subsequent deformation processing.
Since 2011 in japan after nuclear accidents, accident-resistant fuels (ATF) were proposed, which were developed to improve fuel elements and explore fuel rods made of anti-LOCA (coolant starvation condition) accident cladding materials. Composite pipes are one such solution.
A method for encapsulating a blank during the manufacturing process of a clad tube, vacuum electron beam encapsulation [ see the following documents: the invention relates to a Li Smart, Li Relay Wei, Zengqifeng and the like, in particular to a zirconium alloy titanium alloy composite tube cladded by a nuclear fuel element and a preparation method thereof, wherein the Chinese patent publication No. CN 106078086A discloses 2016-11-09; secondly, Li Smart, Li Relay Wei, Zengqifeng and the like, a zirconium alloy titanium alloy composite tube cladded by a nuclear fuel element and a preparation method thereof, wherein the Chinese patent publication No. CN 106128532A discloses 2016-11-16; ③ West House electric company, Water reactor Fuel cladding tube, China invention patent publication No. CN 86101123A, published 1987-1-21], after combining tube blanks, adopting vacuum electron beam welding to keep the vacuum state between the tube blanks gaps. The method has the problems of high processing cost and limited tube blank size due to equipment size.
The metallurgical bonding thermal compounding method between metal layers of the composite pipe, the hot extrusion compounding method [ see the following documents: the invention relates to a Li Smart, Li Relay Wei, Zengqifeng and the like, in particular to a zirconium alloy titanium alloy composite tube cladded by a nuclear fuel element and a preparation method thereof, wherein the Chinese patent publication No. CN 106078086A discloses 2016-11-09; li Smart, Li Relay Wei, Mianqifeng and the like, a zirconium alloy titanium alloy composite pipe for cladding of nuclear fuel elements and a preparation method thereof, wherein the Chinese patent publication No. CN 106128532A, published as 2016-11-16, adopts a packaged pipe blank, is packaged with an inner protective sleeve and an outer protective sleeve, and is heated and then is subjected to hot extrusion processing by an extruder to realize metallurgical compounding. The method has the problems of uneven thickness of the inner layer and the outer layer and high equipment requirement.
The metallurgical bonding thermal compounding method between metal layers of the composite pipe, the hot rotary swaging metallurgical compounding method [ see the literature: liu Xinhua, XieXin, Liu Xuefeng and the like, a preparation method of a high-performance copper/titanium composite pipe, Chinese invention patent publication No. CN 103861888A, published Japanese 2014-06-18, wherein a core rod is inserted into a composite pipe blank, a rotary swaging method is adopted to apply large-pass deformation processing, and water spray cooling is carried out at a rotary swaging outlet, so that metallurgical compounding of the composite pipe is realized. The method has the problems of uneven thickness of the inner layer and the outer layer and poor quality of the inner surface of the tube blank.
Disclosure of Invention
The invention aims to provide a metal seamless composite tube of FeCrAl alloy and T91 ferrite/martensite heat-resistant steel for nuclear fuel cladding of a nuclear reactor and a preparation method thereof, wherein each layer of metal of the cladding tube has different application characteristics, and interlayer metallurgical bonding can improve the LOCA accident resistance of a pressurized water reactor fuel rod or improve the lead corrosion resistance and radiation swelling resistance of a lead-bismuth fast reactor fuel rod.
In order to achieve the purpose, the technical scheme of the invention is as follows:
a kind of nuclear reactor nuclear fuel cladding uses FeCrAl alloy and T91 ferrite/martensite heat-resisting steel composite tube, outer FeCrAl alloy tube and inner layer ferrite/martensite heat-resisting steel tube, form the metallurgical binding course directly between outer FeCrAl alloy tube and inner layer ferrite/martensite heat-resisting steel tube; or an Fe-based transition layer is adopted between the outer-layer FeCrAl alloy pipe and the inner-layer ferrite/martensite heat-resistant steel pipe, and the outer-layer FeCrAl alloy pipe and the inner-layer ferrite/martensite heat-resistant steel pipe respectively form a metallurgical bonding layer with the transition layer.
The FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor is characterized in that a metallurgical bonding layer contains the following elements: fe. One or more of Cr, Mn, Al, Mo, Nb, Ti, V, Si, C, N and rare earth elements.
The thickness of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor is 0.1-0.4 mm, the thickness of the outer FeCrAl alloy tube is 0.05-0.3 mm, the thickness of the metallurgical bonding layer is more than 0-0.1 mm, and the thickness of the transition layer is less than 50% of the thickness of the outer layer.
The preparation method of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor comprises the following steps of (1) forming the composite tube: the inner layer is made of ferrite/martensite heat-resistant steel material, the outer layer is made of FeCrAl alloy material, and an iron-based material auxiliary transition layer is arranged between the inner layer and the outer layer; (2) the preparation method of the metal seamless composite pipe for cladding comprises the following steps: polishing the surface of the seamless composite pipe blank → degassing assembly and packaging of the seamless composite pipe blank → metallurgical compounding of thermal deformation processing → annealing heat treatment → cold rolling and cold drawing and intermediate annealing → final heat treatment → straightening → cleaning → finished product inspection; the method comprises the steps of assembling an outer layer pipe, an intermediate transition layer pipe and an inner layer pipe, exhausting, assembling and packaging to form a seamless composite pipe blank, welding an end head for sealing, heating, forming a metallurgical composite seamless composite pipe by adopting a thermal deformation processing method, and finally processing to form a finished pipe with a required specification through cold deformation or thermal deformation.
The preparation method of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor comprises the following steps:
(a) preparation of seamless composite tube blank
Processing an outer layer FeCrAl alloy into a tube blank;
processing the inner layer ferrite/martensite heat-resistant steel into a pipe blank or a bar stock;
processing the iron-based material of the intermediate transition layer into a tube blank;
(b) surface polishing of seamless composite pipe blank
Respectively carrying out mechanical polishing treatment or chemical polishing treatment on the inner surface and the outer surface of the outer layer pipe, the middle transition layer pipe and the inner layer pipe or the surface of the inner layer rod to reach the surface roughness of Ra0.1 mu m and the clearance between the pipes of each layer is-0.1 mm-2 mm;
(c) assembly package of seamless composite tube blank
Assembling an outer layer tube, a middle transition layer tube and an inner layer ferrite/martensite heat-resistant steel tube or rod of FeCrAl alloy, removing gas in the middle of the tube blank, and immediately welding ends for sealing after exhausting;
(d) thermal deformation processing metallurgy composition
Heating and insulating a FeCrAl alloy outer layer pipe, a middle transition layer pipe and an inner layer ferrite/martensite heat-resistant steel pipe blank after exhausting and packaging, and realizing metallurgical compounding of the composite pipe under the action of high-temperature thermal diffusion and large-pressure deformation by adopting thermal deformation processing, wherein the thermal deformation method comprises hot rotary forging, hot precision forging, hot spinning, hot rolling or hot isostatic pressing;
(e) annealing heat treatment
The tube blank after metallurgical compounding is subjected to sectional heat preservation and heating, the cooling rate is controlled, the internal stress is removed, the tissue form is controlled, and the machinability is improved; and (3) keeping the heating temperature of 700-1000 ℃ for 30-60 minutes, keeping the temperature of the furnace to 300-600 ℃ for 30-90 minutes after cooling, and cooling in air.
The preparation method of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor comprises the steps that the outer layer FeCrAl alloy material in the step (a) is ferrite FeCrAl alloy or an improved type thereof, or oxide dispersion strengthening FeCrAl alloy; wherein the chemical composition of the FeCrAl alloy comprises: 12.0 to 20.0 weight percent of Cr, 4.0 to 7.0 weight percent of Al, 0 to 0.1 weight percent of C, 0.1 to 1.0 weight percent of Nb, 0 to 0.5 weight percent of V, 0.1 to 1.5 weight percent of Si, 0 to 1.5 weight percent of Mn and the balance of Fe; the ferrite/martensite heat-resistant steel in the step (a) is T91, P91 or modified type thereof or CLAM low activation martensite steel.
The preparation method of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor comprises the following steps of (c) assembling and packaging, wherein one of the following methods is adopted:
the method 1 comprises the steps of finishing interference assembly on a polished tube blank layer by layer; immersing the inner-layer tube into a low-temperature solution, wherein the low-temperature solution adopts a liquid nitrogen medium; the inner layer pipe shrinks at low temperature, after being cleaned, the outer layer pipe is assembled, when the room temperature is recovered, the interference assembly is achieved, the interference assembly is respectively realized on the double-layer or multi-layer composite pipe by the method, and the pipe blank is welded and packaged after the assembly;
the method 2, finish the drawing assembly layer by layer to the polished tube blank; after the outer layer pipe and the inner layer pipe are assembled, pipe reducing processing of the pipe heads is carried out at the same time; then, drawing with a core rod to reduce the wall and the diameter of the pipe, realizing exhaust assembly, and welding and packaging the assembled pipe blank;
step 3, after the polished tube blank is assembled layer by layer, reserving a vacuum exhaust tube in each tube gap, and welding and packaging; and after welding, performing vacuum pumping treatment by a vacuum pump, and welding and sealing the exhaust tube after vacuum pumping.
The preparation method of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor comprises the following steps of (d) carrying out hot deformation processing and metallurgical compounding, wherein one of the following methods is adopted:
the method 1 comprises the steps of putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and carrying out hot rolling processing, wherein the diameter is reduced by 1-6 mm, and the feeding speed is 0.2-2 m/min;
the method 2 comprises the steps of putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and carrying out hot rotary swaging and large deformation processing, wherein the diameter is reduced by 1-6 mm, and the feeding speed is 0.5-2 m/min;
the method 3, putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and carrying out hot spinning deformation processing to reduce the diameter by 1-6 mm and feed speed by 0.1-1 m/min;
the method 4 comprises the steps of putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and reducing the diameter by 1-6 mm through hot precision forging and large deformation processing at a feeding speed of 0.5-2 m/min;
and 5, compositely processing the tube blank subjected to exhaust packaging by adopting a hot isostatic pressing mode, wherein the heating temperature is 800-1200 ℃, the temperature is kept for 30-120 min, and the pressure is 100-300 MPa.
The preparation method of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor comprises the following steps of annealing heat treatment, cold rolling cold drawing and intermediate annealing treatment: performing cold rolling on the machined pipe blank by using a cold rolling pipe mill or cold drawing by using a drawing mill, and controlling the reducing and wall-reducing deformation of each pass of the cold rolling pipe, wherein the pass deformation is 5-50%; the intermediate annealing treatment in the cold rolling and cold drawing process of the metal seamless composite pipe adopts a vacuum gas quenching furnace or an atmosphere protection furnace, the heating temperature is 700-1000 ℃, the heat preservation time is 10-60 minutes, the heat preservation time is 30-90 minutes after the furnace is cooled to 300-600 ℃, and the gas is adopted for rapid cooling.
The preparation method of the FeCrAl alloy and T91 ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of the nuclear reactor comprises the following steps of cold rolling and cold drawing, intermediate annealing treatment, and final heat treatment: placing the final finished size pipe into a vacuum gas quenching heat treatment furnace for quenching and tempering heat treatment, and controlling the mechanical property and microstructure of the pipe; quenching and heating at 900-1050 ℃, preserving heat for 5-30 minutes, and cooling by inert gas; tempering and heating at 700-780 ℃, preserving heat for 30-150 minutes, and cooling by inert gas.
The invention has the advantages and beneficial effects that:
1. compared with a single-material seamless tube, the FeCrAl alloy and the T91 ferrite/martensite heat-resistant steel metal seamless composite tube combine the respective advantages of inner and outer layer metals, can improve the corrosion resistance, and simultaneously improve the high-temperature oxidation resistance and the irradiation resistance. The method has obvious effect on improving the safety and reliability of nuclear equipment and industrial equipment. The novel cladding tube is used for a pressurized water reactor, can improve the LOCA accident resistance of fuel rods, is used for a lead bismuth fast reactor, and can improve the lead bismuth corrosion resistance and the irradiation resistance.
2. In view of the defects of the processing technology of the existing single-layer alloy cladding tube and the composite tube, the metal seamless composite tube and the preparation process thereof of the invention have the advantages that the exhaust packaging method of the metal seamless composite tube comprises a drawing exhaust method and a low-temperature interference exhaust packaging method; the metallurgical compounding processing method of the metal seamless composite pipe comprises hot spinning compounding, hot rolling compounding and hot precision forging compounding.
Drawings
FIG. 1 is a longitudinal cross-sectional metallographic photograph of a FeCrAl (outer layer)/Fe alloy/T91 three-layer composite tube with a diameter of 9.5mm × 0.5mm manufactured by a drawing-degassing packaging method and a hot-spinning composite processing method in example 1 of the present invention.
FIG. 2 is a metallographic photograph of a longitudinal cross section of a FeCrAl (outer layer)/Fe alloy/T91 three-layer composite tube with a diameter of 9.5mm × 0.5mm manufactured by a hot-swaging compound processing method, a method for assembling exhaust gas encapsulation by low-temperature interference in example 2 of the present invention.
Detailed Description
In the specific implementation process, the composite pipe structure of the invention is as follows: the inner layer is made of ferrite/martensite heat-resistant steel material, the outer layer is made of FeCrAl alloy material, and an iron-based material auxiliary transition layer is arranged between the inner layer and the outer layer. The preparation method of the metal seamless composite pipe for cladding comprises the following steps: polishing the surface of the seamless composite pipe blank → assembling and packaging the seamless composite pipe blank → metallurgical compounding of thermal deformation processing → annealing heat treatment → cold rolling and cold drawing and intermediate annealing → final heat treatment → straightening → cleaning → inspection of finished products; the method comprises the steps of assembling an outer layer pipe, an intermediate transition layer pipe and an inner layer pipe, exhausting, assembling and packaging to form a seamless composite pipe blank, welding an end head for sealing, heating, performing thermal deformation processing to form a metallurgical composite seamless composite pipe, and finally performing cold deformation or thermal deformation processing to form a finished pipe with required specification.
The following will explain the seamless composite cladding tube for a pressurized water reactor, a lead-bismuth fast reactor and a sodium-cooled fast reactor and the preparation method thereof in detail with reference to specific examples, but the embodiments of the present invention are not limited to the following examples. The yield strength of the FeCrAl (outer layer)/T91 composite tube at room temperature is more than or equal to 350MPa, and the elongation is more than or equal to 15%.
Example 1:
the metal seamless composite tube of the embodiment is a three-layer composite of FeCrAl (outer layer)/Fe alloy (transition layer)/T91 (inner layer), and the FeCrAl alloy comprises the following components: 12.5 wt% of Cr, 4.2 wt% of Al, 0.3wt% of Nb and the balance of Fe; the transition layer is made of iron alloy and comprises the following components: 0.01wt% of C, 0.3wt% of Nb, 0.1wt% of Si, 0.2wt% of Mn0, and the balance of Fe; the inner layer is T91(P91) alloy. The specification is phi 9.5mm (outer diameter) multiplied by 0.5mm (wall thickness), and the main preparation process is as follows:
(1) polishing the tube blank: the inner and outer surfaces of the outer layer tube, the transition tube and the inner layer tube are respectively polished to Ra0.1 mu m, and the clearance between the tubes is about 0.1 mm.
(2) Assembling and packaging the tube blank: and (3) performing core rod drawing assembly on the polished FeCrAl, Fe alloy and T91 tube blanks layer by layer. And after the outer layer pipe and the inner layer pipe are assembled, pipe reducing processing of the pipe head is carried out at the same time. And then drawing the core rod to reduce the wall and the diameter of the pipe so as to realize exhaust assembly. And (5) welding and packaging the assembled pipe blank, wherein the outer diameter of the assembled pipe blank is 25 mm.
(3) The thermal compounding processing adopts a hot spinning method, and the assembled and packaged tube blank is put into a resistance furnace to be heated to 1200 ℃ and is kept warm for 20 minutes. After the core rod is inserted, the metallurgical compounding is realized through hot spinning deformation processing, and the feeding speed is 0.1 m/min. And (3) carrying out 5-pass hot spinning composite processing, reducing the diameter by 5mm in total, and processing into a composite pipe blank with the outer diameter of 20 mm.
(4) Annealing heat treatment: and (3) performing heat preservation and heating on the metallurgically compounded tube blank, preserving the heat at 800 ℃ for 1 hour, preserving the heat for 80 minutes after the temperature is reduced to 600 ℃ in a furnace, air-cooling, removing internal stress, controlling the tissue form and improving the processability.
(5) Cold rolling and intermediate annealing treatment: and (3) cold rolling the machined pipe blank by using a cold rolling pipe mill, and controlling the reduction of the diameter and the wall deformation of each pass. The intermediate annealing treatment adopts a vacuum gas quenching furnace, the annealing heating temperature is 800 ℃, the heat preservation time is 1 hour, the furnace is cooled to 600 ℃, the heat preservation time is 80 minutes, and the argon gas is cooled.
(6) Final heat treatment: and (3) placing the pipe with the final size into a vacuum gas quenching heat treatment furnace for quenching and tempering heat treatment, and controlling the mechanical property and the microstructure of the pipe. Keeping the quenching heating temperature at 1020 ℃ for 10 minutes, and cooling by argon; and (4) carrying out tempering heating at 700-780 ℃ for 90 minutes, and cooling with argon.
(7) Straightening is carried out after the heat treatment of the finished product, and a straightening machine is adopted for straightening.
(8) Cleaning and cleaning the inner surface and the outer surface of the straightened pipe to remove impurities and oil stains on the surface.
(9) And (4) carrying out ultrasonic nondestructive inspection on the cleaned composite pipe, and carrying out 100% nondestructive inspection on the processed composite pipe.
In this example, the composite tube prepared as FeCrAl (outer layer)/Fe alloy (transition layer)/T91 (inner layer) had an outer diameter of 9.5. + -. 0.03mm and a wall thickness of 0.5. + -. 0.03 mm. Wherein, the thickness of the inner layer is 0.30mm, the thickness of the outer layer is 0.14mm, and the thickness of the transition layer is 0.06 mm. The Fe alloy transition layer plays a role: during thermal compounding, the alloy is welded with the outer iron-chromium-aluminum alloy and the inner T91 alloy. Meanwhile, the transition layer plays a role in coordinating deformation during cold rolling and cold drawing deformation, and cold deformation processing is guaranteed. The outer layer and the inner layer respectively form a metallurgical bonding layer with the transition layer, and the thickness of the metallurgical bonding layer is about 0.015 mm.
TABLE 1 tensile Properties of three-layer metal composite tubes (FeCrAl (outer layer)/T91 (inner layer)) prepared in example 1
As shown in FIG. 1, a FeCrAl (outer layer)/Fe alloy (transition layer)/T91 (inner layer) three-layer composite tube having a diameter of 9.5X 0.5mm was produced in a quenched and tempered state. As can be seen from the metallographic photograph of the longitudinal section of the three-layer composite tube made of FeCrAl-Fe alloy-T91, the left side of the picture is made of the T91 alloy and the thickness of the left side of the picture is about 0.30mm, and the right side of the picture is made of the FeCrAl alloy and the thickness of the right side of the picture is about 0.14 mm. The middle layer is made of Fe alloy, the thickness of the middle layer is about 0.06mm, the interface between the three layers is well combined, and no crack or gap exists.
Example 2:
the metal seamless composite tube of the embodiment is a three-layer composite of FeCrAl (outer layer)/Fe alloy (transition layer)/T91 (inner layer), and the FeCrAl alloy comprises the following components: 13.1 wt% of Cr, 4.0 wt% of Al, 0.2wt% of V and the balance of Fe; the transition layer is made of iron alloy and comprises the following components: 0.005wt% of C, 0.3wt% of V, 0.15wt% of Si, 0.2wt% of Mn0, and the balance of Fe; the inner layer is T91(P91) alloy. The specification is phi 9.5mm (outer diameter) multiplied by 0.5mm (wall thickness), and the main preparation process is as follows:
(1) and (3) polishing the tube blank, namely polishing the inner surface and the outer surface of the outer layer tube, the transition tube and the inner layer tube respectively until Ra0.1 mu m and the clearance between the tubes is minus 0.1 mm.
(2) And assembling and packaging the tube blank. And (3) immersing the Fe alloy (transition layer) tube into a low-temperature liquid nitrogen solution, shrinking the transition tube at a low temperature, wiping, assembling the transition tube into an FeCrAl (outer layer) tube, and achieving interference assembly when the room temperature is recovered. Then, the T91 (inner layer) is immersed in a low-temperature liquid nitrogen solution, the T91 (inner layer) tube shrinks at low temperature, and after wiping, the tube is assembled into a FeCrAl (outer layer)/Fe alloy (transition layer) double-layer tube. And (5) welding and packaging the assembled pipe blank, wherein the outer diameter of the assembled pipe blank is 25 mm.
(3) The hot composite processing adopts a hot rotary swaging method, the assembled and packaged tube blank is put into a resistance furnace to be heated to 1200 ℃, the temperature is kept for 20 minutes, and the tube blank is subjected to hot rotary swaging deformation processing, the diameter is reduced by 4mm, and the feeding speed is 0.2 m/min.
(4) Annealing treatment: and (3) performing heat preservation and heating on the metallurgically compounded tube blank, preserving the heat at 800 ℃ for 1 hour, preserving the heat for 80 minutes after the temperature is reduced to 600 ℃ in a furnace, air-cooling, removing internal stress, controlling the tissue form and improving the processability.
(5) Cold rolling and intermediate annealing treatment: and (3) cold rolling the machined pipe blank by using a cold rolling pipe mill, and controlling the reduction of the diameter and the wall deformation of each pass. The intermediate annealing adopts a vacuum gas quenching furnace, the annealing heating temperature is 800 ℃, the temperature is kept for 1 hour, the furnace is cooled to 600 ℃, the temperature is kept for 80 minutes, and the air cooling is carried out.
(6) And finally, placing the pipe with the final size after heat treatment into a vacuum gas quenching heat treatment furnace for quenching and tempering heat treatment, and controlling the mechanical property and the microstructure of the pipe. The quenching heating temperature is 1050 ℃, the temperature is kept for 10 minutes, and argon is used for cooling; tempering and heating at 720 ℃, preserving the temperature for 90 minutes, and cooling by argon.
(7) Straightening is carried out after the heat treatment of the finished product, and a straightening machine is adopted for straightening.
(8) Cleaning and cleaning the inner surface and the outer surface of the straightened pipe to remove impurities and oil stains on the surface.
(9) And (4) carrying out ultrasonic nondestructive inspection on the cleaned composite pipe, and carrying out 100% nondestructive inspection on the processed composite pipe.
As shown in FIG. 2, a FeCrAl (outer layer)/Fe alloy (transition layer)/T91 (inner layer) three-layer composite tube having a diameter of 9.5X 0.51mm was manufactured in a cold-rolled state. As can be seen from the metallographic photograph of the longitudinal section of the three-layer composite tube made of FeCrAl-Fe alloy-T91, the left side of the picture is made of the T91 alloy and the thickness of the left side of the picture is about 0.34mm, and the right side of the picture is made of the FeCrAl alloy and the thickness of the right side of the picture is about 0.15 mm. The middle layer is made of Fe alloy, the thickness of the middle layer is about 0.015-0.020 mm, the interface between the three layers is well combined, and cracks and gaps do not exist.
The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention in further detail, and it should be understood that the above-mentioned embodiments are only illustrative of the present invention and are not intended to limit the scope of the present invention, and any modifications, equivalents, improvements and the like made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. A FeCrAl alloy and ferrite/martensite heat-resistant steel composite tube for nuclear fuel cladding of a nuclear reactor is characterized in that: adopting an Fe-based transition layer between the outer-layer FeCrAl alloy pipe and the inner-layer ferrite/martensite heat-resistant steel pipe, and forming a metallurgical bonding layer between the outer-layer FeCrAl alloy pipe and the inner-layer ferrite/martensite heat-resistant steel pipe and the transition layer respectively; the metallurgical bonding layer is formed by adopting thermal deformation processing, the FeCrAl alloy outer layer pipe, the middle transition layer pipe and the inner layer ferrite/martensite heat-resistant steel pipe blank are heated and insulated after being exhausted and packaged, the metallurgical compounding of the composite pipe is realized under the high-temperature thermal diffusion action and the large-pressure deformation action by adopting the thermal deformation processing, and the thermal deformation method comprises hot rotary forging, hot precision forging, hot spinning, hot rolling or hot isostatic pressing;
wherein the chemical composition of the FeCrAl alloy comprises: 12.0-20.0 wt% of Cr, 4.0-7.0 wt% of Al, 0-0.1 wt% of C, 0.1-1.0 wt% of Nb, 0-0.5 wt% of V, 0.1-1.5 wt% of Si, 0-1.5 wt% of Mn and the balance of Fe; the ferrite/martensite heat-resistant steel is T91, P91 or modified type thereof or CLAM low activation martensite steel; the Fe-based transition layer is an iron alloy and comprises the following chemical components: 0.01wt% of C, 0.3wt% of Nb, 0.1wt% of Si, 0.2wt% of Mn0, and the balance of Fe; or the Fe-based transition layer is an iron alloy and comprises the following chemical components: 0.005wt% of C, 0.3wt% of V, 0.15wt% of Si, 0.2wt% of Mn0, and the balance of Fe.
2. A FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for nuclear fuel cladding for a nuclear reactor as recited in claim 1 wherein the metallurgical bonding layer comprises elements including: fe. One or more of Cr, Mn, Al, Mo, Nb, Ti, V, Si, C, N and rare earth elements.
3. The FeCrAl alloy and ferrite/martensite heat-resistant steel composite tube for the nuclear fuel cladding of a nuclear reactor as set forth in claim 1, wherein the thickness of the ferrite/martensite heat-resistant steel tube as the inner layer is 0.1mm to 0.4mm, the thickness of the FeCrAl alloy tube as the outer layer is 0.05 mm to 0.3mm, the thickness of the metallurgical bonding layer is more than 0mm to 0.1mm, and the thickness of the transition layer is less than 50% of the thickness of the outer layer.
4. A method of making a FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for nuclear fuel cladding for a nuclear reactor according to any of claims 1 to 3, wherein (1) the composite tube has the following structure: the inner layer is made of ferrite/martensite heat-resistant steel material, the outer layer is made of FeCrAl alloy material, and an iron-based material auxiliary transition layer is arranged between the inner layer and the outer layer; (2) the preparation method of the metal seamless composite pipe for cladding comprises the following steps: polishing the surface of the seamless composite pipe blank → degassing assembly and packaging of the seamless composite pipe blank → metallurgical compounding of thermal deformation processing → annealing heat treatment → cold rolling and cold drawing and intermediate annealing → final heat treatment → straightening → cleaning → finished product inspection; the method comprises the steps of assembling an outer layer pipe, an intermediate transition layer pipe and an inner layer pipe, exhausting, assembling and packaging to form a seamless composite pipe blank, welding an end head for sealing, heating, forming a metallurgical composite seamless composite pipe by adopting a thermal deformation processing method, and finally processing to form a finished pipe with a required specification through cold deformation or thermal deformation.
5. The method of making a FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for nuclear fuel cladding for a nuclear reactor of claim 4, comprising the steps of:
(a) preparation of seamless composite tube blank
Processing an outer layer FeCrAl alloy into a tube blank;
processing the inner layer ferrite/martensite heat-resistant steel into a pipe blank or a bar stock;
processing the iron-based material of the intermediate transition layer into a tube blank;
(b) surface polishing of seamless composite pipe blank
Respectively carrying out mechanical polishing treatment or chemical polishing treatment on the inner surface and the outer surface of the outer layer pipe, the middle transition layer pipe and the inner layer pipe or the surface of the inner layer rod to reach the surface roughness of Ra0.1 mu m and the clearance between the pipes of each layer is-0.1 mm-2 mm;
(c) assembly package of seamless composite tube blank
Assembling an outer layer tube, a middle transition layer tube and an inner layer ferrite/martensite heat-resistant steel tube or rod of FeCrAl alloy, removing gas in the middle of the tube blank, and immediately welding ends for sealing after exhausting;
(d) thermal deformation processing metallurgy composition
Heating and insulating a FeCrAl alloy outer layer pipe, a middle transition layer pipe and an inner layer ferrite/martensite heat-resistant steel pipe blank after exhausting and packaging, and realizing metallurgical compounding of the composite pipe under the action of high-temperature thermal diffusion and large-pressure deformation by adopting thermal deformation processing, wherein the thermal deformation method comprises hot rotary forging, hot precision forging, hot spinning, hot rolling or hot isostatic pressing;
(e) annealing heat treatment
The tube blank after metallurgical compounding is subjected to sectional heat preservation and heating, the cooling rate is controlled, the internal stress is removed, the tissue form is controlled, and the machinability is improved; and (3) keeping the heating temperature of 700-1000 ℃ for 30-60 minutes, keeping the temperature of the furnace to 300-600 ℃ for 30-90 minutes, and cooling in air.
6. A method of producing a FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for nuclear fuel cladding for a nuclear reactor as claimed in claim 5, wherein the outer layer FeCrAl alloy material of step (a) is a ferritic FeCrAl alloy or a modified form thereof, or an oxide dispersion strengthened FeCrAl alloy.
7. The method of forming a FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for a nuclear fuel cladding for a nuclear reactor of claim 5, wherein the assembling and packaging of step (c) is performed by one of the following methods:
the method 1 comprises the steps of finishing interference assembly on a polished tube blank layer by layer; immersing the inner-layer tube into a low-temperature solution, wherein the low-temperature solution adopts a liquid nitrogen medium; the inner layer pipe shrinks at low temperature, after being cleaned, the outer layer pipe is assembled, when the room temperature is recovered, the interference assembly is achieved, the interference assembly is respectively realized on the double-layer or multi-layer composite pipe by the method, and the pipe blank is welded and packaged after the assembly;
the method 2, finish the drawing assembly layer by layer to the polished tube blank; after the outer layer pipe and the inner layer pipe are assembled, pipe reducing processing of the pipe heads is carried out at the same time; then, drawing with a core rod to reduce the wall and the diameter of the pipe, realizing exhaust assembly, and welding and packaging the assembled pipe blank;
step 3, after the polished tube blank is assembled layer by layer, reserving a vacuum exhaust tube in each tube gap, and welding and packaging; and after welding, performing vacuum pumping treatment by a vacuum pump, and welding and sealing the exhaust tube after vacuum pumping.
8. The method of forming a FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for nuclear fuel cladding of a nuclear reactor of claim 5, wherein the hot deformation process metallurgical compounding of step (d) is performed by one of the following methods:
the method 1 comprises the steps of putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and carrying out hot rolling processing, wherein the diameter is reduced by 1-6 mm, and the feeding speed is 0.2-2 m/min;
the method 2 comprises the steps of putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and carrying out hot rotary swaging and large deformation processing, wherein the diameter is reduced by 1-6 mm, and the feeding speed is 0.5-2 m/min;
the method 3, putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and carrying out hot spinning deformation processing to reduce the diameter by 1-6 mm and feed speed by 0.1-1 m/min;
the method 4 comprises the steps of putting the assembled and packaged tube blank into a resistance furnace for heating or induction heating, heating to 800-1200 ℃, preserving heat for 3-30 min, and reducing the diameter by 1-6 mm through hot precision forging and large deformation processing at a feeding speed of 0.5-2 m/min;
and 5, compositely processing the tube blank subjected to exhaust packaging by adopting a hot isostatic pressing mode, wherein the heating temperature is 800-1200 ℃, the heat preservation time is 30-120 min, and the pressure is 100-300 MPa.
9. A method of manufacturing a FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for nuclear fuel cladding of a nuclear reactor according to claim 5, characterized in that after the annealing heat treatment, a cold rolling cold drawing and intermediate annealing treatment are performed: performing cold rolling on the machined pipe blank by using a cold rolling pipe mill or cold drawing by using a drawing mill, and controlling the reducing and wall-reducing deformation of each pass of the cold rolling pipe, wherein the pass deformation is 5-50%; the intermediate annealing treatment in the cold rolling and cold drawing process of the metal seamless composite pipe adopts a vacuum gas quenching furnace or an atmosphere protection furnace, the heating temperature is 700-1000 ℃, the heat preservation time is 10-60 minutes, the heat preservation time is 30-90 minutes after the furnace is cooled to 300-600 ℃, and the gas is adopted for rapid cooling.
10. A method of manufacturing a FeCrAl alloy and ferrite/martensite heat resistant steel composite tube for nuclear fuel cladding of a nuclear reactor according to claim 9, characterized in that after cold rolling cold drawing and intermediate annealing treatment, final heat treatment is performed: placing the final finished size pipe into a vacuum gas quenching heat treatment furnace for quenching and tempering heat treatment, and controlling the mechanical property and microstructure of the pipe; quenching and heating at 900-1050 ℃, preserving heat for 5-30 minutes, and cooling by inert gas; tempering and heating at 700-780 ℃, preserving heat for 30-150 minutes, and cooling by inert gas.
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