CN110451968B - Nuclear fuel cladding tube and preparation method thereof - Google Patents

Nuclear fuel cladding tube and preparation method thereof Download PDF

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CN110451968B
CN110451968B CN201810430076.6A CN201810430076A CN110451968B CN 110451968 B CN110451968 B CN 110451968B CN 201810430076 A CN201810430076 A CN 201810430076A CN 110451968 B CN110451968 B CN 110451968B
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carbon
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CN110451968A (en
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黄庆
邵俊琦
袁钦
王霁
周小兵
何流
都时禹
黄峰
黄政仁
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Ningbo Institute of Material Technology and Engineering of CAS
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Abstract

The invention provides a nuclear fuel cladding tube, which is made of an aluminum-silicon-carbon ceramic material or an aluminum-silicon-carbon ceramic-based composite material, or the surface coating of the nuclear fuel cladding tube is made of the aluminum-silicon-carbon ceramic material or the aluminum-silicon-carbon ceramic-based composite material. Wherein, the structural general formula of the aluminum silicon carbon ceramic material is (Al)4C3)n(SiC)mWherein n denotes Al in AlSiC4C3The number of layers of (2) is a natural number; m denotes the number of SiC layers in the AlSiC unit cell and is a natural number. The nuclear fuel cladding tube can meet the performance requirements of structural elements in a fourth generation fission reactor nuclear energy system on high temperature resistance, corrosion resistance, oxidation resistance, neutron irradiation resistance, good neutron irradiation stability and the like, and has a good application prospect.

Description

Nuclear fuel cladding tube and preparation method thereof
Technical Field
The invention relates to the field of nuclear energy key structural materials, in particular to a nuclear fuel cladding tube and a preparation method thereof.
Background
The nuclear energy is an efficient, economic and clean energy source, and through the development of nearly 70 years, the research of the fourth generation nuclear reactor is deepened gradually. In order to improve the energy conversion efficiency, the temperature of the reactor core in the nuclear reactor reaches over 1000 ℃.
The nuclear fuel cladding tube is one of the most harsh important parts in the core structure, and not only is the nuclear fuel directly contacted, but also the nuclear fuel needs to have good high temperature resistance and radiation resistance, and is also the nuclear fuel cladding tube directly contacted with a coolant, such as supercritical water, molten villiaumite, a lead bismuth coolant and the like, under high temperature and high pressure, and the corrosion resistance is required to be excellent. Thus, nuclear fuel cladding materials need to be resistant to high temperatures, corrosion, oxidation, neutron irradiation and good neutron irradiation stability (low radiation swelling and low radiation brittleness). Currently, most nuclear fuel cladding components use zirconium alloys as the preferred material, such as low tin zirconium-4 alloy, Zirlo developed by westinghouse, usaTMAlloys, the NDA and MDA alloys of japan, the M5 alloy of france, and the E635 alloy of soviet union, and the like. However, the zirconium alloy is often reduced in plasticity and becomes brittle after being subjected to neutron irradiation in the reactor, so that irradiation swelling and even distortion deformation occur, the service cycle is short, about 1-1.5 years, frequent replacement is required, and the operating cost of the nuclear reactor is greatly increased. More importantly, the zirconium alloy and water can react with each other at high temperature to generate hydrogen, which is easy to cause hydrogen explosion, and is one of the important reasons of nuclear accidents in the field of Japan Fushima.
Disclosure of Invention
Aiming at the defects of the zirconium alloy as the material of the nuclear fuel cladding element, the invention provides the nuclear fuel cladding tube which has the performances of high temperature resistance, corrosion resistance, oxidation resistance, neutron irradiation resistance and the like.
The technical scheme of the invention is as follows: a nuclear fuel cladding tube, characterized by: the nuclear fuel cladding tube is made of aluminum-silicon-carbon ceramic materials.
The aluminum silicon carbon ceramic material is made of (Al)4C3)n(SiC)mStructural assemblyThe aluminum-silicon-carbon phase material has a layered structure and the general structural formula of the aluminum-silicon-carbon phase material is (Al)4C3)n(SiC)mWherein n denotes Al in AlSiC4C3The number of layers of (2) is a natural number; m denotes the number of SiC layers in the AlSiC unit cell and is a natural number. For example, when n is 1 and m is 1, the silicon carbon ceramic material is composed of a layer of Al4C3Alternately stacked with a layer of SiC, the general formula of the structure is Al4SiC4(ii) a When n is 2 and m is 1, the Al-Si-C ceramic material is formed by two layers of Al4C3Alternately stacked with a layer of SiC, the general formula of the structure is Al8SiC7(ii) a When n is 1 and m is 2, the Al-Si-C ceramic material is formed by a layer of Al4C3Alternately stacked with two layers of SiC, and the general structural formula is Al4Si2C5。
The invention also provides a method for preparing the nuclear fuel cladding tube, which comprises the steps of reacting reactants to generate aluminum silicon carbon ceramic powder, forming the powder into a nuclear fuel cladding tube shape, and finally sintering to obtain the fuel cladding tube.
The reactant can be metal aluminum powder and ceramic precursor polycarbosilane, and the reactants react to generate aluminum silicon carbon ceramic powder. Wherein the ceramic precursor polycarbosilane may contain foreign elements such as Al, Ti, Zr, Hf, Ta, Y, B, N, and the like.
The reactant can be alumina, silicon oxide, silicon carbide and carbon powder, and the reactants react to generate the aluminum-silicon-carbon ceramic powder.
The reactants can be metal aluminum powder, silicon powder and graphite, and the reactants react to generate aluminum silicon carbon ceramic powder.
The reactant may be Al4C3And SiC, and the reactants react to generate the aluminum silicon carbon ceramic powder.
The sintering method is not limited and includes conventional resistance sintering, microwave sintering, hot-pressing sintering, rapid sintering by spark plasma and the like.
In view of the intrinsic brittleness of the ceramic material, the nuclear fuel cladding tube according to the invention is preferably an aluminium silicon carbon ceramic based composite material comprising a reinforcement phase as a matrix in said aluminium silicon carbon ceramic material.
Preferably, the mass of the reinforcing phase accounts for 0.01-99.5 wt% of the mass of the aluminum-silicon-carbon ceramic material.
The reinforcing phase is not limited and may be silicon carbide fiber (SiC fiber, SiC for short)f) Silicon carbide particles (SiC particles, SiC for short), silicon carbide whiskers (SiC whisker, SiC for short)w) Carbon fiber (Carbon fiber, abbreviated as C)f) Zirconium carbide (ZrC), titanium carbide (TiC), titanium silicon carbon (Ti)3SiC2) Titanium aluminum carbon (Ti)3AlC2) And the like, or a combination of two or more thereof.
The invention also provides a method for preparing the nuclear fuel cladding tube, which comprises the steps of mixing the reinforcing phase with reactants, wherein the reactants react to generate aluminum silicon carbon ceramic powder, and the mixture reacts to generate composite powder of the reinforcing phase and the aluminum silicon carbon ceramic; and then forming the composite powder into a nuclear fuel cladding tube shape, and finally sintering to obtain the fuel cladding tube.
Preferably, the reinforcing phase is silicon carbide fiber (SiC fiber), silicon carbide whisker (SiC whisker), or Carbon fiber (Carbon fiber). At this time, as one implementation, the method for preparing the nuclear fuel cladding tube includes the steps of:
(1) pre-weaving silicon carbide fibers, silicon carbide whiskers or carbon fibers into a tubular preform according to the structure of the nuclear fuel cladding tube; uniformly mixing reactants to prepare slurry;
(2) impregnating the slurry into a tubular preform;
(3) calcining the impregnated tubular prefabricated member at high temperature;
(4) and (4) repeating the step (3) for a plurality of times until the relative density of the tubular prefabricated member after high-temperature calcination is higher than 70 percent, thus obtaining the nuclear fuel cladding tube.
In the step (3), the sintering method is not limited, and includes conventional resistance sintering, microwave sintering, hot-pressing sintering, rapid spark plasma sintering and the like.
Compared with the prior art, the invention selects the aluminum silicon carbon ceramic material as the nuclear fuel cladding tube, and has the following beneficial effects:
(1) the aluminum-silicon-carbon ceramic material has good high-temperature mechanical property, and the high-temperature bending strength of the aluminum-silicon-carbon ceramic material is 50% higher than the room-temperature bending strength; in addition, the aluminum-silicon-carbon ceramic material has excellent high-temperature oxidation resistance, and can form a compact alumina and mullite protective film on the surface in a high-temperature oxidation atmosphere, inhibit further oxidation in the aluminum-silicon-carbon ceramic material and be still stably used in a high-temperature oxidation environment at 1800 ℃; in addition, the aluminum silicon carbon ceramic material has good heat conductivity, and the heat conductivity can reach 80 W.m-1·K-1(ii) a Meanwhile, the aluminum-silicon-carbon ceramic material also has stronger corrosion resistance and irradiation resistance, and is similar to silicon carbide; finally, the unique layered structure of the material also enables the material to have good thermal shock resistance and certain damage tolerance. The nuclear fuel cladding tube made of the aluminum-silicon-carbon ceramic material can meet the performance requirements of structural elements in a fourth generation fission reactor nuclear energy system on high temperature resistance, corrosion resistance, oxidation resistance, neutron irradiation resistance, good neutron irradiation stability and the like, and has a good application prospect.
(2) In consideration of the intrinsic brittleness of the ceramic material, the aluminum-silicon-carbon ceramic-based composite material containing the reinforcing phase is selected, so that the reliability and the safety of the nuclear fuel cladding tube are further improved.
(3) Considering the condition that the nuclear fuel cladding tube is provided with the surface coating, the surface coating can be made of aluminum silicon carbon ceramics and composite materials thereof and is used for enhancing the high temperature resistance, corrosion resistance, oxidation resistance and neutron irradiation resistance of the cladding tube matrix.
Drawings
FIG. 1 shows Al in example 1 of the present invention4SiC4XRD pattern of the/SiC composite material;
FIG. 2 shows Al in example 1 of the present invention4SiC4SEM pictures of fracture surfaces of the/SiC composite material;
FIG. 3 shows SiC in example 3 of the present inventionf/Al4SiC4Fracture SE photograph of composite material.
Detailed Description
Example 1:
in this example, the nuclear fuel cladding is silicon carbide (SiC) and aluminum silicon carbon ceramic (Al)4SiC4) Composite material (Al)4SiC4/SiC), the preparation steps are as follows:
(1) and (3) performing cross-linking curing treatment on the silicon carbide and precursor Polycarbosilane (PCS) for 1h at the temperature of 600 ℃ under the argon protective atmosphere to obtain PCS-600 powder.
(2) And (3) carrying out ball milling on an appropriate amount of PCS-600 powder and Al powder, uniformly mixing, drying in vacuum, and carrying out cracking treatment for 2h at 1100 ℃ under the protection of argon.
(3) Performing the mixed powder obtained in the step 2 into the shape of a nuclear fuel cladding tube, and then hot-pressing and sintering at 1700 ℃ for 20min to obtain Al4SiC4A nuclear fuel cladding tube made of/SiC composite material.
Al prepared as described above is shown in FIG. 14SiC4XRD pattern of/SiC nuclear fuel cladding tube can show that the composite material is made of Al4SiC4And SiC, wherein Al4SiC4Is the main phase.
FIG. 2 shows Al obtained as described above4SiC4SEM image of cross section of/SiC nuclear fuel cladding tube, wherein the flaky large crystal grains are Al4SiC4And the smaller size grains are SiC. FIG. 3 shows that the composite material has a compact structure, pores are difficult to find, and Al4SiC4It appears as a transgranular fracture, while SiC is primarily a perigranular fracture.
Example 2:
in this example, the nuclear fuel cladding is silicon carbide (SiC) and aluminum silicon carbon ceramic (Al)4SiC4) Composite material Al of4SiC4Of the structure of/SiC, Al4SiC4the/SiC composite material is prepared by reacting liquid hyperbranched polycarbosilane (LHBPCS) and aluminum powder, and the preparation method comprises the following specific steps:
(1) mixing LHBPCS and a proper amount of aluminum powder, and curing for 2 hours in vacuum at 100 ℃ under the combined action of an initiator tert-butyl peroxybenzoate (TBPB);
(2) grinding the block solidified in the step 1 into powder, and cracking for 1h at 1200 ℃ in an argon protective atmosphere;
(3) performing the powder cracked in the step 2 into a nuclear fuel cladding tube shape, and then performing discharge plasma sintering at 1600 ℃ for 10min to obtain Al4SiC4A nuclear fuel cladding tube made of/SiC composite material.
Al obtained as described above4SiC4Phase composition of the/SiC nuclear fuel cladding tube is similar to that of fig. 1, mainly Al4SiC4A phase and a SiC phase; the microscopic morphology of the cross section is similar to that of FIG. 2, which shows that the structure is compact, the pores are few, and the Al is flaky and large-grain4SiC4Phase dispersed in SiC phase, Al4SiC4It appears as a transgranular fracture, while SiC is primarily a perigranular fracture.
Example 3:
in this example, the nuclear fuel cladding is silicon carbide (SiC)f) With aluminium-silicon-carbon ceramic materials (Al)4SiC4) Composite material Al of4SiC4/SiCfThe preparation method comprises the following steps:
(1) mixing liquid hyperbranched polycarbosilane (LHBPCS) and a proper amount of aluminum powder, and preparing slurry through ultrasonic dispersion and ball milling;
(2) SiC was added according to the structure of the nuclear fuel cladding tubefPre-weaving into a tubular prefabricated part, and soaking the slurry prepared in the step 1 into the tubular prefabricated part for 12 hours while applying pressure of 5 MPa;
(3) impregnating SiCfCracking the tubular prefabricated part at 1600 ℃ for 2h under the argon protective atmosphere;
(4) repeating the step (3) for 5-10 times to obtain the high-density Al4SiC4/SiCfConstituting a nuclear fuel cladding tube.
Al obtained as described above4SiC4/SiCfThe phase composition of the nuclear fuel cladding tube is similar to that of fig. 1, mainly consisting of Al4SiC4Phase and SiC phase.
FIG. 3 shows Al obtained as described above4SiC4/SiCfFracture SEM photograph of nuclear fuel cladding tubeIt can be seen that the composite material is very dense and has a partial fiber pull-out phenomenon.
Example 4:
in this example, the nuclear fuel cladding tube is silicon carbide whisker (SiC)w) With aluminium-silicon-carbon ceramic materials (Al)4SiC4) Composite material Al of4SiC4/SiCwThe preparation method comprises the following steps:
(1) mixing liquid hyperbranched polycarbosilane (LHBPCS) and proper amount of aluminum powder and silicon carbide crystal whisker (SiC)w) Mixing, ultrasonically dispersing, and ball-milling to prepare slurry;
(2) curing the slurry prepared in the step 1 for 2 hours in vacuum at 100 ℃, and grinding the obtained block into powder;
(3) cracking the powder in the step 2 for 1h at 1100 ℃ under the argon protective atmosphere;
(4) performing the powder cracked in the step 3 into a nuclear fuel cladding tube shape, and then performing discharge plasma sintering at 1600 ℃ for 10min to obtain Al4SiC4/SiCwConstituting a nuclear fuel cladding tube.
Al obtained as described above4SiC4/SiCwThe phase composition of the nuclear fuel cladding tube is similar to that of fig. 1, mainly consisting of Al4SiC4Phase and SiC phase. Al obtained as described above4SiC4/SiCwThe fracture morphology of the nuclear fuel cladding was similar to that of figure 3, showing that the composite was very dense with partial whisker pull-out.
Example 5:
in the present embodiment, the nuclear fuel cladding is carbon fiber (C)f) With aluminium-silicon-carbon ceramic materials (Al)4SiC4) Composite material Al of4SiC4/CfThe preparation method comprises the following steps:
(1) dissolving polycarbosilane in xylene, and ball-milling and mixing the polycarbosilane and a proper amount of aluminum powder to prepare slurry;
(2) according to the structure of the nuclear fuel cladding tube, CfPre-weaving into a tubular prefabricated member, and soaking the slurry prepared in the step 1 in the tubular prefabricated member for 20 hours while applying a pressure of 3 MPa;
(3) impregnating CfThe tubular prefabricated part is cracked for 2 hours at the high temperature of 1500 ℃ under the argon protective atmosphere, and Al can be obtained4SiC4/CfA nuclear fuel cladding tube;
(4) repeating the step (3) for 5-10 times to obtain the high-density Al4SiC4/CfA nuclear fuel cladding tube.
Al obtained as described above4SiC4/CfThe phase composition of the nuclear fuel cladding tube is mainly composed of C and Al4SiC4The phase composition has fracture morphology similar to that of FIG. 3, is very compact, and has partial fiber extraction phenomenon.
Example 6:
in this embodiment, the nuclear fuel cladding is made of Al-Si-C ceramic material4SiC4The preparation method comprises the following steps:
(1) and (3) ball-milling and uniformly mixing a proper amount of precursor polycarbosilane PCS powder and Al powder, drying in vacuum, and cracking at 1100 ℃ for 2h under the protection of argon.
(2) Performing the powder obtained in the step 1 into the shape of a nuclear fuel cladding tube, and then hot-pressing and sintering at 1700 ℃ for 20min to obtain Al4SiC4A nuclear fuel cladding of material.
Al obtained from the above4SiC4XRD pattern of nuclear fuel cladding tube can show that the cladding tube is made of Al4SiC4Phase composition. Al obtained as described above4SiC4SEM photographs of sections of the nuclear fuel cladding tubes showed sheet-like structures, showing fracture modes of both transgranular fracture and intergranular fracture.
The above embodiments are described in detail to explain the technical solutions and product features of the present invention, and it should be understood that the above embodiments are only specific examples of the present invention and are not intended to limit the present invention, and any modifications and improvements made within the scope of the principles of the present invention should be included in the protection scope of the present invention.

Claims (6)

1. A method for preparing a nuclear fuel cladding tube, which is characterized by comprising the following steps: the nuclear fuel cladding tube is made of an aluminum-silicon-carbon ceramic matrix composite;
the aluminum-silicon-carbon ceramic matrix composite takes an aluminum-silicon-carbon ceramic material as a matrix, and contains a reinforcing phase;
the structural general formula of the aluminum-silicon-carbon ceramic material is (Al)4C3）n（SiC）mWherein n denotes Al in AlSiC4C3The number of layers of (2) is a natural number greater than 1; m represents the number of SiC layers in the aluminum-silicon-carbon unit cell and is a natural number greater than 1;
crosslinking and curing the reinforced phase and the precursor polycarbosilane in a protective atmosphere to obtain powder; mixing the powder with aluminum powder, drying, and then cracking at 1100-1200 ℃ in a protective atmosphere; and forming the cracked powder into a nuclear fuel cladding tube shape, and finally sintering at 1600-1700 ℃ to obtain the nuclear fuel cladding tube.
2. The method of preparing a nuclear fuel cladding as set forth in claim 1, wherein: the ceramic precursor polycarbosilane comprises one or more of heterogeneous elements of Al, Ti, Zr, Hf, Ta, Y, B and N.
3. The method of preparing a nuclear fuel cladding as set forth in claim 1, wherein: the reinforcing phase is one or the combination of more than two of silicon carbide fiber, silicon carbide particle, silicon carbide whisker, carbon fiber, zirconium carbide, titanium silicon carbon and titanium aluminum carbon.
4. The method of manufacturing a nuclear fuel cladding as set forth in claim 2, wherein: the reinforcing phase is one or the combination of more than two of silicon carbide fiber, silicon carbide particle, silicon carbide whisker, carbon fiber, zirconium carbide, titanium silicon carbon and titanium aluminum carbon.
5. A nuclear fuel cladding tube produced by the production method according to any one of claims 1 to 4, having a surface coating layer; the surface coating is made of an aluminum-silicon-carbon ceramic material; or the surface coating is made of an aluminum-silicon-carbon ceramic matrix composite material, and the aluminum-silicon-carbon ceramic matrix composite material takes an aluminum-silicon-carbon ceramic material as a matrix and contains a reinforcing phase;
the structural general formula of the aluminum-silicon-carbon ceramic material for the surface coating is (Al)4C3）n（SiC）mWherein n denotes Al in AlSiC4C3The number of layers of (2) is a natural number greater than 1; m represents the number of SiC layers in the AlSiC unit cell and is a natural number greater than 1.
6. The nuclear fuel cladding tube of claim 5 wherein: the reinforcing phase in the aluminum-silicon-carbon ceramic-based composite material for the surface coating is one or the combination of more than two of silicon carbide fiber, silicon carbide particle, silicon carbide whisker, carbon fiber, zirconium carbide, titanium-silicon-carbon and titanium-aluminum-carbon.
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