CN106929706A - A kind of zirconium-base alloy in the hot environment for nuclear reactor - Google Patents
A kind of zirconium-base alloy in the hot environment for nuclear reactor Download PDFInfo
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- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
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- C22C16/00—Alloys based on zirconium
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Abstract
The present invention provides the zirconium-base alloy in a kind of hot environment for nuclear reactor, and calculated in weight percent, it includes：Sn：0.36~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%；Individually 0.01~0.09%Cu of addition or compound adds 0.01~0.09%Cu and 0.01~0.20%V；Balance of comprising impurity at least 98% zirconium.Provided by the present invention for the zirconium-base alloy in nuclear reactor hot environment, with excellent decay resistance, the alloy is compared with the ZIRLO alloys of prior art, there is more excellent decay resistance in high temperature pure water and high temperature, it is adaptable to corrosion-resistant zircaloy of the nuclear reactor compared with the fuel rod clad material under high burnup, screen work band and structural member in water containing lithium.
Description
Technical field
The present invention relates to Zirconium alloy material field, more particularly, to a kind of PWR nuclear power plant that can be used as compared with high burnup
The corrosion-resistant zircaloy containing Cu of fuel rod clad material, screen work band and structural member.
Background technology
Zircaloy because thermal neutron absorption cross section is small, thermal conductivity is high, good mechanical property, and with good processing characteristics with
And same UO2Compatibility is good, especially also has good corrosion resistance and enough heat resistances to high-temperature water, high-temperature vapor,
Therefore it is widely used as the cladding materials and core structural material of water-cooled power reactor.With power producer technology towards raising
Fuel burn-up and extension refulling cycle direction are developed, and requirement higher is proposed to can zircaloy.Therefore, being permitted
Many countries are all in research and development novel zirconium alloy.
The performance of zircaloy includes decay resistance, hydrogen sucking function, mechanical property, Flouride-resistani acid phesphatase growth performance and creep resistance
Energy.Wherein, the performance that most critical and being easiest to changes in five big performances is decay resistance.
Influenceing the factor of Corrosion Resistance of Zirconium Alloys includes：Alloying component, heat processing technique, the second phase, oxide type,
Grain morphology and water chemistry etc..A certain amount of hydrogen can be discharged while zircaloy corrosion, a part of quilt of hydrogen produced in reaction
Involucrum absorbs, and the ratio between theoretical hydrogen desorption capacity is referred to as to inhale hydrogen fraction when the hydrogen amount of absorption is with corrosion.Therefore, the corrosion resistance of zircaloy
Can there is proportionate relationship and hydrogen sucking function between, influence the factor of corrosion also to influence to inhale hydrogen simultaneously.
The approach for improving Corrosion Resistance of Zirconium Alloys is mainly change alloying component and optimization processing technology.
At present, although addible alloying element is limited by thermal neutron absorption cross section size in zircaloy, but still
The zircaloy of various series is formd, summing up mainly has Zr-Sn systems, Zr-Nb systems and Zr-Sn-Nb systems three major types.Zr-Sn
Owner will have Zr-2 alloys, Zr-4 alloys and low tin Zr-4 alloys etc., and they belong to first generation zircaloy.In order to reduce nuclear power
Cost, improves fuel availability, it is necessary to increase element burnup, the lithium concentration improved in coolant temperature and cooling agent etc..These
Measure can aggravate the water side corrosion of zirconium alloy cladding, hydrogen-sucking amount increases, promote irradiation growth, the phase of increase pellet and involucrum
Interaction and internal pressure rise high.Although the performance that Zr-2 and Zr-4 alloys using very successful, can not be met under high burnup will
Ask.For example when the element burnup of Japanese presurized water reactor brings up to 48000MWd/tU by 39000MWd/tU, cladding tubes are by Zr-4 alloys
Low tin Zr-4 alloys are changed to, but the latter can not meet the requirement that burnup is further increased to 55000MWd/tU, be that this develops again
New alloy NDA.It is identical with this, the ZIRLO in the U.S., optimization ZIRLO, the M5 alloys of France, E110, E635 alloy of Russia,
The HANA alloys of South Korea, N18, N36 alloy of China is provided to reduce nuclear power cost, higher improves element burnup and develops
Zr-Nb systems or Zr-Sn-Nb systems alloy.
The content of the invention
The present invention in view of the shortcomings of the prior art, proposes the zirconium-base alloy in a kind of hot environment for nuclear reactor.
It is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.36~
0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%；Individually add 0.01~0.09%Cu
Or compound addition 0.01~0.09%Cu and 0.01~0.20%V；Balance of comprising impurity at least 98% zirconium.
Preferably, it is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.36
~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%, Cu：0.01~0.09%, surplus
It is comprising impurity at least 98% zirconium.
Preferably, it is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.36
~0.50%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%, Cu：0.01~0.09%, surplus
It is comprising impurity at least 98% zirconium.
Preferably, it is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.50
~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%, Cu：0.01~0.09%, surplus
It is comprising impurity at least 98% zirconium.
Preferably, it is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.36
~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%, Cu：0.01~0.09%, V：
0.01~0.20%, balance of comprising impurity at least 98% zirconium.
Preferably, it is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.36
~0.50%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%, Cu：0.01~0.09%, V：
0.01~0.20%, balance of comprising impurity at least 98% zirconium.
Preferably, it is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.50
~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%, Cu：0.01~0.09%, V：
0.01~0.20%, balance of comprising impurity at least 98% zirconium.
Compared with prior art, the invention has the advantages that：
Provided by the present invention for the zirconium-base alloy in nuclear reactor hot environment, with excellent decay resistance, should
Alloy has more excellent corrosion resistance in high temperature pure water and high temperature compared with the ZIRLO alloys of prior art in water containing lithium
Can, it is adaptable to corrosion-resistant zircaloy of the nuclear reactor compared with the fuel rod clad material under high burnup, screen work band and structural member：
1) the characteristics of alloy is designed is to keep relatively low Sn contents, close or saturation solid solution slightly above in zirconium alloy substrates
The Nb contents of content and Fe contents higher, while adding a small amount of characteristic alloying element cu or compound addition Cu and V element, limitation
The total amount for adding Cu and V is not more than 0.20%, and considers to match to improve the decay resistance of zircaloy between Cu and V element
And hydrogen sucking function, while the mechanical property of alloy, Flouride-resistani acid phesphatase growth and Flouride-resistani acid phesphatase croop property can also be improved.
2) the Sn elements of zirconium-base alloy of the invention addition 0.36%~0.69%, be taken into full account decay resistance and
Balance between Flouride-resistani acid phesphatase croop property, so that zirconium-base alloy of the invention has excellent decay resistance and Flouride-resistani acid phesphatase creep concurrently
Performance.In addition, zirconium-base alloy of the invention can be divided into two classes according to the content of the Sn elements of addition, class addition 0.36~
0.50% Sn, this kind of alloy is relatively low due to Sn contents, therefore its decay resistance is better, and another kind of addition 0.50~
0.69% Sn, this kind of alloy is slightly higher due to Sn contents, therefore its Flouride-resistani acid phesphatase croop property is better.
3) the Nb elements of present invention addition 0.20%~0.49%, when Sn is contained in alloy, reduce the Nb contents in alloy
Its decay resistance in high-temperature steam can be improved.
4) the Fe elements of present invention addition 0.21%~0.40%, can make up alloy due to Sn contents and the reduction of Nb contents
Cause the shortcoming of mechanical properties decrease, while improving the hydrogen sucking function of alloy, decay resistance and Flouride-resistani acid phesphatase growth performance.
5) in zircaloy add O to reduce irradiation creep function it is bigger, therefore we added in zircaloy it is more
O to improve croop property be more preferable.It can also improve the intensity and Flouride-resistani acid phesphatase growth performance of zircaloy, but O content is too high
It is unfavorable for the processing of zircaloy, so level of the O content control 0.10~0.20%.
6) Cu ratios are added to add other alloying elements more effective in terms of the decay resistance of alloy is improved, in zircaloy containing Nb.
But excessive Cu elements, can make the size of the second phase in zircaloy thick, thus Cu contents be limited in relatively low 0.01~
0.09% level.
7) V has oxygen affinity very high, therefore adds V to be necessary.Second Phase Particle stabilization containing V, can reduce oxidation
The stress and crackle of film, the containing V second zirconium oxide for mutually forming tetragonal crystal is stable, therefore makes the corrosion resistance of zircaloy
Can be good.The addition of V can reduce the hydrogen-sucking amount of alloy, based on the low corrosion rate of alloy and low hydrogen-sucking amount, then promote alloy to have
Low irradiation growth, this will also promote the raising of fuel-assembly burn-up.But the too high zircaloy that can reduce of V content is in high-temperature steam
Decay resistance, therefore V content is limited in 0.01~0.20% relatively low level.
8) zircaloy is processed using traditional handicraft, but cold rolling use low temperature intermediate annealing and low temperature afterwards are finally moved back
Fire, separates out tiny Second Phase Particle, the alloying element content reduced in matrix and the quantity for increasing by the second phase, so as to improve zirconium
The decay resistance of alloy.
Provided by the present invention for the zirconium-base alloy in nuclear reactor hot environment, existing fuel assembly fuel rod is improve
The decay resistance and hydrogen sucking function of involucrum zircaloy, while taking into account tensile property, croop property and irradiation growth performance.
Brief description of the drawings
Fig. 1 is in 360 DEG C/18.6MPa after zircaloy of the present invention is processed using low temperature annealing process with reference ZIRLO alloys
Surrosion curve in pure water.
Fig. 2 be zircaloy of the present invention using low temperature annealing process processing after with refer to ZIRLO alloys 360 DEG C/
Surrosion curve in the 18.6MPa/0.01mol/L LiOH aqueous solution.
Specific embodiment
It is below in conjunction with the accompanying drawings and specific real to enable the above objects, features and advantages of the present invention more obvious understandable
The present invention is further detailed explanation to apply mode.
It is calculated in weight percent for the zirconium-base alloy in nuclear reactor hot environment, including：Sn：0.36~
0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%；Individually add 0.01~0.09%Cu
Or compound addition 0.01~0.09%Cu and 0.01~0.20%V；Balance of comprising impurity at least 98% zirconium.
Two embodiments are shown in Table 1 with the composition of contrast ZIRLO alloys.
Table 1
Remaining impurity content meets the standard of current nuclear-used zirconium alloy, and C, N impurity element that corrosive nature is harmful to are made
Tightened up control, C content is less than 120 μ g/g, and N content is less than 80 μ g/g.
The preparation process and step of the embodiment of the present invention are as follows：
Sponge zirconium+intermediate alloy melting obtains ingot casting → second vacuum melting → forging → third time vacuum melting
Obtain finished product ingot casting → forging (1000 DEG C/1h) → β water quenchings (1050 DEG C/30min, quenching rate is more than 50 DEG C/s) → hot rolling 5-
6 (650 DEG C/50min, be tempered 10min) → vacuum annealings (550 DEG C/4h) → once cold rolling → vacuum annealing (550 DEG C/4h)
→ secondary cold-rolling → vacuum annealing (550 DEG C/4h) → tri- cold rolling → vacuum annealings (550 DEG C/4h) → final cold rolling → final
Vacuum annealing (550 DEG C/5h).
Two kinds of new zirconium alloy materials to being prepared by above-mentioned technique and it is put into autoclave with reference to ZIRLO alloy samples,
Corrosion test is carried out in 360 DEG C/18.6MPa pure water and the 360 DEG C/18.6MPa/0.01mol/L LiOH aqueous solution, them are investigated
Corrosion behavior.Surrosion curve is as shown in Figures 1 and 2.Be can be seen that from accompanying drawing 1：In 360 DEG C/18.6MPa pure water
In, with the extension of etching time, while the surrosion of the 2-in-1 gold of the embodiment of the alloy of embodiment 1 and addition Cu for adding Cu and V
Significantly lower than the ZIRLO alloys of prior art, when eroding to 300d, the corruption of the surrosion than ZIRLO alloy of the alloy of embodiment 1
Erosion weightening reduces 30%, and the surrosion of the 2-in-1 gold of embodiment reduces 30% than the surrosion of ZIRLO alloy；From accompanying drawing 2
It can be seen that：In the 360 DEG C/18.6MPa/0.01mol/L LiOH aqueous solution, with the extension of etching time, while add Cu and
The ZIRLO alloy of the surrosion significantly lower than prior art of the 2-in-1 gold of the embodiment of the alloy of embodiment 1 and addition Cu of V, corrosion
During to 300d, the surrosion of the alloy of embodiment 1 reduces 45%, the corruption of the 2-in-1 gold of embodiment than the surrosion of ZIRLO alloy
Erosion weightening reduces 36% than the surrosion of ZIRLO alloy.These results illustrate the corrosion-resistant of the zircaloy that the present invention is provided
Performance has more excellent decay resistance in high temperature pure water and high temperature than the ZIRLO alloys of prior art in water containing lithium.
The characteristics of in the embodiment of the present invention is：1) alloy unit is added simultaneously on the basis of Zr-Sn-Nb-Fe alloying components
Plain Cu and V individually adds Cu.2) base material uses low temperature intermediate annealing and low temperature final annealing after cold rolling, separates out tiny by the
The quantity of two-phase particle, the second phase of alloying element content and increase reduced in matrix, so as to improve the corrosion resistance of zircaloy
Energy.
It follows that the embodiment of the present invention has the advantages that：
Zirconium-base alloy in the hot environment for nuclear reactor provided in an embodiment of the present invention, with excellent corrosion resistance
Can, the alloy has more excellent corrosion resistant in high temperature pure water and high temperature compared with the ZIRLO alloys of prior art in water containing lithium
Corrosion energy, it is adaptable to which nuclear reactor is closed compared with the corrosion-resistant zirconium of the fuel rod clad material under high burnup, screen work band and structural member
Gold：
1) the characteristics of alloy is designed is to keep relatively low Sn contents, close or saturation solid solution slightly above in zirconium alloy substrates
The Nb contents of content and Fe contents higher, while adding a small amount of characteristic alloying element cu or compound addition Cu and V element, limitation
The total amount for adding Cu and V is not more than 0.20%, and considers to match to improve the decay resistance of zircaloy between Cu and V element
And hydrogen sucking function, while the mechanical property of alloy, Flouride-resistani acid phesphatase growth and Flouride-resistani acid phesphatase croop property can also be improved.
2) embodiment of the present invention zirconium-base alloy addition 0.36%~0.69% Sn elements, be taken into full account it is corrosion-resistant
Balance between performance and Flouride-resistani acid phesphatase croop property, so that zirconium-base alloy of the invention has excellent decay resistance and anti-spoke concurrently
According to croop property.In addition, content of the zirconium-base alloy of the invention according to the Sn elements of addition, can be divided into two classes, class addition
0.36~0.50% Sn, this kind of alloy is relatively low due to Sn contents, therefore its decay resistance is better, and another kind of addition
0.50~0.69% Sn, this kind of alloy is slightly higher due to Sn contents, therefore its Flouride-resistani acid phesphatase croop property is better.
3) the Nb elements of embodiment of the present invention addition 0.20%~0.49%, when Sn is contained in alloy, in reducing alloy
Nb contents can improve its decay resistance in high-temperature steam.
4) the Fe elements of embodiment of the present invention addition 0.21%~0.40%, can make up alloy because Sn contents and Nb contain
Amount is reduced causes the shortcoming of mechanical properties decrease, while improving the hydrogen sucking function of alloy, decay resistance and Flouride-resistani acid phesphatase growth
Energy.
5) in zircaloy add O to reduce irradiation creep function it is bigger, therefore we added in zircaloy it is more
O to improve croop property be more preferable.It can also improve the intensity and Flouride-resistani acid phesphatase growth performance of zircaloy, but O content is too high
It is unfavorable for the processing of zircaloy, so level of the O content control 0.10~0.20%.
6) Cu ratios are added to add other alloying elements more effective in terms of the decay resistance of alloy is improved, in zircaloy containing Nb.
But excessive Cu elements, can make the size of the second phase in zircaloy thick, thus Cu contents be limited in relatively low 0.01~
0.09% level.
7) V has oxygen affinity very high, therefore adds V to be necessary.Second Phase Particle stabilization containing V, can reduce oxidation
The stress and crackle of film, the containing V second zirconium oxide for mutually forming tetragonal crystal is stable, therefore makes the corrosion resistance of zircaloy
Can be good.The addition of V can reduce the hydrogen-sucking amount of alloy, based on the low corrosion rate of alloy and low hydrogen-sucking amount, then promote alloy to have
Low irradiation growth, this will also promote the raising of fuel-assembly burn-up.But the too high zircaloy that can reduce of V content is in high-temperature steam
Decay resistance, therefore V content is limited in 0.01~0.20% relatively low level.
8) zircaloy is processed using traditional handicraft, but cold rolling use low temperature intermediate annealing and low temperature afterwards are finally moved back
Fire, separates out tiny Second Phase Particle, the alloying element content reduced in matrix and the quantity for increasing by the second phase, so as to improve zirconium
The decay resistance of alloy.
Zirconium-base alloy in the hot environment for nuclear reactor provided in an embodiment of the present invention, improves existing fuel assembly
The decay resistance and hydrogen sucking function of fuel rod clad zircaloy, while taking into account tensile property, croop property and irradiation growth
Energy.
Each embodiment is described by the way of progressive in this specification, and what each embodiment was stressed is and other
The difference of embodiment, between each embodiment identical similar portion mutually referring to.For system disclosed in embodiment
For, due to corresponding to the method disclosed in Example, so description is fairly simple, related part is referring to method part illustration
.
Those skilled in the art can realize described function to each specific application using distinct methods, but
It is this realization it is not considered that beyond the scope of this invention.
Obviously, those skilled in the art can carry out various changes and modification without deviating from spirit of the invention to invention
And scope.So, if these modifications of the invention and modification belong to the claims in the present invention and its equivalent technologies scope it
Interior, then the present invention is also intended to including including these changes and modification.
Claims (7)
1. the zirconium-base alloy in a kind of hot environment for nuclear reactor, it is characterised in that calculated in weight percent, including：
Sn：0.36~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%；Independent addition 0.01~
0.09%Cu or compound additions 0.01~0.09%Cu and 0.01~0.20%V；Balance of comprising impurity at least 98% zirconium.
2. the zirconium-base alloy being used in nuclear reactor hot environment as claimed in claim 1, it is characterised in that with weight percent
Than calculating, including：Sn：0.36~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%,
Cu：0.01~0.09%, balance of comprising impurity at least 98% zirconium.
3. the zirconium-base alloy being used in nuclear reactor hot environment as claimed in claim 1, it is characterised in that with weight percent
Than calculating, including：Sn：0.36~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%,
Cu：0.01~0.09%, V：0.01~0.20%, balance of comprising impurity at least 98% zirconium.
4. the zirconium-base alloy being used in nuclear reactor hot environment as claimed in claim 2, it is characterised in that with weight percent
Than calculating, including：Sn：0.36~0.50%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%,
Cu：0.01~0.09%, balance of comprising impurity at least 98% zirconium.
5. the zirconium-base alloy being used in nuclear reactor hot environment as claimed in claim 2, it is characterised in that with weight percent
Than calculating, including：Sn：0.50~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%,
Cu：0.01~0.09%, balance of comprising impurity at least 98% zirconium.
6. the zirconium-base alloy being used in nuclear reactor hot environment as claimed in claim 3, it is characterised in that with weight percent
Than calculating, including：Sn：0.36~0.50%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%,
Cu：0.01~0.09%, V：0.01~0.20%, balance of comprising impurity at least 98% zirconium.
7. the zirconium-base alloy being used in nuclear reactor hot environment as claimed in claim 1, it is characterised in that with weight percent
Than calculating, including：Sn：0.50~0.69%；Nb：0.20~0.49%；Fe：0.21~0.40%；O：0.10~0.20%,
Cu：0.01~0.09%, V：0.01~0.20%, balance of comprising impurity at least 98% zirconium.
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| WO2019162876A1 (en) | 2018-02-21 | 2019-08-29 | Comisión Nacional De Energía Atómica (Cnea) | Zirconium alloys with improved corrosion resistance and service temperature for use in the fuel cladding and core structural parts of a nuclear reactor |
| CN110284027A (en) * | 2019-08-06 | 2019-09-27 | 中国核动力研究设计院 | A kind of zirconium-base alloy of alkali resistance water quality corrosion |
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| CN110284027B (en) * | 2019-08-06 | 2020-04-21 | 中国核动力研究设计院 | Zirconium-based alloy resistant to alkaline water corrosion |
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