CN104451252B - A kind of Li-Pb alloy of used by nuclear reactor and preparation method thereof - Google Patents
A kind of Li-Pb alloy of used by nuclear reactor and preparation method thereof Download PDFInfo
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Abstract
The invention discloses Li-Pb alloy of a kind of used by nuclear reactor and preparation method thereof.This Li-Pb alloy matrix be the mass percentage content of Pb, Li be 0.68 ± 0.05%；Content of impurities is less than 300ppm, the content≤5ppm of single impurity element, and does not contains the element that can produce radioactive product after neutron irradiation.Experiment shows, Li-Pb alloy material of the present invention is to melt three kinds of functions (neutron multiplication, tritium propagation, cooling) in the used by nuclear reactor material of one, it is adaptable to nuclear industry field, particularly fusion reactor field.
Description
Technical field
The present invention relates to liquid metal alloy Material Field, especially relate to a kind of tritium multiplication agent be applicable to fusion reactor, cooling
Agent and the Li-Pb alloy of neutron multiplication agent.
Background technology
Fusion energy be presently recognized that can one of the important channel finally solving mankind's energy crisis and environmental problem, be " peace
Entirely, cleaning, permanent " energy.In fusion reactor, covering is the important component part of nuclear reactor, and its major function is: increase
Grow tritium for fuel recycle, the neutron energy of reactor core is converted into form of thermal energy output, shields with protection magnet coil and outer collarette
Border.Cladding technique is the key technology determining fusion energy application success or failure.
When cladding structure design and technical research, it is necessary to carry out tritium multiplication agent, coolant and the research of neutron multiplication agent and selection.
Wherein can be as the material mainly containing lithium of tritium multiplication agent, lithium (Li) ceramic including lithium, pure or liquid metal eutectic Han lithium
Material；Liquid metal, water and helium can be had as the material of coolant；Can have containing Be or lead as the material of neutron multiplication agent
Compound etc..So, the research of the material of tritium multiplication agent, coolant and neutron multiplication agent selects the utilization to fusion energy to be to pass
Important.
Summary of the invention
The present invention proposes the Li-Pb alloy material of a kind of tritium multiplication agent, coolant and neutron multiplication agent be applicable to fusion reactor,
It has good neutron multiplication ability, high tritium multiplication capacity, high heat conduction and heat-carrying capacity, it is contemplated that can meet as fusion
The use requirement of tritium multiplication agent, coolant and neutron multiplication agent in heap.
The present invention adopts the following technical scheme that
A kind of Li-Pb alloy of used by nuclear reactor, matrix be the mass percentage content of Pb, Li be 0.68 ± 0.05%；Impurity is total
Content is less than 300ppm, the content≤5ppm of single impurity element, and does not contains and can produce radioactive product after neutron irradiation
Element.
In above-mentioned Li-Pb alloy, described impurity element can be the elements such as Fe, Mn, Al, but do not contain N, Ni, Mo,
Nb, Co, Cu etc. are easily generated the element of radioactive product after neutron irradiation.
In above-mentioned Li-Pb alloy, the mass percentage content of Li is preferably 0.68 ± 0.02%.
The preparation method of the Li-Pb alloy of above-mentioned used by nuclear reactor is as follows:
1) in high-purity argon gas environment, dispensing is carried out by the design composition of Pb and Li, by the Pb powder that granularity is 150～250 mesh
Be respectively charged into respective feed hopper with Li powder, first a part of Pb powder loaded stirring pool, start mechanical agitation, then Li powder and
Pb powder enters stirring pool mix homogeneously by respective charging quarrel；
2) in high-purity argon gas environment, the Pb powder mixed and Li powder are dividedly in some parts heating and melting in smelting furnace, carry out simultaneously
Continuous print electromagnetic agitation, Li Yu Pb alloying also releases amount of heat, charge melted heat absorption, controls temperature less than 470 DEG C,
Maintain stirring 15～25 minutes, at 400～450 DEG C, melt is stood 1～3 hour subsequently；
3) in high-purity argon gas environment, the Li-Pb alloy of 400～450 DEG C is filtered by drainage screen, filter dystectic Li
With Pb compound；
4) by step 3) filter after Li-Pb alloy vacuum casting at 270～320 DEG C, it is thus achieved that alloy cast ingot.
Further, in step 2) Li and the Pb composition of on-line checking alloy, and return step 1 according to testing result) fine setting
The charge ratio of Li and Pb, followed by carries out step 2 by Li powder and Pb powder mix homogeneously), after composition detection is qualified, enter step
Rapid 3).
Further, step 4) use unique casting mould to carry out vacuum casting, the casting mould of this uniqueness is to be set by mould
Put the center at a cylindrical cavity, and on the axis direction be perpendicular to cylindrical cavity, have a trunnion axis so that whole casting
Modeling tool can rotate slowly around this trunnion axis, when Liquid LiPb Alloy injection casting mould after, Liquid LiPb Alloy with
Casting mould rotates around this trunnion axis lentamente, cools down molding, so reduces the gravity segregation phenomenon of elemental lithium, further
Ensure the uniformity of lithium content, it is thus achieved that satisfactory alloy cast ingot.
In above-mentioned preparation method, described high-purity argon gas is that 99.99%-99.999% argon is through except the argon after the impurity treatment such as water, deoxygenation
Gas.
Prepare raw material Li that above-mentioned alloy formula used and Pb must be high purity lithium and high purity lead, its impurity do not contain N, Ni,
Mo, Nb, Co, Cu etc. are easily generated the element of radioactive product after neutron irradiation.Single impurity element in i.e. Li and Pb
Content≤5ppm, content of impurities be less than 300ppm.Otherwise, from raw material, impurity component, these impurity are unavoidably brought
Composition, will affect the purity of Li-Pb alloy in the presence of inevitably amount and composition, also will directly affect fusion reactor blanket and run
The production of nuclear fuel tritium and extraction in journey, and strictly control the content of impurity in Li-Pb alloy and be possible not only to reduce tritium in covering
Hold-up, it is simple to the extraction of tritium, the most also can avoid the impurity deposition produced in covering running, and especially strong neutron irradiation can
Can cause the generation of Long-lived Radionuclides, therefore it is required that the content of element easily-activated in alloy is strictly limited, also
Total impurities content in alloy is carried out strict defining and control.
The present invention compared with prior art has the advantage that the present invention is optimized design to existing Li-Pb alloy formula so that
When Li content is less, fusing point is relatively low, and boiling point is high, and in the case of having obvious security advantages, the tritium still with excellence increases
Grow performance.It is embodied in following several respects:
1) Li-Pb alloy that the present invention provides, fusing point 235 DEG C, Liquid LiPb Alloy can flow, and the temperature rising space is big, this
The temperature space of sample can be with existing metal material (austenitic steel, ferritic steel, martensitic stain less steel, vanadium alloy etc.) conduct
Nuclear reactor structure material.Experimentation shows, liquid metal lithium lead and austenitic steel, ferritic steel/martensitic stain less steel, vanadium
The maximum compatible temperature of alloy is respectively 400 DEG C, 480 DEG C and 650 DEG C.
2) in the Li-Pb alloy that the present invention provides, the content of lead Pb is very big (99.3wt%), owing to Pb (n, 2n) reacts, and its neutron times
Energization power is relatively strong, and lead is effective neutron multiplication material, has the highest immunity to irradiation damage, it is not necessary to make again
With the neutron multiplication agent (such as Be) of high cost, it it is one of high tritium multiplication capacity essential condition.Further, the neutron shield of Pb
Characteristic is also very good.
3) in the Li-Pb alloy that the present invention provides, lithium is fine tritium-breeding material, and neutron and lithium react generation tritium, 6Li isotope ground
Aboundresources on ball.Liquid LiPb Alloy can flow, and can supplement the 6Li isotope consumed by real-time online, is a kind of without the longevity
The fertile material that life limits；Also it is one of high tritium multiplication capacity essential condition.And multiplication agent itself is also tritium circulating carrier,
In addition tritium dissolubility wherein is the lowest, can carry tritium at out-pile real-time online.
4) present invention provides the heat conduction that had of Li-Pb alloy and heat-carrying capacity, be good coolant, it is allowed to design high power
Density, high thermal efficiency cladding systems.Liquid LiPb Alloy flows, and heat band to out-pile real-time online is taken heat generating.
5) Li-Pb alloy that the present invention provides and water and air do not have volatile reaction, and safety is high.
6) Liquid LiPb Alloy that the present invention provides has, to tokamak complex geometry, well adapting to property.
Therefore, the Liquid LiPb Alloy that the present invention provides melts three kinds of functions (neutron multiplication, tritium propagation, cooling) in one
Used by nuclear reactor material, it is adaptable to nuclear industry field, particularly fusion reactor field.
Detailed description of the invention
Below by way of detailed description of the invention, the invention will be further described, but this is not limitation of the present invention, this area skill
Art personnel are according to the basic thought of the present invention, and various modifications may be made or improves, but without departing from the basic think of of the present invention
Think, the most within the scope of the present invention.
Embodiment one
Li-Pb alloy is prepared according to following step:
(1) argon (99.999%) must be carried out except the process of the impurity such as water, deoxygenation before using.Procedure below is all in high-purity argon
Compression ring border is carried out.
(2) (it is easy after neutron irradiation that its impurity does not contains N, Ni, Mo, Nb, Co, Cu etc. to use high purity lithium and high purity lead
Produce the element of radioactive product；Content of impurities is less than 300ppm, the content≤5ppm of single impurity element) it is raw material,
Raw material Pb and Li is processed into powder by high-purity argon gas environment respectively, granularity: Pb be 250 mesh, Li be 250 mesh.
(3) Pb powder and Li powder uniformly mix: carry out dispensing, Pb powder and Li powder according to design composition and be respectively charged into respective charging
Bucket；Entering stirring pool when carrying out mechanical agitation, Pb powder is introduced into a part, starts machine mixer stirring, then Li powder and
Pb powder enters stirring pool by respective charging quarrel and mixes, and stirs 20 minutes, allows Li powder and Pb powder be fully contacted mixing all
Even.
(4) wash heat stove and mold: smelting furnace is heated to 400 DEG C, is evacuated to 1.5Pa, keeps 5 minutes, is filled with 0.1MPa
High-purity argon gas, keeps 4 minutes；It is evacuated to 1Pa again, keeps 3 minutes, be filled with 0.1MPa high-purity argon gas, keep 4 minutes；
It is repeated 2 times, removes in smelting furnace, smelting furnace inner surface and smelting furnace interior surface layers waste gas.Mold is heated to 450 DEG C, protects
Holding 30 minutes, baking is removed in mold, mold inner surface and mold interior surface layers waste gas.
(5) Li with Pb alloying: the lithium Hydrocerussitum (Ceruse) mixed homogeneously is entered smelting furnace in batches, adds heat fusing, melt is carried out simultaneously
Electromagnetic Continuous stirs；Li Yu Pb alloy chemical conversion Li-Pb alloy, and release substantial amounts of heat, charge melted heat absorption, observe temperature
Change, control temperature less than 470 DEG C, maintain stirring 20 minutes, at 400 DEG C, melt is stood 3 hours subsequently.
(6) on-line checking Li and Pb composition foundation testing result return to the charge ratio of step (3) fine setting Li and Pb, fusion
After refining alloying component is qualified, 400 DEG C of Li-Pb alloys is filtered by drainage screen, filter dystectic Li and Pb compound,
Impurity content is less than 290ppm.
(7) vacuum casting, after 270 DEG C of Liquid LiPb Alloys inject unique casting mould, Liquid LiPb Alloy is with casting die
Tool rotates around this trunnion axis lentamente, cools down molding, so can reduce the gravity segregation phenomenon of elemental lithium, be further ensured that
The uniformity of lithium content, it is thus achieved that satisfactory alloy cast ingot.
Experimental test: this Li-Pb alloy fusing point 235 DEG C, tests at 300 DEG C, and this Liquid LiPb Alloy density is 9500kg/m3,
Specific heat capacity is 190J/ (kg K), and pyroconductivity is 15w/ (m K), and heat transfer coefficient is 1000w/ (m2K), the coefficient of viscosity is
0.188(10-6m2s-1), electrical conductivity is 0.85 × 106(A·V-1·m-1), resistivity is 1.1765 (V A-1M), during dissolving, volume increases
3.5%, Pr number 2.38 × 10-2。
Embodiment two
Li-Pb alloy is prepared according to following step:
(1) argon (99.995%) must be carried out except the process of the impurity such as water, deoxygenation before using.
(2) (it is easy after neutron irradiation that its impurity does not contains N, Ni, Mo, Nb, Co, Cu etc. to use high purity lithium and high purity lead
Produce the element of radioactive product；Content of impurities is less than 300ppm, the content≤5ppm of single impurity element) it is raw material,
Raw material Pb and Li is processed into powder by high-purity argon gas environment respectively, granularity: Pb be 200 mesh, Li be 200 mesh.
(3) Pb and Li solid powder mixing: carry out dispensing, Pb powder and Li powder according to the design composition of Li and Pb and fill respectively
Enter respective feed hopper；When entrance stirring pool carries out mechanical agitation, Pb powder is introduced into a part, starts machine mixer stirring,
Then Li powder and Pb powder enter stirring pool mixing by respective charging quarrel, stir 30 minutes, make Li powder and Pb powder abundant
Contact mix homogeneously.
(4) wash heat stove and mold: smelting furnace is heated to 450 DEG C, is evacuated to 1.8Pa, keeps 5 minutes, is filled with 0.2MPa
High-purity argon gas, keeps 5 minutes；It is evacuated to 1.5Pa again, keeps 5 minutes, be filled with 0.15MPa high-purity argon gas, keep 5
Minute；It is repeated 2 times, removes in smelting furnace, smelting furnace inner surface and smelting furnace interior surface layers waste gas.Mold is heated to 500 DEG C,
Keeping 20 minutes, baking is removed in mold, mold inner surface and mold interior surface layers waste gas.
(5) Li with Pb alloying: the lithium Hydrocerussitum (Ceruse) mixed homogeneously is entered smelting furnace in batches, adds heat fusing, melt is carried out simultaneously
Electromagnetic Continuous stirs；Li Yu Pb alloy chemical conversion Li-Pb alloy, and release substantial amounts of heat, charge melted heat absorption, observe temperature
Change, control temperature less than 470 DEG C, maintain stirring 25 minutes, at 420 DEG C, melt is stood 2 hours subsequently.
(6) on-line checking Li and Pb composition foundation test result return to the charge ratio of step (3) fine setting Li and Pb, fusion
After refining alloying component is qualified, 420 DEG C of Li-Pb alloys is filtered by drainage screen, filter dystectic Li and Pb compound,
Impurity content is less than 280ppm.
(7) vacuum casting, after 300 DEG C of Liquid LiPb Alloys inject unique casting mould, Liquid LiPb Alloy is with casting die
Tool rotates around this trunnion axis lentamente, cools down molding, so reduces the gravity segregation phenomenon of elemental lithium, be further ensured that lithium
The uniformity of content, it is thus achieved that satisfactory alloy cast ingot.
Above procedure is all carried out in high-purity argon gas environment.
Experimental test: this Li-Pb alloy fusing point 236 DEG C, tests at 300 DEG C, and this Liquid LiPb Alloy density is 9600kg/m3,
Specific heat capacity is 191J/ (kg K), and pyroconductivity is 14w/ (m K), and heat transfer coefficient is 1000w/ (m2K), the coefficient of viscosity is
0.187(10-6m2s-1), electrical conductivity is 0.84 × 106(A·V-1·m-1), resistivity is 1.1665 (V A-1M), during dissolving, volume increases
3.4%, Pr number 2.37 × 10-2。
To sum up two embodiment testing inspection show: (mass percent of each composition is: matrix is to be optimized design Li-Pb alloy
Pb；Li:0.68 ± 0.05%；Content of impurities is less than 300ppm, the content≤5ppm of single impurity element.Described impurity unit
The specific requirement of element is: the elements such as Fe, Mn, Al, does not contains N, Ni, Mo, Nb, Co, Cu etc. after neutron irradiation
It is easily generated the element of radioactive product) stable performance, in the range of test error, each physical parameter is consistent.
This Li-Pb alloy fusing point 235 DEG C, more much higher than room temperature, Liquid LiPb Alloy can flow, but the pipeline of current-carrying, equipment
It is considered as preheating, it is to avoid freezing blocking；Fusing point is higher, and security performance is higher.The temperature rising space is big, such temperature space
Available existing metal material (austenitic steel, ferritic steel/martensitic stain less steel, vanadium alloy etc.) is tied as nuclear reactor covering
Structure material.
Experimentation shows, liquid metal lithium lead and austenitic steel, ferritic steel/martensitic stain less steel, the maximum compatibility of vanadium alloy
Temperature is respectively 400 DEG C, 480 DEG C and 650 DEG C.Such temperature space can be with existing metal material (austenitic steel, ferrum element
Body steel/martensitic stain less steel, vanadium alloy etc.) as the cladding structure material in nuclear reactor.
Testing inspection shows: this Li-Pb alloy specific heat capacity is 190J/ (kg K), and heat conductivity is 15w/ (m K), and heat transfer coefficient is
1000w/(m2K), heat conduction and heat-carrying capacity are good, are good coolant and catalyst carrier, it is allowed to design high power density, high heat
Efficiency cladding systems.Liquid LiPb Alloy flows, and heat band to out-pile real-time online is taken heat generating.Boiling point is high, and catalyst carrier can
Working at ambient pressure, fusion reactor cooling system can not use high pressure, and security performance is higher.
Testing inspection shows: isotope hydrogen and deuterium with tritium carry out solubility test in this Liquid LiPb Alloy, find that hydrogen and deuterium exist
This Liquid LiPb Alloy dissolubility is the lowest, therefore the dissolubility that tritium is wherein is the lowest, and Liquid LiPb Alloy itself is also that tritium follows in addition
Ring carrier, can carry tritium at out-pile real-time online.
Test shows: this Li-Pb alloy and water and air do not have explosive reaction.Although liquid lithium is the most active metal,
Security performance is poor, but this Li-Pb alloy formula is optimized design so that less at Li content, carry out Li-Pb alloy and water and
Air reaction is tested, and does not has explosivity, compares safety.
Therefore, this Liquid LiPb Alloy is applicable to nuclear industry field as neutron multiplication agent, tritium multiplication agent, heat-carrying coolant, special
It it not fusion reactor field.
Claims (5)
1. a preparation method for Li-Pb alloy, the matrix of described Li-Pb alloy is that the mass percentage content of Pb, Li is
0.68 ± 0.05%；Content of impurities is less than 300ppm, the content≤5ppm of single impurity element, and does not contains through neutron spoke
Can produce the element of radioactive product after according to, its preparation method comprises the following steps:
1) in high-purity argon gas environment, dispensing is carried out by the design composition of Pb and Li, by the Pb powder that granularity is 150～250 mesh
It is respectively charged into respective feed hopper with Li powder, first a part of Pb powder is loaded stirring pool, start mechanical agitation, then
Li powder and Pb powder enter stirring pool mix homogeneously by respective charging quarrel；
2) in high-purity argon gas environment, by step 1) the Pb powder that mixes and Li powder be dividedly in some parts heating and melting in smelting furnace,
Carrying out continuous print electromagnetic agitation, Li Yu Pb alloying also releases amount of heat, charge melted heat absorption simultaneously, controls temperature
Degree, less than 470 DEG C, maintains stirring 15～25 minutes, at 400～450 DEG C, melt is stood 1～3 hour subsequently；
3) in high-purity argon gas environment, the Li-Pb alloy of 400～450 DEG C is filtered by drainage screen, filter dystectic Li
With Pb compound；
4) by step 3) filter after Li-Pb alloy vacuum casting at 270～320 DEG C, it is thus achieved that alloy cast ingot.
2. preparation method as claimed in claim 1, it is characterised in that in step 2) Li and the Pb composition of on-line checking alloy,
And according to testing result return step 1) fine setting Li and Pb charge ratio, Li powder and Pb powder mix homogeneously are followed by entered
Row step 2), after composition detection is qualified, enter step 3).
3. preparation method as claimed in claim 1, it is characterised in that step 4) vacuum casting time casting mould is arranged on one
The center of cylindrical cavity, and on the axis direction be perpendicular to cylindrical cavity, have a trunnion axis so that whole casting mould
Can rotate slowly around this trunnion axis, after Liquid LiPb Alloy injects casting mould, Liquid LiPb Alloy is with casting
Mould rotates around this trunnion axis lentamente, cools down molding.
4. preparation method as claimed in claim 1, it is characterised in that described high-purity argon gas is that 99.99%-99.999% argon is through removing
Argon after impurity treatment.
5. preparation method as claimed in claim 1, it is characterised in that the raw material Li used and Pb are high purity lithium and high purity lead,
Do not contain the impurity element that can produce radioactive product after neutron irradiation.
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Citations (5)
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|---|---|---|---|---|
| DE1533246B1 (en) * | 1966-12-19 | 1972-03-09 | Cerjak Horst Dipl Ing Dr | CREEP RESISTANT LEAD ALLOYS |
| US5768329A (en) * | 1996-01-30 | 1998-06-16 | Northrop Grumman Corporation | Apparatus for accelerator production of tritium |
| CN101440437A (en) * | 2008-12-31 | 2009-05-27 | 中国科学院等离子体物理研究所 | Preparation of lithium-lead alloy |
| CN101440446A (en) * | 2008-12-31 | 2009-05-27 | 中国科学院等离子体物理研究所 | Industrial lithium-lead alloy |
| CN101876013A (en) * | 2010-06-13 | 2010-11-03 | 中国铝业股份有限公司 | Li-Pb alloy for nuclear industry |
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2014
- 2014-12-11 CN CN201410763690.6A patent/CN104451252B/en active Active
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE1533246B1 (en) * | 1966-12-19 | 1972-03-09 | Cerjak Horst Dipl Ing Dr | CREEP RESISTANT LEAD ALLOYS |
| US5768329A (en) * | 1996-01-30 | 1998-06-16 | Northrop Grumman Corporation | Apparatus for accelerator production of tritium |
| CN101440437A (en) * | 2008-12-31 | 2009-05-27 | 中国科学院等离子体物理研究所 | Preparation of lithium-lead alloy |
| CN101440446A (en) * | 2008-12-31 | 2009-05-27 | 中国科学院等离子体物理研究所 | Industrial lithium-lead alloy |
| CN101876013A (en) * | 2010-06-13 | 2010-11-03 | 中国铝业股份有限公司 | Li-Pb alloy for nuclear industry |
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