CN103045916A - Composite shielding material and preparation method thereof - Google Patents
Composite shielding material and preparation method thereof Download PDFInfo
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- CN103045916A CN103045916A CN201210570726XA CN201210570726A CN103045916A CN 103045916 A CN103045916 A CN 103045916A CN 201210570726X A CN201210570726X A CN 201210570726XA CN 201210570726 A CN201210570726 A CN 201210570726A CN 103045916 A CN103045916 A CN 103045916A
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Abstract
The invention relates to a composite shielding material and a preparation method thereof, in particular to the composite shielding material applied to nuclear radiation places such as nuclear reactor, spent fuel assembly storage and radioactive substance storage and transportation and the like. The composite shielding material is characterized by comprising the following components in percentage by weight: 0 to 30 percent of w and compound thereof, 0 to 70 percent of B4C, 0 to 90 percent of aluminum or aluminum alloy, 0 to 8 percent of other elements and the like. The composite shielding material comprising tungsten B4C/aluminum alloy is uniform in distribution of W2B5 and B4C, high in densification degree, high in strength and toughness, and particularly applicable to the field of neutron/gamma ray shielding.
Description
Technical field
The invention belongs to the composite shielding material field, relate in particular to composite shielding material for nuclear radiation places such as nuclear reactor, irradiated fuel assembly storage and radioactive substance storings and preparation method thereof.
Background technology
In the radiation that the fields such as nuclear reactor, irradiated fuel assembly storage produce, the shielding problem that will pay attention to especially is the large gamma-radiation of neutron radiation and penetration power, the field that produces neutron radiation generally all is accompanied by gamma-radiation, in order to reduce the suffered irradiation of human body and equipment, in the shielding neutron radiation, also should shield gamma-ray irradiation.The materials such as the paraffin that general hydrogen content is higher, polyethylene, polypropylene are good Moderation of the fast neutrons materials, boron oxide, boric acid and the norbide etc. that contain lithium fluoride, lithiumbromide, the lithium hydroxide of elemental lithium and contain boron are good thermal neutron absorbing materials, also fine with the tungsten effect to the shielding of fast neutron simultaneously, because the material of its 10cm thickness can reach 93% to the shielding rate of neutron.Shielding preferably to gamma-radiation, material is lead, tungsten and other heavy metals etc.These materials and matrix material thereof have been widely used in various nuclear reactor shielding harness and have brought into play considerable effect.
At present use more composite shielding material to be lead-boron polythene, the comprehensive shielded effect of such material is better, but because material is as matrix take polymkeric substance, therefore its use temperature only is 80-100 ℃, mechanical property is also relatively poor, be generally 10MPa-20MPa, can not satisfy the service requirements in the neutron shield field that thermotolerance and mechanical property are had higher requirements.Al-B
4C has the advantage of aluminium and norbide concurrently, and density is low, and hardness is high, thermal-neutron capture cross-section is high, and is cheap, good toughness, have good mechanical mechanics property and thermal neutron absorptive character, since the eighties in last century, be subject to the extensive attention of radio-protective researcher.But Al-B
4The anti-gamma-radiation poor-performing of C, and present Al-B
4The C development concentrates on Al-B mostly
4C composite manufacture aspect, the research of the relevant comprehensive shielded performance of its neutron/gamma-radiation does not almost have.Therefore, be badly in need of further optimizing Al-B
4The comprehensive shielded performance of C matrix material is with its application potential in the nucleus screening field of abundant expansion.
Summary of the invention
For solving above technical problem, the object of the present invention is to provide a kind of composite shielding material with neutron radiation shielding properties and gamma-radiation shielding properties, and can adopt respective components according to neutron and gamma-rays distribution situation, its component comprises W and compound thereof, B
4C, aluminum or aluminum alloy and other element.
Solve a kind of composite shielding material of above technical problem among the present invention, it is characterized in that: the component by following weight per-cent forms: the W of 0-30% or the compound of W, the B of 0-70%
4C, the aluminum or aluminum alloy of 0-90%, other element of 0-8%.
The compound of described W or W is W, WO
3, W
2O
5Or W
2B
5Deng.
Described other element is Ti, Si, Mg, Zr, V, Cr or its compound, rare earth element.
The compound of described above-mentioned element is TiB
2, TiO
2, SiO
2, MgO, ZrO
2, V
2O
5, Cr
2O
3, Y
2O
3Or La
2O
3Deng.
With B
4C, aluminum or aluminum alloy are main raw, significantly improve the gamma ray shielding performance of material by adding an amount of W and compound thereof, add other a small amount of element as the reactive sintering agent, to improve B
4The wettability of C and aluminium is controlled its surface reaction, the over-all propertieies such as the nuclear radiation shield performance of raising material and mechanical property.
At existing B
4On the basis of C/Al neutron shielding material, introduce W and compound thereof with good gamma-radiation performance, by the shielding properties of Monte Carlo method Calculating material, optimize composite material compositions, make B
4The C/Al matrix material has good neutron shield performance and gamma-radiation shielding properties simultaneously.
Prepare a kind of method of composite shielding material, it is characterized in that: step is as follows:
Step 1, take by weighing the W of raw material weight per-cent: 0-30% or the compound of W; The B of 0-70%
4C; The aluminum or aluminum alloy of 0-90%; Other element of 0-8%;
Step 2, mix each component material, carry out ball milling in the ball grinder of packing into, inject argon gas in the ball grinder as protective atmosphere, Ball-milling Time 2-25h obtains mixed powder behind the ball milling;
Step 3, mixed powder are packed into and are adopted cold isostatic compaction behind the soft mode, and pressure is 100-270MPa, time 5-60min; The material of soft mode is PVC, and shape per sample, size are made mould with PVC and carried out cold isostatic compaction.
Step 4, the base of will colding pressing carry out HIP sintering, and hot isostatic pressing gas is argon gas, and temperature is 680-1200 ℃, and pressure is 30-150MPa, and the time is 0-180min;
Step 5, the material behind the hot isostatic pressing is namely got composite shielding material after the demoulding.
Ball grinder is stainless steel jar mill, and abrading-ball is sintered carbide ball.The main component of sintered carbide ball is WC, contains equally W in the B4C/Al matrix material, therefore, selects Wimet can reduce the introducing of impurity element as abrading-ball.Take argon gas as gaseous media, can prevent the oxidation of aluminium and other metal when ball milling and hot isostatic pressing.
Because norbide and aluminium need good wetting of under the high temperature about 1200 ℃ ability, and in this temperature range, aluminium and B
4C can generate more Al at the interface
4C
3The fragility phase reduce interface bond strength, and molten aluminium alloy volatilizees easily under the high temperature, causes waste of raw materials, and experimental installation is also had certain harm.Therefore, how effectively to reduce the temperature of reaction of matrix material, the generation that the control surface reaction is particularly controlled the high-temperature brittleness phase is technological difficulties of the present invention.The present invention adopts hot isostatic pressing technique to prepare powder metallurgy B
4The C/ aluminium alloy solves B
4C and Al are difficult to wetting problem at low temperature, greatly reduce sintering temperature (sintering temperature can be reduced to the fusing point of a little higher than Al), reduce surface reaction speed, avoid harmful and generate mutually, effectively control the composite material interface phase structure, optimize the mechanical property of matrix material.
The present invention satisfies the nuclear radiation shield field to the requirement of shielding material at comprehensive shielded aspect of performance, developed a kind of composite shielding material with good neutron radiation shielding properties and gamma-radiation shielding properties, and can be according to the composite shielding material of neutron and gamma-rays distribution situation employing respective components.Adopt the tungstenic B of above-mentioned technique preparation
4C/ aluminium alloy compound shielding material W
2B
5And B
4C is evenly distributed, and densification degree is high, and intensity and toughness are good, is specially adapted to neutron/gamma shielding field.
Composite shielding material of the present invention has good neutron radiation shielding properties and gamma-radiation shielding properties, and can be according to the matrix material of neutron and gamma-rays distribution situation employing respective components.More traditional composite shielding material is compared, and the neutron radiation shielding is had good performance, simultaneously the gamma-radiation shielding properties is improved 5-20% or more.
Specific embodiment
Embodiment 1
Take by weighing raw material weight per-cent WO
315%, B
4C's 15%, aluminium alloy 67%, Ti 3%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt the YG8 sintered carbide ball, Ball-milling Time 24h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 250MPa, 18 ℃ of temperature, time 10min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 900 ℃, and hot isostatic pressing pressure is 120MPa, and the hot isostatic pressing soaking time is 1h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4C/Al composite shielding material.
Embodiment 2
Take by weighing raw material weight per-cent WO
325%, B
4C's 10%, Al 60%, TiO
25%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 24h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 200MPa, 25 ℃ of temperature, time 20min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 800 ℃, and hot isostatic pressing pressure is 80MPa, and the hot isostatic pressing soaking time is 3h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 3
Take by weighing raw material weight per-cent WO
35%, B
4C's 20%, Al 72%, Cr3%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 22h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 180MPa, 20 ℃ of temperature, time 30min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 680 ℃, and hot isostatic pressing pressure is 140MPa, and the hot isostatic pressing soaking time is 1h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 4
W by weight percentage
2B
510%; B
4C's 45%; Aluminium alloy 40%; SiO
25% takes by weighing raw material.Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt the YG8 sintered carbide ball, Ball-milling Time 24h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 250MPa, 22 ℃ of temperature, time 5min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 800 ℃, and hot isostatic pressing pressure is 100MPa, and the hot isostatic pressing soaking time is 1h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4C/ aluminium alloy compound shielding material.Adopt the tungstenic B of above-mentioned technique preparation
4C/ aluminium alloy compound shielding material W
2B
5And B
4C is evenly distributed, and densification degree is high, and intensity and toughness are good, is specially adapted to neutron/gamma shielding field.
Embodiment 5
Take by weighing raw material weight per-cent W
2B
55%, B
4C's 25%, Al 67%, rare earth 3%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 23h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 150MPa, 24 ℃ of temperature, time 40min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 700 ℃, and hot isostatic pressing pressure is 150MPa, and the hot isostatic pressing soaking time is 1.5h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 6
Take by weighing raw material weight per-cent W
2B
525%, B
4C10%'s, Al 60%, MgO5%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 20h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 150MPa, 23 ℃ of temperature, time 50min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 1100 ℃, and hot isostatic pressing pressure is 100MPa, and the hot isostatic pressing soaking time is 2.5h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 7
Take by weighing raw material weight per-cent WO
315%, B
4C's 30%, aluminium alloy 50%, Ti 5%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt the YG8 sintered carbide ball, Ball-milling Time 15h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 250MPa, 24 ℃ of temperature, time 60min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 900 ℃, and hot isostatic pressing pressure is 120MPa, and the hot isostatic pressing soaking time is 1h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4C/Al composite shielding material.
Embodiment 8
Take by weighing raw material weight per-cent W 30%, B
4C's 30%, Al 32%, TiB
28%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 10h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 270MPa, 19 ℃ of temperature, time 15min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 1000 ℃, and hot isostatic pressing pressure is 90MPa, and the hot isostatic pressing soaking time is 2h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 9
Take by weighing raw material weight per-cent W2%, B
4C's 68%, Al 23%, Zr7%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 2h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 270MPa, 22 ℃ of temperature, time 20min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 1200 ℃, and hot isostatic pressing pressure is 30MPa, and the hot isostatic pressing soaking time is 3h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 10
Take by weighing raw material weight per-cent W
2O
530%, B
4C's 50%, Al 15%, ZrO
25%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 22h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 150MPa, 23 ℃ of temperature, time 25min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 900 ℃, and hot isostatic pressing pressure is 100MPa, and the hot isostatic pressing soaking time is 2h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 11
Take by weighing raw material weight per-cent W
2O
56%, B
4C's 15%, Al 75%, V
2O
54%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 25h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 120MPa, 25 ℃ of temperature, time 30min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 850 ℃, and hot isostatic pressing pressure is 250MPa, and the hot isostatic pressing soaking time is 1h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 12
Take by weighing raw material weight per-cent W
2O
50%, B
4C's 50%, Al 45%, V5%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, use dehydrated alcohol as ball-milling medium, Ball-milling Time 25h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 120MPa.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 750 ℃, and hot isostatic pressing pressure is 250MPa, and the hot isostatic pressing soaking time is 1h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 13
Take by weighing raw material weight per-cent W 3%, B
4C's 5%, Al 90%, Cr
2O
32%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 22h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 200MPa, 22 ℃ of temperature, time 20min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 1000 ℃, and hot isostatic pressing pressure is 90MPa, and the hot isostatic pressing soaking time is 2h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material.
Embodiment 14
Take by weighing raw material weight per-cent W 10%, B
4C70%'s, Al17%, Y
2O
33%; Each component material is mixed by prescription, carry out ball milling in the stainless steel jar mill of packing into, adopt sintered carbide ball, Ball-milling Time 22h; Powder behind the ball milling soft mode of packing into carries out cold isostatic compaction, and isostatic cool pressing pressure is 220MPa, 25 ℃ of temperature, time 25min.The base of will the colding pressing HIP sintering after the jacket sealing of packing into, hot isostatic pressing gas is argon gas, and hip temperature is 900 ℃, and hot isostatic pressing pressure is 120MPa, and the hot isostatic pressing soaking time is 2h.To can prepare tungstenic B behind the material release behind the hot isostatic pressing
4The C/Al composite shielding material
Performance index:
Table 1 contains WO
3B
4The composition of C/Al matrix material and shielding properties
Table 2 contains W
2B
5B
4The composition of C/Al or Al alloy composite and shielding properties
Table 2 contains W, W
2O
5B
4The composition of C/Al or Al alloy composite and shielding properties
Annotate: 1. the thick 4cm of shielding material, diameter 100cm.
2. neutron energy is the Cf-252 fission spectrum, and energy of γ ray is 661keV.
More than table is found out the tungstenic B for preparing among the present invention
4C/ aluminium alloy compound shielding material W
2B
5And B
4C is evenly distributed, and densification degree is high, and intensity and toughness are good, is specially adapted to neutron/gamma shielding field.More traditional composite shielding material is compared, and the neutron radiation shielding is had good performance, simultaneously the gamma-radiation shielding properties is improved 5-20% or more.
Claims (6)
1. composite shielding material, it is characterized in that: the component by following weight per-cent forms: the W of 0-30% or the compound of W, the B of 0-70%
4C, the aluminum or aluminum alloy of 0-90%, other element of 0-8%.
2. a kind of composite shielding material according to claim 1, it is characterized in that: the compound of described W or W is W, WO
3, W
2O
5Or W
2B
5
3. a kind of composite shielding material according to claim 1, it is characterized in that: described other element is Ti, Si, Mg, Zr, V, Cr or its compound, rare earth element.
4. a kind of composite shielding material according to claim 3, it is characterized in that: the compound of described other element is TiB
2, TiO
2, SiO
2, MgO, ZrO
2, V
2O
5, Cr
2O
3, Y
2O
3Or La
2O
3
5. prepare a kind of method of composite shielding material, it is characterized in that: step is as follows:
Step 1, take by weighing the W of raw material weight per-cent: 0-30% or the compound of W; The B of 0-70%
4C; The aluminum or aluminum alloy of 0-90%; Other element of 0-8%;
Step 2, mix each component material, carry out ball milling in the ball grinder of packing into, inject argon gas in the ball grinder as protective atmosphere, Ball-milling Time 2-25h obtains mixed powder;
Step 3, mixed powder are packed into and are adopted cold isostatic compaction behind the soft mode, and pressure is 100-270MPa, time 5-60min;
Step 4, the base of will colding pressing carry out HIP sintering, and hot isostatic pressing gas is argon gas, and temperature is 680-1200 ℃, and pressure is 30-150MPa, and the time is 20-180min;
Material behind step 5, the hot isostatic pressing namely gets composite shielding material after the demoulding.
6. the method for a kind of composite shielding material described in according to claim 5, it is characterized in that: described ball grinder is stainless steel jar mill, abrading-ball is sintered carbide ball.
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