CN112552600A - Neutron shielding material for rotational molding and rotational molding product with neutron shielding effect - Google Patents

Neutron shielding material for rotational molding and rotational molding product with neutron shielding effect Download PDF

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CN112552600A
CN112552600A CN202110199506.XA CN202110199506A CN112552600A CN 112552600 A CN112552600 A CN 112552600A CN 202110199506 A CN202110199506 A CN 202110199506A CN 112552600 A CN112552600 A CN 112552600A
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boron
rotational molding
neutron shielding
neutron
parts
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CN112552600B (en
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雷伟伟
成鹏
于广益
姜朋飞
刘天宇
翁伟
费楚然
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Cgn High Tech Nuclear Materials Technology Suzhou Co ltd
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Cgn High Tech Nuclear Materials Technology Suzhou Co ltd
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    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K13/00—Use of mixtures of ingredients not covered by one single of the preceding main groups, each of these compounds being essential
    • C08K13/04—Ingredients characterised by their shape and organic or inorganic ingredients
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
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    • B32B27/18—Layered products comprising a layer of synthetic resin characterised by the use of special additives
    • B32B27/20—Layered products comprising a layer of synthetic resin characterised by the use of special additives using fillers, pigments, thixotroping agents
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    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
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    • B32—LAYERED PRODUCTS
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    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
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    • C08K3/38—Boron-containing compounds
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    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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    • C08K7/02—Fibres or whiskers
    • C08K7/04—Fibres or whiskers inorganic
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    • C08K7/02—Fibres or whiskers
    • C08K7/04—Fibres or whiskers inorganic
    • C08K7/06—Elements
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F1/00—Shielding characterised by the composition of the materials
    • G21F1/02—Selection of uniform shielding materials
    • G21F1/10—Organic substances; Dispersions in organic carriers
    • G21F1/103—Dispersions in organic carriers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2250/00—Layers arrangement
    • B32B2250/03—3 layers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2250/00—Layers arrangement
    • B32B2250/24—All layers being polymeric
    • B32B2250/242—All polymers belonging to those covered by group B32B27/32
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    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/20—Properties of the layers or laminate having particular electrical or magnetic properties, e.g. piezoelectric
    • B32B2307/212—Electromagnetic interference shielding
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Abstract

The invention relates to a neutron shielding material for rotational molding and a rotational molding product with a neutron shielding effect, wherein the neutron shielding material for rotational molding comprises a material A and a material B, wherein the material A comprises the following components in parts by weight: 100 parts of polypropylene, 0.2-1 part of first antioxidant, 0.1-0.5 part of first lubricant, 10-25 parts of heavy metal compound and 10-30 parts of boron-containing element fiber; the material B comprises: 100 parts of polypropylene, 0.2-1 part of second antioxidant, 0.1-0.5 part of second lubricant and 5-20 parts of compound containing boron element; the boron-containing compound is a non-fibrous material. The neutron shielding material for rotational molding has the advantages of simple preparation process, good heat resistance of the material and higher radiation shielding efficiency, and the formed rotational molding product with the neutron shielding effect can be designed in structure, so that the radiation shielding requirements of different facilities are met, and the influence of neutrons on personnel and environment can be effectively reduced.

Description

Neutron shielding material for rotational molding and rotational molding product with neutron shielding effect
Technical Field
The invention relates to the technical field of neutron shielding, in particular to a neutron shielding material for rotational molding and a rotational molding product with a neutron shielding effect.
Background
Rotational molding or rotational molding, in which a certain amount of plastic powder prepared in advance is added into a mold, the mold performs spatial spherical motion along with a rotating arm of a machine and is heated, the plastic powder is gradually melted and attached to the molding surface of the mold under the action of gravity, heat conduction and heat radiation, and then the product is obtained by cooling and demolding. The rotational molding process can mold hollow plastic products with large surface area, uniform thickness and smooth inner and outer surfaces, such as large storage tanks, containers, yachts and the like.
With the rapid development of industries such as nuclear energy, irradiation processing, nondestructive testing, radiation therapy and the like, high-energy rays are widely applied to various fields such as industry, medical treatment, scientific research and the like. Common high-energy rays include X-rays, gamma rays, neutrons and the like, and the problems of irradiation and protection of the high-energy rays are always the key points of attention. The radiation hazard effectiveness generated by neutrons is about 2.5 times of that of rays, the neutron shielding is more complex than the simple gamma ray shielding, the shielding of fast neutrons and thermal neutrons is considered, and the condition that a shielding material reacts with neutrons to emit gamma rays is also considered, so that the shielding and the protection of neutrons in actual work become more complex. The neutron shielding material has wide application in the fields of national defense scientific research, radioactive medicine, nuclear industry, aerospace and the like, can prevent neutron rays from entering the activity space of a human body, and protects the safety of personnel.
The traditional neutron shielding material mainly uses boron-based or lead-based polyethylene composite shielding material as a main body. The material has good effects on the deceleration of fast neutrons and the capture of slow neutrons, and has been widely applied since the development and the success in the last 80 th century. Although the boron-based or lead-based polyethylene composite shielding material has the comprehensive effect of shielding neutrons and rays, the boron-based or lead-based polyethylene composite shielding material has extremely short service life and frequent use and replacement due to poor heat resistance and low strength and is not suitable for being applied to a working environment with temperature requirements. The traditional neutron shielding material is prepared by directly blending polymer and fillers such as lead, boron and the like, the obtained neutron shielding material has low shielding efficiency, and the good shielding efficiency can be achieved only by high filler addition and large thickness.
In addition, the equipment in the nuclear experiment and the application process has different shapes and complex structures. At present, most of the commonly used neutron shielding materials are of plate or sheet structures, and are difficult to process into shielding protection devices with large sizes and complex shapes, so that the neutron shielding materials are more limited in practical application, and the using effect is not ideal.
Disclosure of Invention
In order to solve the technical problems, the invention aims to provide a neutron shielding material for rotational molding and a rotational molding product with a neutron shielding effect.
The invention provides a neutron shielding material for rotational molding, which comprises a material A and a material B, wherein:
the material A comprises the following components in parts by weight:
100 parts of polypropylene, 0.2-1 part of first antioxidant, 0.1-0.5 part of first lubricant, 10-25 parts of heavy metal compound and 10-30 parts of boron-containing element fiber;
the B material comprises the following components in parts by weight:
100 parts of polypropylene, 0.2-1 part of second antioxidant, 0.1-0.5 part of second lubricant and 5-20 parts of compound containing boron element; the boron-containing compound is a non-fibrous material.
Further, the mass ratio of the material A to the material B is 1:2-2: 1.
Furthermore, the impact strength of the polypropylene in the materials A and B at the notch of the simply supported beam is more than or equal to 20KJ/m2And the melt index at 230 ℃ and under the condition of 2.16kg is 10-50g/10 min.
Further, the heavy metal compound is one or more of tungsten oxide, barium carbonate, barium sulfate, lead acetate, lead oxide, lead octoate, bismuth oxide and bismuth hydroxide, the particle size of the heavy metal compound is 200-1000 meshes, and the purity is more than 99%.
Further, the boron-containing fiber is a boron fiber and/or a boron nitride fiber, and the length of the boron-containing fiber is 3-10 mm.
Further, the compound containing the boron element is one or more of boron oxide, boric acid, boron nitride and boron carbide, the particle size is 200-1000 meshes, and the purity is more than 99%.
Further, the first antioxidant and the second antioxidant are respectively and independently selected from one or more of antioxidant 1010, antioxidant 168, antioxidant 1076, antioxidant 445, antioxidant 245, antioxidant 3114, antioxidant 1035, antioxidant 1098, antioxidant 1024, antioxidant 300, antioxidant 618, antioxidant 626, antioxidant DSTDP, antioxidant DLTDP, antioxidant RD, antioxidant MBZ and antioxidant 330. Preferably, the first antioxidant and the second antioxidant are each independently selected from one or more of antioxidant 1010, antioxidant 168 and antioxidant 1076.
Further, the first lubricant and the second lubricant are respectively and independently selected from one or more of zinc stearate, calcium stearate, ethylene bis stearamide, stearic acid amide, glyceryl stearate, erucamide, oleic acid amide, silicone, polyethylene wax and polypropylene wax. Preferably, the first lubricant and the second lubricant are respectively and independently selected from one or more of calcium stearate, zinc stearate, ethylene bis stearamide and erucamide.
Further, the material A and the material B also comprise additives, and the additives in the material A and the material B are respectively and independently selected from one or more of light stabilizer, coupling agent, antistatic agent, nucleating agent, flame retardant, toner and processing aid.
The contents of the lubricant, light stabilizer, nucleating agent, flame retardant, toner and processing aid are not particularly limited and may be conventional contents well known to those skilled in the art or may be appropriately adjusted according to the requirements of actual conditions.
The second purpose of the invention is to disclose a preparation method of a rotational molding product with neutron shielding effect, which is prepared by adopting the neutron shielding material for rotational molding and comprises the following steps:
(1) melting and blending polypropylene, a first antioxidant, a first lubricant and a heavy metal compound, granulating and grinding the mixture, and then uniformly mixing the ground powder and boron-containing fiber to obtain a material A;
melting and blending polypropylene, a second antioxidant, a second lubricant and a compound containing boron, granulating and grinding to obtain a material B;
(2) performing rotational molding on the material A, wherein the components in the material A sequentially form a gamma-ray absorption layer and a neutron absorption layer from outside to inside; and after the material A is melted and formed, adding a material B for rotational molding, wherein the material B is formed into a neutron slowing layer on the inner side of the neutron absorption layer.
Further, in the step (1), the melt blending may be performed by a single screw extruder, a twin screw extruder or an internal mixer, and the melt blending processing temperature is 190 ℃ to 230 ℃. The milling powder can be made by a plastic mill, and the technological parameters are milling current of 60-90A and milling disc rotating speed of 2000-4000 rpm.
Preferably, step (1) is as follows:
preparing raw materials according to the weight, and stirring polypropylene, a first antioxidant, a first lubricant and a heavy metal compound in a high-speed mixer at the speed of 50rpm for 8 minutes to obtain a mixture 1; after the mixture 1 is melted and blended, granulating and grinding; stirring the ground powder and the boron-containing fiber in a high-speed mixer at the speed of 30rpm for 3 minutes to obtain a material A;
preparing raw materials according to the weight, and stirring polypropylene, a second antioxidant, a second lubricant and a boron-containing compound in a high-speed mixer at the speed of 50rpm for 8 minutes to obtain a mixture 2; and (3) melting and blending the mixture 2, and granulating and grinding to obtain a material B.
In the rotational molding process of the neutron shielding material for rotational molding, the polypropylene powder in the material A is firstly melted and adhered to the inner surface of a mold, the boron-containing element fiber in the material A has larger length and is gathered in the inner layer of the material A, and the heavy metal compound is gathered in the polypropylene at the outermost layer. After the material A is completely melted, the material B is added. The formed rotational moulding product has a multilayer structure and comprises an outer layer and an intermediate layer formed by material A and an inner layer formed by material B, wherein the polypropylene and the compound containing boron (derived from material B) of the innermost layer can moderate fast neutrons to be used as a neutron slowing layer, the intermediate fiber layer containing boron (derived from material A) can absorb slow neutrons to be used as a neutron absorbing layer, and the heavy metal compound (derived from material A) of the outermost layer can absorb secondary gamma rays to be used as a gamma ray absorbing layer.
The invention also claims a rotational molding product with neutron shielding effect prepared by the preparation method, which comprises an outer layer and an intermediate layer formed by the material A and an inner layer formed by the material B, wherein the outer layer is a gamma ray absorption layer, the intermediate layer is a neutron absorption layer, and the inner layer is a neutron moderating layer.
By the scheme, the invention at least has the following advantages:
1. the neutron shielding material for rotational molding disclosed by the invention respectively uses boron-containing element fiber and a boron-containing compound, and the boron-containing element fiber and the boron-containing compound are distributed at different positions of a product after molding, so that different neutron absorption effects can be realized. The boron-containing compound is distributed in the innermost layer of the product and can be used for moderating fast neutrons, the boron-containing fiber is distributed in the middle layer of the product and can be used for absorbing slow neutrons, and the heavy metal compound in the outermost layer can be used for absorbing gamma rays. The neutron shielding material disclosed by the invention is reasonable in formula design, and a product with better shielding efficiency can be obtained only by using a lower filler addition amount and a smaller product thickness through the forming method.
2. The preparation method of the special rotational molding material is simple, the molded product has a multilayer structure, can simultaneously realize neutron moderation and absorption, shields secondary gamma rays, greatly improves the neutron shielding efficiency of the material, and meets the comprehensive shielding requirement of radiation protection. The formed product has smooth inner and outer surfaces, high mechanical strength, good heat resistance, wide application temperature range and neutron transmissivity less than 2%. The shielding and protecting device with different sizes and complex shapes can be prepared according to the forming die, and the using requirements under different scenes are met.
The foregoing is a summary of the present invention, and in order to provide a clear understanding of the technical means of the present invention and to be implemented in accordance with the present specification, the following is a preferred embodiment of the present invention and is described in detail below.
Drawings
FIG. 1 is a schematic cross-sectional view of a rotomoulded article having neutron shielding effectiveness according to the present invention;
description of reference numerals:
a 1-gamma ray absorbing layer; 2-a neutron absorbing layer; 3-neutron moderation layer.
Detailed Description
The following examples are given to further illustrate the embodiments of the present invention. The following examples are intended to illustrate the invention but are not intended to limit the scope of the invention.
Examples
TABLE 1 formulation composition of materials A and B
Figure 375647DEST_PATH_IMAGE001
Figure 837853DEST_PATH_IMAGE002
Figure 857761DEST_PATH_IMAGE003
The neutron shielding material for rotational molding in the embodiment is used for preparing rotational molding products, and the steps are as follows:
(1) preparing raw materials according to weight, and stirring polypropylene, a first antioxidant, a first lubricant and a heavy metal compound in a high-speed mixer at a speed of 50rpm for 8 minutes to obtain a first mixture; melting and blending the first mixture, granulating and grinding; stirring the ground powder and the boron-containing fiber in a high-speed mixer at the speed of 30rpm for 3 minutes to obtain a material A;
preparing raw materials according to the weight, and stirring polypropylene, a second antioxidant, a second lubricant and a boron-containing compound in a high-speed mixer at the speed of 50rpm for 8 minutes to obtain a second mixture; and (4) melting and blending the second mixture, granulating and grinding to obtain material B. The melt blending can be carried out by a single screw extruder, a double screw extruder or an internal mixer, and the melt blending processing temperature is 210 ℃. The milling powder can be made by a plastic mill, and the technological parameters are milling current 75A and milling disc rotating speed 3000 rpm.
(2) Performing rotational molding on the material A, wherein the components in the material A sequentially form a gamma-ray absorption layer 1 and a neutron absorption layer 2 from outside to inside; and after the material A is melted and formed, adding the material B for rotational molding, and forming the neutron moderating layer 3 by the material B. The structure of the rotomoulded article produced is shown in figure 1.
The rotomoulded articles prepared above were tested for their performance under the following test conditions:
and (3) testing the bending property: testing according to ISO-178 standard;
impact strength of the simply supported beam notch: testing according to ISO-179 standard;
load deformation temperature: testing according to ISO-75 standard;
vicat softening point: testing according to ISO-306 standard;
and (3) testing neutron shielding performance: the activity of the neutron source placed in a paraffin case is 1.11 multiplied by 10 by adopting an Am-Be neutron source test10Bq, a cylindrical opening with the depth of 13cm and the diameter of 11cm is arranged at one end from the source box surface to the detector, and the neutron detector is3He proportional counter tube, placed 50cm from the source and facing the source box opening. The sample is located between the source and the counter tube, against the source box opening. And a NaI gamma spectrometer detector is closely attached to the neutron detector to measure secondary gamma rays generated by the neutron shielding material.
The results are shown in Table 2.
TABLE 2 results of Performance test of shaped articles of different materials
Figure 467210DEST_PATH_IMAGE004
The above is only a preferred embodiment of the present invention, and is not intended to limit the present invention, it should be noted that, for those skilled in the art, many modifications and variations can be made without departing from the technical principle of the present invention, and these modifications and variations should also be regarded as the protection scope of the present invention.

Claims (10)

1. A neutron shielding material for rotational molding is characterized in that: comprises a material A and a material B, wherein,
the material A comprises the following components in parts by weight:
100 parts of polypropylene, 0.2-1 part of first antioxidant, 0.1-0.5 part of first lubricant, 10-25 parts of heavy metal compound and 10-30 parts of boron-containing element fiber;
the material B comprises the following components in parts by weight:
100 parts of polypropylene, 0.2-1 part of second antioxidant, 0.1-0.5 part of second lubricant and 5-20 parts of compound containing boron element; the boron-containing compound is a non-fibrous material.
2. The neutron shielding material for rotational molding according to claim 1, wherein: the mass ratio of the material A to the material B is 1:2-2: 1.
3. The neutron shielding material for rotational molding according to claim 1, wherein: the impact strength of the gaps of the polypropylene simple-supported beams in the materials A and B is more than or equal to 20kJ/m2And the melt index at 230 ℃ and under the condition of 2.16kg is 10-50g/10 min.
4. The neutron shielding material for rotational molding according to claim 1, wherein: the heavy metal compound is one or more of tungsten oxide, barium carbonate, barium sulfate, lead acetate, lead oxide, lead octoate, bismuth oxide and bismuth hydroxide, and the particle size of the heavy metal compound is 200-1000 meshes.
5. The neutron shielding material for rotational molding according to claim 1, wherein: the boron-containing fiber is a boron fiber and/or a boron nitride fiber, and the length of the boron-containing fiber is 3-10 mm.
6. The neutron shielding material for rotational molding according to claim 1, wherein: the compound containing the boron element is one or more of boron oxide, boric acid, boron nitride and boron carbide, and the particle size is 200-1000 meshes.
7. The neutron shielding material for rotational molding according to claim 1, wherein: the material A and the material B also comprise additives, and the additives in the material A and the material B are respectively and independently selected from one or more of light stabilizer, coupling agent, antistatic agent, nucleating agent, flame retardant, toner and processing aid.
8. A method for preparing a rotomoulded product with neutron shielding effect, which is characterized by adopting the neutron shielding material for rotomoulding of any one of claims 1 to 7, and comprises the following steps:
(1) melting and blending polypropylene, a first antioxidant, a first lubricant and a heavy metal compound, granulating and grinding the mixture, and then uniformly mixing the ground powder and boron-containing fiber to obtain a material A;
melting and blending polypropylene, a second antioxidant, a second lubricant and a compound containing boron, granulating and grinding to obtain a material B;
(2) performing rotational molding on the material A, wherein the components in the material A sequentially form a gamma-ray absorption layer and a neutron absorption layer from outside to inside; and after the material A is subjected to melt molding, adding a material B for rotational molding, wherein the material B is formed into a neutron slowing layer on the inner side of the neutron absorption layer.
9. The method of claim 8, wherein: in the step (1), a single-screw extruder, a double-screw extruder or an internal mixer is adopted for melt blending, and the melt blending processing temperature is 190-230 ℃.
10. The rotomoulded article having a neutron shielding effect produced by the production method according to claim 8, comprising an outer layer and an intermediate layer formed from material A, and an inner layer formed from material B, wherein the outer layer comprises a gamma ray absorbing layer, the intermediate layer comprises a neutron absorbing layer, and the inner layer comprises a neutron slowing layer.
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