WO2016202291A1 - 用于屏蔽放射性射线的屏蔽材料及其制备方法 - Google Patents

用于屏蔽放射性射线的屏蔽材料及其制备方法 Download PDF

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WO2016202291A1
WO2016202291A1 PCT/CN2016/086223 CN2016086223W WO2016202291A1 WO 2016202291 A1 WO2016202291 A1 WO 2016202291A1 CN 2016086223 W CN2016086223 W CN 2016086223W WO 2016202291 A1 WO2016202291 A1 WO 2016202291A1
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shielding
shielding material
barite
less
fine aggregate
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PCT/CN2016/086223
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English (en)
French (fr)
Inventor
张敏娟
陈韦霖
刘渊豪
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南京中硼联康医疗科技有限公司
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Priority to EP16811032.8A priority Critical patent/EP3293161B1/en
Publication of WO2016202291A1 publication Critical patent/WO2016202291A1/zh
Priority to US15/826,998 priority patent/US10636534B2/en

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    • 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
    • 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
    • G21F1/04—Concretes; Other hydraulic hardening materials
    • G21F1/042—Concretes combined with other materials dispersed in the carrier
    • G21F1/047—Concretes combined with other materials dispersed in the carrier with metals
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B14/00—Use of inorganic materials as fillers, e.g. pigments, for mortars, concrete or artificial stone; Treatment of inorganic materials specially adapted to enhance their filling properties in mortars, concrete or artificial stone
    • C04B14/02—Granular materials, e.g. microballoons
    • C04B14/04—Silica-rich materials; Silicates
    • C04B14/22—Glass ; Devitrified glass
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B14/00—Use of inorganic materials as fillers, e.g. pigments, for mortars, concrete or artificial stone; Treatment of inorganic materials specially adapted to enhance their filling properties in mortars, concrete or artificial stone
    • C04B14/02—Granular materials, e.g. microballoons
    • C04B14/36—Inorganic materials not provided for in groups C04B14/022 and C04B14/04 - C04B14/34
    • C04B14/368—Baryte
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B24/00—Use of organic materials as active ingredients for mortars, concrete or artificial stone, e.g. plasticisers
    • C04B24/04—Carboxylic acids; Salts, anhydrides or esters thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B28/00—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements
    • C04B28/02—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements containing hydraulic cements other than calcium sulfates
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B28/00—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements
    • C04B28/02—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements containing hydraulic cements other than calcium sulfates
    • C04B28/04—Portland cements
    • 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
    • G21F1/04—Concretes; Other hydraulic hardening materials
    • 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
    • G21F1/04—Concretes; Other hydraulic hardening materials
    • G21F1/042—Concretes combined with other materials dispersed in the carrier
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2103/00—Function or property of ingredients for mortars, concrete or artificial stone
    • C04B2103/30—Water reducers, plasticisers, air-entrainers, flow improvers
    • C04B2103/302—Water reducers
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
    • C04B2111/00474—Uses not provided for elsewhere in C04B2111/00
    • C04B2111/00862—Uses not provided for elsewhere in C04B2111/00 for nuclear applications, e.g. ray-absorbing concrete

Definitions

  • the invention relates to a shielding material, in particular to a shielding material for shielding radioactive rays; the invention also relates to a method for preparing a shielding material, in particular to a method for preparing a shielding material for shielding radioactive rays.
  • the shielding material used to shield radioactive rays is a new type of material that can effectively protect the human body from harmful radiation.
  • the development and application of shielding materials for shielding radioactive rays has been developed with the development and application of the atomic energy industry and nuclear technology.
  • nuclear technology has not only been used in national defense construction, but has also penetrated into many fields such as industry, agriculture, and medical care, such as nuclear power generation, industrial applications of isotopes, medical testing and drug manufacturing, and the sealing of nuclear waste.
  • how to prevent the damage of various rays generated by nuclear radiation to the human body has become a problem that cannot be ignored in the utilization of nuclear technology.
  • Radioactive rays mainly include X-rays, alpha rays, beta rays, gamma rays, neutron rays, proton rays, and the like. Their penetration ability is different. Alpha, beta particles and protons have a charge, and when they interact with the atomic electric field of the protective substance, their energy is reduced, and even a small thickness of protective material can completely block them. Therefore, the concrete used to shield radioactive rays is mainly shielded by X-rays, gamma rays and neutron rays.
  • X-ray is an electromagnetic wave with a very short wavelength and a large energy.
  • the wavelength of X-ray is shorter than the wavelength of visible light (about 0.001-100 nm, and the wavelength of X-ray applied in medicine is about 0.001-0.1 nm).
  • Its photon energy is tens of thousands to hundreds of thousands times greater than the photon energy of visible light.
  • X-rays have a short wavelength and a large energy. When they are applied to a substance, only a part of them are absorbed by the substance, and most of them are transmitted through the interatomic space, showing a strong penetrating power.
  • the ability of X-rays to penetrate a substance is related to the energy of X-ray photons.
  • the penetrating power of X-rays is also related to the density of matter. By using this property of difference absorption, substances with different densities can be distinguished.
  • ⁇ ray is a high-energy, high-frequency electromagnetic wave with great penetrating power.
  • the protective substance When it passes through the protective substance, it can be gradually absorbed, but only when the protective material exceeds a certain thickness, it can be completely absorbed.
  • Neutrons are particles that have no charge in the nucleus.
  • Neutron rays are the neutron flux of these uncharged neutrons. According to the size of energy and the speed of motion, neutron rays are divided into slow neutrons, medium-speed neutrons, and fast neutrons.
  • the nucleus can only capture slow neutrons.
  • Fast neutrons can only decelerate by colliding with the nucleus, but The nucleus of some substances and the neutron collide to produce a second gamma ray.
  • Medium-speed neutrons can be slowed down to the required energy by the light element nucleus.
  • Radiation rays generated by atomic reactors and accelerators are mainly concentrated in gamma rays and neutron rays, and even if X-rays are generated, they are small in amount and low in energy, and shielding materials for shielding radioactivity can easily achieve shielding of X-rays. Therefore, the protection problems of atomic reactors and accelerators mainly come down to the problem of protecting gamma rays and neutron rays.
  • Ordinary concrete is an inexpensive and satisfactory shielding material for shielding radioactive rays, but its density is not large and the combined water is not much. Therefore, the thickness of the conventional concrete structure needs to be increased.
  • the radiation-proof concrete not only the bulk density is high, but also the combined water is required, and the concrete is required to have good homogeneity.
  • the shrinkage of the concrete structure during construction and use should be minimal, and defects such as voids and cracks are not allowed.
  • concrete is required to have a certain structural strength and fire resistance.
  • a shielding material for shielding radioactive rays which is suitably composed of light elements and heavy elements and has good mechanical properties, water resistance and construction properties.
  • the material containing light and heavy elements may be in a layered arrangement or a homogeneous mixture.
  • the shielding material is composed of water, cementing material, fine aggregate, coarse aggregate and admixture, wherein fine
  • the aggregate consists of borosilicate glass and barite sand.
  • the coarse aggregate consists of lead stone and barite.
  • the boron element content in the borosilicate powder accounts for 0.5% to 1% of the total weight of the shielding material; barite sand and heavy
  • the content of barium sulfate in the spar is 71%-75% of the total weight of the shielding material; the other content is water, cementitious material and admixture, and the sum of all components is 100% of the total weight of the shielding material.
  • the cementing material is P.II 52.5 type Portland cement
  • the admixing agent is one or more of a water reducing agent, an early strength agent, a retarder, a pumping agent and a swelling agent.
  • the density of the shielding material is 3.46 to 3.55 g/cm 3 .
  • the admixture is selected from a polycarboxylic acid type water reducing agent.
  • the shielding material in this embodiment is suitable for use in neutron capture therapy for neutron and gamma ray-containing radiation sources.
  • An aspect of an embodiment of the present invention provides a method of preparing a shielding material for shielding radioactive rays, comprising the steps of:
  • Boron glass is crushed and sieved to obtain a boron glass powder for fine aggregate having a particle diameter of less than 4.75 mm and not less than 75 ⁇ m;
  • the lead stone is crushed and sieved to obtain a lead stone for coarse aggregate having a particle diameter of 5 mm or more and 10 mm or less;
  • the water and the admixture container are pre-stirred with a part of the mixture for a preset time t, wherein 30s ⁇ t ⁇ 60s;
  • the mixer is stirred and discharged.
  • Another aspect of an embodiment of the present invention provides a method of preparing a shielding material for shielding radioactive rays, comprising the steps of:
  • Boron glass is crushed and sieved to obtain a boron glass powder for fine aggregate having a particle diameter of less than 4.75 mm and not less than 75 ⁇ m;
  • the water and the admixture container are pre-stirred with a part of the mixture for a preset time t, wherein 30s ⁇ t ⁇ 60s;
  • the mixer is stirred and discharged.
  • Figure 1 is an energy spectrum of neutrons and gamma rays in a radiation source exiting a beam exit from a neutron capture treatment used in an embodiment of the present invention.
  • Embodiments 1 to 3 of the present invention is a neutron shielding effect according to Embodiments 1 to 3 of the present invention and a comparative example at different thicknesses.
  • Embodiments 1 to 3 of the present invention is a gamma ray shielding effect according to Embodiments 1 to 3 of the present invention and a comparative example at different thicknesses.
  • the following examples employ a neutron capture therapeutic source containing neutrons and gamma rays to highlight the effects of shielding neutrons and gamma rays of the following embodiments of the shielding material for shielding radioactive rays of the present invention.
  • FIG. 1 shows the energy spectrum of neutrons and gamma rays in the radiation source from the beam exit of the neutron capture treatment, considering the neutron and gamma ray intensity 4.5 meters away from the beam exit.
  • the figure below shows the energy spectrum distribution before the beam hits the front shield wall.
  • the embodiments of the present invention are exemplified only by the source of the radiation, and do not limit the kind of the source of the radiation, which is well known to those skilled in the art, and the teachings and the teachings according to the embodiments of the present invention are used for shielding in the embodiments of the present invention.
  • the shielding material for radioactive rays can also be used for other radiation sources having different energy spectra including neutrons and gamma rays.
  • the shielding material in the following embodiments is composed of water, cementing material, fine aggregate, coarse aggregate and admixture, wherein the fine aggregate is composed of borosilicate powder and barite sand, and the coarse aggregate is composed of lead stone and barite.
  • the cementing material selected for the shielding material is P.II 52.5 type Portland cement, and the admixture is one or more of a water reducing agent, an early strength agent, a retarder, a pumping agent and a swelling agent, the first type
  • the density of the shielding material is 3.46 to 3.55 g/cm 3
  • the density of the second shielding material is 3.73 to 4.01 g/cm 3 .
  • the admixture can be determined according to specific embodiments, and preferably, the admixture in the examples is a polycarboxylic acid-based water reducing agent. The specific development of the embodiment will be described below.
  • the shielding material consists of water, cementitious material, fine aggregate, coarse aggregate and admixture.
  • the weight of water accounts for 2.48% of the total weight of the shielding material
  • the cementitious material is selected from Portland cement of P.II52.5
  • the fine aggregate is composed of borosilicate glass and barite sand
  • the coarse aggregate is composed of barite.
  • the admixture is selected from the group consisting of polycarboxylic acid type water reducing agent, wherein the weight of boron element accounts for 0.51% of the total weight of the shielding material, and the barium sulfate content accounts for 75.33% of the total weight of the shielding material.
  • Other contents are gelling materials and admixtures, all components. The sum of the contents is 100% of the total weight of the shielding material.
  • the preparation process mainly comprises: 1. crushing and sieving the barite ore to obtain a barite sand for fine aggregate having a particle diameter of less than 4.75 mm and not less than 75 ⁇ m; 2. being broken by the barite ore, Screening to obtain barite for coarse aggregate having a particle diameter of not less than 4.75 mm; 3. crushing and sieving the boron glass to obtain boron for fine aggregate having a particle diameter of less than 4.75 mm and not less than 75 ⁇ m. Glass powder; 4. Put cement, coarse aggregate and fine aggregate into the container to form part of the mixture; 5. Pre-stir the water and the admixture container with the partial mixture for a preset time t, where 30s ⁇ t ⁇ 60s; 6. Mixer and discharge.
  • either a mixer or a dump truck can be used, but the applicable range should be considered. It is important that the shielding material is transported and poured as close as possible to the state at the end of the agitation. Transportation must be fast, and the time from the start of the agitation to the delivery to the site should be controlled. According to the current national standard "Concrete Quality Control Standards" GB 50164, when the outside temperature is lower than 25 °C, the truck is transported by mixer, and the concrete is equal to or higher than C30. Not more than 90min; when it exceeds 25 °C, concrete of C30 or more should not be greater than 60min.
  • the current national standard "premixed concrete" GB/T 14902 stipulates that the concrete conveyed by the mixer truck should be discharged within 1.5h; the concrete transported by the dump truck should be discharged within 1.0h; when the maximum temperature is lower than 25 At °C, the delivery time can be extended by 0.5h.
  • the 90 min is stipulated that the longer the time, the greater the slump loss of the concrete, and the workability of the concrete cannot be guaranteed.
  • the performance can not meet the requirements, it can be adjusted by adding the admixture on the basis of the test and verification, and no water is allowed.
  • Technical measures such as admixture with a retarding effect to extend the concrete setting time are usually used.
  • the strength grade of the shielding material is C30 or C40, the standard value of the axial compressive strength of the shielding material should be 17.1-22.8N/mm 2 or higher, and the standard value of the axial tensile strength of the shielding material should be 1.70 ⁇ 2.05N/ Mm 2 or higher.
  • the cement type is selected from P.II52.5 type Portland cement, that is, the clinker + gypsum content is greater than or equal to 95% of the total weight of the cement, and the granulated blast furnace slag content is less than or equal to 5% of the total weight of the cement or the limestone content is less than or equal to 5% of the total weight of the cement.
  • the clinker mainly contains raw materials of CaO, SiO 2 , Al 2 O 3 and Fe 2 O 3 , and is ground to a fine powder to be partially melted to obtain a hydraulic gelling substance containing calcium silicate as a main mineral component.
  • the calcium silicate mineral is not less than 66%, and the mass ratio of calcium oxide to silicon oxide is not less than 2.0.
  • gypsum for the selection of gypsum, if natural gypsum is selected, it should meet the gypsum or mixed gypsum of Class G or M class II or higher specified in GB/T 5483; if industrial by-product gypsum is used, calcium sulfate should be used as the main component. The industrial by-products should be tested and proved to be harmless to the performance of the cement before use.
  • the insoluble matter (mass fraction) of the chemical index of P.II52.5 type Portland cement should be less than or equal to 1.50%, the loss on ignition (mass fraction) should be less than or equal to 3.5%, and the sulfur trioxide (mass fraction) should be less than or equal to 3.5%, magnesium oxide (mass fraction) should be less than or equal to 6.0%, and chloride ion (mass fraction) should be less than or equal to 0.06%.
  • the silicate cement grade is 52.5, the forming 3-day compressive strength is greater than or equal to 23.0 MPa, the flexural strength is greater than or equal to 4.0 MPa, the forming 28-day compressive strength is greater than or equal to 52.5 MPa, and the flexural strength is greater than or equal to 7.0 MPa.
  • the borosilicate powder accounts for 17% of the weight of the fine aggregate, and the barite sand accounts for 83% of the weight of the fine aggregate.
  • the shielding material had a bulk density (i.e., density) of 3,554 kg/m 3 and a sand ratio of 32.1%.
  • the water-to-binder ratio was 0.37, and the admixture dosage was 1.80%. Calculated according to the total demand of 500 tons, the weight of various substances required is listed in Table 1 below.
  • the shielding material consists of water, cementitious materials, fine aggregates, coarse aggregates and admixtures.
  • the weight of water accounts for 2.51% of the total weight of the shielding material
  • the cementitious material is selected from Portland cement of P.II52.5
  • the fine aggregate is composed of borosilicate glass and barite sand
  • the coarse aggregate is composed of barite.
  • the admixture is selected from the group consisting of polycarboxylic acid type water reducing agent, wherein the weight of boron element accounts for 0.75% of the total weight of the shielding material, the barium sulfate content accounts for 73.07% of the total weight of the shielding material, and the other content is gelling material and admixture, all components. The sum of the contents is 100% of the total weight of the shielding material.
  • the preparation method is the same as that of the first embodiment. According to the ratio and the preparation method, the borosilicate powder accounts for 26% of the weight of the fine aggregate, and the barite sand accounts for 74% of the weight of the fine aggregate.
  • the shielding material had a bulk density (i.e., density) of 3,508 kg/m 3 and a sand ratio of 31.0%.
  • the water-to-binder ratio was 0.37, and the admixture dosage was 1.80%. Calculated according to the total demand of 500 tons, the weight of various substances required is listed in Table 3 below.
  • the shielding material consists of water, cementitious materials, fine aggregates, coarse aggregates and admixtures.
  • the weight of water accounts for 2.55% of the total weight of the shielding material
  • the cementitious material is selected from Portland cement of P.II52.5
  • the fine aggregate is composed of borosilicate glass and barite sand
  • the coarse aggregate is composed of barite.
  • the admixture is selected from the group consisting of polycarboxylic acid type water reducing agent, wherein the weight of boron element accounts for 1.00% of the total weight of the shielding material, the barium sulfate content accounts for 70.76% of the total weight of the shielding material, and other contents are gelling materials and admixtures, all components. The sum of the contents is 100% of the total weight of the shielding material.
  • the preparation method is the same as that of the first embodiment. According to the ratio and the preparation method, the borosilicate powder accounts for 36% of the weight of the fine aggregate, and the barite sand accounts for 64% of the weight of the fine aggregate.
  • the shielding material has a bulk density (i.e., density) of 3457 kg/m 3 and a sand ratio of 29.8%.
  • the water-to-binder ratio was 0.37, and the admixture dosage was 1.80%. Calculated according to the total demand of 500 tons, the weight of various substances required is listed in Table 3 below.
  • Comparative Example 1 is a radiation shielding material commonly used in the market, and the weight percentage of the elements contained therein is as listed in Table 4 below:
  • Comparative Example 2 is another barite radiation shielding material whose weight is as listed in Table 5 below:
  • the shielding material in Comparative Example 1 is very cheap, but it requires very thick materials to meet the standard requirements; the shielding material in Comparative Example 2 is cheaper but requires a thicker thickness; boron-containing polyethylene + lead Although the shielding material of the brick is very thin and can meet the standard requirements, the price is very expensive.
  • the shielding material is not only moderately thick but also inexpensive.
  • the shielding material in the embodiment has obvious advantages in comparison with the comparative examples in both neutron and gamma shielding, and the effect is more remarkable with the increase of thickness.
  • the capture section of 10 B pairs of neutrons obeys the 1/v characteristic in the range of energy below 500 keV, so as the neutron energy decreases, the reaction cross section also increases.
  • the neutron of 0.025 eV has about 3866 states ( barn) captures the cross section, so the superheated neutrons are decelerated by the concrete to slow neutrons and are absorbed by the 10 B element.
  • 0.5% boron content plays a good neutron shielding effect, and the first and second ratios are in the middle. There is no significant difference in the sub-shield, and even the ordinary barite concrete shielding neutron in the second ratio is less effective. It can be seen that for the mixed radiation field of the neutron capture treatment, at least 0.5% of boron is incorporated into the concrete. It is very necessary.
  • the two comparative examples in Figure 3 clearly show that the barite concrete has a good ⁇ shielding effect, mainly because the barium sulfate in the barite enhances the apparent density of the concrete, that is, the higher the barium sulfate content and the apparent density. The larger the gamma shielding effect, the better.
  • the concrete developed by our company changes the content of three different borons on the basis of barite, highlighting the necessity of adding at least 0.5% boron to the concrete.
  • the ordinary barite concrete in the second ratio is comparatively proportional.
  • the general concrete has been significantly improved, but the effect of the embodiment 1 is greatly improved after adding 0.5% of boron.

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Abstract

一种用于屏蔽放射性射线的屏蔽材料及其制备方法。该屏蔽材料由水、胶凝材料、细骨料、粗骨料和外加剂组成，其中细骨料由硼玻璃粉和重晶石砂组成，粗集料由重晶石组成；硼玻璃粉中的硼元素含量占屏蔽材料总重量的0.5%-1%；重晶石砂和重晶石中的硫酸钡含量占屏蔽材料总重量的71%-75%；其他含量为水、胶凝材料和外加剂，所有成分的含量总和为屏蔽材料总重量的100%。

Description

用于屏蔽放射性射线的屏蔽材料及其制备方法 技术领域
本发明涉及一种屏蔽材料，尤其涉及一种用于屏蔽放射性射线的屏蔽材料；本发明还涉及一种屏蔽材料的制备方法，尤其涉及一种用于屏蔽放射性射线的屏蔽材料的制备方法。
背景技术
用于屏蔽放射性射线的屏蔽材料是一种能够有效防护对人体有害射线辐射的新型材料。用于屏蔽放射性射线的屏蔽材料的研制和应用是随着原子能工业和核技术的发展应用而发展起来的。近些年来，核技术不仅用于国防建设，而且已大量渗透到工业、农业、医疗等各个领域，如核能发电、同位素在工业上的应用、医疗检测及药物制造、核废料的封固等。在生产应用过程中，如何防止核辐射产生的各种射线对人体的伤害，已经是核技术利用中一个不可忽视的问题。
放射性射线主要包括X射线、α射线、β射线、γ射线、中子射线及质子射线等。它们的穿透能力是不同的。α、β粒子和质子具有电荷，当它们和防护物质的原子电场相互作用时，其能量降低，甚至厚度很小的防护材料也能完全挡住它们。因此用于屏蔽放射性射线的混凝土主要屏蔽的是X射线、γ射线和中子射线。
X射线是一种波长极短，能量很大的电磁波，X射线的波长比可见光的波长更短(约在0.001～100纳米，医学上应用的X射线波长约在0.001～0.1纳米之间)，它的光子能量比可见光的光子能量大几万至几十万倍。X射线因其波长短，能量大，照在物质上时，仅一部分被物质所吸收，大部分经由原子间隙而透过，表现出很强的穿透能力。X射线穿透物质的能力与X射线光子的能量有关，X射线的波长越短，光子的能量越大，穿透力越强。X射线的穿透力也与物质密度有关，利用差别吸收这种性质可以把密度不同的物质区分开来。
γ射线是一种高能量高频率的电磁波，具有极大的穿透能力。当它穿过防护物质，可以被逐渐吸收，但只有防护材料超过某一厚度时，才能完全被吸收。
中子是原子核中不具有电荷的粒子，中子射线即是这些不具电荷的中子构成的中子流。按能量的大小和运动的速度，中子射线又分为慢速中子、中速中子、快速中子，原子核只能俘获吸收慢中子，快中子只有通过与原子核碰撞才能减速，但某些物质的原子核和中子碰撞时会产生第二次γ射线。中速中子通过轻元素原子核可以减速到被俘获要求的能量。
原子反应堆和加速器产生的放射线射线主要集中在γ射线和中子射线，即使产生了X射线也是少量的且能量较低，用于屏蔽放射性的屏蔽材料能够容易的实现对X射线的屏蔽。因此，原子反应堆和加速器的防护问题主要归结为防护γ射线和中子射线的问题。
对于γ射线，物质的密度愈大，防护性能愈好。几乎所有的材料对γ射线都具有一定的防护能力，但是采用密度小的轻质材料时，则要求防护结构的厚度很大，这样增加了建筑面积和容积。采用铅、锌、钢铁等比重大的材料防护γ射线效果很高，防护结构可以做的较薄， 但这些材料价格昂贵。
对于快速中子和中速中子射线，不但需要重元素而且需要充分多的轻元素，最好含有较多的水，因为水中含有最轻元素氢，在这方面水具有优良的防护效果；对于慢速中子射线，则需要考虑含有吸收或屏蔽慢速中子的材料。
普通混凝土是低廉而满意的用于屏蔽放射性射线的屏蔽材料，但是其密度不大，结合水不多。因此，采用普通混凝土结构时的厚度需要增加。
对防辐射混凝土不但要求容重高含结合水多，而且要求混凝土具有良好的均质性。混凝土结构在施工和使用期中的收缩应最小，不允许存在空洞、裂纹等缺陷。除此之外，还要求混凝土具有一定的结构强度和耐火性。
因此，针对现有技术的缺陷，有必要提出一种由轻元素和重元素有适当组成的、具有良好的力学性能、防水性能和施工性能的用于屏蔽放射性射线的屏蔽材料。含轻、重元素的材料可以是分层布置，也可以是均匀的混合物。
发明内容
为了克服现有技术的缺陷，本发明的实施例中提出一种用于屏蔽放射性射线的屏蔽材料，该屏蔽材料由水、胶凝材料、细骨料、粗骨料和外加剂组成，其中细骨料由硼玻璃粉和重晶石砂组成，粗骨料由铅石和重晶石组成；硼玻璃粉中的硼元素含量占屏蔽材料总重量的0.5％～1％；重晶石砂和重晶石中的硫酸钡含量占屏蔽材料总重量的71％～75％；其他含量为水、胶凝材料和外加剂，所有成分的含量总和为屏蔽材料总重量的100％。
作为一种优选地，胶凝材料为P.II 52.5型硅酸盐水泥，外加剂为减水剂、早强剂、缓凝剂、泵送剂、膨胀剂中的一种或多种，所述屏蔽材料的密度为3.46～3.55g/cm3。
进一步地，外加剂选用聚羧酸系减水剂。
该实施例中的屏蔽材料适用于中子捕获治疗的包含中子和伽马射线的辐射源。
本发明的实施例的一方面提出了一种用于屏蔽放射性射线的屏蔽材料的制备方法，包括如下步骤：
由重晶石矿石经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的重晶石砂；
由重晶石矿石经破碎、筛分而得粒径不小于4.75mm的用于粗骨料的重晶石；
将硼玻璃经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的硼玻璃粉；
将铅石经破碎、筛分而得粒径大于等于5mm且小于等于10mm的用于粗骨料的铅石；
将水泥、粗骨料和细骨料投入容器内形成部分混合料；
将水和外加剂容器内，与部分混合料一起预搅拌预设时间t，其中30s≤t≤60s；
搅拌机搅拌出料。
本发明的实施例的另一方面提出了另一种用于屏蔽放射性射线的屏蔽材料的制备方法，包括如下步骤：
由重晶石矿石经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的重晶石砂；
由重晶石矿石经破碎、筛分而得粒径不小于4.75mm的用于粗骨料的重晶石；
将硼玻璃经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的硼玻璃粉；
将水泥、粗骨料和细骨料投入容器内形成部分混合料；
将水和外加剂容器内，与部分混合料一起预搅拌预设时间t，其中30s≤t≤60s；
搅拌机搅拌出料。
本发明实施例的有益效果在于：
1、很好的屏蔽中子和伽马射线(光子)的性能；
2、成本低廉；
3、厚度适中。
附图说明
图1是本发明实施例中使用的从中子捕获治疗的射束出口出来的放射源中的中子和伽马射线的能谱。
图2是本发明实施例一至三与对比例于不同厚度下的中子屏蔽效果。
图3是本发明实施例一至三与对比例于不同厚度下的伽马射线屏蔽效果。
具体实施方式
下面我们结合具体的实施例来对本发明的用于屏蔽放射性射线的屏蔽材料做进一步地详细阐述，以求更为清楚明了地理解其组成和作用，但不能以此来限制本发明的保护范围。
以下实施例采用中子捕获治疗的包含中子和伽马射线的放射源，从而以突出本发明的用于屏蔽放射性射线的屏蔽材料的以下实施例的屏蔽中子和伽马射线的效果。具体请参照图1，其显示出从中子捕获治疗的射束出口出来的放射源中的中子和伽马射线的能谱，考虑距射束出口4.5米外的中子和伽马射线强度，下图为射束打到正前方屏蔽墙前的能谱分布，大多数中子落在超热中子能区(0.5～10eV)，而伽马射线能量分布较均匀于0.1～10MeV范围。本发明的实施例仅以此放射源来举例，并不以此限制放射源的种类，本领域技术人员熟知的，根据本发明的实施例的教导和启示，本发明实施例中的用于屏蔽放射性射线的屏蔽材料也可用于其他包含中子和伽马射线的具有不同能谱的放射源。
以下实施例中的屏蔽材料由水、胶凝材料、细骨料、粗骨料和外加剂组成，其中细骨料由硼玻璃粉和重晶石砂组成，粗骨料由铅石和重晶石组成；硼玻璃粉中的硼元素含量占屏蔽材料总重量的0.5％～1％；重晶石砂和重晶石中的硫酸钡含量占屏蔽材料总重量的71％～75％；其他含量为水、胶凝材料和外加剂，所有成分的含量总和为屏蔽材料总重量的100％。
屏蔽材料选用的胶凝材料为P.II 52.5型硅酸盐水泥，外加剂为减水剂、早强剂、缓凝剂、泵送剂、膨胀剂中的一种或多种，第一种屏蔽材料的密度为3.46～3.55g/cm3，第二种屏 蔽材料的密度为3.73～4.01g/cm3。本领域技术人员熟知的，选用其他类型的胶凝材料也能实现；外加剂可根据具体的实施例来确定，作为优选地，实施例中的外加剂选用聚羧酸系减水剂。下面将以实施例具体的展开说明。
实施例一
请参照表一，屏蔽材料由水、胶凝材料、细骨料、粗骨料和外加剂组成。水的重量占屏蔽材料总重量的2.48％，胶凝材料选用P.II52.5型硅酸盐水泥，细骨料由硼玻璃粉和重晶石砂组成，粗骨料由重晶石组成，外加剂选用聚羧酸系减水剂，其中，硼元素的重量占屏蔽材料总重量的0.51％，硫酸钡含量占屏蔽材料总重量的75.33％，其他含量为胶凝材料和外加剂，所有成分的含量总和为屏蔽材料总重量的100％。
制备工艺主要包括：1.由重晶石矿石经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的重晶石砂；2.由重晶石矿石经破碎、筛分而得粒径不小于4.75mm的用于粗骨料的重晶石；3.将硼玻璃经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的硼玻璃粉；4.将水泥、粗骨料和细骨料投入容器内形成部分混合料；5.将水和外加剂容器内，与部分混合料一起预搅拌预设时间t，其中30s≤t≤60s；6.搅拌机搅拌出料。
在一些需要场外运输的场合，可以选择采用搅拌车或翻斗车两种运输工具，但需考虑适用的范围。屏蔽材料尽量以近似搅拌结束时的状态进行运输、浇筑至关重要。运输必须快捷，应控制从搅拌开始到运至现场的时间，根据现行国家标准《混凝土质量控制标准》GB 50164的规定，在外界气温低于25℃时，采用搅拌车运输，大于等于C30的混凝土不宜大于90min；超过25℃时，大于等于C30的混凝土不宜大于60min。现行国家标准《预拌混凝土》GB/T 14902中规定采用搅拌车运送的混凝土，宜在1.5h内卸料；采用翻斗车运送的混凝土，宜在1.0h内卸料；当最高气温低于25℃时，运送时间可延长0.5h。规定90min是考虑到时间越长混凝土的坍落度损失就会越大，不能保证混凝土的工作性。实际应用时，当性能不能满足要求时，可以再试验验证的基础上通过加入外加剂进行调整，不允许加水。通常采用掺加有缓凝效果的外加剂来延长混凝土凝结时间等技术措施。
屏蔽材料的强度等级为C30或C40，屏蔽材料的轴心抗压强度标准值应达到17.1～22.8N/mm2或者更高，屏蔽材料的轴心抗拉强度标准值应达到1.70～2.05N/mm2或者更高。
水泥品种选用P.II52.5型硅酸盐水泥，即熟料+石膏的含量大于等于水泥总重量的95％，粒化高炉矿渣的含量小于等于水泥总重量的5％或者石灰石的含量小于等于水泥总重量的5％。其中熟料主要含有CaO、SiO2、Al2O3、Fe2O3的原料，按适当比例磨成细粉烧至部分熔融所得以硅酸钙为主要矿物成分的水硬性胶凝物质。其中硅酸钙矿物不小于66％，氧化钙和氧化硅质量比不小于2.0。其中关于石膏的选用，如果选用天然石膏应符合GB/T 5483中规定的G类或M类二级(含)以上的石膏或混合石膏；如果选用工业副产石膏，需以硫酸钙为主要成分的工业副产物，采用前应经过试验证明对水泥性能无害。P.II52.5型硅酸盐水泥的化学指标中的不溶物(质量分数)应小于等于1.50％，烧失量(质量分数)应小于等于3.5％，三氧化硫(质量分数)应小于等于3.5％，氧化镁(质量分数)应小于等于6.0％，氯离子(质量分数) 应小于等于0.06％。硅酸盐的水泥等级为52.5，成型3天抗压强度大于等于23.0Mpa，抗折强度大于等于4.0MPa，成型28天抗压强度大于等于52.5MPa，抗折强度大于等于7.0Mpa。
按照此配比及制备方法制出的屏蔽材料，其中硼玻璃粉占细骨料重量的17％，重晶石砂占细骨料重量的83％。该屏蔽材料的容重(即密度)为3554kg/m3，砂率为32.1％。水胶比为0.37，外加剂掺量为1.80％。按需求总量500吨计算，所需的各种物质的重量如下表一所列。
表一：实施例一中的重量配比
Figure PCTCN2016086223-appb-000001
与实施例一中使用的相同材料、条件或方法的，请参照实施例一中的叙述，在实施例二～三中将不再赘述。
实施例二
请参照表二，屏蔽材料由水、胶凝材料、细骨料、粗骨料和外加剂组成。水的重量占屏蔽材料总重量的2.51％，胶凝材料选用P.II52.5型硅酸盐水泥，细骨料由硼玻璃粉和重晶石砂组成，粗骨料由重晶石组成，外加剂选用聚羧酸系减水剂，其中，硼元素的重量占屏蔽材料总重量的0.75％，硫酸钡含量占屏蔽材料总重量的73.07％，其他含量为胶凝材料和外加剂，所有成分的含量总和为屏蔽材料总重量的100％。
其制备方法与实施例一相同。按照此配比及制备方法制出的屏蔽材料，其中硼玻璃粉占细骨料重量的26％，重晶石砂占细骨料重量的74％。该屏蔽材料的容重(即密度)为3508kg/m3，砂率为31.0％。水胶比为0.37，外加剂掺量为1.80％。按需求总量500吨计算，所需的各种 物质的重量如下表三所列。
表二：实施例二中的重量配比
Figure PCTCN2016086223-appb-000002
实施例三
请参照表三，屏蔽材料由水、胶凝材料、细骨料、粗骨料和外加剂组成。水的重量占屏蔽材料总重量的2.55％，胶凝材料选用P.II52.5型硅酸盐水泥，细骨料由硼玻璃粉和重晶石砂组成，粗骨料由重晶石组成，外加剂选用聚羧酸系减水剂，其中，硼元素的重量占屏蔽材料总重量的1.00％，硫酸钡含量占屏蔽材料总重量的70.76％，其他含量为胶凝材料和外加剂，所有成分的含量总和为屏蔽材料总重量的100％。
其制备方法与实施例一相同。按照此配比及制备方法制出的屏蔽材料，其中硼玻璃粉占细骨料重量的36％，重晶石砂占细骨料重量的64％。该屏蔽材料的容重(即密度)为3457kg/m3，砂率为29.8％。水胶比为0.37，外加剂掺量为1.80％。按需求总量500吨计算，所需的各种物质的重量如下表三所列。
表三：实施例三中的重量配比
Figure PCTCN2016086223-appb-000003
下面引入两个市面上常用的用于屏蔽放射性射线的屏蔽材料与本发明实施例中的用于屏蔽放射性射线的屏蔽材料作比较。
对比例一
对比例一为市面上常用的一种辐射屏蔽材料，其含有的元素的重量百分比如下表四所列：
表四：对比例一中的元素及其含量
元素 H B O Al Si S Fe Ca Ba Na Pb Mg C K
含量 0.8％ - 47.3％ 3.6％ 14.5％ 0.3％ 1.1％ 24.7％ - - - 2.4％ 5.0％ 0.2％
对比例二
对比例二为另一种重晶石辐射屏蔽材料，其重量配比如下表五所列：
表五：对比例二中的物质及其重量配比
Figure PCTCN2016086223-appb-000004
以上各实施例及对比例中的屏蔽材料含有的元素及各元素所占屏蔽材料总重量的百分比请参照如下表六：
表六：实施例及对比例中的元素及其含量
Figure PCTCN2016086223-appb-000005
各个实施例及对比例中的屏蔽材料的防辐射性能指标请参照表七，由此可以看出，在同等厚度50cm的条件下，实施例一～五中的屏蔽材料不论是对中子屏蔽还是对光子屏蔽的性能都要远远好于对比例一和二。
表七：实施例及对比例的防辐射性能指标
Figure PCTCN2016086223-appb-000006
从屏蔽材料厚度及价格因素来考虑，尤其是中子捕获治疗的射源经各种屏蔽材料衰减至周围剂量当量率2.5μSv/h(作为一种建议当作参考)所需厚度，请见表八，对比例一中的屏蔽材料虽然价格非常便宜，但是需要非常厚的材料才能达到标准的要求；对比例二中的屏蔽材料虽然价格便宜但是需要的厚度也比较厚；含硼聚乙烯+铅砖的屏蔽材料虽然厚度非常薄就能达到标准的要求，但是其价格非常的昂贵。而实施例一～三中的屏蔽材料在达到标准的前提条件下，不仅厚度适中，而且价格也很便宜。
表八：屏蔽材料的厚度及价格
Figure PCTCN2016086223-appb-000007
下面请参见图2和图3，以评估各种屏蔽材料在不同厚度下的有效剂量表现。
由图2和图3可看出实施例中的屏蔽材料相较对比例不论在中子还是γ屏蔽上均有明显的优势，且伴随厚度增加其效果愈加显著。
10B对中子的捕获截面在能量低于500keV的范围内遵守1/v的特性，因此随着中子能量的降低，反应截面也随之增高，如0.025eV的中子具有约3866邦(barn)捕获截面，因此超热中子通过混凝土减速至慢中子后大量被10B元素所吸收，实施例一0.5％的硼含量即发挥良好的中子屏蔽效果，对比例一和二在中子屏蔽上并无显着差异，甚至对比例二中的普通重晶石混凝土屏蔽中子的效果更差，可见对于中子捕获治疗的混合辐射场，在混凝土中掺入至少0.5％的硼元素是十分必要的。
图3的两个对比例明显看出重晶石混凝土有较好的γ屏蔽效果，主要由于重晶石中的硫酸钡提升其混凝土的表观密度，亦即硫酸钡含量越高、表观密度越大、γ屏蔽效果越好。我司研制的混凝土在重晶石的基础下，变化三种不同硼的含量，凸显混凝土中添加至少0.5％的硼的必要，对比例二中的普通的重晶石混凝土虽较对比例一中的一般混凝土有明显改善，但实施例一加了0.5％的硼后可见其效果大幅改进。
将混凝土搅拌均匀后，由混凝土运输车运送到施工工地，参照如下的方法进行性能检测：GB/T50557-2010《重晶石抗辐射混凝土应用技术规范》、GB/T50081-2002《普通混凝土力学性能性能试验方法标准》，检测结果如表九所示：
表九：本发明各实施例中所述混凝土的性能参数
Figure PCTCN2016086223-appb-000008
以上所述仅为本发明的优选实施例，对本发明而言仅是说明性的，而非限制性的；本领域普通技术人员理解，在本发明权利要求所限定的精神和范围内可对其进行许多改变，修改， 甚至等效变更，但都将落入本发明的保护范围。

Claims (5)

  1. 一种用于屏蔽放射性射线的屏蔽材料，其特征在于：所述屏蔽材料由水、胶凝材料、细骨料、粗骨料和外加剂组成，其中细骨料由硼玻璃粉和重晶石砂组成，粗骨料由重晶石组成；硼玻璃粉中的硼元素含量占屏蔽材料总重量的0.5％～1％；重晶石砂和重晶石中的硫酸钡含量占屏蔽材料总重量的71％～75％；其他含量为水、胶凝材料和外加剂，所有成分的含量总和为屏蔽材料总重量的100％。
  2. 根据权利要求1所述的用于屏蔽放射性射线的屏蔽材料，其特征在于：胶凝材料为P.II52.5型硅酸盐水泥，外加剂为减水剂、早强剂、缓凝剂、泵送剂、膨胀剂中的一种或多种，所述屏蔽材料的密度为3.46～3.55g/cm3。
  3. 根据权利要求2所述的用于屏蔽放射性射线的屏蔽材料，其特征在于：外加剂为聚羧酸系减水剂。
  4. 根据权利要求1所述的用于屏蔽放射性射线的屏蔽材料，其特征在于所述屏蔽材料适用于中子捕获治疗的包含中子和伽马射线的辐射源。
  5. 一种如权利要求1所述的用于屏蔽放射性射线的屏蔽材料的制备方法，其特征在于：所述制备方法包括如下步骤：
    由重晶石矿石经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的重晶石砂；
    由重晶石矿石经破碎、筛分而得粒径不小于4.75mm的用于粗骨料的重晶石；
    将硼玻璃经破碎、筛分而得粒径小于4.75mm且不小于75μm的用于细骨料的硼玻璃粉；
    将水泥、粗骨料和细骨料投入容器内形成部分混合料；
    将水和外加剂容器内，与部分混合料一起预搅拌预设时间t，其中30s≤t≤60s；
    搅拌机搅拌出料。
PCT/CN2016/086223 2015-06-19 2016-06-17 用于屏蔽放射性射线的屏蔽材料及其制备方法 WO2016202291A1 (zh)

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