CN115611513B - Radiation-resistant glass material and preparation method and application thereof - Google Patents
Radiation-resistant glass material and preparation method and application thereof Download PDFInfo
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- 239000011521 glass Substances 0.000 title claims abstract description 138
- 230000005855 radiation Effects 0.000 title claims abstract description 109
- 239000000463 material Substances 0.000 title claims abstract description 98
- 238000002360 preparation method Methods 0.000 title claims abstract description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 60
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 claims abstract description 54
- 238000006243 chemical reaction Methods 0.000 claims abstract description 42
- 238000012986 modification Methods 0.000 claims abstract description 31
- 230000004048 modification Effects 0.000 claims abstract description 31
- 239000000377 silicon dioxide Substances 0.000 claims abstract description 30
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 claims abstract description 29
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims abstract description 29
- 239000000292 calcium oxide Substances 0.000 claims abstract description 29
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims abstract description 29
- 239000000395 magnesium oxide Substances 0.000 claims abstract description 29
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims abstract description 29
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims abstract description 27
- 229910001887 tin oxide Inorganic materials 0.000 claims abstract description 27
- 235000012239 silicon dioxide Nutrition 0.000 claims abstract description 25
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims abstract description 24
- 229910001928 zirconium oxide Inorganic materials 0.000 claims abstract description 24
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims abstract description 21
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 9
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 9
- 239000001301 oxygen Substances 0.000 claims abstract description 9
- 229910001938 gadolinium oxide Inorganic materials 0.000 claims description 25
- 229940075613 gadolinium oxide Drugs 0.000 claims description 25
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 claims description 25
- 239000003365 glass fiber Substances 0.000 claims description 22
- CXKCTMHTOKXKQT-UHFFFAOYSA-N cadmium oxide Inorganic materials [Cd]=O CXKCTMHTOKXKQT-UHFFFAOYSA-N 0.000 claims description 20
- CFEAAQFZALKQPA-UHFFFAOYSA-N cadmium(2+);oxygen(2-) Chemical compound [O-2].[Cd+2] CFEAAQFZALKQPA-UHFFFAOYSA-N 0.000 claims description 20
- 238000002844 melting Methods 0.000 claims description 17
- 230000008018 melting Effects 0.000 claims description 17
- 238000000034 method Methods 0.000 claims description 15
- 230000004927 fusion Effects 0.000 claims description 5
- 239000011810 insulating material Substances 0.000 claims description 4
- 230000007797 corrosion Effects 0.000 abstract description 5
- 238000005260 corrosion Methods 0.000 abstract description 5
- 150000001875 compounds Chemical class 0.000 abstract description 4
- 239000002245 particle Substances 0.000 description 16
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 10
- 238000012360 testing method Methods 0.000 description 8
- 238000010521 absorption reaction Methods 0.000 description 7
- 238000002474 experimental method Methods 0.000 description 7
- 230000008569 process Effects 0.000 description 7
- 239000011449 brick Substances 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- 238000002425 crystallisation Methods 0.000 description 5
- 230000008025 crystallization Effects 0.000 description 5
- 239000012535 impurity Substances 0.000 description 5
- 238000013461 design Methods 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- 230000008859 change Effects 0.000 description 3
- 239000011819 refractory material Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 2
- 229910052810 boron oxide Inorganic materials 0.000 description 2
- QXJJQWWVWRCVQT-UHFFFAOYSA-K calcium;sodium;phosphate Chemical compound [Na+].[Ca+2].[O-]P([O-])([O-])=O QXJJQWWVWRCVQT-UHFFFAOYSA-K 0.000 description 2
- 230000001276 controlling effect Effects 0.000 description 2
- 229910052593 corundum Inorganic materials 0.000 description 2
- 239000010431 corundum Substances 0.000 description 2
- JKWMSGQKBLHBQQ-UHFFFAOYSA-N diboron trioxide Chemical compound O=BOB=O JKWMSGQKBLHBQQ-UHFFFAOYSA-N 0.000 description 2
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 description 2
- 230000005251 gamma ray Effects 0.000 description 2
- 238000009413 insulation Methods 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 239000011777 magnesium Substances 0.000 description 2
- 239000005304 optical glass Substances 0.000 description 2
- 230000000737 periodic effect Effects 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 238000010298 pulverizing process Methods 0.000 description 2
- 239000011208 reinforced composite material Substances 0.000 description 2
- 238000005491 wire drawing Methods 0.000 description 2
- 229910052726 zirconium Inorganic materials 0.000 description 2
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- KKCBUQHMOMHUOY-UHFFFAOYSA-N Na2O Inorganic materials [O-2].[Na+].[Na+] KKCBUQHMOMHUOY-UHFFFAOYSA-N 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 239000008395 clarifying agent Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
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- 239000000446 fuel Substances 0.000 description 1
- 239000000156 glass melt Substances 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
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- 238000000465 moulding Methods 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- 238000005191 phase separation Methods 0.000 description 1
- 238000002601 radiography Methods 0.000 description 1
- 238000001959 radiotherapy Methods 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
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- 238000006467 substitution reaction Methods 0.000 description 1
- 238000000584 ultraviolet--visible--near infrared spectrum Methods 0.000 description 1
Abstract
The invention provides a radiation-resistant glass material, a preparation method and application thereof, and relates to the technical field of glass, wherein the radiation-resistant glass material comprises the following components in percentage by mole: 58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide and 0.1 to 0.7 percent of network modification body; wherein the network modification body is at least one compound formed by combining an element with a neutron capture reaction cross section not smaller than 100b and an oxygen element. The radiation-resistant glass material provided by the invention has excellent high-dose radiation resistance, excellent mechanical property and corrosion resistance.
Description
Technical Field
The invention relates to the technical field of glass, in particular to a radiation-resistant glass material and a preparation method and application thereof.
Background
With the continuous development of science and technology, the application range of the optical glass material and the glass fiber reinforced composite material is expanded, and the optical glass material and the glass fiber reinforced composite material are widely applied to medical equipment such as chest radiography, irradiation sterilization, radiotherapy equipment and the like, high-energy large devices such as fusion stacks and fission stacks and the like, and the fields such as aerospace, ships, new energy sources, electronic communication and the like. However, the internal structure of the common glass and the composite material thereof can be changed in the irradiation environment, and electronic defects and impurity atoms are generated, so that the performance and the service life of the common glass are influenced. The existing radiation-resistant glass material has radiation resistance, but the radiation resistance is still poor under high-dose radiation, and the mechanical property and the temperature resistance of the existing radiation-resistant glass material are also lost. Therefore, it is necessary to develop a radiation-resistant glass material with high-dose radiation intensity, which meets the requirements of shielding, insulation, heat insulation and other mechanical and thermal stability under the high-energy radiation environment.
Disclosure of Invention
The embodiment of the invention provides a radiation-resistant glass material, a preparation method and application thereof, and the radiation-resistant glass material has excellent high-dose radiation resistance, excellent mechanical properties and good corrosion resistance and temperature resistance.
In a first aspect, the invention provides a radiation resistant glass material comprising the following components in mole percent: 58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide and 0.1 to 0.7 percent of network modification body; wherein the network modification body is at least one compound formed by combining an element with a neutron capture reaction cross section not smaller than 100b and an oxygen element.
Preferably, the network modification comprises at least one of boron oxide, cadmium oxide, gadolinium oxide.
Preferably, the network modifying body consists of cadmium oxide and gadolinium oxide.
More preferably, the molar ratio of cadmium oxide to gadolinium oxide in the network modification is not greater than 1:1.
More preferably, the molar ratio of cadmium oxide to gadolinium oxide in the network modification is 1:1.
Preferably, the radiation resistant glass material comprises the following components in mole percent: 58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide, 0 to 0.7 percent of cadmium oxide and 0.1 to 0.6 percent of gadolinium oxide.
Preferably, the radiation resistant glass material comprises the following components in mole percent: 60-65% of silicon dioxide, 5-7% of aluminum oxide, 14-16% of calcium oxide, 10-15% of magnesium oxide, 0.8-1.0% of barium oxide, 0.3-0.5% of tin oxide, 0.5-1.0% of zirconium oxide and 0.2-0.5% of network modification body.
Preferably, the radiation resistant glass material comprises the following components in mole percent: 65.6% of silicon dioxide, 4.8% of aluminum oxide, 15.4% of calcium oxide, 12.3% of magnesium oxide, 0.8% of barium oxide, 0.2% of tin oxide, 0.5% of zirconium oxide and 0.34% of gadolinium oxide.
Preferably, the radiation-resistant glass material has a comprehensive neutron capture reaction cross section of 10-180 b.
In a second aspect, the present invention also provides a method for preparing the radiation resistant glass material based on the first aspect, the preparation method comprising the following steps:
58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide and 0.1 to 0.7 percent of network modification are evenly mixed, and the radiation-resistant glass material is obtained through melting and forming.
Preferably, the radiation resistant glass material is glass fiber.
More preferably, the glass fibers have a diameter of 8 to 22. Mu.m.
The melting temperature is 1500-1600 ℃.
In a third aspect, the invention provides an application of a radiation-resistant glass material, which is applied to the field of radiation-resistant materials.
Preferably, the radiation resistant glass material is used as an insulating material for a magnetic field coil of a thermonuclear fusion reactor.
Compared with the prior art, the invention has at least the following beneficial effects:
According to the invention, on the basis of the neutron capture reaction cross section of the element, the oxide with the high neutron capture reaction cross section is added into the radiation-resistant glass material, so that the deceleration and absorption of irradiation particles can be effectively realized, the intrinsic structure of the glass is protected, the radiation-resistant performance of the glass material is improved, and the high-dose radiation resistance of the glass is realized; meanwhile, the oxide with the high neutron capture reaction cross section is used as a network modification body, so that the prepared radiation-resistant glass material has excellent mechanical property, good environmental corrosion resistance and temperature resistance, and good technological property.
The radiation-resistant glass material, such as glass fiber, prepared by the invention has no obvious phenomena of embrittlement, shrinkage, pulverization and heat conductivity coefficient increase after being irradiated by gamma rays with the irradiation dose of 1.02X10 7 Gy, and the prepared glass fiber still has good mechanical properties. The radiation-resistant glass material prepared by the invention can resist high-dose accumulated radiation for a long time in space environment, and can meet the requirement of service life of the radiation-resistant glass material more than 10 years.
Drawings
Fig. 1 is a graph showing absorption decay rates of the radiation resistant glass materials provided in examples 1 to 3 of the present invention before and after irradiation.
Detailed Description
For the purpose of making the objects, technical solutions and advantages of the embodiments of the present invention more apparent, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention and the accompanying drawings, and it is apparent that the described embodiments are some embodiments of the present invention, but not all embodiments, and all other embodiments obtained by those skilled in the art without making any inventive effort based on the embodiments of the present invention are within the scope of protection of the present invention.
The embodiment of the invention provides a radiation-resistant glass material, which comprises the following components in percentage by mole: silica 58-67% (e.g., may be 58%, 58.5%, 59%, 60%, 60.5%, 61%, 62%, 63%, 65%, 66%, or 67%), alumina 4-8% (e.g., may be 4%, 4.5%, 5%, 5.5%, 6%, 6.5%, 7%, 7.5%, or 8%), calcium oxide 12-18% (e.g., may be 12%, 12.5%, 13%, 13.5%, 14%, 15%, 16%, 16.5%, 17%, 17.5%, or 18%), magnesium oxide 7-18% (e.g., may be 7%, 7.5%, 8%, 8.5%, 9%, 9.5%, 10%, 10.5%, 11%, 11.5%, 12%, 12.5%, 13%, 13.5%, 14%, 15%, 16%, 16.5%, 17%, 17.5%, or 18%), barium oxide 0.5-1.2% (e.g., may be 0.5%, 0.55%, 0.6%, 0.65%, 0.7%, 0.75%, 0.8%, 0.9%, 1.0%, 1.05%, 1.1%, 1.15%, or 1.2%), tin oxide 0.1-0.8% (e.g., may be 0.1%, 0.15%, 0.2%, 0.25%, 0.3%, 0.4%, 0.5%, 0.55%, 0.6%, 0.65%, 0.7%, 0.75%, or 0.8%), zirconium oxide 0.5-1.2% (e.g., may be 0.5%, 0.6%, 0.7%, 0.8%, 0.9%, 1.0%, 1.05%, 1.1%, 1.15%, or 1.2%), network modifications 0.1-0.7% (e.g., may be 0.1%, 0.15%, 0.2%, 0.3%, 0.4%, 0.5%, 0.55%, or 0.65% >, or 0.0.7%). Wherein the network modification body is at least one compound formed by combining an element with a neutron capture reaction cross section not smaller than 100b and an oxygen element.
It should be noted that, a person skilled in the art may directly obtain an element having a neutron capture reaction cross section of not less than 100b, for example, the element may be a Cd element having a neutron capture reaction cross section of 2450b or a Gd element having a neutron capture reaction cross section of 49000 b. The network modification is at least one oxide meeting the above conditions.
Specifically, in the present invention, the radiation resistant glass material further includes unavoidable impurities, and the mole percentage of the impurities in the radiation resistant glass material is less than 0.5%. The impurities include Fe 2O3、Na2O、K2 O and the like.
In the invention, the silicon dioxide is a network forming body of a glass structure and provides a foundation for the mechanical property, chemical stability and irradiation performance of the glass material. However, the content of the silicon dioxide needs to be regulated and controlled according to the performance design, when the content of the silicon dioxide is too low, the glass network forming bodies are fewer, and the irradiation resistance and the mechanical property of the glass network forming bodies are reduced; however, if the content of silicon dioxide is too high, the viscosity of the glass is too high, the melting is difficult, and meanwhile, the glass melt is easy to crystallize, which is unfavorable for the subsequent glass fiber forming. The present invention therefore selects a silica content of 58 to 67 mole percent.
In the invention, alumina exists in a glass structure as a network forming body, and enters the glass network structure as [ AlO 4 ] tetrahedron, so that densification of the glass network structure can be enhanced, the phase separation tendency of glass is reduced, crystal nucleus formation is inhibited to improve the forming process performance of subsequent glass fibers, and meanwhile, the mechanical strength, modulus and chemical corrosion resistance of the glass fibers are improved, but a large amount of network exosomes appear when the introducing amount is too high, so that the glass melting temperature is too high and the crystallization tendency is enhanced. The present invention therefore selects an alumina content of 4 to 8 mole percent.
In the invention, calcium oxide and magnesium oxide belong to the outer body of the glass network structure, and free oxygen is mainly provided in the glass component to promote the intermediate to form a tetrahedral structure so as to enhance the network density of the glass material; meanwhile, the high-temperature viscosity of the glass is reduced, and the crystallization tendency is improved, so that the mechanical property and the forming technological property of the glass material are improved. Therefore, the invention selects the content of calcium oxide to be 12-18 mol percent and the content of magnesium oxide to be 7-18 mol percent.
The neutron capture reaction cross section of Si element is 0.171b, which is known to those skilled in the art; the neutron capture reaction section of Al element is 0.232b; the neutron capture reaction section of Mg element is 0.063b; the neutron capture reaction section of Ca element is 0.43b; the neutron capture reaction section of the Ba element is 1.3b; the neutron capture reaction section of Sn element is 0.626b; the neutron capture reaction cross section of Zr element is 0.184b.
In the invention, the non-oxygen elements in the silicon dioxide, the aluminum oxide, the calcium oxide and the magnesium oxide all have smaller neutron capture reaction cross sections, and in the irradiation process, the collision probability of irradiation rays or photons can be effectively reduced due to the small atomic radius, the irradiation resistance is improved, and the damage of a glass structure is reduced. The calcium oxide and the magnesium oxide belong to alkaline earth metal oxides, ca and Mg belong to light elements in the periodic table, and have radiation resistance; meanwhile, the introduction of calcium oxide and magnesium oxide can further improve the chemical stability and irradiation resistance of the glass material.
In the invention, barium oxide belongs to an outer body of a glass network structure in a glass structure, free oxygen can be provided, glass melting is promoted, glass fiber drawing is improved, meanwhile, the radius of Ba 2+ ions is large, the neutron capture reaction section of Ba is 1.3b, and is a heavy metal element with the largest neutron capture reaction section in alkaline earth metal elements, so that the barium oxide has better deceleration effect and higher ray capture capability on irradiated ions, and the kinetic energy of rays can be effectively reduced through collision with high-energy particles or photons, thereby reducing the probability of damaging the glass structure and further improving irradiation resistance. The content of the barium oxide is 0.5-1.2 mol percent.
In the invention, tin oxide belongs to a network modification body in a glass structure, has bond energy of 192.6kJ/mol, can ensure that glass liquid has better clarifying effect above 1560 ℃, and can be used as a clarifying agent in glass melting. Meanwhile, the tin oxide has the characteristics of better conductivity and reflection of infrared radiation, and is beneficial to protecting the body structure of the glass material and improving the temperature resistance of the glass material in the irradiation process. Therefore, the tin oxide content selected in the invention is 0.1-0.5 mol percent.
In the invention, zirconia belongs to the outer body of the glass network structure in the glass structure, so that the high-temperature viscosity of the glass can be increased, the thermal expansion coefficient is reduced, and the alkali resistance of the glass material is obviously improved. The Zr 4+ has large ionic radius, can also slow down the radiation particles, namely slow down the particles, and reduce the irradiation damage of the glass material body structure. Therefore, in order to ensure that the zirconia fully exerts its effect, the zirconia content selected in the present invention is 0.5 to 1.2 mole percent.
The invention adopts at least one compound formed by combining elements with neutron capture reaction cross sections not smaller than 100b and oxygen elements as network modification bodies, and fills the network modification bodies in gaps of a glass network structure, and in the irradiation process, the probability of collision with irradiation particles is higher, namely the probability of nuclear reaction is higher, and the reactivity is higher, so that the network modification bodies can realize the speed reduction and absorption of the irradiation particles, reduce or even avoid the damage of the irradiation particles to the glass network structure, and further obviously improve the irradiation resistance of the radiation resistant glass material. Experiments prove that when the content of the network change body is 0.1-0.7 mol percent, the comprehensive neutron capture reaction cross section of the prepared radiation-resistant glass material is 10-180 b, namely the radiation-resistant glass material has excellent radiation resistance, and experiments prove that the larger the comprehensive neutron capture reaction cross section is, the more excellent the radiation resistance is.
In the invention, because the elements contained in the network modification body have high neutron capture reaction cross sections, the specific design of the irradiation resistance of the radiation-resistant glass material can be realized according to the actual use requirement by selecting oxides formed by elements with different high neutron capture reaction cross sections and controlling the mole percentage of the oxides and consuming irradiation particles by virtue of the collision and absorption of the oxides to the irradiation particles.
According to some preferred embodiments, the network modifying body comprises at least one of boron oxide, cadmium oxide, gadolinium oxide.
At least one kind is a mixture of any one or any plurality of kinds mixed in any proportion.
According to some preferred embodiments, the network modifying body consists of cadmium oxide and gadolinium oxide.
According to some preferred embodiments, the molar ratio of cadmium oxide to gadolinium oxide in the network modification is not greater than 1:1 (e.g., may be 1:1, 0.9:1, 0.8:1, 0.7:1, or 0.6:1, etc.).
According to some more preferred embodiments, the molar ratio of cadmium oxide to gadolinium oxide in the network modification is 1:1.
According to some preferred embodiments, the radiation resistant glass material comprises the following components in mole percent: 58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide, 0 to 0.7 percent of cadmium oxide and 0.1 to 0.6 percent of gadolinium oxide.
The mole percentage of cadmium oxide may be 0 to 0.7%, for example, 0%,0.05%, 0.1%, 0.15%, 0.2%, 0.25%, 0.3%, 0.35%, 0.4%, 0.45%, 0.5%, 0.55%, 0.6%, 0.65% or 0.7%.
The mole percentage of gadolinium oxide may be 0.1 to 0.6%, for example, 0.1%, 0.15%, 0.2%, 0.25%, 0.3%, 0.35%, 0.4%, 0.45%, 0.5%, 0.55% or 0.6%.
In the invention, cadmium oxide is used as a network modification body in a glass structure, is filled in gaps of the network structure, has single bond energy of 83.7kJ/mol, and can remarkably increase the density of the glass material. Meanwhile, the neutron capture reaction section of Cd is 2450b, the probability of collision with irradiation particles is extremely high in the irradiation process, and the effect of decelerating or absorbing the irradiation particles is achieved, so that the network structure of the glass is protected, and the damage to the glass structure after collision is small due to the fact that the network structure belongs to a network change body. Experiments prove that the cadmium oxide content selected by the invention is 0-0.7 mol percent.
In the invention, gadolinium oxide is taken as a network modification body in a glass structure, 1 electron is arranged on 7 electron orbits of Gd, and the Gd is the unpaired electron with the largest number in rare earth elements, and in the periodic table of elements, gd has the highest neutron capture reaction section 49000b, and the probability of collision with particles during irradiation is highest, so that the particle has the most obvious decelerating and absorbing effects, and the glass network structure can be excellently protected. Experiments prove that the gadolinium oxide content selected by the invention is 0.1-0.6 mol percent.
According to some preferred embodiments, the radiation resistant glass material comprises the following components in mole percent: 60-65% (e.g., may be 60%, 60.5%, 61%, 61.5%, 62%, 62.5%, 63%, 63.5%, 64%, 64.5%, or 65%), 5-7% (e.g., may be 5%, 5.5%, 6%, 6.5%, or 7%), 14-16% (e.g., may be 14%, 14.5%, 15%, 15.5%, or 16%), 10-15% (e.g., may be 10%, 10.5%, 11%, 11.5%, 12%, 12.5%, 13%, 13.5%, 14%, 14.5%, or 15%) of silica, 10-15% (e.g., may be 10%, 10.5%, 11%, 11.5%, 12.5%, 13.5%, or 15%), barium oxide 0.8-1.0% (e.g., may be 0.8%, 0.85%, 0.9%, 0.95%, or 1.0%), tin oxide 0.3-0.5% (e.g., may be 0.3%, 0.35%, 0.4%, 0.45%, or 0.5%), zirconium oxide 0.5-1.0% (e.g., may be 0.5%, 0.55%, 0.6%, 0.65%, 0.7%, 0.75%, 0.79%, 0.85%, 0.9%, 0.95%, or 0.99%), network modification 0.2-0.5% (e.g., may be 0.21%, 0.25%, 0.29%, 0.35%, 0.4%, 0.45%, or 0.5%).
According to some more preferred embodiments, the radiation resistant glass material comprises the following components in mole percent: 65.6% of silicon dioxide, 4.8% of aluminum oxide, 15.4% of calcium oxide, 12.3% of magnesium oxide, 0.8% of barium oxide, 0.2% of tin oxide, 0.5% of zirconium oxide and 0.34% of gadolinium oxide.
According to some preferred embodiments, the radiation resistant glass material has a combined neutron capture reaction cross section of 10 to 180b.
In the invention, the characteristic of additivity of glass property is utilized, and the comprehensive neutron capture reaction section is calculated by the following formula:
Wherein F is used for representing the comprehensive neutron capture reaction section; k is used for representing each component in the radiation-resistant glass material, and n is used for representing the total number of component types in the radiation-resistant glass material; a k is used to characterize the mole percent of the kth component; omega k is used to characterize the neutron capture reaction cross section of the non-oxygen element in the kth component. Experiments prove that the radiation-resistant glass material has a comprehensive neutron capture reaction section calculated according to the formula, and a conclusion that the larger the comprehensive neutron capture reaction section is, the more excellent the radiation-resistant performance is. Therefore, the radiation-resistant glass material based on the elemental neutron capture reaction cross-section design provided by the invention has more excellent radiation resistance.
The invention also provides a preparation method of the radiation-resistant glass material, which comprises the following steps:
58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide and 0.1 to 0.7 percent of network change body by mole percent are evenly mixed, and the radiation-resistant glass material is obtained through melting and forming.
According to some preferred embodiments, the radiation resistant glass material is glass fiber.
Specifically, in the invention, kiln melting can be performed by adopting a mode of oxy-fuel combustion, electric melting or thermal power combination, so that homogeneous glass is formed. The kiln used for melting glass can be made of refractory materials with high temperature resistance and glass liquid corrosion resistance, such as electric melting high-zirconium bricks, compact zirconium bricks, electric melting mullite bricks and the like. The glass fiber can also be produced by adopting a platinum furnace with a refractory material compact zirconia brick, corundum brick, electro-fused chromium zirconia corundum brick and mullite structure to perform two-step wire drawing, namely, glass is firstly melted according to the components and the mole percentages thereof, and then the glass is drawn. The kiln passage with the refractory material structure can also be used for one-step wire drawing to produce glass fiber.
According to some more preferred embodiments, the glass fibers have a diameter of 8 to 22 μm (e.g., may be 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 14 μm, 15 μm, 16 μm, 18 μm, 20 μm, or 22 μm).
According to some preferred embodiments, the temperature of the melting is 1500-1600 ℃ (e.g., may be 1500 ℃, 1520 ℃, 1550 ℃, 1580 ℃, 1590 ℃, or 1600 ℃).
The invention also provides application of the radiation-resistant glass material, which is applied to the field of radiation-resistant materials.
According to some preferred embodiments, a radiation resistant glass material is used as an insulating material for the magnetic field coils of a thermonuclear fusion reactor.
In order to more clearly illustrate the technical scheme and advantages of the invention, a radiation-resistant glass material, a preparation method and application thereof are described in detail through a plurality of embodiments.
The particle size of each component raw material used in the following examples is less than 200 mesh, and unavoidable impurities are present in the finally produced radiation resistant glass material.
Example 1
The radiation resistant glass material comprises the following components in mole percent: 65.54% of silicon dioxide, 4.83% of aluminum oxide, 15.38% of calcium oxide, 12.31% of magnesium oxide, 0.8% of barium oxide, 0.2% of tin oxide, 0.5% of zirconium oxide and 0.34% of gadolinium oxide. The components are accurately weighed according to the proportion, the weighed components are evenly mixed to obtain a batch, the batch is pneumatically mixed and conveyed to a kiln feed inlet, an automatic feeder is adopted for feeding, a clear and homogenized glass liquid is obtained by melting in a full electric melting or kiln at 1600 ℃, the glass liquid is prepared into glass spheres, the melted glass spheres are remelted in a platinum furnace at 1550 ℃, and the continuous glass fiber with the diameter of 8-22 mu m is obtained by adopting more than 400 bushing plates and controlling the glass fiber forming process parameters, namely the radiation resistant glass material.
Example 2
Example 2 is substantially the same as example 1 except that:
The radiation resistant glass material comprises the following components in mole percent: silica 65.60%, alumina 4.82%, calcium oxide 15.38%, magnesium oxide 12.30%, barium oxide 0.8%, tin oxide 0.2%, zirconium oxide 0.5%, cadmium oxide 0.23% and gadolinium oxide 0.17%.
Example 3
Example 3 is substantially the same as example 1 except that:
the radiation resistant glass material comprises the following components in mole percent: 65.56% of silicon dioxide, 4.82% of aluminum oxide, 15.37% of calcium oxide, 12.29% of magnesium oxide, 0.8% of barium oxide, 0.2% of tin oxide, 0.5% of zirconium oxide and 0.45% of cadmium oxide.
Example 4
Example 4 is substantially the same as example 1 except that:
The radiation resistant glass material comprises the following components in mole percent: silica 64.99%, alumina 4.78%, calcium oxide 13.06%, magnesium oxide 15.23%, barium oxide 0.79%, tin oxide 0.2%, zirconium oxide 0.49% and cadmium oxide 0.45%.
Example 5
Example 5 is substantially the same as example 1 except that:
58% of silicon dioxide, 8% of aluminum oxide, 18% of calcium oxide, 12% of magnesium oxide, 1.2% of barium oxide, 0.8% of tin oxide, 1.2% of zirconium oxide and 0.34% of gadolinium oxide.
Example 6
Example 6 is substantially the same as example 1 except that:
65.54% of silicon dioxide, 4.83% of aluminum oxide, 15.38% of calcium oxide, 12.31% of magnesium oxide, 0.8% of barium oxide, 0.2% of tin oxide, 0.5% of zirconium oxide and 0.1% of gadolinium oxide.
Example 7
Example 7 is substantially the same as example 1 except that:
67% of silicon dioxide, 4% of aluminum oxide, 12% of calcium oxide, 15% of magnesium oxide, 0.5% of barium oxide, 0.1% of tin oxide, 0.9% of zirconium oxide and 0.34% of gadolinium oxide.
Comparative example 1
Comparative example 1 is substantially the same as example 1 except that:
The radiation resistant glass material comprises the following components in mole percent: 63.89% of silicon dioxide, 4.70% of aluminum oxide, 14.97% of calcium oxide, 14.97% of magnesium oxide, 0.78% of barium oxide, 0.2% of tin oxide and 0.49% of zirconium oxide.
Comparative example 2
Comparative example 2 is substantially the same as example 1 except that:
The radiation resistant glass material comprises the following components in mole percent: 63.35% of silicon dioxide, 4.66% of aluminum oxide, 12.73% of calcium oxide, 17.82% of magnesium oxide, 0.77% of barium oxide, 0.2% of tin oxide and 0.48% of zirconium oxide.
The prepared radiation resistant glass materials prepared in examples 1 to 4 and comparative examples 1 and 2 were subjected to mechanical property test, gamma-ray irradiation test, crystallization upper limit temperature and high temperature viscosity measurement as samples, and comprehensive neutron capture reaction cross sections of the samples were calculated according to the foregoing formulas, and the test results are shown in table 1. The test conditions of the gamma-ray irradiation test are as follows: the activity of the cobalt source is about 9 ten thousand curies, the dose rate is 11034Gy/h, and the total irradiation dose is 1.02X10 7 Gy; testing the crystallization upper limit temperature of glass by adopting a gradient crystallization temperature test furnace; high temperature viscosity was measured using a BROOKFIELD high temperature viscometer in the United states. The elastic modulus of the material is calculated by adopting a dynamic method and measuring the propagation speed of ultrasonic waves or sound waves in a sample.
TABLE 1
For the samples, UV-VIS-NIR spectrum tests are respectively carried out before and after irradiation, absorption attenuation changes before and after irradiation are compared, and absorption attenuation rate curves obtained through calculation are shown in a graph in fig. 1 (wherein the curves correspond to the example 1, the example 2 and the example 3 from bottom to top in sequence); wherein, the measuring wavelength range is 300-1300 nm; the abscissa of fig. 1 represents wavelength (unit nm), and the ordinate represents absorption decay rate.
As can be seen from FIG. 1, the radiation-resistant glass material prepared in example 1 has the best radiation resistance, and is consistent with the design concept of the invention, namely, the network structure of the glass can be better protected by introducing oxide with a high neutron capture reaction section to slow down or absorb radiation particles, and meanwhile, the combination of the table 1 and FIG. 1 further proves that the radiation-resistant glass material obtained by the method of the invention has the better comprehensive neutron capture reaction section and the better radiation resistance.
Meanwhile, experiments prove that after the radiation-resistant glass materials prepared in the embodiments 1 to 7 are irradiated by gamma rays with the irradiation dose of 1.02X10 7 Gy, the glass fibers are free from obvious phenomena of embrittlement, shrinkage, pulverization and heat conductivity increase, and the prepared glass fibers still have good mechanical properties. The radiation-resistant glass material prepared by the invention can resist high-dose accumulated radiation for a long time in space environment, and can meet the requirement of service life of the radiation-resistant glass material more than 10 years.
As can be seen from Table 1, the radiation resistant glass material prepared in the examples of the present invention is resistant to high dose irradiation and has high strength and high modulus. Meanwhile, according to the forming temperature, the invention improves the fiber forming process performance, reduces the production difficulty and is more suitable for industrial continuous production. It can be seen from examples 3 and 4 that the difference in molding temperature is large due to the variation in the contents of calcium oxide and magnesium oxide. Further, experiments prove that the radiation-resistant glass material prepared by the invention can be applied to an environment of 800-900 ℃ (for example, the temperature can be 800 ℃, 820 ℃, 850 ℃, 880 ℃ or 900 ℃), and has excellent temperature resistance; and the tensile strength of the glass fiber is about 3000MPa. Therefore, the radiation-resistant glass fiber prepared according to the proportion of the components and the dosage thereof not only has excellent high-dose radiation resistance, but also has excellent mechanical property and temperature resistance, and can be used as an insulating material of a magnetic field coil of a thermonuclear fusion reactor, and also can be used in the fields of aerospace, deep space exploration and the like which relate to particle radiation.
Finally, it should be noted that: the above embodiments are only for illustrating the technical solution of the present invention, and are not limiting; although the invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some technical features thereof can be replaced by equivalents; such modifications and substitutions do not depart from the spirit and scope of the technical solutions of the embodiments of the present invention. The invention is not described in detail in a manner known to those skilled in the art.
Claims (12)
1. A radiation resistant glass material, characterized in that it comprises the following components in mole percent: 58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide and 0.1 to 0.7 percent of network modification body; wherein the network modification comprises 0-0.7% of cadmium oxide and 0.1-0.6% of gadolinium oxide; the comprehensive neutron capture reaction cross section of the radiation-resistant glass material is 10-180 b;
the comprehensive neutron capture reaction section is calculated by the following formula:
Wherein F is used for representing the comprehensive neutron capture reaction section; k is used for representing each component in the radiation-resistant glass material, and n is used for representing the total number of component types in the radiation-resistant glass material; a k is used to characterize the mole percent of the kth component; omega k is used to characterize the neutron capture reaction cross section of the non-oxygen element in the kth component.
2. The radiation resistant glass material according to claim 1, wherein,
The network modification consists of cadmium oxide and gadolinium oxide.
3. The radiation resistant glass material according to claim 2, wherein,
The molar ratio of cadmium oxide to gadolinium oxide in the network modification is not greater than 1:1.
4. The radiation resistant glass material according to claim 2, wherein,
The molar ratio of cadmium oxide to gadolinium oxide in the network modification is 1:1.
5. The radiation resistant glass material according to claim 1, wherein,
The radiation-resistant glass material comprises the following components in mole percent: 60-65% of silicon dioxide, 5-7% of aluminum oxide, 14-16% of calcium oxide, 10-15% of magnesium oxide, 0.8-1.0% of barium oxide, 0.3-0.5% of tin oxide, 0.5-1.0% of zirconium oxide and 0.2-0.5% of network modification body.
6. The radiation resistant glass material according to any of claims 1 to 5, wherein,
The radiation-resistant glass material comprises the following components in mole percent: 65.6% of silicon dioxide, 4.8% of aluminum oxide, 15.4% of calcium oxide, 12.3% of magnesium oxide, 0.8% of barium oxide, 0.2% of tin oxide, 0.5% of zirconium oxide and 0.34% of gadolinium oxide.
7. The method of producing a radiation resistant glass material according to any one of claims 1 to 6, characterized in that the method of producing comprises the steps of:
58 to 67 percent of silicon dioxide, 4 to 8 percent of aluminum oxide, 12 to 18 percent of calcium oxide, 7 to 18 percent of magnesium oxide, 0.5 to 1.2 percent of barium oxide, 0.1 to 0.8 percent of tin oxide, 0.5 to 1.2 percent of zirconium oxide and 0.1 to 0.7 percent of network modification are evenly mixed, and the radiation-resistant glass material is obtained through melting and forming.
8. The method according to claim 7, wherein,
The radiation-resistant glass material is glass fiber.
9. The method according to claim 7, wherein,
The diameter of the glass fiber is 8-22 mu m.
10. The method according to claim 7, wherein,
The melting temperature is 1500-1600 ℃.
11. Use of a radiation resistant glass material according to any one of claims 1 to 6 or a radiation resistant glass material prepared according to the preparation method of any one of claims 7 to 10, characterized in that the radiation resistant glass material is used in the field of radiation resistant materials.
12. The use according to claim 11, characterized in that the radiation resistant glass material is used as an insulating material for the magnetic field coils of thermonuclear fusion reactors.
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