CN115611513A - 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 135
- 230000005855 radiation Effects 0.000 title claims abstract description 96
- 239000000463 material Substances 0.000 title claims abstract description 95
- 238000002360 preparation method Methods 0.000 title abstract description 7
- 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 41
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 claims abstract description 31
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims abstract description 31
- 239000000292 calcium oxide Substances 0.000 claims abstract description 31
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims abstract description 31
- 239000000395 magnesium oxide Substances 0.000 claims abstract description 31
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims abstract description 31
- 239000000377 silicon dioxide Substances 0.000 claims abstract description 30
- 238000012986 modification Methods 0.000 claims abstract description 29
- 230000004048 modification Effects 0.000 claims abstract description 29
- 235000012239 silicon dioxide Nutrition 0.000 claims abstract description 28
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims abstract description 28
- 229910001887 tin oxide Inorganic materials 0.000 claims abstract description 28
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims abstract description 24
- 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
- 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
- 150000001875 compounds Chemical class 0.000 claims abstract description 5
- 239000003607 modifier Substances 0.000 claims abstract description 5
- 229910001938 gadolinium oxide Inorganic materials 0.000 claims description 26
- 229940075613 gadolinium oxide Drugs 0.000 claims description 26
- 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 26
- 239000003365 glass fiber Substances 0.000 claims description 24
- 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 16
- 230000008018 melting Effects 0.000 claims description 15
- 238000000034 method Methods 0.000 claims description 15
- 230000004927 fusion Effects 0.000 claims description 5
- 238000002156 mixing Methods 0.000 claims description 5
- 239000011810 insulating material Substances 0.000 claims description 4
- 238000004519 manufacturing process Methods 0.000 claims description 4
- 229910052810 boron oxide Inorganic materials 0.000 claims description 3
- JKWMSGQKBLHBQQ-UHFFFAOYSA-N diboron trioxide Chemical compound O=BOB=O JKWMSGQKBLHBQQ-UHFFFAOYSA-N 0.000 claims description 3
- 230000007797 corrosion Effects 0.000 abstract description 4
- 238000005260 corrosion Methods 0.000 abstract description 4
- 239000002245 particle Substances 0.000 description 16
- 238000010521 absorption reaction Methods 0.000 description 11
- 230000008569 process Effects 0.000 description 9
- 238000012360 testing method Methods 0.000 description 9
- 238000002474 experimental method Methods 0.000 description 7
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 6
- 239000011449 brick Substances 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 5
- 239000012535 impurity Substances 0.000 description 5
- 238000002425 crystallisation Methods 0.000 description 4
- 230000008025 crystallization Effects 0.000 description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 3
- -1 can be 60% Chemical compound 0.000 description 3
- 238000013461 design Methods 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- 239000011819 refractory material Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 229910052726 zirconium Inorganic materials 0.000 description 3
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 2
- 238000004364 calculation method Methods 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
- 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
- 239000000203 mixture Substances 0.000 description 2
- 239000005304 optical glass Substances 0.000 description 2
- 230000000737 periodic effect Effects 0.000 description 2
- 238000010298 pulverizing process Methods 0.000 description 2
- 239000011208 reinforced composite material Substances 0.000 description 2
- 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
- 230000008859 change Effects 0.000 description 1
- 238000011976 chest X-ray Methods 0.000 description 1
- JUVGUSVNTPYZJL-UHFFFAOYSA-N chromium zirconium Chemical compound [Cr].[Zr] JUVGUSVNTPYZJL-UHFFFAOYSA-N 0.000 description 1
- 238000005352 clarification Methods 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
- 238000010924 continuous production Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000000280 densification Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 238000012681 fiber drawing Methods 0.000 description 1
- 230000004992 fission Effects 0.000 description 1
- 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
- 238000005259 measurement Methods 0.000 description 1
- 239000006060 molten glass Substances 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 229910052863 mullite Inorganic materials 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
- 230000001105 regulatory effect Effects 0.000 description 1
- 230000003595 spectral effect Effects 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 238000004659 sterilization and disinfection Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 238000001392 ultraviolet--visible--near infrared spectroscopy Methods 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
- 238000005491 wire drawing Methods 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C4/00—Compositions for glass with special properties
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/04—Glass compositions containing silica
- C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
- C03C3/095—Glass compositions containing silica with 40% to 90% silica, by weight containing rare earths
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/04—Glass compositions containing silica
- C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
- C03C3/083—Glass compositions containing silica with 40% to 90% silica, by weight containing aluminium oxide or an iron compound
- C03C3/085—Glass compositions containing silica with 40% to 90% silica, by weight containing aluminium oxide or an iron compound containing an oxide of a divalent metal
- C03C3/087—Glass compositions containing silica with 40% to 90% silica, by weight containing aluminium oxide or an iron compound containing an oxide of a divalent metal containing calcium oxide, e.g. common sheet or container glass
-
- 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
- G21F1/06—Ceramics; Glasses; Refractories
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Geochemistry & Mineralogy (AREA)
- Life Sciences & Earth Sciences (AREA)
- Organic Chemistry (AREA)
- Ceramic Engineering (AREA)
- Physics & Mathematics (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Glass Compositions (AREA)
Abstract
The invention provides a radiation-resistant glass material and 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 modifier; wherein the network modification is at least one compound formed by combining an element with a neutron capture reaction cross section of not less than 100b and an oxygen element. The radiation-resistant glass material provided by the invention has excellent high-dose irradiation resistance, and also has 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 optical glass materials and glass fiber reinforced composite materials is expanded, and the optical glass materials and the glass fiber reinforced composite materials are widely applied to medical equipment such as chest X-rays, radiation sterilization and radiotherapy instruments, high-energy devices such as fusion reactors and fission reactors, and the fields of aerospace, ships, new energy, 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, so that electronic defects and impurity atoms are generated, and the performance and the service life of the glass are influenced. Although the existing radiation-resistant glass material has radiation resistance, the radiation resistance is still poor under high-dose radiation, and the mechanical property and the temperature resistance are also lost. Therefore, it is necessary to develop a radiation-resistant glass material with high radiation intensity, which can meet the requirements of mechanical and thermal stability of shielding, insulation, heat insulation and the like in high-energy radiation environment.
Disclosure of Invention
The embodiment of the invention provides a radiation-resistant glass material, and a preparation method and application thereof.
In a first aspect, the present 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 modifier; wherein the network modification is at least one compound formed by combining an element with a neutron capture reaction cross section of not less than 100b and an oxygen element.
Preferably, the network modification comprises at least one of boron oxide, cadmium oxide, gadolinium oxide.
Preferably, the network modification consists of cadmium oxide and gadolinium oxide.
More preferably, the molar ratio of cadmium oxide to gadolinium oxide in the network modification is not more than 1.
More preferably, the molar ratio of cadmium oxide to gadolinium oxide in the network modification is 1.
Preferably, the radiation-resistant glass material comprises the following components in mole percentage: 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 percentage: 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.
Preferably, the radiation-resistant glass material comprises the following components in mole percentage: 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 comprehensive neutron capture reaction cross section of the radiation-resistant glass material is 10-180 b.
In a second aspect, the present invention also provides a method for preparing a radiation-resistant glass material based on the above first aspect, the method comprising the steps of:
mixing 58-67% of silicon dioxide, 4-8% of aluminum oxide, 12-18% of calcium oxide, 7-18% of magnesium oxide, 0.5-1.2% of barium oxide, 0.1-0.8% of tin oxide, 0.5-1.2% of zirconium oxide and 0.1-0.7% of the network modifier in percentage by mole, melting and forming to obtain the radiation-resistant glass material.
Preferably, the radiation-resistant glass material is glass fiber.
More preferably, the glass fiber has a diameter of 8 to 22 μm.
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 at least has the following beneficial effects:
according to the invention, based on the neutron capture reaction section of an element, by adding the oxide with a high neutron capture reaction section into the radiation-resistant glass material, the deceleration and absorption of irradiated particles can be effectively realized, the intrinsic structure of the glass is protected, the irradiation resistance of the glass material is improved, and the high-dose irradiation resistance of the glass is further realized; meanwhile, the oxide with the high neutron capture reaction 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 process performance.
The radiation-resistant glass material prepared by the invention, such as glass fiber, is irradiated by gamma rays with the dosage of 1.02 multiplied by 10 7 After Gy irradiation, no obvious phenomena of embrittlement, shrinkage, pulverization and increase of heat conductivity coefficient are generated in the glass fiber, and the prepared glass fiber still has good mechanical properties. The radiation-resistant glass material prepared by the invention can resist high-dose accumulated irradiation in a space environment for a long time and can meet the requirement of the service life of the glass material more than 10 years.
Drawings
FIG. 1 is a graph showing absorption decay rates before and after irradiation of the radiation-resistant glass materials provided in examples 1 to 3 of the present invention.
Detailed Description
To make the objects, technical solutions and advantages of the embodiments of the present invention clearer and more complete, the technical solutions in the embodiments of the present invention will be described below with reference to the embodiments of the present invention and the accompanying drawings, it is obvious that the described embodiments are some, but not all embodiments of the present invention, and all other embodiments obtained by a person of ordinary skill in the art without making creative efforts based on the embodiments of the present invention belong to the protection scope of the present invention.
The embodiment of the invention provides a radiation-resistant glass material which comprises the following components in percentage by mole: 58 to 67% (e.g., can be 58%, 58.5%, 59%, 60%, 60.5%, 61%, 62%, 63%, 65%, 66%, or 67%), 4 to 8% (e.g., can be 4%, 4.5%, 5%, 5.5%, 6%, 6.5%, 7%, 7.5%, or 8%), 12 to 18% (e.g., can be 12%, 12.5%, 13%, 13.5%, 14%, 15%, 16%, 16.5%, 17%, 17.5%, or 18%), 7 to 18% (e.g., can 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%) (e.g., can 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 to 1.2% (e.g., can 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 to 0.8% (e.g., can 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 to 1.2% (e.g., can be 0.5%, 0.6%, 0.7%, 0.8%, 0.9%, 1.0%, 1.05%, 1.1%, 1.15%, or 1.2%), network variants 0.1 to 0.7% (e.g., can be 0.1%, 0.15%, 0.2%, 0.3%, 0.4%, 0.5%, 0.55%, or 0.2%); wherein the network modification is at least one compound formed by combining an element with a neutron capture reaction cross section of not less 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 Cd element having a neutron capture reaction cross section of 2450b, or Gd element having a neutron capture reaction cross section of 49000 b. The network modification is at least one oxide satisfying the above conditions.
Specifically, in the present invention, the radiation-resistant glass material further includes inevitable impurities, and the mole percentage of the impurities in the radiation-resistant glass material is less than 0.5%. The impurities comprise Fe 2 O 3 、Na 2 O、K 2 O, and the like.
In the invention, the silicon dioxide is a network former of the glass structure, and provides a basis for the mechanical property, the chemical stability and the irradiation property of the glass material. However, the content of the silicon dioxide needs to be regulated and controlled according to performance design, when the content of the silicon dioxide is too low, the glass network forming body is less, and the irradiation resistance and the mechanical property of the glass network forming body are reduced; however, if the content of the 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 not beneficial to the subsequent glass fiber forming. The invention therefore selects a silica content of between 58 and 67 mol%.
In the present invention, the alumina is present as network formers in the glass structure as [ AlO ] 4 ]The tetrahedron enters the glass network structure, so that the densification of the glass network structure can be enhanced, the phase splitting tendency of glass is reduced, the formation of crystal nuclei is inhibited to improve the forming process performance of subsequent glass fibers, and the mechanical strength, the modulus and the chemical corrosion resistance of the glass fibers are improved. Therefore, the content of the alumina is selected to be 4 to 8 mol percent.
In the invention, calcium oxide and magnesium oxide belong to the external body of a glass network structure, and mainly provide free oxygen in the glass components to promote the intermediate to form a tetrahedral structure so as to enhance the network compactness 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 process property of the glass material are improved. Therefore, the invention selects the calcium oxide content of 12-18 mol percent and the magnesium oxide content of 7-18 mol percent.
As is well known to those skilled in the art, the neutron capture reaction cross section of Si element is 0.171b; the neutron capture reaction section of the Al element is 0.232b; the neutron capture reaction section of the 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 the Sn element is 0.626b; the neutron capture reaction cross section of the Zr element was 0.184b.
In the invention, non-oxygen elements in silicon dioxide, aluminum oxide, calcium oxide and magnesium oxide all have smaller neutron capture reaction cross sections, and in the irradiation process, because the atomic radius is small, the collision probability of irradiation rays or photons can be effectively reduced, the irradiation resistance is improved, and the damage of a glass structure is reduced. Calcium oxide and magnesium oxide belong to alkaline earth metal oxides, ca and Mg belong to light elements in the front part of the periodic table of the elements, and the calcium oxide and the magnesium oxide have the radiation resistance; meanwhile, the introduction of calcium oxide and magnesium oxide can further improve the chemical stability and the irradiation resistance of the glass material.
In the invention, the barium oxide belongs to the outer body of a glass network structure in the glass structure, can provide free oxygen, promotes glass melting and improves glass fiber drawing, and meanwhile, the Ba 2+ The Ba has large ion radius, the neutron capture reaction section of the Ba is 1.3b, the Ba is a heavy metal element with the largest neutron capture reaction section in alkaline earth metal elements, has better deceleration effect and higher ray capture capacity on irradiated ions, and can effectively reduce the kinetic energy of rays through collision with high-energy particles or photons, thereby reducing the probability of damage of a glass structure and further improving the irradiation resistance. The invention selects the content of barium oxide to be 0.5-1.2 mol percent.
In the invention, the tin oxide belongs to a network modification in the glass structure, the bond energy is 192.6kJ/mol, the glass liquid has better clarification effect at the temperature of more than 1560 ℃, and the tin oxide can be used as a clarifier for glass melting. Meanwhile, the tin oxide has the characteristics of better conductivity and infrared radiation reflection, 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 content of the tin oxide selected by the invention is 0.1-0.5 mol percent.
In the invention, the zirconia belongs to the external body of a glass network structure in the glass structure, so that the high-temperature viscosity of the glass can be increased, the thermal expansion coefficient can be reduced, and the alkali resistance of the glass material can be obviously improved. Zr 4+ The large ionic radius can also slow down the radiation particles, i.e. slow the particles, and reduce the radiation damage of the glass material body structure. Thus, to ensure that the zirconia performs its function adequately, the zirconia content selected for the present invention is from 0.5 to 1.2 mole percent.
The invention adopts at least one compound formed by combining the element with the neutron capture reaction section not less than 100b and the oxygen element as the network modification body, and fills the network modification body in the gap of the glass network structure, and in the irradiation process, because the element neutron capture reaction section not less than 100b is contained, the probability of collision with the irradiation particles is higher, namely the probability of nuclear reaction is higher, and the reaction activity is higher, thus the network modification body can realize the deceleration and absorption of the irradiation particles, reduce and even avoid the damage of the irradiation particles to the glass network structure, and further obviously improve the irradiation resistance of the irradiation-resistant glass material. Experiments prove that when the content of the network modification is 0.1-0.7 mol%, the comprehensive neutron capture reaction section of the prepared radiation-resistant glass material is 10-180 b, namely, the radiation-resistant glass material has excellent radiation resistance, and the experiment proves that the larger the comprehensive neutron capture reaction 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 radiation resistance of the radiation-resistant glass material can be realized according to actual use requirements by selecting oxides formed by the elements with different high neutron capture reaction cross sections and controlling the mole percentage of the oxides and consuming the irradiated particles through the collision and absorption of the oxides on the irradiated particles.
According to some preferred embodiments, the network modification comprises at least one of boron oxide, cadmium oxide, gadolinium oxide.
At least one of them is a mixture of any one or more of them mixed in any ratio.
According to some preferred embodiments, the network modification consists of cadmium oxide and gadolinium oxide.
According to some preferred embodiments, the molar ratio of cadmium oxide and gadolinium oxide in the network modification is no greater than 1.
According to some more preferred embodiments, the molar ratio of cadmium oxide and gadolinium oxide in the network modification is 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 molar 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 molar 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 in the glass structure and is filled in gaps of the network structure, the single bond energy is 83.7kJ/mol, and the density of the glass material can be obviously increased. Meanwhile, the neutron capture reaction section of Cd is 2450b, the probability of collision with the 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. Experiments prove that the content of the cadmium oxide selected by the invention is 0-0.7 mol%.
In the invention, gadolinium oxide is used as a network modification in a glass structure, 1 electron is on 7 electron orbitals of Gd, which is the largest unpaired electron in rare earth elements, in the current periodic table of elements, gd has the highest neutron capture reaction cross section 49000b, the probability of collision with particles during irradiation is highest, and the deceleration and absorption effects on the particles are most remarkable, so that the gadolinium oxide can play an excellent protection role on the network structure of the glass. Experiments prove that the content of the gadolinium oxide selected by the invention is 0.1-0.6 mol%.
According to some preferred embodiments, the radiation-resistant glass material comprises the following components in mole percent: 60 to 65% silica (e.g., can be 60%, 60.5%, 61%, 61.5%, 62%, 62.5%, 63%, 63.5%, 64%, 64.5%, or 65%), 5 to 7% alumina (e.g., can be 5%, 5.5%, 6%, 6.5%, or 7%), 14 to 16% calcium oxide (e.g., can be 14%, 14.5%, 15%, 15.5%, or 16%), 10 to 15% magnesium oxide (e.g., can be 10%, 10.5%, 11%, 11.5%, 12%, 12.5%, 13%, 13.5%, 14%, 14.5%, or 15%), 0.8 to 1.0% (e.g., may be 0.8%, 0.85%, 0.9%, 0.95%, or 1.0%), 0.3 to 0.5% (e.g., may be 0.3%, 0.35%, 0.4%, 0.45%, or 0.5%), 0.5 to 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%), 0.2 to 0.5% (e.g., may be 0.21%, 0.25%, 0.29%, 0.35%, 0.4%, 0.45%, or 0.5%) of barium oxide, 0.3 to 0.5% (e.g., may be 0.3%, 0.35%, 0.9%, 0.45%, or 0.5%).
According to some more preferred embodiments, the radiation-resistant glass material comprises, 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 an integrated neutron capture reaction cross-section in the range of 10 to 180b.
It should be noted that, in the present invention, by utilizing the characteristic that the glass property has additivity, the comprehensive neutron capture reaction cross section is calculated by the following formula:
wherein F is used for representing a 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. The k The mole percentage used to characterize the kth component; omega k For characterizing the neutron capture reaction cross section of the non-oxygen element in the kth component. Experiments prove that the method is as followsThe comprehensive neutron capture reaction section of the radiation-resistant glass material is obtained through calculation according to the formula, and the conclusion that the larger the comprehensive neutron capture reaction section is, the more excellent the radiation resistance is obtained. Therefore, it is further confirmed that the radiation-resistant glass material designed based on the elemental neutron capture reaction cross section 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:
mixing 58-67% of silicon dioxide, 4-8% of aluminum oxide, 12-18% of calcium oxide, 7-18% of magnesium oxide, 0.5-1.2% of barium oxide, 0.1-0.8% of tin oxide, 0.5-1.2% of zirconium oxide and 0.1-0.7% of network modifier in percentage by mole, melting and forming to obtain the radiation-resistant glass material.
According to some preferred embodiments, the radiation resistant glass material is glass fiber.
Specifically, in the present invention, the furnace melting can be performed by oxy-fuel combustion, electro-melting or a combination of fire and electricity to form homogeneous glass. The kiln for melting glass can be made of refractory material with high temperature resistance and molten glass corrosion resistance, such as high-zirconium fused brick, compact zirconium brick, mullite fused brick, etc. The glass fiber can also be produced by adopting a platinum-substituting furnace with a refractory material compact zirconium brick, a corundum brick, an electric melting chromium zirconium corundum brick and a mullite structure to carry out two-step wire drawing, namely, the glass is firstly melted according to the components and the mol percent thereof, and then the glass is drawn into the glass fiber. The glass fiber can also be produced by one-step drawing through the kiln passage with the refractory material structure.
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 melting is 1500-1600 ℃ (for example, 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, radiation resistant glass materials are used as insulating materials for the magnetic field coils of the thermonuclear fusion reactor.
In order to more clearly illustrate the technical scheme and advantages of the present invention, a radiation-resistant glass material, a preparation method thereof and applications thereof are described in detail by using several embodiments.
The particle size of each raw material of the components used in the following examples is less than 200 mesh, and unavoidable impurities are present in the finally prepared radiation-resistant glass material.
Example 1
The radiation-resistant glass material comprises the following components in percentage by mole: 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. Accurately weighing the components according to the proportion, uniformly mixing the weighed components to obtain a batch, pneumatically mixing and conveying the batch to a furnace charging port, feeding the batch by using an automatic feeder, melting the batch by using an all-electric melting furnace or a kiln at 1600 ℃ to obtain clarified and homogenized glass liquid, preparing the glass liquid into glass balls, melting the melted glass balls at 1550 ℃ by using a platinum-substituting furnace, and controlling the forming process parameters of the glass fibers by using a bushing plate with the diameter of more than 400 so as to obtain the continuous glass fibers with the diameter of 8-22 mu m, 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 percentage by mole: 65.60% of silicon dioxide, 4.82% of aluminum oxide, 15.38% of calcium oxide, 12.30% of magnesium oxide, 0.8% of barium oxide, 0.2% of tin oxide, 0.5% of zirconium oxide, 0.23% of cadmium oxide and 0.17% of gadolinium oxide.
Example 3
Example 3 is essentially the same as example 1, except that:
the radiation-resistant glass material comprises the following components in mole percentage: 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 essentially the same as example 1, except that:
the radiation-resistant glass material comprises the following components in mole percentage: 64.99 percent of silicon dioxide, 4.78 percent of aluminum oxide, 13.06 percent of calcium oxide, 15.23 percent of magnesium oxide, 0.79 percent of barium oxide, 0.2 percent of tin oxide, 0.49 percent of zirconium oxide and 0.45 percent of cadmium oxide.
Example 5
Example 5 is essentially 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 essentially 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 essentially 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 percentage by mole: 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 percentage: 63.35 percent of silicon dioxide, 4.66 percent of aluminum oxide, 12.73 percent of calcium oxide, 17.82 percent of magnesium oxide, 0.77 percent of barium oxide, 0.2 percent of tin oxide and 0.48 percent of zirconium oxide.
The prepared radiation-resistant glass materials prepared in examples 1 to 4 and comparative examples 1 and 2 were used as samples to perform mechanical property tests, gamma ray irradiation tests, crystallization upper limit temperature and high temperature viscosity measurements, and the comprehensive neutron capture reaction cross section of the samples was calculated according to the above formula, and the test results are shown in table 1. Wherein, the test conditions of the gamma ray irradiation test are as follows: the activity of the cobalt source is about 9 ten thousand Curie, the dose rate is 11034Gy/h, and the total irradiation dose is 1.02 multiplied by 10 7 Gy; testing the crystallization upper limit temperature of the glass by adopting a gradient crystallization temperature test furnace; the high temperature viscosity was measured using a Brookfield high temperature viscometer in the United states. The elastic modulus of the material is calculated by testing the propagation speed of ultrasonic waves or sound waves in a sample by adopting a dynamic method.
TABLE 1
For the sample, respectively carrying out UV-VIS-NIR spectral tests before and after irradiation, comparing the absorption attenuation changes before and after irradiation, and obtaining an absorption attenuation rate curve through calculation as shown in figure 1 (wherein the curves correspond to example 1, example 2 and example 3 from bottom to top in sequence); wherein the measuring wavelength range is 300-1300 nm; the abscissa of fig. 1 is the wavelength (unit nm) and the ordinate is the absorption decay rate.
Absorption decay Rate, i.e., (alpha) Front side -α Rear end )/α Front side ，α Front side And alpha Rear end The absorption coefficients before and after the irradiation of the glass sheet are respectively, and the absorption attenuation rate versus wavelength curve is characterizedOne method of making a glass material superior or inferior in irradiation resistance is that the lower the peak value, the better the irradiation resistance, and conversely, the worse. 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 present invention, that is, by introducing an oxide with a high neutron capture reaction cross section, and slowing down or absorbing the irradiated particles, the network structure of the glass can be better protected. Meanwhile, it is further confirmed by combining table 1 and fig. 1 that the irradiation resistance of the radiation-resistant glass material calculated by the method of the present invention is more excellent as the comprehensive neutron capture reaction cross section is larger.
Meanwhile, experiments prove that the radiation-resistant glass materials prepared in the embodiments 1 to 7 of the invention have the radiation dose of 1.02 multiplied by 10 after being irradiated by gamma rays 7 After Gy irradiation, no obvious phenomena of embrittlement, shrinkage, pulverization and increase of thermal conductivity coefficient are generated in the glass fiber, and the prepared glass fiber still has good mechanical properties. The radiation-resistant glass material prepared by the invention can resist high-dose accumulated irradiation for a long time in a 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 by the embodiment of the invention is resistant to high-dose irradiation and has high strength and high modulus. Meanwhile, according to the forming temperature, the invention improves the forming process performance of the fiber, 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 the molding temperature is large due to the change in the contents of calcium oxide and magnesium oxide. Furthermore, experiments prove that the radiation-resistant glass material prepared by the invention can be applied to the environment with the temperature of 800-900 ℃ (for example, 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 mixture ratio of the components and the dosage thereof has excellent high-dose irradiation resistance, excellent mechanical property and temperature resistance, can be used as an insulating material of a magnetic field coil of a thermonuclear fusion reactor, and can also be used in the fields relating to particle radiation, such as aerospace, deep space exploration and the like.
Finally, it should be noted that: the above examples are only intended to illustrate the technical solution of the present invention, and not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it should be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention. The invention has not been described in detail and is not limited thereto.
Claims (10)
1. An irradiation-resistant glass material, characterized in that the irradiation-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 and 0.1 to 0.7 percent of network modification; wherein the network modification is at least one compound formed by combining an element with a neutron capture reaction cross section of not less than 100b and an oxygen element.
2. Radiation-resistant glass material according to claim 1,
the network modification comprises at least one of boron oxide, cadmium oxide and gadolinium oxide.
3. Radiation-resistant glass material according to claim 1,
the network modification consists of cadmium oxide and gadolinium oxide.
4. Radiation-resistant glass material according to claim 3,
the molar ratio of cadmium oxide to gadolinium oxide in the network modification is not more than 1; more preferably 1.
5. Radiation-resistant glass material according to claim 1,
the radiation-resistant glass material comprises the following components in mole percentage: 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.
6. Radiation-resistant glass material according to claim 1,
the radiation-resistant glass material comprises the following components in mole percentage: 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.
7. Radiation-resistant glass material according to one of claims 1 to 6,
the radiation-resistant glass material comprises the following components in percentage by mole: 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.
8. The method for producing a radiation-resistant glass material according to any one of claims 1 to 7, characterized in that it comprises the following steps:
mixing 58-67% of silicon dioxide, 4-8% of aluminum oxide, 12-18% of calcium oxide, 7-18% of magnesium oxide, 0.5-1.2% of barium oxide, 0.1-0.8% of tin oxide, 0.5-1.2% of zirconium oxide and 0.1-0.7% of the network modifier in percentage by mole, melting and forming to obtain the radiation-resistant glass material.
9. The method of claim 8,
the radiation-resistant glass material is glass fiber; preferably, the diameter of the glass fiber is 8 to 22 μm; and/or
The melting temperature is 1500-1600 ℃.
10. Use of a radiation-resistant glass material according to any one of claims 1 to 7 or produced according to the production method of claim 8 or 9, characterized in that the radiation-resistant glass material is used in the field of radiation-resistant materials, preferably as an insulating material for magnetic field coils of thermonuclear fusion reactors.
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