CN111908931A - Low-carbon aluminum silicon carbide carbon brick containing nano carbon and preparation method thereof - Google Patents
Low-carbon aluminum silicon carbide carbon brick containing nano carbon and preparation method thereof Download PDFInfo
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- CN111908931A CN111908931A CN202010700556.7A CN202010700556A CN111908931A CN 111908931 A CN111908931 A CN 111908931A CN 202010700556 A CN202010700556 A CN 202010700556A CN 111908931 A CN111908931 A CN 111908931A
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- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 163
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 138
- 239000011449 brick Substances 0.000 title claims abstract description 112
- 229910021392 nanocarbon Inorganic materials 0.000 title claims abstract description 97
- 229910010271 silicon carbide Inorganic materials 0.000 title claims abstract description 88
- CSDREXVUYHZDNP-UHFFFAOYSA-N alumanylidynesilicon Chemical compound [Al].[Si] CSDREXVUYHZDNP-UHFFFAOYSA-N 0.000 title claims abstract description 62
- 238000002360 preparation method Methods 0.000 title claims abstract description 26
- 239000002994 raw material Substances 0.000 claims abstract description 72
- 239000011230 binding agent Substances 0.000 claims abstract description 32
- 229910052593 corundum Inorganic materials 0.000 claims abstract description 27
- 239000010431 corundum Substances 0.000 claims abstract description 27
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims abstract description 20
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 20
- 239000002245 particle Substances 0.000 claims abstract description 18
- 229910001570 bauxite Inorganic materials 0.000 claims abstract description 15
- 239000000395 magnesium oxide Substances 0.000 claims abstract description 10
- 238000000034 method Methods 0.000 claims description 20
- 239000000843 powder Substances 0.000 claims description 16
- 238000005229 chemical vapour deposition Methods 0.000 claims description 15
- 239000000835 fiber Substances 0.000 claims description 15
- 238000002156 mixing Methods 0.000 claims description 14
- 239000000203 mixture Substances 0.000 claims description 14
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 13
- 238000000227 grinding Methods 0.000 claims description 12
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 10
- -1 carbon aluminum silicon Chemical compound 0.000 claims description 10
- 239000004917 carbon fiber Substances 0.000 claims description 10
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 9
- 235000019580 granularity Nutrition 0.000 claims description 9
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 9
- 238000003756 stirring Methods 0.000 claims description 9
- 238000010438 heat treatment Methods 0.000 claims description 8
- 239000011248 coating agent Substances 0.000 claims description 7
- 238000000576 coating method Methods 0.000 claims description 7
- 239000007787 solid Substances 0.000 claims description 7
- 238000000465 moulding Methods 0.000 claims description 5
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 claims description 4
- 230000032683 aging Effects 0.000 claims description 4
- 238000001035 drying Methods 0.000 claims description 4
- 239000010419 fine particle Substances 0.000 claims description 4
- 239000011521 glass Substances 0.000 claims description 4
- 239000002120 nanofilm Substances 0.000 claims description 4
- 239000005011 phenolic resin Substances 0.000 claims description 4
- 229920001568 phenolic resin Polymers 0.000 claims description 4
- 239000002912 waste gas Substances 0.000 claims description 4
- 238000007599 discharging Methods 0.000 claims description 3
- 238000002844 melting Methods 0.000 claims description 3
- 230000008018 melting Effects 0.000 claims description 3
- 238000012216 screening Methods 0.000 claims description 3
- 238000005245 sintering Methods 0.000 claims description 3
- 238000005303 weighing Methods 0.000 claims description 3
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 claims description 2
- 229910052796 boron Inorganic materials 0.000 claims description 2
- 229920001187 thermosetting polymer Polymers 0.000 claims description 2
- 239000003795 chemical substances by application Substances 0.000 claims 1
- 230000001089 mineralizing effect Effects 0.000 claims 1
- 230000001976 improved effect Effects 0.000 abstract description 16
- 230000003647 oxidation Effects 0.000 abstract description 15
- 238000007254 oxidation reaction Methods 0.000 abstract description 15
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 abstract description 15
- 229910002804 graphite Inorganic materials 0.000 abstract description 12
- 239000010439 graphite Substances 0.000 abstract description 12
- 230000002829 reductive effect Effects 0.000 abstract description 10
- 239000006185 dispersion Substances 0.000 abstract description 7
- 230000008595 infiltration Effects 0.000 abstract description 5
- 238000001764 infiltration Methods 0.000 abstract description 5
- 238000001179 sorption measurement Methods 0.000 abstract description 5
- 239000013078 crystal Substances 0.000 abstract description 4
- 239000002904 solvent Substances 0.000 abstract description 4
- 229910003481 amorphous carbon Inorganic materials 0.000 abstract description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 50
- 229910052742 iron Inorganic materials 0.000 description 25
- 229910052751 metal Inorganic materials 0.000 description 21
- 239000002184 metal Substances 0.000 description 21
- 230000035939 shock Effects 0.000 description 15
- 230000008569 process Effects 0.000 description 12
- 230000003628 erosive effect Effects 0.000 description 11
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 10
- 239000002131 composite material Substances 0.000 description 9
- 230000000694 effects Effects 0.000 description 9
- 238000004519 manufacturing process Methods 0.000 description 9
- 229910052710 silicon Inorganic materials 0.000 description 9
- 239000010703 silicon Substances 0.000 description 9
- 239000002893 slag Substances 0.000 description 7
- 230000007797 corrosion Effects 0.000 description 6
- 238000005260 corrosion Methods 0.000 description 6
- 238000005516 engineering process Methods 0.000 description 6
- 150000004767 nitrides Chemical class 0.000 description 6
- 239000011819 refractory material Substances 0.000 description 6
- 239000000463 material Substances 0.000 description 5
- 230000035515 penetration Effects 0.000 description 5
- 229910052903 pyrophyllite Inorganic materials 0.000 description 5
- 229910052849 andalusite Inorganic materials 0.000 description 4
- 239000003963 antioxidant agent Substances 0.000 description 4
- 238000001816 cooling Methods 0.000 description 4
- 239000011148 porous material Substances 0.000 description 4
- 238000004321 preservation Methods 0.000 description 4
- 230000003014 reinforcing effect Effects 0.000 description 4
- 238000005299 abrasion Methods 0.000 description 3
- 230000002411 adverse Effects 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 239000007767 bonding agent Substances 0.000 description 3
- 238000003763 carbonization Methods 0.000 description 3
- 238000013329 compounding Methods 0.000 description 3
- 230000007547 defect Effects 0.000 description 3
- 239000010410 layer Substances 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- 238000003723 Smelting Methods 0.000 description 2
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 2
- 230000003078 antioxidant effect Effects 0.000 description 2
- 238000005336 cracking Methods 0.000 description 2
- 238000005262 decarbonization Methods 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000007888 film coating Substances 0.000 description 2
- 238000009501 film coating Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 230000017525 heat dissipation Effects 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 230000000670 limiting effect Effects 0.000 description 2
- 239000004570 mortar (masonry) Substances 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 238000009991 scouring Methods 0.000 description 2
- 238000009865 steel metallurgy Methods 0.000 description 2
- 238000009628 steelmaking Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000002344 surface layer Substances 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- 229910000838 Al alloy Inorganic materials 0.000 description 1
- 241000872198 Serjania polyphylla Species 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 239000004411 aluminium Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- SNAAJJQQZSMGQD-UHFFFAOYSA-N aluminum magnesium Chemical compound [Mg].[Al] SNAAJJQQZSMGQD-UHFFFAOYSA-N 0.000 description 1
- 238000013475 authorization Methods 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 230000008878 coupling Effects 0.000 description 1
- 238000010168 coupling process Methods 0.000 description 1
- 238000005859 coupling reaction Methods 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000006477 desulfuration reaction Methods 0.000 description 1
- 230000023556 desulfurization Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 230000008030 elimination Effects 0.000 description 1
- 238000003379 elimination reaction Methods 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 238000011010 flushing procedure Methods 0.000 description 1
- 238000000265 homogenisation Methods 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 229910021421 monocrystalline silicon Inorganic materials 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 230000036961 partial effect Effects 0.000 description 1
- 229910021420 polycrystalline silicon Inorganic materials 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 230000033764 rhythmic process Effects 0.000 description 1
- 239000002210 silicon-based material Substances 0.000 description 1
- 238000007711 solidification Methods 0.000 description 1
- 230000008023 solidification Effects 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 235000019587 texture Nutrition 0.000 description 1
- 230000008354 tissue degradation Effects 0.000 description 1
- 230000007306 turnover Effects 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/10—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on aluminium oxide
- C04B35/101—Refractories from grain sized mixtures
- C04B35/103—Refractories from grain sized mixtures containing non-oxide refractory materials, e.g. carbon
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/34—Non-metal oxides, non-metal mixed oxides, or salts thereof that form the non-metal oxides upon heating, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3427—Silicates other than clay, e.g. water glass
- C04B2235/3463—Alumino-silicates other than clay, e.g. mullite
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- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/36—Glass starting materials for making ceramics, e.g. silica glass
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- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/38—Non-oxide ceramic constituents or additives
- C04B2235/3817—Carbides
- C04B2235/3826—Silicon carbides
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- C04B2235/40—Metallic constituents or additives not added as binding phase
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- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/42—Non metallic elements added as constituents or additives, e.g. sulfur, phosphor, selenium or tellurium
- C04B2235/422—Carbon
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- C04B2235/5216—Inorganic
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- C04B2235/9607—Thermal properties, e.g. thermal expansion coefficient
Abstract
The invention discloses a low-carbon aluminum silicon carbide carbon brick containing nano carbon and a preparation method thereof. By applying the nano carbon film and the dispersible nano carbon which are coated on the surfaces of all, part or all of the high-alumina bauxite chamotte, brown corundum and sub-white corundum raw material particles, the oxidation resistance of the nano carbon is improved by utilizing the characteristics that the nano carbon film and the dispersible nano carbon are mainly amorphous carbon, contain a small amount of graphite crystal, can be infiltrated by a solvent and the like, the infiltration and adsorption of the nano carbon film and the dispersible nano carbon on an organic binder are improved, the uniform dispersion of the nano carbon in the magnesia carbon brick is realized, the size of carbon particles in the alumina silicon carbide carbon brick is greatly reduced by controlling the thickness of the nano carbon film and the dispersible nano carbon, the contact frequency of the refractory raw material of the alumina silicon carbide carbon brick and the carbon particles is obviously improved, and the performance of the carbon particles under the condition of low carbon content is ensured.
Description
Technical Field
The invention belongs to the technical field of refractory materials, and particularly relates to a low-carbon aluminum silicon carbide carbon brick containing nano carbon and a preparation method thereof.
Background
The hot metal ladle is used for conveying hot molten iron between blast furnace iron making and converter steel making processes, and the intermittent smelting mode of the converter requires that the molten iron is added at intervals according to the production rhythm of the converter, so that the intermittent service condition of the hot metal ladle, the rapid cooling and oxidation of the cold air of the refractory material lining after iron adding and the rapid heating of the high-temperature molten iron during iron receiving are caused, and therefore, the refractory material lining of the hot metal ladle is required to bear the large-temperature-difference thermal shock impact of the rapid cooling of the air and the rapid heating of the high-temperature molten iron, and the erosion and penetration of the high-temperature molten iron and molten iron scouring in the iron adding process. With the continuous progress of the steel metallurgy production process, the continuous aggravation of the manufacturing cost pressure and the continuous improvement of the quality requirement of users on steel grades, the low-cost molten iron pretreatment technology is widely popularized and applied, however, in the molten iron pretreatment process, the severe stirring and scouring and the multiphase high-temperature metallurgical reaction in the molten iron tank further deteriorate the service working condition of the molten iron tank, the service life of the molten iron tank is continuously reduced, and therefore, higher requirements are provided for the lining refractory material of the molten iron tank.
The aluminum silicon carbide carbon brick effectively ensures the erosion resistance, the thermal shock resistance and the erosive wear resistance of the aluminum silicon carbide carbon brick by introducing a large amount of graphite carbon sources and silicon carbide and utilizing the high temperature resistance, infiltration resistance, erosion resistance, high thermal conductivity, oxidation resistance, abrasion resistance and the like of graphite and the high temperature resistance, erosion resistance, high thermal conductivity, oxidation resistance, abrasion resistance and the like of silicon carbide, and is widely applied to hot metal ladles of domestic and foreign iron and steel metallurgy enterprises, thereby achieving the positive effects of prolonging the service life of the hot metal ladles and reducing the production cost. At present, the conventional aluminum silicon carbide carbon brick is a non-burning carbon-containing composite refractory material which takes alumina, silicon carbide and carbon raw materials as main components and takes phenolic resin and the like as a bonding agent, wherein the mass fraction of carbon is usually 8-16%. However, due to the oxidability of graphite, the oxidation and decarbonization of the surface layer of the aluminum silicon carbide carbon brick in the hot metal ladle baking process and the empty ladle after iron charging are caused, particularly, the oxidation layer decarbonization is more serious in the baking process, the corrosion and penetration of the refractory brick are aggravated, the cracking of the texture structure of the brick surface layer, the thermal shock crack stripping and the erosion abrasion are further caused, and the further prolonging of the service life of the hot metal ladle is restricted; meanwhile, due to the high thermal conductivity of the graphite and the silicon carbide, the surface heat dissipation of the hot metal tank is high, the temperature of the hot metal is greatly reduced, the heat balance of the converter smelting is influenced, and the steel-making cost of the converter is increased; in addition, the use of a large amount of high-purity graphite and silicon carbide raw materials and the addition of high-price antioxidants cause the high-performance aluminum silicon carbide carbon brick to be expensive, and the application economy of the brick is influenced.
Aiming at the defects, domestic scholars develop a great deal of research work and obtain a certain effect of improving the service performance of the existing aluminum silicon carbide carbon brick. Such as:
the Chinese patent' Tian Ximing, Guo Jingna, flood and other, an aluminum silicon carbide carbon brick added with silicon carbide-metal silicon composite powder, authorization notice number: CN 102757245B "discloses a raw material composition of a low-cost aluminum silicon carbide carbon brick and a preparation method thereof, wherein the raw material composition in percentage by weight is as follows: 40-75% of bauxite clinker, 10-25% of corundum, 8-10% of graphite, 4-15% of silicon carbide-metal silicon composite powder, 0-15% of silicon carbide and 0-4% of metal silicon, wherein the sum of the weight percentages of the components is 100%, and an additional bonding agent is added, and the weight percentage of the additional bonding agent is 3-4 wt% of the sum of the weight percentages of the components; the preparation method is mainly characterized in that waste mortar generated in the cutting process of the polycrystalline silicon or monocrystalline silicon material is firstly treated to obtain the silicon carbide-metal silicon composite powder, and then the aluminum silicon carbide carbon brick is prepared by taking the composite powder as a raw material, so that the production cost is reduced, and the use effect is improved. However, the method has complex process, the components of the composite powder obtained by treating the waste mortar are difficult to keep stable, the stability of the product is influenced, and the service cycle of the product is difficult to control.
Chinese patent' Feng construction, Fan pioneer, slowly fragrant Ru etc., an aluminium carborundum carbon brick for torpedo tank and its preparation method, application publication number: CN102603314A patent technology discloses components of an aluminum silicon carbide carbon brick added with nitride and a preparation method thereof, wherein the components comprise the following components in percentage by weight: 10-30% of special-grade alumina, 15-35% of 1-3 mm sub-white corundum, 5-15% of silicon carbide, 2-10% of andalusite, 5-15% of flake graphite, 5-15% of 325-mesh sub-white corundum, 1-10% of nitride, 2-3% of metal aluminum powder and 3-5% of phenolic resin. Through high-temperature expansion of andalusite, the volume stability of the brick body in the service process is improved, through preferential oxidation of nitride, the problem of tissue degradation caused by oxidation of graphite and silicon carbide in the brick body is prevented, and through reinforcing and toughening and pore filling of needle-shaped SiC crystals formed by decomposition of the nitride, the infiltration and diffusion of slag are prevented, and the anti-erosion capacity of the brick body is improved. However, the nitride is expensive, and the large addition amount of the nitride causes high production cost of the product, thereby affecting the economic performance of the patent technology; meanwhile, the addition of metal aluminum powder can affect the high-temperature use performance of the aluminum silicon carbide carbon brick.
The Chinese patent' Wangchun, Chenschi, Fangyi, etc., a semi-light aluminum silicon carbide carbon brick and a preparation method thereof, the application publication number is: CN 108083785A discloses a composition and a preparation method of a geothermal conductivity aluminum silicon carbide carbon brick, which is characterized in that guyana alumina is used for replacing common high-alumina and corundum, and the characteristics of little impurity, high purity, high apparent porosity and low density of guyana alumina are utilized to prepare the semi-light aluminum silicon carbide carbon brick with low density, good thermal shock stability, erosion resistance and low thermal conductivity, thereby achieving the purposes of reducing the temperature drop of molten iron and reducing the manufacturing cost. However, no actual production application report is found at present, and the erosion wear resistance of the alloy is required to be further verified.
Chinese patent "wanese, fang yineng, wu bin, etc., a method for preparing a low carbon aluminum silicon carbide carbon brick, issued publication no: CN 03588493B ", wherein the raw material components by weight percentage are: 60-85% of an aluminum oxide raw material, 1-10% of silicon carbide, 2-5% of a carbon raw material, 3-5% of a binding agent, 1-5% of an antioxidant and 0.01-0.5% of organic silicon fiber; al in the alumina raw material2O3The average weight percentage of the aluminum silicon carbide carbon brick is 75-98%, the addition of the organic silicon fibers ensures that the carbon content is reduced to below 7%, the good thermal shock stability of the aluminum silicon carbide carbon brick is ensured, the thermal conductivity of the aluminum silicon carbide carbon brick is reduced by more than 20%, and the purposes of energy conservation and consumption reduction are achieved. But has the problem that the carbon black with the particle size of-1000 meshes is easy to agglomerate, and the dispersion uniformity of the carbon material in a brick body and the stability of the product quality are influenced.
The Chinese patent 'Duchun, Lixing' and aluminum silicon carbide carbon brick for hot metal bottle and the preparation method thereof, application publication number: CN 106007741A ", discloses a formula of an aluminum silicon carbide carbon brick containing andalusite, pyrophyllite and silicon carbide superfine powder raw materials but no graphite carbon source, and through the micro-expansion of the andalusite under service conditions, brick joints are reduced, molten iron leakage is avoided, the thermal shock stability of the product is improved, and the stripping phenomenon is thoroughly solved; the corrosion and penetration of molten iron and slag to the brick body are blocked through a glaze surface formed by pyrophyllite glazing under the service condition, the phenomenon of sticking to the brick is eliminated, and the corrosion rate is reduced; by introducing the superfine powder of silicon carbide, the oxidation resistance and the scour resistance of the brick body are improved, and the service life of the aluminum silicon carbide carbon brick is prolonged. However, the introduction of the superfine powder silicon carbide increases the cost of raw materials for making bricks, meanwhile, the addition of a large proportion of pyrophyllite has a certain influence on the high-temperature strength of the brick body, the high-temperature corrosion resistance of the pyrophyllite is to be further verified, and in addition, the elimination of the carbon raw material and the corrosion and permeation resistance of the pyrophyllite also need to be verified in production and application.
In summary, the scholars in China have developed patent technologies of various characteristic aluminum silicon carbide carbon bricks by research on novel antioxidants, application of semi-light materials, compounding of raw material components, low carbon and development of low-cost technologies and the like aiming at adverse effects on service performance such as easy oxidation, high heat conduction and sintering shrinkage of conventional aluminum silicon carbide carbon bricks and economic problems caused by high cost, and the research on the single-index obviously improved effect is achieved under laboratory conditions.
Disclosure of Invention
The invention aims to provide a low-carbon aluminum silicon carbide carbon brick containing nano carbon and a preparation method thereof, aiming at the defects of the technology, the low-carbon aluminum silicon carbide carbon brick has the characteristics of low total carbon content (less than or equal to 6%), low thermal conductivity, large volume density, high mechanical strength, excellent oxidation resistance, slag corrosion permeation resistance, heat peeling resistance and the like, and achieves the comprehensive purposes of prolonging the service life of a hot metal ladle, reducing the heat dissipation loss of the surface of the ladle wall, reducing the temperature drop of molten iron and the like.
In order to achieve the purpose, the raw materials of the low-carbon aluminum silicon carbide carbon brick containing the nano-carbon comprise a main raw material and an auxiliary raw material, wherein the main raw material comprises the following components in percentage by weight:
the auxiliary raw materials comprise an organic binder, anhydrous alcohol, polyvinyl alcohol fibers and chopped carbon fibers, wherein the weight of the anhydrous alcohol accounts for 0-3% of the total weight of the main raw material, the weight of the organic binder accounts for 3-5% of the total weight of the main raw material, the weight of the polyvinyl alcohol fibers accounts for 0.05-0.15% of the total weight of the main raw material, and the weight of the chopped carbon fibers accounts for 0-0.2% of the total weight of the main raw material;
the two high-alumina bauxite chamottes, the two brown corundum and the sub-white corundum are arranged from small to large according to the granularity, at least one raw material is taken from small to large to coat a nano carbon film, the thickness of the nano carbon film is 20-200 nanometers, the fixed carbon content of the nano carbon film is more than or equal to 90 percent, the fixed carbon content of the dispersible nano carbon is more than or equal to 80 percent, and the total carbon content of the low-carbon aluminum silicon carbide carbon brick containing the nano carbon is less than or equal to 6 percent.
Further, Al in the bauxite chamotte2O3The weight percentage content is more than or equal to 85 percent.
Furthermore, the melting point of the polyvinyl alcohol fiber is less than or equal to 90 ℃, and the water-soluble temperature is more than or equal to 55 ℃.
Furthermore, the diameter of the chopped fiber is 5-9 μm, the length of the chopped fiber is 0.5-2.5 mm, and the carbon content is more than or equal to 95 wt%.
Further, the antioxidant is at least one of silicon metal powder and magnesium-aluminum alloy powder, the sintering mineralizer is at least one of glass flake powder and boron glass powder, and the organic binder is thermosetting phenolic resin.
Further, the sub-white corundum is coated with nano carbon.
Further, the brown corundum and the sub-white corundum with the granularity of 0.15-1 mm are coated with nano carbon.
Further, the two brown corundum and sub-white corundum are coated with nano carbon.
Further, the two kinds of high bauxite chamotte, the two kinds of brown corundum and the sub-white corundum are all coated with nano carbon.
The preparation method of the low-carbon aluminum silicon carbide carbon brick containing the nano-carbon comprises the following steps:
1) crushing, finely grinding and screening the main raw materials according to the granularity requirement;
2) performing chemical vapor deposition on the surfaces of bauxite chamotte, brown fused alumina and sub-white fused alumina with different granularities to coat a nano carbon film, wherein the fixed carbon content of the nano carbon film is more than or equal to 90 percent, and the thickness of the nano carbon film is 20-200 nanometers; and collecting fine particle products in waste gas discharged by a chemical vapor deposition device in the preparation process of the carbon nano-film to obtain the required dispersible nano-carbon, wherein the particle size is 20-200 nanometers, and the content of fixed carbon is more than or equal to 80 percent;
3) weighing corresponding raw materials according to the raw material composition and weight percentage in claim 1, adding the organic binding agent and absolute ethyl alcohol into a stirring tank, and stirring and mixing for 10-15 minutes to obtain the organic binding agent which is uniformly diluted by the absolute ethyl alcohol;
4) adding the solid raw materials weighed in the step 3) into a wheel-grinding type mixer, carrying out wheel-grinding mixing for 10-15 minutes, adding the diluted organic binder, carrying out wheel-grinding mixing for 15-25 minutes, discharging, and standing for ageing for 8-15 hours to obtain a brick-making mixture;
5) adding the brick making mixture prepared in the step 4) into a mould, and preparing a green brick by adopting a combined type friction brick press through striking molding, wherein the striking molding pressure is 150-200 MPa, and the striking frequency is not lower than 12 times;
6) and naturally placing the formed green brick for 16-24 hours for forming, and then, putting the green brick into a drying kiln for heat treatment, wherein the curing temperature is 180-240 ℃, and the curing time is 18-24 hours, so that the required low-carbon magnesia carbon brick is prepared.
The preparation method comprises the following steps of coating a nano carbon film on the surface of fused magnesia by chemical vapor deposition, wherein the nano carbon film is prepared by adopting equipment disclosed by a powder rotating chemical vapor deposition device (application publication No. CN 103668112A) applied in Chinese patent, acetylene is used as a carbon source gas, the chemical vapor deposition temperature is 650-750 ℃, the deposition time is 0.5-5 hours, and the nano carbon film is coated on the surface of the fused magnesia by chemical vapor deposition, the fixed carbon content of the nano carbon film is more than or equal to 90%, and the thickness of the nano carbon film can be controlled within the range of 20-200 nanometers. And collecting fine particle products in waste gas discharged by a chemical vapor deposition device in the preparation process of the carbon nano-film to obtain the required dispersible nano-carbon, wherein the particle size or the thickness of the required dispersible nano-carbon is 20-200 nanometers, and the content of the fixed carbon is more than or equal to 80 percent. Under the chemical vapor deposition process conditions, the nano carbon film and the dispersible nano carbon are mainly amorphous carbon, contain a small amount of graphite crystal and can be soaked by a solvent.
Compared with the prior art, the invention has the following beneficial effects:
the low-carbon aluminum silicon carbide carbon brick of the invention improves the inoxidizability of the nano carbon, improves the infiltration and adsorption of the nano carbon film and the dispersible nano carbon on an organic binding agent, realizes the uniform dispersion of the nano carbon in the magnesia carbon brick, greatly reduces the size of carbon particles in the aluminum silicon carbide carbon brick by controlling the size of the nano carbon film and the dispersible nano carbon with the thickness of 20-200 nanometers through the application of the nano carbon film and the dispersible nano carbon coated on the surfaces of three raw material particles of non-complete, partial or complete high-alumina bauxite clinker, brown alumina and sub-white corundum, and the characteristic that the nano carbon film and the dispersible nano carbon are mainly amorphous carbon, contain a small amount of graphite crystal, can be infiltrated by a solvent, and the like, obviously improves the contact frequency of the refractory raw material of the aluminum silicon carbide carbon brick and the carbon particles, ensures the performance of the carbon particles under the condition of low carbon content, and in addition, through the introduction mode of the nano carbon coated on the surfaces, the method not only ensures the extremely high contact frequency and contact interface area of the refractory raw material of the aluminum silicon carbide carbon brick and carbon particles, but also realizes the high-efficiency compact composition of different types of raw materials and the optimized coupling of material performance, and improves the thermal shock resistance of the low-carbon aluminum silicon carbide carbon brick and further improves the comprehensive use performance of the low-carbon aluminum silicon carbide carbon brick by absorbing the thermal expansion and cold contraction deformation of nano-pores generated by the flexibility among nano-particles, the escape of volatile components of a binder resin and the control of a carbonization process on the basis of greatly reducing the carbon content of the aluminum silicon carbide carbon brick, reducing the thermal conductivity and reducing the heat loss on the surface of a molten iron tank, thereby achieving the comprehensive use effects of delaying the damage process of the low-carbon aluminum silicon carbide carbon brick, prolonging the service life of the molten iron tank, reducing the consumption cost of refractory materials, improving the turnover rate of the molten iron tank.
Aiming at the adverse effect of low carbonization on the thermal shock stability of the magnesia carbon brick, the invention further realizes the volatilization of an organic binder and the rapid discharge of cracking and deflation of the binder through the low-temperature melting and high-temperature carbonization shrinkage of the added polyvinyl alcohol explosion-proof fiber and the residual fine pores, prevents the formation of the microcracks of the heat treatment of the low-carbon aluminum silicon carbide carbon brick and enhances the heterogeneous toughening effect of the pores; the application performance of the low-carbon aluminum silicon carbide carbon brick is improved and the thermal shock stability is improved through the high strength, excellent high-temperature performance, good erosion resistance and drawing toughening effect of the added chopped carbon fibers, and the winding and agglomeration in the conventional stirring, mixing and dispersing process of the carbon fibers are avoided through the limitation of the length of the chopped carbon fibers, so that the uniform dispersion of the chopped carbon fibers is ensured. Through compounding of multiple reinforcing and toughening materials in the low-carbon aluminum silicon carbide carbon brick, the multiphase composite reinforcing and toughening effect of the low-carbon aluminum silicon carbide carbon brick is realized, the thermal shock stability of the low-carbon aluminum silicon carbide carbon brick is further improved, thermal shock cracks are prevented from being stripped and damaged, and the adverse influence of low-carbon on the thermal shock stability of the aluminum silicon carbide carbon brick is effectively overcome.
According to the invention, aiming at the microstructure characteristics of the nano carbon film and the dispersible nano carbon coated on the surface of the refractory raw material particles and the characteristics of good surface wettability and organic solvent adsorption, anhydrous alcohol is added into a commercially available organic binding agent for dilution in the preparation method, so that the problems of poor rheological property and difficult dispersion in the refractory raw material of the organic binding agent caused by the adsorption of the nano carbon film and the dispersible nano carbon on the solvent in the organic binding agent are avoided, and the dispersion uniformity of the organic binding agent in the material mixing process is ensured; through the control of the wheel milling mixing time of the solid raw materials of various specifications and types and the diluted organic binding agent added in the preparation method, the uniform mixing and dispersion of the organic binding agent in the solid raw material mixture are realized under the condition of realizing the uniform mixing of the solid raw materials, and the sufficient infiltration, permeation and adsorption of the binding agent on the surface of the solid raw material are realized through long-time standing and ageing, so that the high-efficiency exertion of the functions of the binding agent is realized, and the compactness and the bonding strength of the low-carbon aluminum silicon carbide carbon brick are improved. The green brick density is improved and the apparent porosity is reduced by limiting the molding pressure and the striking frequency in the preparation method; the formed green brick is naturally placed, so that further permeation, diffusion and homogenization of the binding agent and volatilization of the organic solvent are facilitated, and the defects caused by rapid volatilization of the organic solvent in the heat treatment process are avoided; the full solidification of organic bonding is ensured and the bonding strength of the low-carbon aluminum silicon carbide carbon brick is improved by limiting the heat treatment temperature and time in the green brick drying kiln in the preparation method.
By scientific and reasonable selection of the novel nano carbon source, raw material component proportion and optimization of the preparation method, the physical and chemical properties of the prepared low-carbon aluminum silicon carbide carbon brick are as follows: the total carbon content is less than or equal to 6 percent, and the volume density is 2.80-2.90 g/cm3The normal temperature flexural strength is more than 55MPa, the heat conductivity coefficient is less than or equal to 6.0 w/m.DEG.C, 1100 DEG.CThe water-cooling thermal shock stability times is more than or equal to 25, the oxidation resistance test is carried out under the air atmosphere of heat preservation for 1h at 1450 ℃, the thickness of the oxidation layer of the sample is less than or equal to 1.3mm, the slag resistance test is carried out under the carbon-buried atmosphere of heat preservation for 3h at 1500 ℃, and the slag erosion and penetration are not obvious. Therefore, the performance indexes of the low-carbon aluminum silicon carbide carbon brick are obviously superior to those of the conventional aluminum silicon carbide carbon brick.
Detailed Description
The present invention will be described in further detail with reference to specific examples and comparative examples to facilitate a clearer understanding of the present invention, but the present invention is not limited thereto.
Example 1
The raw materials of the low-carbon aluminum silicon carbide carbon brick containing the nano carbon comprise a main raw material and an auxiliary raw material, wherein the main raw material comprises the following components in percentage by weight:
the auxiliary raw materials comprise an organic binder, absolute ethyl alcohol, polyvinyl alcohol fibers and chopped carbon fibers, wherein the weight of the absolute ethyl alcohol accounts for 1% of the total weight of the main raw material, the weight of the organic binder accounts for 3% of the total weight of the main raw material, the weight of the polyvinyl alcohol fibers accounts for 0.05% of the total weight of the main raw material, and the weight of the chopped carbon fibers accounts for 0.2% of the total weight of the main raw material;
the preparation method comprises the following steps:
1) crushing, finely grinding and screening the main raw materials according to the granularity requirement;
2) the method comprises the steps of performing chemical vapor deposition coating of a nano carbon film on the surfaces of two high-alumina bauxite chamottes, two brown corundum and sub-white corundum, and performing chemical vapor deposition coating of the nano carbon film on the surface of fused magnesia by adopting equipment disclosed by a powder rotary chemical vapor deposition device (application publication No. CN 103668112A) in Chinese patent application, wherein acetylene is carbon source gas, the chemical vapor deposition temperature is 650-750 ℃, the deposition time is 0.5-5 hours, so that the preparation of the fused magnesia coated with the nano carbon film is completed, the fixed carbon content of the nano carbon film is more than or equal to 90%, and the thickness of the nano carbon film can be controlled within the range of 20-200 nanometers. Collecting fine particle products in waste gas discharged by a chemical vapor deposition device in the preparation process of the carbon nano-film to obtain the required dispersible nano-carbon, wherein the particle size or the thickness of the required dispersible nano-carbon is 20-200 nanometers, and the content of fixed carbon is more than or equal to 80 percent;
3) weighing corresponding raw materials according to the composition and weight percentage of the raw materials, adding the organic binding agent and absolute ethyl alcohol into a stirring tank, and stirring and mixing for 10 minutes to obtain the organic binding agent which is uniformly diluted by the absolute ethyl alcohol;
4) adding the solid raw materials weighed in the step 3) into a wheel-grinding type mixer, carrying out wheel-grinding mixing for 10 minutes, adding the diluted organic binder, carrying out wheel-grinding mixing for 25 minutes, discharging, and standing for ageing for 8 hours to obtain a brick-making mixture;
5) adding the brick making mixture prepared in the step 4) into a mould, and adopting a composite friction brick press to perform striking forming to prepare a green brick, wherein the striking forming pressure is 150MPa, and the striking frequency is not lower than 12 times;
6) and naturally placing the formed green brick for 16 hours for forming, and then, putting the green brick into a drying kiln for heat treatment, wherein the curing temperature is 180 ℃, and the curing time is 18 hours, so that the required low-carbon magnesia carbon brick is prepared.
Example 2
The same procedure as in example 1 was repeated, except that the two kinds of bauxite chamottes and the brown fused alumina raw material having a particle size of 1 to 3mm were not coated with a nanocarbon film.
Example 3
The procedure of example 1 was repeated, except that the surfaces of the two kinds of bauxite chamottes and the two kinds of brown fused alumina raw material particles were not coated with a nanocarbon film.
Example 4
The procedure of example 1 was repeated, except that the surfaces of the two types of raw bauxite chamotte particles were not coated with a nanocarbon film.
According to the embodiments 1-4, the prepared low-carbon aluminum silicon carbide carbon brick has the following physical and chemical properties: the total carbon content is less than or equal to 6 percent, and the volume density is 2.80-2.90 g/cm3Normal temperature bending strengthThe temperature is more than 55MPa, the heat conductivity coefficient is less than or equal to 6.0w/m DEG C, the water-cooling thermal shock stabilization frequency at 1100 ℃ is more than or equal to 25 times, the oxidation resistance experiment is carried out at 1450 ℃ under the air atmosphere with the heat preservation time of 1h, the thickness of the oxidation layer of the sample is less than or equal to 1.3mm, the slag resistance experiment is carried out at 1500 ℃ under the carbon-buried atmosphere with the heat preservation time of 3h, and the slag erosion and the penetration are not. Therefore, the performance indexes of the low-carbon aluminum silicon carbide carbon brick are obviously superior to those of the conventional aluminum silicon carbide carbon brick, the requirement of the hot metal ladle on severe use working conditions under the condition of high-proportion pretreatment of hot metal can be met, the use requirement of the KR desulfurization hot metal ladle with severe stirring and flushing can be met, and the purpose of prolonging the service life of the hot metal ladle can be achieved.
And with the increase of the total amount of the nano carbon film coating raw materials and the reduction of the addition amount of the dispersible nano carbon, the performance of the prepared low-carbon aluminum silicon carbide carbon brick is continuously improved, namely in the embodiments 1-4, with the increase of the sequence number of the embodiments, the performance of the low-carbon aluminum silicon carbide carbon brick is continuously reduced, and the performance of the embodiment 1 is optimal. Therefore, the improvement of the adding proportion of the nano carbon film coating raw materials is one of the key means for improving the low-carbon aluminum silicon carbide carbon brick; in addition, because the coating thickness of the nano carbon film is extremely thin, in order to reduce the amount of raw materials coated by the nano carbon film and reduce the coating cost of the nano carbon film, the use of the dispersible nano carbon is an important means for ensuring the reasonable carbon content in the low-carbon aluminum silicon carbide carbon brick; in addition, the compounding and the composite effect of various reinforcing and toughening materials are important measures for preventing the low-carbon aluminum silicon carbide carbon brick from being stripped and damaged by thermal shock.
Claims (10)
1. A low carbon aluminum silicon carbide carbon brick containing nano carbon is characterized in that: the raw materials of the low-carbon aluminum silicon carbide carbon brick containing the nano carbon comprise a main raw material and an auxiliary raw material, wherein the main raw material comprises the following components in percentage by weight:
the auxiliary raw materials comprise an organic binder, anhydrous alcohol, polyvinyl alcohol fibers and chopped carbon fibers, wherein the weight of the anhydrous alcohol accounts for 0-3% of the total weight of the main raw material, the weight of the organic binder accounts for 3-5% of the total weight of the main raw material, the weight of the polyvinyl alcohol fibers accounts for 0.05-0.15% of the total weight of the main raw material, and the weight of the chopped carbon fibers accounts for 0-0.2% of the total weight of the main raw material;
the two high-alumina bauxite chamottes, the two brown corundum and the sub-white corundum are arranged from small to large according to the granularity, at least one raw material is taken from small to large to coat a nano carbon film, the thickness of the nano carbon film is 20-200 nanometers, the fixed carbon content of the nano carbon film is more than or equal to 90 percent, the fixed carbon content of the dispersible nano carbon is more than or equal to 80 percent, and the total carbon content of the low-carbon aluminum silicon carbide carbon brick containing the nano carbon is less than or equal to 6 percent.
2. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: al in the high bauxite chamotte2O3The weight percentage content is more than or equal to 85 percent.
3. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: the melting point of the polyvinyl alcohol fiber is less than or equal to 90 ℃, and the water-soluble temperature is more than or equal to 55 ℃.
4. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: the diameter of the chopped fiber is 5-9 mu m, the length of the chopped fiber is 0.5-2.5 mm, and the carbon content is more than or equal to 95 wt%.
5. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: the sintering and mineralizing agent is at least one of glass flake powder and boron glass powder, and the organic binder is thermosetting phenolic resin.
6. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: and carrying out nano carbon coating on the sub-white corundum.
7. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: and performing nano carbon coating on the brown corundum and the sub-white corundum with the granularity of 0.15-1 mm.
8. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: and the two brown corundum and sub-white corundum are coated with nano carbon.
9. The nanocarbon-containing low carbon aluminum silicon carbide carbon brick according to claim 1, wherein: and the two high bauxite chamottes, the two brown corundum and the sub-white corundum are all coated with nano carbon.
10. A method for preparing the low-carbon aluminum silicon carbide carbon brick containing nano-carbon according to claim 1, which is characterized in that: the preparation method comprises the following steps:
1) crushing, finely grinding and screening the main raw materials according to the granularity requirement;
2) performing chemical vapor deposition on the surfaces of bauxite chamotte, brown fused alumina and sub-white fused alumina with different granularities to coat a nano carbon film, wherein the fixed carbon content of the nano carbon film is more than or equal to 90 percent, and the thickness of the nano carbon film is 20-200 nanometers; and collecting fine particle products in waste gas discharged by a chemical vapor deposition device in the preparation process of the carbon nano-film to obtain the required dispersible nano-carbon, wherein the particle size is 20-200 nanometers, and the content of fixed carbon is more than or equal to 80 percent;
3) weighing corresponding raw materials according to the raw material composition and weight percentage in claim 1, adding the organic binding agent and absolute ethyl alcohol into a stirring tank, and stirring and mixing for 10-15 minutes to obtain the organic binding agent which is uniformly diluted by the absolute ethyl alcohol;
4) adding the solid raw materials weighed in the step 3) into a wheel-grinding type mixer, carrying out wheel-grinding mixing for 10-15 minutes, adding the diluted organic binder, carrying out wheel-grinding mixing for 15-25 minutes, discharging, and standing for ageing for 8-15 hours to obtain a brick-making mixture;
5) adding the brick making mixture prepared in the step 4) into a mould, and preparing a green brick by adopting a combined type friction brick press through striking molding, wherein the striking molding pressure is 150-200 MPa, and the striking frequency is not lower than 12 times;
6) and naturally placing the formed green brick for 16-24 hours for forming, and then, putting the green brick into a drying kiln for heat treatment, wherein the curing temperature is 180-240 ℃, and the curing time is 18-24 hours, so that the required low-carbon magnesia carbon brick is prepared.
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