US20100210444A1 - Large refractory article and method for making - Google Patents

Large refractory article and method for making Download PDF

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Publication number
US20100210444A1
US20100210444A1 US12/704,897 US70489710A US2010210444A1 US 20100210444 A1 US20100210444 A1 US 20100210444A1 US 70489710 A US70489710 A US 70489710A US 2010210444 A1 US2010210444 A1 US 2010210444A1
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Prior art keywords
refractory
green
support plates
sintered
article
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US12/704,897
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Randy L. Rhoads
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Corning Inc
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Corning Inc
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Assigned to CORNING INCORPORATED reassignment CORNING INCORPORATED ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: RHOADS, RANDY L.
Publication of US20100210444A1 publication Critical patent/US20100210444A1/en
Priority to US13/363,589 priority patent/US9169162B2/en
Abandoned legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • 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
    • C04B35/48—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 zirconium or hafnium oxides, zirconates, zircon or hafnates
    • C04B35/481—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 zirconium or hafnium oxides, zirconates, zircon or hafnates containing silicon, e.g. zircon
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03B—MANUFACTURE, SHAPING, OR SUPPLEMENTARY PROCESSES
    • C03B17/00—Forming molten glass by flowing-out, pushing-out, extruding or drawing downwardly or laterally from forming slits or by overflowing over lips
    • C03B17/06—Forming glass sheets
    • C03B17/064—Forming glass sheets by the overflow downdraw fusion process; Isopipes therefor
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • 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
    • C04B35/447—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 phosphates, e.g. hydroxyapatite
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • 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
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
    • C04B2235/3225—Yttrium oxide or oxide-forming salts thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/74—Physical characteristics
    • C04B2235/77—Density
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/94—Products characterised by their shape
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/96—Properties of ceramic products, e.g. mechanical properties such as strength, toughness, wear resistance
    • C04B2235/9607—Thermal properties, e.g. thermal expansion coefficient
    • C04B2235/9623—Ceramic setters properties

Definitions

  • This invention is directed to a method of making a large refractory article, and in particular, large refractory blocks or forming bodies, such as an isopipe used in the manufacture of glass.
  • refractory articles e.g. blocks
  • These articles are typically formed by first forming a green refractory body, then heating, or firing, the green body to drive off any moisture, burn off organic binders that might be present, and densify the body by causing individual particles comprising the body to coalesce. This densification is accompanied by shrinking or contraction of the body, wherein the final sintered article is smaller than the original green body (e.g. the length of the article decreases).
  • the frictional forces between a small green body and the structure supporting the green body within the furnace or kiln are not so great that excessive stress is introduced into the body during the shrinkage of the body.
  • frictional forces can create large stress in the body.
  • the final sintered article is massive (e.g. having a mass in excess of 450 kg), and frictional forces can result in induced stresses that can fracture the body, either during the sintering, or later when the sintered article is used.
  • the ability to sinter the precursor green body is significantly compromised., i.e. there is a increasing tendency for the sintering to produce cracks in the body.
  • a large, sintered refractory article such as, for example, a monolithic (single piece) sintered refractory article.
  • a sintered refractory article comprising a mass greater than 450 kg, a porosity less than 20% and a length greater than 250 cm.
  • the sintered refractory article is an isostatically pressed refractory article.
  • the sintered refractory article is a monolithic article.
  • the refractory article has a porosity less than 15%.
  • the refractory article has a porosity less than 10%.
  • the mass in some instances can be greater than 1000 kg.
  • the refractory article may comprise a trough, and forming surfaces that converge at a root, such as an isopipe used in the manufacture of glass, and in particular glass sheet.
  • the refractory article may, for example, comprise zircon or xenotime.
  • a method of making a glass sheet comprising heating a batch material in a furnace to produce a molten glass, flowing the molten glass over converging forming surfaces of a refractory body to form the glass sheet (12) and wherein the refractory body has a mass greater than 450 kg and a length greater than 250 cm.
  • the mass of the refractory body may, for example, be greater than 1000 kg.
  • the refractory body may comprise zircon or xenotime, or a combination thereof.
  • a method of forming a sintered refractory article comprising positioning a green refractory body on a plurality of support plates separated by gaps, wherein the support plates are supported by a plurality of support members.
  • the green refractory body may comprise zirconium silicate for example, wherein the sintered refractory article comprises zircon.
  • the sintered refractory article may comprise xenotime.
  • a joint material is disposed in the gaps between adjacent support plates.
  • Each of the support members includes an arcuate upper surface having a constant radius of curvature and an arcuate lower surface also having a constant radius of curvature.
  • the radius of curvature of the arcuate upper surface is equal to the radius of curvature of the arcuate lower surface.
  • a radius of curvature of the upper and lower arcuate surfaces is preferably at least 30 cm.
  • a center of gravity of each support member is displaced from the support member center of rotation.
  • a layer of setter material is disposed between the green refractory body and the support plates. The green refractory body is then heated to form a sintered refractory article. During the heating the green refractory body contracts. This causes the support plates to translate in response to the green refractory body contraction, and the support members rotate in response to the translation of the support plates.
  • the method is particularly useful for the production of relatively large refractory bodies, such as those wherein the longest dimension of the sintered refractory article is at least about 250 cm and/or a mass of the sintered refractory article is at least about 450 kg.
  • a method of forming a sintered refractory article comprising positioning a green refractory body weighing at least 450 kg. on a plurality of support plates, wherein the support plates are supported by a plurality of support members and adjacent support plates are separated by gaps, each of the support members being a section of a cylinder.
  • the green refractory body may comprise zirconium silicate for example.
  • the green refractory body is next heated to form a sintered refractory article.
  • the green refractory body contracts, causing the support plates to translate in response to the contraction of the green refractory body and the support members to rotate in response to the translation of the support plates.
  • a method of forming a sintered refractory article comprising forming a green refractory body by isostatically pressing a powdered refractory material, positioning the green refractory body on a plurality of support plates in a furnace, wherein the support plates are supported by a plurality of support members and adjacent support plates are separated by gaps, each of the support members being a section of a cylinder.
  • the green refractory body is then heated to form a sintered refractory article.
  • the green refractory body contracts, causing the support plates to translate in response to the contraction of the green refractory body and the support members to rotate in response to the translation of the support plates.
  • the method is particularly effective when producing articles wherein the longest dimension of the sintered refractory article is at least about 250 cm and/or a mass of the sintered refractory article is at least about 450 kg.
  • the sintered refractory article has a mass greater than 1000 kg.
  • a radius of curvature of the upper and lower arcuate surfaces that comprise each support member is at least 30 cm.
  • a joint material may be disposed in the gaps between adjacent support plates.
  • a center of gravity of the support members is displaced from a center of rotation of the support members.
  • FIG. 1 is a cross sectional side view of an exemplary glass melting system in accordance with an embodiment of the present invention.
  • FIG. 2 is a cross sectional side view of an isopipe that may be used in the glass making system of FIG. 1 .
  • FIG. 3 is a cross sectional side view of an apparatus for sintering a large green refractory body to form a sintered refractory article
  • FIG. 4 is a perspective view of a support member.
  • FIG. 5 is a cross sectional view of the support member of FIG. 4 wherein the support member is a section of a cylinder.
  • FIG. 6 is a perspective view of two support members according to FIG. 4 supporting a support plate.
  • FIG. 7 is a cross sectional side view of a sintered refractory article after completion of the sintering process in the apparatus of FIG. 3 , showing the rotation of the supporting members.
  • green refractory body refers to an un-sintered refractory body.
  • a refractory material is an inorganic, non-metallic material that retains its strength at high temperature.
  • the refractory material may be crystalline, or partially crystalline, e.g. a ceramic material. Accordingly, refractory material as described herein exhibit chemical and physical properties that make the material applicable for structures, or as components of systems, that are exposed to a temperature of at least about 538° C.
  • a refractory body is a body formed from a refractory material. The refractory body may be green (un-sintered) or a sintered refractory article.
  • a green refractory body will be considered green, or un-sintered, until the sintering process has reached conclusion and the body becomes a sintered refractory article.
  • the sintering process may be considered complete when the body has reached a porosity (open or closed or a combination thereof) of equal to or less than about 10%. Completion of the sintering process may vary depending upon the final use of the article resulting from the sintering, and must be considered in the context thereof. Generally speaking, the sintering process is complete when the resultant refractory article has reached a density wherein the article capable of being used for its intended purpose, not including any post-sintering processes (e.g. milling, coating etc.) that does not include additional densification.
  • post-sintering processes e.g. milling, coating etc.
  • Refractory blocks may be manufactured that exhibit superior resistance to deformation during the glass making process, and can exhibit excellent corrosion resistance, depending on the refractory material or materials selected.
  • Glass manufacturing system 10 includes melting vessel 14 , fining vessel 16 , mixing vessel 18 , delivery vessel 20 and forming body 22 (e.g., isopipe 22 ).
  • Melting vessel 14 is where glass batch materials are introduced as shown by arrow 24 and melted to form molten glass 26 .
  • Fining vessel 16 is connected to the melting vessel by melting vessel to finer connecting tube 28 . Fining vessel 16 receives molten glass 26 from melting vessel 14 and removes bubbles from the molten glass.
  • Fining vessel 16 is connected to mixing vessel 18 by fining vessel to mixing vessel connecting tube 30 .
  • Mixing vessel 18 is connected to delivery vessel 20 by mixing vessel to delivery vessel connecting tube 32 .
  • Delivery vessel 20 delivers molten glass 26 through downcomer 33 into inlet 34 and on to forming body 22 (e.g., isopipe 22 ) which forms glass sheet 12 .
  • Forming body 22 comprises a suitable refractory material (e.g. zircon) and is described in greater detail below with respect to FIG. 2 .
  • Isopipe 22 includes trough 36 that receives molten glass 26 .
  • Molten glass 26 fills and overflows walls 38 of trough 36 and runs down as two separate streams along two converging sides 39 a and 39 b (on the backside of FIG. 2 and not shown) of the isopipe before fusing together at root 40 .
  • Root 40 is where the two sides 39 a and 39 b meet and where the two flows of molten glass flowing down the sides of the isopipe join before being drawn downward and cooled to form glass sheet 12 .
  • isopipe 22 and glass manufacturing system 10 can have different configurations and components other that those shown in FIGS. 1 and 2 and still be considered within the scope of the present invention
  • a suitable refractory material or mixture of materials are placed in a compliant bladder, for example a rubber bladder, having a predetermined shape.
  • the refractory materials are powdered.
  • the bladder may be vibrated as it is filled with the refractory powder to ensure a homogeneous distribution of powder in the bladder.
  • the refractory powder typically might include binders, and be produced, for instance, by forming a slurry of various metal oxides, a binder and a dispersant in water.
  • the refractory powder may, for instance, comprise zircon (zirconium silicate) or xenotime. The slurry may then be spray dried to produce a dry refractory power.
  • the bladder is sealed and placed into a container into which a fluid, such as water, can be injected at high pressure (pressures can be in excess of 1400 kg/cm 2 ).
  • a fluid such as water
  • the fluid surrounds the sealed bladder, and applies a uniform pressure against the surface of the bladder, thereby isostatically pressing the bladder and its contents.
  • the high pressure applied to the refractory powder within the bladder causes the refractory powder particles to adhere and form a porous rigid body having a predetermined shape.
  • the green body or green refractory body When the body has been isostatically pressed for a time sufficient to form a porous body capable of holding its shape under routine process handling (e.g. moving from one location to another), hereinafter the green body or green refractory body.
  • the green refractory body is removed from the bladder and heated for a time and at a temperature sufficient to burn off the binder and sinter the green body into a dense shape having a low porosity, for example, a porosity equal to or less than about 20%, preferably less than about 15% and more preferably less than about 10%.
  • the green refractory body may be heated, for example, in a furnace (e.g. kiln).
  • Isopipe lengths can exceed 250 cm in length, and the isopipe can have a mass of 450 kg or more.
  • very large isopipes can exceed a mass of 500 kg, 600 kg, 700 kg, 800 kg, or 900 kg. In some instances an isopipe can even exceed a mass of 1000 kg.
  • the shear size of such a large, and preferably monolithic (single piece), sintered refractory article presents challenges to its manufacture, not least of which is supporting the green refractory body during the firing or sintering process in such a way that shrinkage or contraction of the body is accommodated without incurring stresses in the body that may lead to cracking, either of the green refractory body, the finally sintered refractory article, or at any stage in between.
  • the following description will be directed to the manufacture of an isopipe as described above, with the understanding that the sintering methods disclosed may be used in the densification of any large refractory body without regard to its end use.
  • FIG. 3 Shown in FIG. 3 is a cross sectional view of an embodiment of an apparatus for supporting a large green refractory body 42 comprising a plurality of support members 44 , the plurality of support members supporting a plurality of support plates 46 .
  • Each support member includes an arcuate upper surface 48 and an arcuate lower surface 50 , best seen in FIGS. 4 and 5 .
  • the arcuate upper surface cross section is preferably an arc having a first radius of curvature r 1 .
  • the arcuate lower surface cross section of each support member is preferably an arc having a second radius of curvature r 2 .
  • the length of the upper surface arc is shorter than the length La 2 of the lower arcuate surface (e.g. the length of the lower surface arc), and the center of gravity G of the support member is closer to the lower arcuate surface than the center of rotation R of the support member.
  • Support members 44 may be arranged on floor 52 of sintering furnace 54 (e.g. kiln) in parallel rows, with the lower arcuate surface of each support member in contact with sintering furnace floor 52 .
  • Support plates 46 are arranged on top of support members 44 such that each support plate 46 is supported by at least two support members. In turn, each support plate 46 is separated from an adjacent support plate by gap 56 .
  • Each gap 56 may in turn be filled with a compliant material, hereinafter joint material 58 , capable of withstanding the sintering environment without significant degradation.
  • joint material 58 should be capable of accommodating a narrowing of the gap (or conversely a widening of the gap) between adjacent support plates, both as a result of the thermal expansion of the support plates during the sintering process, and movement of the support plates resulting from contraction of the green body during sintering.
  • the joint material may comprise fiber glass, an asbestos wool (although asbestos is not considered preferable due to its health hazards), or an asbestos replacement material that can be formed into a resilient gap filler.
  • a layer of setter material may optionally be deposited overtop the support plates 46 to produce a compliant bed 60 that resists damage to the green refractory body 42 (or resulting sintered refractory article), and helps to distribute the weight of the green refractory body on the support plates.
  • the setter material accommodates shrinkage of the green refractory body over the length of an individual support plate.
  • the setter material may be any suitable granular material, or grog, including, but not limited to silica, alumina, high duty fireclay, cordierite or zirconia.
  • the granules of the setter material are substantially spherical to promote sliding and thereby reduce friction between the green refractory body and the setter material during contraction of the green refractory body.
  • the support plates accommodate contraction of the un-sintered body over the plurality of support plates 46
  • the setter material when used, aids in accommodating contraction of the body over a single plate. The setter material is prevented from slipping through the gaps between adjacent support plates by the joint material.
  • the individual particles of the green refractory body reach a flow temperature.
  • the particles subsequently coalesce and the body becomes denser.
  • This density increase is accompanied by a shrinking (densification) of the green refractory body that is generally proportional to the dimension of interest of the body.
  • the amount of contraction along the length of the green refractory body is generally proportional to the length.
  • the body may contract by 30 cm or more at its extremes.
  • each end of the body moves 15 cm. toward the center of the body and the body overall contracts by a total of 30 cm.
  • Overall changes in length will vary depending, inter alia, on the material comprising the body and the degree of densification.
  • the support plates are pulled inward (the plates translate inward toward the center of the body). This inward movement is transmitted to the support members through the support plates, causing the support members to rotate toward the center of the body.
  • each support plate will translate inward toward the center of the body without undergoing a change in vertical displacement. More simply put, each support plate will move inward a certain distance according to its position along the length of the body, but will not change its vertical height above the floor of the furnace. Thus, the sintering body does not experience stress from uneven support plates (unevenness from one plate to another along the length of the body). This may be more easily understood if one envisions each support member as being a cylinder.
  • the support plate can be translated in a direction perpendicular to the length of the cylinder, with the cylinders rolling beneath the support plate. Because the radius of curvature of each cylinder is constant, the height of the support plate above the surface over which the cylinders roll, the height of the support plate above the supporting furnace floor does not change (unless the surface over which the cylinders roll changes height).
  • the support members may be cylinders, but extra care must be taken to prevent unwanted rotation of the support members (e.g. by placing a layer of setter material on the furnace floor).
  • the center of the body may, if desired, be supported by a stationary support, such as a pillar, table, or other suitable supporting structure that does not need to translate or rotate.
  • the furnace is heated to a temperature or temperatures suitable for sintering the body according to a heating schedule appropriate for the particular body.
  • the furnace may be cooled according to a predetermined cooling schedule, and the sintered refractory article removed from the furnace.
  • the sintered refractory article can have a mass of 500 kg, 600 kg, 700 kg, 800 kg, or 900 kg. In some instances the sintered refractory article can even exceed a mass of 1000 kg.
  • Post-sintering processing may be carried out according to the nature and use of the article.
  • additional machining of the article may be undertaken (drilling, grinding etc.) as necessary. Additional machining may be performed, for example, to produce a forming body (e.g. isopipe) for the manufacture of glass (e.g. glass sheet).
  • a forming body e.g. isopipe
  • glass e.g. glass sheet

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Structural Engineering (AREA)
  • Composite Materials (AREA)
  • Compositions Of Oxide Ceramics (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Furnace Housings, Linings, Walls, And Ceilings (AREA)
  • Furnace Charging Or Discharging (AREA)
US12/704,897 2009-02-19 2010-02-12 Large refractory article and method for making Abandoned US20100210444A1 (en)

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US13/363,589 US9169162B2 (en) 2009-02-19 2012-02-01 Large refractory article and method for making

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WO2012058194A1 (en) * 2010-10-29 2012-05-03 Corning Incorporated Large xenotime ceramic block and dry process for making the same
CN105330329A (zh) * 2015-11-23 2016-02-17 安徽农业大学 一种多孔杨木微结构的TiO2陶瓷
CN106116671A (zh) * 2016-06-27 2016-11-16 安徽梅兰园林景观工程有限公司 一种用于园林景观的节能砖及其制备方法
FR3038702A1 (fr) * 2015-07-06 2017-01-13 Snecma Outillage destine a supporter une preforme en poudre pendant un traitement thermique
FR3038703A1 (fr) * 2015-07-06 2017-01-13 Snecma Outillage destine a supporter une preforme en poudre pendant un traitement thermique
GB2544577A (en) * 2015-07-06 2017-05-24 Safran Aircraft Engines Tooling for use during heat treatment to support a preform made of powder
CN106892645A (zh) * 2017-01-10 2017-06-27 绍兴职业技术学院 一种彩色竹纤维煤矸石砖
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CN107141000A (zh) * 2017-06-03 2017-09-08 嘉兴新耐建材有限公司 一种抗结皮耐磨浇注料
CN107188564A (zh) * 2017-07-14 2017-09-22 陕西师范大学 一种高介电性能的Eu3+掺杂铌酸锶钙钠发光铁电陶瓷材料及其制备方法
CN107304125A (zh) * 2016-04-18 2017-10-31 宁夏有礼文化旅游产业有限公司 一种兼具瓷器和陶器优点的沙瓷及其制备方法
CN107488049A (zh) * 2017-08-21 2017-12-19 李楠 一种Al2O3‑SiO2质球形轻质耐火材料骨料
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CN107573091A (zh) * 2017-09-21 2018-01-12 李小兵 紫砂陶粒、紫砂陶粒的制备方法和应用及灌装酒
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