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WO1989001923A1 - Produits ceramiques en zircone partiellement stabilise a la magnesie et leur procede de production - Google Patents

Produits ceramiques en zircone partiellement stabilise a la magnesie et leur procede de production Download PDF

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Publication number
WO1989001923A1
WO1989001923A1 PCT/US1988/000709 US8800709W WO8901923A1 WO 1989001923 A1 WO1989001923 A1 WO 1989001923A1 US 8800709 W US8800709 W US 8800709W WO 8901923 A1 WO8901923 A1 WO 8901923A1
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WO
WIPO (PCT)
Prior art keywords
mixture
magnesium
temperature
ceramic
magnesium oxide
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/US1988/000709
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English (en)
Inventor
David G. Wirth
Jack D. Sibold
Brian Seegmiller
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Coors Porcelain Co
Original Assignee
Coors Porcelain Co
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from PCT/US1987/002176 external-priority patent/WO1988001723A1/fr
Application filed by Coors Porcelain Co filed Critical Coors Porcelain Co
Priority to BR888807674A priority Critical patent/BR8807674A/pt
Priority to CA000565217A priority patent/CA1313035C/fr
Publication of WO1989001923A1 publication Critical patent/WO1989001923A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • 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
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/64—Burning or sintering processes
    • 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
    • C04B35/486—Fine ceramics

Definitions

  • zirconias are known to be partially stabilized by calcia (U.S. Patent No. 4,067,745, issued January 10, 1978, to Garvie et al.), yttria (Canadian Patent No. 1,154,793, issued October 4, 1983, to Otagiri et al.), and magnesia (U.S. Patent No. 4,279,655, issued on July 21, 1981, to Garvie et al. and PCT Application No. PCT/AU83/00069, International Clar- cation No. WO 83/04247 filed on May 27, 1983, by Common ⁇ wealth Scientific and Industrial Research Organization) .
  • the methods described therein are directed to the controlled formation of a specified microstructure and are reported to produce ceramics having good thermal shock resistance and strength.
  • One method involves the use
  • PCT/AU83/00069 describes another method in which zirconias having a higher content of silica may be used
  • silica has been extracted and/or the need to use metal oxide additives for zirconias having a content of silica greater than 0.03 weight percent result in an expensive and time-consuming process. It would therefore to be advantageous to have a process for the preparation of
  • aging is used herein to refer to "isothermal hold” (i.e., maintaining a particular soak temperature for a period of time during the cooling
  • PCT Application No. PCT/AU83/00069 describes a process for making magnesia partially-stabilized zirconias using metal oxide additives.
  • This reference discloses the use of an isothermal hold to control the extent to which tetragonal precipitates are transformed in the cubic grain matrix. It also discloses that by controlling the transformation of tetragonal precipitates to the monoclinic form, the amount of grain matrix monoclinic zirconia in the final product can be controlled. Consequently, this reference teaches that an aging process is required when substantial tetragonal precipitates are desired in the final product. It would therefore be advantageous to have a process that eliminates the expensive and time-consuming aging step.
  • the present invention has advantageously been found to overcome the above-identified problems of the known processes.
  • the process of the present invention surprisingly produced stronger ceramics compared to a process using zirconia having a silica content of up to about 0.03 weight percent.
  • a further advantage of the present invention is the elimination of the aging step thought necessary to produce magnesia partially- stabilized zirconias having a metastable tetragonal phase microstructure within a cubic grain phase.
  • the present invention comprises a process for making a magnesia partially-stabilized zirconia ceramic which comprises the steps of: (1) forming a first mixture by combining zirconium dioxide powder, having a silica content of up to about 0.5 percent by weight, with a magnesium-containing component consisting of magnesium oxide, a magnesium oxide forming material or mixtures thereof, said magnesium component being present in an amount to provide a magnesium oxide content of about 2.6 to about 3.8 weight percent of said zirconia ceramic; (2) compacting said first mixture to form a compacted mixture; (3) heating the compacted mixture to a soak temperature in the range of about 1675°C and about 1800°C to form a sintered ceramic; (4) cooling the sintered ceramic continuously to a temperature in the range of about 800°C and 1400°C at a rate such that tetragonal precipitates are formed and substantially maintained in the tetragonal phase throughout a constant cooling period; and (5) further cooling said sintered ceramic to ambient temperature without aging to provide said zirconia
  • the instant invention involves a process for making magnesia partially- stabilized zirconia comprises the steps of: (1) forming a first mixture by mixing zirconium dioxide powder, having a silica content of up to about 0.5 weight percent , and a magnesium-containing component consisting of magnesium oxide, a magnesium oxide forming material or mixture thereof, said magnesium component being present in an amount to provide a magnesium oxide content from about 2.6 to about 3.8 weight percent of the zirconia ceramic material; (2) calcining said first mixture to form a calcined mixture; (3) compacting said calcined mixture to a desired shape to form a compacted mixture; (4) heating said compacted mixture to a soak temperature in the range of about 1675°C and about
  • the instant invention involves a process for making magnesia partially- stabilized zirconia comprises the steps of: (1) mixing zirconium dioxide powder, having a silica content of up to about 0.5 weight percent, and a magnesium-containing material consisting of magnesium oxide, a magnesium oxide forming material or mixtures thereof, said magnesium component being present in an amount to provide a magnesium oxide content from about 2.6 to about 3.8 weight percent of the zirconia ceramic material; (2) calcining said first mixture to form a calcined mixture; (3) milling said calcined mixture to form a milled mixture; (4) drying said milled mixture to form a dried mixture; (5) compacting said dried mixture to form a compacted mixture; (6) heating said compacted mixture to a soak temperature in the range of about 1675°C and about 1800°C to form a sintered ceramic; (7) cooling said sintered ceramic continuously to a temperature in the range of about 800°C to about 1400°C at a rate between about 200°C and about
  • magnesia partially- stabilized zirconia ceramics are provided by any of the processes described above having a flexural strength greater than about 350 MPa, a critical stress intensity factor greater than about 5 MPam 1 /2 f anc i a weibull modulus greater than about 10.
  • magnesia partially- stabilized zirconias can be made using zirconia having a higher silica content than previously thought possible without the use of metal oxide additives. It has also been found that surprisingly an aging step thought to be necessary to control the formation of the desired microstructure can be eliminated.
  • the present invention further relates to the production of magnesia partially-stabilized zirconia ceramics capable of being used for a variety of purposes, including, for example, hot metal extrusion dies, wire drawing capstans, paper machine foils, projectiles and wear-resistant and/or corrosion- resistant articles.
  • zirconium dioxide powder is combined with a magnesium-containing component which provides a magnesium oxide level of about 2.6 to about 3.8 weight percent of the final ceramic.
  • the zir ⁇ conium dioxide powder consists essentially of up to about 0.5 weight percent silica.
  • the process is particularly preferred with zirconium dioxide having a silica content of between about 0.05 weight percent and 0.35 weight percent.
  • the zirconium dioxide powder can further comprise up to about 40 weight percent hafnia.
  • the zirconium dioxide powder can also contain Ti0 2 , Fe 2 0 3 and S0 3 in amounts normally found in commercially available zirconium dioxide raw materials, e.g., up to about 0.2 weight percent Ti0 2 , up to about 0.06 weight percent Fe 2 0 3 , and up to about 0.3 weight percent S0 3 .
  • Magnesium- ⁇ ontaining materials useful as the magnesium component in the instant invention include magnesium oxide, a magnesium oxide forming material such as magnesium oxalate, magnesium acetate, magnesium hydroxide, magnesium carbonate, and mixtures of these materials either with or without magnesium oxide. The hydrates of any of these magnesium compounds can also be used.
  • extra silica- scavenging metal oxides having an affinity for silica are not added to the zirconium dioxide-magnesium mixture.
  • metal oxide or “metal oxides” are used herein to refer to materials which can react or interact with silica when heated and the terms specifically exclude magnesium oxide and magnesium oxide forming materials.
  • Such silica-scavenging metal oxides which are used in prior art processes include, for example, strontium oxide, barium oxide, rare earth oxides and mixtures thereof.
  • the zirconium dioxide powder and the magnesium- containing material are combined by methods commonly used in the art, such as with a ball-mill, a twin-cone blender, or a V-blender. These materials are normally combined at ambient temperature.
  • the resulting powder mixture can be calcined or milled directly. Calcination of the powder mixture is preferred for ease of handling the subsequent process steps and is accomplished at a temperature between about 800°C and about 1700°C, preferably between about 1000°C and about 1600°C, and more preferably about 1200°C and about 1500°C. As is known to those skilled in the ceramic art, the calcination time can be adjusted to ensure that the bulk of the powdered mixture will reach the desired calcination temperature. The calcination time is normally between about 4 and 12 hours, preferably about 6 to about 10, and more preferably about 8 hours.
  • Milling can be accomplished by conventional dry- milling or wet-milling processes, until the median particle size is preferably less than about 3.0 microns, and more preferably between about 1.2 and about 2.6 microns. If the mixture is wet-milled, water and standard commercially available deflocculants are added to the milling slurry to form a flowable, high-solids content slurry normally having less than about 90% solids. The deflocculants are added as necessary and in amounts sufficient to suspend particles and to lower the viscosity of the wet-milled mixture. Commercially available anti-foaming agents, commonly used for this purpose and known to those skilled in the art, are preferably added to the milling slurry to minimize foaming.
  • the dry-milled or wet-milled mixture can be transferred to a slurry tank.
  • binders in cera ⁇ mics include resins such as poly(vinyl butyral) , poly (ethylene glycol) , poly(ethylene oxide) , poly(vinyl alcohol) , methyl cellulose, vinyl acetate latex, para- finic hydrocarbons, poly(N, N* -ethylene-Bis- Stearamide) , polymeric quinoline, potato starch, aqueous acrylic emulsions, poly(ethylene glycol) resins of molecular weight from about 7,000 to about 20,000 and poly (ethylene oxide) resins of molecular weight from about 10,000 to about 300,000. Mixtures of such binders
  • the amount of binder needed depends on the method of formation and the particular binder used and can be readily determined by those skilled in the art. Ordinarily the level of binder is between about 0.1 and about 7 weight percent of the
  • the wet-milled mixture is subsequently dried.
  • a convenient method of drying is by spray drying. Commercially available devices generally known to those skilled in the art can be used to dry the mixture until
  • the moisture content is no greater than about 0.5 weight percent water.
  • the preferred particle size varies depending on the method of compaction. All screen designations given below are based on the Tyler Equivalent (TE) mesh sizes. For dry pressing, the
  • 20 particle distribution after drying is preferably in the range of about 20 percent less than TE 48 mesh and greater than TE .80 mesh, about 20 percent less than TE 200 mesh, with the remainder within this range.
  • the particle distribution is
  • the dried powder mixture can then be formed into a compact of the desired shape by standard commercial
  • the formed compact is then heated from ambient temperature at a rate of between about 25°C per hour and about 250°C per hour, preferably between about 50°C and about 100°C per hour, to a soak temperature of between about 1675°C and about 1800 o C, preferably between about
  • the soak temperature is maintained for between about 1 and about 10 hours, and preferably about 2 to 6 hours.
  • the preferred soak time depends on the size of the compact; i.e., for larger compacts, a longer soak time is preferred to ensure the formation of a substantially single phase cubic structure and to obtain the preferred density of above about 5.3 grams per cubic centimeter (g/cc) .
  • the sintered ceramic is then cooled without aging at a rate between about 200°C and about 1000°C per hour, preferably about 250°C to about 500°C per hour, to a . temperature between about 800°C and 1400°C, preferably » between about 800°C and about 1100°C.
  • This cooling rate can be accomplished at a more rapid cooling rate followed by a slower cooling rate to provide an average cooling rate within the above-stated ranges.
  • This cooling rate must be controlled to the stated preferred temperatures so that tetragonal phases precipitate and are maintained without substantially transforming into the monoclinic phase. If the compact is cooled too slowly from about 1720°C, it is presently believed that tetragonal phases transform to the monoclinic form resulting in loss of strength.
  • the compact is allowed to cool too rapidly, a weaker ceramic is produced because it is believed that the tetragonal precipitates are too. small to transform into the monoclinic phase upon applied stress.
  • the sintered ceramic is then cooled to ambient temperature without aging.
  • the cooling rate at this point has not been found to be critical. Any means known in the art can be used, including, for example, 5 furnace cooling, subjecting the sintered material to room temperature, or shutting off all rate-controlling instruments.
  • the term "without aging" is used herein to mean that the sintered ceramic is not subjected to an isothermal hold or an annealing process; i.e., the l ⁇ sintered ceramic is continuously cooled to ambient temperature and is not reheated to annealing conditions. Subsequent surface finishing can be performed if desired.
  • the present invention also relates to magnesia
  • a ceramic article was prepared using zirconium dioxide powder reported to contain 99 percent zirconium
  • hafnium dioxide 20 dioxide plus hafnium dioxide in which the hafnium dioxide accounted for approximately 2 weight percent of the total, about 0.2 weight percent Si0 2 , about 0.15 weight percent Ti0 2 , about 0.02 weight percent Fe 0 , and about 0.25 weight percent S0 3 .
  • the material was
  • the zirconium dioxide powder was mixed with reagent grade magnesium carbonate in proportions such that the effective magnesium oxide content upon firing comprised 3.0 weight percent of the mixture.
  • the mixed powders were calcined at about 1440°C for about 8 hours.
  • the calcined mixture was wet-milled to provided an average particle size of about 1.5 micrometer.
  • An organic binder was added to the wet-milled slurry in an amount of approximately 1.7 weight percent based upon the dry calcined mixture.
  • the binder consisted of a 20,000 molecular weight polyethy ⁇ lene glycol) resin.
  • the resulting slurry was spray dried to form a powder.
  • the resulting powder was isostatically pressed at about 20 kpsi to form a compact having the approximate dimensions of 0.25 inches (") x 0.125" x 2.0" and weighing about 5.91 grams.
  • the compact was then formed on a lathe to the desired shape.
  • the formed compact was fired by heating from ambient temperature at a rate of about 100°C per hour to about 1720°C. This temperature was maintained for approximately 4 hours after which the sintered article was cooled at an average rate of about 400°C per hour to 1000°C.
  • the sintered-article was then furnace cooled to room temperature and subsequently finished to the desired configuration by diamond grinding.
  • the resulting ceramic product exhibited a flexural strength of 610 MPa, a critical stress intensity factor of 11 MPam 1 /2 / an( i had a density factor of 5.77 g/cc.
  • EXAMPLE 2 A ceramic article was prepared using zirconium dioxide powder reported to contain 99 percent zirconium dioxide plus hafnium dioxide in which the hafnium dioxide accounted for approximately 2 weight percent of the total, about 0.2 weight percent Si0 , about 0.15 weight percent Ti0 2 , about 0.02 weight percent Fe 0 3 , and about 0.25 weight percent S0 3 . The material was also reported to have about 0.30 weight percent loss on ignition at 1400°C, a tamped bulk density of 2.4 g/cm 3 , an average particle size of 14 microns, and a specific surface area of between 2 and 4 m 2 /g.
  • the zirconium dioxide powder was mixed with reagent grade magnesium carbonate in proportions such that the effective magnesium oxide content of the final ceramic comprised 3.0 weight percent of the mixture.
  • the mixed powders were calcined at about 1440°C for about 8 hours.
  • the calcined mixture was wet-milled to provided median particle size of about 1.5 microns.
  • An organic binder was added to the wet-milled slurry in an amount of approximately 1.7 weight percent based upon the dry calcined mixture.
  • the binder consisted of a polyethy ⁇ lene glycol) resin of molecular weight between about 15,000 and about 20,000.
  • the resulting slurry was spray dried to form a powder.
  • the resulting powder was isostatically pressed at about 20 kpsi to form a compact having the approximate dimensions of 0.25" x 0.125" x 2.0" and weighing about 5.88 grams.
  • the compact was then formed on a lathe to the desired shape.
  • the formed compact was fired by heating from ambient temperature at a rate of about 100°C and about 150°C per hour to about 1720°C. This temperature was maintained for approximately 2 hours after which the sintered article was cooled at an average rate of about 400°C per hour to 1000°C. From room temperature the sintered article was reheated at a rate of about 100°C per hour to a soak temperature of 1100°C. This temperature was maintained for approximately 2 hours, after which the annealed article was cooled to room temperature.
  • the final cera ic material produced by this method exhibited a flexural strength of 365 MPa, a critical stress intensity factor of 7 MPam 1 / 2 and had a density factor of 5.74 g/cc.
  • a ceramic material was prepared in the same manner as Example 2, except that (1) about 0.25 weight percent
  • a ceramic material was prepared in the same manner as Example 2, except that the Si0 2 content of the zirconium dioxide powder was 0.01 weight percent.
  • the final ceramic material made by this method exhibited a flexural strength of 520 MPa and had a density of 5.55 g/cc.
  • a ceramic material was prepared in the same manner as Example 3 except that the sintered article was reheated from room temperature at a rate of about 100°C per hour to an aging temperature of 1100°C. This temperature was maintained for approximately 2 hours after which the aged article was cooled to room temperature.
  • the ceramic article exhibited a flexural strength of 410 MPa and had a density of 5.76 g/cc.
  • Example 2 shows the effect of an aging period on such properties
  • Example 3 describes the effect of adding a silica-scavenging metal oxide.
  • Example 4 surprisingly shows that use of a zirconium dioxide powder having a very low silica content produced worse results than use of a zirconium pqwder having a 0.2 weight percent silica.
  • Example 5 describes a process that uses a metal oxide additive and aging which also produced a weaker and less dense ceramic compared with the ceramic produced by the present invention.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Organic Chemistry (AREA)
  • Composite Materials (AREA)
  • Inorganic Chemistry (AREA)
  • Compositions Of Oxide Ceramics (AREA)

Abstract

Un procédé de production de produits céramiques en zircone partiellement stabilisé à la magnésie est décrit. Le procédé consiste à combiner du bioxyde de zirconium ayant une teneur en silice allant jusqu'à 0,5 % en poids avec un composant contenant du magnésium. Ce mélange est ensuite compacté, chauffé et refroidi à une vitesse contrôlée, sans vieillissement, pour former des produits céramiques en zircone.
PCT/US1988/000709 1987-08-31 1988-02-26 Produits ceramiques en zircone partiellement stabilise a la magnesie et leur procede de production Ceased WO1989001923A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
BR888807674A BR8807674A (pt) 1987-08-31 1988-02-26 Ceramicas de zirconia parcialmente estabilizada com magnesia e processo para fabricar as mesmas
CA000565217A CA1313035C (fr) 1987-08-31 1988-04-27 Ceramique de zircone partiellement stabilisee a la magnesie et procede de fabrication

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
PCT/US1987/002176 WO1988001723A1 (fr) 1986-09-03 1987-08-31 Projectile pour munitions en ceramique
FRPCT/US87/02176 1987-08-31

Publications (1)

Publication Number Publication Date
WO1989001923A1 true WO1989001923A1 (fr) 1989-03-09

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PCT/US1988/000709 Ceased WO1989001923A1 (fr) 1987-08-31 1988-02-26 Produits ceramiques en zircone partiellement stabilise a la magnesie et leur procede de production

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AU (1) AU1542388A (fr)
BR (1) BR8807674A (fr)
WO (1) WO1989001923A1 (fr)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5525559A (en) * 1993-02-13 1996-06-11 Tioxide Specialties Limited Preparation of mixed powders
WO1998008778A1 (fr) * 1996-08-29 1998-03-05 The University Of Queensland Materiaux ceramiques
US9193630B2 (en) 2009-12-24 2015-11-24 Saint-Gobain Centre De Recherches Et D'etudes Europeen Powder comprising stabilized zirconia granules and a binder having Tg of 25C or lower
US9309155B2 (en) 2009-12-24 2016-04-12 Saint-Gobain Centre De Recherches Et D'etudes Europeen Powder comprising ceramic granules and low Tg binder
CN115010172A (zh) * 2022-07-27 2022-09-06 郑州振中电熔新材料有限公司 一种抗热冲击镁锆陶瓷粉体及其制备方法
CN115894016A (zh) * 2022-12-14 2023-04-04 圣泉(扬州)新材料科技有限公司 一种氧化锆陶瓷制备方法

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1983004247A1 (fr) * 1982-06-01 1983-12-08 Commonwealth Scientific And Industrial Research Or Materiaux ceramiques de zircone et leur procede de fabrication
US4659680A (en) * 1984-08-20 1987-04-21 Corning Glass Works Stabilized zirconia bodies of improved toughness

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1983004247A1 (fr) * 1982-06-01 1983-12-08 Commonwealth Scientific And Industrial Research Or Materiaux ceramiques de zircone et leur procede de fabrication
US4659680A (en) * 1984-08-20 1987-04-21 Corning Glass Works Stabilized zirconia bodies of improved toughness

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5525559A (en) * 1993-02-13 1996-06-11 Tioxide Specialties Limited Preparation of mixed powders
WO1998008778A1 (fr) * 1996-08-29 1998-03-05 The University Of Queensland Materiaux ceramiques
US9193630B2 (en) 2009-12-24 2015-11-24 Saint-Gobain Centre De Recherches Et D'etudes Europeen Powder comprising stabilized zirconia granules and a binder having Tg of 25C or lower
US9309155B2 (en) 2009-12-24 2016-04-12 Saint-Gobain Centre De Recherches Et D'etudes Europeen Powder comprising ceramic granules and low Tg binder
EP2516352B1 (fr) * 2009-12-24 2019-02-20 Saint-Gobain Centre De Recherches Et D'etudes Europeen Poudre de granules de céramique
CN115010172A (zh) * 2022-07-27 2022-09-06 郑州振中电熔新材料有限公司 一种抗热冲击镁锆陶瓷粉体及其制备方法
CN115894016A (zh) * 2022-12-14 2023-04-04 圣泉(扬州)新材料科技有限公司 一种氧化锆陶瓷制备方法

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Publication number Publication date
BR8807674A (pt) 1990-08-07
AU1542388A (en) 1989-03-31

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