CN113045312A - High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof - Google Patents

High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof Download PDF

Info

Publication number
CN113045312A
CN113045312A CN202110306052.1A CN202110306052A CN113045312A CN 113045312 A CN113045312 A CN 113045312A CN 202110306052 A CN202110306052 A CN 202110306052A CN 113045312 A CN113045312 A CN 113045312A
Authority
CN
China
Prior art keywords
powder
thermal conductivity
yttrium
entropy
glass
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.)
Granted
Application number
CN202110306052.1A
Other languages
Chinese (zh)
Other versions
CN113045312B (en
Inventor
刘虎林
李慧贤
刘长青
薛云龙
伍媛婷
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.)
Shaanxi University of Science and Technology
Original Assignee
Shaanxi University of Science and Technology
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
Application filed by Shaanxi University of Science and Technology filed Critical Shaanxi University of Science and Technology
Priority to CN202110306052.1A priority Critical patent/CN113045312B/en
Publication of CN113045312A publication Critical patent/CN113045312A/en
Application granted granted Critical
Publication of CN113045312B publication Critical patent/CN113045312B/en
Active legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Images

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
    • C04B35/01—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
    • C04B35/49—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 also titanium oxides or titanates
    • 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
    • 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
    • C04B38/00—Porous mortars, concrete, artificial stone or ceramic ware; Preparation 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
    • C04B2235/02—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
    • C04B2235/02—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
    • C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3251—Niobium oxides, niobates, tantalum oxides, tantalates, 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
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/50—Constituents or additives of the starting mixture chosen for their shape or used because of their shape or their physical appearance
    • C04B2235/54—Particle size related information
    • C04B2235/5418—Particle size related information expressed by the size of the particles or aggregates thereof
    • C04B2235/5445—Particle size related information expressed by the size of the particles or aggregates thereof submicron sized, i.e. from 0,1 to 1 micron
    • 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
    • C04B2235/65—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/656—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes characterised by specific heating conditions during heat treatment
    • C04B2235/6562—Heating rate
    • 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
    • C04B2235/65—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/656—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes characterised by specific heating conditions during heat treatment
    • C04B2235/6565—Cooling rate
    • 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
    • C04B2235/65—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/656—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes characterised by specific heating conditions during heat treatment
    • C04B2235/6567—Treatment time
    • 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
    • C04B2235/76—Crystal structural characteristics, e.g. symmetry
    • 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
    • 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

Landscapes

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

Abstract

The invention discloses a high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and a preparation method thereof, wherein the preparation method comprises the following steps: 1) according to the mol content percentage, 33.9 to 43.5 percent of Y2O3Powder of 3.6-25.5 mol% ZrO2Powder, 3.6-25.5% HfO2Powder and 3.6 to 25.5 percent of TiO2Powder and 0-15.2% of Ta2O5Powder and 0-15.2% of Nb2O5Ball-milling and mixing 4-5 kinds of powder in the powder, drying, granulating, sieving and then carrying out compression molding on the mixed powder to obtain a green body; 2) putting the green body obtained in the step 1 into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1400-1650 ℃ at a heating rate of 3-10 ℃/min, preserving the heat for 0.5-3 h, and then cooling the green bodyCooling to 1000 ℃ at a cooling rate of 5-10 ℃/min, and cooling with a furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity. The ceramic prepared by the invention has the characteristics of compactness, high thermal conductivity and glass-like characteristic along with the temperature change relationship.

Description

High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof
Technical Field
The invention belongs to the technical field of ceramic materials, and particularly relates to a high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and a preparation method thereof.
Background
Thermal Barrier Coatings (TBCs) are one of the key technologies and materials in aircraft engines, and can effectively reduce the operating temperature of heated components and improve the Thermal efficiency of the engine. At present, the mainstream thermal barrier coating ceramic material, namely yttrium-stabilized zirconia ceramic (YSZ), has the defects of easy sintering resistance and easy phase change at high temperature and the like.
Therefore, the development of a novel thermal barrier coating ceramic material with excellent high-temperature performance is one of the research hotspots in the field of structural ceramics at present. Wherein the key property of such ceramic materials is low thermal conductivity, e.g. A2B2O7(A ═ La, Sm, Er, Eu, Nd, Gd, Y, Yb, etc.; B ═ Zr, Ti, Hf, Ce, etc.) type oxides have very low high temperature thermal conductivity due to complex crystal structure, large mass and radius of metallic elements; meanwhile, the oxide has the characteristics of high melting point, excellent chemical stability, large thermal expansion coefficient and the like, so that the oxide becomes an important candidate material for the thermal barrier coating.
A large number of researches show that the scattering effect of crystal lattices on phonons can be enhanced by utilizing the vacancy defects and the substitutional impurity defects formed by solid solution doping, and the method is one of effective ways for reducing the thermal conductivity of materials. And 4-5 elements are doped at or near the equimolar ratio to form a multi-principal-element compound (also called a high-entropy compound), so that the concentration of point defects can be increased to a greater extent, lattice distortion is caused, and the thermal conductivity of the material is greatly reduced. Therefore, in recent years, high entropy has become regulation A2B2O7A new approach of thermal conductivity of ceramic.
Chinese patent publication No. CN111908922A discloses a low-temperature synthesized rare earth hafnate high-entropy ceramic powder and a preparation method thereof, and the high-entropy (5RE hafnate structure) with pyrochlore structure is obtained by combining a combustion method and high-temperature heat treatment0.2)2Hf2O7Ceramic powder, wherein rare earth element RE is La, Ce, Nd, Pr, Sm, Eu.
Publication No. CN110272278A discloses pyrochlore type high-entropy ceramic powder for thermal barrier coating and a preparation method thereof, wherein the chemical formula of the high-entropy ceramic powder is RE2Zr2O7Wherein RE is 3-7 of rare earth elements Y, La, Pr, Nd, Sm, Eu and Gd; the ceramic body (the density is 70%) obtained by sintering the ceramic powder has the thermal conductivity of about 1 W.m < -1 > K < -1 >.
Published paper "z.zhao, et al., (La)0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7:A novel high-entropy ceramic with low thermal conductivity and sluggish grain growth rate,Journal of Materials Science&Technology,35(2019)2647-2651, "reports a pyrochlore-type high-entropy oxide ceramic having a room-temperature thermal conductivity of 0.76 W.m-1·K-1(ceramic compactness 96%).
In view of the foregoing, the above-developed A for thermal barrier coating2B2O7The type high-entropy pyrochlore oxides are A-site high-entropy materials, the related elements are rare earth metal elements, and the production cost is high.
Chinese patent publication No. CN111533557A discloses a pyrochlore type high-entropy oxide solidified body and a preparation method thereof, wherein RE is obtained by solid-phase reaction2M2O7The high-entropy oxide comprises 3-6 RE elements of Y, La, Nd, Sm, Eu and Gd, and 3-6 transition metal elements of Ti, Zr, Hf, Nb, Ta and Ce. The patent document A2B2O7Both the A site and the B site of the type oxide are subjected to high entropy treatment, but the thermal conductivity of the material is not regulated.
Therefore, in order to reduce the cost and expand the variety of oxide materials for thermal barrier coatings, B-site high-entropy A needs to be developed2B2O7The pyrochlore oxide is used for regulating and controlling the change characteristics of the thermal conductivity of the material along with the temperature.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide the high-entropy yttrium pyrochlore ceramic which has the advantages of simple process, reduced cost and expanded thermal barrier coating material types and has the glass-like thermal conductivity and the preparation method thereof.
In order to achieve the purpose, the invention adopts the technical scheme that:
a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity specifically comprises the following steps;
step 1: according to the mol content percentage, 33.9 to 43.5 percent of Y2O3Powder and ZrO with 3.6-25.5% mole content2Powder, 3.6-25.5% HfO2Powder and 3.6 to 25.5 percent of TiO2Powder and 0-15.2% of Ta2O5Powder and 0-15.2% of Nb2O5Ball-milling and mixing 4-5 kinds of powder in the powder, drying, granulating, sieving and then carrying out compression molding on the mixed powder to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, placing the alumina crucible into a muffle furnace, heating the green body from room temperature to 1400-1650 ℃ at a heating rate of 3-10 ℃/min, preserving heat for 0.5-3 h, then cooling the green body to 1000 ℃ at a cooling rate of 5-10 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
Further, Y in step 12O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5The average grain diameter of the powder is 0.1-1 μm, and the chemical purity is more than 98.0%.
Further, the ball milling mode in the step 1 is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 8-24 hours.
Further, the mixed powder in the step 1 is dried, granulated and then screened by a 200-mesh sieve to be subjected to bidirectional pressure compression molding, and the molding pressure is 30MPa to 100 MPa.
A high entropy yttrium-pyrochlore ceramic having a glass-like thermal conductivity, the high entropy yttrium is sinteredThe molecular formula of the chlorite ceramic is Y2(xMy)2O7Wherein M is 4-5 of Zr, Ti, Hf, Nb and Ta, x takes on the value of 4 or 5, and y takes on the value range of 5-35%.
Further, the high-entropy yttrium pyrochlore ceramic has room temperature thermal conductivity of less than 2.5 W.m-1·K-1And the heat conductivity does not decrease with the temperature at 25-1400 ℃.
Compared with the prior art, the invention has the beneficial effects that:
1) according to the invention, the transition metal elements Zr, Ti, Hf, Ta and Nb are doped and enter the crystal lattice to form the high-entropy yttrium pyrochlore oxide ceramic B, so that the rare earth metal elements in the prior art are replaced, the raw material cost is reduced, the manufacturing process is simple, and the composition range of the thermal barrier coating material is expanded.
2) The high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which is prepared by optimizing component design, has adjustable ceramic microstructure and density, the density is 60-98%, and the high-density ceramic has the room-temperature thermal conductivity lower than 2.5 W.m-1·K-1And the thermal conductivity does not decrease with the temperature at 25-1400 ℃, has the characteristic of glass-like thermal conductivity, has the thermal conductivity lower than that of a typical thermal barrier coating material, namely yttrium-stabilized zirconia ceramic, and can be used as a novel thermal barrier coating candidate material in the field of aerospace.
Drawings
FIG. 1 is an XRD spectrum of a high-entropy yttrium pyrochlore ceramic obtained in example 5 of the present invention;
FIG. 2 is an XRD spectrum of a high-entropy yttrium pyrochlore ceramic obtained in example 8 of the present invention;
FIG. 3 is an SEM spectrum of a high-entropy yttrium pyrochlore ceramic obtained in example 5 of the present invention;
FIG. 4 is a graph of thermal conductivity as a function of temperature for the high entropy yttrium pyrochlore ceramics obtained in examples 5 and 8 of the present invention.
Detailed Description
The present invention will be described in further detail with reference to the following examples, which are not intended to limit the invention thereto.
Example 1
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle diameter of 0.1 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 38.4 percent of Y according to the mol content percentage2O3Powder of ZrO in a proportion of 15.4 mol%2Powder, 15.4% HfO2Powder, 15.4% TiO2Powder, 7.7% Ta2O5Powder and 7.7% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 8 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 100MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1400 ℃ at a heating rate of 3 ℃/min, preserving heat for 3h, then cooling the green body to 1000 ℃ at a cooling rate of 5 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 35% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the ceramic by a laser thermal conductivity meter, wherein the room-temperature thermal conductivity of the material is 1.0 W.m-1·K-1。
Example 2
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle diameter of 0.1 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 38.4 percent of Y according to the mol content percentage2O3Powder of ZrO in a proportion of 15.4 mol%2Powder, 15.4% HfO2Powder, 15.4% TiO2Powder, 7.7% Ta2O5Powder and 7.7% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 10 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 100MPa to obtain a green body;
step 2: and (3) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1500 ℃ at a heating rate of 5 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 7 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 20% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the ceramic by a laser thermal conductivity meter, wherein the room-temperature thermal conductivity of the material is 1.4 W.m-1·K-1。
Example 3
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle diameter of 0.1 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 38.4 percent of Y according to the mol content percentage2O3Powder of ZrO in a proportion of 15.4 mol%2Powder, 15.4% HfO2Powder, 15.4% TiO2Powder, 7.7% Ta2O5Powder and 7.7% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is a wet roller typeBall milling is carried out, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 12 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 30MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1500 ℃ at a heating rate of 7 ℃/min, preserving heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 9 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 30% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the ceramic by a laser thermal conductivity meter, wherein the room-temperature thermal conductivity of the material is 1.1 W.m-1·K-1。
Example 4
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle diameter of 0.1 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 38.4 percent of Y according to the mol content percentage2O3Powder of ZrO in a proportion of 15.4 mol%2Powder, 15.4% HfO2Powder, 15.4% TiO2Powder, 7.7% Ta2O5Powder and 7.7% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 14 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 9 ℃/min, preserving heat for 0.5h, then cooling the green body to 1000 ℃ at a cooling rate of 10 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 30% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the ceramic by a laser thermal conductivity meter, wherein the room-temperature thermal conductivity of the material is 1.2 W.m-1·K-1。
Example 5
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 38.4 percent of Y according to the mol content percentage2O3Powder of ZrO in a proportion of 15.4 mol%2Powder, 15.4% HfO2Powder, 15.4% TiO2Powder, 7.7% Ta2O5Powder and 7.7% Nb2O5Ball milling and mixing the 4-5 powder in the powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 16 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (3) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 10 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 6 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity of 98% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), and performing laser heatingThe conductivity of the compact ceramics is measured by a conductivity meter, and the room temperature thermal conductivity of the material is 1.8 W.m-1·K-1。
Example 6
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 1 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 38.4 percent of Y according to the mol content percentage2O3Powder of ZrO in a proportion of 15.4 mol%2Powder, 15.4% HfO2Powder, 15.4% TiO2Powder, 7.7% Ta2O5Powder and 7.7% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 18 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 4 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 7 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 95% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 2.1 W.m-1·K-1。
Example 7
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: average particle diameters areY of 0.5 μm and chemical purity greater than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 38.4 percent of Y according to the mol content percentage2O3Powder of ZrO in a proportion of 15.4 mol%2Powder, 15.4% HfO2Powder, 15.4% TiO2Powder, 7.7% Ta2O5Powder and 7.7% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 20 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1650 ℃ at the heating rate of 6 ℃/min, preserving heat for 0.5h, then cooling the green body to 1000 ℃ at the cooling rate of 8 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 99% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, wherein the room-temperature thermal conductivity of the material is 2.0 W.m-1·K-1。
Example 8
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 36.3 percent of Y according to the mol content percentage2O3Powder of ZrO in a molar ratio of 18.2%2Powder, 18.2%HfO2Powder, 18.2% TiO2Powder, 9.1% Ta2O5Powder and 0% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 20 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 6 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 8 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity of 98% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 1.8 W.m-1·K-1。
Example 9
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 36.3 percent of Y according to the mol content percentage2O3Powder of ZrO in a molar ratio of 18.2%2Powder, 18.2% HfO2Powder, 18.2% TiO2Powder, 9.1% Ta2O5Powder and 0% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 24 hours; drying the mixed powder, granulating, sieving with 200 mesh sieve, pressurizing in two directions, and mixingCompression molding is carried out under the pressure of 50MPa to obtain a green body;
step 2: and (3) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 10 ℃/min, preserving heat for 3h, then cooling the green body to 1000 ℃ at a cooling rate of 8 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 97% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 1.9 W.m-1·K-1。
Example 10
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 43.5 percent of Y according to the mol content percentage2O3Powder of ZrO based on a molar content of 8.7%2Powder, 8.7% HfO2Powder, 8.7% TiO2Powder, 15.2% Ta2O5Powder and 15.2% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 20 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, placing the alumina crucible in a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 8 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 10 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity of 96% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 2.1 W.m-1·K-1。
Example 11
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 34.0 percent of Y according to the mol content percentage2O3Powder, 23.7% ZrO2Powder, 16.9% HfO2Powder, 23.7% TiO2Powder, 1.7% Ta2O5Powder and 0% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 9 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 4 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 6 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 97% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 2.1 W.m-1·K-1。
Example 12
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 36.3 percent of Y according to the mol content percentage2O3Powder of 3.6 mol% ZrO2Powder, 25.5% HfO2Powder, 25.5% TiO2Powder, 9.1% Ta2O5Powder and 0% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 11 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (3) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 10 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 9 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity of 96% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 2.0 W.m-1·K-1。
Example 13
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 37.7 percent of Y according to the mol content percentage2O3Powder of ZrO in a molar ratio of 18.9%2Powder, 15.1% HfO2Powder, 15.1% TiO2Powder, 0% Ta2O5Powder and 13.2% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 22 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 7 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 7 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 95% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 2.4 W.m-1·K-1。
Example 14
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 36.3 percent of Y according to the mol content percentage2O3Powder of ZrO in a molar ratio of 25.5%2Powder, 3.6% HfO2Powder, 25.5% TiO2Powder, 9.1% Ta2O5Powder and 0% Nb2O5Ball milling and mixing 4-5 kinds of powderCombining; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 24 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 9 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 9 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity of 96% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 2.1 W.m-1·K-1。
Example 15
The invention provides a preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, which comprises the following steps of;
step 1: taking Y with average particle size of 0.5 μm and chemical purity of more than 98.0%2O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5Powder, 33.9% of Y according to mol content percentage2O3Powder of ZrO in a molar ratio of 25.5%2Powder, 25.5% HfO2Powder, 3.6% TiO2Powder, 11.5% Ta2O5Powder and 0% Nb2O5Ball milling and mixing 4-5 kinds of powder; the ball milling mode is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 16 hours; drying and granulating the mixed powder, sieving the powder by a 200-mesh sieve, and performing two-way pressurization and compression molding under the pressure of 50MPa to obtain a green body;
step 2: and (3) putting the green body obtained in the step (1) into an alumina crucible, putting the alumina crucible into a muffle furnace, heating the green body from room temperature to 1600 ℃ at a heating rate of 10 ℃/min, preserving the heat for 2h, then cooling the green body to 1000 ℃ at a cooling rate of 6 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
And step 3: polishing the obtained high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity, measuring the porosity to be 97% by a drainage method, analyzing the phase structure by XRD (X-ray diffraction), analyzing the microstructure by SEM (scanning Electron microscope), measuring the thermal conductivity of the compact ceramic by a laser thermal conductivity meter, and measuring the thermal conductivity of the material at room temperature to be 1.9 W.m-1·K-1。
Experimental analysis shows that in examples 1-4, dense ceramics cannot be obtained due to low sintering temperature or short heat preservation time, and meanwhile, when the forming pressure is lower than 30MPa, the green density is too low, and when the forming pressure is higher than 100MPa, the green body is easy to crack.
In examples 5, 6, 8 and 9, ceramics with a density of more than 95% can be obtained. When the particle size of the initial raw material is larger, the grain size of the obtained high-entropy ceramic is larger; when the holding time is too long, the crystal grains are easy to grow abnormally.
In example 7, the material was easily reacted with the alumina crucible due to the excessively high sintering temperature.
The ceramics obtained in the examples 5, 6 and 10 are biphase high-entropy ceramics, the ceramics obtained in the examples 8, 9 and 11 to 14 are single-phase high-entropy ceramics, and the room-temperature thermal conductivity of the corresponding ceramics is 2.5 W.m-1·K-1The following.
FIGS. 1 and 2 are XRD patterns of the high-entropy yttrium pyrochlore ceramics obtained in examples 5 and 8, which show that the main phases in the materials are all high-entropy yttrium pyrochlore structures.
FIG. 3 is an SEM image of the high entropy yttrium pyrochlore ceramic of example 5 showing that the two phases of the material have different grain sizes.
FIG. 4 shows the high-entropy carbide powder with thermal conductivity curves of the compact high-entropy yttrium pyrochlore ceramics obtained in examples 5 and 8 along with the temperature, wherein the room-temperature thermal conductivities of the materials are all 1.8 W.m-1·K-1And has obvious glass-like thermal conductivity characteristics.
In conclusion, the high-entropy yttrium pyrochlore with glass-like thermal conductivity is prepared by optimizing component designThe ceramic has adjustable microstructure and density, the density is 60-98%, and the high-density ceramic has the room temperature thermal conductivity lower than 2.5 W.m-1·K-1And the thermal conductivity does not decrease with the temperature at 25-1400 ℃, has the obvious characteristic of glass-like thermal conductivity, has the thermal conductivity lower than that of a typical thermal barrier coating material, namely yttrium-stabilized zirconia ceramic, and can be used as a novel thermal barrier coating candidate material in the field of aerospace.

Claims (6)

1. A preparation method of high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity is characterized by comprising the following steps:
step 1: according to the mol content percentage, 33.9 to 43.5 percent of Y2O3Powder and ZrO with 3.6-25.5% mole content2Powder, 3.6-25.5% HfO2Powder and 3.6 to 25.5 percent of TiO2Powder and 0-15.2% of Ta2O5Powder and 0-15.2% of Nb2O5Ball-milling and mixing 4-5 kinds of powder in the powder, drying, granulating, sieving and then carrying out compression molding on the mixed powder to obtain a green body;
step 2: and (2) putting the green body obtained in the step (1) into an alumina crucible, placing the alumina crucible into a muffle furnace, heating the green body from room temperature to 1400-1650 ℃ at a heating rate of 3-10 ℃/min, preserving heat for 0.5-3 h, then cooling the green body to 1000 ℃ at a cooling rate of 5-10 ℃/min, and cooling the green body along with the furnace to obtain the high-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity.
2. A method of preparing a high entropy yttrium pyrochlore ceramic having a glass-like thermal conductivity according to claim 1 wherein: y described in step 12O3Powder, ZrO2Powder, HfO2Powder, TiO2Powder, Ta2O5Powder and Nb2O5The average grain diameter of the powder is 0.1-1 μm, and the chemical purity is more than 98.0%.
3. A method of preparing a high entropy yttrium pyrochlore ceramic having a glass-like thermal conductivity according to claim 1 wherein: the ball milling mode in the step 1 is wet roller ball milling, ethanol is used as a ball milling medium, yttrium-stabilized zirconia balls are used as milling balls, and the ball milling mixing time is 8-24 h.
4. A method of preparing a high entropy yttrium pyrochlore ceramic having a glass-like thermal conductivity according to claim 1 wherein: and (2) drying and granulating the mixed powder in the step (1), and then sieving the powder by a 200-mesh sieve for bidirectional pressure compression molding, wherein the molding pressure is 30-100 MPa.
5. A high entropy yttrium pyrochlore ceramic having a glass-like thermal conductivity and produced by the method of claim 1, wherein: the molecular formula of the high-entropy yttrium pyrochlore ceramic is Y2(xMy)2O7Wherein M is 4-5 of Zr, Ti, Hf, Nb and Ta, x takes on the value of 4 or 5, and y takes on the value range of 5-35%.
6. A high entropy yttrium pyrochlore ceramic having a glass-like thermal conductivity according to claim 5 wherein: the high-entropy yttrium pyrochlore ceramic has a room temperature thermal conductivity of less than 2.5 W.m-1·K-1And the heat conductivity does not decrease with the temperature at 25-1400 ℃.
CN202110306052.1A 2021-03-23 2021-03-23 High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof Active CN113045312B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202110306052.1A CN113045312B (en) 2021-03-23 2021-03-23 High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202110306052.1A CN113045312B (en) 2021-03-23 2021-03-23 High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof

Publications (2)

Publication Number Publication Date
CN113045312A true CN113045312A (en) 2021-06-29
CN113045312B CN113045312B (en) 2022-05-27

Family

ID=76514288

Family Applications (1)

Application Number Title Priority Date Filing Date
CN202110306052.1A Active CN113045312B (en) 2021-03-23 2021-03-23 High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof

Country Status (1)

Country Link
CN (1) CN113045312B (en)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113264769A (en) * 2021-07-08 2021-08-17 昆明理工大学 High-entropy stable rare earth tantalate/niobate ceramic and preparation method thereof
CN113354414A (en) * 2021-07-08 2021-09-07 昆明理工大学 Entropy-stabilized RE2O3-AO2-B2O5Oxide ceramic and preparation method thereof
CN114349501A (en) * 2022-01-28 2022-04-15 郑州轻工业大学 ZYTO system composite ceramic material and preparation method thereof
CN117229054A (en) * 2023-08-03 2023-12-15 广东省科学院新材料研究所 Sintering-resistant high-entropy ceramic thermal barrier coating powder material for plasma spraying physical vapor deposition and preparation method thereof
WO2024021527A1 (en) * 2022-07-29 2024-02-01 中国航发北京航空材料研究院 Lanthanum-gadolinium-samarium-based high-entropy thermal barrier coating and preparation method therefor
CN117684115A (en) * 2023-12-12 2024-03-12 杭钢金属陶瓷(安吉)有限公司 Multi-element high-entropy stable yttrium oxide thermal barrier coating material and preparation method thereof

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6258467B1 (en) * 2000-08-17 2001-07-10 Siemens Westinghouse Power Corporation Thermal barrier coating having high phase stability
US20170321559A1 (en) * 2016-05-09 2017-11-09 General Electric Company Thermal barrier system with bond coat barrier
US20200157692A1 (en) * 2017-03-20 2020-05-21 General Electric Company Articles for high temperature service
CN111533557A (en) * 2020-03-27 2020-08-14 东华大学 Pyrochlore type high-entropy oxide solidified body and preparation method thereof
CN111978087A (en) * 2019-05-22 2020-11-24 北京理工大学 Composite material and preparation method and application thereof

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6258467B1 (en) * 2000-08-17 2001-07-10 Siemens Westinghouse Power Corporation Thermal barrier coating having high phase stability
US20170321559A1 (en) * 2016-05-09 2017-11-09 General Electric Company Thermal barrier system with bond coat barrier
US20200157692A1 (en) * 2017-03-20 2020-05-21 General Electric Company Articles for high temperature service
CN111978087A (en) * 2019-05-22 2020-11-24 北京理工大学 Composite material and preparation method and application thereof
CN111533557A (en) * 2020-03-27 2020-08-14 东华大学 Pyrochlore type high-entropy oxide solidified body and preparation method thereof

Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113264769A (en) * 2021-07-08 2021-08-17 昆明理工大学 High-entropy stable rare earth tantalate/niobate ceramic and preparation method thereof
CN113354414A (en) * 2021-07-08 2021-09-07 昆明理工大学 Entropy-stabilized RE2O3-AO2-B2O5Oxide ceramic and preparation method thereof
CN113264769B (en) * 2021-07-08 2022-07-22 昆明理工大学 High-entropy stable rare earth tantalate/niobate ceramic and preparation method thereof
CN114349501A (en) * 2022-01-28 2022-04-15 郑州轻工业大学 ZYTO system composite ceramic material and preparation method thereof
CN114349501B (en) * 2022-01-28 2023-03-24 郑州轻工业大学 ZYTO system composite ceramic material and preparation method thereof
WO2024021527A1 (en) * 2022-07-29 2024-02-01 中国航发北京航空材料研究院 Lanthanum-gadolinium-samarium-based high-entropy thermal barrier coating and preparation method therefor
CN117229054A (en) * 2023-08-03 2023-12-15 广东省科学院新材料研究所 Sintering-resistant high-entropy ceramic thermal barrier coating powder material for plasma spraying physical vapor deposition and preparation method thereof
CN117684115A (en) * 2023-12-12 2024-03-12 杭钢金属陶瓷(安吉)有限公司 Multi-element high-entropy stable yttrium oxide thermal barrier coating material and preparation method thereof

Also Published As

Publication number Publication date
CN113045312B (en) 2022-05-27

Similar Documents

Publication Publication Date Title
CN113045312B (en) High-entropy yttrium pyrochlore ceramic with glass-like thermal conductivity and preparation method thereof
CN113023776B (en) Fluorite-structured high-entropy oxide powder for thermal barrier coating and preparation method thereof
Zhao et al. High-entropy (Y0. 2Nd0. 2Sm0. 2Eu0. 2Er0. 2) AlO3: A promising thermal/environmental barrier material for oxide/oxide composites
CN111763087B (en) Series of cubic fluorite type high-entropy cerium oxide nano-powder and preparation method thereof
Liu et al. Structural evolution and thermophysical properties of (SmxGd1− x) 2Zr2O7 (0≤ x≤ 1.0) ceramics
Jin et al. ZrO2-doped Y2O3 transparent ceramics via slip casting and vacuum sintering
CN112919908B (en) Novel perovskite structure high-entropy ceramic and preparation method thereof
CN110002871B (en) Two-phase rare earth tantalate ceramic and preparation method thereof
CN110606740A (en) High-entropy rare earth hafnate ceramic material and preparation method thereof
CN114478005B (en) Tetragonal phase thermal barrier coating material and preparation method thereof
Zhou et al. Fabrication and characterization of novel powder reconstitution derived nanostructured spherical La2 (Zr0. 75Ce0. 25) 2O7 feedstock for plasma spraying
CN113501543B (en) High-entropy rare earth zirconate nano aerogel and preparation method and application thereof
CN110002873B (en) Porous tantalate ceramic and preparation method thereof
CN114956818A (en) Low-thermal-conductivity high-entropy cerate ceramic material and preparation method thereof
Guedes-Silva et al. Effect of rare-earth oxides on properties of silicon nitride obtained by normal sintering and sinter-HIP
CN108439977B (en) High-temperature low-thermal-conductivity hafnium oxide-based thermal barrier coating material and preparation method thereof
CN114751744A (en) Ceric acid rare earth based high-entropy ceramic material and preparation method thereof
JP7328484B2 (en) High thermal expansion coefficient orthophosphate thermal barrier coating material and its production method
Zhou et al. Fabrication and luminescent properties of Nd3+‐doped Lu2O3 transparent ceramics by pressureless sintering
Iyasara et al. La and Sm co-doped SrTiO3-δ thermoelectric ceramics
CN108939944B (en) Non-metal ion doped perovskite type mixed conductor hydrogen permeation membrane and preparation method and application thereof
Kim et al. Effect of ZnO and TiO2 doping on the sintering behavior of Y2O3 ceramics
CN116903368A (en) Multielement co-doped yttrium aluminum garnet Dan Rezhang coating material and preparation method thereof
CN115010491B (en) High-entropy rare earth tantalate ceramic material and preparation method thereof
JP2011020902A (en) Strontium titanate sintered compact and method for producing the same

Legal Events

Date Code Title Description
PB01 Publication
PB01 Publication
SE01 Entry into force of request for substantive examination
SE01 Entry into force of request for substantive examination
GR01 Patent grant
GR01 Patent grant