CN113562765A - Preparation of high-entropy rare earth tantalate RETaO by molten salt method4Method for preparing spherical powder - Google Patents
Preparation of high-entropy rare earth tantalate RETaO by molten salt method4Method for preparing spherical powder Download PDFInfo
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- 150000003839 salts Chemical class 0.000 title claims abstract description 63
- 239000000843 powder Substances 0.000 title claims abstract description 54
- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 40
- 150000002910 rare earth metals Chemical class 0.000 title claims abstract description 37
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- 238000000034 method Methods 0.000 claims abstract description 47
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims abstract description 28
- 238000001354 calcination Methods 0.000 claims abstract description 28
- 238000007873 sieving Methods 0.000 claims abstract description 21
- 238000001035 drying Methods 0.000 claims abstract description 18
- 239000002245 particle Substances 0.000 claims abstract description 17
- 238000000498 ball milling Methods 0.000 claims abstract description 15
- 239000011780 sodium chloride Substances 0.000 claims abstract description 14
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims abstract description 10
- 238000001816 cooling Methods 0.000 claims abstract description 7
- 238000001914 filtration Methods 0.000 claims abstract description 5
- 230000008569 process Effects 0.000 claims abstract description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 3
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 3
- 238000004140 cleaning Methods 0.000 claims abstract description 3
- 229910052747 lanthanoid Inorganic materials 0.000 claims abstract description 3
- 150000002602 lanthanoids Chemical class 0.000 claims abstract description 3
- 229910052727 yttrium Inorganic materials 0.000 claims abstract description 3
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims abstract description 3
- 239000002994 raw material Substances 0.000 claims description 42
- 238000005303 weighing Methods 0.000 claims description 12
- 238000010438 heat treatment Methods 0.000 claims description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- 229910001404 rare earth metal oxide Inorganic materials 0.000 claims description 5
- FKTOIHSPIPYAPE-UHFFFAOYSA-N samarium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Sm+3].[Sm+3] FKTOIHSPIPYAPE-UHFFFAOYSA-N 0.000 claims description 5
- RSEIMSPAXMNYFJ-UHFFFAOYSA-N europium(III) oxide Inorganic materials O=[Eu]O[Eu]=O RSEIMSPAXMNYFJ-UHFFFAOYSA-N 0.000 claims description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 3
- 229910000421 cerium(III) oxide Inorganic materials 0.000 claims description 3
- 229910052593 corundum Inorganic materials 0.000 claims description 3
- NLQFUUYNQFMIJW-UHFFFAOYSA-N dysprosium(III) oxide Inorganic materials O=[Dy]O[Dy]=O NLQFUUYNQFMIJW-UHFFFAOYSA-N 0.000 claims description 3
- VQCBHWLJZDBHOS-UHFFFAOYSA-N erbium(III) oxide Inorganic materials O=[Er]O[Er]=O VQCBHWLJZDBHOS-UHFFFAOYSA-N 0.000 claims description 3
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 claims description 3
- PLDDOISOJJCEMH-UHFFFAOYSA-N neodymium oxide Inorganic materials [O-2].[O-2].[O-2].[Nd+3].[Nd+3] PLDDOISOJJCEMH-UHFFFAOYSA-N 0.000 claims description 3
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 3
- FIXNOXLJNSSSLJ-UHFFFAOYSA-N ytterbium(III) oxide Inorganic materials O=[Yb]O[Yb]=O FIXNOXLJNSSSLJ-UHFFFAOYSA-N 0.000 claims description 3
- JYTUFVYWTIKZGR-UHFFFAOYSA-N holmium oxide Inorganic materials [O][Ho]O[Ho][O] JYTUFVYWTIKZGR-UHFFFAOYSA-N 0.000 claims description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 2
- 229910003443 lutetium oxide Inorganic materials 0.000 claims description 2
- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 claims description 2
- 239000007858 starting material Substances 0.000 claims description 2
- ZIKATJAYWZUJPY-UHFFFAOYSA-N thulium (III) oxide Inorganic materials [O-2].[O-2].[O-2].[Tm+3].[Tm+3] ZIKATJAYWZUJPY-UHFFFAOYSA-N 0.000 claims description 2
- 230000015572 biosynthetic process Effects 0.000 abstract description 3
- 238000002156 mixing Methods 0.000 abstract description 3
- 238000003786 synthesis reaction Methods 0.000 abstract description 3
- 239000013078 crystal Substances 0.000 abstract description 2
- 239000000203 mixture Substances 0.000 abstract 3
- 238000005054 agglomeration Methods 0.000 abstract 1
- 230000002776 aggregation Effects 0.000 abstract 1
- 239000006185 dispersion Substances 0.000 abstract 1
- 239000001103 potassium chloride Substances 0.000 abstract 1
- 230000035484 reaction time Effects 0.000 abstract 1
- 230000000694 effects Effects 0.000 description 8
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 description 8
- 239000000047 product Substances 0.000 description 7
- 238000012360 testing method Methods 0.000 description 6
- 239000012720 thermal barrier coating Substances 0.000 description 6
- 101710134784 Agnoprotein Proteins 0.000 description 4
- 239000000919 ceramic Substances 0.000 description 4
- 239000003153 chemical reaction reagent Substances 0.000 description 4
- 239000008367 deionised water Substances 0.000 description 4
- 229910021641 deionized water Inorganic materials 0.000 description 4
- 239000000706 filtrate Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 229910001961 silver nitrate Inorganic materials 0.000 description 4
- 238000005406 washing Methods 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 4
- 150000003841 chloride salts Chemical class 0.000 description 3
- 238000005245 sintering Methods 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- 230000008859 change Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000005469 granulation Methods 0.000 description 1
- 230000003179 granulation Effects 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000013589 supplement Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G35/00—Compounds of tantalum
- C01G35/006—Compounds containing, besides tantalum, two or more other elements, with the exception of oxygen or hydrogen
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/01—Particle morphology depicted by an image
- C01P2004/03—Particle morphology depicted by an image obtained by SEM
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/30—Particle morphology extending in three dimensions
- C01P2004/32—Spheres
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Compounds Of Alkaline-Earth Elements, Aluminum Or Rare-Earth Metals (AREA)
- Manufacture Of Metal Powder And Suspensions Thereof (AREA)
Abstract
The invention discloses a method for preparing high-entropy rare earth tantalate RETaO by a molten salt growth method4The method of spherical powder, wherein RE is at least one of yttrium, aluminum and lanthanide rare earth elements. The preparation method of the rare earth tantalate spherical powder comprises the following steps of2O3And Ta2O5Mixing the mixture with equimolar mixture, adding the mixture and KCl and NaCl mixed molten salt into a ball mill for ball milling, drying, sieving, calcining, cooling, cleaning, filtering, drying for the second time, and sieving to obtain the finished product. The method has the advantages of low synthesis temperature, short reaction time, simple process, high purity of synthesized products, high sphericity rate, good fluidity, controllable crystal form and morphology of powder particles, no agglomeration, easy dispersion and the like.
Description
1.1.1 technical field
The invention relates to the technical field of ceramic powder preparation,in particular to a method for preparing high-entropy rare earth tantalate RETaO by a molten salt growth method4A method for preparing spherical powder.
1.1.2 background Art
In recent years, "high entropy" has become a hot direction in the field of material research, i.e., the development of new materials with superior properties by introducing structural entropy. Based on four high entropy effects: (1) the thermodynamic high entropy effect; (2) the effect of lattice distortion; (3) a hysteresis diffusion effect; (4) the 'mixing effect' of the multi-principal element shows excellent properties such as high strength, high toughness, corrosion resistance, wear resistance, excellent thermal property, excellent electrical property and the like, so that the 'high entropy' can obviously improve the comprehensive properties of the material.
The high-entropy ceramics have the advantages of high melting point, high hardness, high toughness, low thermal conductivity, corrosion resistance and the like, and show great development potential in the field of Thermal Barrier Coatings (TBCs). Wang et al use the high entropy Effect on RETaO4The comprehensive performance of the ceramics is optimized, and the (5 RE) is systematically researched0.2)TaO4The phase structure, the ferroelastic toughening mechanism, the thermal property and the mechanical property of the (5 RE)0.2)TaO4Has great application potential in TBCs. Tangan powder and the like are used for preparing yttria-stabilized zirconia (YSZ) hollow sphere powder serving as a thermal barrier coating material, and the comprehensive performance of the yttria-stabilized zirconia (YSZ) hollow sphere powder is improved to a certain extent. The preparation of rare earth tantalate thermal barrier coating powders is a very critical step in the preparation of TBCs, and its quality directly affects the performance of the coating. Chinese patent CN109627000A discloses a rare earth tantalum/niobate (RETa/NbO)4) The ceramic powder and the preparation method thereof have the problems of low powder purity, high synthesis temperature, loss in the centrifugal spray granulation process and the like in the calcination process.
1.1.3 summary of the invention
In view of the above, the invention aims to provide a molten salt method for preparing high-entropy rare earth tantalate RETaO4Method for preparing rare earth tantalate RETaO with high purity, high sphericity and good fluidity from spherical powder4Spherical powder.
In order to achieve the purpose, the invention provides the following technical scheme:
1. preparation of high-entropy rare earth tantalate RETaO by molten salt method4The method for preparing spherical powder is characterized by comprising the following steps:
(1) weighing raw materials and molten salt, taking absolute ethyl alcohol as a medium, and carrying out ball milling uniformly in a ball mill;
(2) drying and sieving the product obtained in the step (1), and then heating and calcining;
(3) cooling and cleaning the product obtained in the step (2);
(4) filtering, secondary drying and sieving the powder washed in the step (3) to obtain the powder;
the rare earth tantalate RETaO4In the formula (II), RE is at least one of yttrium, aluminum and lanthanide rare earth elements.
The raw material is RE2O3And Ta2O5Said RE2O3Is Y2O3、Al2O3、La2O3、Ce2O3、Nd2O3、Pm2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、Dy2O3、Ho2O3、Er2O3、Tm2O3、Yb2O3、Lu2O3At least one of;
the molten salt is a mixed salt of KCl and NaCl.
Preferred in the present invention, the raw material RE in the step (1)2O3And Ta2O5In a molar ratio of 1: 1, purity of the starting Material>99.99 percent and the grain diameter is 1-80 mu m.
In the invention, preferably, in the step (1), the purity of the molten salt is more than 99.99%, the particle size is 1-80 μm, and the mass ratio of KCl to NaCl is (1-5): (1-2), the mass ratio of the raw materials to the molten salt is (1-2): (1-7).
Further preferably, in the invention, the mass ratio of the molten salt KCl to NaCl in the step (1) is optimized to be 5:1, optimizing the mass ratio of the raw materials to the molten salt to be 1: 6.
in the invention, the rotation speed of the ball milling in the step (1) is preferably 350r/min, and the ball milling time is preferably 12 h.
In the present invention, preferably, the drying in step (2) is drying at 90 ℃ for 24 hours, and the sieving is 400-mesh sieving.
In the invention, preferably, the calcining temperature in the step (2) is 600-1200 ℃, the time is 4-8h, and the heating rate is 5-10 ℃/min.
In the present invention, it is further preferred that the calcination temperature in step (2) is 800 ℃ and the calcination time is 6 hours.
In the invention, preferably, the drying in the step (4) is drying at 90 ℃ for 24 hours, and the sieving is performed by sieving with a 100-mesh sieve and then sieving with a 400-mesh sieve.
2. High-entropy rare earth tantalate RETaO prepared by the method4Spherical powder.
The invention has the beneficial effects that:
1. rare earth tantalate synthesized by molten salt method4The spherical powder has high purity and low synthesis temperature.
2. The method can control the morphology and the particle size of the powder by controlling the proportion of the molten salt to the raw material, the molten salt components, the calcination temperature and the calcination time, and obtain the rare earth tantalate RETaO with high sphericity rate and good fluidity4Spherical powder.
3. The rare earth tantalate RETaO prepared by the invention4The spherical powder has the characteristics of uniform particle size, excellent performance, stable quality, strong controllability, suitability for industrial production and the like.
1.1.4 description of the drawings
In order to make the object, technical scheme and beneficial effect of the invention more clear, the invention provides the following drawings for explanation:
FIG. 1 shows the preparation of (Y) by the molten salt method in example 10.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4An XRD pattern of (a);
FIG. 2 shows the preparation of (Y) by the molten salt method in example 10.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4SEM spectrum of (d).
1.1.5 detailed description
The present invention is further described with reference to the following drawings and specific examples so that those skilled in the art can better understand the present invention and can practice the present invention, but the examples are not intended to limit the present invention.
Example 1
In this example, a molten salt method is used to prepare high-entropy rare earth tantalate (Y)0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4The method for preparing the spherical powder comprises the following steps:
according to 1/5: 1/5: 1/5: 1/5: 1/5: 1 molar ratio of Y2O3、Ce2O3、Sm2O3、Gd2O3、Dy2O3And Ta2O5Total 5kg, purity of raw material and molten salt>99.99%, the particle diameter is 1-80 μm, and the ratio of (1-5): (1-2) weighing a mixed salt of KCl and NaCl according to the proportion shown in Table 1, and mixing the KCl and NaCl according to the proportion of 1: 3, weighing raw materials and molten salt, pouring the raw materials and the molten salt into a ball milling tank, and ball milling the raw materials for 12 hours (350r/min) in a planetary ball mill by using absolute ethyl alcohol as a medium, wherein the chemical reaction formula of the raw materials is as follows: RE2O3+Ta2O5＝2RETaO4. Drying the reacted product at 90 deg.C for 24 hr, sieving with 400 mesh sieve, calcining in resistance furnace at 1000 deg.C and 6 hr respectively at a heating rate of 5 deg.C/min, cooling with the furnace after calcination, taking out the powder when the temperature is reduced to room temperature, repeatedly washing the obtained product with heated deionized water for several times to remove excessive chloride salt until silver nitrate (AgNO) is used3) Reagent test filtrate does not contain Cl-Filtering the washed powder, drying at 90 ℃ for 24 hours, sieving with a 100-mesh sieve, sieving with a 400-mesh sieve, testing the particle size of the powder by using a laser particle sizer, testing the flowability by using a Hall flow meter, observing the morphology of the powder particles by using a scanning electron microscope, and calculating the sphericity ratio.
FIG. 1 is an XRD pattern of high-entropy rare earth tantalate synthesized by molten salt method, which is compared with a single-phase PDF standard card, GdTaO4(PDF: 24-0441) and DyTaO4(PDF: 12-0379) PeakHas a slight shift in the position of (A), which is a shift in the peak due to the lattice distortion of the crystal structure caused by the high entropy effect, the increase in the defect concentration, etc., and the high entropy rare earth tantalate (Y) is found by comparison with a single phase standard card0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4The purity is high. As shown in FIG. 2, the observation (Y) was carried out by a Scanning Electron Microscope (SEM)0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4The microscopic morphology and sphericity ratio of the spherical powder show that the particle size is 40-90 μm, and the sphericity ratio>99%, it is clear from Table 1 that KCl and NaCl in a ratio of 5:1 have a good sphericity ratio and fluidity.
TABLE 1 ratio of KCl and NaCl in molten salt to rare earth tantalate (Y)0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4Relationship between sphericity and fluidity
Example 2
In this example, a molten salt method is used to prepare high-entropy rare earth tantalate (Lu)1/3Pm1/3Eu1/3)TaO4The method for preparing the spherical powder comprises the following steps:
according to 1/3: 1/3: 1/3: weighing Lu at a molar ratio of 12O3、Pm2O3、Eu2O3And Ta2O55kg in total, according to the weight ratio of 5:1 proportion weighing KCl and NaCl mixed salt, raw material and molten salt purity>99.99%, the particle size is 1-80 μm, and the mass ratio (1-2): (2-7) weighing raw materials and molten salt, pouring the raw materials and the molten salt into a ball milling tank, as shown in Table 2, ball milling the raw materials and the molten salt for 12 hours (350r/min) in a planetary ball mill by using absolute ethyl alcohol as a medium, drying the raw materials at 90 ℃ for 24 hours, sieving the raw materials by using a 400-mesh sieve, then placing the raw materials into a resistance furnace for calcination, wherein the calcination temperature and the calcination time are 900 ℃ and 6 hours respectively, the heating rate is 5 ℃/min, cooling the raw materials with the furnace after the calcination is finished, taking out powder after the temperature is reduced to the room temperature, and repeatedly washing the obtained product by using heated deionized water for several times to remove redundant productsChloride salt until silver nitrate (AgNO) is used3) Reagent test filtrate does not contain Cl-The washed powder was filtered, dried at 90 ℃ for 24 hours, sieved first with 100 mesh and then with 400 mesh, the particle size of the powder was measured with a laser particle sizer, the flowability was measured with a hall flow meter, and the ratio of raw material to molten salt was found to be 1: (5-7), the powder has better sphericity rate and fluidity.
TABLE 2 raw materials and molten salt ratio and rare earth tantalate (Lu)1/3Pm1/3Eu1/3)TaO4Relationship between sphericity and fluidity
Example 3
In this example, a molten salt method is used to prepare high-entropy rare earth tantalate (Y)1/4Al1/4Sm1/4Er1/4)TaO4The method for preparing the spherical powder comprises the following steps:
according to 1/4: 1/4: 1/4: 1/4: 1 molar ratio of Y2O3、Al2O3、Sm2O3、Er2O3And Ta2O55kg in total, according to the weight ratio of 5:1 proportion weighing KCl and NaCl mixed salt, raw material and molten salt purity>99.99%, the particle size is 1-80 μm, and the mass ratio is 1: 6 weighing raw materials and molten salt, pouring the raw materials and the molten salt into a ball milling tank, ball milling the raw materials and the molten salt for 12 hours (350r/min) in a planetary ball mill by using absolute ethyl alcohol as a medium, drying the raw materials for 24 hours at 90 ℃, sieving the raw materials by a 400-mesh sieve, then placing the raw materials into a resistance furnace for calcination, wherein the calcination temperature and the calcination time are respectively (600-1200 ℃) and 6 hours, the heating rate is 5 ℃/min, cooling the raw materials along with the furnace after the calcination is finished, taking out powder after the temperature is reduced to the room temperature, repeatedly washing the obtained product by using heated deionized water for several times to remove redundant chloride salt until silver nitrate (AgNO) is used3) Reagent test filtrate does not contain Cl-Filtering the washed powder, drying at 90 deg.C for 24 hr, sieving with 100 mesh sieve, sieving with 400 mesh sieve, and measuring the particle diameter by laser particle sizerThe range is 40 μm-90 μm, the fluidity is (32-97s)/50g by using Hall flow meter, the data in Table 3 shows that the powder has better sphericity ratio and fluidity when the calcining temperature is 600-1000 ℃.
TABLE 3 calcination temperature and rare earth tantalates (Y)1/4Al1/4Sm1/4Er1/4)TaO4Relationship between sphericity and fluidity
Example 4
In this example, a molten salt method is used to prepare high-entropy rare earth tantalate (Er)1/6Sm1/6Pm1/6Nd1/6Yb1/6Eu1/6)TaO4The method for preparing the spherical powder comprises the following steps:
according to 1/6: 1/6: 1/6: 1/6: 1/6: 1/6: weighing Er according to the molar ratio of 12O3、Sm2O3、Pm2O3、Nd2O3、Yb2O3、 Eu2O3And Ta2O55kg in total, according to the weight ratio of 5:1 proportion weighing KCl and NaCl mixed salt, raw material and molten salt purity>99.99%, the particle size is 1-80 μm, and the mass ratio is 1: 6 weighing raw materials and molten salt, pouring the raw materials and the molten salt into a ball milling tank, ball milling the raw materials and the molten salt for 12h (350r/min) in a planetary ball mill by using absolute ethyl alcohol as a medium, drying the raw materials for 24h at 90 ℃, sieving the raw materials by a 400-mesh sieve, then placing the raw materials into a resistance furnace for calcination, wherein the calcination temperature and the calcination time are respectively 900 ℃ and (1-10h), the heating rate is 5 ℃/min, cooling the raw materials along with the furnace after the calcination is finished, taking out the powder body after the temperature is reduced to the room temperature, repeatedly washing the obtained product by heated deionized water for several times to remove the redundant chloride salt until silver nitrate (AgNO) is used3) Reagent test filtrate does not contain Cl-The washed powder was filtered, dried at 90 ℃ for 24 hours, and sieved first through 100 mesh and then through 400 mesh.
High-entropy rare earth tantalate (Er) prepared by the scheme1/6Sm1/6Pm1/6Nd1/6Yb1/6Eu1/6)TaO4The spherical powder has better sphericity ratio and fluidity, and the grain size is increased along with the extension of sintering time. Please supplement the graph or table of the relationship between sintering time (1-10h) and grain size, the effect is best when the sintering time is 4-8 h.
The above-mentioned embodiments are merely preferred embodiments for fully illustrating the present invention, and the scope of the present invention is not limited thereto. The equivalent substitution or change made by the technical personnel in the technical field on the basis of the invention is all within the protection scope of the invention. The protection scope of the invention is subject to the claims.
Claims (10)
1. Preparation of high-entropy rare earth tantalate RETaO by molten salt method4The method for preparing spherical powder is characterized by comprising the following steps:
(1) weighing raw materials and molten salt, taking absolute ethyl alcohol as a medium, and carrying out ball milling uniformly in a ball mill;
(2) drying and sieving the product obtained in the step (1), and then heating and calcining;
(3) cooling and cleaning the product obtained in the step (2);
(4) filtering, secondary drying and sieving the powder washed in the step (3) to obtain the high-entropy rare earth tantalate RETaO4Spherical powder;
the rare earth tantalate RETaO4In the formula, RE is at least one of yttrium, aluminum and lanthanide rare earth elements;
the raw material is RE2O3And Ta2O5Said RE2O3Is Y2O3、Al2O3、La2O3、Ce2O3、Nd2O3、Pm2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、Dy2O3、Ho2O3、Er2O3、Tm2O3、Yb2O3、Lu2O3At least one of;
the molten salt is a mixed salt of KCl and NaCl.
2. The molten salt method for preparing high-entropy rare earth tantalate (RETaO) according to claim 14The method for preparing spherical powder is characterized by comprising the following steps: raw material RE in step (1)2O3And Ta2O5In a molar ratio of 1: 1, purity of the starting Material>99.99 percent and the grain diameter is 1-80 mu m.
3. The molten salt method for preparing high-entropy rare earth tantalate (RETaO) according to claim 14The method for preparing spherical powder is characterized by comprising the following steps: purity of molten salt in step (1)>99.99%, the particle size is 1-80 μm, and the mass ratio of KCl to NaCl is (1-5): (1-2), the mass ratio of the raw materials to the molten salt is (1-2): (1-7).
4. The molten salt method for preparing high-entropy rare earth tantalate (RETaO) according to claim 34The method for preparing spherical powder is characterized by comprising the following steps: in the step (1), the mass ratio of the molten salt KCl to NaCl is optimized to be 5:1, optimizing the mass ratio of the raw materials to the molten salt to be 1: 6.
5. the molten salt method for preparing high-entropy rare earth tantalate (RETaO) according to claim 14The method for preparing spherical powder is characterized by comprising the following steps: the rotation speed of ball milling in the step (1) is 350r/min, and the ball milling time is 12 h.
6. The molten salt method for preparing high-entropy rare earth tantalate (RETaO) according to claim 14The method for preparing spherical powder is characterized by comprising the following steps: in the step (2), the drying is carried out at 90 ℃ for 24 hours, and the sieving is carried out by a 400-mesh sieve.
7. The molten salt method for preparing high-entropy rare earth tantalate (RETaO) according to claim 14The method for preparing spherical powder is characterized by comprising the following steps: in the step (2), the calcining temperature is 600-1200 ℃, the calcining time is 4-8h, and the heating rate is 5 ℃/min.
8. The molten salt method of claim 7 for preparing high-entropy rare earth tantalate (RETaO)4The method for preparing spherical powder is characterized by comprising the following steps: the calcining temperature in the step (2) is 800 ℃, and the time is 6 h.
9. The molten salt method for preparing high-entropy rare earth tantalate (RETaO) according to claim 14The method for preparing spherical powder is characterized by comprising the following steps: and (4) drying at 90 ℃ for 24h, wherein the sieving is to sieve through 100 meshes and then through 400 meshes.
10. High entropy rare earth tantalate RETaO prepared by the process of any one of claims 1 to 94Spherical powder.
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| CN116462505A (en) * | 2023-01-29 | 2023-07-21 | 昆明理工大学 | High-entropy rare earth tantalate oxygen ion insulator material and preparation method thereof |
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| CN114230339A (en) * | 2022-01-17 | 2022-03-25 | 北京理工大学 | Rare earth tantalate high-entropy ceramic material and preparation method and application thereof |
| CN114230339B (en) * | 2022-01-17 | 2022-11-08 | 北京理工大学 | Rare earth tantalate high-entropy ceramic material and preparation method and application thereof |
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| CN116462505B (en) * | 2023-01-29 | 2024-04-12 | 昆明理工大学 | High-entropy rare earth tantalate oxygen ion insulator material and preparation method thereof |
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