CN114044671A - Method for preparing high-entropy rare earth tantalate hollow sphere powder by centrifugal spray granulation method - Google Patents
Method for preparing high-entropy rare earth tantalate hollow sphere powder by centrifugal spray granulation method Download PDFInfo
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- 238000000034 method Methods 0.000 title claims abstract description 50
- 239000007921 spray Substances 0.000 title claims abstract description 48
- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 44
- 150000002910 rare earth metals Chemical class 0.000 title claims abstract description 38
- 238000005469 granulation Methods 0.000 title claims abstract description 37
- 230000003179 granulation Effects 0.000 title claims abstract description 35
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 70
- 239000008367 deionised water Substances 0.000 claims abstract description 60
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 60
- 239000002245 particle Substances 0.000 claims abstract description 59
- 239000002002 slurry Substances 0.000 claims abstract description 39
- 238000000227 grinding Methods 0.000 claims abstract description 36
- 238000001035 drying Methods 0.000 claims abstract description 33
- 239000002994 raw material Substances 0.000 claims abstract description 25
- 238000007873 sieving Methods 0.000 claims abstract description 25
- 239000011230 binding agent Chemical group 0.000 claims abstract description 22
- 238000000498 ball milling Methods 0.000 claims abstract description 20
- 239000002518 antifoaming agent Substances 0.000 claims abstract description 18
- 238000005303 weighing Methods 0.000 claims abstract description 18
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims abstract description 14
- 238000001354 calcination Methods 0.000 claims abstract description 11
- 238000002156 mixing Methods 0.000 claims abstract description 7
- 238000002360 preparation method Methods 0.000 claims abstract description 6
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 claims abstract description 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 50
- 239000011805 ball Substances 0.000 claims description 39
- 239000003292 glue Substances 0.000 claims description 13
- 229910001404 rare earth metal oxide Inorganic materials 0.000 claims description 12
- 230000002572 peristaltic effect Effects 0.000 claims description 10
- 238000002844 melting Methods 0.000 claims description 9
- 230000008018 melting Effects 0.000 claims description 9
- KBPLFHHGFOOTCA-UHFFFAOYSA-N caprylic alcohol Natural products CCCCCCCCO KBPLFHHGFOOTCA-UHFFFAOYSA-N 0.000 claims description 6
- 239000000084 colloidal system Substances 0.000 claims description 6
- 229910052747 lanthanoid Inorganic materials 0.000 claims description 6
- 150000002602 lanthanoids Chemical class 0.000 claims description 6
- VQCBHWLJZDBHOS-UHFFFAOYSA-N erbium(III) oxide Inorganic materials O=[Er]O[Er]=O VQCBHWLJZDBHOS-UHFFFAOYSA-N 0.000 claims description 5
- 238000010438 heat treatment Methods 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
- FIXNOXLJNSSSLJ-UHFFFAOYSA-N ytterbium(III) oxide Inorganic materials O=[Yb]O[Yb]=O FIXNOXLJNSSSLJ-UHFFFAOYSA-N 0.000 claims description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 4
- 229910000421 cerium(III) oxide Inorganic materials 0.000 claims description 4
- 229910052593 corundum Inorganic materials 0.000 claims description 4
- NLQFUUYNQFMIJW-UHFFFAOYSA-N dysprosium(III) oxide Inorganic materials O=[Dy]O[Dy]=O NLQFUUYNQFMIJW-UHFFFAOYSA-N 0.000 claims description 4
- RSEIMSPAXMNYFJ-UHFFFAOYSA-N europium(III) oxide Inorganic materials O=[Eu]O[Eu]=O RSEIMSPAXMNYFJ-UHFFFAOYSA-N 0.000 claims description 4
- 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 4
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 4
- 229910003443 lutetium oxide Inorganic materials 0.000 claims description 4
- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 claims description 4
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 4
- 238000006243 chemical reaction Methods 0.000 claims description 3
- 238000009826 distribution Methods 0.000 claims description 3
- JYTUFVYWTIKZGR-UHFFFAOYSA-N holmium oxide Inorganic materials [O][Ho]O[Ho][O] JYTUFVYWTIKZGR-UHFFFAOYSA-N 0.000 claims description 3
- TVMXDCGIABBOFY-UHFFFAOYSA-N n-Octanol Natural products CCCCCCCC TVMXDCGIABBOFY-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
- 238000005245 sintering Methods 0.000 claims description 3
- 238000003756 stirring Methods 0.000 claims description 3
- 239000000126 substance Substances 0.000 claims description 3
- 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 3
- 239000012856 weighed raw material Substances 0.000 claims description 3
- 238000001914 filtration Methods 0.000 claims description 2
- 239000000463 material Substances 0.000 description 21
- 239000000203 mixture Substances 0.000 description 10
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- 239000013078 crystal Substances 0.000 description 4
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- 239000012720 thermal barrier coating Substances 0.000 description 4
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Abstract
The invention discloses a centrifugal spray granulation method for preparing high-entropy rare earth tantalateThe preparation method of the hollow sphere powder comprises the following steps: step one, weighing raw material YAR in proportion2O3Oxide and tantalum pentoxide Ta2O5After ball milling and mixing uniformly, drying, sieving and calcining to obtain blocky tantalate; step two, crushing the blocky tantalite, adding the powder and primary deionized water into a grinding machine for grinding to obtain slurry with the required particle size range, and placing the slurry into a filter pressFiltering, drying and sieving to obtain dried powder, adding secondary deionized water and binder into the dried powder, adding defoaming agent to obtain spray granulation preform, drying and sieving to obtain rare earth tantalateHollow sphere powder. The hollow spherical powder prepared by the method has uniform particles, good fluidity and high product purity.
Description
Technical Field
The invention belongs to the technical field of split preparation of ceramics, and particularly relates to a method for preparing high-entropy rare earth tantalate hollow sphere powder by a centrifugal spray granulation method.
Background
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) a lattice distortion effect; (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 ceramic has the advantages of high melting point, high hardness, high toughness, low thermal conductivity, corrosion resistance and the like, and shows great development potential in the field of TBCs. At present, the new ferroelastic material rare earth tantalate RETaO4Ceramic has become a key material for the research of thermal barrier coatings, and is considered as a new generation thermal barrier coating material with the most potential due to the extremely high melting point, low thermal conductivity, high thermal expansion coefficient, good thermal performance and good mechanical performance. There is a need to further reduce the thermal conductivity of the coating, improve its flow properties, and improve the thermal protection of the coating.
Disclosure of Invention
The invention aims to provide a centrifugal spray granulation method for preparing high-entropy rare earth tantalateThe hollow spherical powder prepared by the method of the hollow sphere powder has uniform particles, good fluidity and high product purity.
The invention adopts the following technical scheme: centrifugal spray granulation method for preparing high-entropy rare earth tantalateYAR is at least two of trivalent lanthanide series rare earth elements, or at least one of lanthanide series rare earth elements and at least one of Y or Al; raw material YAR2O3The ratio of the oxides is 1/x: 1/x2O3Oxide and Ta2O5The ratio of (1/x: 1/x) to (1/x: 1), wherein x is the number of trivalent elements; the preparation method comprises the following steps:
step one, weighing raw materials according to a proportion, carrying out ball milling and mixing on the weighed raw materials in a ball mill, drying, sieving and calcining to obtain blocky tantalate, wherein the chemical reaction formula is as follows:the chemical formula of various trivalent oxides is shown, x is the number of trivalent elements, x is more than or equal to 2, i is the sequence of the trivalent elements, and i is more than or equal to 1 and less than or equal to x;
step two, crushing the blocky tantalate, adding powder and primary deionized water into a grinder for grinding, detecting the particle size distribution of particles in the slurry by using a laser particle sizer to obtain slurry in a required particle size range, placing the slurry in a filter press for filtering and drying, sieving to obtain dried powder, adding secondary deionized water and a binder into the dried powder, simultaneously adding a defoaming agent to obtain a spray granulation preform, spray granulating the preform, drying, and sieving to obtain the rare earth tantalateHollow sphere powder;
the mass ratio of the drying powder to the secondary deionized water to the binder to the defoaming agent is 1-10: 1-5: 0.3-1: 0.001-1, and the defoaming agent is n-octanol.
Further, the raw material YAR2O3The oxide being Y2O3、Al2O3Or rare earth oxide RE2O3(ii) a Rare earth oxide RE2O3Is La2O3、Ce2O3、Nd2O3、Pm2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、 Dy2O3、Ho2O3、Er2O3、Tm2O3、Yb2O3Or Lu2O3;
Tantalum pentoxide Ta2O5And YAR2O3The molar ratio of the oxides is 1: 1.
Furthermore, the purity of the raw materials is more than 99.9%, and the particle size is 40-50 μm.
Further, in the first step, in the ball milling process, the ratio of the zirconia balls to the raw materials to the deionized water is 1-10: 1-5: 1-3, the rotating speed of the ball mill is 100-600 r/min, and the ball milling time is 1-30 h.
Further, in the first step, the drying temperature is 60-100 ℃, the drying time is 1-48 hours, and the powder is sieved by a 100-800-mesh sieve during sieving; the calcination temperature is 1100-1700 ℃, and the sintering time is 2-30 hours.
Further, in the spray granulation process, the preform slurry is stirred by a stirrer until the spray granulation is completed.
Further, in the second step, a crusher is used for crushing the blocky tantalate to 0.001-1 mm of powder, and the zirconia balls, the powder and the deionized water are weighed according to the proportion of 1-10: 1-5: 1-3 and are placed in a grinder for grinding; the grinding time is 180-3600 min, the rotating speed of the grinding machine is 100-600 r/min, and the particle size of the particles in the slurry is 500-2000 nm after grinding.
Further, the adhesive is formed by preparing a colloid by a glue melting machine, heating deionized water to 90-100 ℃ according to the ratio of the deionized water to adhesive powder of 1-10: 1-7, adding the adhesive powder, keeping the temperature and stirring for 100-600 min.
Further, in the second step, the air inlet temperature of the spray granulator is 100-400 ℃, the air outlet temperature is 100-300 ℃, the frequency of the spray head is 1-50 Hz, the feeding rate is reflected by the frequency of the peristaltic pump, and the frequency range is 1-50 Hz.
Further, the drying temperature is 30-100 ℃, the drying time is 1-48h, the materials are sequentially sieved by 100-300 meshes and 400-2000 meshes during sieving, and the intermediate of the two sieves is taken to obtain the rare earth tantalateHollow sphere powder.
The invention has the beneficial effects that: 1. preparing the obtained rare earth tantalateThe hollow sphere powder has high sphericity rate, good fluidity, high hollow rate and uniform particle size. 2. During granulation, the crystal grain appearance, the crystal grain size and the hollow rate of spherical powder are adjusted by changing the water-material ratio, the slurry-glue ratio, the spray head frequency and the feeding rate, so that the operation is convenient.
Drawings
FIG. 1 is the rare earth tantalate (Y) prepared in example 10.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4XRD spectrum of hollow sphere powder;
FIG. 2 is the rare earth tantalate (Y) prepared in example 10.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4SEM image of the hollow sphere powder.
Detailed Description
The present invention will be described in detail below with reference to the accompanying drawings and specific embodiments.
The invention relates to a centrifugal spray granulation method for preparing high-entropy rare earth tantalateYAR is at least two of trivalent lanthanide series rare earth elements, or at least one of lanthanide series rare earth elements and at least one of Y or Al; raw material YAR2O3The ratio of the oxides is 1/x: 1/x2O3Oxide and Ta2O5The ratio of (1/x: 1/x) to (1/x: 1), wherein x is the number of trivalent elements; the method comprises the following steps:
step one, weighing raw materials according to a proportion, carrying out ball milling and mixing on the weighed raw materials in a ball mill, drying, sieving and calcining to obtain blocky tantalate, wherein the chemical reaction formula is as follows:the chemical formula of various trivalent oxides is shown, x is the number of trivalent elements, x is more than or equal to 2, i is the sequence of the trivalent elements, and i is more than or equal to 1 and less than or equal to x;
the purity of the raw material is more than 99.9 percent, and the particle size is 40-50 mu m.
Raw material YAR2O3The oxide being Y2O3、Al2O3Or rare earth oxide RE2O3(ii) a Rare earth oxide RE2O3Is La2O3、Ce2O3、Nd2O3、Pm2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、Dy2O3、Ho2O3、 Er2O3、Tm2O3、Yb2O3Or Lu2O3(ii) a Tantalum pentoxide (Ta)2O5) And the trivalent oxide YAR2O3The molar ratio of (A) to (B) is 1: 1.
In the ball milling process, the ratio of the zirconia balls to the raw materials to the deionized water is 1-10: 1-5: 1-3, the rotating speed of the ball mill is 100-600 r/min, and the ball milling time is 1-30 h;
the drying temperature is 60-100 ℃, the drying time is 1-48 hours, and the powder is sieved by a sieve of 100-800 meshes during sieving; the calcining temperature is 1100-1700 ℃, and the sintering time is 2-30 hours;
secondly, crushing the blocky tantalite in the first step, crushing the blocky tantalite by using a crusher to obtain 0.001-1 mm powder, adding the powder and primary deionized water into a grinding machine for grinding, detecting the particle size distribution of particles in the slurry by using a laser particle sizer to obtain slurry in a required particle size range, weighing zirconia balls, the powder and the deionized water according to the proportion of 1-10: 1-5: 1-3, and placing the zirconia balls, the powder and the deionized water into the grinding machine for grinding; the grinding time is 180-3600 min, the rotating speed of the grinding machine is 100-600 r/min, and the particle size range of the particles in the slurry after grinding is 500-2000 nm. Placing the slurry in a filter press to filter most of water and then drying, then adding secondary deionized water and a binder into the dried powder, simultaneously adding a defoaming agent to remove bubbles on the surface layer to obtain a spray granulation preform, spray granulation, in the spray granulation process, stirring the preform slurry by using a stirrer until the spray granulation is finished, adjusting the morphology of crystal grains, the size of the crystal grains and the hollow rate of spherical powder by changing the water-material ratio, the ratio of the slurry to the glue, the frequency of a spray nozzle and the feeding rate, placing the prepared powder in an oven to dry and then sieving to obtain the rare earth tantalate with high sphericity rate, good fluidity and uniform particle sizeHollow sphere powder. During granulation, the air inlet temperature of the spray granulator is 100-400 ℃, the air outlet temperature is 100-300 ℃, the frequency of a nozzle is 1-35 Hz, the feeding rate is reflected by the frequency of a peristaltic pump, and the frequency range is 1-50 Hz. Drying at 30-100 ℃ for 1-48h, sequentially sieving by 100-300 meshes and 400-2000 meshes during sieving, and taking the intermediate of the two sieves to obtain the rare earth tantalateHollow sphere powder.
During ball milling, weighing zirconia balls, powder and deionized water according to the proportion of 1-10: 1-5: 1-3, and placing the mixture into a grinding machine for grinding; the grinding time is 180-3600 min, the rotating speed of the grinding machine is 100-600 r/min, and the particle size of the particles in the slurry is 500-2000 nm after grinding.
The adhesive PVA/PTFE/CMC/PP/PE/PVDF/PVB is prepared into colloid by a glue melting machine, the ratio of deionized water to adhesive powder is 1-10: 1-7, the deionized water is heated to 90-100 ℃, and then the adhesive powder is added, and the mixture is stirred for 100-600 min under the condition of heat preservation.
The defoaming agent is n-octanol, and the mass ratio of the drying powder, the secondary deionized water, the binder and the defoaming agent is 1-10: 1-5: 0.3-1: 0.001-1.
When the powder with the hollow structure prepared by the invention is sprayed, the hollow powder can be melted into flat particles and adhered to the substrate, and the coating thickness of the formed flat particle spraying is more uniform, the defects are fewer, the porosity is moderate, the phonon mean free path is reduced, and the thermal conductivity is extremely low. In addition, the powder with the hollow sphere structure transfers heat at high temperature through air, and the thermal conductivity coefficient of the air is extremely low and is about 0.023W/m.k, so that the thermal conductivity of the powder as a thermal barrier coating is further reduced.
Example 1
This example illustrates the preparation of high-entropy rare earth tantalate (Y) by centrifugal spray granulation0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4The method for preparing the hollow sphere powder comprises the following steps:
weighing Y according to the molar ratio of 1/5: 1/5: 1/5: 1: 5: 1/5: 12O3 2.2581kg、Ce2O3 3.2824kg、 Sm2O33.4872kg、Gd2O3 3.625kg、Dy2O33.73kg and Ta2O522.095kg of 38.4777kg, 77kg of zirconia balls and 23kg of deionized water are weighed, the ratio of the zirconia balls to the raw materials to the deionized water is 10: 5: 3, the zirconia balls, the raw materials and the deionized water are placed in a ball milling tank to be mixed, sealed and then placed on a planetary ball mill to be milled for 800min, and the rotating speed is 300r/min, so that the mixture is uniformly mixed. Then placing the ball-milled slurry in a filter press to filter most of the water, drying at 80 deg.C for 30 hr, sieving with 200 mesh sieve, calcining at 1700 deg.C for 20And (5) obtaining block-shaped powder after hours.
Crushing the calcined blocky powder by using a crusher, taking 35kg of blocky powder, weighing 70kg of zirconia balls, 35kg of crushed powder and 21kg of deionized water according to the proportion of 10: 5: 3, placing the crushed powder and the crushed powder into a grinder for grinding, wherein the grinding process is lossy, the grinding time is 600min, the rotating speed of the grinder is 400r/min, and during grinding, a laser particle size analyzer is adopted to test the particle size of the powder in the slurry, and the particle size of the powder is ground to 1200 nm. The ground slurry was placed in a filter press to filter most of the water, then dried at 80 ℃ for 30 hours, sieved through a 200 mesh sieve, and the undersize material was taken.
Weighing 1kg of PVB powder and 10kg of deionized water, placing in a glue melting machine, heating to 90 ℃, and preserving heat for 400min to prepare a glue. In order to obtain slurry with optimal viscosity, the influence of the ratio of the crushed and dried powder to the deionized water on the sphericity rate and the fluidity of the powder is obtained by a controlled variable method, as shown in table 1. Therefore, the dried powder and the secondary deionized water are weighed according to the table 1, namely 30kg of the dried powder, 1.5kg of the binder colloid and 6g of the defoaming agent are weighed according to the ratio of the powder to the secondary deionized water of 1-10: 1-5, the mass ratio of the dried powder to the secondary deionized water to the binder colloid is 1-10: 1-5: 0.5: 0.002, the mixture is uniformly stirred by a stirrer, the speed of the stirrer is 200r/min, the slurry is granulated by a spray drying device to prepare the spherical powder, the air inlet temperature of a spray granulator is 290 ℃, the air outlet temperature is 180 ℃, the frequency of a spray head is 41Hz, and the frequency of a peristaltic pump is 43 Hz; drying the prepared spherical powder at 80 ℃ for 20h to obtain tantalate spherical powder for thermal spraying, sequentially sieving by 300 meshes and 2000 meshes, taking the intermediate of the two sieves to obtain the powder particle size measured by a laser particle sizer, wherein the particle size range is 10-100 mu m, and measuring the fluidity by a Hall flow meter, wherein the fluidity is the best fluidity which is 42s/50g when the ratio of the powder to deionized water is 6: 4 as shown in Table 1. As shown in fig. 1, the XRD pattern and YTaO were measured4(PDF:24-1415)、SmTaO4(PDF:24-1010)GdTaO4(PDF: 24-0441) and DyTaO4(PDF: 12-0379) compared with the corresponding PDF standard card, the shift of the main peak is found, which is the doping effect causing the XRD peak to be emittedGreen shift, the high entropy (Y) of the synthesis of the invention, as found by comparison with the main peak0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4High purity and less impurities. As can be seen from FIG. 2, (Y) prepared0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4The sphericity ratio is preferably calculated as the ratio of spherical particles to total particles in fig. 2.
TABLE 1 Water to Material ratio and rare earth tantalates (Y)0.2Ce0.2Sm0.2Gd0.2Dy0.2)TaO4Relationship between sphericity and fluidity
Example 2
In this example, a centrifugal spray granulation method is used to prepare high-entropy rare earth tantalate (Nd)1/3Sm1/3Eu1/3)TaO4The method for preparing the hollow sphere powder comprises the following steps
Nd is weighed according to the molar ratio of 1/3: 1/3: 1/3: 12O36.7296、Sm2O36.9744kg、Eu2O33.5192kg and Ta2O513.257kg of 30.4802kg, weighing 61kg of zirconia balls and 18.3kg of deionized water, wherein the ratio of the zirconia balls to the raw materials to the deionized water is 10: 5: 3, placing the zirconia balls, the raw materials and the deionized water in a ball milling tank, mixing, sealing, placing on a planetary ball mill, and ball milling for 800min at the rotating speed of 300r/min to uniformly mix. And then placing the ball-milled slurry in a filter press to filter most of water, drying at 80 ℃ for 30 hours, sieving with a 200-mesh sieve, taking undersize materials, and calcining at 1700 ℃ for 20 hours to obtain blocky powder.
Crushing 25kg of calcined blocky powder by using a crusher, wherein the particle size of the crushed blocky powder is 0.1-1 mm, weighing 50kg of zirconia balls, 25kg of crushed powder and 15kg of deionized water according to the proportion of 10: 5: 3, placing the weighed materials into a grinding machine for grinding, and when grinding, testing the particle size of the powder in the slurry by using a laser particle sizer, wherein the particle size of the powder is ground to 1200nm, the ball milling time is 600min, and the rotating speed of the ball mill is 400 r/min. The ground slurry was placed in a filter press to filter most of the water, then dried at 80 ℃ for 30 hours and sieved through a 200 mesh sieve, and the undersize material was taken.
Weighing 1kg of PVB powder and 10kg of deionized water, placing in a glue melting machine, heating to 90 ℃, and preserving heat for 400min to prepare a glue. In order to obtain a slurry with an optimal viscosity, the influence of the ratio of the binder obtained by the controlled variable method on the powder sphericity ratio and flowability is shown in table 2. Therefore, the dried powder and the secondary deionized water are weighed according to the table 2, 20kg of the dried powder, 13.3kg of the secondary deionized water, the binder are weighed according to the ratio of the powder to the binder of 1-10: 1-5, and 6.7g of the defoaming agent. The mass ratio of the dried powder, the secondary deionized water, the binder and the defoaming agent is 6: 4: 0.5: 0.002, the mixture is uniformly stirred by a stirrer, the speed of the stirrer is 200r/min, the slurry is granulated by spray drying equipment to prepare spherical powder, the air inlet temperature of a spray granulator is 290 ℃, the air outlet temperature is 180 ℃, the frequency of a spray head is 41Hz, and the frequency of a peristaltic pump is 43 Hz; drying the prepared spherical powder at 80 ℃ for 20h to obtain tantalate spherical powder for thermal spraying, sequentially sieving by 100-300 meshes and 400-2000 meshes, testing the particle size of the powder by using a laser particle sizer, wherein the particle size range is 10-100 mu m, testing the fluidity by using a Hall flow meter, and testing rare earth tantalate (Nd) when the ratio of the ball-milled slurry to deionized water is 10: 1 as shown in Table 21/3Sm1/3Eu1/3)TaO4The sphericity ratio was 99%, and the fluidity was the best 37s/50 g.
TABLE 2 slurry to Binder ratio vs. rare earth tantalate (Nd)1/3Sm1/3Eu1/3)TaO4Relationship between sphericity and fluidity
Example 3
This example illustrates the preparation of high-entropy rare earth tantalate (Y) by centrifugal spray granulation1/4Al1/4Er1/4Yb1/4)TaO4The method for preparing the hollow sphere powder comprises the following steps:
weighing Y according to the molar ratio of 1/4: 1/4: 1/4: 1/4: 12O32.2581kg、Al2O31.0196kg、Er2O33.8252kg、Yb2O33.941kg and Ta2O517.676 kg of 28.7199kg, weighing 57kg of zirconia balls and 19kg of deionized water, wherein the ratio of the zirconia balls to the raw materials to the deionized water is 10: 5: 3, putting the zirconia balls, the raw materials and the deionized water into a ball milling tank, mixing, sealing, and then putting the mixture on a planetary ball mill for ball milling for 800min at the rotating speed of 300r/min to uniformly mix. And then placing the ball-milled slurry in a filter press to filter most of water, drying at 80 ℃ for 30 hours, sieving with a 200-mesh sieve, taking undersize materials, and calcining at 1700 ℃ for 20 hours to obtain blocky powder.
Crushing 25kg of calcined blocky powder by using a crusher, wherein the particle size of the crushed blocky powder is 0.1-1 mm, weighing 50kg of zirconia balls, 25kg of crushed powder and 15kg of deionized water according to the proportion of 10: 5: 3, placing the weighed materials into a grinding machine for grinding, and when grinding, testing the particle size of the powder in the slurry by using a laser particle sizer, wherein the particle size of the powder is ground to 1200nm, the ball milling time is 600min, and the rotating speed of the ball mill is 400 r/min. The ground slurry was placed in a filter press to filter most of the water, then dried at 80 ℃ for 30 hours and sieved through a 200 mesh sieve, and the undersize material was taken.
1kg of PVB powder and 10kg of deionized water are weighed and placed in a glue melting machine to be heated to 90 ℃, and the temperature is kept for 400min to prepare the glue. The influence of the nozzle frequency on the powder sphericity and flowability was obtained by the controlled variable method, as shown in table 3. 20kg of dried powder, 13kg of secondary deionized water, 1.7kg of binder and 7g of defoaming agent after grinding, filter pressing and sieving, wherein the mass ratio of the dried powder to the secondary deionized water to the binder to the defoaming agent is 6: 4: 0.5: 0.002, the dried powder to the secondary deionized water to the binder to the defoaming agent is uniformly stirred by a stirrer, the speed of the stirrer is 200r/min, slurry is granulated by spray drying equipment to prepare spherical powder, the spherical powder is sequentially sieved by 100-300 meshes and 400-2000 meshes, and materials between two sieves are taken. In the granulation process, the air inlet temperature of the spray granulator is 290 ℃, the air outlet temperature is 180 ℃, the frequency of the spray head is 1-50 Hz, and the frequency of the peristaltic pump is 43Hz as shown in Table 3; drying the prepared spherical powder at 80 ℃ for 20h to obtain the rare earth for thermal sprayingTantalate (Y)1/4Al1/4Er1/4Yb1/4)TaO4The hollow sphere powder is tested to have a particle size range of 10-100 μm by a laser particle sizer, and a flowability by a hall flow meter, as shown in table 3, when the frequency of the nozzle is 32Hz, the sphericity ratio is 98%, and the flowability is the best 39s/50 g.
TABLE 3 shower frequency and rare earth tantalate (Y)1/4Al1/4Er1/4Yb1/4) Relationship between sphericity and fluidity
Example 4
In this example, a centrifugal spray granulation method is used to prepare high-entropy rare earth tantalate (Y)1/6La1/6Pm1/6Er1/ 6Yb1/6Lu1/6)TaO4The method for preparing the hollow sphere powder comprises the following steps:
weighing Y according to the molar ratio of 1/6: 1/6: 1/6: 1/6: 1/6: 1/6: 12O3 2.2581kg、La2O3 3.2582kg、 Pm2O3 3.38kg、Er2O3 3.8252kg、Yb2O3 3.941kg、Lu2O33.9794kg and Ta2O526.514kg of 47.1559kg, 94kg of zirconia balls and 31.3kg of deionized water are weighed, the ratio of the zirconia balls to the raw materials to the deionized water is 10: 5: 3, the zirconia balls, the raw materials and the deionized water are placed in a ball milling tank to be mixed, sealed and then placed on a planetary ball mill to be ball milled for 800min, and the rotating speed is 300r/min, so that the mixture is uniformly mixed. And then placing the ball-milled slurry in a filter press to filter most of water, drying at 80 ℃ for 30 hours, sieving with a 200-mesh sieve, taking undersize materials, and calcining at 1700 ℃ for 20 hours to obtain blocky powder.
42kg of calcined blocky powder is crushed by a crusher, the particle size after crushing is 0.1 mm-1 mm, 84kg of zirconia balls, 42kg of crushed powder and 25.2kg of primary deionized water are weighed according to the proportion of 10: 5: 3 and are placed in a grinder to be ground, when grinding is carried out, a laser particle size analyzer is adopted to test the particle size of the powder in slurry, the particle size of the powder is ground to 1200nm, the ball-milling time is 600min, and the rotating speed of the ball mill is 400 r/min. The ground slurry was placed in a filter press to filter most of the water, then dried at 80 ℃ for 30 hours and sieved through a 200 mesh sieve, and the undersize material was taken.
Weighing 1kg of PVB powder and 10kg of deionized water, placing in a glue melting machine, heating to 90 ℃, and preserving heat for 400min to prepare a glue. The influence of the peristaltic pump frequency on the powder sphericity and flowability was obtained by the controlled variable method, as shown in table 4. 35kg of dried powder, 23.3kg of secondary deionized water, 2.9kg of binder colloid and 12g of defoaming agent, wherein the mass ratio of the dried powder to the secondary deionized water to the binder to the defoaming agent is 6: 4: 0.5: 0.002, the mixture is uniformly stirred by a stirrer, the speed of the stirrer is 200r/min, slurry is granulated by spray drying equipment to prepare spherical powder, the air inlet temperature of a spray granulator is 290 ℃, the air outlet temperature is 180 ℃, the frequency of a spray nozzle is 41Hz, and the frequency of a peristaltic pump is 43 Hz; drying the prepared spherical powder at 80 ℃ for 20h to obtain tantalate spherical powder for thermal spraying, sequentially sieving by 100-300 meshes and 400-2000 meshes, and taking the material between the two sieves. The particle size of the powder was measured by a laser particle sizer, the particle size ranged from 10 μm to 100 μm, and the flowability was measured by a hall flow meter, as shown in table 4, when the peristaltic pump frequency was 35Hz, the sphericity ratio was 99%, and the flowability was the best, 32s/50 g.
TABLE 4 peristaltic pump frequency and rare earth tantalate (Y)1/6La1/6Pm1/6Er1/6Yb1/6Lu1/6)TaO4Relationship between sphericity and fluidity
Claims (10)
1. A method for preparing high-entropy rare earth tantalate hollow sphere powder by a centrifugal spray granulation method is characterized in thatYAR is at least two trivalent lanthanide rare earth elements, or at least one lanthanide rare earth element and at least one of Y or Al; raw material YAR2O3The ratio between the oxides is 1/x: 1/x: .....: 1/x, raw material YAR2O3Oxide and Ta2O5The ratio of (A) to (B) is 1/x: 1/x: .....: 1/x: 1, wherein x is the number of trivalent elements; the preparation method comprises the following steps:
step one, weighing raw materials according to a proportion, carrying out ball milling and mixing on the weighed raw materials in a ball mill, drying, sieving and calcining to obtain blocky tantalate, wherein the chemical reaction formula is as follows: the chemical formula of various trivalent oxides is shown, x is the number of trivalent elements, x is more than or equal to 2, i is the sequence of the trivalent elements, and i is more than or equal to 1 and less than or equal to x;
step two, crushing the blocky tantalate, adding powder and primary deionized water into a grinder for grinding, detecting the particle size distribution of particles in the slurry by using a laser particle sizer to obtain slurry in a required particle size range, placing the slurry in a filter press for filtering and drying, sieving to obtain dried powder, adding secondary deionized water and a binder into the dried powder, simultaneously adding a defoaming agent to obtain a spray granulation preform, spray granulating the preform, drying, and sieving to obtain the rare earth tantalateHollow sphere powder;
the mass ratio of the drying powder to the secondary deionized water to the binder to the defoaming agent is 1-10: 1-5: 0.3-1: 0.001-1, wherein the defoaming agent is n-octanol.
2. The centrifugal spray granulation method for preparing the high-entropy rare earth tantalate hollow sphere powder according to claim 1Method of bulk, characterized in that the raw material YAR2O3The oxide being Y2O3、Al2O3Or rare earth oxide RE2O3(ii) a Rare earth oxide RE2O3Is La2O3、Ce2O3、Nd2O3、Pm2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、Dy2O3、Ho2O3、Er2O3、Tm2O3、Yb2O3Or Lu2O3;
Tantalum pentoxide Ta2O5And YAR2O3The mole ratio of the oxides is 1: 1.
3. the method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method according to claim 1 or 2, wherein the purity of the raw materials is more than 99.9%, and the particle size is 40-50 μm.
4. The method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method according to claim 3, wherein in the first step, in the ball milling process, the ratio of zirconia balls to raw materials to deionized water is 1-10: 1-5: 1-3, the rotating speed of the ball mill is 100-600 r/min, and the ball milling time is 1-30 h.
5. The method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method according to claim 4, wherein in the first step, the drying temperature is 60-100 ℃, the drying time is 1-48 hours, and the powder is sieved by a 100-800-mesh sieve; the calcination temperature is 1100-1700 ℃, and the sintering time is 2-30 hours.
6. The method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method as claimed in claim 5, wherein in the spray granulation process, the preform slurry is stirred by a stirrer until the spray granulation is finished.
7. The method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method according to claim 6, wherein in the second step, a crusher is used for crushing the blocky tantalate into powder with the particle size of 0.001-1 mm, and the particle size is determined according to the following formula of 1-10: 1-5: weighing zirconia balls, powder and deionized water in a proportion of 1-3, and putting the zirconia balls, the powder and the deionized water into a grinder for grinding; the grinding time is 180-3600 min, the rotating speed of the grinding machine is 100-600 r/min, and the particle size of the particles in the slurry is 500-2000 nm after grinding.
8. The method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method as claimed in claim 7, wherein the binder is prepared into a colloid by a glue melting machine, and the ratio of deionized water to the binder powder is 1-10: 1-7, heating deionized water to 90-100 ℃, adding binder powder, keeping the temperature, and stirring for 100-600 min.
9. The method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method according to claim 8, wherein in the second step, during granulation, the air inlet temperature of a spray granulator is 100-400 ℃, the air outlet temperature is 100-300 ℃, the frequency of a nozzle is 1-50 Hz, the feeding rate is reflected by the frequency of a peristaltic pump, and the frequency range is 1-50 Hz.
10. The method for preparing the high-entropy rare earth tantalate hollow sphere powder by the centrifugal spray granulation method according to claim 9, wherein after granulation, the drying temperature is 30-100 ℃, the drying time is 1-48 hours, during sieving, the powder is sequentially sieved by 100-300 meshes and 400-2000 meshes, and the intermediate of the two sieves is taken to obtain the rare earth tantalate hollow sphere powderHollow sphere powder.
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