CN114014653A - Preparation method of potassium tantalate niobate ceramic chip with adjustable dielectric constant - Google Patents
Preparation method of potassium tantalate niobate ceramic chip with adjustable dielectric constant Download PDFInfo
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- 239000000919 ceramic Substances 0.000 title claims abstract description 85
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 title claims abstract description 62
- 229910052700 potassium Inorganic materials 0.000 title claims abstract description 62
- 239000011591 potassium Substances 0.000 title claims abstract description 62
- 238000002360 preparation method Methods 0.000 title claims abstract description 18
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 claims abstract description 46
- 239000000463 material Substances 0.000 claims abstract description 34
- 238000005245 sintering Methods 0.000 claims abstract description 34
- 238000000034 method Methods 0.000 claims abstract description 32
- 229910000027 potassium carbonate Inorganic materials 0.000 claims abstract description 23
- 238000010438 heat treatment Methods 0.000 claims abstract description 19
- ZKATWMILCYLAPD-UHFFFAOYSA-N niobium pentoxide Inorganic materials O=[Nb](=O)O[Nb](=O)=O ZKATWMILCYLAPD-UHFFFAOYSA-N 0.000 claims abstract description 14
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 claims abstract description 12
- 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 12
- 238000007599 discharging Methods 0.000 claims abstract description 11
- 239000003292 glue Substances 0.000 claims abstract description 10
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims abstract description 10
- 230000015572 biosynthetic process Effects 0.000 claims abstract description 9
- 230000008569 process Effects 0.000 claims abstract description 9
- 238000003786 synthesis reaction Methods 0.000 claims abstract description 9
- 239000011230 binding agent Substances 0.000 claims abstract description 7
- 238000005469 granulation Methods 0.000 claims abstract description 7
- 230000003179 granulation Effects 0.000 claims abstract description 7
- 238000003825 pressing Methods 0.000 claims abstract description 7
- 239000010955 niobium Substances 0.000 claims description 18
- 239000000203 mixture Substances 0.000 claims description 14
- 239000003990 capacitor Substances 0.000 claims description 8
- 238000000227 grinding Methods 0.000 claims description 7
- 238000000498 ball milling Methods 0.000 claims description 5
- 238000007873 sieving Methods 0.000 claims description 5
- 238000001816 cooling Methods 0.000 claims description 4
- 239000006185 dispersion Substances 0.000 claims description 4
- 238000001035 drying Methods 0.000 claims description 4
- 229910052758 niobium Inorganic materials 0.000 claims description 4
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 4
- 239000002904 solvent Substances 0.000 claims description 4
- 229910052715 tantalum Inorganic materials 0.000 claims description 4
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 4
- 238000004519 manufacturing process Methods 0.000 claims 1
- 229910010293 ceramic material Inorganic materials 0.000 abstract description 7
- 239000013078 crystal Substances 0.000 abstract description 6
- 230000008901 benefit Effects 0.000 abstract description 2
- 238000002425 crystallisation Methods 0.000 abstract description 2
- 230000008025 crystallization Effects 0.000 abstract description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 11
- 238000006243 chemical reaction Methods 0.000 description 7
- 239000000843 powder Substances 0.000 description 7
- 239000002994 raw material Substances 0.000 description 6
- 239000001993 wax Substances 0.000 description 6
- 239000012535 impurity Substances 0.000 description 5
- 239000012071 phase Substances 0.000 description 5
- 238000005054 agglomeration Methods 0.000 description 4
- 230000002776 aggregation Effects 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- 229910052573 porcelain Inorganic materials 0.000 description 4
- 238000005303 weighing Methods 0.000 description 4
- 238000004146 energy storage Methods 0.000 description 3
- 238000004321 preservation Methods 0.000 description 3
- 230000009467 reduction Effects 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 2
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- 229910000484 niobium oxide Inorganic materials 0.000 description 2
- 230000010287 polarization Effects 0.000 description 2
- 229910001936 tantalum oxide Inorganic materials 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
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- 125000003158 alcohol group Chemical group 0.000 description 1
- 239000003985 ceramic capacitor Substances 0.000 description 1
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- 238000012512 characterization method Methods 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
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- 230000000694 effects Effects 0.000 description 1
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- 230000002349 favourable effect Effects 0.000 description 1
- 239000012634 fragment Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
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- 239000007790 solid phase Substances 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
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- 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
- C04B35/495—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 vanadium, niobium, tantalum, molybdenum or tungsten oxides or solid solutions thereof with other oxides, e.g. vanadates, niobates, tantalates, molybdates or tungstates
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G4/00—Fixed capacitors; Processes of their manufacture
- H01G4/002—Details
- H01G4/018—Dielectrics
- H01G4/06—Solid dielectrics
- H01G4/08—Inorganic dielectrics
- H01G4/12—Ceramic dielectrics
- H01G4/1209—Ceramic dielectrics characterised by the ceramic dielectric material
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- 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
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Abstract
The invention belongs to the field of inorganic nonmetallic materials, relates to the preparation of artificial crystals and functional ceramic materials, and particularly relates to a preparation method of a potassium tantalate-niobate ceramic chip with adjustable dielectric constant, wherein tantalum pentoxide, niobium pentoxide and potassium carbonate are sintered and pre-synthesized to obtain a polycrystalline material, the polycrystalline material is crushed and ground, then a binder is added for wax frying and granulation, and then the polycrystalline material is sequentially subjected to dry pressing into pieces, heating and glue discharging, and sintering into ceramic to obtain the potassium tantalate-niobate ceramic chip; wherein, the potassium carbonate is added in excess, the sintering pre-synthesis temperature is 700-800 ℃, and the sintering process of the sintered ceramic is carried out according to a set temperature program. The potassium tantalate-niobate ceramic chip prepared by the method has the advantages of high purity, good crystallization, large size and high dielectric constant, and the dielectric constant can be adjusted according to the requirements.
Description
Technical Field
The invention belongs to the field of inorganic nonmetallic materials, relates to the preparation of artificial crystals and functional ceramic materials, and particularly relates to a preparation method of a potassium tantalate-niobate ceramic chip with an adjustable dielectric constant.
Background
The information in this background section is only for enhancement of understanding of the general background of the invention and is not necessarily to be construed as an admission or any form of suggestion that this information forms the prior art that is already known to a person of ordinary skill in the art.
As the inventor researches, the potassium tantalate niobate (KTa)1-xNbxO3(ii) a Abbreviated as KTN) ceramics have obstacles in specific applications: in the existing preparation method, ions cannot be freely transported, so that the uniform large-volume KTN ceramic sheet is difficult to prepare, and the application of the material is limited; the traditional preparation method causes serious volatilization of potassium component, and causes deviation of KTN stoichiometric ratio; the growth and hard agglomeration of crystal grains can also directly influence the performance of the ceramic wafer; the properties of ceramic materials prepared by different processes and different parameters can also vary greatly. In addition, the dielectric constant of the existing potassium tantalate niobate ceramic is small and is difficult to adjust according to requirements.
Disclosure of Invention
In order to solve the defects of the prior art, the invention aims to provide the preparation method of the potassium tantalate-niobate ceramic chip with the adjustable dielectric constant.
In order to achieve the purpose, the technical scheme of the invention is as follows:
on the one hand, the preparation method of the potassium tantalate niobate ceramic chip with the adjustable dielectric constant comprises the steps of sintering tantalum pentoxide, niobium pentoxide and potassium carbonate to obtain a polycrystalline material, crushing and grinding the polycrystalline material, adding a binder to stir-fry and granulate, and then sequentially performing dry pressing into sheets, heating and glue discharging, and sintering into ceramic to obtain the potassium tantalate niobate ceramic chip; wherein, the potassium carbonate is added in excess, the sintering pre-synthesis temperature is 700-800 ℃, and the sintering process of the sintered ceramic is carried out according to a set temperature program.
In order to improve the purity of the prepared potassium tantalate niobate ceramic chip, the method adopts sintering pre-synthesis (700-800 ℃) to form a polycrystalline material, and the polycrystalline material is used as a raw material to prepare the potassium tantalate niobate ceramic chip, so that the reduction of the purity can be avoided. In order to avoid that the potassium component volatilizes to influence the stoichiometric ratio of KTN, thereby influencing the phase composition of the potassium tantalate-niobate ceramic chip and further influencing the performance of the potassium tantalate-niobate ceramic chip, the potassium carbonate is excessively added, so that the stoichiometric ratio of KTN can be avoided. According to the invention, through the matching of wax frying granulation, dry pressing into pieces, heating and glue discharging, and sintering into porcelain, the potassium tantalate niobate ceramic piece with large size and high performance can be obtained, and particularly, the sintering into porcelain is carried out through a set temperature program, so that the generation of impurities can be avoided, and the growth and hard agglomeration of crystal grains can be avoided, thereby ensuring the performance of the potassium tantalate niobate ceramic piece.
The potassium tantalate-niobate ceramic chip prepared by the method has the characteristics of large volume, high purity, good crystallization and the like. Experiments show that the potassium tantalate niobate ceramic plate also has the advantage of high dielectric constant, and the dielectric constant can be adjusted according to the adjustment of the adding proportion of the tantalum pentoxide and the niobium pentoxide.
Thus, in a second aspect, a potassium tantalate niobate ceramic sheet is obtained by the above-described preparation method.
In a third aspect, the dielectric constant adjusting method of the potassium tantalate-niobate ceramic chip comprises the preparation method of the potassium tantalate-niobate ceramic chip with the adjustable dielectric constant, wherein the dielectric constant of the potassium tantalate-niobate ceramic chip is adjusted by adjusting the molar ratio of tantalum pentoxide to niobium pentoxide.
The dielectric constant is a macroscopic physical quantity reflecting the polarization behavior of a dielectric, and the stronger the polarization capability of the dielectric under the action of an electric field, the larger the dielectric constant. The dielectric capacitor has the limitation that the energy storage density is low, and the improvement of the energy storage density is the research focus of the dielectric capacitor, while the high dielectric constant and the high dielectric strength are the key points for realizing the high energy storage density of the dielectric material. The ferroelectric ceramic with high dielectric constant can be applied to large-capacity capacitors, high-frequency micro capacitors, high-voltage capacitors, multilayer ceramic capacitors and the like, and the nonlinear change of the dielectric constant along with an external field can be applied to dielectric amplifiers, phase shifters and the like. Therefore, in the fourth aspect of the present invention, a use of the above potassium tantalate niobate ceramic sheet in a dielectric capacitor is provided.
The invention has the beneficial effects that:
1. the preparation method selects a proper amount of high-purity tantalum oxide, niobium oxide and an excessive potassium carbonate reagent, uniformly mixes the tantalum oxide, the niobium oxide and the excessive potassium carbonate reagent, synthesizes KTN polycrystal material, and then prepares the ceramic material by using the KTN polycrystal material as a raw material, thereby ensuring the high purity of the potassium tantalate-niobate sintered ceramic.
2. The invention adopts the technical steps of ball milling, drying, grinding and sieving, wax frying, granulation, tabletting, glue discharging, sintering to form porcelain and the like, and is simple, efficient and energy-saving.
3. The invention designs a sintering procedure aiming at the preparation of potassium tantalate niobate ceramic, has accurate time and speed of temperature rise, heat preservation and temperature reduction, effectively avoids the generation of impurities and ensures the high performance of the material.
4. The high-purity KTN ceramic wafer prepared by the method has the size of 3 cm in diameter and 3 mm in thickness, and is beneficial to processing to meet the size requirement of device application.
5. The dielectric constant value of the KTN material is adjusted by adjusting the stoichiometric proportion of the reaction raw materials, the regularity between the KTN material and the KTN material is obtained by repeated experiments, and the potassium tantalate niobate ceramic chip with the corresponding dielectric constant can be prepared according to the requirements of devices.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, are included to provide a further understanding of the invention, and are incorporated in and constitute a part of this specification, illustrate exemplary embodiments of the invention and together with the description serve to explain the invention and not to limit the invention.
Fig. 1 shows XRD patterns of KTN ceramic sheets of different compositions prepared in accordance with an embodiment of the present invention.
Fig. 2 is a photograph of a KTN ceramic sheet of different composition prepared in an embodiment of the present invention.
Fig. 3 is a comparison graph of the highest dielectric constant values of KTN ceramic sheets of different compositions prepared in accordance with an embodiment of the present invention.
Detailed Description
It is to be understood that the following detailed description is exemplary and is intended to provide further explanation of the invention as claimed. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of exemplary embodiments according to the invention. As used herein, the singular forms "a", "an" and "the" are intended to include the plural forms as well, and it should be understood that when the terms "comprises" and/or "comprising" are used in this specification, they specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof, unless the context clearly indicates otherwise.
In view of the defects of small size, low performance and the like of the existing potassium tantalate niobate ceramic, the invention provides a preparation method of a potassium tantalate niobate ceramic chip with adjustable dielectric constant.
The invention provides a typical implementation mode of a potassium tantalate niobate ceramic chip with adjustable dielectric constant, which comprises the steps of sintering tantalum pentoxide, niobium pentoxide and potassium carbonate to obtain a polycrystalline material, crushing and grinding the polycrystalline material, adding a binder to carry out wax frying granulation, and then sequentially carrying out dry pressing into sheets, heating and glue discharging and sintering into porcelain to obtain the potassium tantalate niobate ceramic chip; wherein, the potassium carbonate is added in excess, the sintering pre-synthesis temperature is 700-800 ℃, and the sintering process of the sintered ceramic is carried out according to a set temperature program.
According to the invention, a polycrystalline material is formed by sintering and pre-synthesizing (700-800 ℃), and the polycrystalline material is used as a raw material to prepare the potassium tantalate-niobate ceramic chip, so that the reduction of the purity can be avoided. According to the invention, excessive potassium carbonate is added, so that the stoichiometric ratio of KTN can be avoided, and the large-size and high-performance potassium tantalate-niobate ceramic chip can be obtained through the matching of wax frying granulation, dry pressing into pieces, heating and glue discharging and sintering into ceramic. The ceramic is sintered by setting a temperature program, so that impurities can be avoided, and the growth and hard agglomeration of crystal grains can be avoided, thereby ensuring the performance of the potassium tantalate niobate ceramic chip.
The set temperature program refers to heating to a set temperature, carrying out heat preservation sintering, and then cooling; wherein, in the process of heating to the set temperature, the process is divided into at least two sections of heating processes, and the heat preservation is needed for a period of time between the adjacent heating processes. In some embodiments of this embodiment, the set temperature program is: heating the mixture to 450-550 ℃ for 1.5-2.5 h at room temperature, heating the mixture to 1250-1300 ℃ for 5-7 h, then preserving heat for 8-10 h, and finally naturally cooling the mixture to room temperature. The potassium tantalate niobate ceramic chip obtained by the sintering procedure can be better free from impurity generation, and simultaneously, the growth and hard agglomeration of crystal grains are avoided, so that the performance of the potassium tantalate niobate ceramic chip is ensured. The room temperature refers to the temperature of an indoor environment, and is generally 15-30 ℃.
In some examples of this embodiment, the amount of potassium carbonate added is 1.15 to 1.25 times the theoretical amount of potassium carbonate. The stoichiometric ratio of KTN can be better ensured. The addition amount of the potassium carbonate refers to the actual addition amount of the potassium carbonate for preparing the target potassium tantalate niobate ceramic chip, and the theoretical amount of the potassium carbonate refers to the theoretical addition amount of the potassium carbonate for preparing the target potassium tantalate niobate ceramic chip.
In some examples of this embodiment, the sintering pre-synthesis time is 10 to 15 hours.
In some examples of this embodiment, tantalum pentoxide, niobium pentoxide, and potassium carbonate are mixed together, briquetted, and then presynthesized by sintering.
In some examples of this embodiment, the polycrystalline material is crushed and ground by: and adding the polycrystal material into a dispersion solvent for ball milling, drying, grinding and sieving. And adding a dispersion solution for wet milling to avoid the influence of fragments generated by ball milling on purity. The dispersion solvent is preferably alcohol.
The wax-frying granulation is that the binder is heated and melted, the ground polycrystal material is added and mixed under the stirring condition, then the mixture is sieved, and the binder is solidified when the mixture is sieved and cooled, so that granules are formed.
In some examples of this embodiment, the temperature of the heating and the discharging is 450 to 550 ℃. The glue discharging effect is better, and the performance of the potassium tantalate niobate ceramic plate can be better ensured. The rubber discharging time is preferably 3-5 h.
In another embodiment of the invention, the potassium tantalate niobate ceramic plate is obtained by the preparation method.
In a third embodiment of the invention, a method for adjusting the dielectric constant of a potassium tantalate-niobate ceramic sheet is provided, which comprises the above method for preparing the potassium tantalate-niobate ceramic sheet with adjustable dielectric constant, and the dielectric constant of the potassium tantalate-niobate ceramic sheet is adjusted by adjusting the molar ratio of tantalum pentoxide to niobium pentoxide.
In some examples of this embodiment, the molar ratio of tantalum to niobium is 1:0.25 to 4. Research shows that in the molar ratio range, the dielectric constant of the potassium tantalate-niobate ceramic plate is changed regularly along with the adjustment of the molar ratio, and particularly, the dielectric constant is changed more obviously when the molar ratio of tantalum to niobium is adjusted within the range of 2: 3-3: 2.
In a fourth embodiment of the invention, the application of the potassium tantalate niobate ceramic chip in a dielectric capacitor is provided.
In order to make the technical solutions of the present invention more clearly understood by those skilled in the art, the technical solutions of the present invention will be described in detail below with reference to specific embodiments.
Example 1: the preparation method of the KTN ceramic sheet material generally adopts a solid-phase process, and comprises the following specific steps: according to formula KTa0.2Nb0.8O3Weighing 0.1mol of high-purity Ta according to the stoichiometric ratio of chemical reaction2O5Reagent 44.20g and 0.4mol of high-purity Nb2O5106.30g reagent, because potassium carbonate is volatile during the high temperature sintering reaction, the excessive high purity K is weighed2CO30.6mol of reagent and 82.80g of weight. Mixing the three raw materials, putting the mixture into a mixer to mix for 30 hours, completely mixing the raw materials uniformly, briquetting and sintering the mixture, and carrying out sintering pre-synthesis on the KTN polycrystal material at the constant temperature of 750 ℃ for 12 hours. Crushing the polycrystal material, adding alcohol as a dispersing solvent, carrying out ball milling, taking out the polycrystal material after 48 hours, drying at the constant temperature of 60 ℃ for 40 hours, then grinding into fine powder, and sieving by using a 60-mesh sieve. And adding paraffin wax into the screened fine powder as an adhesive, frying the wax for 2 hours to ensure that the fine powder is fully and uniformly mixed, and quickly sieving and granulating the fine powder by using a 60-mesh sieve after the wax frying is finished so as to ensure that the powder particles are uniform. Placing the granulated powder into a corresponding rulerIn a steel die, pressing the powder into a cylindrical sheet with the diameter of 3 cm and the thickness of 3 mm by a hydraulic machine, and then carrying out glue removal on the pressed sheet material at the constant temperature of 500 ℃ for 4 hours. And (3) carrying out high-temperature sintering after the binder removal is finished, wherein the sintering procedure comprises the steps of heating the room temperature to 500 ℃ for 2 hours, heating the 500 ℃ to 1260 ℃ for 6 hours, keeping the temperature for 9 hours, and finally cooling to the room temperature. After 500 ℃, the heating rate is reduced because the slow temperature rise is favorable for the synthesis to be fully performed after the high-temperature reaction starts to be performed. And finally obtaining the high-quality KTN ceramic wafer with regular appearance and good density, as shown in figures 1-2. The highest dielectric constant value is 1.22 multiplied by 10 under the measurement condition of different temperatures of 10kHz4As shown in fig. 3.
Example 2: the ceramic sheet was prepared by the same procedure as above except for the difference of KTa0.4Nb0.6O3Weighing 0.2mol of high-purity Ta according to the stoichiometric ratio of chemical reaction2O588.35g of reagent and 0.3mol of high-purity Nb2O579.75g of reagent. Finally sintering to obtain KTa0.4Nb0.6O3The ceramic material is shown in figures 1-2. The highest dielectric constant value is 1.45 multiplied by 10 under the measurement condition of different temperatures of 10kHz4As shown in fig. 3.
Example 3: the ceramic sheet was prepared by the same procedure as above except for the difference of KTa0.6Nb0.4O3Weighing 0.3mol of high-purity Ta according to the stoichiometric ratio of chemical reaction2O5132.55g of reagent and 0.2mol of high-purity Nb2O553.15g of reagent. Finally sintering to obtain KTa0.6Nb0.4O3The ceramic material is shown in figures 1-2. The highest dielectric constant value is 2.53 multiplied by 10 under the measurement condition of different temperatures of 10kHz4As shown in fig. 3.
Example 4: the ceramic sheet was prepared by the same procedure as above except for the difference of KTa0.8Nb0.2O3Weighing 0.4mol of high-purity Ta according to the stoichiometric ratio of chemical reaction2O5176.70g of reagent and 0.1mol of high-purity Nb2O526.60g of reagent. Finally sintering to obtain KTa0.8Nb0.2O3The ceramic material is shown in figures 1-2. The highest dielectric constant value is 2.89 x 10 under the measurement condition of different temperatures of 10kHz4As shown in fig. 3.
The phase structure of the KTN ceramic sheet prepared in the embodiments 1 to 4 of the present invention was tested by an EMPYREAN X-ray diffractometer manufactured by parnacaceae, netherlands, and the results are shown in fig. 1, which indicates that the phase of the material is completely coincident with potassium tantalate niobate, no impurity phase is generated, the crystallinity of the reaction product is good, and the purity is high.
Fig. 2 is a photograph of the KTN ceramic sheets prepared in examples 1 to 4 of the present invention, and it can be seen that the ceramic sheets have smooth and regular shapes, good ceramic density, and a size of 3 cm in diameter.
Dielectric constant of the KTN ceramic sheets prepared in examples 1 to 4 of the present invention was measured by a dielectric temperature spectrum measuring system using a bridge method, and the characterization of the dielectric constant was achieved by measuring the dielectric capacitance, and the results are shown in fig. 3, which shows that the highest dielectric constant values of the potassium tantalate niobate ceramic sheets with different components are different, KTa0.2Nb0.8O3And KTa0.4Nb0.6O3，KTa0.6Nb0.4O3And KTa0.8Nb0.2O3The highest dielectric constant values of the two groups are not much different, from KTa0.4Nb0.6O3To KTa0.6Nb0.4O3The highest dielectric constant value is obviously increased, so that the adjustable range of the dielectric property in the component range is larger.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. A preparation method of a potassium tantalate niobate ceramic chip with adjustable dielectric constant is characterized in that tantalum pentoxide, niobium pentoxide and potassium carbonate are sintered and pre-synthesized to obtain a polycrystalline material, the polycrystalline material is crushed and ground, then a binder is added for wax frying and granulation, and then the polycrystalline material is sequentially subjected to dry pressing into pieces, heating and glue discharging, and sintering into ceramic to obtain the potassium tantalate niobate ceramic chip; wherein, the potassium carbonate is added in excess, the sintering pre-synthesis temperature is 700-800 ℃, and the sintering process of the sintered ceramic is carried out according to a set temperature program.
2. The method for preparing the potassium tantalate niobate ceramic sheet with adjustable dielectric constant as claimed in claim 1, wherein the temperature setting procedure is as follows: heating the mixture to 450-550 ℃ for 1.5-2.5 h at room temperature, heating the mixture to 1250-1300 ℃ for 5-7 h, then preserving heat for 8-10 h, and finally naturally cooling the mixture to room temperature.
3. The method for preparing the potassium tantalate-niobate ceramic sheet with adjustable dielectric constant of claim 1, wherein the addition amount of the potassium carbonate is 1.15-1.25 times of the theoretical amount of the potassium carbonate.
4. The method for preparing the potassium tantalate-niobate ceramic sheet with adjustable dielectric constant of claim 1, wherein the tantalum pentoxide, the niobium pentoxide and the potassium carbonate are mixed uniformly, pressed into a compact, and then sintered to be pre-synthesized.
5. The method for preparing the potassium tantalate niobate ceramic sheet with adjustable dielectric constant as claimed in claim 1, wherein the process of crushing and grinding the polycrystalline material comprises: and adding the polycrystal material into a dispersion solvent for ball milling, drying, grinding and sieving.
6. The method for preparing the potassium tantalate-niobate ceramic sheet with adjustable dielectric constant of claim 1, wherein the sintering pre-synthesis time is 10-15 h;
or the heating and glue discharging temperature is 450-550 ℃.
7. A method for adjusting the dielectric constant of a potassium tantalate niobate ceramic sheet, which is characterized by comprising the method for preparing the potassium tantalate niobate ceramic sheet with the adjustable dielectric constant of any one of claims 1 to 6, wherein the dielectric constant of the potassium tantalate niobate ceramic sheet is adjusted by adjusting the molar ratio of tantalum pentoxide to niobium pentoxide.
8. The method for adjusting the dielectric constant of the potassium tantalate niobate ceramic sheet as claimed in claim 7, wherein the molar ratio of tantalum to niobium is 1: 0.25-4; preferably, the molar ratio of tantalum to niobium is 2:3 to 3: 2.
9. A potassium tantalate niobate ceramic sheet, characterized by being obtained by the production method as claimed in any one of claims 1 to 6.
10. Use of the potassium tantalate niobate ceramic sheet of claim 9 in a dielectric capacitor.
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