CN107140968B - High-temperature lead-free piezoelectric ceramic and preparation method thereof - Google Patents
High-temperature lead-free piezoelectric ceramic and preparation method thereof Download PDFInfo
- Publication number
- CN107140968B CN107140968B CN201710330695.3A CN201710330695A CN107140968B CN 107140968 B CN107140968 B CN 107140968B CN 201710330695 A CN201710330695 A CN 201710330695A CN 107140968 B CN107140968 B CN 107140968B
- Authority
- CN
- China
- Prior art keywords
- hours
- feo
- temperature
- polarization
- drying
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Fee Related
Links
- 239000000919 ceramic Substances 0.000 title claims abstract description 25
- 238000002360 preparation method Methods 0.000 title description 14
- 230000010287 polarization Effects 0.000 claims abstract description 34
- 238000000034 method Methods 0.000 claims abstract description 8
- 238000009768 microwave sintering Methods 0.000 claims abstract description 7
- 239000000463 material Substances 0.000 claims description 21
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 20
- 238000000498 ball milling Methods 0.000 claims description 20
- 238000001035 drying Methods 0.000 claims description 20
- WMWLMWRWZQELOS-UHFFFAOYSA-N bismuth(iii) oxide Chemical compound O=[Bi]O[Bi]=O WMWLMWRWZQELOS-UHFFFAOYSA-N 0.000 claims description 15
- 239000002994 raw material Substances 0.000 claims description 15
- 230000002194 synthesizing effect Effects 0.000 claims description 15
- 230000005684 electric field Effects 0.000 claims description 11
- 229910002915 BiVO4 Inorganic materials 0.000 claims description 10
- 229910052782 aluminium Inorganic materials 0.000 claims description 10
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 10
- AYJRCSIUFZENHW-UHFFFAOYSA-L barium carbonate Chemical compound [Ba+2].[O-]C([O-])=O AYJRCSIUFZENHW-UHFFFAOYSA-L 0.000 claims description 10
- RKTYLMNFRDHKIL-UHFFFAOYSA-N copper;5,10,15,20-tetraphenylporphyrin-22,24-diide Chemical compound [Cu+2].C1=CC(C(=C2C=CC([N-]2)=C(C=2C=CC=CC=2)C=2C=CC(N=2)=C(C=2C=CC=CC=2)C2=CC=C3[N-]2)C=2C=CC=CC=2)=NC1=C3C1=CC=CC=C1 RKTYLMNFRDHKIL-UHFFFAOYSA-N 0.000 claims description 7
- 238000009694 cold isostatic pressing Methods 0.000 claims description 5
- 229910052593 corundum Inorganic materials 0.000 claims description 5
- 238000005469 granulation Methods 0.000 claims description 5
- 230000003179 granulation Effects 0.000 claims description 5
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 claims description 5
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 5
- 239000000843 powder Substances 0.000 claims description 5
- 229910000029 sodium carbonate Inorganic materials 0.000 claims description 5
- CDBYLPFSWZWCQE-UHFFFAOYSA-L sodium carbonate Substances [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 claims description 5
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims description 5
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 5
- 230000000737 periodic effect Effects 0.000 claims description 4
- 238000013329 compounding Methods 0.000 claims description 2
- 230000015572 biosynthetic process Effects 0.000 abstract description 3
- 230000028161 membrane depolarization Effects 0.000 abstract description 3
- 239000000203 mixture Substances 0.000 abstract description 3
- 238000003786 synthesis reaction Methods 0.000 abstract description 2
- 238000000462 isostatic pressing Methods 0.000 abstract 1
- 230000007547 defect Effects 0.000 description 10
- 230000000694 effects Effects 0.000 description 6
- 238000005245 sintering Methods 0.000 description 6
- 229910002902 BiFeO3 Inorganic materials 0.000 description 5
- 229910010293 ceramic material Inorganic materials 0.000 description 4
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 229910052709 silver Inorganic materials 0.000 description 3
- 239000004332 silver Substances 0.000 description 3
- 230000002411 adverse Effects 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 238000007747 plating Methods 0.000 description 2
- 229910052573 porcelain Inorganic materials 0.000 description 2
- 230000004044 response Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 150000001875 compounds Chemical group 0.000 description 1
- 230000008878 coupling Effects 0.000 description 1
- 238000010168 coupling process Methods 0.000 description 1
- 238000005859 coupling reaction Methods 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005272 metallurgy Methods 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/26—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 ferrites
- C04B35/2675—Other ferrites containing rare earth metals, e.g. rare earth ferrite garnets
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
- C04B35/62605—Treating the starting powders individually or as mixtures
- C04B35/62645—Thermal treatment of powders or mixtures thereof other than sintering
- C04B35/62675—Thermal treatment of powders or mixtures thereof other than sintering characterised by the treatment temperature
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/64—Burning or sintering processes
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/009—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone characterised by the material treated
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/45—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
- C04B41/50—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials
- C04B41/51—Metallising, e.g. infiltration of sintered ceramic preforms with molten metal
- C04B41/5116—Ag or Au
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/80—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone of only ceramics
- C04B41/81—Coating or impregnation
- C04B41/85—Coating or impregnation with inorganic materials
- C04B41/88—Metals
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3201—Alkali metal oxides or oxide-forming salts thereof
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3205—Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
- C04B2235/3215—Barium oxides or oxide-forming salts thereof
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3217—Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
- C04B2235/3239—Vanadium oxides, vanadates or oxide forming salts thereof, e.g. magnesium vanadate
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
- C04B2235/3251—Niobium oxides, niobates, tantalum oxides, tantalates, or oxide-forming salts thereof
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3281—Copper oxides, cuprates or oxide-forming salts thereof, e.g. CuO or Cu2O
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3298—Bismuth oxides, bismuthates or oxide forming salts thereof, e.g. zinc bismuthate
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Ceramic Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Structural Engineering (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Compositions Of Oxide Ceramics (AREA)
Abstract
A high-temperature lead-free piezoelectric ceramic is characterized by having a general composition formula: (1-x)Bi0.96La0.06FeO3‑xBa0.97(Na1/ 2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4(ii) a WhereinxRepresents a molar fraction of 0.05<x<0.4. The ceramic is prepared by combining stepwise synthesis, isostatic pressing, microwave sintering and polarization methods with different voltage types, and the series of products are environment-friendly, have good stability, excellent piezoelectric property and high temperature stability, have the depolarization temperature of more than 500 ℃, and are suitable for being applied in the high-temperature field.
Description
Technical Field
The invention relates to a lead-free piezoelectric ceramic material applied in the high temperature field, in particular to an ABO3Bi of perovskite structure0.96La0.06FeO3A lead-free piezoelectric ceramic with high temperature stability and a preparation method thereof.
Background
The high-temperature piezoelectric sensor has the advantages of simple structure, small volume, quick response, long service life and external interference
Small size, and can be widely used in atomic energy, aerospace, automobile, metallurgy, petrochemical industry, etc
And measuring dynamic and impact. With the rapid development of these industrial fields, the operating environment of these electronic devices is very harsh, and higher requirements are put on the upper limit of the operating temperature of the piezoelectric material. At present, the high-temperature piezoelectric material and the device mainly use single crystal materials, have complex production process and high price and are not beneficial to large-scale application. The piezoelectric ceramic can be prepared into devices in any shapes, and has simple preparation process and lower cost. Therefore, the development of high-temperature piezoelectric ceramic materials having excellent properties has been urgently required.
BiFeO3The base piezoelectric ceramic has excellent piezoelectric performance and high-temperature stability, is a green and environment-friendly lead-free material system, and has wide application prospect in the field of high-temperature piezoelectric sensors. Due to BiFeO3Bi for sintering system ceramics3+Volatile, Fe3+Ion valence change (Fe)3+→Fe2+) The oxygen vacancy is generated, so that the room-temperature leakage current is large, and the polarization is difficult, so that the application of the system ceramic in the field of piezoelectric materials is less. The defect is BiFeO3The important characteristics of the base piezoelectric ceramics are also key factors for determining the piezoelectric ferroelectric performance. The variation of chemical bonds between the defects and adjacent ions, the coupling between the defects and electric domains, and the internal electric field formed by the defects have obvious influence on the insulativity, the piezoelectric property and the temperature characteristic of the material. Meanwhile, doping effects and atmosphere sintering are closely related to the generation of defects. However, these defects are unstable at high temperatures and are unstable to BiFeO3The piezoelectric properties and high temperature stability of the base piezoelectric ceramics are adversely affected. Therefore, the functional effect of the defects is utilized to optimize the defect structure and improve the piezoelectric property, the temperature characteristic and the high-temperature conductance of the ceramic, and the method is a new technical support in the current piezoelectric ceramic development.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a high-temperature lead-free piezoelectric ceramic and a preparation method thereof. The ceramic material has excellent piezoelectric performance, high temperature stability and depolarization temperature not lower than 500 ≥oC. Environment-friendly, good stability, good piezoelectric property, and is suitable for 500oC or above. The method has the advantages of simple preparation process and low cost.
The technical scheme for realizing the purpose of the invention is as follows:
a high-temperature lead-free piezoelectric ceramic has a general composition formula:
(1-x)Bi0.96La0.06FeO3-xBa0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4(ii) a WhereinxRepresents a molar fraction of 0.05<x<0.4。
The preparation method of the high-temperature lead-free piezoelectric ceramic comprises the following steps:
(1) first step with electronic grade Bi2O3、Fe2O3And La2O3As raw material, according to the stoichiometric formula Bi0.96La0.06FeO3Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing Bi with a three-way distortion structure in a high-alumina crucible at 720 ℃ for 2 hours0.96La0.06FeO3A main crystalline phase;
(2) second step with electronic grade Ta2O5、BaCO3、CuO、Na2CO3And Al2O3As raw material, according to the stoichiometric formula Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3Preparing materials; ball milling for 12 hours by using absolute ethyl alcohol as a medium, drying, and pre-synthesizing Ba with a tetragonal distortion structure in a high-aluminum crucible at 1050 ℃ for 2 hours0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3A main crystalline phase;
(3) the third step is to use electronic grade Bi2O3And V2O5As raw material, according to the stoichiometric formula BiVO4Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing BiVO in a high-aluminum crucible at 550 ℃ for 2 hours4A main crystalline phase;
(4) the fourth step is to synthesize the synthesized Bi0.96La0.06FeO3、Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3、BiVO4Powder according to (1-x)Bi0.96La0.06FeO3-xBa0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3
+0.05BiVO4Stoichiometric compounding of whereinxRepresents a molar fraction of 0.05<x<0.4）；
(5) Ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and adding 5% PVA for granulation; cold isostatic pressing under 150MPa pressure;
(6) microwave sintering, keeping the temperature at 850-;
(7) and (3) polarization, namely applying 10 periodic sawtooth wave circular polarization with a polarization electric field of 5000V/mm and a frequency of 1Hz, and then applying 15 periodic square wave circular polarization with a polarization electric field of 6000V/mm and a frequency of 1Hz and a polarization temperature of 100 ℃.
The method is carried out by adding BiFeO3The A position of the compound is added with 0.06 of La to form stable three-side structure distortion transition phase boundary composition Bi0.96La0.06FeO3Adding Ba of low tetragonal distortion structure0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3(wherein the A site is added with a complex small ionic radius (Na)1/2Al1/2)2+Forming a mesoscopic tetragonal structure), constructing a trigonal-tetragonal quasi homomorphic phase boundary, and superposing the mesoscopic structure of the nano-polarity micro-region to generate a charged domain wall structure and amplify piezoelectric response;
BiVO is added simultaneously in the method4Sintering is assisted, and the volatilization of Bi at the A position is compensated; and the sawtooth wave-square wave high-voltage cyclic polarization is combined to induce the formation of defective dipoles, and simultaneously, a domain wall nail-removing effect is generated, a dipole polarization enhancement effect and a stable electric domain effect corresponding to the polarity can be generated, so that the adverse effect of high-temperature charged defects is overcome, and a positive effect can be generated, and therefore, the piezoelectric performance and the high-temperature stability can be improved simultaneously.
The method adopts step-by-step synthesis and microwave sintering, and has the advantages of low sintering temperature, short heat preservation time, fine and uniform crystal grains and high density.
The ceramic material has excellent piezoelectric performance, high temperature stability and depolarization temperature not lower than 500 ≥oC. Environment-friendly, good stability, good piezoelectric property, and is suitable for 500oC or above. The method has the advantages of simple preparation process and low cost.
Detailed Description
The present invention will be further illustrated with reference to the following specific examples, which are not intended to limit the invention thereto.
Example 1:
the preparation comprises the following components: 0.96Bi0.96La0.06FeO3-0.04Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4The high-temperature lead-free piezoelectric ceramic.
The preparation method comprises the following steps:
(1) first step with electronic grade Bi2O3、Fe2O3And La2O3As raw material, according to the stoichiometric formula Bi0.96La0.06FeO3Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing Bi with a three-way distortion structure in a high-alumina crucible at 720 ℃ for 2 hours0.96La0.06FeO3A main crystalline phase;
(2) second step with electronic grade Ta2O5、BaCO3、CuO、Na2CO3And Al2O3As raw material, according to the stoichiometric formula Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3Preparing materials; ball milling for 12 hours by using absolute ethyl alcohol as a medium, drying, and pre-synthesizing Ba with a tetragonal distortion structure in a high-aluminum crucible at 1050 ℃ for 2 hours0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3A main crystalline phase;
(3) the third step is to use electronic grade Bi2O3And V2O5As raw material, according to the chemical formulaQuantitative BiVO4Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing BiVO in a high-aluminum crucible at 550 ℃ for 2 hours4A main crystalline phase;
(4) the fourth step is to synthesize the synthesized Bi0.96La0.06FeO3、Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3、BiVO4Powder of 0.96Bi0.96La0.06FeO3-0.04Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4Proportioning in a stoichiometric mode;
(5) ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and adding 5% PVA for granulation; cold isostatic pressing under 150MPa pressure;
(6) microwave sintering, keeping the temperature at 850 ℃ for 20 minutes, sintering into porcelain, and plating silver electrodes on two sides;
(7) and (3) polarization, namely applying 10 sawtooth wave circular polarization with a polarization electric field of 5000V/mm and a frequency of 1Hz, and then applying 15 square wave circular polarization with a polarization electric field of 6000V/mm, a frequency of 1Hz and a polarization temperature of 100 ℃.
The piezoelectric properties of the piezoelectric ceramics were measured by IRE standard after the obtained sample was left to stand for 24 hours. The performance measurements are as follows:
| d 33(pC/N) | Qm | k p | εr | tanδ(%) | T d(°C) | T c(°C) |
| 142 | 165 | 0.28 | 582 | 1.05 | 587 | 673。 |
example 2:
the preparation comprises the following components: 0.9Bi0.96La0.06FeO3-0.1Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4The high-temperature lead-free piezoelectric ceramic.
The preparation method comprises the following steps:
(1) first step with electronic grade Bi2O3、Fe2O3And La2O3As raw material, according to the stoichiometric formula Bi0.96La0.06FeO3Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing Bi with a three-way distortion structure in a high-alumina crucible at 720 ℃ for 2 hours0.96La0.06FeO3A main crystalline phase;
(2) second step with electronic grade Ta2O5、BaCO3、CuO、Na2CO3And Al2O3As raw material, according to the stoichiometric formula Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3Preparing materials; ball milling for 12 hours by using absolute ethyl alcohol as a medium, drying, and pre-synthesizing Ba with a tetragonal distortion structure in a high-aluminum crucible at 1050 ℃ for 2 hours0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3A main crystalline phase;
(3) the third step is to use electronic grade Bi2O3And V2O5As raw material, according to the stoichiometric formula BiVO4Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing BiVO in a high-aluminum crucible at 550 ℃ for 2 hours4A main crystalline phase;
(4) the fourth step is to synthesize the synthesized Bi0.96La0.06FeO3、Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3、BiVO4Powder of 0.9Bi0.96La0.06FeO3-0.1Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4Proportioning in a stoichiometric mode;
(5) ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and adding 5% PVA for granulation; cold isostatic pressing under 150MPa pressure;
(6) microwave sintering, keeping the temperature at 880 ℃ for 20 minutes, sintering into porcelain, and plating silver electrodes on two sides;
(7) and (3) polarization, namely applying 10 sawtooth wave circular polarization with a polarization electric field of 5000V/mm and a frequency of 1Hz, and then applying 15 square wave circular polarization with a polarization electric field of 6000V/mm, a frequency of 1Hz and a polarization temperature of 100 ℃.
The piezoelectric properties of the piezoelectric ceramics were measured by IRE standard after the obtained sample was left to stand for 24 hours.
The performance measurements are as follows:
| d 33(pC/N) | Qm | k p | εr | tanδ(%) | T d(°C) | T c(°C) |
| 172 | 109 | 0.33 | 625 | 1.16 | 523 | 638。 |
example 3:
the preparation comprises the following components: 0.88Bi0.96La0.06FeO3-0.12Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4The high-temperature lead-free piezoelectric ceramic.
The preparation method comprises the following steps:
(1) first step with electronic grade Bi2O3、Fe2O3And La2O3As raw material, according to the stoichiometric ratioFormula Bi0.96La0.06FeO3Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing Bi with a three-way distortion structure in a high-alumina crucible at 720 ℃ for 2 hours0.96La0.06FeO3A main crystalline phase;
(2) second step with electronic grade Ta2O5、BaCO3、CuO、Na2CO3And Al2O3As raw material, according to the stoichiometric formula Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3Preparing materials; ball milling for 12 hours by using absolute ethyl alcohol as a medium, drying, and pre-synthesizing Ba with a tetragonal distortion structure in a high-aluminum crucible at 1050 ℃ for 2 hours0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3A main crystalline phase;
(3) the third step is to use electronic grade Bi2O3And V2O5As raw material, according to the stoichiometric formula BiVO4Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing BiVO in a high-aluminum crucible at 550 ℃ for 2 hours4A main crystalline phase;
(4) the fourth step is to synthesize the synthesized Bi0.96La0.06FeO3、Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3、BiVO4Powder of 0.88Bi0.96La0.06FeO3-0.12Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4Proportioning in a stoichiometric mode;
(5) ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and adding 5% PVA for granulation; cold isostatic pressing under 150MPa pressure;
(6) microwave sintering, wherein the temperature is kept at 890 ℃ for 20 minutes, the ceramic is sintered, and electrodes are plated with silver on two sides;
(7) and (3) polarization, namely applying 10 sawtooth wave circular polarization with a polarization electric field of 5000V/mm and a frequency of 1Hz, and then applying 15 square wave circular polarization with a polarization electric field of 6000V/mm, a frequency of 1Hz and a polarization temperature of 100 ℃.
The piezoelectric properties of the piezoelectric ceramics were measured by IRE standard after the obtained sample was left to stand for 24 hours.
The performance measurements are as follows:
| d 33(pC/N) | Qm | k p | εr | tanδ(%) | T d(°C) | T c(°C) |
| 179 | 101 | 0.36 | 711 | 1.12 | 518 | 597。 |
the contents of the present invention will be further clearly understood from the examples given above, but they are not intended to limit the present invention.
Claims (2)
1. A high-temperature lead-free piezoelectric ceramic is characterized by comprising the following general formula:
(1-x)Bi0.96La0.06FeO3-xBa0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4(ii) a WhereinxRepresents a molar fraction of 0.05<x<0.4。
2. The method for preparing a high-temperature lead-free piezoelectric ceramic according to claim 1, comprising the steps of:
(1) first step with electronic grade Bi2O3、Fe2O3And La2O3As raw material, according to the stoichiometric formula Bi0.96La0.06FeO3Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing Bi with a three-way distortion structure in a high-alumina crucible at 720 ℃ for 2 hours0.96La0.06FeO3A main crystalline phase;
(2) second step with electronic grade Ta2O5、BaCO3、CuO、Na2CO3And Al2O3As raw material, according to the stoichiometric formula Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3Preparing materials; ball milling for 12 hours by using absolute ethyl alcohol as a medium, drying, and pre-synthesizing Ba with a tetragonal distortion structure in a high-aluminum crucible at 1050 ℃ for 2 hours0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3A main crystalline phase;
(3) the third step is to use electronic grade Bi2O3And V2O5As raw material, according to the stoichiometric formula BiVO4Preparing materials; ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and pre-synthesizing BiVO in a high-aluminum crucible at 550 ℃ for 2 hours4A main crystalline phase;
(4) the fourth step is to synthesize the synthesized Bi0.96La0.06FeO3、Ba0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3、BiVO4Powder according to (1-x)Bi0.96La0.06FeO3-xBa0.97(Na1/2Al1/2)0.03(Cu1/3Ta2/3)O3+0.05BiVO4Stoichiometric compounding of whereinxRepresents a molar fraction of 0.05<x<0.4；
(5) Ball milling for 12 hours by taking absolute ethyl alcohol as a medium, drying, and adding 5% PVA for granulation; cold isostatic pressing under 150MPa pressure;
(6) microwave sintering, keeping the temperature at 850-;
(7) and (3) polarization, namely applying 10 periodic sawtooth wave circular polarization with a polarization electric field of 5000V/mm and a frequency of 1Hz, and then applying 15 periodic square wave circular polarization with a polarization electric field of 6000V/mm and a frequency of 1Hz and a polarization temperature of 100 ℃.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201710330695.3A CN107140968B (en) | 2017-05-11 | 2017-05-11 | High-temperature lead-free piezoelectric ceramic and preparation method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201710330695.3A CN107140968B (en) | 2017-05-11 | 2017-05-11 | High-temperature lead-free piezoelectric ceramic and preparation method thereof |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN107140968A CN107140968A (en) | 2017-09-08 |
| CN107140968B true CN107140968B (en) | 2020-04-17 |
Family
ID=59777798
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201710330695.3A Expired - Fee Related CN107140968B (en) | 2017-05-11 | 2017-05-11 | High-temperature lead-free piezoelectric ceramic and preparation method thereof |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN107140968B (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110550954A (en) * | 2019-09-18 | 2019-12-10 | 昆明贵研新材料科技有限公司 | Core-shell lanthanum-doped bismuth ferrite/silicon dioxide composite ceramic and preparation method thereof |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6692721B2 (en) * | 2002-01-15 | 2004-02-17 | Samsung Electro-Mechanics Co., Ltd. | Method for preparing barium titanate powder by oxalate synthesis |
| CN102249678A (en) * | 2011-06-16 | 2011-11-23 | 桂林电子科技大学 | Lead-free and bismuth-free piezoelectric ceramics |
| CN104649660A (en) * | 2015-03-10 | 2015-05-27 | 桂林电子科技大学 | Bismuth-ferrite-based high-temperature piezoelectric and dielectric energy storage ceramic and preparation method thereof |
| CN104961451A (en) * | 2015-07-01 | 2015-10-07 | 西北工业大学 | Bismuth lanthanum ferrite ceramic and preparation method thereof |
| CN105948736A (en) * | 2016-05-03 | 2016-09-21 | 哈尔滨工业大学 | Lithium oxide-trivalent oxide co-doped ABO3 structure-based high-temperature stability piezoelectric ceramic material and preparation method thereof |
-
2017
- 2017-05-11 CN CN201710330695.3A patent/CN107140968B/en not_active Expired - Fee Related
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6692721B2 (en) * | 2002-01-15 | 2004-02-17 | Samsung Electro-Mechanics Co., Ltd. | Method for preparing barium titanate powder by oxalate synthesis |
| CN102249678A (en) * | 2011-06-16 | 2011-11-23 | 桂林电子科技大学 | Lead-free and bismuth-free piezoelectric ceramics |
| CN104649660A (en) * | 2015-03-10 | 2015-05-27 | 桂林电子科技大学 | Bismuth-ferrite-based high-temperature piezoelectric and dielectric energy storage ceramic and preparation method thereof |
| CN104961451A (en) * | 2015-07-01 | 2015-10-07 | 西北工业大学 | Bismuth lanthanum ferrite ceramic and preparation method thereof |
| CN105948736A (en) * | 2016-05-03 | 2016-09-21 | 哈尔滨工业大学 | Lithium oxide-trivalent oxide co-doped ABO3 structure-based high-temperature stability piezoelectric ceramic material and preparation method thereof |
Non-Patent Citations (1)
| Title |
|---|
| Dielectric aging behavior in A-site hybrid-doped BaTiO3 ceramics;T.Sarrein 等;《Current Applied Physics》;20110316;第S90-S94页 * |
Also Published As
| Publication number | Publication date |
|---|---|
| CN107140968A (en) | 2017-09-08 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| Yang et al. | A novel lead-free ceramic with layered structure for high energy storage applications | |
| Li et al. | Simultaneously enhanced energy storage density and efficiency in novel BiFeO3-based lead-free ceramic capacitors | |
| Chen et al. | Room temperature multiferroic properties of Ni-doped Aurivillus phase Bi5Ti3FeO15 | |
| Zhu et al. | Piezoelectric, ferroelectric and ferromagnetic properties of (1− x) BiFeO 3–x BaTiO 3 lead-free ceramics near morphotropic phase boundary | |
| CN110272270B (en) | Bismuth ferrite-barium titanate-based high-temperature lead-free piezoelectric ceramic with low dielectric loss and high-temperature stability and preparation method thereof | |
| Chi et al. | Manifestation of ferroelectromagnetism in multiferroic BiMnO3 | |
| Thongbai et al. | Improved dielectric and nonlinear electrical properties of fine‐grained CaCu3Ti4O12 ceramics prepared by a glycine‐nitrate process | |
| Fang et al. | Structure and electrical properties of bismuth and sodium modified SrBi2Nb2O9 ferroelectric ceramics | |
| Zhang et al. | Preparation and Microwave Dielectric Properties of Ultra‐low Temperature Sintering Ceramics in K 2 O–MoO 3 Binary System | |
| Hussain et al. | High‐temperature piezoelectric properties of 0‐3 type CaBi4Ti4O15: x wt% BiFeO3 composites | |
| Cen et al. | Structural, ferroelectric and piezoelectric properties of Mn-modified BiFeO 3–BaTiO 3 high-temperature ceramics | |
| Lv et al. | Enhanced Electrical Properties of Quenched (1–x) Bi1–y Sm y FeO3–x BiScO3 Lead-Free Ceramics | |
| Supriya | Highly tunable multifunctional rare earth based Bi0. 5-xCexNa0. 5TiO3 perovskites via site selective doping engineering | |
| Pang et al. | A new multiferroic ternary solid solution system of BiFeO3–Pb (Fe1/2Nb1/2) O3–PbTiO3 | |
| Xu et al. | Dielectric properties of Zn-doped CCTO ceramics by sol-gel method | |
| Kaswan et al. | Crystal structure refinement, enhanced magnetic and dielectric properties of Na0. 5Bi0. 5TiO3 modified Bi0. 8Ba0. 2FeO3 ceramics | |
| CN111170735B (en) | Ceramic material with high electric energy storage efficiency and preparation method thereof | |
| JP2009242230A (en) | Method for producing alkali niobate perovskite crystal | |
| CN107140968B (en) | High-temperature lead-free piezoelectric ceramic and preparation method thereof | |
| Chupakhina et al. | Synthesis, structure and dielectric properties of new ceramics with K2NiF4-type structure | |
| CN115093216A (en) | Barium titanate doped lead-free ceramic with high electrostriction and low hysteresis and preparation method thereof | |
| CN110791732B (en) | Preparation method of nickel-doped bismuth ferrite film system material | |
| CN103193469B (en) | Nine-layer-structure titanium iron bismuth cobalt oxide multiferroic ceramic material and preparation method thereof | |
| Yao et al. | Microstructure, ferro-piezoelectric and thermal stability of SiO 2 modified BiFeO 3–BaTiO 3 high temperature piezoceramics | |
| CN109970443B (en) | Rubidium and cerium co-doped bismuth calcium niobate based high-temperature piezoelectric ceramic and preparation method thereof |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| GR01 | Patent grant | ||
| GR01 | Patent grant | ||
| CF01 | Termination of patent right due to non-payment of annual fee |
Granted publication date: 20200417 |