CN117164357B - Five-element high-power piezoelectric ceramic material and preparation method thereof - Google Patents
Five-element high-power piezoelectric ceramic material and preparation method thereof Download PDFInfo
- Publication number
- CN117164357B CN117164357B CN202310002993.5A CN202310002993A CN117164357B CN 117164357 B CN117164357 B CN 117164357B CN 202310002993 A CN202310002993 A CN 202310002993A CN 117164357 B CN117164357 B CN 117164357B
- Authority
- CN
- China
- Prior art keywords
- piezoelectric ceramic
- mixing
- powder
- milling
- ball
- 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.)
- Active
Links
- 229910010293 ceramic material Inorganic materials 0.000 title claims abstract description 29
- 238000002360 preparation method Methods 0.000 title abstract description 11
- 239000000463 material Substances 0.000 claims abstract description 17
- KOPBYBDAPCDYFK-UHFFFAOYSA-N caesium oxide Chemical compound [O-2].[Cs+].[Cs+] KOPBYBDAPCDYFK-UHFFFAOYSA-N 0.000 claims abstract description 15
- 229910001942 caesium oxide Inorganic materials 0.000 claims abstract description 15
- 229910001289 Manganese-zinc ferrite Inorganic materials 0.000 claims abstract description 14
- JIYIUPFAJUGHNL-UHFFFAOYSA-N [O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[Mn++].[Mn++].[Mn++].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Zn++].[Zn++] Chemical compound [O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[Mn++].[Mn++].[Mn++].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Fe+3].[Zn++].[Zn++] JIYIUPFAJUGHNL-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229910019653 Mg1/3Nb2/3 Inorganic materials 0.000 claims abstract description 13
- 239000000126 substance Substances 0.000 claims abstract description 8
- 239000000843 powder Substances 0.000 claims description 87
- 239000000919 ceramic Substances 0.000 claims description 79
- 238000002156 mixing Methods 0.000 claims description 51
- 238000000498 ball milling Methods 0.000 claims description 42
- 239000002994 raw material Substances 0.000 claims description 35
- 238000001035 drying Methods 0.000 claims description 34
- 239000000203 mixture Substances 0.000 claims description 33
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 27
- 239000002245 particle Substances 0.000 claims description 27
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 27
- 238000001354 calcination Methods 0.000 claims description 23
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 22
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 22
- ZKATWMILCYLAPD-UHFFFAOYSA-N niobium pentoxide Chemical compound O=[Nb](=O)O[Nb](=O)=O ZKATWMILCYLAPD-UHFFFAOYSA-N 0.000 claims description 22
- 238000005245 sintering Methods 0.000 claims description 21
- 238000005303 weighing Methods 0.000 claims description 21
- 239000011572 manganese Substances 0.000 claims description 20
- ACNRWWUEFJNUDD-UHFFFAOYSA-N lead(2+);distiborate Chemical compound [Pb+2].[Pb+2].[Pb+2].[O-][Sb]([O-])([O-])=O.[O-][Sb]([O-])([O-])=O ACNRWWUEFJNUDD-UHFFFAOYSA-N 0.000 claims description 18
- 238000000227 grinding Methods 0.000 claims description 12
- LEDMRZGFZIAGGB-UHFFFAOYSA-L strontium carbonate Chemical compound [Sr+2].[O-]C([O-])=O LEDMRZGFZIAGGB-UHFFFAOYSA-L 0.000 claims description 11
- 229910000018 strontium carbonate Inorganic materials 0.000 claims description 11
- FFQALBCXGPYQGT-UHFFFAOYSA-N 2,4-difluoro-5-(trifluoromethyl)aniline Chemical compound NC1=CC(C(F)(F)F)=C(F)C=C1F FFQALBCXGPYQGT-UHFFFAOYSA-N 0.000 claims description 9
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 9
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 claims description 8
- 239000011656 manganese carbonate Substances 0.000 claims description 8
- 229910000016 manganese(II) carbonate Inorganic materials 0.000 claims description 8
- 238000000034 method Methods 0.000 claims description 8
- GHPGOEFPKIHBNM-UHFFFAOYSA-N antimony(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Sb+3].[Sb+3] GHPGOEFPKIHBNM-UHFFFAOYSA-N 0.000 claims description 7
- 239000011777 magnesium Substances 0.000 claims description 7
- ZBSCCQXBYNSKPV-UHFFFAOYSA-N oxolead;oxomagnesium;2,4,5-trioxa-1$l^{5},3$l^{5}-diniobabicyclo[1.1.1]pentane 1,3-dioxide Chemical compound [Mg]=O.[Pb]=O.[Pb]=O.[Pb]=O.O1[Nb]2(=O)O[Nb]1(=O)O2 ZBSCCQXBYNSKPV-UHFFFAOYSA-N 0.000 claims description 7
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 6
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 6
- 239000011230 binding agent Substances 0.000 claims description 6
- 239000011248 coating agent Substances 0.000 claims description 6
- 238000000576 coating method Methods 0.000 claims description 6
- 239000003921 oil Substances 0.000 claims description 6
- 238000005498 polishing Methods 0.000 claims description 6
- 238000003825 pressing Methods 0.000 claims description 6
- 230000001681 protective effect Effects 0.000 claims description 6
- 229910052710 silicon Inorganic materials 0.000 claims description 6
- 239000010703 silicon Substances 0.000 claims description 6
- 229910052709 silver Inorganic materials 0.000 claims description 6
- 239000004332 silver Substances 0.000 claims description 6
- ADCOVFLJGNWWNZ-UHFFFAOYSA-N antimony trioxide Inorganic materials O=[Sb]O[Sb]=O ADCOVFLJGNWWNZ-UHFFFAOYSA-N 0.000 claims description 3
- 238000004519 manufacturing process Methods 0.000 claims description 3
- YEAUATLBSVJFOY-UHFFFAOYSA-N tetraantimony hexaoxide Chemical compound O1[Sb](O2)O[Sb]3O[Sb]1O[Sb]2O3 YEAUATLBSVJFOY-UHFFFAOYSA-N 0.000 claims description 3
- 238000005065 mining Methods 0.000 claims description 2
- 239000010955 niobium Substances 0.000 claims 7
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims 4
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims 2
- 239000011787 zinc oxide Substances 0.000 claims 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims 1
- 229910052748 manganese Inorganic materials 0.000 claims 1
- 229910052758 niobium Inorganic materials 0.000 claims 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims 1
- 230000000052 comparative effect Effects 0.000 description 11
- 230000008878 coupling Effects 0.000 description 6
- 238000010168 coupling process Methods 0.000 description 6
- 238000005859 coupling reaction Methods 0.000 description 6
- 230000005684 electric field Effects 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- XMFOQHDPRMAJNU-UHFFFAOYSA-N lead(II,IV) oxide Inorganic materials O1[Pb]O[Pb]11O[Pb]O1 XMFOQHDPRMAJNU-UHFFFAOYSA-N 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- 239000011701 zinc Substances 0.000 description 3
- 229910000859 α-Fe Inorganic materials 0.000 description 3
- 229910002056 binary alloy Inorganic materials 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000009661 fatigue test Methods 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- 229910052451 lead zirconate titanate Inorganic materials 0.000 description 1
- HFGPZNIAWCZYJU-UHFFFAOYSA-N lead zirconate titanate Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ti+4].[Zr+4].[Pb+2] HFGPZNIAWCZYJU-UHFFFAOYSA-N 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000026683 transduction Effects 0.000 description 1
- 238000010361 transduction Methods 0.000 description 1
Landscapes
- Compositions Of Oxide Ceramics (AREA)
Abstract
The invention relates to a five-membered high-power piezoelectric ceramic material and a preparation method thereof, wherein the piezoelectric ceramic material is prepared by taking Pb1‑ xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/ 3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3 as a basic formula and adding a manganese-zinc ferrite material and cesium oxide, and the total chemical formula of the piezoelectric ceramic material is ：Pb1‑xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/ 2Nb1/2)O3-m2MnZnFe2O4-m3 cesium oxide. The five-element high-power piezoelectric ceramic material has high quality factors (Qm), kp and d33, and the high Qm is not at the cost of reducing kp and d 33.
Description
Technical Field
The invention relates to the technical field of piezoelectric ceramic materials, in particular to a five-element high-power piezoelectric ceramic material and a preparation method thereof.
Background
In recent years, high-power transducer devices and piezoelectric materials have taken an increasing importance in the industrial and scientific fields, and are widely used in sensors, drivers, transformers, various types of underwater acoustic, electroacoustic and ultrasonic transducers, and the like. In the age of rapid development of technology and industry in China at present, some key formulas and production process technologies for lead zirconate titanate-based piezoelectric ceramic materials which are applied on a large scale are still monopolized abroad, so that the cost for applying the piezoelectric ceramic materials in various fields in China is extremely high and is limited by people.
Most piezoelectric ceramics are difficult to realize practical application in the field of high-power transduction (P8 material series) devices, and are mainly expressed in the following aspects: first, the mechanical quality factor Qm (the mechanical quality factor Qm is as high as possible, usually more than 1300), the electromechanical coupling coefficient kp, the dielectric loss tan δ, and the piezoelectric constant d33 (the piezoelectric constant d33 is as high as possible, usually more than 300 pC/N), the fatigue resistance, and other key performance parameters are required, but it is sometimes difficult to achieve both high mechanical quality factor Qm and high piezoelectric constant d33 at the same time, for example, the high Qm is obtained at the cost of lowering kp and d 33.
Disclosure of Invention
In order to overcome the above technical problems in the prior art, a first object of the present invention is to provide a five-membered high-power piezoelectric ceramic material, wherein the piezoelectric ceramic material is prepared by adding a manganese-zinc ferrite material and cesium oxide in a Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3 -doped manner, and the piezoelectric ceramic material has a general chemical formula of ：Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3-m2MnZnFe2O4-m3 cesium oxide, wherein x=0.04-0.12, y=0.2, z=0.2, m1=0.02, m2=0.1-1.5%, m3=0.02-0.5%, and the percentages of m2 and m3 are mole percentages.
Compared with the prior art, the invention has the beneficial effects that: the five-element high-power piezoelectric ceramic material has good comprehensive performance parameters, and the quality factor (Qm) of the whole product is improved by introducing the Mn-Zn ferrite material, so that the quality factor of the material is improved. Meanwhile, the material improves the fatigue resistance of the product by introducing cesium oxide. In addition, the five-element high-power piezoelectric ceramic material has high quality factors (Qm), kp and d33, and the high Qm is not at the cost of reducing kp and d 33.
The second aim of the invention is to provide a preparation method of a five-membered high-power piezoelectric ceramic material, which comprises the following steps:
s1, respectively weighing Pb 3O4、SrCO3、ZrO2、TiO2 according to stoichiometric ratio, mixing the Pb 3O4、SrCO3、ZrO2、TiO2 into raw material mixture, then ball-milling the mixture for 6 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 1-3 mu m, drying wet powder, calcining the wet powder at 1000-1100 ℃ for 2-4 hours, and then repeating the ball-milling mixture and the drying to obtain Pb 1-xSrxZr0.5Ti0.5O3 lead strontium zirconate titanate two-element system piezoelectric ceramic powder;
s2, respectively weighing Pb 3O4、MnCO3、Sb2O3 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing for 6 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 3-5 mu m, drying wet powder, calcining at 800-900 ℃ for 2-4 hours, and then repeating ball-milling and mixing and drying to obtain Pb (Mn 1/3Sb2/3)O3 lead antimonate piezoelectric ceramic powder;
s3, respectively weighing Pb 3O4、MgO、Nb2O5 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing with alcohol or water as medium to make D50 particle size of 1-3 μm, drying wet powder, calcining at 1000-1060 ℃ for 2-4 hours, and repeating ball-milling and mixing and drying to obtain Pb (Mg 1/3Nb2/3)O3 lead magnesium niobate piezoelectric ceramic powder;
S4, respectively weighing Pb 3O4、Sb2O3、Nb2O5 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing with alcohol or water as medium to obtain D50 particle size of 3-5 μm, drying wet powder, calcining at 800-900 ℃ for 2-4 hours, and repeating ball-milling and mixing and calcining to obtain Pb (Sb 1/2Nb1/2)O3 lead antimonate piezoelectric ceramic powder;
s5, respectively weighing Fe 2O3、Mn3O4 and ZnO according to a stoichiometric ratio (the proportion of the manganese zinc ferrite material is Fe 2O356～56.5％,Mn3O4 -42.5%, the balance is ZnO, and the total amount is 100%), mixing to prepare raw material mixture, then ball-milling and mixing with alcohol or water as a medium to enable the D50 particle size to be 1-2 mu m, drying wet powder, calcining at 900-1000 ℃ for 2-4 hours, and then repeating ball-milling and mixing and calcining to obtain MnZnFe 2O4 manganese zinc ferrite powder;
s6, respectively weighing Pb 1-xSrxZr0.5Ti0.5O3 lead strontium zirconate titanate piezoelectric ceramic powder obtained in the step S1, pb (Mn 1/3Sb2/3)O3 lead antimonate piezoelectric ceramic powder obtained in the step S2, pb (Mg 1/3Nb2/3)O3 lead antimonate piezoelectric ceramic powder obtained in the step S3, pb (Sb 1/2Nb1/2)O3 lead antimonate piezoelectric ceramic powder obtained in the step S4, mnZnFe 2O4 manganese zinc ferrite powder obtained in the step S5) and cesium oxide according to stoichiometric proportions, mixing the materials to prepare a raw material mixture, ball-milling the raw material mixture for 12 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 0.5-1.1 mu m, and calcining the wet powder at 1000-1060 ℃ for 2-4 hours after drying to obtain five-element high-power piezoelectric ceramic powder;
S7, grinding the five-element high-power piezoelectric ceramic powder obtained in the step S6, then ball-milling for 10 hours by taking alcohol or water as a medium, grinding the powder to D90 with the particle size of 1.0-1.5 mu m, mixing the dried powder with a binder, granulating, and cold-pressing the powder under the pressure of 300-400MPa to form a wafer with the diameter of 10mm and the thickness of 0.6-1.0mm, thereby obtaining a ceramic blank; sintering the ceramic blank in a protective atmosphere by adopting a powder embedding method in air at normal pressure, wherein the sintering temperature is 1235 ℃, and the sintering time is 2 hours to obtain a piezoelectric ceramic sample;
and S8, coating silver electrodes on two ends of the piezoelectric ceramic sample prepared in the step S7 after polishing treatment, and then placing the piezoelectric ceramic sample in silicon oil at 110 ℃, and preserving heat and pressure for 30 minutes under a direct current field of 5kV/mm to obtain the quinary high-power piezoelectric ceramic.
Further, the temperature rising rate of the sintering temperature in the step S7 is 3-5 ℃/min. The slow heating rate of 3-5 ℃/min is beneficial to improving the quality factor of the material.
Compared with the prior art, the invention has the beneficial effects that:
The invention is to synthesize Pb 1-xSrxZr0.5Ti0.5O3 lead strontium zirconate titanate powder, pb (Mn 1/3Sb2/3)O3 lead antimonate powder, pb (Mg 1/3Nb2/3)O3 lead magnesium niobate powder, pb (Sb 1/2Nb1/2)O3 lead antimonate powder), use it to prepare the high-power piezoelectric ceramic material of five-element system further, it is based on lead strontium zirconate titanate of binary system, increase lead antimonate manganese, lead magnesium niobate, lead antimonate niobate and other ternary system, this preparation method is compared with traditional to mix Pb 3O4、SrCO3、ZrO2、TiO2、MnCO3、Nb2O5, sb 2O3, mgO these compounds and get together and synthesize five-element system substance, can control each component more accurately, will not produce miscellaneous phase, and this preparation method also further ensures the high-power piezoelectric ceramic material of five-element system prepared has high quality factor (Qm), kp and d33. In addition, this preparation method does not adopt the high-cost mode such as the hot-pressed sintering, the cost is low, it is easier to produce in batches.
Detailed Description
The present invention will now be further described with reference to specific embodiments, it being apparent that some, but not all embodiments of the invention are described. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
A ferroelectric analyzer (TF 2000 analyzer, aixacct, aachen, germany) is adopted to perform a fatigue test and a unidirectional fatigue test for the electric hysteresis loop and the field strain performance of a sample, the electric field adopts a unidirectional triangular wave electric field with the amplitude of 10kV/mm and the frequency of 50Hz, and the strain performance of the sample is tested after 1000 loading cycles.
The starting materials Pb3O4、SrCO3、ZrO2、TiO2、MnCO3、Sb2O3、MgO、Nb2O5、Fe2O3、Mn3O4、ZnO and the like used in the following examples of the present invention were chemically pure or analytically pure. The piezoelectric ceramic provided by the embodiment of the invention is prepared according to the following method, and the difference is that x, y, z, m, m2 and m3 are different in value.
The five-membered high-power piezoelectric ceramic material is prepared by taking Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3 as a basic formula and adding a doped manganese zinc ferrite material and cesium oxide, wherein the general chemical formula of the piezoelectric ceramic material is ：Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3-m2MnZnFe2O4-m3 cesium oxide, x=0.04-0.12, y=0.2, z=0.2, m1=0.02, m2=0.1-1.5, m3=0.02-0.5, and the percentages of m2 and m3 are mole percent. The preparation method of the five-membered high-power piezoelectric ceramic material comprises the following steps:
S1, respectively weighing Pb 3O4、SrCO3、ZrO2、TiO2 according to stoichiometric ratio, mixing the Pb 3O4、SrCO3、ZrO2、TiO2 into raw material mixture, then ball-milling the mixture for 6 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 1-3 mu m, drying wet powder, calcining the wet powder at 1000-1100 ℃ for 2-4 hours, and then repeating the ball-milling mixture and the drying to obtain Pb 1-xSrxZr0.5Ti0.5O3 lead strontium zirconate titanate binary system piezoelectric ceramic;
S2, respectively weighing Pb 3O4、MnCO3、Sb2O3 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing for 6 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 3-5 mu m, drying wet powder, calcining at 800-900 ℃ for 2-4 hours, and then repeating ball-milling and mixing and drying to obtain Pb (Mn 1/3Sb2/3)O3 lead antimonate piezoelectric ceramic;
S3, respectively weighing Pb 3O4、MgO、Nb2O5 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing with alcohol or water as medium to obtain D50 particle size of 3-5 μm, drying wet powder, calcining at 1000-1060 ℃ for 2-4 hours, and repeating ball-milling and mixing and drying to obtain Pb (Mg 1/3Nb2/3)O3 lead magnesium niobate piezoelectric ceramic;
S4, respectively weighing Pb 3O4、Sb2O3、Nb2O5 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing with alcohol or water as medium to obtain D50 particle size of 3-5 μm, drying wet powder, calcining at 800-900 ℃ for 2-4 hours, and repeating ball-milling and mixing and drying to obtain Pb (Sb 1/2Nb1/2)O3 lead antimonate piezoelectric ceramic;
S5, respectively weighing Fe 2O3、Mn3O4 and ZnO according to a stoichiometric ratio (the proportion of the manganese zinc ferrite material is Fe 2O356～56.5％,Mn3O4 -42.5%, the balance is ZnO, and the total amount is 100%), mixing to prepare raw material mixture, then ball-milling and mixing with alcohol or water as a medium to enable the D50 particle size to be 1-2 mu m, drying wet powder, calcining at 900-1000 ℃ for 2-4 hours, and then repeating ball-milling and mixing and drying to obtain MnZnFe 2O4 manganese zinc ferrite;
S6, respectively weighing Pb 1-xSrxZr0.5Ti0.5O3 lead strontium zirconate titanate piezoelectric ceramic obtained in the step S1, pb (Mn 1/3Sb2/3)O3 lead antimonate piezoelectric ceramic obtained in the step S2, pb (Mg 1/3Nb2/3)O3 lead magnesium niobate piezoelectric ceramic obtained in the step S3, pb (Sb 1/2Nb1/2)O3 lead antimonate piezoelectric ceramic obtained in the step S5), mnZnFe 2O4 manganese zinc ferrite and cesium oxide) obtained in the step S4 according to stoichiometric ratio, mixing the materials to prepare raw material mixture, then ball-milling the raw material mixture for 12 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 0.5-1.1 mu m, drying wet powder, and calcining at 1000-1060 ℃ for 2-4 hours to obtain five-membered high-power piezoelectric ceramic powder;
S7, grinding the five-element high-power piezoelectric ceramic powder obtained in the step S6, then ball-milling for 10 hours by taking alcohol or water as a medium, grinding the powder to D90 with the particle size of 1.0-1.5 mu m, mixing the dried powder with a binder, granulating, and cold-pressing the powder into a wafer with the diameter of 10mm and the thickness of 0.6-1.0mm under the pressure of 300-400MPa to obtain a ceramic blank; sintering the ceramic blank in a protective atmosphere by adopting a powder embedding method in air at normal pressure, wherein the sintering temperature is 1235 ℃, the heating rate is 3-5 ℃/min, and the sintering time is 2 hours, so that a piezoelectric ceramic sample is obtained;
and S8, coating silver electrodes on two ends of the piezoelectric ceramic sample prepared in the step S7 after polishing treatment, and then placing the piezoelectric ceramic sample in silicon oil at 110 ℃, and preserving heat and pressure for 30 minutes under a direct current field of 5kV/mm to obtain the quinary high-power piezoelectric ceramic.
The preparation methods employed in comparative examples 1 to 3 are conventional preparation methods, which are specifically as follows:
comparative example 1:
S1, accurately weighing ,Pb3O4、SrCO3、ZrO2、TiO2、MnCO3、Sb2O3、MgO、Nb2O5 and other raw materials according to a chemical formula Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3(, wherein x=0.04, y=0.20, z=0.20 and m1=0.02), mixing the raw materials to prepare a raw material mixture, ball-milling the raw material mixture with alcohol or water as a medium to obtain a D50 particle size of 3-5 mu m, drying wet powder, and calcining at 1000-1060 ℃ for 2-4 hours to obtain Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3 piezoelectric ceramic powder;
s2, grinding the five-element high-power piezoelectric ceramic powder obtained in the step S1 of the comparative example 1, then ball-milling for 10 hours by taking alcohol or water as a medium, grinding the powder to obtain powder with the D90 particle size of 1.0-1.5 mu m, mixing the dried powder with a binder, granulating, and cold-pressing the powder into a wafer with the diameter of 10mm and the thickness of 0.6-1.0mm under the pressure of 300-400MPa to obtain a ceramic blank; sintering the ceramic blank in a protective atmosphere by adopting a powder embedding method in air at normal pressure, wherein the sintering temperature is 1235 ℃, the heating rate is 3-5 ℃/min, and the sintering time is 2 hours, so that a piezoelectric ceramic sample is obtained;
And S3, coating silver electrodes on two ends of the piezoelectric ceramic sample prepared in the step S2 of the comparative example 1 after polishing treatment, and then placing the piezoelectric ceramic sample in silicon oil at 110 ℃, and preserving heat and pressure for 30 minutes under a direct current electric field of 5kV/mm to obtain the five-membered high-power piezoelectric ceramic.
Comparative example 2:
S1, accurately weighing ,Pb3O4、SrCO3、ZrO2、TiO2、MnCO3、Sb2O3、MgO、Nb2O5 and other raw materials according to a chemical formula Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3(, wherein x=0.08, y=0.20, z=0.20 and m1=0.02), mixing the raw materials to prepare a raw material mixture, ball-milling the raw material mixture with alcohol or water as a medium to obtain a D50 particle size of 3-5 mu m, drying wet powder, and calcining at 1000-1060 ℃ for 2-4 hours to obtain Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3 piezoelectric ceramic powder;
s2, grinding the five-element high-power piezoelectric ceramic powder obtained in the step S1 of the comparative example 2, then ball-milling for 10 hours by taking alcohol or water as a medium, grinding the powder to obtain powder with the D90 particle size of 1.0-1.5 mu m, mixing the dried powder with a binder, granulating, and cold-pressing the powder into a wafer with the diameter of 10mm and the thickness of 0.6-1.0mm under the pressure of 300-400MPa to obtain a ceramic blank; sintering the ceramic blank in a protective atmosphere by adopting a powder embedding method in air at normal pressure, wherein the sintering temperature is 1235 ℃, the heating rate is 3-5 ℃/min, and the sintering time is 2 hours, so that a piezoelectric ceramic sample is obtained;
And S3, coating silver electrodes on two ends of the piezoelectric ceramic sample prepared in the step S2 of the comparative example 2 after polishing treatment, and then placing the piezoelectric ceramic sample in silicon oil at 110 ℃, and preserving heat and pressure for 30 minutes under a direct current electric field of 5kV/mm to obtain the five-membered high-power piezoelectric ceramic.
Comparative example 3:
S1, accurately weighing ,Pb3O4、SrCO3、ZrO2、TiO2、MnCO3、Sb2O3、MgO、Nb2O5 and other raw materials according to a chemical formula Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3(, wherein x=0.12, y=0.20, z=0.20 and m1=0.02), mixing the raw materials to prepare a raw material mixture, ball-milling the raw material mixture with alcohol or water as a medium to obtain a D50 particle size of 3-5 mu m, drying wet powder, and calcining at 1000-1060 ℃ for 2-4 hours to obtain Pb1-xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3 piezoelectric ceramic powder;
S2, grinding the five-element high-power piezoelectric ceramic powder obtained in the step S1 of the comparative example 3, then ball-milling for 10 hours by taking alcohol or water as a medium, grinding the powder to obtain powder with the D90 particle size of 1.0-1.5 mu m, mixing the dried powder with a binder, granulating, and cold-pressing the powder into a wafer with the diameter of 10mm and the thickness of 0.6-1.0mm under the pressure of 300-400MPa to obtain a ceramic blank; sintering the ceramic blank in a protective atmosphere by adopting a powder embedding method in air at normal pressure, wherein the sintering temperature is 1235 ℃, the heating rate is 3-5 ℃/min, and the sintering time is 2 hours, so that a piezoelectric ceramic sample is obtained;
And S3, coating silver electrodes on two ends of the piezoelectric ceramic sample prepared in the step S2 of the comparative example 3 after polishing treatment, and then placing the piezoelectric ceramic sample in silicon oil at 110 ℃, and preserving heat and pressure for 30 minutes under a direct current electric field of 5kV/mm to obtain the five-membered high-power piezoelectric ceramic.
Examples, comparative examples and corresponding test data
As can be seen from comparison of the test data of examples 1-3, that is, when x is in the range of (0.04-0.12), the dielectric constant, the electromechanical coupling coefficient kp, d33 (pC/N) and the Q value all show increasing trend as x increases. When x=0.08, the dielectric constant, the electromechanical coupling coefficient kp, d33 (pC/N) reach the maximum value, and the performance is optimal. When x exceeds 0.08, the dielectric constant, the electromechanical coupling coefficient kp and the d33 (pC/N) Q value all show a decreasing trend as x increases.
As can be seen from comparison of the test data of examples 4-6, the Mn-Zn ferrite material doped with m2 can greatly improve the Q value. That is, M2 has a tendency that the Q value increases and decreases with an increase in M2 in the range of (m2=0.1 to 1.5%). Equivalent m2=0.8%, reaches maximum value, Q value reaches 1350, and performance is optimal.
As can be seen from comparison of the test data of examples 7-9, cesium oxide doped, the fatigue resistance (strain attenuation) is improved; as m3 increases, fatigue (strain decay) is resisted. When m3=0.3%, the fatigue resistance (strain attenuation) reaches a maximum value, and when the strain attenuation is further increased, the fatigue resistance is reduced.
As can be seen from the above examples and comparison of test data: the dielectric constant, the electromechanical coupling coefficient kp and the d33 (pC/N) compressive strength tan delta (%) all show parabolic trend change, and then the dielectric constant, the electromechanical coupling coefficient kp, the d33 (pC/N), the Qm and the fatigue resistance of the piezoelectric ceramic are improved by matching with the Mn-Zn ferrite material and cesium oxide, so that the stability of the product quality is finally improved.
The foregoing is a further detailed description of the invention in connection with the preferred embodiments, and it is not intended that the invention be limited to the specific embodiments described. It will be apparent to those skilled in the art that several simple deductions or substitutions may be made without departing from the spirit of the invention, and these should be considered to be within the scope of the invention.
Claims (5)
1. The five-membered high-power piezoelectric ceramic material is characterized in that the piezoelectric ceramic material is prepared by taking Pb1- xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3 as a basic formula and adding a doped manganese zinc ferrite material and cesium oxide, wherein the total chemical formula of the piezoelectric ceramic material is ：Pb1- xSrxZr0.5Ti0.5O3-yPb(Mn1/3Sb2/3)O3-zPb(Mg1/3Nb2/3)O3-m1Pb(Sb1/2Nb1/2)O3-m2MnZnFe2O4-m3 cesium oxide, x=0.04-0.12, y=0.2, z=0.2, m1=0.02, m2=0.1-1.5, m3=0.02-0.5, and the percentages of m2 and m3 are mole percentages; the five-membered high-power piezoelectric ceramic material comprises the following raw materials: lead strontium zirconate titanate piezoelectric ceramic, lead manganese antimonate piezoelectric ceramic, lead magnesium niobate piezoelectric ceramic, lead niobium antimonate piezoelectric ceramic, manganese zinc ferrite and cesium oxide.
2. The five-membered high-power piezoelectric ceramic material according to claim 1, wherein: the manganese zinc ferrite comprises the following raw materials: iron oxide, manganese oxide and zinc oxide.
3. A method for preparing the five-membered high-power piezoelectric ceramic material according to claim 1, comprising the steps of:
S1, respectively weighing Pb 3O4、SrCO3、ZrO2、TiO2 according to stoichiometric ratio, mixing the Pb 3O4、SrCO3、ZrO2、TiO2 into raw material mixture, then ball-milling the mixture for 6 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 1-3 mu m, drying wet powder, calcining the wet powder at 1000-1100 ℃ for 2-4 hours, and then repeatedly ball-milling the mixture and drying the wet powder to obtain Pb 1-xSrxZr0.5Ti0.5O3 lead strontium zirconate titanate two-element system piezoelectric ceramic powder;
s2, respectively weighing Pb 3O4、MnCO3、Sb2O3 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing for 6 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 3-5 mu m, drying wet powder, calcining at 800-900 ℃ for 2-4 hours, and then repeating ball-milling and mixing and drying to obtain Pb (Mn 1/3Sb2/3)O3 lead antimonate piezoelectric ceramic powder;
s3, respectively weighing Pb 3O4、MgO、Nb2O5 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing with alcohol or water as medium to make D50 particle size of 1-3 μm, drying wet powder, calcining at 1000-1060 ℃ for 2-4 hours, and repeating ball-milling and mixing and drying to obtain Pb (Mg 1/3Nb2/3)O3 lead magnesium niobate piezoelectric ceramic powder;
s4, respectively weighing Pb 3O4、Sb2O3、Nb2O5 according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing with alcohol or water as medium to obtain D50 particle size of 3-5 μm, drying wet powder, calcining at 800-900 ℃ for 2-4 hours, and repeating ball-milling and mixing and drying to obtain Pb (Sb 1/2Nb1/2)O3 lead antimonate piezoelectric ceramic powder;
S5, respectively weighing Fe 2O3、Mn3O4 and ZnO according to stoichiometric ratio, mixing to prepare raw material mixture, ball-milling and mixing with alcohol or water as a medium to enable the D50 particle size to be 1-2 mu m, drying wet powder, calcining at 900-1000 ℃ for 2-4 hours, and repeating ball-milling and mixing and drying to obtain MnZnFe 2O4 manganese zinc ferrite powder;
s6, respectively weighing Pb 1-xSrxZr0.5Ti0.5O3 lead strontium zirconate titanate piezoelectric ceramic powder obtained in the step S1, pb (Mn 1/3Sb2/3)O3 lead antimonate piezoelectric ceramic powder obtained in the step S2, pb (Mg 1/3Nb2/3)O3 lead antimonate piezoelectric ceramic powder obtained in the step S3, pb (Sb 1/2Nb1/2)O3 lead antimonate piezoelectric ceramic powder obtained in the step S4, mnZnFe 2O4 manganese zinc ferrite powder obtained in the step S5) and cesium oxide according to stoichiometric proportions, mixing the materials to prepare a raw material mixture, ball-milling the raw material mixture for 12 hours by taking alcohol or water as a medium, enabling the D50 particle size to be 0.5-1.1 mu m, and calcining the wet powder at 1000-1060 ℃ for 2-4 hours after drying to obtain five-element high-power piezoelectric ceramic powder;
s7, grinding the five-element high-power piezoelectric ceramic powder obtained in the step S6, then ball-milling for 10 hours by taking alcohol or water as a medium, grinding the powder to D90 with the particle size of 1.0-1.5 mu m, mixing the dried powder with a binder, granulating, and cold-pressing to form a wafer under the pressure of 300-400MPa to obtain a required ceramic blank; sintering the ceramic blank in a protective atmosphere by adopting a powder embedding method in air at normal pressure, wherein the sintering temperature is 1235 ℃, and the sintering time is 2 hours to obtain a piezoelectric ceramic sample;
and S8, coating silver electrodes on two ends of the piezoelectric ceramic sample prepared in the step S7 after polishing treatment, and then placing the piezoelectric ceramic sample in silicon oil at 110 ℃, and preserving heat and pressure for 30 minutes under a direct current field of 5kV/mm to obtain the quinary high-power piezoelectric ceramic.
4. The method for producing a five-membered high-power piezoelectric ceramic material according to claim 3, wherein the wafer in step S7 has a diameter of 10mm and a thickness of 0.6 to 1.0mm.
5. The method for producing a five-membered high-power piezoelectric ceramic material according to claim 3, wherein the temperature rise rate of the sintering temperature in step S7 is 3 to 5 ℃/min.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202310002993.5A CN117164357B (en) | 2023-01-03 | 2023-01-03 | Five-element high-power piezoelectric ceramic material and preparation method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202310002993.5A CN117164357B (en) | 2023-01-03 | 2023-01-03 | Five-element high-power piezoelectric ceramic material and preparation method thereof |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN117164357A CN117164357A (en) | 2023-12-05 |
| CN117164357B true CN117164357B (en) | 2024-07-19 |
Family
ID=88934206
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202310002993.5A Active CN117164357B (en) | 2023-01-03 | 2023-01-03 | Five-element high-power piezoelectric ceramic material and preparation method thereof |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN117164357B (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN118652117B (en) * | 2024-05-28 | 2025-01-21 | 湖南省新化县鑫星电子陶瓷有限责任公司 | A multi-element piezoelectric ceramic sensor material and preparation method thereof |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1803708A (en) * | 2006-01-19 | 2006-07-19 | 湖北大学 | Low temperature sintered PMMSN titanic acid piezoelectric ceramic material and preparation method thereof |
Family Cites Families (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0788220B2 (en) * | 1986-07-02 | 1995-09-27 | 科学技術庁無機材質研究所長 | Manufacturing method of easily sinterable ceramic powder for high-density dielectric ceramics |
| JP5119176B2 (en) * | 2009-01-30 | 2013-01-16 | 東海ゴム工業株式会社 | Dielectric material manufacturing method and dielectric film manufactured thereby |
| JP5521957B2 (en) * | 2010-05-24 | 2014-06-18 | 三菱マテリアル株式会社 | Ferroelectric thin film and thin film capacitor using the ferroelectric thin film |
| PT2729179T (en) * | 2011-06-06 | 2020-11-25 | Starpharma Pty Ltd | Macromolecules |
-
2023
- 2023-01-03 CN CN202310002993.5A patent/CN117164357B/en active Active
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1803708A (en) * | 2006-01-19 | 2006-07-19 | 湖北大学 | Low temperature sintered PMMSN titanic acid piezoelectric ceramic material and preparation method thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| CN117164357A (en) | 2023-12-05 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN111302797B (en) | Potassium-sodium niobate-based leadless piezoelectric ceramic and preparation method thereof | |
| CN100465131C (en) | A kind of sodium potassium niobate lithium-based lead-free piezoelectric ceramics and preparation method thereof | |
| JP2001019542A (en) | Piezoelectric ceramics and piezoelectric devices using the same | |
| CN109553413B (en) | A textured piezoelectric ceramic and its preparation method and use | |
| CN102260079B (en) | A "receive/transmit" dual-purpose PZT-Pb(Sb2/3Mn1/3) ternary piezoelectric ceramic material and its preparation method | |
| CN117164357B (en) | Five-element high-power piezoelectric ceramic material and preparation method thereof | |
| CN115385683B (en) | A piezoelectric ceramic material with high Curie temperature and piezoelectric coefficient and preparation method thereof | |
| US20110017936A1 (en) | Piezoelectric ceramic and piezoelectric ceramic composition | |
| CN114133243A (en) | High-dielectric-constant high-voltage electric strain emission type piezoelectric ceramic material and preparation method thereof | |
| CN117326866B (en) | Cerium-manganese co-doped lead zirconate titanate-based piezoelectric ceramic material and preparation method thereof | |
| US3963631A (en) | Method of preparing ferroelectric ceramics | |
| CN115894020B (en) | A PMNZT-based piezoelectric ceramic with high voltage coefficient and its preparation method and application | |
| JP2884635B2 (en) | Piezoelectric ceramics and method of manufacturing the same | |
| CN112759390A (en) | Has high kpPSN-PZT piezoelectric ceramic and preparation method thereof | |
| CN114621009B (en) | Lead magnesium niobate-lead titanate-based piezoelectric ceramic material and preparation method thereof | |
| US3549536A (en) | Lead zirconate-titanate containing manganese additive | |
| CN105218090A (en) | Obvious anisotropic high-performance lead zirconates based piezoelectric ceramic materials of a kind of electromechanical coupling factor and preparation method thereof | |
| CN105218092B (en) | It is a kind of to be provided simultaneously with big displacement and low delayed lead zirconate titanate based piezoelectric ceramic materials and preparation method thereof | |
| CN103524129A (en) | Piezoceramic material for ultrasonic emission-type transducers and preparation method | |
| JP2884631B2 (en) | Piezoelectric ceramics and manufacturing method thereof | |
| KR101172797B1 (en) | manufacturing process of composition and the composition thereby for advanced piezoelectricity including CeO2 addition | |
| JP2866986B2 (en) | Piezoelectric ceramic composition | |
| CN116354718B (en) | Antimony manganese-lead zirconate titanate-based piezoelectric ceramic material and preparation method thereof | |
| CN117843363B (en) | A quaternary piezoelectric ceramic material and preparation method thereof | |
| CN114605150B (en) | High-density, low-loss and high-dielectric-constant 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 |