WO2005061413A1 - 圧電磁器およびその製造方法 - Google Patents
圧電磁器およびその製造方法 Download PDFInfo
- Publication number
- WO2005061413A1 WO2005061413A1 PCT/JP2004/019091 JP2004019091W WO2005061413A1 WO 2005061413 A1 WO2005061413 A1 WO 2005061413A1 JP 2004019091 W JP2004019091 W JP 2004019091W WO 2005061413 A1 WO2005061413 A1 WO 2005061413A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- oxide
- piezoelectric ceramic
- piezoelectric
- content
- perovskite
- Prior art date
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- 238000004519 manufacturing process Methods 0.000 title claims abstract description 11
- 229910052573 porcelain Inorganic materials 0.000 title abstract description 4
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims abstract description 16
- 239000000203 mixture Substances 0.000 claims description 51
- 239000000919 ceramic Substances 0.000 claims description 48
- 239000010955 niobium Substances 0.000 claims description 32
- 229910052721 tungsten Inorganic materials 0.000 claims description 31
- 239000010937 tungsten Substances 0.000 claims description 31
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 30
- 229910052758 niobium Inorganic materials 0.000 claims description 26
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 26
- 229910052715 tantalum Inorganic materials 0.000 claims description 26
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 26
- 229910000906 Bronze Inorganic materials 0.000 claims description 21
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 21
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 claims description 21
- 239000010974 bronze Substances 0.000 claims description 21
- KUNSUQLRTQLHQQ-UHFFFAOYSA-N copper tin Chemical compound [Cu].[Sn] KUNSUQLRTQLHQQ-UHFFFAOYSA-N 0.000 claims description 21
- 229910052700 potassium Inorganic materials 0.000 claims description 21
- 239000011591 potassium Substances 0.000 claims description 21
- 229910052760 oxygen Inorganic materials 0.000 claims description 20
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 18
- 239000001301 oxygen Substances 0.000 claims description 18
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- 239000011572 manganese Substances 0.000 claims description 16
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 14
- 229910052744 lithium Inorganic materials 0.000 claims description 14
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 12
- 229910052710 silicon Inorganic materials 0.000 claims description 12
- 239000010703 silicon Substances 0.000 claims description 12
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- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 11
- 229910017052 cobalt Inorganic materials 0.000 claims description 11
- 239000010941 cobalt Substances 0.000 claims description 11
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 11
- 229910052708 sodium Inorganic materials 0.000 claims description 11
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 10
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 10
- 229910052748 manganese Inorganic materials 0.000 claims description 10
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 9
- 229910052738 indium Inorganic materials 0.000 claims description 9
- 229910052759 nickel Inorganic materials 0.000 claims description 9
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- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 claims description 8
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 8
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- 229910052733 gallium Inorganic materials 0.000 claims description 8
- 229910052732 germanium Inorganic materials 0.000 claims description 8
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 claims description 8
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- 238000000034 method Methods 0.000 claims description 6
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- 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 description 11
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- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 8
- 229910052735 hafnium Inorganic materials 0.000 description 7
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 description 7
- AYJRCSIUFZENHW-UHFFFAOYSA-L barium carbonate Chemical compound [Ba+2].[O-]C([O-])=O AYJRCSIUFZENHW-UHFFFAOYSA-L 0.000 description 6
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 5
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 5
- 229910052791 calcium Inorganic materials 0.000 description 5
- 239000011575 calcium Substances 0.000 description 5
- 239000011777 magnesium Substances 0.000 description 5
- DEXFNLNNUZKHNO-UHFFFAOYSA-N 6-[3-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperidin-1-yl]-3-oxopropyl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C1CCN(CC1)C(CCC1=CC2=C(NC(O2)=O)C=C1)=O DEXFNLNNUZKHNO-UHFFFAOYSA-N 0.000 description 4
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- 229910052788 barium Inorganic materials 0.000 description 4
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- 229910052451 lead zirconate titanate Inorganic materials 0.000 description 4
- 229910052749 magnesium Inorganic materials 0.000 description 4
- 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 4
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- 238000005245 sintering Methods 0.000 description 4
- YLZOPXRUQYQQID-UHFFFAOYSA-N 3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-1-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]propan-1-one Chemical compound N1N=NC=2CN(CCC=21)CCC(=O)N1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F YLZOPXRUQYQQID-UHFFFAOYSA-N 0.000 description 3
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- 239000011656 manganese carbonate Substances 0.000 description 3
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- 229910000016 manganese(II) carbonate Inorganic materials 0.000 description 3
- XMWCXZJXESXBBY-UHFFFAOYSA-L manganese(ii) carbonate Chemical compound [Mn+2].[O-]C([O-])=O XMWCXZJXESXBBY-UHFFFAOYSA-L 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
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- 239000011787 zinc oxide Substances 0.000 description 2
- OHVLMTFVQDZYHP-UHFFFAOYSA-N 1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-2-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]ethanone Chemical compound N1N=NC=2CN(CCC=21)C(CN1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)=O OHVLMTFVQDZYHP-UHFFFAOYSA-N 0.000 description 1
- LDXJRKWFNNFDSA-UHFFFAOYSA-N 2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-1-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]ethanone Chemical compound C1CN(CC2=NNN=C21)CC(=O)N3CCN(CC3)C4=CN=C(N=C4)NCC5=CC(=CC=C5)OC(F)(F)F LDXJRKWFNNFDSA-UHFFFAOYSA-N 0.000 description 1
- JQMFQLVAJGZSQS-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-N-(2-oxo-3H-1,3-benzoxazol-6-yl)acetamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)NC1=CC2=C(NC(O2)=O)C=C1 JQMFQLVAJGZSQS-UHFFFAOYSA-N 0.000 description 1
- CONKBQPVFMXDOV-QHCPKHFHSA-N 6-[(5S)-5-[[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]methyl]-2-oxo-1,3-oxazolidin-3-yl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)C[C@H]1CN(C(O1)=O)C1=CC2=C(NC(O2)=O)C=C1 CONKBQPVFMXDOV-QHCPKHFHSA-N 0.000 description 1
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- DFGKGUXTPFWHIX-UHFFFAOYSA-N 6-[2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]acetyl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)C1=CC2=C(NC(O2)=O)C=C1 DFGKGUXTPFWHIX-UHFFFAOYSA-N 0.000 description 1
- LLQHSBBZNDXTIV-UHFFFAOYSA-N 6-[5-[[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]methyl]-4,5-dihydro-1,2-oxazol-3-yl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC1CC(=NO1)C1=CC2=C(NC(O2)=O)C=C1 LLQHSBBZNDXTIV-UHFFFAOYSA-N 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
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- 241000282693 Cercopithecidae Species 0.000 description 1
- NEAPKZHDYMQZCB-UHFFFAOYSA-N N-[2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]ethyl]-2-oxo-3H-1,3-benzoxazole-6-carboxamide Chemical compound C1CN(CCN1CCNC(=O)C2=CC3=C(C=C2)NC(=O)O3)C4=CN=C(N=C4)NC5CC6=CC=CC=C6C5 NEAPKZHDYMQZCB-UHFFFAOYSA-N 0.000 description 1
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- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- UTBYQPSPFXHANA-UHFFFAOYSA-N [K].[Na].[Li] Chemical compound [K].[Na].[Li] UTBYQPSPFXHANA-UHFFFAOYSA-N 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 229910002113 barium titanate Inorganic materials 0.000 description 1
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
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- 239000000470 constituent Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- AJNVQOSZGJRYEI-UHFFFAOYSA-N digallium;oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Ga+3].[Ga+3] AJNVQOSZGJRYEI-UHFFFAOYSA-N 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
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- 230000001747 exhibiting effect Effects 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- WIHZLLGSGQNAGK-UHFFFAOYSA-N hafnium(4+);oxygen(2-) Chemical compound [O-2].[O-2].[Hf+4] WIHZLLGSGQNAGK-UHFFFAOYSA-N 0.000 description 1
- 230000002706 hydrostatic effect Effects 0.000 description 1
- 229910003437 indium oxide Inorganic materials 0.000 description 1
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 description 1
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 1
- 229910052808 lithium carbonate Inorganic materials 0.000 description 1
- MVDSPIQMADQKKM-UHFFFAOYSA-N lithium potassium sodium Chemical compound [Li+].[Na+].[K+] MVDSPIQMADQKKM-UHFFFAOYSA-N 0.000 description 1
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 description 1
- 239000001095 magnesium carbonate Substances 0.000 description 1
- 229910000021 magnesium carbonate Inorganic materials 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 150000003891 oxalate salts Chemical class 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
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- BITYAPCSNKJESK-UHFFFAOYSA-N potassiosodium Chemical compound [Na].[K] BITYAPCSNKJESK-UHFFFAOYSA-N 0.000 description 1
- 229910000027 potassium carbonate Inorganic materials 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- HYXGAEYDKFCVMU-UHFFFAOYSA-N scandium oxide Chemical compound O=[Sc]O[Sc]=O HYXGAEYDKFCVMU-UHFFFAOYSA-N 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 229910000029 sodium carbonate Inorganic materials 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
- 229910001887 tin oxide Inorganic materials 0.000 description 1
- 150000003657 tungsten Chemical class 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
Classifications
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Definitions
- the present invention relates to a piezoelectric ceramic which contains a composition containing a perovskite-type oxidized product and a tungsten bronze-type oxidized product, and is suitable for a vibrating element such as an actuator, a sounding body or a sensor, and the production thereof. About the method.
- An actuator using a piezoelectric ceramic uses a piezoelectric phenomenon because it generates mechanical strain and stress when an electric field is applied.
- This actuator has features such as being able to obtain a very small amount of displacement with high precision and generating a large amount of stress. For example, it is used for positioning a precision machine tool or an optical device.
- piezoelectric ceramics used in actuators lead zirconate titanate (PZT), which has excellent piezoelectric properties, has been most frequently used.
- PZT lead zirconate titanate
- lead zirconate titanate contains a large amount of lead, adverse effects on the global environment such as elution of lead by acid rain have recently become a problem. Therefore, the development of a lead-free piezoelectric ceramic that replaces lead zirconate titanate is desired.
- Low-pressure ceramics containing no lead include, for example, barium titanate (BaTiO 3) as a main component.
- This piezoelectric ceramic has excellent relative permittivity ⁇ r and electromechanical coupling coefficient kr, and is promising as a piezoelectric material for actuators.
- a piezoelectric ceramic not containing lead for example, a piezoelectric ceramic containing lithium potassium sodium niobate as a main component is known (see JP-A-49-125900 or JP-B-57-6713). ).
- This piezoelectric ceramic is expected as a piezoelectric material because of its excellent electromechanical coupling coefficient kr, which has a high Curie temperature of 350 ° C or higher.
- a composite of sodium potassium niobate and a tungsten bronze type iris see Japanese Patent Application Laid-Open No. 9-165262 has been reported.
- piezoelectric ceramics that do not contain these lead have a problem that the piezoelectric characteristics are low compared to lead-based piezoelectric ceramics, and a sufficiently large generated displacement cannot be obtained. Furthermore, the piezoelectric ceramic mainly composed of sodium potassium lithium niobate has a problem that sodium, potassium and lithium are volatilized at the time of firing and it is difficult to fire immediately.
- the present invention has been made in view of a powerful problem, and an object of the present invention is to obtain a large amount of generated displacement, easy to fire, low pollution, environmental friendliness and ecological.
- An object of the present invention is to provide a piezoelectric ceramic which is excellent from a viewpoint and a method for manufacturing the same.
- a piezoelectric ceramic according to the present invention contains a composition containing a first perovskite oxide, a second perovskite oxide, and a tungsten bronze oxide, and has a first perovskite force.
- the oxide of the oxide type includes a first element containing sodium (Na) and potassium (K), a second element containing at least niobium in the group consisting of niobium (Nb) and tantalum (Ta), and oxygen ( O), the second perovskite-type oxidized product comprises a third element containing an alkaline earth metal element, a fourth element containing zirconium (Zr), and oxygen,
- the content of the second perovskite oxide in the above is less than 10 mol%.
- the content of potassium in the first element is preferably in the range of 10 mol% to 90 mol%.
- the first element preferably further contains lithium, and the lithium content in the first element is preferably 10 mol% or less.
- the content of the tungsten bronze oxidized product in the composition is preferably 1 mol% or less. It is preferable that the tungsten bronze oxidized product is composed of a fifth element containing an alkaline earth metal element, a sixth element containing at least niobium from the group consisting of niobium and tantalum, and oxygen.
- the content of tantalum in the total of the second element and the sixth element is preferably in the range of Omol% to 1 Omol%.
- the composition contains this composition as a main component and, as an accessory component, at least one element from Group 3 to Group 14 of the long-periodic periodic table, particularly manganese (Mn).
- manganese manganese
- cobalt (Co) iron (Fe), nickel (Ni), zinc ( ⁇ ⁇ ), scandium (Sc), titanium (Ti), zirconium (Zr), hafnium (Hf), aluminum (A1 ), Gallium (Ga), indium (In), silicon (Si), germanium (Ge), and tin (Sn).
- the method for manufacturing a piezoelectric ceramic according to the present invention is characterized in that the first perovskite is made of a first element containing sodium and potassium, a second element containing at least niobium from the group consisting of niobium and tantalum, and oxygen.
- a second perovskite oxide having a third element containing at least one of alkaline earth metal elements, a fourth element containing zirconium, and oxygen power, and a tungsten bronze type A piezoelectric ceramic containing an oxide is manufactured, and an element constituting a first perovskite oxide, an element constituting a second perovskite oxide, and an element constituting a tungsten bronze oxide are produced. And a step of calcining the resulting mixture.
- a first open ovskite oxide containing sodium, potassium and niobium, a second open ovskite oxide containing an alkaline earth metal element and zirconium Since it contains a tungsten bronze oxide and the content of the second perovskite oxide in the main component is less than 10 mol%, the amount of generated displacement can be increased. Further, it can be easily fired. Therefore, the possibility of use of piezoelectric ceramics and piezoelectric elements that do not contain lead or contain little lead can be enhanced.
- a piezoelectric material that is extremely low in terms of environmental pollution and ecological aspects, has a low risk of lead being released into the environment even after it is distributed and disposed of in markets where lead volatilization is low during firing.
- Porcelain and piezoelectric elements can be used.
- the generated displacement can be further increased.
- the generated displacement can be further increased.
- the tungsten bronze type iris is composed of a third element containing an alkaline earth metal element, a fourth element containing at least niobium in the group consisting of niobium and tantalum, and oxygen. By doing so, more excellent piezoelectric characteristics can be obtained. [0017] Furthermore, if the content of tantalum in the total of the second element and the sixth element is set to 10 mol% or less, the generated displacement can be further increased.
- the piezoelectric characteristics can be further improved.
- the sinterability is improved and the piezoelectric property is improved.
- the characteristics can be improved.
- manganese is added to manganese, and at least one of cobalt, iron, nickel, zinc, scandium, titanium, zirconium, hafnium, aluminum, gallium, indium, silicon, germanium and tin is added as a second subcomponent. If the total content of the second subcomponent in terms of the substance is contained within the range of 0.01% by mass or more and 1% by mass or less of the main component, the piezoelectric characteristics can be further improved.
- the elements constituting the first perovskite oxide, the second perovskite oxide, and the tungsten bronze oxide are mixed. Since the mixture containing the constituent elements is calcined, the piezoelectric ceramic of the present invention can be easily obtained, and the piezoelectric ceramic of the present invention can be realized.
- FIG. 1 is a configuration diagram showing a piezoelectric element using a piezoelectric ceramic according to one embodiment of the present invention.
- FIG. 2 is a flowchart showing a method for manufacturing a piezoelectric ceramic and a piezoelectric element according to one embodiment of the present invention.
- FIG. 3 is a configuration diagram showing a displacement measuring device used for measuring a generated displacement amount in an example of the present invention.
- the piezoelectric ceramic according to one embodiment of the present invention has, as main components, a composition including a first solid-state vesicular oxide, a second perovskite-type oxide, and a tungsten bronze-type oxide. Contains a substance.
- the first perovskite-type iris, the second perovskite-type iris, and the tungsten bronze-type iris are completely dissolved in the solid solution. It does not have to be completely dissolved.
- the first vesiculated porcelain iris comprises a first element, a second element, and oxygen.
- the first element contains at least sodium and potassium, and preferably also contains lithium.
- the second element contains at least niobium, and preferably also contains tantalum. In such a case, more excellent piezoelectric characteristics can be obtained by not containing lead or reducing the content of lead. It is also a power that can raise the Curie temperature and broaden the operating temperature range.
- the chemical formula of the first perovskite-type oxidized product is represented by, for example, ⁇ 1.
- the content of potassium in the first element is preferably in the range of 10 mol% to 90 mol%. That is, for example, X in Chemical Formula 1 is preferably in a molar ratio within the range of 0.1 ⁇ x ⁇ 0.9. If the content of potassium is too small, the relative permittivity ⁇ r, the electromechanical coupling coefficient kr, and the amount of generated displacement cannot be sufficiently increased. If the content of potassium is too large, the potassium This is a force that is very volatile and difficult to bake.
- the content of lithium in the first element is preferably Omol% or more and 10mol% or less. That is, for example, y in Chemical Formula 1 is preferably in the range of 0 ⁇ y ⁇ 0.1 in molar ratio. If the content of lithium is too large, the relative permittivity ⁇ r, the electromechanical coupling coefficient kr, and the generated displacement cannot be sufficiently increased.
- the composition ratio of the first element to the second element is in the range of 0.95 to 1.05 in molar ratio. Preferably, there is. If it is less than 0.95, the relative permittivity ⁇ r, the electromechanical coupling coefficient kr, and the amount of generated displacement will be small, and if it exceeds 1.05, the sintering density will decrease, making polarization difficult. It is.
- the second perovskite-type oxidized product comprises at least a third element containing an alkaline earth metal element, a fourth element containing at least zirconium, and oxygen.
- the alkaline earth metal element at least one selected from the group consisting of magnesium, calcium, strontium and barium is preferred. In such a case, more excellent piezoelectric characteristics can be obtained.
- the chemical formula of the second perovskite-type oxidized product is represented by, for example, Chemical formula 2.
- Ml represents the third element.
- the composition ratio of the third element, the fourth element (Zr), and oxygen is determined stoichiometrically, and the stoichiometric compositional power may be different.
- the tungsten bronze oxidized product is composed of a fifth element, a sixth element, and oxygen.
- the fifth element preferably contains, for example, at least one element selected from the group consisting of magnesium, calcium, strontium, and barium, more preferably containing at least an alkaline earth metal element.
- the sixth element contains, for example, at least niobium, and preferably also contains tantalum. In such a case, it is possible to obtain more excellent piezoelectric properties by not containing lead or by reducing the content of lead.
- the chemical formula of this tungsten bronze type oxide is represented, for example, by Chemical Formula 3.
- M2 (Nb !. w Ta w) 2 0 6
- M2 represents a fifth element
- w is a value within a range of 0 ⁇ w ⁇ l.
- the composition ratio of the fifth element, the sixth element (NbTa) and oxygen was determined stoichiometrically,
- the sixth element may be the same as or different from the second element.
- the content of tantalum in the total with the elements of 6 is preferably 10 mol% or less! / ⁇
- the first perovskite oxide, the second perovskite oxide, and tundast oxide The composition ratio with the bronze-type oxidized product is preferably in the range shown in Chemical formula 4 in molar ratio. That is, the content of the second perovskite-type oxidized product in the composition is preferably greater than Omol% and less than 10 mol%.
- the relative dielectric constant ⁇ r and the generated displacement can be increased, while if the content of the second perovskite oxide is too large, sintering occurs. It becomes difficult. It is preferable that the content of the tungsten bronze type iris is more than Omol% and 1 mol% or less.
- the inclusion of the tungsten bronze type oxidizing material facilitates sintering, and can increase the relative dielectric constant ⁇ r, the electromechanical coupling coefficient kr, and the amount of generated displacement. This is because if the content of the substance is too large, the electromechanical coupling coefficient kr and the generated displacement are reduced.
- A represents the first perovskite-type iris
- B represents the second perovskite-type iris
- C represents a tungsten bronze-type oxide
- m represents 0 ⁇ m ⁇ 0.1 and 11 are values in the range of 0 ⁇ 11 ⁇ 0.01.
- the piezoelectric ceramic may further include at least one of the elements belonging to Groups 3 to 14 of the long-period type periodic table as a sub-component obtained by adding the above-described composition as the main component. preferable. This is because the piezoelectric characteristics can be further improved.
- This subcomponent may be present, for example, as an oxidizing substance, by diffusing into a part of the composition of the main component, which may be present at the grain boundaries of the main component composition.
- manganese is contained as a first subcomponent as a subcomponent. It is also a force that can improve piezoelectric characteristics by improving sinterability.
- the content of manganese is preferably in the range of 0.1% by mass or more and 1% by mass or less of the main component in terms of manganese oxide (MnO). It is also a force that can improve the sinterability within this range.
- cobalt in addition to manganese, as a second sub-component, cobalt, iron, nickel, zinc, scandium, titanium, zirconium, hafnium, aluminum, gallium, indium, silicon, germanium and tin It is preferable to contain at least one of these. This is because these have a function of improving the piezoelectric characteristics separately from the improvement of the sinterability.
- the content of the second subcomponent is determined based on the oxides (Co O, Fe O, NiO, ZnO, Sc O, TiO, ZrO, Hf
- the content is preferably in the range of 0.01% by mass to 1% by mass of the main component. This is because the characteristics can be improved within this range.
- the piezoelectric ceramic may contain lead (Pb), but the content is preferably 1% by mass or less, more preferably not containing any lead. It minimizes the volatilization of lead during firing and the release of lead into the environment after it has been marketed and disposed of as a piezoelectric component, and has reduced pollution, environmental friendliness and ecological aspects. Is preferred.
- the piezoelectric ceramic is preferably used, for example, as a material for a vibration element such as an actuator which is a piezoelectric element, a sounding body or a sensor.
- FIG. 1 shows a configuration example of a piezoelectric element using the piezoelectric ceramic according to the present embodiment.
- the piezoelectric element includes a piezoelectric substrate 1 made of the piezoelectric ceramic of the present embodiment, and a pair of electrodes 2 and 3 provided on a pair of opposing surfaces la and lb of the piezoelectric substrate 1, respectively.
- the piezoelectric substrate 1 is polarized, for example, in the thickness direction, that is, in the direction opposite to the electrodes 2 and 3, and when a voltage is applied through the electrodes 2 and 3, the piezoelectric substrate 1 spreads longitudinally in the thickness direction and expands in the radial direction. It starts to vibrate!
- the electrodes 2 and 3 are made of, for example, a metal such as gold (Au), and are provided on the entire opposing surfaces la and lb of the piezoelectric substrate 1, respectively. These electrodes 2 and 3 are electrically connected to, for example, an external power supply (not shown) via wires (not shown).
- Au gold
- the piezoelectric ceramic and the piezoelectric element having such a configuration can be manufactured, for example, as follows.
- FIG. 2 is a flowchart showing a method of manufacturing this piezoelectric ceramic.
- an oxidized powder containing, for example, sodium, potassium, lithium, niobium, tantalum, an alkaline earth metal element and zirconium is prepared as necessary.
- an oxidized powder containing at least one element from Group 3 to Group 14 of the long-periodic table such as manganese
- an oxide powder containing at least one of the following: iron, nickel, zinc, scandium, titanium, zirconium, hafnium, ethanol, gallium, indium, silicon, germanium, and tin are examples of the following: iron, nickel, zinc, scandium, titanium, zirconium, hafnium, ethanol, gallium, indium, silicon, germanium, and tin.
- Step S101 As the raw materials of these main components and subcomponents, those which can be converted into oxides by firing, such as carbonates or oxalates which can be converted into oxides, may be used. Next, after these materials are sufficiently dried, they are weighed so that the final composition is in the above-mentioned range (Step S101).
- the raw materials for the second perovskite-type oxidized product are sufficiently mixed in an organic solvent or water by a ball mill or the like, dried, and then dried at 1000 ° C.—1200 ° C. for 2 hours. By firing for 4 hours, a second perovskite-type oxidized product is prepared (Step S102).
- the second perovskite-type oxidized product After preparing the second perovskite-type oxidized product, the second perovskite-type oxidized product, the raw material of the first perovskite-type oxide, and the raw material of the tungsten bronze-type oxide And the raw materials of the auxiliary components are sufficiently mixed in an organic solvent or water by a ball mill or the like. After that, the mixture is dried, press-molded, and calcined at 750 ° C to 1100 ° C for 1 hour to 4 hours (step S103).
- the production of the second perovskite-type oxidized product and the mixing of the second perovskite-type oxidized product with the raw materials of the other main components are performed in such a manner that the second perovskite-type oxidized material is mixed with the first perovskite-type oxidized product. This is because if the raw material of the oxide is mixed and fired, it reacts with the first gasket-type oxide and does not produce the second perovskite-type oxide.
- the calcined product is sufficiently pulverized in an organic solvent or water by a ball mill or the like, dried again, and granulated by adding a binder. After the granulation, the granulated powder is press-formed using a uniaxial press forming machine or a hydrostatic pressing machine (CIP) (Step S104).
- CIP hydrostatic pressing machine
- the molded body is heated to remove the binder, and then fired at 950 ° C. to 1350 ° C. for 2 to 14 hours (step S 105).
- the obtained sintered body is processed as necessary to form a piezoelectric substrate 1, electrodes 2 and 3 are provided, and a polarization treatment is performed by applying an electric field in heated silicone oil ( Step S106).
- Step S106 the above-described piezoelectric ceramic and the piezoelectric element shown in FIG. 1 are obtained.
- the first porous buskite oxide containing sodium, potassium and niobium, and the second porous cubic oxide containing alkali earth metal element and zirconium It contains a bouskite-type oxide and a tungsten bronze-type oxide.
- the content of the perovskite-type oxidized product of No. 2 is set to less than 10 mol%, the relative dielectric constant ⁇ r, electromechanical coupling coefficient kr, and generated displacement can be increased. Also, it can be easily fired.
- the composition ratio of the first element to the second element is a molar ratio. If it is set to fall within the range of 0.95 or more and 1.05 or less, the relative permittivity ⁇ r, electromechanical coupling coefficient kr, and generated displacement can be further increased.
- the electromechanical coupling coefficient kr and the generated displacement can be further increased.
- the tungsten bronze-type oxidizing material is composed of a fifth element containing an alkaline earth metal element, a sixth element containing at least niobium in the group consisting of niobium and tantalum, and oxygen.
- the fifth element includes at least one of the group consisting of magnesium, calcium, stonium, and barium, more excellent piezoelectric characteristics can be obtained.
- the piezoelectric characteristics can be further improved.
- the sinterability is improved and the piezoelectric property is improved.
- the characteristics can be improved.
- manganese is added to manganese, and at least one of cobalt, iron, nickel, zinc, scandium, titanium, zirconium, hafnium, aluminum, gallium, indium, silicon, germanium and tin is added as a second subcomponent. If the total content of the second subcomponent in terms of the substance is contained within the range of 0.01% by mass or more and 1% by mass or less of the main component, the piezoelectric characteristics can be further improved.
- the second perovskite-type oxide, the raw material of the element constituting the first perovskite-type oxide, and the raw material of the element constituting the tungsten bronze-type oxide are mixed and calcined. ⁇ By firing, the piezoelectric ceramic according to the present embodiment can be easily obtained, and the piezoelectric ceramic according to the present embodiment can be realized.
- a piezoelectric element as shown in FIG. 1 was manufactured by the steps shown in FIG. This embodiment will be described with reference to FIGS. 1 and 2 using the reference numerals shown in FIG.
- Manganese carbonate (MnCO) powder is prepared as a raw material for sub-components.
- the amount of the manganese carbonate powder, which is the raw material of the subcomponent, was 0.5% by mass based on the total mass of the raw material of the main component.
- the strontium carbonate powder and the zirconium oxide powder are mixed in water by a ball mill, dried, and then fired at 1100 ° C for 2 hours to obtain a second zirconium perovskite-type oxide powder.
- Strontium acid was produced (see FIG. 2; step S102).
- this strontium zirconate, a raw material of another main component, and a raw material of an auxiliary component are mixed in water by a ball mill, dried, and press-formed at 850 ° C. — Calcined at 1000 ° C for 2 hours (see Fig. 2: Step S103).
- the mixture was pulverized in water using a ball mill, dried again, and granulated by adding polyvinyl alcohol. After granulation, the granulated powder was formed into disk-shaped pellets with a diameter of 17 mm by a uniaxial press forming machine at a pressure of about 40 MPa. (See FIG. 2: Step S104).
- the molded body was heated at 650 ° C. for 4 hours to remove the binder, and was further calcined at 950 ° C. to 1350 ° C. for 4 hours (see FIG. 2: Step S105). Thereafter, the fired body was processed into a disc having a thickness of 0.6 mm to produce a piezoelectric substrate 1.
- Silver paste was printed on both sides and baked at 650 ° C. to form electrodes 2 and 3. After forming electrodes 2 and 3, 30 ° C—250 ° C An electric field of 3 kVZmm-lOkVZmm was applied in the silicone oil for 1 minute to 30 minutes to perform polarization treatment (see FIG. 2; step S106).
- the piezoelectric elements of Examples 1 and 2 were obtained.
- a sample 13 is sandwiched between a pair of electrodes 11 and 12, a displacement of the sample 13 when a direct current is applied is detected by a displacement sensor 14, and a generated displacement amount is obtained by a displacement detector 15. Things.
- Table 1 shows the results.
- the generated displacement shown in Table 1 is the value obtained by dividing the measured value by the sample thickness and multiplying by 100 (measured value Z sample thickness x 100).
- Example 1-1 As Comparative Example 1-1 with respect to the present example, except that strontium zirconate, which is the second perovskite-type oxidized product, was not included, that is, the value of m in Chemical Formula 5 was set to 0. Except for the above, a piezoelectric element was manufactured in the same manner as in Example 1-1, Example 1-2. In addition, as Comparative Example 1-2 with respect to the present example, except that the content of strontium zirconate in the main component was set to 10 mol%, that is, the value of m in Chemical formula 5 was set to 0.1, the other examples were the same as those in Example 1-2. A piezoelectric element was produced in the same manner as in 1 and 1-2. The contents of the subcomponents are the same as in Examples 1-1, 1-2.
- the second perovskite-type iris may be contained in the main component within a range of less than 10 mol% in addition to the first perovskite-type iris.
- a piezoelectric element was produced in the same manner as in Example 1-2, except that the composition shown in Fig. 6 was included as a main component. At that time, in Example 1-3-1-5, the third element (Ml in Chemical Formula 6) was changed as shown in Table 2.
- Raw materials for magnesium, calcium and barium include basic magnesium carbonate (4MgCO -Mg (OH) 4 ⁇ ⁇ ) powder, carbonate
- Example 1-3-1-5 the relative permittivity ⁇ r, the electromechanical coupling coefficient kr, and the displacement generated when an electric field of 3 kVZmm were applied were measured in the same manner as in Example 1-2. did. Them The results are shown in Table 2 together with the results of Example 1-2 and Comparative Example 1-1.
- Example 1-2 As shown in Table 2, according to Example 1-3-1-5, as in Example 1-2, the relative dielectric constant ⁇ r and the amount of generated displacement were higher than those in Comparative Example 1-1. Large values were obtained. That is, even if the third element is changed, the piezoelectric characteristics can be improved and the generated displacement can be increased.
- a piezoelectric element was produced in the same manner as in Examples 1-1 and 1-2, except that the composition shown in Fig. 7 was included as a main component.
- the composition of the first element (the values of X and y in Chemical formula 7) and the strontium zirconate zirconate, which is the second perovskite-type oxidant,
- the content (the value of m in Chemical formula 7) was varied as shown in Table 3.
- the contents of the subcomponents are the same as in Examples 1-1 and 1-2.
- Example 2-7 0.8 0 0.08 0.31 507 25.5 0.048
- Comparative Examples 2-1 to 2-6 with respect to this example were the same as those of Example 2-1-2-2 except that strontium zirconate, which is the second perovskite-type oxidized product, was not included. A piezoelectric element was produced in the same manner as in 7. Of these, Comparative Example 2-1 corresponds to Example 2-1; Comparative Example 2-2 corresponds to Examples 2-2 and 2-3; Comparative Example 2-3 corresponds to Example 2-4. Comparative Example 2-4 corresponds to Example 2-5, Comparative Example 2-5 corresponds to Example 2-6, and Comparative Example 2-6 corresponds to Example 2-7.
- Example 2-1-2-7 and Comparative example 2-1-2-6 the relative dielectric constant ⁇ r and the electromechanical coupling coefficient kr were set in the same manner as in Examples 1-1 and 1-2.
- the displacement generated when an electric field of 3 kVZmm was applied was measured. Table 3 shows the results.
- Example 2-1-2-7 As shown in Table 3, according to Example 2-1-2-7, as in Examples 1-1 and 1-2, the relative dielectric constant ⁇ r and the amount of generated displacement were higher than those of the comparative example. Large values were obtained for In addition, as the value of X in Chemical Formula 7 increases, that is, as the content of potassium increases, the relative permittivity ⁇ r, the electromechanical coupling coefficient kr, and the generated displacement increase, exhibiting a maximum value. There was a tendency to be smaller. That is, when the content of potassium in the first element is 10 mol% or more and 90 mol% or less, the piezoelectric characteristics can be improved and the generated displacement can be increased.
- the relative permittivity ⁇ r, electromechanical coupling coefficient kr, and generated displacement tended to be larger.
- the piezoelectric characteristics could be improved and the generated displacement could be increased.
- a piezoelectric element was prepared in the same manner as in Example 1-1, 1-2, except that the composition shown in Example 8 was included as a main component.
- the content of tantalum (the values of z and w in Chemical Formula 8) and the content of strontium zirconate, which is the second perovskite-type oxide (Chemical Formula 8) m value) was changed as shown in Table 4.
- the contents of the auxiliary components were the same as in Examples 1-1 and 1-2, and tantalum (Ta 2 O 3) powder was used as a raw material for tantalum.
- a piezoelectric element was produced in the same manner as in Example 3-1 except that the fibrous component shown in FIG. 9 was used as a main component and the subcomponents shown in Table 5 or Table 6 were further added.
- the raw materials of the second sub-component include oxidized cobalt (Co O) powder, iron oxide (Fe O) powder, oxidized nickel (NiO) powder.
- silicon (SiO) powder silicon dioxide (GeO) powder or tin oxide (SnO) powder
- Example 4-2 0.31 Co 0.2 944 47.2 0.120
- Example 5-1 0.31 Fe 0.2 943 44.5 0.113
- Example 5-3 0.31 Zn 0.2 948 46.1 0.118
- Example 5-4 0.31 Sc 0.2 979 45.1 0.117
- Example 5-5 0.31 Ti 0.2 1117 42.3 0.117
- Example 5-6 0.31 Zr 0.2 1200 40.8 0.117
- Example 5-7 0.31 Hf 0.2 1060 43.2 0.117
- Example 5-8 0.31 Al 0.2 1038 41.2 0.110
- Example 5-9 0.31 Ga 0.2 1116 41.5 0.115
- Example 5-10 0.31 In 0.2 1055 41.1 0.111
- Example 5-11 0.31 Si 0,2 1028 40.3 0.107
- Example 5-12 0.31 Ge 0.2 1100 43.4 0.119
- Example 5-13 0.31 Sn 0.2 1050 42.0 0.113
- Examples 4-1 to 4-3, 5 to 15-13 also have the same relative permittivity ⁇ r, electromechanical coupling coefficient kr, and 3 kVZmm as in Examples 1-1 and 1-2. The amount of displacement generated when an electric field was applied was measured. Tables 5 and 6 show the results together with the results of Example 3-1.
- Example 4-1-4-3 in which cobalt was added as the second subcomponent, the generated displacement was larger than that in Example 3-1 not including the second subcomponent. The quantity was obtained.
- the content of cobalt as the second auxiliary component was increased as a component. When the heat was applied, the amount of generated displacement increased, showed a maximum value, and then decreased.
- the second subcomponent at least one selected from the group consisting of cobalt, iron, nickel, zinc, scandium, titanium, zirconium, hafnium, aluminum, gallium, indium, silicon, germanium, and tin is contained.
- the piezoelectric characteristics can be further improved.
- the content of the second subcomponent, in terms of oxide was preferably in the range of 0.01% by mass or more and 1% by mass or less based on the main component.
- the present invention has been described with reference to the embodiments and examples. However, the present invention can be variously modified without being limited to the above embodiments and examples.
- the force described in the case of containing the composition of the first perovskite oxide, the second open ovskite oxide, and the tungsten bronze oxide is described.
- This composition may further contain components other than the first perovskite-type iris, the second perovskite-type iris, and the tungsten bronze-type iris.
- the composition of the main component contains, as the first element, sodium, potassium, and at least sodium and potassium in the group that also has a lithium force
- the second element Contains at least niobium in the group consisting of niobium and tantalum, contains at least one of alkaline earth metal elements as the third element, contains at least titanium as the fourth element, and contains the fifth element Contain at least one of the alkaline earth metal elements, and as the sixth element at least one of the group niobium and tantalum
- these first, second, third, fourth, fifth, and sixth elements include other elements. It may further contain.
- a single-layer piezoelectric element has been described as an example.
- the present invention can be similarly applied to a piezoelectric element having another structure such as a multilayer structure.
- the present invention can be applied to other piezoelectric elements such as a vibrating element such as an actuator, a sounding body, and a sensor as examples of the piezoelectric element.
- a vibrating element such as an actuator and a piezoelectric element such as a sounding body and a sensor.
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WO2006114914A1 (ja) * | 2005-04-18 | 2006-11-02 | Murata Manufacturing Co., Ltd. | 誘電体セラミック組成物及び積層セラミックコンデンサ |
CN100594198C (zh) * | 2005-04-28 | 2010-03-17 | 株式会社村田制作所 | 压电陶瓷组合物及该压电陶瓷组合物的制造方法以及压电陶瓷电子部件 |
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JP3654408B2 (ja) * | 1998-02-18 | 2005-06-02 | 株式会社村田製作所 | 圧電磁器組成物 |
TWI228728B (en) * | 2001-05-29 | 2005-03-01 | Murata Manufacturing Co | Piezoelectric ceramic composition, piezoelectric ceramic element and method for producing piezoelectric ceramic composition |
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- 2004-12-21 EP EP20040807448 patent/EP1702906B1/en active Active
- 2004-12-21 CN CNB2004800382725A patent/CN100432014C/zh active Active
- 2004-12-21 US US10/583,447 patent/US20070152183A1/en not_active Abandoned
- 2004-12-21 WO PCT/JP2004/019091 patent/WO2005061413A1/ja active Application Filing
- 2004-12-21 KR KR20067012354A patent/KR100821542B1/ko active IP Right Grant
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JP2002160967A (ja) * | 2000-11-20 | 2002-06-04 | Matsushita Electric Ind Co Ltd | 圧電磁器組成物 |
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Also Published As
Publication number | Publication date |
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JP4513948B2 (ja) | 2010-07-28 |
CN1898182A (zh) | 2007-01-17 |
KR20060105788A (ko) | 2006-10-11 |
EP1702906A4 (en) | 2011-04-27 |
EP1702906A1 (en) | 2006-09-20 |
US20070152183A1 (en) | 2007-07-05 |
CN100432014C (zh) | 2008-11-12 |
TW200529481A (en) | 2005-09-01 |
EP1702906B1 (en) | 2012-08-29 |
TWI249258B (en) | 2006-02-11 |
KR100821542B1 (ko) | 2008-04-14 |
JP2005179143A (ja) | 2005-07-07 |
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