CN1541977A - Sodium bismuth titanate base nonleaded piezoelectric ceramic - Google Patents
Sodium bismuth titanate base nonleaded piezoelectric ceramic Download PDFInfo
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- CN1541977A CN1541977A CNA2003101108782A CN200310110878A CN1541977A CN 1541977 A CN1541977 A CN 1541977A CN A2003101108782 A CNA2003101108782 A CN A2003101108782A CN 200310110878 A CN200310110878 A CN 200310110878A CN 1541977 A CN1541977 A CN 1541977A
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Abstract
The lead-free bismuth sodium titanate piezoelectric ceramic composition is one perovskite type environment consistency piezoelectric ceramic composition. The composition has the general expression of (1-x-y-z)Bi1-wNawTiO3+xBi0.5K0.5TiO3+yBaTiO3+zSrTiO3+aMalphaObeta, where x is 0-1, y 0-1, z 0-1, (x+y+z) 0-1, w 0.3-0.7; MalphaObeta is doping oxide(s) in the content an of 0-10 %; M is +1~+6 valent element capable of forming solid oxide, such as Na, K, Li, Al, Cu, etc. with alpha and beta being atom number. The piezoelectric ceramic composition has d33 up to 190 pC/N, kp up to 24.0 % and stable technological process, may be produced via traditional piezoelectric ceramic preparation process and industrial material, and is practical.
Description
One, technical field
The present invention relates to a kind of novel polynary lead-free piezoelectric ceramics composition, belong to perovskite structure environment compatibility piezoelectric ceramics field.
Two, background technology
Find the piezoelectricity of barium titanate ceramics from middle 1940s after, constitutional features is that the research and development of piezoelectric ceramics of AB O3 type are very active, and the components and parts of piezoelectric ceramics and making have been widely used in particularly information industry field of industry.With Pb-based lanthanumdoped zirconate titanates (Pb (Ti, Zr) O
3) being the lead base two component system of representative, the A position is Pb; The B position is Ti, Zr and with Pb-based lanthanumdoped zirconate titanates (Pb (Ti, Zr) O
3) be base-material, add the 3rd constituent element, as with lead magnoniobate PMN-PT [Pb (Mg
1/3Nb
2/3) O
3-PbTiO
3] being representative, the A position is Pb, the B position is Mg
1/3Nb
2/3All have good piezoelectricity ferro performance and high Curie temperature with the lead base ternary system piezoelectric ceramic of Ti.The piezoelectric ceramics overwhelming majority who uses in the industrial production is such lead base piezoelectric ceramics.
But, PbO in the lead base piezoceramic material or Pb
3O
4Content accounts for 70% of raw material total amount.PbO or Pb
3O
4At high temperature volatile, cause severe contamination and harm for the mankind and ecotope thereby make in the treating processes of lead base piezoelectric ceramics after producing, use and discarding.In recent years, seek piezoelectric ceramics system lead-free, superior performance and be subjected to the pay attention to day by day of countries in the world.
Common leadless piezoelectric ceramics system has four classes: BaTiO at present
3Based leadless piezoelectric ceramics, bismuth laminated leadless piezoelectric ceramic, base metal niobate leadless piezoelectric ceramics and Bi
0.5Na
0.5TiO
3Based leadless piezoelectric ceramics.More than the characteristics of four class leadless piezoelectric ceramicss be: BaTiO3 base piezoelectric ceramic Curie temperature is 120 ℃ only, and piezoelectric property is medium; The Curie temperature height of bismuth laminated leadless piezoelectric ceramic, but piezoelectric activity is low; The base metal niobate leadless piezoelectric ceramics then is difficult to sinter into fine and close pottery; Bi
0.5Na
0.5TiO
3Based leadless piezoelectric ceramics has the Curie temperature height, easily add other constituent element modification becomes the research focus of non-lead base piezoelectric ceramics to improve characteristics such as piezoelectric property.
Bi
0.5Na
0.5TiO
3Be that the A position is by compound ion Bi
0.5Na
0.5The ABO that constitutes
3The perovskite typed ferroelectrics, A position compound ion Bi
0.5Na
0.5By Bi
3+(A1 position) and Na
+(A2 position) constitutes.Simple Bi
0.5Na
0.5TiO
3The pottery coercive field is very big
(73Kv/cm), the polarization difficulty is difficult to practicability, must be to Bi
0.5Na
0.5TiO
3It is low to obtain coercive field to carry out modification, presses
The good leadless piezoelectric ceramics system of electricity ferroelectric properties.At present common to Bi
0.5Na
0.5TiO
3Adding method that other constituent element carries out modification has merely with+divalent alkaline-earth metal ions and partly replaces A position ion Bi
0.5Na
0.5Or merely+1 the alkalimetal ion of valency partly replaces the Na of A2 position
+Document 1 (JAPANESE JOURNAL OF APPLIED PHYSICS, Vol 30,9B, 1991,9, p2236-2239), to have provided composition formula be (1-x) Bi to document 2 (Journal of Inorganic Materials, Vol 15, No5,2000,12)
0.5Na
0.5TiO
3-xBaTiO
3The leadless piezoelectric ceramics system, d
33=125pC/N, k
p=29%; It is Bi that document 3 (phys.stat.sol. (a) 157,499 (1996)) has provided composition formula
0.5Na
0.5TiO
3-Bi
0.5K
0.5TiO
3The leadless piezoelectric ceramics system, d
33=96pC/N, k
p=21%; It is Bi that document 4 (Ferroelectrics.1997, Vol 196, p 175-178) and document 5 (Key Engineering Materials Vols, 157-158 (1999) are p.57-64) have provided composition formula respectively
0.5Na
0.5TiO
3-1/2 (Bi
2O
3Sc
2O
3), Bi
0.5Na
0.5TiO
3-NaNbO
3The leadless piezoelectric ceramics system, d
33=71-92pC/N, k
pBe about 15%; It is (Bi that document 6 (Ferroelectrics.1995, Vol 169, p 317-325) and 7 (Ferroelectrics.1990, Vol 106, p 375-380) have provided composition formula
1/2Na
1/2)
1-x(Sr
1/2Ca
1/2)
xTiO
3, (Bi
1/2Na
1/2)
1-x(Sr
aPb
bCa
c)
xTiO
3The leadless piezoelectric ceramics system, d
33=82pC/N, k
p=12-20.3%.It is (1-x) Bi that patent CN85100513, JP2001-48642 provide composition formula
0.5Na
0.5TiO
3-xBaTiO
3Piezoelectric ceramic composition, k
p=20.2%, ε
33/ ε
0=290, d
33=159pC/N; It is [Bi that patent JP11-217262, JP2000-22235 provide composition formula
0.5(Na
1-xK
x)
0.5] TiO
3Piezoelectric ceramic composition, k
p=21.1%, ε
33/ ε
0=611.It is Bi that patent DE19530592C2 has provided composition formula
0.5Na
0.5TiO
3-BaTiO
3-CaTiO
3Piezoelectric ceramic composition, said composition has thickness and big characteristics of electromechanical coupling factor anisotropy radially, k
p=16%; It is [Bi that patent JP2000-44335 has provided composition formula
0.5(Na
1-xLi
x)
0.5] TiO
3Piezoelectric ceramic composition, k
p=23.4%, ε
33/ ε
0=432.
Three, summary of the invention
Purpose of the present invention is exactly in order to overcome the inherent defective of existing lead base piezoelectric ceramics system own, to improve existing BaTiO
3Base lead-free battery performance, proposed a class novel form leadless piezoelectric ceramics by the polynary lead-free material.This piezoelectric ceramics adopts the traditional ceramics prepared, and technology stability is good, has good piezoelectricity ferro performance, has approached the product performance of lead base pottery, has practicality.
For realizing purpose of the present invention, the present invention is directed to ABO
3The perovskite typed piezoelectricity system (Bi of structure
0.5Na
0.5) TiO
3, a class A position compound ion Bi has been proposed
0.5Na
0.5By alkaline-earth metal ions Ba
2+And Sr
2+The compound ion of forming partly replaces, with
The time A2 position ion Na
+By alkalimetal ion K
+Part replaces formed novel lead-free piezoceramic material, can use general formula (1-x-y-z) Bi
(1-w)Na
wTiO
3+ xBi
0.5K
0.5TiO
3+ yBaTiO
3+ zSrTiO
3Represent that the x in the formula, y, z and w represent the shared atomicity (being atomic percent) in each constituent element of respective element material in the compound ion.The atomicity summation of all elements on the A position should be 1,0<x in the formula<1,0<y<1,0<z<1,0<(x+y+z)<1,0.3≤w≤0.7.
The piezoceramic material that the present invention proposes can also be added other metals by the base-material that the front general formula is represented as hotchpotch, and promptly base-material+hotchpotch is formed, and its performance is optimized more.Can be expressed as with general formula: [(1-x-y-z) Bi
(1-w)Na
wTiO
3+ xBi
0.5K
0.5TiO
3+ yBaTiO
3+ zSrTiO
3]+M
αO
β(wt%), M in general formula
αO
βThe expression hotchpotch.The shared ratio of hotchpotch is 0-10wt%; The shared ratio of base-material is 90-100wt%.M
αO
βBe one or more doping oxides, M represents this class+1-+6 valency and can form the element of solid-oxide with oxygen, as Na, K, Li, Al, Cu, Fe, Ce, Pr, Nd, Sm, Gd, Dy, Er, Yb, Y, Sc, Mn, Ca, Ba, Sr, Mg, Si etc.; α and β represent the atomicity of corresponding element M and oxygen in the relevant oxide compound respectively.
Polynary lead-free piezoelectric ceramics of the present invention has good piezoelectricity ferro performance, detects the piezoelectric constant d of this system piezoelectric ceramics through material property
33Can reach more than the 190pC/N percentage coupling k
pCan reach more than 24.0% residual polarization P
r(34.6 μ C/cm greatly
2), coercive field low (25.7Kv/cm), ferroelectric hysteresis loop rectangle degree good (as shown in Figure 1).Advantage of the present invention is: the leadless piezoelectric ceramics excellent property has had the performance level of Industrial products; Its process stabilizing can adopt conventional piezoelectric ceramics processing and industrial starting material to obtain, and sintering temperature is about about 1200 ℃, than low about 50-100 ℃ of lead base piezoelectric ceramics, has practicality.
Four, description of drawings
Fig. 1 is the ferroelectric hysteresis loop figure of leadless piezoelectric ceramics under the normal temperature that records.
Five, embodiment
Prepare leadless piezoelectric ceramics of the present invention and can adopt technical pure or chemical pure Bi
2O
3, Na
2CO
3, BaCO
3, SrCO
3, CaCO
3, TiO
2, M
αO
βBe raw material, can select the associated metal oxide compound as required as hotchpotch M
αO
βConcrete preparation method is: press general formula (1-x-y-z) Bi
(1-w)Na
wTiO
3+ xBi
0.5K
0.5TiO
3+ yBaTiO
3+ zSrTiO
3The stoichiometric ratio raw materials weighing, behind abundant ball milling mixing, in the alumina crucible of packing into, carry out pre-burning at 800-900 ℃, soaking time is 4-6 hour.Add modification hotchpotch M in the pre-burning synthetic powder
αO
βWt%, levigate through ball milling again, thorough mixing, adding additives, moulding, plastic removal are at last at 1100-12250 ℃ of following sintering 2-3 hour.Ceramic plate behind the sintering is by last silver electrode, and in 100-120 ℃ silicone oil, polarization is 10-15 minute under the voltage of 3-4kV/mm.
Preparation system system (1-x-y-z) Bi
(1-w)Na
wTiO
3+ xBi
0.5K
0.5TiO
3+ yBaTiO
3+ zSrTiO
3(92-100wt%) or add hotchpotch M
αO
βThe prescription and the performance index of leadless piezoelectric ceramics (0-8wt%) are as follows:
Embodiment 1:
Prescription:
[0.82Bi
0.5Na
0.5TiO
3+0.15Bi
0.5K
0.5TiO
3+0.02BaTiO
3+0.01SrTiO
3](95wt%)+Y
2O
3(5wt%)
Performance:
d
33(pC/N) tg δ (%) ε
33/ ε
0k
p(%) Qm Poisson's ratio
186 3.3 1089 24.0 78 0.286
Embodiment 2:
Prescription:
[0.78Bi
0.6Na
0.4TiO
3+0.15Bi
0.5K
0.5TiO
3+0.02BaTiO
3+0.05SrTiO
3](99wt%)+Na
2O(1wt%)
Performance:
d
33(pC/N) tg δ (%) ε
33/ ε
0k
p(%) Qm Poisson's ratio
169 3.9 1208 19.6 67 0.292
Embodiment 3:
Prescription:
[0.68Bi
0.6Na
0.4TiO
3+0.15Bi
0.5K
0.5TiO
3+0.02BaTiO
3+0.15SrTiO
3](96wt%)+Li
2O(4wt%)
Performance:
d
33(pC/N) tg δ (%) ε
33/ ε
0k
p(%) Qm Poisson's ratio
192 4.3 1227 24.6 77 0.288
Embodiment 4:
Prescription:
[0.82Bi
0.5Na
0.5TiO
3+0.1Bi
0.5K
0.5TiO
3+0.06BaTiO
3+0.02SrTiO
3](95wt%)+Fe
2O
3(5wt%)
Performance:
d
33(pC/N) tg δ (%) ε
33/ ε
0k
p(%) Qm Poisson's ratio
160 3.2 956 18.2 82 0.279
Embodiment 5:
Prescription:
0.87Bi
0.3Na
0.7TiO
3+0.05Bi
0.5K
0.5TiO
3+0.06BaTiO
3+0.02SrTiO
3
Performance:
d
33(pC/N) tg δ (%) ε
33/ ε
0k
p(%) Qm Poisson's ratio
143 4.9 931 16.3 100 0.279
Embodiment 6:
Prescription:
[0.78Bi
0.5Na
0.5TiO
3+0.15Bi
0.5K
0.5TiO
3+0.02BaTiO
3+0.05SrTiO
3](94wt%)+La
2O
3(6wt%)
Performance:
d
33(pC/N) tg δ (%) ε
33/ ε
0k
p(%) Qm Poisson's ratio
151 4.3 995 18.3 62 0.289
Embodiment 7:
Prescription:
[0.78Bi
0.5Na
0.5TiO
3+0.15Bi
0.5K
0.5TiO
3+0.02BaTiO
3+0.05SrTiO
3](92wt%)+CeO
2(2wt%)+Nb
2O
5(6wt%)
Performance:
d
33(pC/N) tg δ (%) ε
33/ ε
0k
p(%) Qm Poisson's ratio
160 3.7 1195 19.0 70 0.293
Claims (6)
1. bismuth-sodium titanate base lead-free piezoelectric ceramic is at ABO
3The A position is compound ion Bi in the structure
0.5Na
0.5, it is characterized in that by the A position by alkaline-earth metal ions Ba
2+And Sr
2+The compound ion of forming partly replaces, simultaneously A2 position ion Na
+By alkalimetal ion K
+Part replaces the lead-free piezoceramic material that constitutes.
2. piezoelectric ceramics as claimed in claim 1 is characterized in that by general formula (1-x-y-z) Bi
(1-w)Na
wTiO
3+ xBi
0.5K
0.5TiO
3+ yBaTiO
3+ zSrTiO
3The material of expression constitutes, 0<x in the formula<1,0<y<1,0<z<1,0<(x+y+z)<1,0.3≤w≤0.7.
3. as the piezoelectric ceramics of claim 1 or 2, it is characterized in that having added one or more doping oxides, hotchpotch content is 0-10wt%, and the content of all the other base material is 90-100wt%, is expressed as (1-x-y-z) Bi with general formula
(1-w)Na
wTiO
3+ xBi
0.5K
0.5TiO
3+ yBaTiO
3+ zSrTiO
3, M
αO
βBe one or more doping oxides, M is for+1-+6 valency and can form element Na, K, Li, Al, Cu, Fe, Ce, Pr, Nd, Sm, Gd, Dy, Er, Yb, Y, Sc, Mn, Ca, Ba, Sr, Mg or the Si of solid-oxide with oxygen.
4. piezoelectric ceramics as claimed in claim 3 is characterized in that by composition formula [0.82Bi
0.5Na
0.5TiO
3+ 0.15Bi
0.5K
0.5TiO
3+ 0.02BaTiO
3+ 0.01SrTiO
3] (95wt%)+Y
2O
3(5wt%) or [0.78Bi
0.6Na
0.4TiO
3+ 0.15Bi
0.5K
0.5TiO
3+ 0.02BaTiO
3+ 0.05SrTiO
3] (99wt%)+Na
2O (1wt%) or [0.68Bi
0.6Na
0.4TiO
3+ 0.15Bi
0.5K
0.5TiO
3+ 0.02BaTiO
3+ 0.15SrTiO
3] (96wt%)+Li
2O (4wt%) or [0.82Bi
0.5Na
0.5TiO
3+ 0.1Bi
0.5K
0.5TiO
3+ 0.06BaTiO
3+ 0.02SrTiO
3] (95wt%)+Fe
2O
3(5wt%) or [0.78Bi
0.5Na
0.5TiO
3+ 0.15Bi
0.5K
0.5TiO
3+ 0.02BaTiO
3+ 0.05SrTiO
3] (94wt%)+La
2O
3(6wt%) material of expression constitutes.
5. as the piezoelectric ceramics of claim 1 or 2, it is characterized in that by composition formula 0.87Bi
0.3Na
0.7TiO
3+ 0.05Bi
0.5K
0.5TiO
3+ 0.06BaTiO
3+ 0.02SrTiO
3The material of expression constitutes.
6. piezoelectric ceramics as claimed in claim 3 is characterized in that by composition formula [0.78Bi
0.5Na
0.5TiO
3+ 0.15Bi
0.5K
0.5TiO
3+ 0.02BaTiO
3+ 0.05SrTiO
3] (92wt%)+CeO
2(2wt%)+Nb
2O
5(6wt%) material of expression constitutes.
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CN 200310110878 CN1290796C (en) | 2003-11-07 | 2003-11-07 | Sodium bismuth titanate base nonleaded piezoelectric ceramic |
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CN 200310110878 CN1290796C (en) | 2003-11-07 | 2003-11-07 | Sodium bismuth titanate base nonleaded piezoelectric ceramic |
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CN1329340C (en) * | 2005-09-09 | 2007-08-01 | 北京工业大学 | Preparation method of leadless piezo-electric ceramic K0.5Bi0.5TiO3 nanometer wire and its sintering body |
CN100347129C (en) * | 2005-12-27 | 2007-11-07 | 中国科学院上海硅酸盐研究所 | Nanometer bismuth titanate aqueous casting slurry and preparation method thereof |
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2003
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CN112898016A (en) * | 2013-08-07 | 2021-06-04 | Pi陶瓷有限责任公司 | Lead-free piezoceramic material based on sodium bismuth titanate (BNT) |
CN103708829A (en) * | 2013-12-19 | 2014-04-09 | 桂林电子科技大学 | Abnormal piezoelectric anisotropy lead-free piezoelectric ceramic and texturing preparation method thereof |
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