CN104425702A - Composite piezoelectric element - Google Patents
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- CN104425702A CN104425702A CN201410391861.7A CN201410391861A CN104425702A CN 104425702 A CN104425702 A CN 104425702A CN 201410391861 A CN201410391861 A CN 201410391861A CN 104425702 A CN104425702 A CN 104425702A
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Abstract
A composite piezoelectric element is provided to be improved in bending resistance. The composite piezoelectric element (101) includes a flexible substrate (19), a first electrode layer (11) arranged on the substrate (19), a piezoelectric body layer (13) arranged on the first electrode layer (11) and having resin and piezoelectric particles, and a second electrode layer (12) arranged on the piezoelectric body layer (13). The composite piezoelectric element is characterized in that the piezoelectric body layer (13) includes two first piezoelectric body layers (13A, 13B) and a second piezoelectric body layer (13C) between the two first piezoelectric body layers (13A, 13B), wherein the concentration of volume percent of the piezoelectric particles of the second piezoelectric body layer (13C) is lower than that of the first piezoelectric body layers (13A, 13B).
Description
Technical field
The present invention relates to the piezoelectric element used in actuator, various transducer and generating etc.
Background technology
Piezoelectric element is used to the energy conversion between electric energy and mechanical energy, is widely used in actuator or various transducer.And then, be investigated the application in generating in recent years.
Consider such piezoelectric element to be layered on film base material, to be applied to situation about being required in flexible various goods.In patent documentation 1 (past case 1), disclose the piezoelectric element 810 on the surperficial 832a of the supporting mass 832 being layered in flexible base, board as shown in Figure 11.Figure 11 is the schematic diagram of the electronic component 830 representing the piezoelectric element 810 using past case 1.Piezoelectric element 810 shown in Figure 11 by the 1st conductive elastomer base material 822 on the surperficial 832a being layered in supporting mass 832, be layered in the piezoelectrics 820 on the 1st conductive elastomer base material 822 and the 2nd conductive elastomer base material 824 be located on the surperficial 820a of piezoelectrics 820 is formed.
But, in the piezoelectric element 810 of past case 1, when using piezoelectricity single crystals or piezoelectric ceramic in piezoelectrics 820, because piezoelectrics 820 are more crisp, so only can by supporting mass 832 slight curve.In addition, even the piezoelectric compound (composite) that dispersion is mixed with piezoelectrics particle equably in macromolecule matrix to be used in the situation in piezoelectrics 820, when supporting mass 832 is bent significantly, the possibility that piezoelectrics 820 occur crackle is larger.On the other hand, use the high molecular situation of piezoelectricity in piezoelectrics 820 under, bending bending tolerance is likely improved, but in piezoelectricity macromolecule, the piezoelectric property of wishing can not be obtained.
So, in patent documentation 2 (past case 2), as the macromolecule matrix of piezoelectric compound, propose in fig. 12 and use elastomeric generating element 901.Figure 12 is the thickness direction general profile chart of the structure of the generating element 901 of the static capacity change type representing past case 2, in Figure 12, (a) represents by the state A before applying compression stress in the stacking direction on generating element 901, and in Figure 12, (b) represents and be applied in the state B of compression stress.Generating element 901 shown in Figure 12 possesses and in dielectric elastomer 910, to disperse the mixture of strong dielectric particle 911 (composite) layer 912 and form as the pair of electrodes be equipped on the two sides of mixture layer 912 and electrode 921 and electrode 922.
Further, if the state A of generating element 901 from Figure 12 shown in (a), generating element 901 is applied compression stress in the stacking direction, then dielectric elastomer 910 strain, becomes the state B in Figure 12 shown in (b).On the other hand, if compression stress is removed, then state A to be got back to from state B.In the generating element 901 of past case 2, in order to stretch significantly in a thickness direction, use thermosetting elastomer or thermoplastic elastomer (TPE) as dielectric elastomer 910.Pass through especially from this state A to state B or the contrary change from state B to state A, between electrode 921 and electrode 922, potential difference occurs, the change of this potential difference can be taken out as electric power by generating element 901.
In order to be taken out more by this electric power, it is greatly effective for making the concentration of volume percent (vol%) of the strong dielectric particle 911 of the mixture layer 912 of generating element 901 become large, surface charge density is become.On the other hand, if the concentration of volume percent of strong dielectric particle 911 is excessive, then the Young's modulus of mixture layer 912 uprises, and brings harmful effect to strain, and durability likely step-down.So, the concentration of volume percent describing the strong dielectric particle 911 in mixture layer 912 preferably about 10 ~ 60%.
Patent documentation 1: JP 2013-21176 publication
Patent documentation 2: JP 2012-164917 publication
But in the generating element 901 of past case 2, the intensity about bending direction is not made open, can think for bending more weak.Particularly, if the concentration of volume percent of strong dielectric particle 911 is brought up to about 50% in order to improve performance, then the Young's modulus of mixture layer 912 uprises, and has the problem really declined for bending tolerance.
Summary of the invention
The present invention solves the problem, and object is to provide a kind of compound piezoelectric element improved for bending tolerance.
In order to solve this problem, compound piezoelectric element of the present invention possesses: flexible substrate; 1st electrode layer, arranges over the substrate; Piezoelectric body layer, is disposed on the 1st electrode layer, has resin and piezoelectric particles; 2nd electrode layer, is disposed on this piezoelectric body layer; It is characterized in that, the 2nd piezoelectric body layer that above-mentioned piezoelectric body layer has two the 1st piezoelectric body layers and is disposed between above-mentioned two the 1st piezoelectric body layers; 2nd piezoelectric body layer is compared with above-mentioned 1st piezoelectric body layer, and the concentration of volume percent of above-mentioned piezoelectric particles is low.
Accordingly, compound piezoelectric element of the present invention due to the concentration of volume percent of the piezoelectric particles of the 2nd piezoelectric body layer lower, so the improving for bending tolerance of the 2nd piezoelectric body layer.Therefore, compared with situation about forming with by the individual layer of the higher piezoelectric body layer of the concentration of volume percent of piezoelectric particles, improving for bending tolerance with the 2nd piezoelectric body layer, piezoelectric body layer also bending tolerance improves.Further, owing to having made the structure clipped with the 1st piezoelectric body layer that the concentration of volume percent of piezoelectric particles is higher, so the performance making the 1st piezoelectric body layer is preferential, the overall piezoelectric property of piezoelectric body layer can not decline significantly.Thereby, it is possible to be provided in the compound piezoelectric element maintaining and improve while piezoelectric property, for bending tolerance.
In addition, the feature of compound piezoelectric element of the present invention is, the above-mentioned concentration of volume percent of the above-mentioned piezoelectric particles of above-mentioned 1st piezoelectric body layer is 50 ~ 65vol%.
Accordingly, piezoelectric particles is fully filled in the 1st piezoelectric body layer, so can obtain higher piezoelectric property.
In addition, the feature of compound piezoelectric element of the present invention is, the strong dielectric particle of above-mentioned piezoelectric particles to be crystal structure be perovskite structure.
Accordingly, the piezoelectric property of piezoelectric body layer can be made to improve.Thereby, it is possible to the compound piezoelectric element providing output performance good.
In addition, the feature of compound piezoelectric element of the present invention is, above-mentioned strong dielectric particle is potassium niobate; The averaged particles footpath of above-mentioned potassium niobate is 400nm ~ 500nm, and the transition temperature of iris-regular crystal is more than 223 DEG C and less than 228 DEG C, and the transition temperature of regular crystal-cubic crystal is more than 420 DEG C and less than 430 DEG C.
Accordingly, by using above-mentioned potassium niobate, the piezoelectric property of piezoelectric body layer can be made to improve further.Thereby, it is possible to provide output performance better compound piezoelectric element.
In addition, the feature of compound piezoelectric element of the present invention is, above-mentioned substrate be use PET, PEN, PI, PE, PPS, aromatic polyamide resin (Japanese: ア ラ ミ De Trees fat) certain material insulating film or be filled with in above-mentioned material inorganic filler be equipped with in the film of filler certain; Above-mentioned resin is non-crystalline polyester or polyurethane; Modulus of elasticity under-40 DEG C of environment of above-mentioned 2nd piezoelectric body layer is below 1.5GPa, preferably below 0.5GPa, and the yield strength under-40 DEG C of environment is more than 15MPa, preferably more than 30MPa.
Accordingly, even if under-40 DEG C of environment, also the 2nd piezoelectric body layer can be bent with less radius of curvature.Therefore, with the bending fully tolerance of the 2nd piezoelectric body layer, the bending fully tolerance of piezoelectric body layer can be obtained.Further, by using above-mentioned substrate and resin, even if under-40 DEG C of environment, the sufficient flexibility of compound piezoelectric element can also be obtained.
In addition, the feature of compound piezoelectric element of the present invention is, the above-mentioned concentration of volume percent of the above-mentioned piezoelectric particles of above-mentioned two the 1st piezoelectric body layers is identical.
Accordingly, the performance of piezoelectric body layer can not be tied down (impact, Japanese: draw I ず ら れ Ru) by the performance of lower the 1st piezoelectric body layer of concentration of volume percent.Thereby, it is possible to guarantee the sufficient piezoelectric property of piezoelectric body layer.In addition, can raw material be used when manufacturing piezoelectric body layer, easily can manufacture piezoelectric body layer.
In addition, the feature of compound piezoelectric element of the present invention is, above-mentioned 2nd piezoelectric body layer is than above-mentioned 1st piezoelectrics thickness.
Accordingly, in piezoelectric body layer entirety, compared with the 1st piezoelectric body layer, the large percentage of the 2nd piezoelectric body layer that bending tolerance is higher, so the bending tolerance of piezoelectric body layer entirety improves further.Thereby, it is possible to provide the compound piezoelectric element that bending tolerance improves further.
Compound piezoelectric element of the present invention due to the concentration of volume percent of the piezoelectric particles of the 2nd piezoelectric body layer lower, so the improving for bending tolerance of the 2nd piezoelectric body layer.Therefore, compared with situation about forming with by the individual layer of the higher piezoelectric body layer of the concentration of volume percent of piezoelectric particles, improving for bending tolerance with the 2nd piezoelectric body layer, piezoelectric body layer also bending tolerance improves.Further, owing to having made the structure clipped with the 1st piezoelectric body layer that the concentration of volume percent of piezoelectric particles is higher, so the performance making the 1st piezoelectric body layer is preferential, the piezoelectric property of piezoelectric body layer can not decline significantly.Thereby, it is possible to be provided in the compound piezoelectric element maintaining and improve while piezoelectric property, for bending tolerance.
Accompanying drawing explanation
Fig. 1 is the structure chart of the compound piezoelectric element that the 1st execution mode of the present invention is described, is its plane graph.
Fig. 2 is the structure chart of the compound piezoelectric element that the 1st execution mode of the present invention is described, is the end view observed from the Y2 side shown in Fig. 1.
Fig. 3 (a) is the figure of the compound piezoelectric element that the 1st execution mode of the present invention is described, is the cutaway view of the III-III line shown in Fig. 1.
Fig. 3 (b) is the figure of the compound piezoelectric element that the 1st execution mode of the present invention is described, is the cutaway view of the IV-IV line shown in Fig. 1.
Fig. 4 illustrates the method for split pole process and the concept map of principle, in Fig. 4, (a) represents the initial state of piezoelectric body layer, in Fig. 4, (b) represents the state being applied with voltage on the thickness direction of piezoelectric body layer, and in Fig. 4, (c) represents the state that split pole process terminates.
Fig. 5 is the measurement result of the physical property of the piezoelectric particles used in the compound piezoelectric element of the 1st execution mode of the present invention, is the curve chart that the Differential Scanning Calorimetry of potassium niobate is measured.
Fig. 6 is the measurement result of the compound piezoelectric element of the 1st execution mode for the present invention, is the curve chart that the piezoelectric element changed the concentration of volume percent of piezoelectric particles applies output voltage values when vibrating.
Fig. 7 is the measurement result of the compound piezoelectric element of the 1st execution mode for the present invention, is the curve chart of the output voltage values of the piezoelectric element changed the average grain diameter of potassium niobate when being applied with vibration.
Fig. 8 is the measurement result of the compound piezoelectric element of the 1st execution mode for the present invention, is the curve chart of the minimum profile curvature radius calculated representing the piezoelectrics epithelium corresponding with the amount of piezoelectric particles.
Fig. 9 is the figure of the variation 1 of the compound piezoelectric element that the 1st execution mode for the present invention is described, is the end view compared with Fig. 2.
Figure 10 is the figure of the variation 2 of the compound piezoelectric element that the 1st execution mode for the present invention is described, is the cutaway view compared with Fig. 3 (a).
Figure 11 is the schematic diagram of the electronic component representing the piezoelectric element using past case 1.
Figure 12 is the thickness direction general profile chart of the structure of the generating element of the static capacity change type representing past case 2, in Figure 12, (a) expression is applied the state A before compression stress in the stacking direction on generating element, and in Figure 12, (b) expression has been applied in the state B of compression stress.
Embodiment
Hereinafter, with reference to the accompanying drawings of embodiments of the present invention.
[the 1st execution mode]
Fig. 1 is the structure chart of the compound piezoelectric element 101 that the 1st execution mode of the present invention is described, is its plane graph.In addition, in FIG, in order to make explanation easy understand, the part covering parts 15 is outward omitted.Fig. 2 is the structure chart of the compound piezoelectric element 101 that the 1st execution mode of the present invention is described, is the end view observed from the Y2 side shown in Fig. 1.Fig. 3 (a) is the figure of the compound piezoelectric element 101 that the 1st execution mode of the present invention is described, is the cutaway view of the III-III line shown in Fig. 1, and Fig. 3 (b) is the cutaway view of the IV-IV line shown in Fig. 1.In addition, Fig. 1 to Fig. 3 (b) is used to the structure chart making explanation easy understand, thus the size of thickness direction (Z1-Z2 direction) from actual have different significantly.
The compound piezoelectric element 101 of the 1st execution mode of the present invention, as shown in Fig. 1 to Fig. 3 (b), possesses flexible substrate 19, the 1st electrode layer 11 be disposed on substrate 19, is disposed in the piezoelectric body layer 13 on the 1st electrode layer 11 and the 2nd electrode layer 12 that is disposed on piezoelectric body layer 13 and forming.In addition, also possess and cover parts 15 for what compound piezoelectric element 101 was protected from external environment condition and be used for supplying electric power to compound piezoelectric element 101 or taking out two portion of terminal (171,172) of electric power from compound piezoelectric element 101 outward.
The substrate 19 of compound piezoelectric element 101 uses polyimides (PI, Polyimide) film, has flexibility thickness about 25 ~ 125 μm.Particularly, be that the bending of a few about mmR also has sufficient tolerance for radius.In addition, substrate 19 for flexibility preferably uses polyimide film (PI), but also can be other synthetic resin, such as PETG (PET, Polyethylene terephthalate), PEN (PEN, Polyethylenenaphthalate), polyphenylene sulfide (PPS, Poly Phenylene Sulfide), polyethylene (PE, Polyethylene), the insulating film of aromatic polyamide resin (aromatic polyamide, Aromatic polyamid).In addition, also can be the film that filler is housed being filled with inorganic filler in above-mentioned material.
1st electrode layer 11 of compound piezoelectric element 101 is as shown in Fig. 1 to Fig. 3 (b), the stacked one side side being located at substrate 19, the powder of silver of the conductivity that is scattered here and there with 25 ~ 70 (vol%) in the matrix in phenolic resins, its thickness is about 5 ~ 15 μm.
2nd electrode layer 12 of compound piezoelectric element 101 is as shown in Fig. 1 to Fig. 3 (b), the stacked one side side being located at substrate 19, as shown in Fig. 3 (a), Fig. 3 (b), clip piezoelectric body layer 13 with the 1st electrode layer 11 and to be stackedly formed on piezoelectric body layer 13.In addition, the 2nd electrode layer 12 is same with the 1st electrode layer 11, and the powder of silver of the conductivity that is scattered here and there with 20 ~ 70 (vol%) in the matrix in phenolic resins, its thickness is about 5 ~ 20 μm.As the material of the electroconductive component of these the 1st electrode layers 11 and the 2nd electrode layer 12, preferably use silver, but also can be carbon.When being set to carbon, the powder of carbon of the conductivity that is scattered here and there with 5 ~ 70 (vol%) in the matrix in phenolic resins.
In addition, the making of the 1st electrode layer 11 and the 2nd electrode layer 12 is mixed with silver powder by the solvent of the phenolic resins containing curing agent, glycol monobutyl ether acetate (Carbitol acetate) etc. and makes conductivity silver paste and use the method for silk screen printing etc. to carry out.Specifically, the 1st electrode layer 11 is coated on substrate 19 by this conductivity silver paste, heats, and make its dry and sclerosis and formed, and the 2nd electrode layer 12 is coated on piezoelectric body layer 13 by this conductivity silver paste, heats, and make its dry and sclerosis and formed.
In addition, in the operation identical with the 1st electrode layer 11, construction drawing 1 and the portion of terminal shown in Fig. 3 (a) 171, and in the operation identical with the 2nd electrode layer 12, construction drawing 1 and the portion of terminal shown in Fig. 3 (b) 172.This portion of terminal 171 and portion of terminal 172 are formed, easily to carry out supply or the taking-up of electric power in the mode being drawn out to the end of substrate 19 from the end of the 1st electrode layer 11 or the end of the 2nd electrode layer 12.
In addition, use phenolic resins as the adhesive of conductivity silver paste, but also can be other synthetic resin, such as, as the polyurethane resin, epoxy resin etc. of thermosetting resin or the mylar, allyl resin etc. as thermoplastic resin.In addition, use silver powder as the conductive filling of conductivity silver paste, but also can be other conductive filling, the carbon dust of such as graphite, nano-sized carbon etc. or the metal powder of copper, nickel etc.
The piezoelectric body layer 13 of compound piezoelectric element 101, as shown in Fig. 1 to Fig. 3 (b), is located at the one side side of substrate 19, is stackedly formed on the 1st electrode layer 11.Further, piezoelectric body layer 13 is configured to the 2nd piezoelectric body layer 13C that has two the 1st piezoelectric body layers (13A, 13B) and be disposed between two the 1st piezoelectric body layers (13A, 13B).
In addition, piezoelectric body layer 13 is dispersed with piezoelectric particles in the matrix of amorphous polyester resin or polyurethane resin, in the 1st execution mode of the present invention, uses the strong dielectric particle of the crystal structure of perovskite structure as this piezoelectric particles.Thereby, it is possible to make the piezoelectric property of piezoelectric body layer 13 improve, the compound piezoelectric element 101 that output performance is good can be provided.
In addition, in the 1st execution mode of the present invention, as this strong dielectric particle, particularly preferably be and use potassium niobate (KNbO
3).This potassium niobate use that averaged particles footpath is 400 ~ 500nm, the transition temperature of iris-regular crystal is more than 223 DEG C and less than 228 DEG C, the transition temperature of regular crystal-cubic crystal is more than 420 DEG C and the particle of less than 430 DEG C.Thereby, it is possible to make the piezoelectric property of piezoelectric body layer 13 improve further.Thereby, it is possible to provide output performance better compound piezoelectric element 101.
In addition, this piezoelectric body layer 13 owing to being such with composite wood that is synthetic resin, so have flexibility.Particularly, because amorphous polyester resin or polyurethane resin have the flexibility of appropriateness at normal temperatures, even if so piezoelectric body layer 13 is out of shape, the crackle etc. occurred in piezoelectric body layer 13 also can be suppressed.And then amorphous polyester resin and polyurethane resin are generally used widely, can easily and obtain cheaply, so can preferably use.
In 1st piezoelectric body layer (13A, 13B) of piezoelectric body layer 13, the concentration of volume percent of piezoelectric particles (being potassium niobate in the 1st execution mode of the present invention) is adjusted to 50 ~ 65vol%.Thus, piezoelectric particles is fully filled in the 1st piezoelectric body layer (13A, 13B), can obtain higher piezoelectric property.In addition, the concentration of volume percent of piezoelectric particles is adjusted to identical by the 1st piezoelectric body layer 13A and the 1st piezoelectric body layer 13B.
On the other hand, the concentration of volume percent of piezoelectric particles adjusts lower than the 1st piezoelectric body layer (13A, 13B) by the 2nd piezoelectric body layer 13C of piezoelectric body layer 13.Specifically, can 0.01 ~ 60vol% be set to, preferably be set to 10 ~ 50vol%.In addition, when the concentration of volume percent of the piezoelectric particles of the 2nd piezoelectric body layer 13C is more than 50vol%, also the concentration of volume percent of the piezoelectric particles of the 1st piezoelectric body layer (13A, 13B) is adjusted to the concentration of volume percent higher than the 2nd piezoelectric body layer 13C.
Thus, the concentration of volume percent of the piezoelectric particles of the 2nd piezoelectric body layer 13C is lower, so the improving for bending bending tolerance of the 2nd piezoelectric body layer 13C.Therefore, compared with situation about forming with by the individual layer of the higher piezoelectrics of the concentration of volume percent of piezoelectric particles, with the raising for bending bending tolerance of the 2nd piezoelectric body layer 13C, piezoelectric body layer 13 also bending tolerance improves.And, due to the structure for being clipped by higher the 1st piezoelectric body layer 13A of the concentration of volume percent of piezoelectric particles and the 1st piezoelectric body layer 13B, so the performance making the 1st piezoelectric body layer (13A, 13B) is preferred, the piezoelectric property of piezoelectric body layer 13 entirety can not decline significantly.Thereby, it is possible to the compound piezoelectric element 101 improved while being provided in maintenance piezoelectric property, for bending bending tolerance.In addition, by the layer that the concentration of volume percent that clips piezoelectric particles is lower, the piezoelectric body layer 13 of piezoelectric property while the use amount reducing expensive piezoelectric particles can be formed in, is maintained.
In addition, elastic modulus E under-40 DEG C of environment of the 2nd piezoelectric body layer 13C used in the 1st execution mode of the present invention is below 1.5GPa, preferably below 0.5GPa, and the yield strength σ under-40 DEG C of environment is more than 15MPa, preferably more than 30MPa.Here, when the 2nd piezoelectric body layer 13C has certain thickness t, according to elastic modulus E and yield strength σ, the minimum profile curvature radius R of the 2nd piezoelectric body layer 13C can be calculated by following formula (A).
(A)σ＝E×t/(2×R)
σ: yield strength, E: modulus of elasticity, t: thickness, R: minimum profile curvature radius
Such as, when the thickness t of the 2nd piezoelectric body layer 13C is 20 μm, if elastic modulus E be 1.5GPa, yield strength σ is 15MPa, then minimum profile curvature radius R may be calculated 1mm.
Thus, under-40 DEG C of environment, also the 2nd piezoelectric body layer 13C can be bent with less radius of curvature.Therefore, with the bending fully tolerance of the 2nd piezoelectric body layer 13C, the bending fully tolerance of piezoelectric body layer 13 can be obtained.Further, by using resin in above-mentioned substrate 19 and adhesive, under-40 DEG C of environment, the sufficient flexibility of compound piezoelectric element 101 can also be obtained.In addition, as piezoelectric particles, preferably use the potassium niobate (KNbO of strong dielectric
3), but lithium niobate (LiNbO can be used
3), sodium niobate (NaNbO
3), barium titanate (BaTiO
3), zincic acid bismuth titanates (Bi (Zn/Ti) O
3), cobalt acid bismuth (BiCoO
3), lead zirconate titanate (Pb (Zr/Ti) O
3) etc.
In addition, in the 1st execution mode of the present invention, the concentration of volume percent of the piezoelectric particles of the 1st piezoelectric body layer 13A and the 1st piezoelectric body layer 13B is adjusted to identical.Thus, the performance of piezoelectric body layer 13 can not be tied down (impact) by the performance of certain of lower the 1st piezoelectric body layer 13A of concentration of volume percent or the 1st piezoelectric body layer 13B.Thereby, it is possible to guarantee the sufficient piezoelectric property of piezoelectric body layer 13.In addition, when manufacturing piezoelectric body layer 13, identical raw material can be used, can easily manufacture piezoelectric body layer 13.Thereby, it is possible to make compound piezoelectric element 101 cheaply.
In addition, in the 1st execution mode of the present invention, as shown in Fig. 3 (a), Fig. 3 (b), the 2nd piezoelectric body layer 13C becomes thicker than the 1st piezoelectric body layer (13A, 13B).Thus, in piezoelectric body layer 13 entirety, compare the 1st piezoelectric body layer (13A, 13B), bend the ratio change of the 2nd higher piezoelectric body layer 13C of tolerance greatly, so the bending tolerance of piezoelectric body layer 13 entirety improves further.Thereby, it is possible to the compound piezoelectric element 101 providing bending tolerance to improve further.
The making of piezoelectric body layer 13 uses solvable amorphous polyester resin or polyurethane resin first in a solvent, the solvent of this adhesive resin and glycol monobutyl ether acetate etc. is mixed with the mix proportion of hope with the plastochondria of potassium niobate, make it disperse equably with the mixer of 3 rollers etc., make dielectric paste.Now, the 1st dielectric paste coordinated with the ratio of hope by the plastochondria of adhesive resin and potassium niobate is made in the mode of concentration of volume percent of the piezoelectric particles corresponding to the 1st piezoelectric body layer (13A, 13B).Equally, the 2nd dielectric paste coordinated with the ratio of hope by the plastochondria of adhesive resin and potassium niobate is made in the mode of concentration of volume percent of the piezoelectric particles corresponding to the 2nd piezoelectric body layer 13C.
Then, use the method for silk screen printing etc., to make the mode that the 1st electrode layer 11 covers the one side side of substrate 19 apply the 1st dielectric paste, and make its drying and harden and make the 1st piezoelectric body layer 13A.The thickness of the 1st piezoelectric body layer 13A after this sclerosis preferably about 3 ~ 10 μm.Then, the same method using silk screen printing etc., applies the 2nd dielectric paste in the mode making the 1st piezoelectric body layer 13A cover the one side side of substrate 19, and makes its drying and harden and make the 2nd piezoelectric body layer 13C.The thickness of the 2nd piezoelectric body layer 13C after this sclerosis preferably about 10 ~ 50 μm.
Then, apply the 1st dielectric paste to make the 2nd piezoelectric body layer 13C cover the mode of the one side side of substrate 19, and make its drying and harden and make the 1st piezoelectric body layer 13B.The thickness of the 1st piezoelectric body layer 13B after this sclerosis is same with the 1st piezoelectric body layer 13A, preferably about 3 ~ 10 μm.In addition, in above-mentioned dielectric paste (the 1st dielectric paste, the 2nd dielectric paste), also can suitably use a small amount of curing agent, also can add defoamer.In addition, also can carry out making the surface of the plastochondria of potassium niobate support the process of silane couplent.Particularly, by carrying out interpolation or the silane couplent process of defoamer, the defect of gassing etc. in piezoelectric body layer 13 can be prevented, the poor flow of the thickness direction of piezoelectric body layer 13 can be reduced.
Finally, split pole process is carried out to formed piezoelectric body layer 13.Fig. 4 illustrates the method for split pole process and the concept map of principle, in Fig. 4, (a) represents the initial state of piezoelectric body layer 13, in Fig. 4, (b) represents the state being applied with voltage on the thickness direction of piezoelectric body layer 13, and in Fig. 4, (c) represents the state that split pole process terminates.In addition, in the drawings, plastochondria NB and adhesive resin (mylar or the polyurethane resin) PP of potassium niobate is illustrated as piezoelectric body layer 13.
In split pole process, the piezoelectric body layer 13 of formation is heated to the temperature of vicinity of Curie temperatures, from the portion of terminal 171 shown in Fig. 1 and Fig. 3 (a), Fig. 3 (b) and portion of terminal 172, as shown in (b) in Fig. 4, with 1 ~ 10 (V/ μm) left and right, the direct voltage corresponding with the thickness of piezoelectric body layer 13 is applied to piezoelectric body layer 13.Further, after getting back to normal temperature, make short circuit between the 1st electrode layer 11 and the 2nd electrode layer 12, the removing of unnecessary electric capacity is terminated.In addition, the applying of direct voltage preferably 4 ~ 6 (V/ μm).Like this, piezoelectric body layer 13 can initial condition from Fig. 4 shown in (a) process to the state of the split pole shown in (c) in Fig. 4 simply.
As above, the 1st electrode layer 11, piezoelectric body layer 13 and the 2nd electrode layer 12 are the structures being dispersed with filler in synthetic resin, so can have sufficient flexibility accordingly with the flexibility of substrate 19.
Finally, in the 1st execution mode of the present invention, in order to be provided with from external environment condition protection by compound piezoelectric element 101, cover parts 15.In addition, when replacing the powder of silver and use the powder of the carbon of conductivity in the 1st electrode layer 11 and the 2nd electrode layer 12, have and this outer situation covering parts 15 also can not be set.
In addition, cover in the making of parts 15 outside, use the insulating properties cream based on the polyurethane resin of the insulating properties containing pigment, the method of same use silk screen printing etc. by this insulating properties cream to cover the 2nd electrode layer 12 mode on the whole and to apply stacked, and heat, make its dry and sclerosis.The outer thickness covering parts 15 after this sclerosis is about 10 ~ 100 μm.In addition, beyond polyurethane resin, also can use acrylic resin, mylar, epoxy resin etc.So like this, compound piezoelectric element 101 such shown in Fig. 1 to Fig. 3 (b) is formed.Owing to using simple and cheap silk screen print method in the formation of this compound piezoelectric element 101, so compound piezoelectric element 101 easily can be made and can make cheaply.
For the effect of the compound piezoelectric element 101 of the 1st execution mode of the present invention formed as described above, the embodiment referring to the compound piezoelectric element 101 of actual fabrication is described.
< embodiment >
First, the sample (sample) of the compound piezoelectric element 101 used in the measurements is specifically described.The sample (sample) of compound piezoelectric element 101 uses thickness to be that polyimides (PI) film of 75 μm is as substrate 19.In addition, as the 1st electrode layer 11 and the 2nd electrode layer 12, to be used at 260 DEG C heating and within 30 minutes, to make it solidify and the film that obtains, its thickness is 5 μm, the silver powder of the conductivity containing 40 (vol%) in the matrix in phenolic resins.In addition, as covering parts 15 outward, to be used at 150 DEG C heating and within 10 minutes, to make it solidify and the film that obtains, its thickness is 10 μm, based on the polyurethane resin of the insulating properties containing pigment.
In addition, as the 1st piezoelectric body layer 13A and the 1st piezoelectric body layer 13B, being used at 260 DEG C heating makes it solidify in 20 minutes and the film that obtains, its thickness is 5 μm, containing the plastochondria of 60 (vol%) as the potassium niobate of strong dielectric particle in the matrix in the thermoplastic resin of amorphous polyester resin.
Fig. 5 is the measurement result of the physical property of the piezoelectric particles used in the compound piezoelectric element 101 of the 1st execution mode of the present invention, is the curve chart of the differential scanning calorimetry (DSC, Differentialscanning calorimetry) of potassium niobate.Transverse axis represents temperature, and the longitudinal axis represents heat flow.As shown in Figure 5, the averaged particles footpath of the plastochondria of potassium niobate used herein is 400nm, and the transition temperature of iris-regular crystal is 223.6 DEG C, and the transition temperature of regular crystal-cubic crystal is 424 DEG C (A1 (solid line) shown in Fig. 5).In addition, in order to compare, the particle (C2 (single dotted broken line) shown in Fig. 5) that the particle (C1 (dotted line) shown in Fig. 5) that use averaged particles footpath is 200nm, the transition temperature of iris one regular crystal is 208.6 DEG C, the transition temperature of regular crystal-cubic crystal is 411.9 DEG C and averaged particles footpath are 200nm, the transition temperature of iris-regular crystal is 208.6 DEG C, the transition temperature of regular crystal-cubic crystal is 411.9 DEG C, also produces duplicate.
In addition, as the 2nd piezoelectric body layer 13C, use some to heat at 260 DEG C to make it solidify in 20 minutes and the film that obtains, its thickness is 10 μm, the plastochondria of the potassium niobate as strong dielectric particle containing 20 ~ 60vol% in the matrix in the thermoplastic resin of amorphous polyester resin.In addition, in order to compare, make the structure that the 2nd piezoelectric body layer 13C is not set, also making the duplicate of the piezoelectrics of only one deck.
Then, split pole process is carried out to the sample (sample) of the compound piezoelectric element 101 produced as described above.Split pole process by being heated to 250 DEG C, apply the direct voltage of 1 hour 100V from the portion of terminal 171 shown in Fig. 1 and Fig. 3 (a), Fig. 3 (b) and portion of terminal 172 pairs of piezoelectric body layers 13 and carry out.
For the sample produced as described above, its sensitivity is measured.In the measurement, the sample (sample) being formed with piezoelectric body layer 13 is applied to occur the such vibration of the displacement of 0.5mm with the frequency of 2Hz, measures output voltage now.Further, suppose that this output voltage the greater is the piezoelectrics that sensitivity is higher.
Fig. 6 is the measurement result of the compound piezoelectric element 101 of the 1st execution mode for the present invention, is the curve chart that the piezoelectric element changed the concentration of volume percent of piezoelectric particles applies output voltage values when vibrating.Transverse axis is the percent by volume containing piezoelectric particles, and the longitudinal axis is output voltage values.SP1 (solid line) in figure is the measurement result of the sample of the amount of the plastochondria of the potassium niobate changed in the 2nd piezoelectric body layer 13C, and the CS1 (dotted line) in figure is the measurement result of the duplicate of the piezoelectrics of only one deck.Fig. 7 is the measurement result of the compound piezoelectric element 101 of the 1st execution mode for the present invention, is the curve chart that the piezoelectric element changed the average grain diameter of potassium niobate applies output voltage values when vibrating.Transverse axis is the average grain diameter of potassium niobate, and the longitudinal axis is output voltage values.SP2 in figure is the measurement result of average grain diameter for 400nm of the potassium niobate used in the present embodiment, the measurement result of to be the average grain diameter of potassium niobate the be duplicate of 200nm and 800nm of CS2 and CS3 in figure.
The compound piezoelectric element 101 of the 1st execution mode of the present invention as shown in Figure 6, even if the amount of the plastochondria of the potassium niobate in the 2nd piezoelectric body layer 13C declines, also can not decline significantly as the comparative example be only made up of the piezoelectrics of one deck.This is because, owing to having made the structure clipped with the concentration of volume percent of piezoelectric particles the 1st higher piezoelectric body layer 13A and the 1st piezoelectric body layer 13B, so the performance making the 1st piezoelectric body layer (13A, 13B) is preferential, the piezoelectric property of piezoelectric body layer 13 entirety can not decline significantly.And then, the compound piezoelectric element 101 of the 1st execution mode of the present invention due to the concentration of volume percent being disposed in the 2nd piezoelectric body layer 13C piezoelectric particles compared with the 1st piezoelectric body layer (13A, 13B) between two the 1st piezoelectric body layers (13A, 13B) lower, so the improving for bending bending tolerance of the 2nd piezoelectric body layer 13C.Therefore, compared with situation about forming with the performance in order to improve piezoelectrics and by the individual layer of piezoelectrics of the concentration of volume percent that improve piezoelectric particles, improving for bending bending tolerance with the 2nd piezoelectric body layer 13C, piezoelectric body layer 13 also bending tolerance improves.Thereby, it is possible to the compound piezoelectric element 101 improved while being provided in maintenance piezoelectric property, for bending bending tolerance.
In addition, the compound piezoelectric element 101 of the 1st execution mode of the present invention due to the concentration of volume percent of the piezoelectric particles of the 1st piezoelectric body layer (13A, 13B) be 50 ~ 65vol%, so piezoelectric particles is fully filled in the 1st piezoelectric body layer (13A, 13B).Thus, even if make the concentration of volume percent step-down of the piezoelectric particles of the 2nd piezoelectric body layer 13C, also higher piezoelectric property can be obtained.Such as shown in Figure 6, even if the concentration of volume percent of the piezoelectric particles of the 1st piezoelectric body layer (13A, 13B) is 60vol%, the concentration of volume percent of the piezoelectric particles of the 2nd piezoelectric body layer 13C is 40vol%, also can obtain the output voltage values of more than 250mV, higher sensitivity can be obtained.
And then, because piezoelectric particles is the strong dielectric particle of perovskite structure, so the piezoelectric property of piezoelectric body layer 13 can be made to improve.Thereby, it is possible to the compound piezoelectric element 101 providing output performance good.
In addition, because the concentration of volume percent of the piezoelectric particles by the 1st piezoelectric body layer 13A and the 1st piezoelectric body layer 13B is adjusted to identical, so the performance of piezoelectric body layer 13 can not be tied down (impact) by the performance of certain of lower the 1st piezoelectric body layer 13A of concentration of volume percent or the 1st piezoelectric body layer 13B.Thereby, it is possible to guarantee the sufficient piezoelectric property of piezoelectric body layer 13.In addition, when manufacturing piezoelectric body layer 13, identical raw material can be used, can easily manufacture piezoelectric body layer 13.Thereby, it is possible to make compound piezoelectric element 101 cheaply.
In addition, the compound piezoelectric element 101 of the 1st execution mode of the present invention uses potassium niobate as the strong dielectric particle being piezoelectric particles, but preferably use that averaged particles footpath is 400 ~ 500nm, the transition temperature of iris-regular crystal is more than 223 DEG C and less than 228 DEG C, the transition temperature of regular crystal-cubic crystal is more than 420 DEG C and the potassium niobate of less than 430 DEG C.Thus, as shown in Figure 7, the piezoelectric property of piezoelectric body layer 13 can be made to improve further.Thereby, it is possible to provide output performance better compound piezoelectric element 101.
In addition, except the measurement sample of above-mentioned sensitivity characteristic, also make some epithelium samples containing the plastochondria of 20 ~ 60vol% potassium niobate in order to the measurement use of flexural property, (Shimadzu Seisakusho Ltd.'s (strain) makes to use cupping machine, model: オ ー ト グ ラ Off AGS-J500N), measure modulus of elasticity and the yield strength of some epithelium samples.As condition when measuring, measure under the environment of-40 DEG C.In addition, the convenience of epithelium sample in order to be measured by cupping machine of use, uses the sample of the 100 μm thickness thicker than the thickness 10 ~ 50 μm of the 2nd piezoelectric body layer 13C preferably used as reality.
As a result, the modulus of elasticity of epithelium sample TP1 (containing potassium niobate 20vol%) is 0.35Gpa, and yield strength is 35Mpa; The modulus of elasticity of epithelium sample TP2 (containing potassium niobate 35vol%) is 0.98Gpa, and yield strength is 25Mpa; The modulus of elasticity of epithelium sample TP3 (containing potassium niobate 50vol%) is 1.4Gpa, and yield strength is 15.8Mpa; The modulus of elasticity of epithelium sample TP4 (containing potassium niobate 60vol%) is 1.9Gpa, and yield strength is 5.4Mpa.Use this modulus of elasticity and yield strength, calculate the minimum profile curvature radius of epithelium sample (TP1, TP2, TP3, TP4).Fig. 8 is the measurement result of the compound piezoelectric element 101 of the 1st execution mode for the present invention, is the curve chart of the minimum profile curvature radius calculated representing the piezoelectrics epithelium corresponding with the amount of piezoelectric particles.
As shown in Figure 8, when the amount of the plastochondria of potassium niobate is below 50vol%, minimum profile curvature radius diminishes significantly.Amount due to the plastochondria of this potassium niobate is that the modulus of elasticity of the epithelium sample TP3 of 50vol% is 1.4Gpa, yield strength is 15.8Mpa, so can think the modulus of elasticity neighbouring by this and the yield strength epithelium characteristic as the 2nd piezoelectric body layer 13C.In addition, more preferably, be that (modulus of elasticity is 0.35Gpa for the epithelium sample TP1 of 20vol% by the amount of the plastochondria of this potassium niobate, yield strength is 35Mpa) with the amount of the plastochondria of potassium niobate be 35vol% epithelium sample TP2 (modulus of elasticity is 0.98Gpa, and yield strength is 25Mpa) between modulus of elasticity and yield strength as the epithelium characteristic of the 2nd piezoelectric body layer 13C.
According to the above results, the modulus of elasticity of the 2nd piezoelectric body layer 13C under-40 DEG C of environment is below 1.5GPa, preferably below 0.5GPa, and the yield strength under-40 DEG C of environment is more than 15MPa, preferably more than 30MPa.Thus, 2nd piezoelectric body layer 13C also can bend with less radius of curvature by the compound piezoelectric element 101 of the 1st execution mode of the present invention under-40 DEG C of environment, so bend tolerance with the sufficient of the 2nd piezoelectric body layer 13C, the bending fully tolerance of piezoelectric body layer 13 can be obtained.Further, by using resin in above-mentioned substrate and adhesive, under-40 DEG C of environment, the sufficient flexibility of compound piezoelectric element 101 can also be obtained.
In addition, because the 2nd piezoelectric body layer 13C is thicker than the 1st piezoelectric body layer (13A, 13B), so in piezoelectric body layer 13 entirety, compare the 1st piezoelectric body layer (13A, 13B), the ratio of the 2nd piezoelectric body layer 13C that bending tolerance is higher becomes large.Therefore, the bending tolerance of piezoelectric body layer 13 entirety improves further.Thereby, it is possible to the compound piezoelectric element 101 providing bending tolerance to improve further.
In addition, the present invention is not limited to above-mentioned execution mode, such as, can be out of shape as follows and implement, and these execution modes also belong to technical scope of the present invention.
Fig. 9 is the figure of the variation 1 of the compound piezoelectric element 101 that the 1st execution mode for the present invention is described, is the end view of the compound piezoelectric element C101 compared with Fig. 2.Figure 10 is the figure of the variation 2 of the compound piezoelectric element 101 that the 1st execution mode for the present invention is described, is the compound piezoelectric element C102 cutaway view compared with Fig. 3 (a).
< variation 1>
In above-mentioned 1st execution mode, to make in the stacked structure comprising the element of piezoelectric body layer 13 in the one side side of substrate 19, but as shown in Figure 9, also can to have made in the opposing face side of substrate 19 the also stacked structure comprising the element of piezoelectric body layer C13.
< variation 2>
In above-mentioned 2nd execution mode, by the 2nd piezoelectric body layer 13C of piezoelectric body layer 13 1 layer of formation, but be not limited thereto, such as shown in Figure 10, also can be the piezoelectric body layer C23 be made up of the 2nd piezoelectric body layer (23C, 33C) of 2 layers, also can be more than 2 layers.
The present invention is not limited to above-mentioned execution mode, can suitably change in the scope not departing from object of the present invention.
Label declaration
11 the 1st electrode layers
12 the 2nd electrode layers
13, C13, C23 piezoelectric body layer
13A, 13B the 1st piezoelectric body layer
13C, 23C, 33C the 2nd piezoelectric body layer
19 substrates
101, C101, C102 compound piezoelectric element
Claims (10)
1. a compound piezoelectric element, possesses:
Flexible substrate;
1st electrode layer, arranges over the substrate;
Piezoelectric body layer, is disposed on the 1st electrode layer, has resin and piezoelectric particles; And
2nd electrode layer, is disposed on this piezoelectric body layer;
The feature of this compound piezoelectric element is,
The 2nd piezoelectric body layer that above-mentioned piezoelectric body layer has two the 1st piezoelectric body layers and is disposed between above-mentioned two the 1st piezoelectric body layers;
2nd piezoelectric body layer is compared with above-mentioned 1st piezoelectric body layer, and the concentration of volume percent of above-mentioned piezoelectric particles is low.
2. compound piezoelectric element as claimed in claim 1, is characterized in that,
The above-mentioned concentration of volume percent of the above-mentioned piezoelectric particles of above-mentioned 1st piezoelectric body layer is 50 ~ 65vol%.
3. compound piezoelectric element as claimed in claim 1 or 2, is characterized in that,
The strong dielectric particle of above-mentioned piezoelectric particles to be crystal structure be perovskite structure.
4. compound piezoelectric element as claimed in claim 3, is characterized in that,
Above-mentioned strong dielectric particle is potassium niobate;
The averaged particles footpath of above-mentioned potassium niobate is 400nm ~ 500nm, and the transition temperature of iris-regular crystal is more than 223 DEG C and less than 228 DEG C, and the transition temperature of regular crystal-cubic crystal is more than 420 DEG C and less than 430 DEG C.
5. the compound piezoelectric element according to any one of Claims 1 to 4, is characterized in that,
Above-mentioned substrate be use PETG and PET, PEN and PEN, polyimides and PI, polyethylene and PE, polyphenylene sulfide and PPS, aromatic polyamide resin certain material insulating film or be filled with in above-mentioned material inorganic filler add in Packed film certain;
Above-mentioned resin is non-crystalline polyester or polyurethane;
The modulus of elasticity of above-mentioned 2nd piezoelectric body layer under-40 DEG C of environment is below 1.5GPa, preferably below 0.5GPa, and the yield strength under-40 DEG C of environment is more than 15MPa, preferably more than 30MPa.
6. the compound piezoelectric element according to any one of Claims 1 to 4, is characterized in that,
The above-mentioned concentration of volume percent of the above-mentioned piezoelectric particles of above-mentioned two the 1st piezoelectric body layers is identical.
7. the compound piezoelectric element according to any one of Claims 1 to 4, is characterized in that,
Above-mentioned 2nd piezoelectric body layer is than above-mentioned 1st piezoelectrics thickness.
8. compound piezoelectric element as claimed in claim 5, is characterized in that,
The above-mentioned concentration of volume percent of the above-mentioned piezoelectric particles of above-mentioned two the 1st piezoelectric body layers is identical.
9. compound piezoelectric element as claimed in claim 5, is characterized in that,
Above-mentioned 2nd piezoelectric body layer is than above-mentioned 1st piezoelectrics thickness.
10. compound piezoelectric element as claimed in claim 6, is characterized in that,
Above-mentioned 2nd piezoelectric body layer is than above-mentioned 1st piezoelectrics thickness.
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| JP6875206B2 (en) * | 2016-06-23 | 2021-05-19 | 日本化学工業株式会社 | Fillers for composite piezo materials, composite piezo elements and composite piezo materials |
| US11239409B2 (en) | 2016-06-23 | 2022-02-01 | Nippon Chemical Industrial Co., Ltd. | Piezoelectric material filler, composite piezoelectric material, composite piezoelectric device, composite piezoelectric material filler, and method for producing alkali niobate compound |
| IT201600118202A1 (en) | 2016-11-22 | 2018-05-22 | Atom Spa | COMPOSITE MATERIAL WITH ELECTROSTRICTIVE PROPERTIES FOR A MECHANICAL ENERGY RECOVERY DEVICE |
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