JP2007027692A - Stacked piezo-electric element and fuel injection device using it - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a stacked piezo-electric element that excels in durability having a large displacement amount under high voltage and high pressure capable of controlling the change of the displacement amount, even in the case of continuous driving for a long period of time, and to provide a fuel injection device using it. <P>SOLUTION: The piezo-electric element is composed of a lamination of multiple piezo-electric material layers 11 and metallic layers 12 that are piled alternatively. The multiple metal layers 12 consist of multiple metal layers 12b that has low filling factor of the metal constituting the metal layer 12 than that of the metal layer 12a adjoining at both sides in the laminated direction. This fuel injection device is equipped with a vessel 31 having a jet hole 33 and the piezo-electric element stored inside the vessel 31, and is configured so that liquid filled in the vessel 31 may be discharged from the jet hole 33 by the drive of the piezo-electric element. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

  The present invention relates to a multilayer piezoelectric element (hereinafter sometimes simply referred to as “element”) and an ejection device, and more particularly, to a multilayer piezoelectric element and an ejection device suitable for long-term continuous driving under high voltage and high pressure. About.

  2. Description of the Related Art Conventionally, piezoelectric actuators using stacked piezoelectric elements include piezoelectric actuators in which piezoelectric layers and metal layers are alternately stacked. In general, piezoelectric actuators are classified into two types: a co-fired type and a stack type in which piezoelectric ceramics made of one piezoelectric material and plate-like metal layers are alternately stacked. Of these, simultaneous firing type piezoelectric actuators are often used from the viewpoint of lowering the voltage and reducing the manufacturing cost. The co-fired type piezoelectric actuator can be easily thinned and is excellent in miniaturization and durability.

  FIG. 9A is a perspective view showing a conventional laminated piezoelectric element, and FIG. 9B is a partial perspective view showing a laminated state of a piezoelectric layer and a metal layer in FIG. 9A. . FIG. 10 is a partially enlarged cross-sectional view showing a multilayer structure in a conventional multilayer piezoelectric element. As shown in FIG. 9, the multilayer piezoelectric element includes a multilayer body 103 and a pair of external electrodes 105 formed on side surfaces facing each other. The laminated body 103 is formed by alternately laminating piezoelectric layers 101 and metal layers 102. Inactive layers 104 are stacked on both end surfaces of the stacked body 103 in the stacking direction. The metal layer 102 is not formed on the entire main surface of the piezoelectric layer 101 and has a so-called partial electrode structure. The metal layers 102 of this partial electrode structure are laminated so as to be exposed on different side surfaces of the laminated body 103 every other layer, and are connected to the pair of external electrodes 105 every other layer.

  A conventional method for manufacturing a multilayer piezoelectric element is as follows. That is, first, a metal paste is printed on a ceramic green sheet containing the raw material of the piezoelectric layer 101 with a pattern having a predetermined metal layer structure as shown in FIG. Next, a plurality of green sheets printed with a metal paste are laminated to produce a laminated molded body, which is fired to obtain a laminated body 103. Thereafter, a metal paste is applied to the opposite side surfaces of the laminated body 103, and then fired to form a pair of external electrodes 105 to obtain a laminated piezoelectric element shown in FIG. 9A (see, for example, Patent Document 1). .

  Here, in general, an alloy of silver and palladium is often used as the metal layer 102. Further, in order to simultaneously fire the piezoelectric layer 101 and the metal layer 102, the metal composition of the metal layer 102 is often set to 70% by mass of silver and 30% by mass of palladium (see, for example, Patent Document 2). Thus, the metal layer 102 made of a silver-palladium alloy is used instead of the metal layer made only of silver for the following reason.

  That is, when the metal layer 102 is composed only of silver not containing palladium, when a potential difference is applied between the opposing metal layers 102, the silver in the metal layer 102 moves from the positive electrode to the negative electrode in the opposing metal layer 102. This is because a so-called ion migration phenomenon occurs in which ions move along the element surface. This phenomenon tends to occur remarkably in a high temperature and high humidity atmosphere.

  On the other hand, conventionally, a metal paste prepared with substantially the same metal component ratio and metal concentration has been used for the purpose of forming the metal layer 102 having substantially the same metal filling rate. When this metal paste is screen-printed on a ceramic green sheet, the laminated body 103 is manufactured with the mesh density and resist thickness set to substantially the same conditions. As shown in FIG. 10, the metal layer 102 formed of this metal paste has voids 102 'formed substantially uniformly.

  In addition, when the ceramic green sheets are pressed and laminated, the metal layer 102 has a partial electrode structure, so that the pressed state differs between a portion where the metal layer 102 overlaps and a portion where the metal layer 102 does not overlap. As a result, even in the same plane of the metal layer 102, the density of the metal layer may be non-uniform. Therefore, a method of forming a recess in the ceramic sheet of the portion where the metal layer 102 is formed to make the metal filling rate uniform. Has been proposed (see, for example, Patent Document 3).

  By the way, when the multilayer piezoelectric element is used as a piezoelectric actuator, a lead wire (not shown) is connected and fixed to the external electrode 105 by soldering, and is driven by applying a predetermined potential between the external electrodes 105. In recent years, multilayer piezoelectric elements used in such applications are required to have a large displacement under a large pressure while being reduced in size. Therefore, the multilayer piezoelectric element is required to be used even under severe conditions in which a higher electric field (voltage) is applied and continuously driven for a long time.

  In order to meet the above requirement, that is, the requirement of continuous driving for a long time under high voltage and high pressure, Patent Document 4 describes an element provided with a layer in which the thickness of the piezoelectric layer 101 is changed. In other words, stress relaxation is achieved by utilizing the fact that the amount of displacement varies with other layers due to the difference in thickness.

  In the co-fired multilayer piezoelectric element, it has been attempted to form a uniform metal layer so that a voltage is uniformly applied to all piezoelectric bodies. In particular, attempts have been made to make the metal composition of the metal layer uniform in order to make the conductivity of each metal layer uniform and to make the surface area of the portion in contact with the piezoelectric body uniform.

  However, unlike ordinary multilayer electronic components such as capacitors, the multilayer piezoelectric element continuously undergoes dimensional changes when driven. Therefore, when all the piezoelectric bodies are driven in close contact with each other through the metal layer, the laminated piezoelectric element undergoes driving deformation as a unit. For this reason, the stress due to the deformation of the element concentrates on the outer peripheral portion of the central part of the element which expands when compressed and constricts when stretched. When such a laminated piezoelectric element is continuously driven for a long time under high voltage and high pressure, delamination (delamination) occurs at the interface (lamination interface) between the piezoelectric layer and the metal layer for the above reasons. It sometimes occurred. In particular, stress is concentrated on the interface between the active layer that undergoes piezoelectric displacement and the inactive layer that does not undergo piezoelectric displacement, and this interface is the origin of delamination.

  In addition, a resonance phenomenon in which the displacement behaviors of the piezoelectric layers coincide with each other may generate a beeping sound, or a harmonic signal that is an integral multiple of the driving frequency may be generated to generate a noise component.

  In addition, when a multilayer piezoelectric element that continuously undergoes dimensional changes is driven for a long time, the element temperature rises, and when the energy for this element temperature rise exceeds the heat dissipation amount, the element temperature rises at an accelerated rate. This causes a phenomenon that the amount of displacement of the piezoelectric body decreases as the temperature rises, and further, the amount of displacement of the piezoelectric body rapidly decreases due to the high temperature of the piezoelectric layer above the Curie point of the piezoelectric material. It was. Accordingly, a metal layer having a small specific resistance has been demanded in order to suppress an increase in element temperature.

  Furthermore, since the amount of displacement of the piezoelectric body has a characteristic that changes depending on the environmental temperature, when a conventional multilayer piezoelectric element is used as an actuator used for a drive element such as a fuel injection device, the element temperature increases. The amount of displacement of the piezoelectric body may change.

  As a method for improving the above problem, a method as shown in Patent Document 4 has been made, but it cannot be said that the improvement is sufficient under severe conditions such as continuous driving for a long period of time under high voltage and high pressure. Stress was concentrated on the outer periphery of the part, causing cracks or peeling, and the amount of displacement sometimes changed.

JP-A-61-133715 Japanese Utility Model Publication No. 1-130568 JP-A-10-199750 JP-A-60-86880

  An object of the present invention is to provide a laminated piezoelectric element excellent in durability that has a large amount of displacement under a high voltage and a high pressure and can suppress a change in the amount of displacement even when continuously driven for a long period of time. It is providing the injection device using this.

  As a result of intensive studies to solve the above problems, the present inventors have determined that a plurality of metal layers in the multilayer piezoelectric element have a specific metal filling rate different from the metal layers on both sides adjacent to each other in the stacking direction. In the case of containing a plurality of elements, the stress applied to the element can be dispersed, so that a large amount of displacement can be obtained, the resonance phenomenon can be suppressed, and the element is continuously driven for a long time under high voltage and high pressure. Even in this case, the present inventors have found a new fact that a change in the amount of displacement can be suppressed and delamination of the laminated portion can be suppressed, and a laminated piezoelectric element having excellent durability can be obtained. It came to complete.

That is, the multilayer piezoelectric element of the present invention has the following configuration.
(1) In a stacked piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, the plurality of metal layers are on both sides of a metal filling rate adjacent to each other in the stacking direction. A multilayer piezoelectric element comprising a plurality of low-filling metal layers lower than the metal layer.
(2) The multilayer piezoelectric element according to (1), wherein the plurality of low-filling metal layers are respectively disposed with a plurality of metal layers other than the low-filling metal layer interposed therebetween.
(3) The multilayer piezoelectric element according to (1) or (2), wherein the plurality of low-filling metal layers are regularly arranged in a stacking direction.
(4) The plurality of metal layers include a plurality of high-filling metal layers in which a filling rate of a metal constituting the metal layer is higher than metal layers on both sides adjacent to each other in the stacking direction. The multilayer piezoelectric element according to any one of the above.

(5) In the multilayer piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, the plurality of metal layers are on both sides where the filling rate of the metal constituting the metal layer is adjacent in the stacking direction. A multilayer piezoelectric element comprising a plurality of highly filled metal layers higher than the metal layer.
(6) The multilayer piezoelectric element according to (5), wherein the plurality of high-filling metal layers are respectively disposed with a plurality of metal layers other than the high-filling metal layer interposed therebetween.
(7) The multilayer piezoelectric element according to (5) or (6), wherein a plurality of the highly filled metal layers are regularly arranged in the stacking direction.
(8) The plurality of metal layers include a plurality of low-filling metal layers in which the filling rate of the metal constituting the metal layer is lower than the metal layers on both sides adjacent to each other in the stacking direction. The multilayer piezoelectric element according to any one of the above.
(9) The multilayer piezoelectric element according to (4) or (8), wherein a metal layer adjacent to the low-filling metal layer in the stacking direction is the high-filling metal layer.
(10) The multilayer piezoelectric element according to (4) or (8), wherein the metal layers on both sides adjacent to the low-filling metal layer in the stacking direction are the high-filling metal layers.

(11) The high-filling metal layer has a peak metal filling rate, and has an inclined region in which the metal filling rate gradually decreases from the high-filling metal layer to two or more metal layers in the stacking direction. (4) The laminated piezoelectric element according to any one of (10).
(12) The low-filling metal layer is composed of a plurality of partial metal layers arranged in a state of being separated from each other through a gap, as described in (1) to (4) and (8) to (10). The multilayer piezoelectric element according to any one of the above.
(13) Among the plurality of metal layers, a metal layer in which the metal filling rate is lower than the metal layers on both sides adjacent to each other in the stacking direction is a low filling metal layer, and the metal filling rate is in the stacking direction. A metal layer higher than the metal layers on both sides adjacent to each other is a highly filled metal layer, the metal filling rate in the other metal layers excluding the low filled metal layer and the highly filled metal layer is X, and in the low filled metal layer The multilayer piezoelectric element according to any one of (1) to (12), wherein a filling factor ratio (Y / X) is in a range of 0.1 to 0.9, where Y is a metal filling factor.
(14) Among the plurality of metal layers, a metal layer in which the metal filling rate is lower than the metal layers on both sides adjacent to each other in the stacking direction is a low filling metal layer, and the metal filling rate is in the stacking direction. The metal layer higher than the metal layers on both sides adjacent to each other is a highly filled metal layer, the metal filling rate in the other metal layers excluding the low filled metal layer and the highly filled metal layer is X, and in the highly filled metal layer The multilayer piezoelectric element according to any one of (1) to (13), wherein a filling factor ratio (Z / X) is in a range of 1.05 to 2, where Z is a metal filling factor.
(15) The metal layer is mainly composed of a metal selected from Group 8-11 elements of the periodic table, and the content of Group 8-10 elements of the periodic table in the metal layer is M1 (mass%), Any of the above (1) to (14) satisfying the relationship of 0 <M1 ≦ 15, 85 ≦ M2 <100, M1 + M2 = 100 when the content of the Group 11 element of the periodic table is M2 (mass%) The multilayer piezoelectric element according to claim 1.
(16) The group 8-10 elements of the periodic table in the metal layer are at least one selected from Ni, Pt, Pd, Rh, Ir, Ru, and Os, and the group 11 elements of the periodic table are Cu The laminated piezoelectric element according to (15), which is at least one selected from Ag, Au, and Ag.
(17) The multilayer piezoelectric element according to any one of (1) to (15), wherein the metal layer includes Cu as a main component.
(18) In a stacked piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, an inactive layer made of a piezoelectric material is formed at both ends in the stacking direction. The stacked piezoelectric element, wherein the metal layer adjacent to the active layer is a low-fill metal layer in which a metal filling rate in the metal layer is lower than a metal filling rate in a metal layer adjacent in the stacking direction.
(19) In a stacked piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, an inactive layer made of a piezoelectric material is formed at both ends in the stacking direction. The stacked piezoelectric element, wherein the metal layer adjacent to the active layer is a high-fill metal layer in which a metal filling rate in the metal layer is higher than a metal filling rate in a metal layer adjacent in the stacking direction.

  (20) A container having an ejection hole and the multilayer piezoelectric element according to any one of (1) to (19) housed in the container, wherein the liquid filled in the container An ejecting apparatus configured to be ejected from the ejection holes by driving a laminated piezoelectric element.

  According to the multilayer piezoelectric element of the present invention, the plurality of metal layers include a plurality of metal layers having specific metal filling ratios different from the metal layers on both sides adjacent to each other in the stacking direction. It will be placed in the element. In other words, the displacement of the piezoelectric layer around the low-filling metal layer is small, the displacement of the piezoelectric layer around the high-filling metal layer is large, and different displacement points are dispersed in the element. If the metal layers having different displacements are dispersed and arranged in the element as described above, suppression of element deformation due to stress concentration is alleviated, so that the displacement amount of the entire piezoelectric element can be increased. In addition, since stress concentration due to deformation of the piezoelectric element can be suppressed, delamination that occurs in the laminated portion can be suppressed even when the piezoelectric element is continuously driven for a long time under high voltage and high pressure. Furthermore, by arranging a plurality of predetermined metal layers, it is possible to suppress the resonance phenomenon that occurs when the displacements (dimensional changes) of the piezoelectric elements are aligned. Generation of a signal can be prevented and noise of the control signal can be suppressed.

In particular, according to the multilayer piezoelectric elements described in (4) and (8) to (11), stress due to element deformation is concentrated around the high-filling metal layer having a high metal filling rate, and the displacement is small and the metal filling rate. Since the piezoelectric layer around the low-filling metal layer having a low thickness can act as a stress relaxation layer, suppression of element deformation due to stress concentration can be further relaxed.
According to the multilayer piezoelectric element described in (15), the metal layer is mainly composed of a metal selected from Group 8 to 11 elements of the Periodic Table, and Group 8 to 10 elements of the Periodic Table in the metal layer; Since the content of the Group 11 element in the periodic table satisfies a predetermined relationship, the piezoelectric layer and the metal layer can be simultaneously fired, and as a result, the interface between the piezoelectric layer and the metal layer can be obtained. The (lamination interface) can be firmly bonded and delamination can be further suppressed. Moreover, even if the element is displaced and stress is applied to the metal layer, the metal layer itself can be expanded and contracted, so that the stress is not concentrated on one point, and the durability is excellent.
The multilayer piezoelectric element of the present invention can provide a highly reliable injection device with excellent durability because the desired displacement does not change effectively even when continuously driven.

<Laminated piezoelectric element>
Hereinafter, an embodiment of a multilayer piezoelectric element of the present invention will be described in detail with reference to the drawings. FIG. 1A is a perspective view showing a multilayer piezoelectric element of the present embodiment, and FIG. 1B is a partial perspective view showing a laminated state of a piezoelectric layer and a metal layer in FIG. It is. FIG. 2 is a partial enlarged cross-sectional view showing the multilayer structure of the multilayer piezoelectric element according to this embodiment. FIG. 3 is a partially enlarged cross-sectional view showing the highly filled metal layer according to the present embodiment. FIG. 4 is a partially enlarged cross-sectional view showing another laminated structure of the laminated piezoelectric element according to the present embodiment. FIG. 5 is a partial enlarged cross-sectional view showing another laminated structure of the laminated piezoelectric element according to the present embodiment. FIG. 6 is a schematic explanatory diagram for explaining the voids of the piezoelectric layer according to the present embodiment.

  As shown in FIG. 1, the multilayer piezoelectric element of the present embodiment includes a multilayer body 13 in which a plurality of piezoelectric layers 11 and a plurality of metal layers 12 are alternately stacked. A pair of external electrodes 15 are disposed on the side surface (one external electrode is not shown).

  As shown in FIG. 1B, the metal layer 12 is not formed on the entire main surface of the piezoelectric layer 11, but has a so-called partial electrode structure. The plurality of metal layers 12 of this partial electrode structure are arranged so as to be exposed on opposite side surfaces of the laminated body 13 every other layer. Thereby, the metal layer 12 is electrically connected to the pair of external electrodes 15 every other layer. The pair of external electrodes 15 may be formed on adjacent side surfaces.

As shown in FIG. 1A, inactive layers 14 formed of piezoelectric layers are stacked on both ends of the stacked body 13 in the stacking direction. When this multilayer piezoelectric element is used as a piezoelectric actuator, the lead wires may be connected and fixed to the pair of external electrodes 15 by soldering, and the lead wires may be connected to the external voltage supply unit. By applying a predetermined voltage between the adjacent metal layers 12 through the lead wires from the external voltage supply unit, each piezoelectric layer 11 is displaced by the inverse piezoelectric effect. This is because the metal layer 12 is formed of a metal material such as a silver-palladium alloy, which will be described later, so that when a predetermined voltage is applied to each piezoelectric body 11 through the metal layer 12, the piezoelectric body 11 is displaced by the inverse piezoelectric effect. Has the effect of causing it.
On the other hand, the inert layer 14 has only the metal layer 12 disposed on one main surface side, and the metal layer 12 is not disposed on the other main surface side. Does not occur.

  Here, as shown in FIG. 2, the plurality of metal layers 12 according to the present embodiment have a metal filling rate of the metal layer 12 higher than the metal layers (metal layers 12 a) on both sides adjacent to each other in the stacking direction. A plurality of low low filling metal layers 12b are included. Thereby, the displacement of the piezoelectric layer around the low filling metal layer 12b is small, and the displacement of the piezoelectric layer around the metal layer 12a having a larger metal filling rate than the low filling metal layer 12b is large. Therefore, since the metal layers with different displacements are distributed and arranged in the element, the displacement amount of the entire piezoelectric element can be increased, and when it is continuously driven for a long time under high voltage and high pressure. Even so, it is possible to suppress delamination that occurs in the stacked portion. Further, since the resonance phenomenon can be suppressed, it is possible to prevent the generation of a roaring sound. Furthermore, since generation of harmonic signals can be prevented, control signal noise can also be suppressed.

  A portion of the plurality of piezoelectric layers 11 that is driven and deformed is a portion sandwiched between the metal layers 12. Therefore, it is preferable to form the low filling metal layer 12b in a portion of the plurality of metal layers 12 that overlap with each other via the piezoelectric layer 11. Thereby, it is possible to reliably suppress the resonance phenomenon that occurs when the displacements (dimensional changes) of the piezoelectric elements are aligned.

  The plurality of low-filling metal layers 12b are preferably disposed with a plurality of other metal layers other than the low-filling metal layer 12b interposed therebetween. As other metal layers of this embodiment, there are a metal layer 12a shown in FIG. 2 and a high filling metal layer 12c described later shown in FIG. Here, the low filling metal layer 12b has a metal filling rate lower than other metal layers (metal layer 12a, high filling metal layer 12c). Therefore, the low filling metal layer 12b is more flexible than the other metal layers, and can be deformed and relaxed when stress is applied during driving (stress relaxation effect). That is, the low filling metal layer 12b functions as a stress relaxation layer.

  In particular, in the present embodiment, it is preferable that the plurality of low filling metal layers 12b are regularly arranged in the stacking direction. This is because it is effective to dispose the stress relaxation layer regularly in order to disperse the stress applied to the entire element. The laminated body 13 is preferably formed by laminating at least three piezoelectric layers 11 and has a portion where the low filling metal layer 12b is repeatedly arranged in a predetermined order.

  The plurality of low filling metal layers 12b are regularly arranged in the stacking direction means that the number of other metal layers (metal layer 12a, high filling metal layer 12c) existing between the low filling metal layers 12b is different. Of course, in the case of any of the low filling metal layers 12b, the layers of the other metal layers 12 existing between the low filling metal layers 12b to such an extent that the stress is almost uniformly distributed in the stacking direction. It is a concept that includes cases where numbers are approximate. Specifically, the number of other metal layers 12 existing between the low-filling metal layers 12b is within a range of ± 20% with respect to the average value of each layer number, preferably ± with respect to the average value of each layer number. It should be within the range of 10%, more preferably all are the same.

  The metal layer 12a which is the other metal layer is a metal layer whose metal filling rate is higher than that of the low filling metal layer 12b. The metal layer 12 a is a main metal layer, and the main metal layer means a metal layer having the largest number of metal layers having the same metal filling rate in the metal layer 12. The metal layer 12a, which is the main metal layer, preferably occupies the number of layers equal to or more than 1/3 of the total number of metal layers in order from the one close to the average metal filling rate of all the metal layers. This is because the function required of the main metal layer 12a functions stably as an electrode for driving the multilayer piezoelectric element. For this purpose, a voltage applied to the element is uniformly applied to each piezoelectric layer 11. This is because it is required to perform the piezoelectric displacement uniformly. Therefore, when the main metal layer 12a is 1/3 or more of the total number of metal layers in order from the one close to the average metal filling rate of all the metal layers, the voltage applied to the element is uniformly applied to each piezoelectric layer 11. Therefore, the piezoelectric layer 11 does not drive and deform non-uniformly, and the element is uniformly driven and deformed, resulting in a durable element. Furthermore, since the piezoelectric layer 11 in contact with the main metal layer 12a does not concentrate stress, the amount of displacement increases, and the piezoelectric layer 11 in contact with the low-filling metal layer 12b becomes a stress relaxation layer. While maintaining the displacement, it is possible to avoid stress concentration on the element. As a result, the displacement amount is increased and the durability is excellent.

In order to increase the response speed by aligning the phase of displacement, the main metal layer 12a is in the order of closer to the average metal filling rate of all metal layers in order of 70% or more of the total number of metal layers, preferably 80% or more, More preferably, it is 90% or more, and more preferably 90 to 99%. If it is 90% or more, the displacement phase is uniform and a higher response speed can be obtained. However, if it exceeds 99%, the phases are completely aligned, and the element emits a beat sound.
In addition, the total number of layers of the metal layer 12 is arbitrarily selected according to the use and is not particularly limited, but is usually 2 to 10,000 layers, preferably 5 to 1000 layers.

  Of the plurality of metal layers 12, the number of main metal layers 12a is preferably the largest. As a result, since the voltage applied to the element is uniformly applied to each piezoelectric layer 11, the piezoelectric layer 11 is not non-uniformly driven and deformed, and further, the phase of displacement is aligned, so that the element is uniform. It is not only a high response speed but also a durable laminated piezoelectric element due to drive deformation.

The main metal layer 12a is preferably a metal layer other than the metal layer having the highest metal filling rate and the metal layer having the lowest metal filling rate in the metal layer 12. This is because the stress of the multilayer piezoelectric element being driven is applied to the piezoelectric layer 11 in the vicinity of the metal layer 12 having the highest metal filling rate, so that the main metal layer 12a is the metal having the highest metal filling rate. If it is other than the layer, a highly durable multilayer piezoelectric element in which the piezoelectric layer 11 in contact with the metal layer 12a is firmly adhered can be obtained. Further, since the element displacement of the piezoelectric layer 11 in contact with the metal layer 12 with a low metal filling rate is weak, if the main metal layer 12a is other than the metal layer with the lowest metal filling rate, the displacement of the stacked piezoelectric element is not. It will never get smaller. That is, by making the main metal layer 12a other than the metal layer having the highest metal filling rate and the metal layer having the lowest filling rate among all the metal layers 12, driving displacement is large and durable. A multilayer piezoelectric element can be obtained.
Furthermore, since the magnitude of displacement of the piezoelectric layer 11 can be controlled by changing the metal filling rate of the metal layer 12, there is no need to change the thickness of the piezoelectric layer 11, and the mass productivity is excellent. Moreover, it is preferable that the main metal layer 12a is comprised by the substantially same metal filling rate. As a result, the displacement is further increased, responsiveness is fast, and durability is improved.

  As shown in FIG. 3, the plurality of metal layers 12 include a plurality of highly filled metal layers 12 c in which the metal filling rate of the metal layer 12 is higher than the metal layers (metal layers 12 a) on both sides adjacent to each other in the stacking direction. It is preferable to include. As shown in FIG. 6, the high filling metal layer 12c having a high metal filling rate has few defective portions not filled with metal such as voids 12c ′ in the metal layer. The piezoelectric layer 11 in contact with 12c becomes a portion having a large displacement when a voltage is applied to the element. For this reason, when the element is driven, the stress is concentrated (stress concentration effect) because the element has a large displacement. By disposing such an electrode layer in the element, the stress can be dispersed without concentrating the stress on one point of the element. Therefore, a highly reliable laminated piezoelectric element having excellent durability is obtained.

  The high filling metal layer 12c is a metal layer having a metal filling rate higher than that of the low filling metal layer 12b and the main metal layer 12a. That is, the metal filling ratios of the main metal layer 12a, the low filling metal layer 12b, and the high filling metal layer 12c are such that the high filling metal layer 12c> the main metal layer 12a> the low filling metal layer 12b. As a result, the main metal layer 12a becomes a metal layer other than the metal layer having the highest metal filling rate and the metal layer having the lowest filling rate among all the metal layers 12, so that the drive displacement is large and the durability is high. A certain laminated piezoelectric element can be obtained. In addition, the metal layers 12 having different displacements are surely arranged in the element. That is, the displacement of the piezoelectric layer 11 around the low filling metal layer 12b is small, and the displacement of the piezoelectric layer 11 around the high filling metal layer 12c is large. As a result, the effect of disposing metal layers having different displacements in the element can be exhibited more efficiently.

  Specifically, the metal filling rate in other metal layers (that is, the main metal layer 12a) excluding the low filling metal layer 12b and the high filling metal layer 12c is X, and the metal filling rate in the low filling metal layer 12b is Y. , The ratio (Y / X) of the filling rate should be in the range of 0.1 to 0.9, preferably 0.3 to 0.9, more preferably 0.5 to 0.8. Thereby, the stress relaxation effect of the low filling metal layer 12b occurs and the element shape is maintained. In particular, when the ratio (Y / X) is 0.3 to 0.9, the piezoelectric layer 11 adjacent to the low filling metal layer 12b is also driven to be displaced, so that the displacement of the element is large and the durability is high. A piezoelectric element can be obtained. Furthermore, when the ratio (Y / X) is 0.5 to 0.8, the displacement of the element is larger and a laminated piezoelectric element having higher durability can be obtained. The specific values of X and Y may be arbitrarily selected according to the composition of the metal layer 12 and the like, and are not particularly limited, but usually X is 45 to 90%, preferably 55 to 85%, More preferably, it is 60 to 80%, Y is 3 to 60%, preferably 20 to 60%, more preferably 30 to 50%, and X and Y are within this range, and the ratio (Y / X) It is preferable to satisfy.

  On the other hand, when the ratio (Y / X) is smaller than 0.1, the piezoelectric layer 11 and the metal layer are difficult to adhere to each other, so that there is a possibility that delamination occurs in the laminated body, which is larger than 0.9. Then, the stress relaxation effect of the low filling metal layer 12b may be lowered, and a portion where stress is concentrated at one point of the device appears, which may reduce the durability of the device.

  Further, when the metal filling rate in other metal layers (that is, the main metal layer 12a) excluding the low filling metal layer 12b and the high filling metal layer 12c is X, and the metal filling rate in the high filling metal layer 12c is Z. The ratio of packing ratio (Z / X) is in the range of 1.05 to 2, preferably 1.05 to 1.5, more preferably 1.1 to 1.2. Thereby, the stress concentration effect of the highly filled metal layer 12c is generated and the element shape is maintained. In particular, when the ratio (Z / X) is 1.05 to 1.5, the piezoelectric layer 11 adjacent to the highly filled metal layer 12c and the piezoelectric layer 11 adjacent to the main metal layer 12a are also displaced in the same manner. Since it is driven, it is possible to obtain a highly durable stacked piezoelectric element in which the displacement of the element is largely uniform. In addition, when the ratio (Z / X) is 1.1 to 1.2, it is possible to obtain a multilayer piezoelectric element having a greater element displacement and higher durability. The specific values of X and Z may be arbitrarily selected depending on the composition of the metal layer 12 and the like as in X and Y in the ratio (Y / X), and are not particularly limited. , X is 45 to 90%, preferably 55 to 85%, more preferably 60 to 80%, and Z is 60 to 100%, preferably 70 to 100%, more preferably 72 to 95%.

  On the other hand, when the ratio (Z / X) is greater than 2, the stress concentrates only on the highly filled metal layer 12c, and the interface between the highly filled metal layer 12c and the piezoelectric layer 11 is peeled off. Lamination may occur, and if it is smaller than 1.05, the stress concentration effect of the highly-filled metal layer 12c may be reduced, and a spot where stress is concentrated at one point of the element appears, and the durability of the element decreases. There is a fear.

  The filling rate of the metal constituting the metal layer 12 is a value obtained by measuring the laminated piezoelectric element on a plane cut in the laminating direction. Specifically, when the metal layer 12 is observed on the cut surface with a scanning electron microscope (SEM), a metal microscope, or the like, the metal layer 12 includes not only a metal component but also elements other than metal such as a void and a ceramic component. I can see that Therefore, in the cross section of an arbitrary metal layer, the area of the part composed only of the metal is measured, and the total area of the part composed only of the metal is divided by the total area of the metal layer. The filling rate. By measuring the metal filling rate for each of the metal layer 12a, the low filling metal layer 12b, and the high filling metal layer 12c, each layer can be distinguished.

  In the present embodiment, as shown in FIG. 4, at least a high-filling metal layer 12c having a metal filling rate higher than that of the main metal layer 12a and a low-filling metal layer 12b having a metal filling rate lower than that of the main metal layer 12a are at least It is preferable that the piezoelectric layers 11 are disposed so as to face each other with the piezoelectric layer 11 therebetween. As a result, the stress during driving of the element is concentrated on the highly filled metal layer 12c having a high metal filling rate to disperse the stress applied to the device, and further, the metal filling rate that becomes a stress relaxation layer next to the metal layer collecting the stress. By disposing the low filling metal layer 12b having a low thickness, the stress applied to the element can be efficiently dispersed and relaxed.

  In particular, as shown in FIG. 5, the metal layers on both sides adjacent to the low filling metal layer 12b in the stacking direction are preferably high filling metal layers 12c. As a result, the stress during driving of the element is concentrated on the high-filling metal layer 12c having a high metal filling ratio to disperse the stress applied to the element, and the metal filling ratio that becomes a stress relaxation layer next to the metal layer collecting the stress is low. By disposing the low filling metal layer 12b, the stress applied to the element can be dispersed and relaxed. Further, when the low filling metal layer 12b, which is a stress relaxation layer, is sandwiched between the high filling metal layer 12c, which is a layer for collecting stress, the stress is confined in the low filling metal layer 12b, and the stress of the entire device is dispersed and relaxed. it can. As a result, when the element is used in a piezoelectric actuator, a highly reliable piezoelectric actuator having excellent durability can be provided. In addition, since the one where the number of layers of the low filling metal layer 12b pinched is small can show | play the effect of confining stress more, 1 layer is the optimal number of the layers.

  In addition, the low-fill metal layer 12b, the high-fill metal layer 12c, and the main metal layer 12a are arranged in this order in the stacking direction of the multilayer body 13 via the piezoelectric layer 11, and the main metal layer 12a is filled with metal. It is preferable that the layers are stacked in order of increasing rate. Thereby, the stress applied to the element is concentrated by concentrating the stress during driving of the element on the high filling metal layer 12c, and the low filling metal layer 12b serving as a stress relaxation layer is formed next to the metal layer collecting the stress. By disposing, not only can the stress applied to the element be dispersed and relaxed, but the main metal layer 12a is arranged in descending order of the metal filling rate to gradually disperse the stress collected in the highly filled metal layer 12c. In addition, since the displacement amount of the adjacent piezoelectric layer 11 can be increased by increasing the metal filling rate, a highly reliable multilayer piezoelectric element having a large displacement and excellent durability can be obtained. Can do.

  The high filling metal layer 12c has a peak of metal filling rate, and the inclined region where the metal filling rate gradually decreases from the high filling metal layer 12c to two or more, preferably 2 to 5 or more metal layers in the stacking direction. It is preferable to have. As a result, the stress during driving of the element is concentrated on the highly filled metal layer 12c having a high metal filling rate. However, if a predetermined inclined region is provided, the stress collected on the highly filled metal layer 12c can be gradually dispersed. it can.

  As shown in FIG. 6, the metal layer 12 preferably has predetermined voids 12 a ′, 12 b ′, and 12 c ′. This is because when the metal layer 12 contains an insulating material other than a metal component, when the element is driven, a portion where voltage cannot be applied to the piezoelectric layer 11 is generated. This is because the stress at the time may concentrate on the metal layer 12 and become a starting point of fracture. If the metal layer 12 has a predetermined void (void), when stress is applied to the metal portion, the metal deforms and the stress is dispersed and relaxed by the presence of the void (void) portion. it can. In addition, when the piezoelectric layer 11 in contact with the metal layer 12 is piezoelectrically displaced, there is a void portion, so that the piezoelectric layer 11 is partially clamped and is clamped over the entire surface. As a result, the force with which the piezoelectric layer 11 is constrained becomes smaller and is easily displaced, and the amount of displacement can be increased. As a result, it is possible to obtain a multilayer piezoelectric element having a larger element displacement and higher durability.

  In particular, a void 12a ′ is provided in the main metal layer 12a, and the area ratio (void ratio) occupied by the void 12a ′ with respect to the total cross-sectional area in the cross section of the metal layer 12a is 5 to 70%, preferably 7 It is good that it is -70%, More preferably, it is 10-60%. Thereby, since the amount of displacement becomes large, it is possible to obtain a laminated piezoelectric element having an excellent amount of displacement. In particular, when the void ratio is 7 to 70% or 10 to 60%, the piezoelectric layer 11 can be deformed more smoothly and the metal layer 12 has sufficient conductivity. The amount of displacement of can be increased.

  On the other hand, if the void ratio is less than 5%, the piezoelectric layer 11 is constrained by the metal layer 12 when deformed by applying a voltage, and the deformation of the piezoelectric layer 11 is suppressed, and the deformation of the multilayer piezoelectric element is suppressed. Since the amount is reduced and the internal stress generated is also increased, the durability may be adversely affected. Further, if the void ratio is larger than 70%, an extremely thin portion is generated in the electrode portion, so that the strength of the metal layer 12 itself is lowered, the metal layer 12 is likely to be cracked, and there is a possibility of causing disconnection or the like. Therefore, it is not preferable.

  The ratio (void ratio) of the void to the area of the metal layer 12 is a value obtained by measuring the laminated piezoelectric element on a plane cut in the laminating direction. Specifically, on the cut surface, the area of voids (voids) existing in the metal layer 12 is measured, and the value obtained by dividing the sum of the void areas by the area of the metal layer 12 is multiplied by 100. is there.

The metal layer 12 having voids is mainly composed of metal and voids. When the metal layer 12 is configured in this way, both the metal and the void can be deformed by stress, so that a laminated piezoelectric element with higher durability can be obtained.
In particular, when the low-filling metal layer 12b is mainly composed of a metal and a void, it is possible to obtain a laminated piezoelectric element with higher durability. That is, as shown in FIG. 6, the low filling metal layer 12b is preferably composed of a plurality of partial metal layers arranged in a state of being separated from each other via a void 12b ′. As a result, when the piezoelectric layer 11 in contact with the low filling metal layer 12b is in contact with an unfilled portion of the metal layer such as a void 12b 'in the metal layer, the piezoelectric material at that portion has a voltage applied to the element. Even if it is applied, it is not displaced, and when stress is applied during driving, it can be deformed to relieve the stress (stress relaxation effect). That is, the low filling metal layer 12b formed of the partial metal layer functions as a stress relaxation layer. Therefore, the piezoelectric layer 11 in contact with the metal layer has a small driving displacement, and the stress of the element can be avoided from being concentrated on one point. As a result, a highly reliable multilayer piezoelectric element having excellent durability can be obtained.

  Specifically, the area ratio (void ratio) occupied by the voids 12b 'with respect to the total cross-sectional area in the cross section of the low filling metal layer 12b is preferably 20 to 90%. Thereby, the displacement amount is further increased, and a laminated piezoelectric element having an excellent displacement amount can be obtained.

  The metal layer 12 preferably contains a metal selected from Group 8 to 11 elements of the periodic table as a main component. This is because the above metal composition has high heat resistance, so that the piezoelectric layer 11 and the metal layer 12 having a high firing temperature can be fired simultaneously. Therefore, since the sintering temperature of the external electrode 15 can be made lower than the sintering temperature of the piezoelectric layer 11, severe interdiffusion between the piezoelectric layer 11 and the external electrode 15 can be suppressed.

  Further, when the content of the Group 8-10 elements of the periodic table in the metal layer 12 is M1 (mass%) and the content of the Group 11 elements of the Periodic Table is M2 (mass%), 0 <M1 It is preferable that a metal satisfying the relationship of ≦ 15, 85 ≦ M2 <100, M1 + M2 = 100 is a main component. This is because when M1, which is the content of Group 8 to 10 elements of the periodic table, exceeds 15 mass%, the specific resistance increases, and when the multilayer piezoelectric element is continuously driven, the metal layer 12 generates heat. This is because the generated heat acts on the temperature-dependent piezoelectric body layer 11 to reduce the displacement characteristics, so that the displacement amount of the multilayer piezoelectric element may be small. Further, when the external electrode 15 is formed, the external electrode 15 and the metal layer 12 are mutually diffused and joined. However, when M1 exceeds 15% by mass, the metal layer component is diffused in the external electrode 15. This is because the durability of the multilayer piezoelectric element that changes its dimensions during driving may decrease due to the increased hardness.

  In particular, in order to suppress ion migration of the group 11 element in the metal layer 12 to the piezoelectric layer 11, M1 is preferably set to 0.001 mass% or more and 15 mass% or less. In order to improve the durability of the multilayer piezoelectric element, it is preferable that M1 is 0.1% by mass or more and 10% by mass or less. When heat resistance is excellent and higher durability is required, M1 is preferably 0.5% by mass or more and 9.5% by mass or less, and when higher durability is required, M1 is 2% by mass. % Or more and 8% by mass or less is preferable.

  On the other hand, when M2 which is the content of the group 11 element is less than 85% by mass, the specific resistance of the metal layer 12 increases, and when the multilayer piezoelectric element is continuously driven, the metal layer 12 may generate heat. This is not preferable. In particular, in order to suppress ion migration of the group 11 element in the metal layer 12 to the piezoelectric layer 11, it is preferable to set M2 to 85 mass% or more and 99.999 mass% or less. In order to improve the durability of the multilayer piezoelectric element, M2 is preferably 90% by mass or more and 99.9% by mass or less. When higher durability is required, M2 is preferably 90.5% by mass or more and 99.5% by mass or less, and when higher durability is required, M2 is 92% by mass or more and 98% by mass. % Or less is preferable.

  In particular, when the low-filling metal layer 12b relieves stress, relieving the applied stress means that the applied kinetic energy is converted into thermal energy to release the stress, and the stress relieving portion is heated. Will have. When the temperature of the piezoelectric body rises, the piezoelectric displacement force decreases, and once the temperature rises to the Curie point, even if cooled, the polarization effect is lost and the piezoelectric displacement force is greatly impaired. Therefore, if the low filling metal layer 12b can serve as a heat sink, heat can be dissipated from the stress relaxation portion to the outside of the element.

  Here, by using the metal of the composition of the present invention, the heat dissipation effect is increased, and the stress relaxation effect can be maintained with high durability for a long period of time. In particular, a composition containing high heat conduction silver in a high concentration has the largest heat dissipation effect, and even when oxidized, the heat conductivity does not decline and the electrical conduction characteristics do not decline. An extremely high durability stress relaxation layer can be obtained.

  M1 of group 8-10 elements and M2 of group 11 elements indicating mass% of the metal component in the metal layer 12 can be specified by an analysis method such as an EPMA (Electron Probe Micro Analysis) method.

  The metal component in the metal layer 12 includes at least one group 8-10 element metal selected from Ni, Pt, Pd, Rh, Ir, Ru, Os, and the group 11 element metal Cu, Ag, It is preferably at least one selected from Au. These exemplified metals have a metal composition excellent in mass productivity in recent alloy powder synthesis techniques.

  Of the metal components in the metal layer 12 exemplified above, the group 8-10 element metal is at least one selected from Pt and Pd, and the group 11 element metal is selected from Ag and Au. The above is preferable. Thereby, there is a possibility that the metal layer 12 having excellent heat resistance and small specific resistance can be formed.

  In particular, as for the metal component in the metal layer 12, it is preferable that the metal of a group 8-10 element is Ni. Thereby, the metal layer 12 excellent in heat resistance may be formed. Moreover, it is preferable that the group 11 element metal is Cu. Thereby, there is a possibility that the metal layer 12 having a low hardness and excellent thermal conductivity can be formed.

In particular, Cu has not only high heat conduction characteristics, but when stress is applied from one direction, the crystal orientation is oriented in one direction to which stress is applied, so there is a strong stress relaxation effect that does not break Is generated. Furthermore, when an element is produced by simultaneous firing, a coating layer of highly corrosive CuO is formed on the Cu surface, so that it can be made a highly durable element (in the case of ordinary Cu metal, the surface gradually becomes a Cu ₂ O film) And then combines with moisture in the air to form patina and corrode).

  Moreover, it is preferable that the metal layer 12 is an alloy which has the said metal as a main component. As the alloy, for example, an alloy that is solid-solved such as a silver-palladium alloy (silver 70 to 99.999 mass% -palladium 0.001 to 30 mass%) can control the firing temperature at an arbitrary composition ratio. preferable. Moreover, it is preferable to add an oxide, nitride, or carbide to the metal layer 12 together with the above-described metal composition. Thereby, the strength of the metal layer 12 is increased, and the durability of the multilayer piezoelectric element is improved. In particular, an oxide is more preferable because it interdiffuses with the piezoelectric layer 11 and increases the adhesion strength between the metal layer 12 and the piezoelectric layer 11.

The oxide preferably has a perovskite oxide composed of PbZrO ₃ —PbTiO ₃ as a main component because of its high adhesion strength to the piezoelectric layer 11. The content of the added oxide or the like can be calculated from the area ratio of the composition in the metal layer in the cross-sectional SEM image of the multilayer piezoelectric element.

  It is preferable that the inorganic composition (that is, oxide, nitride, or carbide added together with the metal composition) is 50% by volume or less based on the metal. As a result, the bonding strength between the metal layer 12 and the piezoelectric layer 11 can be made smaller than the strength of the piezoelectric layer 11, and more preferably 30% by volume or less, thereby improving the durability of the multilayer piezoelectric element. Can do.

  The thicknesses of the metal layer 12a, the low filling metal layer 12b, and the high filling metal layer 12c constituting the metal layer 12 may be arbitrarily selected depending on the composition of the metal layer 12, and are not particularly limited. Usually, the thickness of the metal layer 12a is 0.1 to 100 μm, preferably about 0.5 to 10 μm, more preferably about 1 to 5 μm, and the thickness of the low filling metal layer 12b is 0.05 to 100 μm, preferably 0.00. About 1 to 10 μm, more preferably about 0.5 to 5 μm, and the thickness of the highly filled metal layer 12 c is about 0.1 to 200 μm, preferably about 0.5 to 15 μm, more preferably about 1 to 10 μm. .

The piezoelectric layer 11 preferably contains a perovskite oxide as a main component. This is because when the piezoelectric layer 11 is formed of a perovskite-type piezoelectric ceramic material typified by, for example, barium titanate (BaTiO ₃ ) or the like, the piezoelectric strain constant d ₃₃ indicating the piezoelectric characteristics is high. Further, the piezoelectric layer 11 and the metal layer 12 can be fired simultaneously. The piezoelectric layer 11 described above preferably contains a perovskite oxide composed of PbZrO ₃ —PbTiO ₃ having a relatively high piezoelectric strain constant d ₃₃ as a main component.

  In addition, the metal layer 12 is preferably exposed on the side surface of the stacked body 13. This is because, in a portion where the metal layer 12 is not exposed on the side surface of the element, it cannot be displaced at the time of driving. Therefore, a region that is displaced at the time of driving is confined inside the element. For this reason, the stress at the time of displacement tends to concentrate on the boundary, which causes a problem in durability, which is not preferable.

  The laminated body 13 is preferably a polygonal columnar body. This is because if the laminated body 13 is a cylindrical body, the center axis will be shaken unless it is made into a perfect circle. Therefore, a highly accurate circle must be created and stacked. This is because it becomes difficult to use. Further, even if the outer periphery is polished and formed into a cylindrical shape after laminating a substantially circular laminate or after firing, it is difficult to align the central axis of the metal layer 12 with high accuracy. On the other hand, if the laminated body 13 is a polygonal columnar body, the metal layer 12 can be formed on the piezoelectric layer 11 that has determined the reference line, and can be further laminated along the reference line. Since the central axis, which is the drive axis, can be formed using a mass production method, a highly durable element can be obtained.

  Further, as described above, the metal layers 12 whose ends are exposed on the side surfaces of the multilayer piezoelectric element of the present embodiment and the metal layers 12 whose ends are not exposed are alternately configured, but the ends are exposed. It is preferable that a groove is formed in the piezoelectric layer 11 between the metal layer 12 and the external electrode 15 that is not, and an insulator having a Young's modulus lower than that of the piezoelectric layer 11 is formed in the groove. As a result, the stress caused by the displacement during driving can be relieved, so that the heat generation of the metal layer 12 can be suppressed even if the multilayer piezoelectric element is continuously driven.

  Next, another embodiment of the multilayer piezoelectric element of the present invention will be described in detail with reference to the drawings. FIG. 7 is a partial enlarged cross-sectional view showing the multilayer structure of the multilayer piezoelectric element of the present embodiment. In FIG. 7, the same or equivalent parts as those in FIGS. 1 to 6 described above are denoted by the same reference numerals and description thereof is omitted. As shown in FIG. 7, the multilayer piezoelectric element of this embodiment is a multilayer piezoelectric element in which a plurality of piezoelectric layers 11 and a plurality of metal layers 12 are alternately stacked, as in the embodiment described above. It is.

  Here, the plurality of metal layers 12 include a plurality of highly filled metal layers 12c in which the filling rate of the metal constituting the metal layer 12 is higher than the metal layers (metal layers 12a) on both sides adjacent to each other in the stacking direction. Even in such a configuration, the displacement of the piezoelectric layer 11 around the high filling metal layer 12c is large, and the displacement of the piezoelectric layer 11 around the main metal layer 12a having a smaller metal filling rate than the high filling metal layer 12c. Since the metal layer having a different displacement is arranged in the element, the same effects as those of the embodiment described above can be obtained.

The plurality of high-filling metal layers 12c according to the present embodiment is similar to the above-described embodiments in that other metal layers (that is, the main metal layer 12a and the low-filling metal layer 12b) other than the high-filling metal layer 12c are used. It is preferable that each of the layers is disposed. Moreover, it is preferable that the plurality of highly filled metal layers 12c are regularly arranged in the stacking direction. Furthermore, it is preferable that the plurality of metal layers 12 include a plurality of low-filling metal layers 12b in which the filling rate of the metal constituting the metal layer 12 is lower than the metal layers on both sides adjacent to each other in the stacking direction.
Since the configuration other than the above is the same as that of the embodiment described above, the description thereof is omitted.

  Next, an embodiment according to still another multilayer piezoelectric element of the present invention will be described. The laminated piezoelectric element according to this embodiment is a laminated piezoelectric element in which a plurality of piezoelectric layers 11 and a plurality of metal layers 12 are alternately laminated. The metal layer 11 adjacent to the inactive layer 14 is formed of a low-filling metal in which the metal filling rate in the metal layer 11 is lower than the metal filling rate in the metal layer 11 adjacent in the stacking direction. It is a layer (low filling metal layer 12b). Thereby, it is possible to avoid the stress of the element from being concentrated on one point. The reason for this is presumed as follows.

  That is, even when a voltage is applied, the inactive layer that is not sandwiched between the electrodes does not undergo drive deformation, and therefore, the drive deformation is not caused by the metal layer 12 adjacent to the inactive layer 14. Since the portions are in contact with each other, stress concentrates on this boundary portion. At this time, if the metal layer 12 has the same metal filling rate, the stress is concentrated at this boundary portion. Therefore, when the laminated piezoelectric element is continuously operated for a long time under high voltage and high pressure, the stress is reduced. There was a risk of lamination.

  Therefore, when the metal filling rate in the metal layer 11 adjacent to the inert layer 14 is lower than the metal filling rate in the metal layer 11 adjacent in the stacking direction, the low filling metal layer 12b is more flexible than the other metal layers. Therefore, when the element is driven and the piezoelectric layer 11 is deformed, the low filling metal layer 12b itself is deformed to relieve stress (stress relaxation effect). Furthermore, since the inactive layer 14 in contact with the low filling metal layer 12b is formed of a piezoelectric material, it can be deformed by applying stress to relieve the stress. That is, the low filling metal layer 12b and the inert layer 14 produce a synergistic effect of the stress relaxation effect. In addition, since the low filling metal layer 12b itself deforms, the piezoelectric layer 11 sandwiched between the metal layer 12 adjacent to the low filling metal layer 12b coexists with driving deformation due to voltage application and deformation due to stress application. Since the low filling metal layer 12b itself is deformed to relieve stress, deformation due to stress application becomes dominant and deforms for stress relaxation. Therefore, the drive displacement is reduced, and the stress of the element can be avoided from being concentrated on one point.

  Further, the metal layer adjacent to the low filling metal layer 12b in the stacking direction is preferably the high filling metal layer 12c. As a result, the stress during driving of the element is concentrated on the high filling metal layer 12c, the stress applied to the element is dispersed at the end, and the low filling metal layer 12b serving as a stress relaxation layer is disposed next to the metal layer collecting the stress. By doing so, the stress applied to the element can be dispersed and relaxed at the end. Further, when the low-filling metal layer 12b as the stress relaxation layer is sandwiched between the high-filling metal layer 12c and the inert layer 14 that collect stress, the stress is confined in the low-filling metal layer 12b, and the stress of the entire device Can be dispersed and relaxed. As a result, when the element is used in a piezoelectric actuator, a highly reliable piezoelectric actuator having excellent durability can be provided.

  In particular, conventionally, when forming a stacked piezoelectric element having a lower number of stacks, for example, less than 50 layers, the metal filling rate of the piezoelectric layer 11 in the vicinity of the inactive layer 14 approaches that of the inactive layer 14. The amount of deformation was increased, and the amount of deformation was suppressed to prevent the stress from concentrating on the boundary portion. For this reason, in order to form the piezoelectric layer 11, piezoelectric sheets having several kinds of metal filling ratios were prepared and laminated, which was expensive, but the metal layer adjacent to the inert layer 14 11 is a low-fill metal layer (low-fill metal layer 12b) having a lower metal filling rate than the metal filling rate in the metal layer 11 adjacent in the stacking direction. A piezoelectric element can be used. Further, the metal filling rate in the metal layer 11 adjacent to the inert layers 14 at both ends is a low filling metal layer (low filling metal layer 12b) lower than the metal filling rate in the metal layer 11 adjacent in the stacking direction. As a result, it is possible to obtain a multi-layer piezoelectric element having a low cost and high durability.

On the other hand, the multilayer piezoelectric element having a large number of layers further includes a plurality of low-filling metal layers 12b having a lower metal filling rate than the metal layers (metal layers 12a) on both sides adjacent to each other in the stacking direction. Since the piezoelectric layer around the filling metal layer 12b can absorb the local stress of the piezoelectric displacement by the deformation of the low filling metal layer easily, the displacement of the surrounding piezoelectric layer becomes small. The metal layers having different sizes are dispersed and arranged in the element. For this reason, even when it is continuously driven for a long time under a high voltage and a high pressure, suppression of element deformation due to stress concentration is alleviated, so that delamination occurring in the laminated portion can be suppressed. Further, since the resonance phenomenon can be suppressed, it is possible to prevent the generation of a roaring sound. Furthermore, since the generation of harmonic signals can be prevented, the noise of the control signal can also be suppressed, and when used as a piezoelectric actuator, malfunction can be prevented.
Since the configuration other than the above is the same as that of the embodiment described above, the description thereof is omitted.

  Next, an embodiment according to still another multilayer piezoelectric element of the present invention will be described. The laminated piezoelectric element according to this embodiment is a laminated piezoelectric element in which a plurality of piezoelectric layers 11 and a plurality of metal layers 12 are alternately laminated. The layer 14 is formed, and the metal layer 11 adjacent to the inactive layer 14 is a highly filled metal in which the metal filling rate in the metal layer 11 is higher than the metal filling rate in the metal layer 11 adjacent in the stacking direction. This is a layer (highly filled metal layer 12c). As a result, a highly reliable laminated piezoelectric element having excellent durability is obtained. The reason for this is presumed as follows.

  That is, even when a voltage is applied, the inactive layer that is not sandwiched between the electrodes does not undergo drive deformation, and therefore, the drive deformation is not caused by the metal layer 12 adjacent to the inactive layer 14. Since the portions are in contact with each other, stress concentrates on this boundary portion. At this time, if the metal layer 12 has the same metal filling rate, the stress is concentrated at this boundary portion. Therefore, when the laminated piezoelectric element is continuously operated for a long time under high voltage and high pressure, the stress is reduced. There was a risk of lamination.

  Therefore, when the metal filling rate in the metal layer 11 adjacent to the inert layer 14 is higher than the metal filling rate in the metal layer 11 adjacent in the stacking direction, when the piezoelectric layer 11 is deformed by driving the element. The high-filling metal layer 12c has a strong force to restrain both the piezoelectric layer 11 in contact with the high-filling metal layer 12c and the inactive layer 14 in contact with the high-filling metal layer 12c. Since the stress is repelled without deformation of the high-filling metal layer, the piezoelectric layer 11 in contact with the highly-filled metal layer 12c performs a stronger displacement, so that the amount of piezoelectric displacement of the element can be increased.

  Furthermore, when the element is driven, the highly filled metal layer 12c itself is not deformed for the above-described reason, so that stress applied to the entire element is concentrated in the vicinity of the highly filled metal layer 12c (stress concentration effect). Therefore, when such a highly filled metal layer 12c is disposed at the end of the element driving portion, the stress can be distributed to the end of the element without concentration of stress on the driving portion of the element, and the durability is excellent. It becomes a highly reliable multilayer piezoelectric element.

In particular, conventionally, when forming a stacked piezoelectric element having a lower number of stacks, for example, less than 50 layers, the metal filling rate of the piezoelectric layer 11 in the vicinity of the inactive layer 14 approaches that of the inactive layer 14. The amount of deformation was increased, and the amount of deformation was suppressed to prevent the stress from concentrating on the boundary portion. For this reason, in order to form the piezoelectric layer 11, several types of piezoelectric sheets were prepared and laminated, which resulted in a high cost, but the metal layer 11 adjacent to the inert layer 14 was made of metal. By using only a filling rate as a high filling metal layer (high filling metal layer 12c) higher than the filling rate of the metal in the metal layer 11 adjacent in the lamination direction, it is a low cost, high driving force and high durability laminated type. A piezoelectric element can be used. Furthermore, the metal filling rate in the metal layer 11 adjacent to the inert layer 14 at both ends is a low filling metal layer (high filling metal layer 12b) lower than the metal filling rate in the metal layer 11 adjacent in the stacking direction. As a result, it is possible to obtain a multi-layer piezoelectric element having a low cost and high durability.
Since the configuration other than the above is the same as that of the embodiment described above, the description thereof is omitted.

<Manufacturing method>
Next, a manufacturing method of the multilayer piezoelectric element according to the embodiment described above will be described.
First, a calcined powder of a perovskite oxide piezoelectric ceramic made of PbZrO ₃ —PbTiO ₃ or the like, a binder made of an organic polymer such as acrylic or butyral, DBP (dibutyl phthalate), DOP (diethyl phthalate) And a plasticizer such as) are mixed to produce a slurry, and a plurality of ceramic green sheets to be the piezoelectric layer 11 are produced from the slurry by a tape molding method such as a doctor blade method or a calender roll method.

  Next, for example, an organic substance that is bonded and fixed when the acrylic beads are dried and volatilized when fired is added to the metal powder constituting the metal layer 12 such as a silver-palladium alloy, and a binder and a plasticizer are added and mixed. A conductive paste is prepared, and this is printed on the upper surface of each green sheet to a thickness of 1 to 40 μm by screen printing or the like.

  Here, the metal content of the metal layer 12 can be changed by changing the ratio of the organic substance to the metal powder. That is, since the organic material volatilizes during firing, voids are formed in the metal layer 12. Therefore, when the organic matter is small, the metal filling rate is high, and when the organic matter is large, the metal content is low. As content of the organic substance in each concrete metal layer 12a-12c concrete, the metal layer 12a is 0.1-10 mass parts with respect to 100 mass parts of metal powder, Preferably it is 1-5 mass parts, Low filling metal layer 12b is 0.1 to 50 parts by mass, preferably 2 to 10 parts by mass with respect to 100 parts by mass of the metal powder, and the highly filled metal layer 12c is 0 to 5 parts by mass with respect to 100 parts by mass of the metal powder, preferably It is good that it is 0-2 mass parts.

  The organic material is not particularly limited as long as it exhibits a good thermal decomposition behavior at the time of firing, but in addition to the acrylic beads exemplified above, resin beads such as acrylic and α-methylstyrene are available. preferable. The acrylic beads and the resin beads may have a hollow structure. The average particle diameter of acrylic beads and resin beads is preferably about 0.01 to 3 μm.

  Moreover, an organic substance such as acrylic beads is added and mixed with a binder and a plasticizer to prepare an acrylic bead paste, and a binder and a plasticizer are added and mixed into the metal powder constituting the metal layer 12 such as silver-palladium. A conductive paste may be prepared, and acrylic bead paste and conductive paste may be laminated and printed on the upper surface of each green sheet by screen printing or the like. As a result, it is possible to perform printing with excellent mass productivity.

  Then, after laminating a plurality of green sheets printed with conductive paste and removing the binder at a predetermined temperature on the laminate with the weight placed on it, without placing the weight on the metal layer so that a void is formed. The laminated body 13 is produced by baking. The firing temperature is 900 to 1200 ° C, preferably 900 to 1000 ° C. This is because when the firing temperature is 900 ° C. or lower, the firing temperature is low, and firing is insufficient, making it difficult to produce a dense piezoelectric body. Further, when the firing temperature exceeds 1200 ° C., the bonding strength between the metal layer and the piezoelectric body increases.

  At this time, when adding the metal powder constituting the metal layer 12 such as silver-palladium to the green sheet constituting the inert layer 14 or laminating the green sheet of the portion of the inert layer 14, the silver − By printing a slurry made of a metal powder such as palladium, a metal powder 12 and an inorganic compound, a binder and a plasticizer on a green sheet, the shrinkage behavior and shrinkage rate of the inert layer 14 and other parts during sintering Can be made to coincide with each other, so that a dense laminate 13 can be formed.

  In addition, the laminated body 13 is not limited to what is produced by the said manufacturing method, If any laminated body 13 which laminates | stacks the several piezoelectric body layer 11 and the some metal layer 12 alternately can be produced, It may be formed by such a manufacturing method.

  After that, the metal layer 12 whose end is exposed and the metal layer 12 whose end is not exposed are alternately formed on the side surface of the multilayer piezoelectric element, and the metal layer 12 whose end is not exposed is formed between the external electrode 15 and the metal layer 12. A groove is formed in the piezoelectric portion, and an insulator such as resin or rubber having a Young's modulus lower than that of the piezoelectric layer 11 is formed in the groove. Here, the groove is formed on the side surface of the laminate 13 by an internal dicing device or the like.

Next, a binder is added to the glass powder to produce a silver glass conductive paste, which is formed into a sheet and dried (the solvent is scattered), and the raw density of the sheet is controlled to 6 to 9 g / cm ³ . To do. Next, this sheet is transferred to the external electrode formation surface of the columnar laminate 13, the temperature higher than the softening point of the glass, the temperature below the melting point of silver (965 ° C.), and the firing temperature (° C. of the laminate 13 ) At a temperature of 4/5 or less, the binder component in the sheet produced using the silver glass conductive paste is scattered and disappeared, and the external electrode 15 made of a porous conductor having a three-dimensional network structure. Can be formed.

  At this time, the paste constituting the external electrode 15 may be baked after being laminated on the multilayer sheet, or may be baked after being laminated one by one. Baking is better for mass production. And when changing the glass component for each layer, it is sufficient to use a glass component whose amount is changed for each sheet. However, when it is desired to form a very thin glass-rich layer on the surface in contact with the piezoelectric layer 11 most. In other words, a multilayer sheet may be laminated on the laminate 13 after printing a glass-rich paste by a method such as screen printing. At this time, a sheet of 5 μm or less may be used instead of printing.

  The baking temperature of the silver glass conductive paste effectively forms a neck portion, diffuses and joins the silver in the silver glass conductive paste and the metal layer 12, and effectively creates voids in the external electrode 15. The temperature is preferably 500 to 800 ° C. from the viewpoint that the external electrode 15 and the side surface of the columnar laminated body 13 are partially joined. The softening point of the glass component in the silver glass conductive paste is preferably 500 to 800 ° C.

  On the other hand, when the baking temperature is higher than 800 ° C., the sintering of the silver powder of the silver glass conductive paste proceeds excessively, and a porous conductor having an effective three-dimensional network structure cannot be formed. There is a possibility that the electrode 15 becomes too dense, and as a result, the Young's modulus of the external electrode 15 becomes too high to absorb the stress at the time of driving sufficiently and the external electrode 15 is disconnected. Preferably, baking should be performed at a temperature within 1.2 times the softening point of the glass. Further, when the baking temperature is lower than 500 ° C., since the diffusion bonding is not sufficiently performed between the end portion of the metal layer 12 and the external electrode 15, the neck portion is not formed, and the metal layer 12 and the external portion are driven during driving. There is a possibility of causing a spark between the electrodes 15.

  Next, the laminated body 13 on which the external electrode 15 is formed is immersed in a silicone rubber solution, and the silicone rubber solution is vacuum degassed to fill the groove of the laminated body 13 with silicone rubber. The laminated body 13 is pulled up, and the side surface of the laminated body 13 is coated with silicone rubber. Thereafter, the silicone rubber filled in the groove and coated on the side surface of the laminated body 13 is cured to obtain a laminated piezoelectric element.

  When this multilayer piezoelectric element is used for a piezoelectric actuator, a lead wire is connected to the external electrode 15 and a DC voltage of 0.1 to 3 kV / mm is applied to the pair of external electrodes 15 via the lead wire, By subjecting the laminated body 13 to polarization treatment, a piezoelectric actuator using the laminated piezoelectric element of the present invention can be obtained.

  If the lead wire of this piezoelectric actuator is connected to an external voltage supply unit and a voltage is applied to the metal layer 12 via the lead wire and the external electrode 15, each piezoelectric layer 11 is greatly displaced by the reverse piezoelectric effect, Thus, for example, it functions as an automobile fuel injection valve that injects and supplies fuel to the engine. In addition, since this piezoelectric actuator includes the multilayer piezoelectric element of the present invention, it has a large amount of displacement under high voltage and high pressure, and suppresses the change in the amount of displacement even when continuously driven for a long period of time. can do. High voltage and high pressure in the present invention means that an AC voltage of 0 to +300 V is applied to a piezoelectric actuator (multilayer piezoelectric element) at a frequency of 1 to 300 Hz at room temperature.

  Furthermore, a conductive auxiliary member made of a conductive adhesive in which a metal mesh or a mesh-like metal plate is embedded on the outer surface of the external electrode 15 may be formed. In this case, even when a large current is input to the actuator by providing a conductive auxiliary member on the outer surface of the external electrode 15 and the actuator is driven at a high speed, a large current can flow through the conductive auxiliary member. For the reason that the current flowing through 15 can be reduced, the external electrode 15 can be prevented from causing local heat generation and disconnection, and the durability can be greatly improved. Furthermore, since a metal mesh or a mesh-like metal plate is embedded in the conductive adhesive, it is possible to prevent the conductive adhesive from cracking. The metal mesh is a braided metal wire, and the mesh metal plate means a mesh formed by forming holes in a metal plate.

  The conductive adhesive constituting the conductive auxiliary member is preferably made of a polyimide resin in which silver powder is dispersed. That is, by dispersing silver powder having a low specific resistance in a polyimide resin having a high heat resistance, a conductive auxiliary member having a low resistance value and a high adhesive strength can be formed even when used at a high temperature. .

  The conductive particles are preferably non-spherical particles such as flakes and needles. This is because the entanglement between the conductive particles can be strengthened by making the shape of the conductive particles non-spherical particles such as flakes and needles, and the shear strength of the conductive adhesive can be further increased. This is because it can be increased.

  The multilayer piezoelectric element of the present invention is not limited to these, and various modifications can be made without departing from the gist of the present invention. For example, in the above-described embodiment, the example in which the external electrode 15 is formed on the opposite side surface of the stacked body 13 has been described. However, in the present invention, for example, a pair of external electrodes 15 may be formed on adjacent side surfaces.

<Injection device>
Next, an embodiment of an ejection device including the multilayer piezoelectric element of the present invention described above will be described in detail with reference to the drawings. FIG. 8 is a schematic cross-sectional view showing the injection device according to the present embodiment. As shown in FIG. 8, the injection device according to the present embodiment includes a piezoelectric actuator 43 including the multilayer piezoelectric element of the present invention represented by the above embodiment inside a storage container 31 having an injection hole 33 at one end. Is stored.

  Specifically, a needle valve 35 that can open and close the injection hole 33 is disposed in the storage container 31. A fuel passage 37 is disposed in the injection hole 33 so as to communicate with the movement of the needle valve 35. The fuel passage 37 is connected to an external fuel supply source, and fuel is always supplied to the fuel passage 37 at a constant high pressure. Therefore, when the needle valve 35 opens the injection hole 33, the fuel that has been supplied to the fuel passage 37 is jetted into a fuel chamber of an internal combustion engine (not shown) at a constant high pressure.

  An upper end portion of the needle valve 35 has a large inner diameter, and a piston 41 slidable with a cylinder 39 formed in the storage container 31 is disposed. And in the storage container 31, the piezoelectric actuator 43 provided with the above-mentioned lamination type piezoelectric element is stored.

  In such an injection device, when the piezoelectric actuator 43 is extended by applying a voltage, the piston 41 is pressed, the needle valve 35 closes the injection hole 33, and the supply of fuel is stopped. Further, when the application of voltage is stopped, the piezoelectric actuator 43 contracts, the disc spring 45 pushes back the piston 41, and the injection hole 33 communicates with the fuel passage 37 so that fuel is injected.

  As mentioned above, although one Embodiment of this invention was shown, this invention is not limited to embodiment mentioned above. For example, in the above-described embodiment, the case where the multilayer piezoelectric element is used for the injection device has been described. However, the present invention is not limited to this, and for example, a fuel injection device for an automobile engine, a liquid injection device such as an ink jet , Mounted on precision positioning devices such as optical devices, vibration prevention devices, etc., or mounted on combustion pressure sensors, knock sensors, acceleration sensors, load sensors, ultrasonic sensors, pressure sensors, yaw rate sensors, etc. The present invention can be applied to sensor elements and circuit elements mounted on piezoelectric gyros, piezoelectric switches, piezoelectric transformers, piezoelectric breakers, and the like. Moreover, even if it is a thing other than these, if it is an element using a piezoelectric characteristic, it can implement.

  EXAMPLES Hereinafter, although an Example is given and this invention is demonstrated further in detail, this invention is not limited to a following example.

<Production of piezoelectric actuator>
A piezoelectric actuator composed of a multilayer piezoelectric element was produced as follows.
First, a slurry in which a calcined powder of a piezoelectric ceramic mainly composed of lead zirconate titanate (PbZrO ₃ -PbTiO ₃ ) having an average particle diameter of 0.4 μm, a binder, and a plasticizer is prepared, and a doctor blade method is used. A plurality of ceramic green sheets to be the piezoelectric layer 11 having a thickness of 150 μm were produced. Subsequently, the main metal layer 12a, the low filling metal layer 12b, and the high filling metal layer 12c were each printed on one side of the ceramic green sheet by a screen printing method.

Specifically, the main metal layer 12a, the low filling metal layer 12b, and the high filling metal layer 12c were printed as follows.
Main metal layer 12a: Acrylic beads having an average particle diameter of 0.2 μm are added to a silver-palladium alloy (95% by mass of silver—5% by mass of palladium) at a ratio of 10 parts by mass with respect to 100 parts by mass of the silver-palladium alloy. Furthermore, the electrically conductive paste which added the binder was printed so that it might become thickness 3 micrometers on the single side | surface of a sheet | seat.
Low filling metal layer 12b: A conductive paste obtained by adding a binder to a silver-palladium alloy (silver 95% by mass-palladium 5% by mass) is printed on one side of the sheet so as to have a thickness of 1 μm. An acrylic bead paste in which a binder was added to acrylic beads having a diameter of 1 μm was laminated and printed so as to have a thickness of 10 μm. The acrylic beads were blended so as to have a ratio of 5 parts by mass with respect to 100 parts by mass of the silver-palladium alloy.
Highly filled metal layer 12c: A conductive paste obtained by adding a binder to a silver-palladium alloy (silver 95% by mass-palladium 5% by mass) was printed on one side of the sheet so as to have a thickness of 3 μm.

300 sheets on which each metal layer was printed as described above were prepared. Separately, green sheets to become the inactive layer 14 were prepared, and these were laminated in order from the bottom to 30 inactive layers, 300 laminated bodies, and 30 inactive layers to obtain a laminated molded body. .
In addition, when laminating | stacking, it laminated | stacked by the combination shown in Table 1. Details in Table 1 are as follows.
-Ratio of the number of metal layers 12a: Ratio of the number of main metal layers 12a to the total number of metal layers (%)
-Opposite arrangement of the low filling metal layer 12b and the high filling metal layer 12c: whether or not the low filling metal layer 12b and the high filling metal layer 12c are arranged opposite to each other with at least one piezoelectric layer 11 interposed therebetween. The metal layers on both sides of the metal layer 12b are highly filled metal layers 12c: whether or not the metal layers on both sides adjacent to the low filled metal layer 12b in the stacking direction are the highly filled metal layers 12c. Laminate in order of high: In the lamination direction, the low-fill metal layer 12b, the high-fill metal layer 12c, and the main metal layer 12a are arranged in this order via the piezoelectric layer 11, and the main metal layer 12a is disposed in the metal filling rate. Whether they are stacked in descending order

The laminated molded body was pressed, degreased and fired. Firing was held at 800 ° C. for 2 hours, and then fired at 1000 ° C. for 2 hours to obtain a laminate 13. About this laminated body 13, as a result of measuring the metal filling rate of each metal layer 12a-12c, it was as follows.
-Filling ratio X of metal in main metal layer 12a: 70%
-Metal filling rate Y in the low filling metal layer 12b: 45%
-Metal filling rate Z in highly filled metal layer 12c: 85%

  Next, a binder is added to a mixture of a flaky silver powder having an average particle diameter of 2 μm and an amorphous glass powder having a softening point of 640 ° C. with the remainder being silicon whose average particle diameter is 2 μm. 8 parts by mass was added to 100 parts by mass of the total mass of the powder, and mixed well to prepare a silver glass conductive paste. Next, this silver glass conductive paste was formed on a release film by screen printing and dried, and then peeled off from the release film to obtain a sheet of silver glass conductive paste. The sheet of silver glass paste was transferred to the surface of the external electrode 15 of the laminate 13 and laminated, and baked at 700 ° C. for 30 minutes to form the external electrode 15 to obtain a multilayer piezoelectric element.

  A lead wire is connected to the external electrode 15 of the laminated piezoelectric element obtained above, and a 3 kV / mm direct current electric field is applied to the positive electrode and the negative electrode 15 via the lead wire for 15 minutes to perform polarization treatment. A piezoelectric actuator using a multilayer piezoelectric element as shown in FIG. 1 was prepared (Sample Nos. 1 to 9 in Table 1). When a DC voltage of 170 V was applied to the obtained multilayer piezoelectric element, a displacement amount was obtained in the lamination direction in all piezoelectric actuators.

<Evaluation>
A continuous drive test was performed on each of the piezoelectric actuators obtained above. The evaluation method is shown below, and the results are shown in Table 1.
(Evaluation method for continuous drive test)
A test was performed in which each piezoelectric actuator was continuously driven up to 1 × 10 ⁹ times by applying an AC voltage of 0 to +170 V at a frequency of 150 Hz at room temperature. More specifically, the test was performed on 100 samples. The displacement was measured with an optical non-contact micro displacement meter. The amount of displacement in the initial state means the amount of displacement when driven once. Moreover, the laminated part after continuous drive was observed using a metal microscope, SEM, etc., and the presence or absence of delamination was observed. Furthermore, the presence or absence of noise generation of harmonic components and the presence or absence of beat sound generation at 1 kHz were evaluated.

As is clear from Table 1, the sample No. In No. 9, the stress applied to the laminated interface was concentrated on one point and the load increased to cause delamination (delamination), and the noise and noise were generated. On the other hand, sample no. It can be seen that Nos. 1 to 8 have effective displacements required as piezoelectric actuators without significantly decreasing the element displacements even after 1 × 10 ⁹ continuous driving. Therefore, it can be said that a piezoelectric actuator having excellent durability could be produced.

  In particular, the sample No. 1 in which the stress relaxation layer (low filling metal layer 12b) and the stress concentration layer (high filling metal layer 12c) are arranged adjacent to each other via the piezoelectric layer 11 is used. 3 and 4 show that it is possible not only to increase the amount of displacement of the element, but also to produce a laminated actuator with a stable amount of element displacement. Further, the sample No. 1 in which the stress relaxation layer is sandwiched through the piezoelectric layer 11 is used. Nos. 5 to 8 can not only maximize the displacement amount of the element, but also the element displacement amount hardly changes and is extremely excellent in durability, so that a piezoelectric actuator having a stable element displacement amount can be obtained. did it.

  Sample No. in Example 1 above. Each piezoelectric actuator was obtained by changing the composition (Y / X and Z / X) of the metal layer 12 of the piezoelectric actuator No. 8 as shown in Table 2 (Sample Nos. 10 to 15 in Table 2). As a comparative example, the sample No. 1 in Example 1 was used. 9 was also described (Sample No. 15 in Table 2). When a DC voltage of 170 V was applied to the obtained multilayer piezoelectric element, a displacement amount was obtained in the lamination direction in all piezoelectric actuators. Sample No. In the 15 piezoelectric actuators, the filling rate of all the metal layers is set to about 70%. Therefore, in the table, X = 70%, Y = 70%, Z = 70%, and the filling rate ratio Y / X = 1 and Z / X = 1.

Each piezoelectric actuator obtained above (Sample Nos. 10 to 15 in Table 2) was subjected to a continuous drive test in the same manner as in Example 1. The results are shown in Table 2.

  As is apparent from Table 2, the sample Nos. With Y / X larger than 0.9 and Z / X smaller than 1.05. In No. 15, the stress applied to the laminated interface was concentrated on one point and the load increased to cause delamination (delamination), and the generation of noise and noise.

  In contrast, sample no. 10-14, Y / X is in the range of 0.1-0.9 and Z / X is in the range of 1.05-2, so that not only can the displacement of the element be maximized, Since the element displacement amount hardly changed and was extremely excellent in durability, a multilayer actuator with a stable element displacement amount could be obtained. In particular, sample no. Nos. 12 and 13 are Y / X in the range of 0.5 to 0.8, and Z / X is in the range of 1.1 to 1.2. I was able to.

  Sample No. in Example 1 above. Each piezoelectric actuator was obtained by changing the material composition of the metal layer 12 of the piezoelectric actuator of No. 8 as shown in Table 3 (Sample Nos. 16 to 33 in Table 3). When a DC voltage of 170 V was applied to the obtained multilayer piezoelectric element, a displacement amount was obtained in the lamination direction in all piezoelectric actuators.

  For each of the piezoelectric actuators obtained above, a continuous drive test is performed in the same manner as in Example 1, and the initial displacement amount and the displacement amount after the continuous drive are expressed by the formula: [1- (displacement amount after the continuous drive / (Displacement amount in initial state)] × 100, and the displacement rate change rate (%) was calculated. The results are shown in Table 3.

  As apparent from Table 3, the sample No. 32 and 33, the metal composition in the metal layer 12 has a group 8-10 metal content of more than 15% by mass and a group 11 metal content of less than 85% by mass. It can be seen that the specific resistance of the piezoelectric actuator is large, and when the multilayer piezoelectric element is continuously driven, heat is generated and the displacement of the piezoelectric actuator is reduced.

  In contrast, sample no. 16 to 28, when the content of the metal composition in the metal layer 12 is M1 mass% and the content of the group 11b metal is M2 mass%, 0 <M1 ≦ 15, 85 ≦ M2 <100, M1 + M2 = 100% by mass as a main component, so that the specific resistance of the metal layer 12 can be reduced, and the heat generated in the metal layer 12 can be suppressed even when continuously driven. It can be seen that a laminated actuator with a stable displacement can be produced. Sample No. Nos. 29 to 31 can reduce the specific resistance of the metal layer 12 and suppress the heat generated in the metal layer 12 even when continuously driven, so that it is understood that a laminated actuator with a stable element displacement can be produced.

<Production of piezoelectric actuator>
A piezoelectric actuator composed of a multilayer piezoelectric element was produced as follows.
First, 30 sheets on which each metal layer was printed were prepared in the same manner as in Example 1 above. Next, separately from this, a green sheet to be an inactive layer 14 is prepared, and these are laminated in order from the bottom to 5 inactive layers, 30 laminates, and 5 inactive layers to form a laminated molded body. Obtained.
In addition, when laminating | stacking, it laminated | stacked by the combination shown in Table 4. Details in Table 4 are as follows.
Arrangement of the low-filling metal layer 12b and the high-filling metal layer 12c: whether or not the low-filling metal layer 12b and the high-filling metal layer 12c are opposed to each other with at least one piezoelectric layer 11 interposed therebetween.

The laminated molded body was pressed, degreased and fired. Firing was held at 800 ° C. for 2 hours, and then fired at 1000 ° C. for 2 hours to obtain a laminate 13. About this laminated body 13, as a result of measuring the metal filling rate of each metal layer 12a-12c, it was as follows.
-Filling ratio X of metal in main metal layer 12a: 70%
-Metal filling rate Y in the low filling metal layer 12b: 45%
-Metal filling rate Z in highly filled metal layer 12c: 85%

  Next, in the same manner as in Example 1, an external electrode 15 was formed on the multilayer body 13 to obtain a multilayer piezoelectric element. Next, a lead wire is connected to the external electrode 15 of the multilayer piezoelectric element obtained as described above, and a 3 kV / mm DC electric field is applied to the positive and negative external electrodes 15 through the lead wire for 15 minutes to perform polarization treatment. A piezoelectric actuator using a multilayer piezoelectric element as shown in FIG. 1 was prepared (Sample Nos. 34 to 37 in Table 4). When a DC voltage of 170 V was applied to the obtained multilayer piezoelectric element, a displacement amount was obtained in the lamination direction in all piezoelectric actuators.

<Evaluation>
Each piezoelectric actuator obtained above was subjected to a continuous driving test in the same manner as in Example 1. The results are shown in Table 4.

As is apparent from Table 4, the sample No. In No. 37, stress applied to the laminated interface was concentrated on one point, the load increased, delamination (delamination) occurred, and a roar and noise occurred. On the other hand, sample no. It can be seen that Nos. 34 to 36 have effective displacements required as piezoelectric actuators without the element displacements being significantly reduced even after being continuously driven 1 × 10 ⁹ times. Therefore, it can be said that a piezoelectric actuator having excellent durability could be produced.

  In particular, sample No. 1 in which a stress relaxation layer (thin metal layer 12 b) and a stress concentration layer (thick metal layer 12 c) are arranged adjacent to each other via the piezoelectric layer 11. No. 36 can not only increase the amount of displacement of the element but also produce a stacked actuator with a stable amount of element displacement.

(A) is a perspective view which shows the lamination type piezoelectric element concerning one Embodiment of this invention, (b) is a fragmentary perspective view which shows the lamination | stacking state of the piezoelectric material layer and metal layer in (a). . It is a partial expanded sectional view which shows the laminated structure of the lamination type piezoelectric element concerning one Embodiment of this invention. It is a partial expanded sectional view which shows the highly filled metal layer concerning one Embodiment of this invention. It is a partial expanded sectional view which shows the other laminated structure of the lamination type piezoelectric element concerning one Embodiment of this invention. It is a partial expanded sectional view which shows the other laminated structure of the lamination type piezoelectric element concerning one Embodiment of this invention. It is a schematic explanatory drawing for demonstrating the space | gap of the piezoelectric material layer concerning one Embodiment of this invention. It is a partial expanded sectional view which shows the laminated structure concerning one Embodiment of the other laminated piezoelectric element of this invention. It is a schematic sectional drawing which shows the injection apparatus concerning one Embodiment of this invention. (A) is a perspective view which shows the conventional lamination type piezoelectric element, (b) is a fragmentary perspective view which shows the lamination | stacking state of the piezoelectric material layer and metal layer in (a). It is a partial expanded sectional view which shows the laminated structure in the conventional laminated piezoelectric element.

Explanation of symbols

DESCRIPTION OF SYMBOLS 11 Piezoelectric layer 12,12a Metal layer 12b Low filling metal layer 12c High filling metal layer 13 Laminated body 14 Inactive layer 15 External electrode 31 Storage container 33 Injection hole 35 Needle valve 37 Fuel passage 39 Cylinder 41 Piston 43 Piezoelectric actuator 45 Dish Spring

Claims (20)

  In the multi-layer piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, the plurality of metal layers are metal layers on both sides adjacent to each other in a filling direction of a metal constituting the metal layer. A multilayer piezoelectric element comprising a plurality of low-filling metal layers lower than the above.   2. The multilayer piezoelectric element according to claim 1, wherein the plurality of low-filling metal layers are respectively disposed with a plurality of metal layers other than the low-filling metal layer interposed therebetween.   The multilayer piezoelectric element according to claim 1, wherein the plurality of low-filling metal layers are regularly arranged in a stacking direction.   4. The plurality of metal layers include a plurality of highly filled metal layers in which a metal filling rate of the metal layers is higher than metal layers on both sides adjacent to each other in the stacking direction. Multilayer piezoelectric element.   In the multi-layer piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, the plurality of metal layers are metal layers on both sides adjacent to each other in a filling direction of a metal constituting the metal layer. A multilayer piezoelectric element comprising a plurality of higher highly filled metal layers.   The multilayer piezoelectric element according to claim 5, wherein the plurality of highly filled metal layers are respectively disposed with a plurality of metal layers other than the highly filled metal layer interposed therebetween.   The multilayer piezoelectric element according to claim 5 or 6, wherein the plurality of highly filled metal layers are regularly arranged in the stacking direction.   The plurality of metal layers include a plurality of low-filling metal layers in which a filling rate of a metal constituting the metal layer is lower than metal layers on both sides adjacent to each other in the stacking direction. Multilayer piezoelectric element.   The multilayer piezoelectric element according to claim 4 or 8, wherein a metal layer adjacent to the low filling metal layer in the lamination direction is the high filling metal layer.   The multilayer piezoelectric element according to claim 4 or 8, wherein the metal layers on both sides adjacent to the low filling metal layer in the lamination direction are the high filling metal layers.   The high-filling metal layer has a peak of metal filling rate, and has an inclined region where the metal filling rate gradually decreases from the high-filling metal layer to two or more metal layers in the stacking direction. The multilayer piezoelectric element according to any one of 10.   The multilayer piezoelectric element according to any one of claims 1 to 4, 8 to 10, wherein the low-filling metal layer is composed of a plurality of partial metal layers arranged in a state of being separated from each other via a gap.   Among the plurality of metal layers, a metal layer in which the metal filling rate is lower than the metal layers on both sides adjacent to each other in the stacking direction is a low filling metal layer, and the metal filling rate is adjacent in the stacking direction. The metal layer higher than the metal layers on both sides is a highly filled metal layer, the metal filling rate in the other metal layers excluding the low filling metal layer and the high filling metal layer is X, and the metal filling in the low filling metal layer is The multilayer piezoelectric element according to claim 1, wherein when the ratio is Y, the filling ratio (Y / X) is in the range of 0.1 to 0.9.   Among the plurality of metal layers, a metal layer in which the metal filling rate is lower than the metal layers on both sides adjacent to each other in the stacking direction is a low filling metal layer, and the metal filling rate is adjacent in the stacking direction. The metal layer higher than the metal layers on both sides is a highly filled metal layer, the metal filling rate in the other metal layers excluding the low filling metal layer and the high filling metal layer is X, and the metal filling in the highly filled metal layer is The multilayer piezoelectric element according to any one of claims 1 to 13, wherein when the rate is Z, the ratio of packing rate (Z / X) is in the range of 1.05 to 2.   The metal layer is mainly composed of a metal selected from Group 8 to 11 elements of the periodic table, the content of Group 8 to 10 elements of the periodic table in the metal layer is M1 (mass%), and the periodic table The laminated type according to any one of claims 1 to 14, wherein when the content of the Group 11 element is M2 (% by mass), the relationship of 0 <M1 ≦ 15, 85 ≦ M2 <100, M1 + M2 = 100 is satisfied. Piezoelectric element.   The group 8-10 elements of the periodic table in the metal layer are at least one selected from Ni, Pt, Pd, Rh, Ir, Ru and Os, and the group 11 elements of the periodic table are Cu, Ag and The multilayer piezoelectric element according to claim 15, which is at least one selected from Au.   The multilayer piezoelectric element according to claim 1, wherein the metal layer contains Cu as a main component.   In a stacked piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, an inactive layer made of a piezoelectric material is formed at both ends in the stacking direction. An adjacent metal layer is a low-fill metal layer in which a metal filling rate in the metal layer is lower than a metal filling rate in a metal layer adjacent in the stacking direction.   In a stacked piezoelectric element in which a plurality of piezoelectric layers and a plurality of metal layers are alternately stacked, an inactive layer made of a piezoelectric material is formed at both ends in the stacking direction. The adjacent metal layer is a high-fill metal layer in which the metal filling rate in the metal layer is higher than the metal filling rate in the metal layer adjacent in the stacking direction. A container having an ejection hole and the multilayer piezoelectric element according to any one of claims 1 to 19 accommodated in the container, wherein the liquid filled in the container drives the multilayer piezoelectric element. An ejector configured to discharge from the ejection hole.

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