Dielectric composition, dielectric element, electronic component, and multilayer electronic component

Abstract

A dielectric composition with high voltage resistance and favorable reliability, and an electronic component using the composition, the composition containing a tungsten bronze type composite oxide represented by chemical formula (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.6.00xR.sub.x(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.x2.00(Nb.sub.1.00bTa.sub.b).sub.8.00xO.sub.30.00, wherein R is at least one element selected from Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu, and s, t, x, a, b, and d satisfy 0s1.00, 0t1.00, 0s+t1.00, 0x3.00, 0.01a0.98, 0b1.00, 0.02d0.15, and 0.03a+d1.00. At least one element selected from Mn, Mg, Co, V, W, Mo, Li, B, and Al are contained as a sub component in 0.10 mol or more and 20.00 mol or less with respect to 100 mol of the main component.

Claims

1. A dielectric composition comprising, as a main component, a tungsten bronze type composite oxide represented by a chemical formula (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.6.00xR.sub.x(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.x+2.00(Nb.sub.1.00bTa.sub.b).sub.8.00xO.sub.30.00, wherein the R is at least one element selected from Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu, and s, t, x, a, b, and d satisfy 0s1.00, 0t1.00, 0s+t1.00, 0x3.00, 0.01a0.98, 0b1.00, 0.02d0.15, and 0.03a+d1.00.

2. The dielectric composition according to claim 1, wherein at least one selected from Mn, Mg, Co, V, W, Mo, Li, B, and Al is contained as a sub component in 0.10 mol or more and 20.00 mol or less with respect to 100 mol of the main component.

3. The dielectric composition according to claim 1, wherein a substitution amount a of Zr in the chemical formula is 0.50a0.98.

4. A dielectric element comprising the dielectric composition according to claim 1.

5. An electronic component comprising a dielectric layer comprising the dielectric composition according to claim 1.

6. A multilayer electronic component comprising a multilayer portion wherein a dielectric layer comprising the dielectric composition according to claim 1 and an internal electrode layer are alternately stacked.

Description

BRIEF DESCRIPTION OF DRAWINGS

(1) FIGURE illustrates a cross-sectional view of a multilayer ceramic capacitor according to an embodiment of the present invention.

MODE(S) FOR CARRYING OUT THE INVENTION

(2) Hereinafter, embodiments of the present invention will be described.

(3) A dielectric composition according to the present embodiment contains, as a main component,

(4) a tungsten bronze type composite oxide represented by a chemical formula (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.6.00xR.sub.x(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.x2.00(Nb.sub.1.00bTa.sub.b).sub.8.00xO.sub.30.00,

(5) in which the R is at least one element selected from Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu, and

(6) s, t, x, a, b, and d satisfy

(7) 0s1.00,

(8) 0t1.00,

(9) 0s+t1.00,

(10) 0x3.00,

(11) 0.01a0.98,

(12) 0b1.00,

(13) 0.02d0.15, and

(14) 0.03a+d1.00.

(15) When the dielectric composition according to the present embodiment contains, as a main component, a tungsten bronze type composite oxide represented by the chemical formula, high voltage resistance is easily obtained. Regarding the reason for this, the present inventors consider as follows. Since the tungsten bronze type composite oxide as the main component of the present embodiment has a characteristic that the bandgap is wide, electrons in the valence band are difficult to excite to the conduction band so that a carrier concentration of electrons that are a majority carrier involved in conduction can be suppressed. In addition, it is considered that the carrier concentration of conduction electrons that are a majority carrier affects electron avalanche that is a typical breakdown mode of the voltage resistance. In the dielectric composition of the present invention, since the carrier concentration of electrons that are a majority carrier can be suppressed to be low, it is considered that breakdown caused by electron avalanche is difficult to occur. Further, since the bandgap is wide, a certain degree of width of the bandgap can be maintained even when high field strength is applied. Accordingly, it is considered that high voltage resistance is obtained even in high field strength. In addition, since an alkali metal with high volatility is not contained, a lattice defect is difficult to occur and conduction electrons are difficult to generate so that the dielectric composition of the present invention has a characteristic that the specific resistance is also high.

(16) s in the chemical formula represents a substitution amount of Ba, t represents a substitution amount of Ca, and 1.00(s+t) represents a substitution amount of Sr. Since Ba, Ca, and Sr are arbitrary components, the substitution amounts thereof are 0s1.00, 0t1.00, and 01.00(s+t)1.00. Accordingly, the crystal structure of the tungsten bronze type is maintained and high voltage resistance is easily obtained. Further, preferably, when s, t, and 1.00(s+t) in the chemical formula are 0.50s1.00, 0t0.50, and 01.00(s+t)0.50, higher voltage resistance is easily obtained. On the other hand, in a case where K, Na, or the like that is an alkali metal element is contained in addition to Sr, Ba, and Ca, since volatility of the alkali metal element is high, a lattice defect easily occurs by a heat treatment (such as firing process), and as a result, there is a tendency that high voltage resistance is difficult to obtain.

(17) When R in the chemical formula is at least one element selected from Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu, high voltage resistance is easily obtained.

(18) x in the chemical formula represents a substitution amount of R, and R is an arbitrary component and an upper limit of the substitution amount thereof is 3.00. For example, when a tungsten bronze type composite oxide such as (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.6.00(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.2.00(Nb.sub.1.00bTa.sub.b).sub.8.00O.sub.30.00 in the case of x=0, (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.5.00R(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.3.00(Nb.sub.1.00bTa.sub.b).sub.7.00O.sub.30.00 in the case of x=1.00, (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.4.00R.sub.2.00(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.4.00(Nb.sub.1.00bTa.sub.b).sub.6.00O.sub.30.00 in the case of x=2.00, or (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.3.00(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.5.00(Nb.sub.1.00bTa.sub.b).sub.5.00O.sub.30.00 in the case of x=3.00 is used as the main component, high voltage resistance and favorable DC bias characteristics are easily obtained. Particularly in the case of 1.00x3.00, higher voltage resistance and further favorable DC bias characteristics are easily obtained. On the other hand, in a case where x is more than 3.00, for example, in a composite oxide of a chemical formula Ba.sub.200La.sub.4.00(Zr.sub.aSi.sub.d).sub.6.00Nb.sub.4.00O.sub.30.00 or the like, the crystal structure of the tungsten bronze type is difficult to form so that it is difficult to obtain high voltage resistance that is a feature of the present invention.

(19) When a substitution amount d of Si in the chemical formula is 0.02d0.15, favorable DC bias characteristics are easily obtained. The reason for this is considered that Si substituted in the tungsten bronze type composite oxide crystal affects the ion displacement of the crystal. When the substitution amount d of Si exceeds 0.15, there is a tendency that a high specific permittivity cannot be maintained.

(20) When the substitution amount a of Zr in the chemical formula is 0.01a0.98, the bandgap becomes wide so that high voltage resistance is easily obtained. On the other hand, when the substitution amount a is less than 0.01, the action of widening the bandgap is weak, and as a result, high voltage resistance is difficult to obtain.

(21) For this reason, a preferable range of the substitution amount a of Zr in the chemical formula is 0.50a0.98. With the above-described range, the action of widening the bandgap can be strengthened, and as a result, higher voltage resistance is easily obtained.

(22) Also in a case where Nb in the chemical formula is substituted with Ta, the crystal structure of the tungsten bronze type can be maintained, and Ta is an arbitrary component. Moreover, when a substitution amount b of Ta is set to 0.10b1.00, higher voltage resistance is easily obtained.

(23) As the sub component, it is preferable that at least one or more elements selected from Mn, Mg, Co, V, W, Mo, Li, B, and Al are contained. Owing to an interaction between Zr contained in the main component and these elements, high voltage resistance and high specific resistance are easily obtained. Preferably, when the substitution amount a of Zr is 0.80a0.98, the interaction is enhanced so that higher voltage resistance is easily obtained.

(24) When the amount of the sub component is set to 0.10 mol or more and 20.00 mol or less with respect to 100 mol of the main component, high specific resistance of 910.sup.12 cm or more can be obtained at 200 C. Moreover, higher voltage resistance can be obtained even at a high temperature of 175 C. or higher.

(25) Further, other than R contained in the main component, at least one element selected from Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu may be contained as a second sub component. The second sub component is an arbitrary component and an upper limit of the amount thereof is determined in a range within which the object of the invention can be achieved.

(26) Further, other than Si contained in the main component, Si as a third sub component may be contained. The third sub component is an arbitrary component and an upper limit of the amount thereof is determined in a range within which the object of the invention can be achieved.

(27) Incidentally, the dielectric composition may further contain fine impurities or other sub components as long as they do not largely deteriorate dielectric properties that are the effects of the present invention, that is, the specific permittivity, the specific resistance, and the voltage resistance. Therefore, the amount of the main component is not particularly limited, and for example, is 50 mol % or more and 100 mol % or less with respect to the whole dielectric composition containing the main component.

(28) Next, description will be given using a multilayer ceramic capacitor as an example. FIGURE illustrates a multilayer ceramic capacitor according to an embodiment of the present invention. A multilayer ceramic capacitor 1 has a capacitor element main body 10 having a configuration in which a dielectric layer 2 and an internal electrode layer 3 are alternately stacked. A pair of external electrodes 4, which is conductive with each of the internal electrode layers 3 alternately disposed inside the capacitor element main body 10, is formed at both ends of the capacitor element main body 10. The shape of the capacitor element main body 10 is not particularly limited, and is typically a rectangular parallelepiped shape. In addition, the dimension thereof is also not particularly limited, and the dimension may be appropriately determined depending on the use application.

(29) The thickness of the dielectric layer 2 is not particularly limited, and may be appropriately determined depending on the use application of the multilayer ceramic capacitor 1.

(30) The conductive material contained in the internal electrode layer 3 is not particularly limited, and is preferably Ni, Pd, Ag, a PdAg alloy, Cu, or a Cu-based alloy. Incidentally, a trace amount of various components such as P may be contained in about 0.1% by weight or less in Ni, Pd, Ag, a PdAg alloy, Cu, or a Cu-based alloy. In addition, the internal electrode layer 3 may be formed using a commercially available paste for an electrode. The thickness of the internal electrode layer 3 may be appropriately determined depending on the use application or the like.

(31) The conductive material contained in the external electrode 4 is not particularly limited, and Cu, a Cu-based alloy, Ni, a Ni-based alloy, Ag, an AgPd alloy, and the like are typically used. The thickness of the external electrode may be appropriately determined depending on the use application or the like, and typically, is preferably about 5 m to 50 m. As necessary, a coating layer is formed on the surface of the external electrode 4 by plating or the like.

(32) Next, an example of a method for manufacturing the multilayer ceramic capacitor illustrated in FIGURE will be described.

(33) The multilayer ceramic capacitor 1 of the present embodiment is manufactured by producing a green chip by a typical printing method or sheet method using a paste, firing the green chip, then applying an external electrode to the green chip, and firing the obtained product, similarly to a multilayer ceramic capacitor of the related art. Hereinafter, the manufacturing method will be described in detail.

(34) An example of the method for manufacturing the multilayer ceramic capacitor according to the present embodiment will be described.

(35) First, raw materials are prepared such that the main component has a desired proportion, and are mixed and heat-treated (calcined) at 800 C. or higher. Thus, calcined powder can be obtained. Preferably, a heat treatment is performed at 800 C. to 1000 C. such that the particle size of the calcined powder is 0.1 m or more and 5.0 m or less. It is preferable that a different phase such as Ba.sub.5Nb.sub.4O.sub.15 having an anisotropic shape is not contained in the calcined powder.

(36) In the present embodiment, a feature that has not been obtained before can be found when the sub component is not contained and only the main component is heat-treated (calcined) at the time of obtaining the calcined powder. That is, in the tungsten bronze type composite oxide represented by a chemical formula (Sr.sub.1.00(s+t)Ba.sub.sCa.sub.t).sub.6.00xR.sub.x(Ti.sub.1.00(a+d)Zr.sub.aSi.sub.d).sub.x2.00(Nb.sub.1.00bTa.sub.b).sub.8.00xO.sub.30.00 that is the dielectric composition according to the present embodiment, when Ba and Ca are allowed to reliably exist at the position of Sr in the chemical formula, Zr or Si is allowed to reliably exist at the position of Ti, and Ta is allowed to reliably exist at the position of Nb, a new feature that has not been obtained in a manufacturing method of the related art can be obtained. Therefore, it is preferable to confirm that a target element is substituted on the basis of an increase or decrease in lattice constant of the crystal obtained by X-ray diffraction of the calcined powder.

(37) Regarding the raw materials, an oxide mainly configured by Sr, Ba, Ca, Ti, Zr, Nb, Ta, Si, Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, or Lu, or a mixture thereof can be used as raw material powder. Moreover, the raw materials can be appropriately selected from various compounds that become the aforementioned oxide or composite oxide by firing, for example, carbonate, oxalate, nitrate, hydroxide, an organometallic compound, and the like and can be mixed for use. Specifically, SrO or SrCO.sub.3 may be used as a raw material of Sr.

(38) Further, in a case where the dielectric composition according to the present embodiment contains a sub component, a raw material of the sub component is also prepared. The raw material of the sub component is not particularly limited, and oxides of respective components or mixtures thereof can be used as raw material powder. Moreover, the raw materials can be appropriately selected from various compounds that become the aforementioned oxide or composite oxide by firing, for example, carbonate, oxalate, nitrate, hydroxide, an organometallic compound, and the like and can be mixed for use.

(39) The prepared calcined powder of the main components and the raw material of the sub component are weighed to have a predetermined compositional ratio and mixed, thereby obtaining a dielectric composition raw material. Examples of a mixing method include wet mixing performed using a ball mill and dry mixing performed using a dry mixer.

(40) This dielectric composition raw material is prepared in the form of a coating material to prepare a paste for a dielectric layer. The paste for a dielectric layer may be an organic coating material obtained by kneading a dielectric raw material and an organic vehicle or may be an aqueous coating material.

(41) The organic vehicle is obtained by dissolving a binder in an organic solvent. The binder used in the organic vehicle is not particularly limited, and may be appropriately selected from typical various binders such as ethylcellulose and polyvinyl butyral. The organic solvent to be used is also not particularly limited, and may be appropriately selected from various organic solvents such as terpineol, butyl carbitol, and acetone depending on a method to be used such as a printing method or a sheet method.

(42) Further, in a case where the paste for a dielectric layer is produced in the form of an aqueous coating material, an aqueous vehicle obtained by dissolving a water-soluble binder, a dispersant, or the like in water and a dielectric raw material may be kneaded. The water-soluble binder used in the aqueous vehicle is not particularly limited, and for example, polyvinyl alcohol, cellulose, a water-soluble acrylic resin, and the like may be used.

(43) A paste for an internal electrode layer is prepared by kneading the above-described organic vehicle with conductive materials formed from various conductive metals or alloys described above, various oxides, which become the above-described conductive material after firing, an organometallic compound, resinate, or the like.

(44) A paste for an external electrode may be prepared in the similar manner to the paste for an internal electrode layer described above.

(45) The amount of the organic vehicle in each paste described above is not particularly limited, and may be a typical amount, for example, the amount of the binder may be about 1% by weight to 5% by weight and the amount of the solvent may be about 10% by weight to 50% by weight. In addition, additives selected from various dispersants, plasticizers, dielectric materials, insulator materials, and the like may be contained in each paste as necessary. The total amount of these additives is set to preferably 10% by weight or less.

(46) In the case of using a printing method, the paste for a dielectric layer and the paste for an internal electrode layer are printed on a substrate such as PET, stacked, cut in a predetermined shape, and then peeled off from the substrate to obtain a green chip.

(47) Further, in the case of using a sheet method, a green sheet is formed using the paste for a dielectric layer, the paste for an internal electrode layer is printed on the green sheet, and then these are stacked to obtain a green chip.

(48) The green chip is subjected to a binder removal treatment before firing described later. As binder removal conditions, a temperature increase rate is set to preferably 5 C./hr to 300 C./hr, a retention temperature is set to preferably 180 C. to 500 C., and a temperature retention time is set to preferably 0.5 hours to 24 hours. In addition, the atmosphere of the binder removal treatment is set to air or reductive atmosphere.

(49) Further, the retention temperature at the time of firing is preferably 1000 C. to 1400 C. and more preferably 1100 C. to 1360 C. When the retention temperature is less than the above ranges, densification is not sufficient. When the retention temperature exceeds the above ranges, disconnection of the electrode by abnormal sintering of the internal electrode layer and increase in change ratio of capacitance by diffusion of an internal electrode layer constituent material easily occur. In addition, when the retention temperature exceeds the above ranges, there is a concern that dielectric particles coarsen to decrease voltage resistance.

(50) As firing conditions other than the above firing conditions, in order to achieve uniform firing of a chip, the temperature increase rate is set to preferably 50 C./hr to 500 C./hr and more preferably 200 C./hr to 300 C./hr, and in order to control the particle diameter distribution after sintering within a range of 0.1 m to 10.0 m, the temperature retention time is set to preferably 0.5 hours to 24 hours and more preferably 1 hour to 3 hours, and the cooling rate is set to preferably 50 C./hr to 500 C./hr and more preferably 200 C./hr to 300 C./hr.

(51) In the above-described binder removal treatment, for example, a wetter or the like may be used in wetting of N.sub.2 gas, mixed gas, or the like. In this case, the water temperature is preferably about 5 C. to 75 C. In addition, the binder removal treatment, firing, and annealing may be performed consecutively or independently.

(52) The capacitor element main body 10 obtained as described above is polished at the end faces thereof, for example, by barrel polishing, sandblasting, or the like and the paste for an external electrode is applied and fired, thereby forming the external electrode 4. Then, as necessary, a coating layer is formed on the surface of the external electrode 4 by plating or the like.

(53) Hereinbefore, the embodiments of the present invention have been described. The present invention is not limited to the aforementioned embodiments, and can be variously modified in a range not departing from the gist of the present invention.

EXAMPLES

(54) Hereinafter, the present invention will be described in more detail by means of specific examples of the present invention. The present invention is not limited to these examples. Incidentally, specimens marked with in Table 2 are outside the range of the present invention.

(55) As a raw material of the main component, each powder of SrCO.sub.3, BaCO.sub.3, CaCO.sub.3, TiO.sub.2, ZrO.sub.2, Nb.sub.2O.sub.5, Ta.sub.2O.sub.5, Bi.sub.2O.sub.3, Y.sub.2O.sub.3, La.sub.2O.sub.3, Pr.sub.2O.sub.3, Nd.sub.2O.sub.3, Sm.sub.2O.sub.3, Eu.sub.2O.sub.3, Gd.sub.2O.sub.3, Tb.sub.2O.sub.3, Dy.sub.2O.sub.3, Ho.sub.2O.sub.3, Er.sub.2O.sub.3, Tm.sub.2O.sub.3, Yb.sub.2O.sub.3, Lu.sub.2O.sub.3, and SiO.sub.2 was prepared.

(56) These materials were weighed to have the main component composition in Table 1, then wet-mixed with a ball mill, dried, and calcined at 800 C. to obtain calcined powder of the main component. A dielectric composition raw material was prepared. As a raw material of the sub component, each powder of MgO, Co.sub.2O.sub.3, V.sub.2O.sub.5, WO.sub.3, MoO.sub.3, MnO, Li.sub.2CO.sub.3, B.sub.2O.sub.3, Al.sub.2O.sub.3, Fe.sub.3O.sub.4, and SiO.sub.2 was prepared and the main components and the sub components were mixed to respectively have a proportion in Table 1 to obtain dielectric composition raw materials of Specimen No. 1 to Specimen No. 74.

(57) TABLE-US-00001 TABLE 1 Accessory component [mol %] (with respect to 100 mol of main component) 1.00 (s + t) s t Re x a b d Mg Co V W Specimen No. 1 0.00 1.00 0.00 La 2.00 0.30 0.00 0.10 Specimen No. 2 0.20 0.80 0.00 La 2.00 0.30 0.00 0.10 Specimen No. 3 0.50 0.50 0.00 La 2.00 0.30 0.00 0.10 Specimen No. 4 0.80 0.20 0.00 La 2.00 0.30 0.00 0.10 Specimen No. 5 1.00 0.00 0.00 La 2.00 0.30 0.00 0.10 Specimen No. 6 0.00 0.80 0.20 La 2.00 0.30 0.00 0.10 Specimen No. 7 0.00 0.50 0.50 La 2.00 0.30 0.00 0.10 Specimen No. 8 0.00 0.20 0.80 La 2.00 0.30 0.00 0.10 Specimen No. 9 0.00 0.00 1.00 La 2.00 0.30 0.00 0.10 Specimen No. 10 0.80 0.00 0.20 La 2.00 0.30 0.00 0.10 Specimen No. 11 0.50 0.00 0.50 La 2.00 0.30 0.00 0.10 Specimen No. 12 0.20 0.00 0.80 La 2.00 0.30 0.00 0.10 Specimen No. 13 0.10 0.80 0.10 0.00 0.30 0.00 0.10 Specimen No. 14 0.10 0.80 0.10 La 1.00 0.30 0.00 0.10 Specimen No. 15 0.10 0.80 0.10 La 3.00 0.30 0.00 0.10 Specimen No. 16 0.10 0.80 0.10 La 4.00 0.30 0.00 0.10 Specimen No. 17 0.10 0.80 0.10 Y 2.00 0.30 0.00 0.10 Specimen No. 18 0.10 0.80 0.10 Pr 2.00 0.30 0.00 0.10 Specimen No. 19 0.10 0.80 0.10 Nd 2.00 0.30 0.00 0.10 Specimen No. 20 0.10 0.80 0.10 Sm 2.00 0.30 0.00 0.10 Specimen No. 21 0.10 0.80 0.10 Eu 2.00 0.30 0.00 0.10 Specimen No. 22 0.10 0.80 0.10 Gd 2.00 0.30 0.00 0.10 Specimen No. 23 0.10 0.80 0.10 Tb 2.00 0.30 0.00 0.10 Specimen No. 24 0.10 0.80 0.10 Dy 2.00 0.30 0.00 0.10 Specimen No. 25 0.10 0.80 0.10 Ho 2.00 0.30 0.00 0.10 Specimen No. 26 0.10 0.80 0.10 Er 2.00 0.30 0.00 0.10 Specimen No. 27 0.10 0.80 0.10 Tm 2.00 0.30 0.00 0.10 Specimen No. 28 0.10 0.80 0.10 Yb 2.00 0.30 0.00 0.10 Specimen No. 29 0.10 0.80 0.10 Lu 2.00 0.30 0.00 0.10 Specimen No. 30 0.10 0.80 0.10 La, Sm 2.00 0.30 0.00 0.10 Specimen No. 31 0.10 0.80 0.10 Bi 2.00 0.30 0.00 0.10 Specimen No. 32 0.10 0.80 0.10 La 2.00 0.00 0.00 0.10 Specimen No. 33 0.10 0.80 0.10 La 2.00 0.01 0.00 0.10 Specimen No. 34 0.10 0.80 0.10 La 2.00 0.20 0.00 0.10 Specimen No. 35 0.10 0.80 0.10 La 2.00 0.50 0.00 0.10 Specimen No. 36 0.10 0.80 0.10 La 2.00 0.80 0.00 0.10 Specimen No. 37 0.10 0.80 0.10 La 2.00 0.90 0.00 0.10 Specimen No. 38 0.10 0.80 0.10 La 2.00 0.30 0.05 0.10 Specimen No. 39 0.10 0.80 0.10 La 2.00 0.30 0.10 0.10 Specimen No. 40 0.10 0.80 0.10 La 2.00 0.30 0.50 0.10 Specimen No. 41 0.10 0.80 0.10 La 2.00 0.30 1.00 0.10 Specimen No. 42 0.10 0.80 0.10 La 2.00 0.30 0.00 0.00 Specimen No. 43 0.10 0.80 0.10 La 2.00 0.30 0.00 0.02 Specimen No. 44 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 45 0.10 0.80 0.10 La 2.00 0.30 0.00 0.15 Specimen No. 46 0.10 0.80 0.10 La 2.00 0.30 0.00 0.20 Specimen No. 47 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 0.05 Specimen No. 48 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 0.10 Specimen No. 49 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 1.00 Specimen No. 50 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 10.00 Specimen No. 51 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 20.00 Specimen No. 52 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 30.00 Specimen No. 53 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 1.00 Specimen No. 54 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 1.00 Specimen No. 55 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 1.00 Specimen No. 56 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 57 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 58 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 59 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 60 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 61 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 62 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 Specimen No. 63 0.10 0.80 0.10 La 2.00 1.00 0.00 0.00 Specimen No. 64 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 3.00 Specimen No. 65 0.10 0.80 0.10 La 2.00 0.30 0.00 0.10 5.00 1.00 1.00 Specimen No. 66 0.10 0.80 0.10 La 2.00 0.00 1.00 0.10 Specimen No. 67 0.10 0.80 0.10 Pr 2.00 0.80 0.00 0.10 Specimen No. 68 0.10 0.80 0.10 Nd 2.00 0.98 1.00 0.02 Specimen No. 69 0.00 0.00 1.00 Y 0.00 0.01 0.00 0.10 Specimen No. 70 0.00 0.00 1.00 Y 0.00 0.01 0.10 0.10 Specimen No. 71 0.00 0.00 1.00 Y 0.00 0.01 0.00 0.10 1.00 Specimen No. 72 0.00 1.00 0.00 La 2.00 0.30 0.00 0.10 Specimen No. 73 0.00 0.00 1.00 Y 0.00 0.01 0.00 0.10 Specimen No. 74 0.00 0.00 1.00 Y 0.00 0.01 0.10 0.10 Accessory component [mol %] (with respect to 100 mol of main component) Mo Mn Li B Al Fe Si Specimen No. 1 Specimen No. 2 Specimen No. 3 Specimen No. 4 Specimen No. 5 Specimen No. 6 Specimen No. 7 Specimen No. 8 Specimen No. 9 Specimen No. 10 Specimen No. 11 Specimen No. 12 Specimen No. 13 Specimen No. 14 Specimen No. 15 Specimen No. 16 Specimen No. 17 Specimen No. 18 Specimen No. 19 Specimen No. 20 Specimen No. 21 Specimen No. 22 Specimen No. 23 Specimen No. 24 Specimen No. 25 Specimen No. 26 Specimen No. 27 Specimen No. 28 Specimen No. 29 Specimen No. 30 Specimen No. 31 Specimen No. 32 Specimen No. 33 Specimen No. 34 Specimen No. 35 Specimen No. 36 Specimen No. 37 Specimen No. 38 Specimen No. 39 Specimen No. 40 Specimen No. 41 Specimen No. 42 Specimen No. 43 Specimen No. 44 Specimen No. 45 Specimen No. 46 Specimen No. 47 Specimen No. 48 Specimen No. 49 Specimen No. 50 Specimen No. 51 Specimen No. 52 Specimen No. 53 Specimen No. 54 Specimen No. 55 Specimen No. 56 1.00 Specimen No. 57 1.00 Specimen No. 58 1.00 Specimen No. 59 1.00 Specimen No. 60 1.00 Specimen No. 61 1.00 Specimen No. 62 1.00 Specimen No. 63 10.00 Specimen No. 64 3.00 Specimen No. 65 0.05 10.00 Specimen No. 66 Specimen No. 67 Specimen No. 68 5.00 Specimen No. 69 Specimen No. 70 Specimen No. 71 Specimen No. 72 Specimen No. 73 Specimen No. 74

(58) - described in Table 1 indicates that the corresponding component is not contained.

(59) The dielectric composition raw material thus obtained (100 parts by weight), a polyvinyl butyral resin (10 parts by weight), dioctyl phthalate (DOP) (5 parts by weight) as a plasticizer, and alcohol (100 parts by weight) as a solvent were mixed with a ball mill to obtain a paste, thereby producing a paste for a dielectric layer.

(60) Apart from the above, Pd particles (44.6 parts by weight), terpineol (52 parts by weight), ethylcellulose (3 parts by weight), and benzotriazole (0.4 part by weight) were kneaded with a three-roll mill to obtain a slurry, thereby producing a paste for a Pd internal electrode layer. In addition, similarly to the paste for a Pd internal electrode layer, a paste for a Ni internal electrode layer was produced using Ni particles.

(61) A green sheet was formed using the produced paste for a dielectric layer on a PET film to have a thickness after drying of 7 m. Subsequently, an internal electrode layer was printed with a predetermined pattern using the paste for an internal electrode layer on the green sheet, and then the sheet was peeled off from the PET film to produce a green sheet having an internal electrode layer. Incidentally, the green sheets each having an internal electrode layer were produced while the paste for a Pd internal electrode layer was used in the green sheets using Specimen No. 1 to Specimen No. 71 and the paste for a Ni internal electrode layer was used in the green sheets using Specimen No. 72 to Specimen No. 74. Subsequently, a plurality of green sheets having an internal electrode layer were stacked and adhered by pressure to obtain a green multilayer body, and this green multilayer body was cut in a predetermined size to obtain a green chip.

(62) Then, regarding the obtained green chip, Specimen No. 1 to Specimen No. 71 were subjected to a binder removal treatment in air (temperature increase rate: 10 C./hr, retention temperature: 400 C., temperature retention time: 8 hours, atmosphere: in air) and subjected to firing in air (temperature increase rate: 200 C./hr, retention temperature: 1000 C. to 1400 C., temperature retention time: 2 hours, cooling rate: 200 C./hr, atmosphere: in air), and Specimen No. 72 to Specimen No. 74 were subjected to a binder removal treatment in nitrogen (temperature increase rate: 10 C./hr, retention temperature: 350 C., temperature retention time: 8 hours, atmosphere: in nitrogen) and subjected to firing in reductive atmosphere (temperature increase rate: 200 C./hr, retention temperature: 1000 C. to 1400 C., temperature retention time: 2 hours, cooling rate: 200 C./hr, oxygen partial pressure: 10.sup.9 to 10.sup.12 Pa, atmosphere: H.sub.2N.sub.2H.sub.2O mixed gas). Thus, capacitor element main bodies were obtained.

(63) The crystal structure of the dielectric layer of the obtained capacitor element main body was subjected to X-ray diffraction (XRD) measurement, and as a result, it was confirmed that the tungsten bronze type composite oxide was obtained. In addition, the composition of the dielectric composition in the dielectric layer of the obtained capacitor element main body was measured by inductively coupled plasma source mass spectrometry (ICP-MS), and as a result, it was confirmed that the composition in Table 1 was obtained.

(64) The end faces of the obtained capacitor element main body were polished by sandblasting, and then an InGa eutectic alloy was applied as an external electrode to obtain multilayer ceramic capacitor specimens of Specimen No. 1 to Specimen No. 74 having the same shape as the multilayer ceramic capacitor illustrated in FIGURE. The sizes of the obtained multilayer ceramic capacitor specimens were all 3.2 mm1.6 mm1.2 mm, the thickness of the dielectric layer was set to 5.0 m, the thickness of the internal electrode layer was set to 1.5 m, and the number of the dielectric layers interposed between the internal electrode layers was set to 10.

(65) The voltage resistance, the specific permittivity, a change in specific permittivity caused by application of a DC voltage (DC bias characteristics), and the specific resistance of the obtained multilayer ceramic capacitor specimens were measured by the following methods and presented in Table 2.

(66) [Specific Permittivity]

(67) The capacitance C was measured for the multilayer ceramic capacitor specimen at 25 C. by a digital LCR meter (4284A manufactured by YHP) at a frequency of 1 kHz with a signal, which has an input signal level (measurement voltage) of 1 Vrms, being input. Then, the specific permittivity s (no unit of quantity required) was calculated on the basis of the thickness of the dielectric layer, the effective electrode area, and the capacitance C.sub.0 obtained as a result of the measurement. A higher specific permittivity was preferable and the specific permittivity of 300 or more was determined to be favorable.

(68) [DC Bias Characteristics]

(69) The capacitance C.sub.Bias was measured for the multilayer ceramic capacitor specimen at 25 C. by a digital LCR meter (4284A manufactured by YHP) at a frequency of 1 kHz with a signal, which has an input signal level (measurement voltage) of 1 Vrms, being input while electric field application state of a DC voltage of 30 V/m was maintained. The DC bias characteristics were calculated as a change ratio with respect to the capacitance C.sub.0 in an electric field of 0 V/m on the basis of Equation 1.
(Equation 1)
DC bias characteristics={(C.sub.BiasC.sub.0)/C.sub.0}100(1)

(70) In the present example, a case where the DC bias characteristics are within 20% was determined that a decrease in specific permittivity caused by application of a DC voltage is small, which is favorable.

(71) [Specific Resistance]

(72) Insulation resistance was measured for the multilayer ceramic capacitor specimen at 180 C. and 200 C. by a digital resistance meter (R8340 manufactured by ADVANTEST CORPORATION) under conditions of a measurement voltage of 30 V (field strength: 6 V/m) and a measurement time of 60 seconds. A value of specific resistance was calculated from the electrode area of the capacitor specimen and the thickness of the dielectric layer. Higher specific resistance was preferable, and the specific resistance was determined to be favorable when the specific resistance was 1.0010.sup.12 cm or more and more preferably 9.0010.sup.12 cm or more. When the specific resistance is low, leak current increases in the capacitor and malfunction occurs in an electric circuit.

(73) [Voltage Resistance]

(74) A DC voltage was applied to the multilayer ceramic capacitor specimen at 180 C. and 200 C. at a pressure increase rate of 100 V/sec, and a value obtained by dividing a voltage at which leak current exceeds 10 mA by the thickness of the dielectric layer was regarded as voltage resistance (unit: V/m). Higher voltage resistance was preferable, and the voltage resistance was determined to be favorable when the voltage resistance was 150 V/m or more, more preferably 155 V/m or more, further preferably 160 V/m or more, and particularly preferably 175 V/m or more.

(75) TABLE-US-00002 TABLE 2 25 C. 180 C. 200 C. 180 C. 200 C. Specific Specific Specific Voltage Voltage permittivity DC bias resistance resistance resistance resistance [] [%] [cm] [cm] [V/m] [V/m] Specimen No. 1 328 17 3.48E+13 7.82E+12 169 168 Specimen No. 2 326 17 3.48E+13 7.80E+12 167 166 Specimen No. 3 325 18 3.51E+13 7.76E+12 166 164 Specimen No. 4 325 18 3.39E+13 7.48E+12 157 158 Specimen No. 5 324 18 3.29E+13 7.42E+12 155 155 Specimen No. 6 324 16 3.48E+13 7.75E+12 165 164 Specimen No. 7 322 17 3.47E+13 7.71E+12 164 163 Specimen No. 8 322 19 3.33E+13 7.46E+12 156 157 Specimen No. 9 321 18 3.23E+13 7.29E+12 153 153 Specimen No. 10 324 18 3.29E+13 7.37E+12 157 157 Specimen No. 11 323 18 3.25E+13 7.35E+12 155 156 Specimen No. 12 323 17 3.28E+13 7.32E+12 154 154 Specimen No. 13 337 18 2.44E+13 5.53E+12 158 157 Specimen No. 14 332 18 2.79E+13 6.28E+12 167 166 Specimen No. 15 324 16 3.46E+13 7.78E+12 167 167 Specimen No. 16 Specimen No. 17 329 18 3.34E+13 7.51E+12 163 163 Specimen No. 18 323 17 3.45E+13 7.77E+12 165 164 Specimen No. 19 320 18 3.41E+13 7.67E+12 168 167 Specimen No. 20 318 17 3.39E+13 7.63E+12 166 166 Specimen No. 21 316 17 3.37E+13 7.58E+12 166 165 Specimen No. 22 317 16 3.24E+13 7.29E+12 164 164 Specimen No. 23 315 18 3.19E+13 7.18E+12 163 163 Specimen No. 24 313 17 3.30E+13 7.42E+12 167 167 Specimen No. 25 314 18 3.33E+13 7.50E+12 164 164 Specimen No. 26 314 18 3.27E+13 7.35E+12 163 164 Specimen No. 27 312 18 3.17E+13 7.13E+12 164 163 Specimen No. 28 312 17 3.15E+13 7.09E+12 163 165 Specimen No. 29 312 17 3.06E+13 6.88E+12 164 164 Specimen No. 30 320 14 3.42E+13 7.69E+12 167 167 Specimen No. 31 312 17 3.01E+13 6.79E+12 132 127 Specimen No. 32 333 27 2.31E+12 5.68E+11 139 138 Specimen No. 33 330 18 1.44E+13 3.26E+12 166 165 Specimen No. 34 328 17 1.97E+13 4.42E+12 167 166 Specimen No. 35 328 17 3.75E+13 8.21E+12 177 177 Specimen No. 36 327 16 4.56E+13 9.74E+12 177 178 Specimen No. 37 325 16 7.61E+13 1.59E+13 178 179 Specimen No. 38 326 15 3.53E+13 7.93E+12 168 168 Specimen No. 39 322 16 3.60E+13 8.05E+12 171 172 Specimen No. 40 311 15 3.80E+13 8.31E+12 172 173 Specimen No. 41 308 13 4.29E+13 9.18E+12 172 174 Specimen No. 42 341 24 3.40E+13 7.65E+12 166 166 Specimen No. 43 326 17 3.44E+13 7.73E+12 166 164 Specimen No. 44 322 16 3.40E+13 7.64E+12 164 167 Specimen No. 45 317 15 3.37E+13 7.58E+12 165 168 Specimen No. 46 288 15 3.34E+13 7.52E+12 165 165 Specimen No. 47 328 17 3.61E+13 8.12E+12 171 171 Specimen No. 48 325 16 4.16E+13 9.36E+12 181 180 Specimen No. 49 324 16 4.30E+13 9.68E+12 185 186 Specimen No. 50 322 17 4.24E+13 9.53E+12 184 182 Specimen No. 51 321 15 4.09E+13 9.20E+12 181 180 Specimen No. 52 317 16 3.69E+13 8.29E+12 172 172 Specimen No. 53 327 17 4.10E+13 9.23E+12 186 185 Specimen No. 54 326 18 4.19E+13 9.42E+12 183 183 Specimen No. 55 322 16 4.13E+13 9.28E+12 180 180 Specimen No. 56 320 17 4.11E+13 9.24E+12 182 181 Specimen No. 57 327 16 4.29E+13 9.65E+12 185 185 Specimen No. 58 326 17 4.26E+13 9.57E+12 180 182 Specimen No. 59 325 18 4.33E+13 9.73E+12 186 186 Specimen No. 60 321 17 4.30E+13 9.68E+12 185 186 Specimen No. 61 326 17 2.52E+13 5.67E+12 169 169 Specimen No. 62 324 17 4.31E+13 9.66E+12 184 185 Specimen No. 63 324 23 8.73E+13 1.83E+13 204 205 Specimen No. 64 323 15 4.22E+13 9.48E+12 187 187 Specimen No. 65 320 15 4.29E+13 9.65E+12 187 188 Specimen No. 66 316 19 2.43E+12 5.46E+11 138 136 Specimen No. 67 322 17 8.05E+13 1.72E+13 203 204 Specimen No. 68 304 13 9.48E+13 1.98E+13 208 208 Specimen No. 69 319 18 1.21E+13 2.74E+12 152 152 Specimen No. 70 315 16 1.33E+13 2.98E+12 162 161 Specimen No. 71 318 17 4.08E+13 9.17E+12 176 176 Specimen No. 72 327 17 3.35E+13 7.53E+12 169 169 Specimen No. 73 318 16 6.95E+12 1.57E+12 151 151 Specimen No. 74 316 18 1.08E+13 2.43E+12 162 162

(76) - described in Table 2 indicates unmeasurable.

(77) As presented in Table 2, it was possible to confirm that the multilayer ceramic capacitor specimens in which the amounts of Ba, Ca, and Sr as the main components, that is, s, t, and {1.00(s+t)} respectively satisfy 0.00s1.00, 0.00t1.00, and 0.00s+t1.00 have a high specific permittivity and favorable DC bias characteristics, and have high specific resistance and high voltage resistance at a high temperature of 180 C. or higher.

(78) Particularly, it was possible to confirm that in the multilayer ceramic capacitor specimens in which the amounts of Ba, Ca, and Sr as the main components, that is, s, t, and {1.00(s+t)} respectively satisfy 0.50s1.00, 0.00t0.50, and 0.50s+t1.00, the voltage resistance at 200 C. is higher voltage resistance of 155 V/m or more.

(79) It was possible to confirm that, when the content ratios of Sr, Ba, and Ca in the main components are set to 0s1.00, 0t1.00, and 0s+t1.00 that are the ranges of the present invention as described above, high voltage resistance that is rarely different from the voltage resistance at 180 C. is obtained even at 200 C. Further, it was possible to find that, when s, t, and s+t are controlled to 0.50s1.00, 0.00t0.50, and 0.50s+t1.00, the voltage resistance can be enhanced even at 200 C.

(80) As presented in Table 2, it was possible to confirm that the multilayer ceramic capacitor specimens in which the substitution amount x of R as the main component is 0.00x3.00 have high voltage resistance at 200 C. Meanwhile, in the multilayer ceramic capacitor specimen (No. 16) in which x>3.00 is satisfied, the synthesis of the main component was difficult, and thus a measurable specimen was not obtainable. Therefore, it was possible to confirm that the substitution amount x of the R needs to be 0.00x3.00.

(81) As presented in Table 2, it was possible to confirm that the multilayer ceramic capacitors in which R is at least one element selected from Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu have high voltage resistance at 200 C. In addition, it was possible to confirm that the same effect is obtained by using any elements described above, and further, the same effect is obtained by using a combination of a plurality of elements.

(82) Incidentally, as an example of the combination of a plurality of elements, only the case of using two kinds of elements of La and Sm in Specimen No. 30 is described in the example, but it is confirmed that the same effect is obtained by a combination of three, four, or more kinds of elements.

(83) As presented in Table 2, it is possible to confirm that the multilayer ceramic capacitor specimens in which the substitution amount a of Zr as the main component is 0.01a0.98 have high voltage resistance at 200 C. Of them, it is possible to confirm that Specimen No. 35 to Specimen No. 37 in which the substitution amount a of Zr is set to 0.50a0.98 have higher voltage resistance at 200 C. That is, it was possible to find that, also when the substitution amount a of Zr is strictly controlled, the voltage resistance at 200 C. can be further enhanced. On the other hand, it was possible to confirm that Specimen No. 32 in which a=0 is satisfied does not satisfy the specific resistance at 200 C. and the voltage resistance at 200 C.

(84) As presented in Table 2, it is possible to confirm that, even when Nb is substituted with Ta, the same degree of high voltage resistance as in the case of Nb is obtained at 200 C. as understood from the multilayer ceramic capacitors of Specimen No. 38 to Specimen No. 41 in which Nb as the main component is substituted with Ta. Further, it was found that Specimen No. 39 to Specimen No. 41 in which the substitution amount b of Ta is set to 0.10b1.00 have further higher voltage resistance.

(85) As presented in Table 2, in the multilayer ceramic capacitor specimens in which the substitution amount d of Si is 0.02d0.15, DC bias exhibits a favorable value. It was possible to confirm that, in Specimen No. 46 in which the substitution amount of Si is 0.15<d, the specific permittivity is a low value of less than 300.

(86) As presented in Table 2, it is possible to confirm that the multilayer ceramic capacitor specimens in which the molar quantity of the sub component with respect to 100 mol of the main component is 0.10 molthe sub component20.00 mol have a higher value of specific resistance at 200 C. than Specimen No. 1 not containing a sub component.

(87) As presented in Table 2, it was possible to confirm that Specimen No. 47 to No. 60 of the multilayer ceramic capacitor specimens in which at least one selected from Mn, Mg, Co, V, W, Mo, Li, B, and Al is contained as a sub component have higher specific resistance at 200 C. than Specimen No. 61 only containing Fe that is not the above-described sub component.

(88) Also in Specimen No. 72 to Specimen No. 74 produced using a Ni internal electrode by reductive atmosphere firing, it was possible to confirm that the specific resistance at 200 C. and the voltage resistance at 200 C. exhibit high values.

Comparative Example

(89) In Specimen No. 75 and Specimen No. 76 presented in Table 3, multilayer ceramic capacitors were produced using a tungsten bronze type composite oxide containing an alkali metal element as a main component. The specific manufacturing method will be described below. Incidentally, a specimen marked with in Table 3 is a comparative example.

(90) In Specimen No. 75 and Specimen No. 76, tungsten bronze type composite oxide K(Sr.sub.0.3Ba.sub.0.3Ca.sub.0.4).sub.2Nb.sub.5O.sub.15 powder containing an alkali metal element synthesized in advance was prepared as a main component, and MnCO.sub.3 powder that is a raw material of a sub component to be added to the main component was prepared. Then, K(Sr.sub.0.3Ba.sub.0.3Ca.sub.0.4).sub.2Nb.sub.5O.sub.15 powder as the main component and MnCO.sub.3 powder as the raw material of the sub component were weighed and mixed to have a predetermined ratio of the sub component to 100 mol of the main component, thereby preparing mixed powder.

(91) The mixed powder of the main component and the sub component is used as a dielectric composition raw material.

(92) A paste for a dielectric layer was produced in the similar manner to the example, except that the dielectric composition raw material was used, and a green sheet was formed on a PET film to have a thickness after drying of 7 m. Then, an internal electrode layer was printed with a predetermined pattern on the green sheet using a paste for an internal electrode containing Ni as a main component, and then the sheet was peeled off from the PET film to produce a green sheet having an internal electrode layer. Subsequently, a green chip was obtained using the green sheet similarly to the example.

(93) Then, the obtained green chip was subjected to a binder removal treatment (temperature increase rate: 10 C./hr, retention temperature: 350 C., temperature retention time: 8 hours, atmosphere: in nitrogen) and subjected to firing (temperature increase rate: 200 C./hr, retention temperature: 1100 C., temperature retention time: 2 hours, cooling rate: 200 C./hr, oxygen partial pressure: 10.sup.9 to 10.sup.12 Pa, atmosphere: H.sub.2N.sub.2H.sub.2O mixed gas) to obtain a capacitor element main body.

(94) Both end faces of the obtained capacitor element main body were applied with a Ag paste containing B.sub.2O.sub.3SiO.sub.2BaO-based glass frit and subjected to a baking treatment (temperature: 800 C., atmosphere: N.sub.2 gas) to obtain multilayer ceramic capacitors having the same shape as the multilayer ceramic capacitor illustrated in FIGURE. The sizes of the obtained multilayer ceramic capacitors were all 4.5 mm3.2 mm0.5 mm, the thickness of the dielectric layer was set to 6.0 m, the thickness of the internal electrode layer was set to 1.5 m, and the number of the dielectric layers interposed between the internal electrode layers was set to 5.

(95) As for the obtained multilayer ceramic capacitors of Specimen No. 75 and Specimen No. 76, similarly to the example, the specific permittivity, the specific resistance, and the voltage resistance were measured and the results thereof were presented in Table 3.

(96) TABLE-US-00003 TABLE 3 Accessory component [mol %] 25 C. 180 C. 200 C. 180 C. 200 C. (with respect to 100 mol Specific Specific Specific Voltage Voltage Main of main component) permittivity resistance resistance resistance resistance component composition Mn [] [cm] [cm] [V/m] [V/m] Specimen No. 75 K(Sr.sub.0.3Ba.sub.0.3Ca.sub.0.4).sub.2Nb.sub.5O.sub.15 40.00 1900 6.31E+09 1.51E+09 132 134 Specimen No. 76 K(Sr.sub.0.3Ba.sub.0.3Ca.sub.0.4).sub.2Nb.sub.5O.sub.15 5.00 1900 3.98E+09 9.56E+08 132 133

(97) As presented in Table 3, it is possible to confirm that Specimen No. 75 and Specimen No. 76 that are a tungsten bronze type composite oxide containing an alkali metal element as a main component have low values of the voltage resistance and the specific resistance since a lattice defect caused by the alkali metal element with high volatility easily occurs and the conduction electron is easily generated.

INDUSTRIAL APPLICABILITY

(98) The dielectric composition of the present invention can be applied under the environment close to an engine room as an in-vehicle electronic component since the dielectric composition has high voltage resistance and high specific resistance in a high-temperature region of 200 C., and can be also applied to use application as an electronic component mounted in the vicinity of a power device using a SiC- or GaN-based semiconductor.

EXPLANATIONS OF LETTERS OR NUMERALS

(99) 1 MULTILAYER CERAMIC CAPACITOR 2 DIELECTRIC LAYER 3 INTERNAL ELECTRODE LAYER 4 EXTERNAL ELECTRODE 10 CAPACITOR ELEMENT MAIN BODY