KR0160310B1 - Ceramic composition - Google Patents

Abstract

It is a lead-based perovskite compound that can be sintered at low temperature in the magnetic composition for capacitor production, has a high dielectric constant of more than 10000 at room temperature, low temperature change rate of dielectric constant, small drop in capacity when DC bias is applied, and magnesium niobium acid lead _{[Pb (Mg 1/3 Nb 2/3)} O 3], nickel lead niobate _{[Pb (Ni1 / 3 Nb 2} /3) O 3] and three-component composition composed of lead titanate [PbTiO _3] And a magnetic composition wherein Pb ²⁺ ions are substituted with a required amount of Sr ²⁺ ions, Ba ²⁺ ions or Ca ²⁺ ions.

Description

Porcelain composition

FIG. 1 shows [Pb (Mg _1/3 Nb _2/3 ) O ₃ ] -Pb (Ni _1/3 Nb _2/3 ) O ₃ -PbTiO ₃ showing the allowable composition range of the main component of the magnetic composition of the present invention. Three-component composition diagram.

2 is a graph showing the temperature change rate of permittivity in one embodiment of the magnetic composition according to the present invention, wherein x, y and z are 0.50, 0.30 and 0.20, respectively, and the Sr ²⁺ substitution amount is 0, 10 or 30 mole%. .

3 is a graph showing the capacitance change rate observed when DC bias is applied to a multilayer ceramic capacitor against DC field strength per capacitor (determined from Example 2 and Comparative Example 1).

4 is a graph showing the temperature change rate of dielectric constant in another embodiment of the magnetic composition according to the present invention, wherein x, y and z are 0.50, 0.30 and 0.20, respectively, and Ba ²⁺ substitution amount is 0, 10 or 25 mole%. .

5 is a graph showing the capacity change rate observed when DC bias is applied to a multilayer ceramic capacitor versus DC field strength per capacitor (determined from Example 4 and Comparative Example 2).

FIG. 6 is a graph showing the temperature change rate of permittivity in another embodiment of the magnetic composition according to the present invention, wherein x, y and z are 0.50, 0.30 and 0.20, respectively, and Ca ²⁺ substitution amount is 0, 10 or 25 mole%. .

FIG. 7 is a graph showing the capacitance change rate observed when DC bias is applied to a multilayer ceramic capacitor versus DC field strength per capacitor side (determined from Example 6 and Comparative Example 3).

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a magnetic composition, and more particularly to a magnetic composition having a high dielectric constant and insulation resistance and a low dielectric constant reduction rate upon application of a temperature change of the dielectric constant and a DC bias.

When preparing a multilayer capacitor from the magnetic composition, the magnetic composition should be selected to satisfy the condition that the dielectric constant and resistivity should be as high as possible and the dielectric constant drop due to the temperature change rate of the dielectric constant, dielectric loss and DC bias application should be as low as possible. As the ceramic composition of the conventional high dielectric constant is mainly composed of barium titanate (BaTiO ₃₎ well-known and has been already put to practical use. However, this requires a high sintering temperature.

Therefore, the calcium titanate (CaTiO ₃₎ and lead titanate (PbTiO ₃₎ the additive is entered, such as, but the sintering temperature is still above about 1300 ° to improve the temperature characteristics. For this reason, when a magnetic composition consisting mainly of barium titanate is used to produce a multilayer ceramic capacitor, the material for its internal electrodes is of particular expensive such as precious metals (e.g. platinum, palladium) that can withstand such high sintering temperatures. It is limited to metal. In addition, the dielectric constant obtained by such a dielectric ceramic composition is about 8000 at most. The dielectric constant can be increased, but the temperature change rate is impaired. In particular, these magnetic compositions only meet the Y5V properties (-30 to 85 ° C; + 22%, -82%) as defined in the EIA standard.

Although a magnetic composition having a small temperature change rate can be obtained with a conventional material, the dielectric constant of the obtained magnetic composition is too low to be used as a capacitor material (about 2000).

As mentioned above, in order to reduce the manufacturing cost of multilayer ceramic capacitors, it is necessary to develop a magnetic composition that can be sintered at a low temperature of less than 1150 ° C., which is a cheaper capacitor internal electrode material such as mainly composed of silver or nickel. To use. Recently, various lead-based composite perovskite compounds sintered at low temperatures and high in dielectric constant have been reported. For example, magnesium niobate lead [Pb (Mg _1/3 Nb _2/3 ) O ₃ ], nickel niobate lead [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] and lead titanate [PbTiO ₃ ] The three-component composition consisting of a dielectric constant of 10000 or more can be obtained at room temperature (see US Pat. No. 4,712,156). However, these three-component compositions have the drawback that their dielectric constant is greatly influenced by temperature. Moreover, its capacity is greatly reduced upon application of DC bias, and the resulting capacitor is greatly limited in practical use.

Accordingly, an object of the present invention is to provide a magnetic composition having the above three component system, having a high dielectric constant of 10000 or more, an improved temperature change rate, and a low dielectric constant drop upon application of DC bias.

These and other objects and features of the present invention will become apparent from the following description.

According to the invention, magnesium niobate [Pb (Mg _1/3 Nb _2/3 ) O ₃ ], nickel niobate lead [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] and lead titanate [PbTiO ₃ ] Is a three-component composition consisting of [Pb (M g _1/3 Nb _2/3 ) O ₃ ] x [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] y [PbTiO ₃ ] z (where x + When expressed by y + z = 1.0), in this three-component composition diagram, the following composition points

(x = 0.10, y = 0.70, z = 0.20) ... (a)

(x = 0.10, y = 0.475, z = 0.425) ... (b)

(x = 0.625, y = 0.05, z = 0.325) ... (c)

(x = 0.75, y = 0.05, z = 0.20) ... (d)

(x = 0.75, y = 0.15, z = 0.10) ... (e)

(x = 0.50, y = 0.40, z = 0.10) ... (f)

(x = 0.15, y = 0.70, z = 0.15) ... (g)

And a main component composition in the compositional range enclosed by each of the points and surrounded by the seven points (a) to (g), wherein lead ions (Pb ²⁺ ) contain 0.01 to 30 mole% of strontium ions (Sr). ²⁺ ), 0.01-25 mole% of barium ions (Ba ²⁺ ) or 0.01-25 mole% of calcium ions (Ca ²⁺ ) are provided.

_Three components of [Pb (Mg _1/3 Nb _2/3 ) O ₃ ] -Pb (Ni _1/3 Nb _2/3 ) O ₃ -PbTiO ₃ system showing the composition range of the main component composition of the magnetic composition of the present invention The composition diagram is shown in FIG.

In Fig. 1, (a) to (g) are coordinates of a three component compositional diagram, and an allowable composition range is shown by hatched portions in each drawing having a boundary line.

In the magnetic composition of the present invention, the amount of Sr ²⁺ ions substituted with Pb ²⁺ ions of the main component is in the range of 0.01 to 30 mole%, preferably 2 to 20 mole%, and the amount of Ba ²⁺ ions. The amount is 0.01 to 25 mole%, preferably 2 to 20 mole%, and the amount of Ca ²⁺ ions is 0.01 to 25 mole%, preferably 2 to 20 mole%.

Hereinafter, the present invention will be described in more detail with reference to the following non-limiting examples, and the effects actually obtained by the present invention will also be described in comparison with the comparative examples.

Example 1

Lead oxide (Pb)), magnesium oxide (MgO), niobium oxide (Nb ₂ O ₅ ), nickel oxide (NiO), titanium oxide (TiO ₂ ) and strontium carbonate (SrCO ₃ ) were used as starting materials, Each weight is measured so as to have a compounding ratio shown in Tables 1 to 3.

The weighed starting material is wet mixed in a ball mill and calcined at 800 to 850 ° C., the powder is pulverized in a ball mill, filtered and dried, and then placed in an organic binder, sizing and pressed approximately. A cylindrical sample having a diameter of 16 mm and a thickness of approximately 10 mm, and two disc shaped samples having a diameter of approximately 16 mm and a thickness of approximately 2 mm were produced. The former was used for the subsequent sinter density determination.

The pressed disc sample is then subjected to firing for 1 hour at a temperature of 1100 to 1150 ℃. A silver electrode is printed on both sides of the fired disc sample at 600 ° C., and its dielectric loss and capacity are obtained by measuring its capacity and dielectric loss at a frequency of 1 Hz, a voltage of 1 V r.m.s., at room temperature with a digital LCR meter. In addition, the specific resistance of each sample is obtained by measuring the current when applying a DC voltage of 50V to the sample with an insulation resistance tester.

The dielectric constant is obtained from the obtained capacity. In addition, the capacities at −30 ° C. and 85 ° C. were obtained to determine the temperature change rate of permittivity as a comparative value compared to that observed at 20 ° C.

Tables 1 to 3 show the main components [Pb (Mg _1/3 Nb _2/3 ) O ₃ ] x [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] y [PbTiO ₃ ] z of the magnetic composition thus obtained. The compounding ratios x, y, z and the amounts of Sr ²⁺ ions substituted with Pb ₂₊ ions of the main component are shown, and Tables 4 to 6 show dielectric constants, dielectric losses and specific resistances at room temperature, and are obtained at -30 ° C and 85 ° C. The rate of change of the permittivity (relative to the permittivity at 20 ° C.) is shown.

In these tables, an asterisk (*) means that the compounding ratio of the main component of the sample is outside the scope of the present invention, and double asterisk (**) means that the amount of Sr ²⁺ substitution is outside the range defined in the present invention.

Also Sr To clarify the substitution effect, FIG. 2 shows the compounding ratio (x, y, z) as (0.50, 0.30, 0.20) and Sr. The temperature change rate of dielectric constant of the magnetic composition whose substitution amount is 0, 10, or 30 mole% is shown.

As you can see from the data in Figure 2, Sr The effect of suppressing the dielectric constant due to the substitution can be seen, so that the Curie point of the principal component is shifted towards the lower temperature. In addition, as can be seen from the data of Tables 1 to 6, Pb as the main component in the [Pb (MgNb) O]-[Pb (NiNb) O]-[PbTiO] three-component composition Ion Sr The composition of the present invention, which is substituted with ions, has a high permittivity and resistivity at room temperature and a low temperature change rate of the permittivity, and thus has the Y5U properties (-30 to 85 ° C .; + 22%, -56%) defined in the EIA standard. Can be satisfied. In addition, the magnetic composition of the present invention can be sintered at a relatively low temperature of 1150 DEG C or lower, so that a silver palladium alloy can be used as the internal electrode material of the multilayer ceramic capacitor.

Example 2

Lead oxide, magnesium oxide, titanium oxide, and oxidation so that the compounding ratio (x, y, z) of the main component [Pb (MgNb) O] x [Pb (NiNb) O] y [PbTiO] z is (0.50, 0.30, 0.20) Nickel, niobium oxide and strontium carbonate are correctly distributed and 10 mole% Pb Ion Sr The same procedure as used in Example 1 is repeated except that it is substituted with ions to form a dielectric powder.

The dielectric powder thus obtained is dispersed in an organic solvent and kneaded with an organic binder to form a slurry. The slurry thus obtained is formed into a film having a thickness of 40 μm in accordance with the doctor blade technique used these days. After that, an internal electrode paste is printed on the film according to a conventional screen printing method, and then stamping out, lamination, and heat press are applied to form a laminate, and then cut into pieces of a required shape to obtain a green chip for a capacitor. do. The green chip thus obtained is heated to the required temperature so as to remove the binder and fired, and then a silver paste is applied thereto to form an external electrode.

The capacitor has a frequency of 1 kHz and a voltage of 1 V r.m.s. using a digital LCR meter while a DC bias of 0 to 50 V is applied to the multilayer ceramic capacitor by a digital multimeter. Phosphorous alternating current is applied to obtain at room temperature. The result thus obtained is shown in FIG.

Comparative Example 1

The compounding ratio (x, y, z) of the main component [Pb (MgNb) O] x [Pb (NiNb) O] y [PbTiO] z is (0.20, 0.60, 0.20) and Sr The same procedure as used in Example 3 was repeated except that a composition without substitution was used to produce a capacitor, and its capacity upon application of DC bias was determined in the same manner as in Example 2. The results thus obtained are shown in FIG. 2 together with the results obtained in Example 2. FIG.

The result shown in FIG. 3 shows the Pb of the principal component. Ion Sr The capacitor obtained from the magnetic composition of the present invention substituted with ions is Sr It clearly shows that the DC bias characteristic is superior to the capacitor obtained using the composition of Comparative Example 1 without substitution.

Example 3

As a starting material, lead ratio (PbO), magnesium oxide (MgO), niobium oxide (NbO), nickel oxide (NiO), titanium oxide (TiO) and barium carbonate (BaCO) were used, and the compounding ratios shown in Tables 7 to 9 were used. Measure each weight so that

The weighed starting material was wet mixed in a ball mill and calcined at 800 to 850 ° C., and the powder was crushed in a ball mill, filtered and dried, and then placed in an organic binder, pressed and pressed to approximately 16 mm in diameter. A cylindrical sample having a thickness of 10 mm and two disc shaped samples having a diameter of approximately 16 mm and a thickness of approximately 2 mm were produced. The former was used for the subsequent sinter density determination.

The pressed disc sample is then subjected to firing for 1 hour at a temperature of 1100 to 1150 ℃. Silver electrodes are printed on both sides of the calcined disc sample at 600 ° C. and their capacity and dielectric loss are measured at a frequency of 1 Hz, voltage of 1 V r.m.s., at room temperature with a digital LCR meter. In addition, the specific resistance of each sample is obtained by measuring a current when applying a DC voltage of 50V to the sample with an insulation resistance tester. The dielectric constant is obtained from the obtained capacity. In addition, the capacities at −30 ° C. and 85 ° C. were obtained, and the temperature change rate of the dielectric constant as a comparative value with respect to that observed at 20 ° C. was obtained.

Tables 7 to 9 show the compounding ratios x, y and z, Ba of the main component [Pb (MgNb) O] x [Pb (NiNb) O] y [PbTiO] z of the magnetic composition thus obtained. The substitution amount (mole%) is shown, and Tables 10 to 12 show the permittivity at room temperature, the dielectric loss, the resistivity, and the permittivity (for permittivity at 20 ° C.) in this example obtained at −30 ° C. and 85 ° C. The rate of change is shown.

In the above table, an asterisk (*) means that the compounding ratio of the main component of the sample is outside the range defined in the present invention, and double asterisk (**) is Ba Substitution amount means outside the range defined by this invention.

Also Ba In order to clarify the substitution effect, FIG. 4 shows the compounding ratio (x, y, z) as (0.50, 0.30, 0.20) and Ba. The temperature change rate of dielectric constant of the magnetic composition whose substitution amount is 0, 10, or 25 mole% is shown.

As can be seen from the data of Fig. 4, the effect of suppressing the dielectric constant due to Ba substitution can be seen, so that the Curie point of the main component is shifted toward the lower temperature. In addition, as can be seen from the data of Tables 7 to 12, Pb as the main component in the [Pb (MgNb) O]-[Pb (NiNb) O]-[PbTiO] three-component composition Ion Ba The composition of the present invention, which is substituted with ions, has a high permittivity and resistivity at room temperature and a low temperature change rate of the permittivity, and thus has the Y5U properties (-30 to 85 ° C .; + 22%, -56%) defined in the EIA standard. Can be satisfied. In addition, the magnetic composition of the present invention can be sintered at a relatively low temperature of 1150 DEG C or lower, so that a silver palladium alloy can be used as the internal electrode material of the multilayer ceramic capacitor.

Example 4

Lead oxide, magnesium oxide, titanium oxide, and oxidation so that the compounding ratio (x, y, z) of the main component [Pb (MgNb) O] x [Pb (NiNb) O] y [PbTiO] z is (0.50, 0.30, 0.20) Nickel, niobium oxide and barium carbonate are accurately weighed and 10 mole% Pb Ion Ba The same procedure as used in Example 3 is repeated except that it is substituted with ions to form a dielectric powder.

The dielectric powder thus obtained is dispersed in an organic solvent and kneaded with an organic binder to form a slurry. The slurry thus obtained is formed into a film having a thickness of 40 mu m in accordance with the doctor blade technique used these days. After that, an internal electrode paste is printed on the film according to a conventional screen printing method, and then stamping out, lamination, and heat press are applied to form a laminate, and then cut into pieces of a required shape to obtain a green chip for a capacitor. do. The green chip thus obtained is heated to the required temperature so as to remove the binder and fired, and then a silver paste is applied thereto to form an external electrode.

The capacitor has a frequency of 1 kHz and a voltage of 1 V r.m.s. using a digital LCR meter while a DC bias of 0 to 50 V is applied to the multilayer ceramic capacitor by the digital multimeter. It is obtained at room temperature by applying phosphorus alternating current. The results thus obtained are shown in FIG.

Comparative Example 2

Main ingredient [Pb (Mg The blending ratio (x, y, z) of Nb) O] x [Pb (NiNb) O] y [PbTiO] z is (0.20, 0.60, 0.20) and Ba The same procedure as used in Example 4 was repeated except that a composition without substitution was used to make a capacitor, and its capacity upon application of DC bias was determined in the same manner as in Example 4. The results thus obtained are shown in FIG. 5 together with the results obtained in Example 4. FIG.

The result shown in FIG. 5 shows the Pb of the main component. Ion Ba The capacitor obtained from the magnetic composition of the present invention substituted with ions is Ba It clearly shows that the action is better at the time of DC bias application than the capacitor obtained using the composition of Comparative Example 2 without substitution.

Example 5

In this embodiment, lead oxide (PbO), magnesium oxide (MgO), niobium oxide (NbO), nickel oxide (NiO), titanium oxide (TiO) and calcium carbonate (CaCO) were used as starting materials. The weight is measured so as to have the compounding ratio shown in FIGS.

The weighed starting material was wet mixed in a ball mill and calcined at 800 to 850 ° C., and the powder was crushed in a ball mill, filtered and dried, and then placed in an organic binder, pressed and pressed to approximately 16 mm in diameter. A cylindrical sample having a thickness of 10 mm and two disc shaped samples having a diameter of approximately 16 mm and a thickness of approximately 2 mm were produced. The former is used for subsequent sinter density determination.

The pressed disc sample is then subjected to firing for 1 hour at a temperature of 1100 to 1150 ℃. Silver electrodes are printed on both sides of the calcined disc sample at 600 ° C. and their capacity and dielectric loss are measured at a frequency of 1 Hz, voltage of 1 V r.m.s., at room temperature with a digital LCR meter. In addition, the specific resistance of each sample is obtained by measuring a current when applying a DC voltage of 50V to the sample with an insulation resistance tester. The dielectric constant is obtained from the obtained capacity. In addition, the capacities at −30 ° C. and 85 ° C. were obtained, and the temperature change rate of the dielectric constant as a comparative value with respect to that observed at 20 ° C. was obtained.

Tables 13 to 15 show the compounding ratios x, y and z, Ca of the main component [Pb (MgNb) O] x [Pb (NiNb) O] y [PbTiO] z of the magnetic composition thus obtained. The substitution amount (mole%) is shown, and Tables 16 to 18 show the permittivity at room temperature, the dielectric loss, the specific resistance, and the rate of change (relative to the permittivity at 20 ° C) of the permittivity obtained at -30 ° C and 85 ° C.

In these tables, an asterisk (*) means that the compounding ratio of the main component of the sample is outside the range defined in the present invention, and double asterisk (**) is Ca Substitution amount means outside the range defined by this invention.

Also, to clarify the Ca substitution effect, FIG. 6 shows that the compounding ratio (x, y, z) is (0.50, 0.30, 0.20) and Ca The temperature change rate of dielectric constant of the magnetic composition whose substitution amount is 0, 10, or 25 mole% is shown.

As can be seen from the data of FIG. The effect of suppressing the dielectric constant due to the substitution can be seen, so that the Curie point of the principal component is shifted towards the lower temperature. In addition, as can be seen from the data of Tables 13 to 18, Pb as the main component in the [Pb (MgNb) O]-[Pb (NiNb) O]-[PbTiO] three-component composition Ion Ca The composition of the present invention, which is substituted with ions, has a high permittivity and resistivity at room temperature and a low temperature change rate of the permittivity, and thus has the Y5U properties (-30 to 85 ° C .; + 22%, -56%) defined in the EIA standard. Can be satisfied. In addition, the magnetic composition of the present invention can be sintered at a relatively low temperature of 1150 DEG C or lower, so that a silver palladium alloy can be used as the internal electrode material of the multilayer ceramic capacitor.

Example 6

Lead oxide, magnesium oxide, titanium oxide, and oxidation so that the compounding ratio (x, y, z) of the main component [Pb (MgNb) O] x [Pb (NiNb) O] y [PbTiO] z is (0.50, 0.30, 0.20) Nickel, niobium oxide and calcium carbonate are accurately weighed and 10 mole% Pb Ion Ca Except for the substitution with ions, the same process as used in Example 5 is repeated to form the dielectric powder.

The dielectric powder thus obtained is dispersed in an organic solvent and kneaded with an organic binder to form a slurry. The slurry thus obtained is formed into a film having a thickness of 40 mu m in accordance with the doctor blade technique used these days. After that, an internal electrode paste is printed on the film according to a conventional screen printing method, and then stamping out, lamination, and heat press are applied to form a laminate, and then cut into pieces of a required shape to obtain a green chip for a capacitor. do. The green chip thus obtained is heated to the required temperature so as to remove the binder and fired, and then a silver paste is applied thereto to form an external electrode.

The capacitor has a frequency of 1 kHz and a voltage of 1 V r.m.s. using a digital LCR meter while a DC bias of 0 to 50 V is applied to the multilayer ceramic capacitor by the digital multimeter. It is obtained at room temperature by applying phosphorus alternating current. The result thus obtained is shown in FIG.

Comparative Example 3

Main ingredient [Pb (Mg The compounding ratio (x, y, z) of Nb) O] x [Pb (NiNb) O] y [PbTiO] z is (0.20, 0.60, 0.20) and Ca The same procedure as used in Example 6 was repeated except that a composition without substitution was used to produce a capacitor, and its capacity upon application of DC bias was determined in the same manner as in Example 6. The results thus obtained are shown in FIG. 7 together with the results obtained in Example 6. FIG.

The result shown in FIG. 7 shows the Pb of the main component. Ion Ca The capacitor obtained from the magnetic composition of the present invention substituted with ions is Ca It clearly shows that the DC bias characteristics are superior to the capacitor obtained using the composition of Comparative Example 3 without substitution.

Incidentally, the Curie point of the magnetic composition whose compounding ratio of the main component is outside the range defined in the present invention is shifted from room temperature to a temperature higher or lower than room temperature, and thus such a composition has a very low dielectric constant at room temperature and is within the actual temperature range. There is a problem that the temperature change rate of the dielectric constant at is high and its resistivity is low. Also Sr , Ba Or Ca If the amount of substitution is outside the respective ranges defined in the present invention, the resulting composition cannot be used as a material for producing a capacitor because there is a problem that the capacity is too small and the Curie point is out of room temperature.

The magnetic composition of the present invention has a high dielectric constant at room temperature and a low temperature change rate of the dielectric constant, which is Pb of the main component. Ions of Sr Or Ca This is possible because the Curie point of the main component moves toward the lower temperature and the rate of change of the dielectric constant is suppressed by substitution with ions. In addition, when the DC composition is applied to the magnetic composition of the present invention, the capacity is reduced and the specific resistance is Pb. It is larger than when ions are not substituted. Accordingly, the magnetic composition may provide a multilayer ceramic capacitor having excellent temperature change rate of dielectric constant and high reliability. Its firing temperature is also below 1150 [deg.] C., which allows the use of silver-palladium alloy as the electrode material inside the capacitor. Similarly, as described above, the composition can be used in a multilayer ceramic capacitor such as a switching power supply used during DC bias application because the capacity reduction during DC bias application is relatively small.

Claims (6)

_{Three components} consisting of magnesium lead niobate [Pb (Mg _1/3 Nb _2/3 ) O ₃ ], nickel lead niobate [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] and lead titanate [PbTiO ₃ ] The composition was prepared in [Pb (Mg _1/3 Nb _2/3 ) O ₃ ] x [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] y [PbTiO ₃ ] z (where x + y + z = 1.0 When expressed by), in this three-component composition diagram, the following composition points (x = 0.10, y = 0.70, z = 0.20) ... (a) (x = 0.10, y = 0.475, z = 0.425) ... (b) (x = 0.625, y = 0.05, z = 0.325) ... (c) (x = 0.75, y = 0.05, z = 0.20) ... (d) (x = 0.75, y = 0.15, z = 0.10) ... (e) (x = 0.50, y = 0.40, z = 0.10) ... (f) (x = 0.15, y = 0.70, z = 0.15) ... (g) A main component material in the form of a line connecting each point of and in the composition range surrounded by the seven points (a) to (g), wherein Pb ²⁺ ions are 0.01-30 mole% of strontium ions (Sr ²⁺ ). Magnetic composition, characterized in that by replacing with. The magnetic composition of claim 1, wherein the Sr ²⁺ substitution amount is 2 to 20 mole%. _{Three components} consisting of magnesium lead niobate [Pb (Mg _1/3 Nb _2/3 ) O ₃ ], nickel lead niobate [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] and lead titanate [PbTiO ₃ ] The composition was prepared in [Pb (Mg _1/3 Nb _2/3 ) O ₃ ] x [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] y [PbTiO ₃ ] z (where x + y + z = 1.0 When expressed by), in this three-component composition diagram, the following composition points (x = 0.10, y = 0.70, z = 0.20) ... (a) (x = 0.10, y = 0.475, z = 0.425) ... (b) (x = 0.625, y = 0.05, z = 0.325) ... (c) (x = 0.75, y = 0.05, z = 0.20) ... (d) (x = 0.75, y = 0.15, z = 0.10) ... (e) (x = 0.50, y = 0.40, z = 0.10) ... (f) (x = 0.15, y = 0.70, z = 0.15) ... (g) A main component material in the form of a line connecting each point of and in the composition range surrounded by the seven points (a) to (g), wherein Pb ²⁺ ions are converted to 0.01 to 25 mole% of barium ions (Ba ²⁺ ). A magnetic composition comprising a substitution. The magnetic composition of claim 3, wherein the Ba ²⁺ substitution amount is 2 to 20 mole%. Magnesium Lead Niobate [Pb (Mg _1/3 Nb _2/3 ) O ₃ ] Nickel Lead Niobate [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] and Lead Titanate [PbTiO ₃ ] Is [Pb (Mg _1/3 Nb _2/3 ) O ₃ ] x [Pb (Ni _1/3 Nb _2/3 ) O ₃ ] y [PbTiO ₃ ] z (where x + y + z = 1.0) When expressed by, in this three-component composition diagram, the following composition points (x = 0.10, y = 0.70, z = 0.20) ... (a) (x = 0.10, y = 0.475, z = 0.425) ... (b) (x = 0.625, y = 0.05, z = 0.325) ... (c) (x = 0.75, y = 0.05, z = 0.20) ... (d) (x = 0.75, y = 0.15, z = 0.10) ... (e) (x = 0.50, y = 0.40, z = 0.10) ... (f) (x = 0.15, y = 0.70, z = 0.15) ... (g) A main component material in the form of a line connecting each point of and in the composition range surrounded by the seven points (a) to (g), wherein Pb ²⁺ ions are 0.01 to 25 mole% calcium ions (Ca ²⁺ ) Magnetic composition, characterized in that by replacing with. The magnetic composition of claim 5, wherein the Ca ²⁺ substitution amount is 2 to 20 mole%.