CN102060524A - High dielectric constant ceramic powder, ceramic capacitor and manufacture method thereof - Google Patents
High dielectric constant ceramic powder, ceramic capacitor and manufacture method thereof Download PDFInfo
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- 239000000919 ceramic Substances 0.000 title claims abstract description 32
- 239000000843 powder Substances 0.000 title claims abstract description 29
- 239000003985 ceramic capacitor Substances 0.000 title claims abstract description 13
- 238000000034 method Methods 0.000 title claims description 7
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- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 4
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 4
- 238000005538 encapsulation Methods 0.000 claims description 4
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- 238000005516 engineering process Methods 0.000 abstract description 4
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- 239000003990 capacitor Substances 0.000 description 11
- 229910010293 ceramic material Inorganic materials 0.000 description 11
- 239000000463 material Substances 0.000 description 10
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- 229910002113 barium titanate Inorganic materials 0.000 description 3
- 239000003989 dielectric material Substances 0.000 description 3
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- 238000009413 insulation Methods 0.000 description 3
- 229910052573 porcelain Inorganic materials 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 229910002976 CaZrO3 Inorganic materials 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 229910052788 barium Inorganic materials 0.000 description 2
- 229910021523 barium zirconate Inorganic materials 0.000 description 2
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- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明涉及一种具有2F4特性的、BaTiO3一BaZrO3一CaZrO3体系的高介电常数陶瓷粉料，其包括第一组分BaTiO3、第二组分BaZrO3、第三组分CaZrO3，及选自MnCO3，MnO2，ZnO，Sm2O3，CuO，CeO2中的一种或两种以上作为第四组分。用该粉料制得的圆片陶瓷电容器各项性能指标均符合2F4组别的GB标准，适应了电子产品的小型化技术的发展，介电常数高、符合环保要求。The present invention relates to a high dielectric constant ceramic powder with 2F4 characteristics, BaTiO 3 -BaZrO 3 -CaZrO 3 system, which includes the first component BaTiO 3 , the second component BaZrO 3 , and the third component CaZrO 3 , and one or more selected from MnCO 3 , MnO 2 , ZnO, Sm 2 O 3 , CuO, and CeO 2 as the fourth component. All the performance indexes of the disc ceramic capacitor made from the powder meet the GB standard of 2F4 group, adapt to the development of miniaturization technology of electronic products, have high dielectric constant and meet the requirements of environmental protection.
Description
技术领域technical field
本发明涉及一种高介电常数陶瓷粉料及利用这种高介电常数粉料所制得的圆片陶瓷电容器，特别是涉及具有2F4特性的高介电常数陶瓷粉料及利用这种粉料所制得的圆片陶瓷电容器。The invention relates to a high dielectric constant ceramic powder and a disc ceramic capacitor made by using the high dielectric constant powder, in particular to a high dielectric constant ceramic powder with 2F4 characteristics and a capacitor made by using the high dielectric constant ceramic powder. prepared disc ceramic capacitors.
背景技术Background technique
目前，中高压圆片陶瓷电容器广泛应用于中高压电子线路和电力设备，如彩色电视机、激光器、电力阻断器、微波炉、等电器设备中的电容器，其市场较为广阔。为了适应电子产品的小型化技术的发展，在保证圆片电容器的适用性和高性能的前提下尽可能提高电容器的介电常数，以减小圆片电容器的体积，这对电容器的制造工艺和对原材料的选择提出了较高的要求。目前，国内生产使用的具有2F4特性(所谓2F4特性是指-25℃～+85℃，ε/ε20℃在+22％～-82％)的电子陶瓷粉料主要是采用BaTiO3体系的瓷料，但使用的瓷料最高介电常数小于15000，烧结温度在1320℃以上，耐压特性VDC在5-6kv/mm，VAC在2.5-3kv/mm左右。At present, medium and high voltage wafer ceramic capacitors are widely used in medium and high voltage electronic circuits and power equipment, such as capacitors in color TVs, lasers, power blockers, microwave ovens, and other electrical equipment, and their market is relatively broad. In order to adapt to the development of miniaturization technology of electronic products, the dielectric constant of the capacitor should be increased as much as possible under the premise of ensuring the applicability and high performance of the chip capacitor, so as to reduce the volume of the chip capacitor, which has great influence on the manufacturing process and Higher requirements are placed on the selection of raw materials. At present, the domestic production and use of electronic ceramic powders with 2F4 characteristics (the so-called 2F4 characteristics refer to -25°C ~ +85°C, ε/ε20°C at +22% ~ -82%) mainly use BaTiO 3 ceramic materials , but the highest dielectric constant of the ceramic material used is less than 15000, the sintering temperature is above 1320°C, the withstand voltage characteristic VDC is 5-6kv/mm, and the VAC is about 2.5-3kv/mm.
上述现有技术的缺点是：一是介电常数偏低，电容器稳定性差，耐压特性一般，不能适应元件小型化的特点。二是瓷料烧结温度偏高，一般在1320℃以上烧结，增加了生产成本，原因是：采用的材料与配方的匹配性以及添加物的种类、数量等造成。The disadvantages of the above-mentioned prior art are: firstly, the dielectric constant is relatively low, the stability of the capacitor is poor, the withstand voltage characteristic is average, and it cannot adapt to the characteristics of miniaturization of components. The second is that the sintering temperature of the porcelain material is relatively high, generally above 1320°C, which increases the production cost. The reasons are: the matching of the materials used and the formula, as well as the type and quantity of the additives.
发明内容Contents of the invention
针对上述现有技术的不足，本发明提供了一种高介电常数陶瓷粉料，该高介电常数粉料具有2F4特性。Aiming at the deficiencies of the above-mentioned prior art, the present invention provides a high dielectric constant ceramic powder, which has 2F4 characteristics.
另一方面，本发明还提供了由上述高介电常数陶瓷粉料制造的圆片陶瓷电容器以及制备陶瓷电容器的方法。On the other hand, the present invention also provides a disc ceramic capacitor manufactured from the above-mentioned high dielectric constant ceramic powder and a method for preparing the ceramic capacitor.
一种高介电常数陶瓷粉料，其包括第一组分BaTiO3、第二组分BaZrO3、第三组分CaZrO3，其特征在于：还包括总含量占陶瓷粉料重量百分含量为0.1％～2.0％的第四组分，第四组分选自MnCO3、MnO2、ZnO、Sm2O3、CuO、CeO2、中的一种或两种以上。A high dielectric constant ceramic powder, which includes the first component BaTiO 3 , the second component BaZrO 3 , and the third component CaZrO 3 , characterized in that: it also includes a total content of 0.1%-2.0% of the fourth component, the fourth component is selected from one or more of MnCO 3 , MnO 2 , ZnO, Sm 2 O 3 , CuO, CeO 2 .
进一步来说，所述第一组分BaTiO3占陶瓷粉料重量百分含量的80％～95％，且该组分中Ba∶Ti摩尔比的范围为1∶0.90～1.10；所述第二组分BaZrO3占陶瓷粉料重量百分含量的4.5％～15％，且该组分中Ba∶Zr摩尔比的范围为1∶0.90～1.10；所述第三组分CaZrO3占陶瓷粉料重量百分含量的0.5％～3.0％，且该组分中Ca∶Zr摩尔比的范围为1∶0.90～1.10。Further, the first component BaTiO 3 accounts for 80% to 95% by weight of the ceramic powder, and the range of the Ba:Ti molar ratio in this component is 1:0.90 to 1.10; the second Component BaZrO 3 accounts for 4.5% to 15% of the weight percentage of the ceramic powder, and the range of the Ba:Zr molar ratio in the component is 1:0.90 to 1.10; the third component CaZrO 3 accounts for the ceramic powder 0.5%-3.0% by weight, and the molar ratio of Ca:Zr in the component ranges from 1:0.90-1.10.
具体地来说，所述第一组分BaTiO3是把BaCO3、TiO2按比例球磨混合均匀后，在1150～1250℃煅烧2～5小时后获得；所述第二组分BaZrO3是把BaCO3、ZrO2按比例球磨混合均匀后，在1150～1250℃煅烧2～5小时后获得；所述第三组分CaZrO3是把CaCO3、ZrO2按比例球磨混合均匀后，在1170～1270℃煅烧2～5小时后获得。Specifically, the first component BaTiO 3 is obtained by ball milling and mixing BaCO 3 and TiO 2 uniformly in proportion, and calcining at 1150-1250°C for 2-5 hours; the second component BaZrO 3 is After BaCO 3 and ZrO 2 are evenly mixed by ball milling in proportion, they are obtained after calcining at 1150-1250°C for 2-5 hours; the third component CaZrO 3 is obtained by ball-milling CaCO 3 and ZrO 2 in proportion It is obtained after calcining at 1270°C for 2 to 5 hours.
一种以上述高介电常数陶瓷粉料所制得的陶瓷电容器。A ceramic capacitor made from the above-mentioned high dielectric constant ceramic powder.
一种如上所述的陶瓷电容器的制备方法，包括以下步骤：将所述陶瓷粉料的各组分湿磨均匀，磨细后干燥，进行干压成型、挤压或扎膜成型制得生坯；然后依次进行排胶、烧结、超声波清洗；最后进行分选、印银、还原、测试、包封；所述排胶温度是280～400℃，烧结温度是1250℃～1290℃，烧结时间为1～3小时。A method for preparing a ceramic capacitor as described above, comprising the following steps: wet-grinding each component of the ceramic powder evenly, drying after grinding, and performing dry pressing, extrusion or film forming to obtain a green body ; Then carry out debinding, sintering, ultrasonic cleaning in sequence; finally carry out sorting, silver printing, reduction, testing, encapsulation; the debinding temperature is 280-400°C, the sintering temperature is 1250°C-1290°C, and the sintering time is 1 to 3 hours.
对采用本发明上述陶瓷粉体的圆片电容器产品进行测试，其各项技术指标均符合国标2F4标准，主要特征参数为：The disc capacitor product adopting the above-mentioned ceramic powder of the present invention is tested, and its various technical indicators all meet the national standard 2F4 standard, and the main characteristic parameters are:
介电常数(20℃，1kHz)：17000～20000Dielectric constant (20℃, 1kHz): 17000～20000
介质损耗(20℃，1kHz)：＜80×10-4 Dielectric loss (20°C, 1kHz): <80×10 -4
绝缘性能：＞1010 Insulation performance: >10 10
抗电强度：VDC·＞6.0kv/mm，VAC·＞3.2kv/mmDielectric strength: V DC > 6.0kv/mm, V AC > 3.2kv/mm
温度特性：-25℃～+85℃ IΔε/ε20℃I在+22％～-82％Temperature characteristics: -25℃～+85℃ IΔε/ε20℃I at +22%～-82%
烧结特性Ts：1250℃～1290℃Sintering characteristics Ts: 1250℃～1290℃
从以上可知本发明是BaTiO3一BaZrO3一CaZrO3体系的陶瓷粉料，但由于本发明对所用主要原料组分中的摩尔比进行控制，因而产品的性能随着Ba、Ti、Zr、Ca比例的摩尔比变化而变化，适当的Ba、Ti、Zr、Ca的摩尔比有利于瓷体烧结性能的改善和瓷体介电常数的提高，BaTiO3作为主晶相从低成本和工艺成熟考虑比较有利，而且是一种典型的铁电材料以其为基的铁电材料具有较高的介电常数，现在对BaTiO3的改性多数通过取代置换引起的效应来提高峰值，加入量达到80％～95％范围时，使瓷料有较高的介电常数和耐压，同时又有较低的介质损耗，含量过高则难以在本发明温度下烧结，过低则难以获得较高的介电常数。利用第二组份BaZrO3控制瓷料的居里温度点移动，有利于抑制温度系数的漂移，并且Zr能有效地阻止Ti还原且通过置换取代，起到移峰作用，当加入量大于15％时，会使介电常数直线下降达不到本发明要求，少于4.5％时瓷料恶化出现烧不熟的现象。同时第三组份CaZrO3主要是起到展宽峰值的作用，随着其含量在本发明的范围内可获得优良的ε-T曲线，如果加入量少于0.5％起不到展宽峰值的作用，大于3.0％介电常数受到压制而变得降低。本发明通过加入第四组分来调整瓷料的温度系数和烧结温度，使瓷料的温度特性符合2F4特性。其中ZnO是典型的晶粒成长阻滞剂，它的加入不能移动居里点，但能有效控制晶粒生长速度，有利于促进陶瓷的致密性，达到提高陶瓷介质抗电强度的目的。CuO主要起烧结促进和低温烧结剂的作用，能够减缓粒界的移动，抑制晶粒的二次生长。MnCO3或MnO2的加入起到对瓷料的烧结成色稳定作用，更重要还可以调节居里点，使其介电常数提高。Sm2O3的加入也有效地改善烧结，使瓷体具有均匀的晶格，有助耐电强度提高。CeO2对钛酸钡陶瓷的晶粒生长有较大的抑制作用来减小介电常数温度变化率。当中第四组份的总加入量在0.1％--2.0％较为合适，见表1。所以利用本发明陶瓷粉料制得的电容器介电常数提高到17000＜K＜20000，而且直流(交流)耐压特性也有提高，烧结温度也降低到了约1250℃～1290℃左右。这样，使用本发明瓷料不但适应了电子产品的大容量小型化技术的发展，耐压特性高，而且降低烧结温度，大大节约生产厂家的生产成本。From the above, it can be known that the present invention is BaTiO3 - BaZrO3 - CaZrO3 system ceramic powder, but because the present invention controls the mol ratio in the main raw material components used, the performance of the product varies with Ba, Ti, Zr, Ca The molar ratio of the ratio changes. The appropriate molar ratio of Ba, Ti, Zr, and Ca is beneficial to the improvement of the sintering performance of the porcelain body and the increase of the dielectric constant of the porcelain body. BaTiO 3 as the main crystal phase is considered from low cost and mature technology It is more favorable, and it is a typical ferroelectric material. The ferroelectric material based on it has a high dielectric constant. Now most of the modifications to BaTiO 3 increase the peak value through the effect of substitution and replacement, and the addition amount reaches 80 % to 95%, the ceramic material has a higher dielectric constant and withstand voltage, and at the same time has a lower dielectric loss. If the content is too high, it will be difficult to sinter at the temperature of the present invention, and if it is too low, it will be difficult to obtain a higher dielectric constant. Using the second component BaZrO 3 to control the movement of the Curie temperature point of the ceramic material is beneficial to suppress the drift of the temperature coefficient, and Zr can effectively prevent the reduction of Ti and replace it by replacement, which plays a role in shifting the peak. When the amount added is greater than 15% When it is less than 4.5%, the dielectric constant will drop in a straight line and fail to meet the requirements of the present invention. When it is less than 4.5%, the ceramic material will deteriorate and appear undercooked. Simultaneously the 3rd component CaZrO Mainly play the effect of broadening the peak, along with its content can obtain excellent ε-T curve within the scope of the present invention, if the addition is less than 0.5%, can not reach the effect of broadening the peak, More than 3.0% the dielectric constant is suppressed to become lowered. The invention adjusts the temperature coefficient and sintering temperature of the ceramic material by adding the fourth component, so that the temperature characteristic of the ceramic material conforms to the 2F4 characteristic. Among them, ZnO is a typical grain growth retarder. Its addition cannot move the Curie point, but it can effectively control the grain growth rate, which is conducive to promoting the compactness of ceramics and achieving the purpose of improving the dielectric strength of ceramic dielectrics. CuO mainly plays the role of sintering accelerator and low-temperature sintering agent, which can slow down the movement of grain boundaries and inhibit the secondary growth of grains. The addition of MnCO 3 or MnO 2 plays a role in stabilizing the sintering color of ceramic materials, and more importantly, it can also adjust the Curie point to increase its dielectric constant. The addition of Sm 2 O 3 can also effectively improve the sintering, make the ceramic body have a uniform lattice, and help improve the electric strength. CeO 2 has a greater inhibitory effect on the grain growth of barium titanate ceramics to reduce the temperature change rate of the dielectric constant. Among them, the total addition amount of the fourth component is more suitable at 0.1%--2.0%, see Table 1. Therefore, the dielectric constant of the capacitor prepared by using the ceramic powder of the present invention is increased to 17000<K<20000, and the DC (AC) withstand voltage characteristics are also improved, and the sintering temperature is also reduced to about 1250°C-1290°C. In this way, the use of the ceramic material of the present invention not only adapts to the development of large-capacity miniaturization technology of electronic products, but also has high withstand voltage characteristics, and reduces the sintering temperature, which greatly saves the production cost of the manufacturer.
具体实施方式Detailed ways
下面结合实施例对本发明作进一步的说明，但本发明的范围并不限于如下实施方式。The present invention will be further described below in conjunction with examples, but the scope of the present invention is not limited to the following embodiments.
具体实施方式：Detailed ways:
本发明是采用BaTiO3一BaZrO3一CaZrO3体系，然后通过加入第四组份改性添加剂来调节瓷料的性能、采用常规的工艺制成所需瓷料，得到一种符合2F4瓷介特性、高介电常数的环保型介质材料，下面结合实施例对本发明的内容作进一步详述.The present invention adopts BaTiO3 - BaZrO3 - CaZrO3 system, and then adjusts the performance of the ceramic material by adding the fourth component modification additive, and adopts the conventional process to make the required ceramic material, and obtains a kind of ceramic medium that meets the characteristics of 2F4 , high dielectric constant environment-friendly dielectric material, the content of the present invention will be further described below in conjunction with the examples.
选取电子级的BaCO3、TiO2、ZrO2、CaCO3作为原材料，将BaCO3、TiO2按1∶0.9～1.1(如本例中按1∶1)比例称重，将物料置于球磨机中进行湿式混合均匀，随后在空气中以1150～1250℃的温度锻烧1～3小时，从而获得第一组分BaTiO3。Select electronic-grade BaCO 3 , TiO 2 , ZrO 2 , and CaCO 3 as raw materials, weigh BaCO 3 and TiO 2 at a ratio of 1:0.9 to 1.1 (for example, 1:1 in this example), and place the materials in a ball mill Wet mixing is carried out uniformly, followed by calcining in air at a temperature of 1150-1250° C. for 1-3 hours, so as to obtain the first component BaTiO 3 .
将BaCO3、ZrO2，按1∶0.9～1.1(如本例中按1∶1)比例称重，将物料置于球磨机中进行湿式混合均匀，随后在空气中以1150～1250℃的温度锻烧1～3小时，从而获得第二组分BaZrO3。Weigh BaCO 3 and ZrO 2 at a ratio of 1:0.9 to 1.1 (1:1 in this example), put the materials in a ball mill for wet mixing, and then forge in air at a temperature of 1150 to 1250°C. Burn for 1-3 hours to obtain the second component BaZrO 3 .
将CaCO3、ZrO2按1∶0.9～1.1(如本例中按1∶1)比例称重，将物料置于球磨机中进行湿式混合均匀，随后在空气中以1170～1270℃的温度锻烧1～3小时，从而获得第三组分CaZrO3，得到以上主要组份物料后，再按以下方法制得陶瓷电容器。Weigh CaCO 3 and ZrO 2 at a ratio of 1:0.9 to 1.1 (for example, 1:1 in this example), put the materials in a ball mill for wet mixing, and then calcinate them in air at a temperature of 1170 to 1270°C After 1-3 hours, the third component CaZrO 3 is obtained. After the above main component materials are obtained, ceramic capacitors are produced according to the following method.
1、将第一组分BaTiO3、第二组分BaZrO3、第三组分CaZrO3和MnCO3、MnO2、ZnO、Sm2O3、CuO、CeO2、等粉末按表1配方1-10称重，将称好的物料混合置于球磨机中先初步湿磨，后再入砂磨机中进行磨细，然后按配料重量加入固含量为10％而加入量为10％-20％的PVA胶水溶液及适量的分散剂、消泡剂、脱膜剂等，用造粒干燥机进行干燥造粒，再通过干压成型方法制得生坯，然后经过叠片、1270℃烧结1～3小时、超声波清洗、分选、印银、还原、测试、包封、测试，最后获得可在整机上使用的电容器，测得性能如表2中1-10所示。1. Powder the first component BaTiO 3 , the second component BaZrO 3 , the third component CaZrO 3 and MnCO 3 , MnO 2 , ZnO, Sm 2 O 3 , CuO, CeO 2 , etc. according to Table 1 formula 1- 10 Weighing, mix the weighed materials and place them in a ball mill for initial wet grinding, then put them into a sand mill for grinding, and then add 10% solid content and 10%-20% of the ingredients according to the weight of the ingredients. PVA glue aqueous solution and appropriate amount of dispersant, defoamer, release agent, etc., are dried and granulated with a granulation dryer, and then made into a green body by dry pressing, and then laminated and sintered at 1270°C for 1-3 hours. Hours, ultrasonic cleaning, sorting, silver printing, reduction, testing, encapsulation, testing, and finally a capacitor that can be used on the whole machine is obtained, and the measured performance is shown in 1-10 in Table 2.
使用HP4278A电桥测定在1KHz，1Vrms，20℃的电容量(C)和介电损耗(tanδ)，由C通过计算可得到介电常数(ε)。在20℃和85℃，使用绝缘电阻测定仪，测定样品的绝缘电阻(R)，从而获得C与R的乘积，即CR积。测定以20℃为基准的在-25℃，85℃的电容变化率(ΔC/C20℃)；测定以20℃为基准的在-25℃和85℃的电容变化率(ΔC/C20℃)，以及在-25℃至85℃的温度范围内的电容量的变化最大率(ΔC/Cmax)。各种材料配方及性能实施例如表1、表2所示：Use the HP4278A bridge to measure the capacitance (C) and dielectric loss (tanδ) at 1KHz, 1Vrms, 20°C, and the dielectric constant (ε) can be obtained by calculation from C. At 20°C and 85°C, use an insulation resistance tester to measure the insulation resistance (R) of the sample, so as to obtain the product of C and R, that is, the CR product. Measure the capacitance change rate (ΔC/C20°C) at -25°C and 85°C based on 20°C; measure the capacitance change rate (ΔC/C20°C) at -25°C and 85°C based on 20°C, And the maximum rate of change in capacitance (ΔC/Cmax) in the temperature range from -25°C to 85°C. Various material formulations and performance examples are shown in Table 1 and Table 2:
表1：配方组成 (单位：克)Table 1: Formulation composition (unit: gram)
表2：根据上述陶瓷介质材料制得产品性能参数Table 2: Performance parameters of products made according to the above ceramic dielectric materials
上述的陶瓷电容器是圆片电容器，其制备方法主要是采用干压成型、挤压或扎膜等方法制得生坯，然后经过叠片、烧结、超声波清洗、分选、印银、还原、测试、包封、测试，最后获得可在整机上使用的环保电容器。The ceramic capacitor mentioned above is a wafer capacitor, and its preparation method is mainly to make a green body by dry pressing, extrusion or film binding, and then go through lamination, sintering, ultrasonic cleaning, sorting, silver printing, reduction, and testing. , encapsulation, testing, and finally obtain an environmentally friendly capacitor that can be used on the whole machine.
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| CN106518067A (en) * | 2016-10-27 | 2017-03-22 | 盐城工学院 | Ceramic composition, ceramic as well as preparation method and application of ceramic |
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| CN118271087A (en) * | 2024-05-27 | 2024-07-02 | 济南新峨嵋实业有限公司 | Barium zirconate composite ceramic and preparation method thereof |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105347801A (en) * | 2015-11-20 | 2016-02-24 | 中国计量科学研究院 | Nano ceramic material composition, standard capacitor, and preparation method of nano ceramic material composition and standard capacitor |
| CN105347801B (en) * | 2015-11-20 | 2019-02-22 | 中国计量科学研究院 | A kind of nanometer ceramic material composition and standard capacitor and preparation method thereof |
| CN106518067A (en) * | 2016-10-27 | 2017-03-22 | 盐城工学院 | Ceramic composition, ceramic as well as preparation method and application of ceramic |
| CN108249918A (en) * | 2018-01-19 | 2018-07-06 | 北京元六鸿远电子科技股份有限公司 | Low-temperature sintering huge dielectric constant superfine ceramics material and preparation method and application |
| CN118271087A (en) * | 2024-05-27 | 2024-07-02 | 济南新峨嵋实业有限公司 | Barium zirconate composite ceramic and preparation method thereof |
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