CN106588010A - 一种宽温稳定型陶瓷介质材料及其制备方法 - Google Patents

一种宽温稳定型陶瓷介质材料及其制备方法 Download PDF

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CN106588010A
CN106588010A CN201611253575.XA CN201611253575A CN106588010A CN 106588010 A CN106588010 A CN 106588010A CN 201611253575 A CN201611253575 A CN 201611253575A CN 106588010 A CN106588010 A CN 106588010A
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佘延英
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Abstract

本发明公开一种宽温稳定型陶瓷介质材料及其制备方法,所述的介质材料是由以下质量百分比的原料组成:SrNb2O6:35‑58wt%,BaTa2O6:22‑32wt%,CaZrO3:15‑21wt%,Dy2O3:3‑11wt%,MgO:0.3‑0.9wt%,Ag2O:0.1‑0.4wt%。所述的制备方法包括将SrNb2O6等原料按摩尔比进行配料混合后按质量比加入MgO和Ag2O混合物充分搅拌,通过球磨、烘干后预烧,然后进行造粒并烧结,即得。本发明提供的电容器介质材料具有优良的温度稳定性好,有效的增大了储能应用面积,具有良好的节能环保效应和广阔的应用前景。

Description

一种宽温稳定型陶瓷介质材料及其制备方法
技术领域
本发明涉及电容器材料技术领域,具体涉及一种宽温稳定型陶瓷介质材料及其制备方法。
背景技术
在高速发展的当今社会,人们对能源的需求日渐增多,而日益消耗的不可再生能源给整个人类的生存环境带来了巨大的压力,因此寻求并使用清洁能源便成为了环境对人类提出的新课题。近年来,随着科学技术的不断发展,太阳能、风能、热能以及核能都逐步被开发和使用,使得传统能源的占比显著降低。而另一方面,在新能源进行开发和挖掘的同时,能源的有效储存也随之成为了又一研究方向。
在能源转化过程中,可以通过将不同形式的能源转换为电能进行储存,这就意味着储能介质材料对环境的适应能力尤为重要。因此,如何增加介质材料的储能应用面积已达到最大程度的电能储存效率成为了当下亟待解决的问题。
发明内容
针对现有技术的不足,本发明提供了一种宽温稳定型陶瓷介质材料及其制备方法。
为实现上述目的,本发明通过以下技术方案实现:
一种宽温稳定型陶瓷介质材料,由以下质量百分比的原料组成:SrNb2O6:35-58wt%,BaTa2O6:22-32wt%,CaZrO3:15-21wt%,Dy2O3:3-11wt%,MgO:0.3-0.9wt%,Ag2O:0.1-0.4wt%。
优选的,由以下质量百分比的原料组成:SrNb2O6:48wt%,BaTa2O6:29wt%,CaZrO3:19wt%,Dy2O3:3wt%,MgO:0.8wt%,Ag2O:0.2wt%。
所述宽温稳定型陶瓷介质材料的制备步骤如下:
1)将SrNb2O6、BaTa2O6、CaZrO3和Dy2O3作为起始原料按质量百分比进行配料,混合后按质量百分比加入MgO和Ag2O混合物充分搅拌,并加入无水乙醇混合球磨24小时,烘干得到粉末A;
2)将步骤1)中制得的粉末A放入马弗炉中,升温至1050~1200℃预烧4-10小时得到前驱体B;
3)将步骤2)中制得的前驱体B研碎后加入无水乙醇,球磨8-15小时混合均匀,烘干得到粉末C;
4)向步骤3)中制得的粉末C中加入5wt%聚乙烯醇水溶液造粒,过60目筛后压制成型,放入高温炉中升温至1250~1400℃烧结8-12小时后自然冷却至室温,即得。
优选的,所述步骤2)中预烧温度为1180℃,时间为4小时。
优选的,所述步骤3)中球磨时间为12小时。
优选的,所述步骤4)中烧结温度为1300℃,时间为10小时。
本发明有益效果:本发明提供了一种宽温稳定型陶瓷介质材料及其制备方法,原料各组分混合性较好,通过高温固相合成工艺,得到电介质材料在-50-200℃温度范围内具有优良的温度稳定性,均满足电容变化率ΔC/C25≤±15%,有效的增加了电容器的工作范围,使其在多种温度情况下仍然可以发挥储能作用,有效的增大了储能应用面积,具有良好的节能环保效应。本发明提供的电容器介质材料及其制备方法,具有广阔的应用前景。
具体实施方式
实施例1:
一种宽温稳定型陶瓷介质材料,由以下质量百分比的原料组成:SrNb2O6:48wt%,BaTa2O6:29wt%,CaZrO3:19wt%,Dy2O3:3wt%,MgO:0.8wt%,Ag2O:0.2wt%。
制备步骤如下:
1)将SrNb2O6、BaTa2O6、CaZrO3和Dy2O3作为起始原料按质量百分比进行配料,混合后按质量百分比加入MgO和Ag2O混合物充分搅拌,并加入无水乙醇混合球磨24小时,烘干得到粉末A;
2)将步骤1)中制得的粉末A放入马弗炉中,升温至1180℃预烧4小时得到前驱体B;
3)将步骤2)中制得的前驱体B研碎后加入无水乙醇,球磨12小时混合均匀,烘干得到粉末C;
4)向步骤3)中制得的粉末C中加入5wt%聚乙烯醇水溶液造粒,过60目筛后压制成型,放入高温炉中升温至1300℃烧结10小时后自然冷却至室温,即得。
实施例2:
一种宽温稳定型陶瓷介质材料,由以下质量百分比的原料组成:SrNb2O6:35wt%,BaTa2O6:32wt%,CaZrO3:21wt%,Dy2O3:11wt%,MgO:0.6wt%,Ag2O:0.4wt%。
制备步骤如下:
1)将SrNb2O6、BaTa2O6、CaZrO3和Dy2O3作为起始原料按质量百分比进行配料,混合后按质量百分比加入MgO和Ag2O混合物充分搅拌,并加入无水乙醇混合球磨24小时,烘干得到粉末A;
2)将步骤1)中制得的粉末A放入马弗炉中,升温至1200℃预烧6小时得到前驱体B;
3)将步骤2)中制得的前驱体B研碎后加入无水乙醇,球磨8小时混合均匀,烘干得到粉末C;
4)向步骤3)中制得的粉末C中加入5wt%聚乙烯醇水溶液造粒,过60目筛后压制成型,放入高温炉中升温至1250℃烧结12小时后自然冷却至室温,即得。
实施例3:
一种宽温稳定型陶瓷介质材料,由以下质量百分比的原料组成:SrNb2O6:58wt%,BaTa2O6:22wt%,CaZrO3:15wt%,Dy2O3:4wt%,MgO:0.9wt%,Ag2O:0.1wt%。
制备步骤如下:
1)将SrNb2O6、BaTa2O6、CaZrO3和Dy2O3作为起始原料按质量百分比进行配料,混合后按质量百分比加入MgO和Ag2O混合物充分搅拌,并加入无水乙醇混合球磨24小时,烘干得到粉末A;
2)将步骤1)中制得的粉末A放入马弗炉中,升温至1100℃预烧8小时得到前驱体B;
3)将步骤2)中制得的前驱体B研碎后加入无水乙醇,球磨9小时混合均匀,烘干得到粉末C;
4)向步骤3)中制得的粉末C中加入5wt%聚乙烯醇水溶液造粒,过60目筛后压制成型,放入高温炉中升温至1400℃烧结8小时后自然冷却至室温,即得。
实施例4:
一种宽温稳定型陶瓷介质材料,由以下质量百分比的原料组成:SrNb2O6:45wt%,BaTa2O6:26wt%,CaZrO3:21wt%,Dy2O3:7wt%,MgO:0.7wt%,Ag2O:0.3wt%。
制备步骤如下:
1)将SrNb2O6、BaTa2O6、CaZrO3和Dy2O3作为起始原料按质量百分比进行配料,混合后按质量百分比加入MgO和Ag2O混合物充分搅拌,并加入无水乙醇混合球磨24小时,烘干得到粉末A;
2)将步骤1)中制得的粉末A放入马弗炉中,升温至1050℃预烧10小时得到前驱体B;
3)将步骤2)中制得的前驱体B研碎后加入无水乙醇,球磨10小时混合均匀,烘干得到粉末C;
4)向步骤3)中制得的粉末C中加入5wt%聚乙烯醇水溶液造粒,过60目筛后压制成型,放入高温炉中升温至1350℃烧结9小时后自然冷却至室温,即得。
通过将以上实施例分别合成的电介质材料在-50-200℃内进行介电性能测试,测试结果如表1:
表1
当然,上面只是本发明优选的具体实施方式作了详细描述,并非以此限制本发明的实施范围,凡依本发明的原理、构造以及结构所作的等效变化,均应涵盖于本发明的保护范围内。

Claims (6)

1.一种宽温稳定型陶瓷介质材料,其特征在于,由以下质量百分比的原料组成:SrNb2O6:35-58wt%,BaTa2O6:22-32wt%,CaZrO3:15-21wt%,Dy2O3:3-11wt%,MgO:0.3-0.9wt%,Ag2O:0.1-0.4wt%。
2.根据权利要求1所述宽温稳定型陶瓷介质材料,其特征在于,由以下质量百分比的原料组成:SrNb2O6:48wt%,BaTa2O6:29wt%,CaZrO3:19wt%,Dy2O3:3wt%,MgO:0.8wt%,Ag2O:0.2wt%。
3.根据权利要求1或2所述宽温稳定型陶瓷介质材料的制备方法,其特征在于,步骤如下:
1)将SrNb2O6、BaTa2O6、CaZrO3和Dy2O3作为起始原料按质量百分比进行配料,混合后按质量百分比加入MgO和Ag2O混合物充分搅拌,并加入无水乙醇混合球磨24小时,烘干得到粉末A;
2)将步骤1)中制得的粉末A放入马弗炉中,升温至1050~1200℃预烧4-10小时得到前驱体B;
3)将步骤2)中制得的前驱体B研碎后加入无水乙醇,球磨8-15小时混合均匀,烘干得到粉末C;
4)向步骤3)中制得的粉末C中加入5wt%聚乙烯醇水溶液造粒,过60目筛后压制成型,放入高温炉中升温至1250~1400℃烧结8-12小时后自然冷却至室温,即得。
4.根据权利要求3所述宽温稳定型陶瓷介质材料的制备方法,其特征在于,所述步骤2)中预烧温度为1180℃,时间为4小时。
5.根据权利要求3所述宽温稳定型陶瓷介质材料的制备方法,其特征在于,所述步骤3)中球磨时间为12小时。
6.根据权利要求3所述宽温稳定型陶瓷介质材料的制备方法,其特征在于,所述步骤4)中烧结温度为1300℃,时间为10小时。
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Publication number Priority date Publication date Assignee Title
CN111960821A (zh) * 2020-07-27 2020-11-20 苏州瑞玛精密工业股份有限公司 一种微波介质陶瓷材料及其制备方法和应用

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1524792A (zh) * 2003-02-28 2004-09-01 新加坡纳米材料科技有限公司 一种制备各种晶态钙钛矿类化合物粉体的方法
CN101560094A (zh) * 2009-05-27 2009-10-21 武汉理工大学 一种高温稳定型多层陶瓷电容器介质材料及其制备方法

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1524792A (zh) * 2003-02-28 2004-09-01 新加坡纳米材料科技有限公司 一种制备各种晶态钙钛矿类化合物粉体的方法
CN101560094A (zh) * 2009-05-27 2009-10-21 武汉理工大学 一种高温稳定型多层陶瓷电容器介质材料及其制备方法

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111960821A (zh) * 2020-07-27 2020-11-20 苏州瑞玛精密工业股份有限公司 一种微波介质陶瓷材料及其制备方法和应用

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