CN102307825B - 低温烧结陶瓷烧结体及多层陶瓷基板 - Google Patents
低温烧结陶瓷烧结体及多层陶瓷基板 Download PDFInfo
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- CN102307825B CN102307825B CN201080007906.6A CN201080007906A CN102307825B CN 102307825 B CN102307825 B CN 102307825B CN 201080007906 A CN201080007906 A CN 201080007906A CN 102307825 B CN102307825 B CN 102307825B
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Abstract
一种构成具备外部导体膜(4)的多层陶瓷基板(1)的陶瓷层(2)的低温烧结陶瓷烧结体,其中,该低温烧结陶瓷烧结体由非玻璃系的低温烧结陶瓷材料烧结形成,并析出了石英(Quartz)、氧化铝(Alumina)和硅钛钡石(Fresnoite)的各结晶相。由于陶瓷层(2)是非玻璃系的低温烧结陶瓷烧结体,因此其组成不均匀性小,可以低成本并且容易地制造多层陶瓷基板(1)。此外,由于陶瓷层(2)析出了前述的各结晶相,因此与外部导体膜(4)的接合强度高,并且烧结体自身的破坏韧性值大。
Description
技术领域
本发明涉及由非玻璃系的低温烧结陶瓷材料烧成而得到的低温烧结陶瓷烧结体,以及使用该低温烧结陶瓷烧结体而构成的多层陶瓷基板。
背景技术
低温烧结陶瓷(LTCC:Low Temperature Cofired Ceramic)烧结体是将低温烧结陶瓷材料成形为规定的形状并将其烧结而成的。
低温烧结陶瓷材料可与比电阻较小的银或铜等低熔点金属材料共烧成,因此可形成高频特性优良的多层陶瓷基板,例如多用作为信息通信终端上的高频模块用基板材料。
作为低温烧结陶瓷材料,通常是将B2O3-SiO2系玻璃材料混入Al2O3等陶瓷材料中的所谓的玻璃陶瓷复合系。在这个体系中,由于起始原料必需用比较高价的玻璃,并且含有在烧成时易挥发的硼元素,因此得到的基板的组成容易不均匀。因此,为了控制硼的挥发量,不得不使用特殊的调节器(日文:セツタ一)等,其制造工序繁杂。
于是,提出了例如在日本专利特开2002-173362号公报(专利文献1)、日本专利特开2008-044829号公报(专利文献2)以及日本专利特开2008-053525号公报(专利文献3)等中记载的低温烧结陶瓷材料。由于这些文献中记载的低温烧结陶瓷材料的起始原料中不含有玻璃,而且是不含有硼的非玻璃系低温烧结陶瓷材料,因此没有遇到上述的问题。
然而,这些文献中记载的由低温烧结陶瓷材料烧结形成的低温烧结陶瓷烧结体与其表面形成的导体膜的接合强度不是很足够,并且,由于烧结体自身的破坏韧性值小,因此未能得到所期望的强度特性。
专利文献1:日本专利特开2002-173362号公报
专利文献2:日本专利特开2008-044829号公报
专利文献3:日本专利特开2008-053525号公报
发明内容
本发明是鉴于上述情况而完成的发明,其目的在于提供一种起始原料不用玻璃,可以低成本且容易地制造的非玻璃系的低温烧结陶瓷烧结体,该低温烧结陶瓷烧结体与导体膜的接合强度高,并且破坏韧性值大。
本发明的另一目的在于提供一种可靠性高的多层陶瓷基板,该多层陶瓷基板具备由上述低温烧结陶瓷烧结体形成的多个陶瓷层。
本发明的低温烧结陶瓷烧结体的特征在于,由非玻璃系的低温烧结陶瓷材料烧结形成,并析出石英(Quartz)、氧化铝(Alumina)和硅钛钡石(Fresnoite)的各结晶相。
此外,本发明还涉及一种多层陶瓷基板,该多层陶瓷基板具备由多个陶瓷层层叠而形成的层叠体,和设置在该层叠体的表层和内层的以金、银或铜为主成分的导体图形。本发明的多层陶瓷基板的特征在于,上述陶瓷层是由低温烧结陶瓷烧结体构成的,其中,低温烧结陶瓷烧结体由非玻璃系的低温烧结陶瓷材料烧结而形成,并且析出了石英、氧化铝和硅钛钡石的各结晶相。
由于本发明的低温烧结陶瓷烧结体是由非玻璃系的低温烧结陶瓷材料烧结而形成的,因此组成的不均匀性小、成本低。并且,由于不用特殊的调节器也可烧成,所以其制造工序容易实施。此外,由于烧结体析出了石英、氧化铝和硅钛钡石的各结晶相,所以与其表面形成的导体膜的接合强度高,并且由于烧结体自身的破坏韧性值大,因此强度特性优良。
同样地,由于构成本发明的多层陶瓷基板的陶瓷层是由非玻璃系的低温烧结陶瓷材料烧结而形成的,因此本发明的多层陶瓷基板的组成不均匀性小、成本低,并且由于不用特殊的调节器也可烧成,因此可以容易地制造。此外,由于陶瓷层析出了石英、氧化铝和硅钛钡石的各结晶相,因此与其表面形成的外部导体膜的接合强度高。并且,由于烧结体自身的破坏韧性值较大,所以具备该陶瓷层的多层陶瓷基板可以用作为强度特性优良、可靠性高的基板。
附图说明
图1是使用本发明的低温烧结陶瓷烧结体构成的多层陶瓷基板1的图解剖视图。
具体实施方式
本发明的低温烧结陶瓷烧结体由非玻璃系的低温烧结陶瓷材料烧结形成,并析出了石英(Quartz:SiO2)、氧化铝(Alumina:Al2O3)和硅钛钡石(Fresnoite:Ba2TiSi2O8)的各结晶相。在这里,“低温烧结陶瓷烧结体”是指将可以与比电阻较小的金、银或铜等低熔点金属材料共烧成的低温烧结陶瓷材料在例如1050℃以下的烧成温度下烧结而成的烧结体。而且,在起始原料中实质上不含有玻璃成分,但该烧结体自身除了前述的各结晶相以外,还有非晶质部分。这是因为在非玻璃系的低温烧结陶瓷材料烧成时,其起始原料的一部分玻璃化的缘故。
由于本发明的低温烧结陶瓷烧结体是作为上述结晶相的主结晶相,其介电常数εr较小为10以下,所以可以得到适合于构成高频用基板的陶瓷层的低温烧结陶瓷烧结体。并且,如上所述,由于与外部导体膜的接合强度较高,电极剥离强度提高,不易发生所安装的表面安装零部件脱落等问题。此外,由于可以形成破坏韧性值较大的陶瓷层,因此可以得到可靠性优良的多层陶瓷基板。
本发明的低温烧结陶瓷烧结体较好的是还析出了硅钡石(Sanbornite:BaSi2O5)和钡长石(Celsian:BaAl2Si2O8)中的至少一种结晶相。这样,如果析出硅钡石或钡长石的结晶相,则多种结晶相就会有大量存在,其结果为,烧结体的结晶构造变得不均一,即使在烧结体中有裂纹,也可以抑制其延长。更好的是硅钡石和钡长石这两种结晶相都析出。
在本发明的低温烧结陶瓷烧结体中,硅钛钡石结晶相的含有比例较好是在1~20重量%。通过使硅钛钡石结晶相的析出量适当化,抑制结晶相的偏析,可以使外部导体膜的接合强度进一步提高,还可以使电极剥离强度更高。
此外,在本发明的低温烧结陶瓷烧结体中,硅钛钡石结晶相的平均结晶粒径较好为5μm以下。即,当存在规定比例的这种细小的结晶相时,晶界会增加,即使在烧结体中有裂纹,也可以抑制其延长。
此外,构成本发明的低温烧结陶瓷烧结体的非玻璃系低温烧结陶瓷材料较好是含有主成分陶瓷材料和副成分陶瓷材料,实质上不含有Cr氧化物和B氧化物中的任何一种,其中,所述主成分陶瓷材料含有Si氧化物、Ba氧化物和Al氧化物,所述副成分陶瓷材料含有Mn氧化物和Ti氧化物。在这里,“实质上”是指可含有低于0.1重量%的作为杂质的Cr氧化物和B氧化物。即,即使Cr氧化物和B氧化物作为杂质混入,只要其含量低于0.1重量%也可以达到本发明的效果。
更详细地讲,该低温烧结陶瓷材料较好是含有主成分陶瓷材料和副成分陶瓷材料,实质上不含有Cr氧化物及B氧化物中的任何一种,其中,主成分陶瓷材料含有换算成SiO2为48~75重量%的Si、换算成BaO为20~40重量%的Ba以及换算成Al2O3为5~20重量%的Al,相对于100重量份的主成分陶瓷材料,副成分陶瓷材料含有换算成MnO为2~10重量份的Mn以及换算成TiO2为0.1~10重量份的Ti。
由于该低温烧结陶瓷材料是在起始原料中不使用玻璃且不含有硼的非玻璃系的低温烧结陶瓷材料,所以得到的烧结体的组成不易出现不均匀、其烧成工序的管理容易。而且,得到的烧结体具有230MPa以上的弯曲强度,除烧结体自身的强度较高外,将其作为基板使用时,还可成为具有高剥离强度、与外部导体膜的接合强度高且可靠性高的基板。并且,由于结晶化得到促进,因此可以提高对高温、高湿等环境条件的耐受性,还可提高基板的耐化学品性,藉此可以抑制基板成分在镀液中的溶出。还有,由于结晶化得到促进,因此还可得到非晶质部分少、Qf值高的多层陶瓷基板。
在这里,含有换算成SiO2为48~75重量%的Si、换算成BaO为20~40重量%的Ba以及换算成Al2O3为5~20重量%的Al的主成分陶瓷材料是所得烧结体的基本成分,对得到绝缘电阻大、介电常数εr小和介质损耗小的烧结体具有较大贡献。
另一方面,作为副成分陶瓷材料的Mn(特别是MnO2)与SiO2-BaO-Al2O3系主成分陶瓷材料反应,易制成液相成分,在烧成时由于起始原料的粘性下降而作为烧结助剂发挥作用,但与同样作为烧结助剂发挥作用的B2O3相比,挥发性远远要小。因而,在烧成的不均匀性降低、其烧成工序的管理易于进行的同时,也有助于量产性的提高。
另外,虽然详细的机理不是很清楚,但是认为副成分陶瓷材料Ti(特别是TiO2)可以增加由低温烧结陶瓷材料形成的陶瓷层和由铜等低熔点金属材料形成的外部导体膜之间的反应性,通过其共烧成工序,可提高烧结体和导体膜的接合强度,即,陶瓷层和外部导体膜之间的接合强度。其结果是,安装在多层陶瓷基板上的半导体器件等有源元件或芯片电容器等无源元件和多层陶瓷基板间形成牢固的焊接接合,可以抑制因其坠落等冲击造成的接合破坏。
另外,作为副成分陶瓷材料替代上述的Ti,或者在Ti之外添加,该低温烧结陶瓷材料也可以含有Fe(特别是Fe2O3)。这种情况下,其含有量以和Ti氧化物的合计量计,相对于100重量份的主成分陶瓷材料,较好是0.1~10重量份。该Fe也可以增加陶瓷层与外部导体膜之间的反应性,通过其共烧成工序,可以提高烧结体与导体膜之间的接合强度,即,陶瓷层与外部导体膜之间的接合强度。
另外,由于该低温烧结陶瓷材料实质上不含有B氧化物(特别是B2O3),因此可减小其烧成时组成的不均匀性,不用特殊的调节器也可以,使得其烧成工序的管理变得容易。并且,由于实质上不含有Cr氧化物(特别是Cr2O3),因此可抑制以微波为代表的高频带宽上的Qf值的降低,如在3GHz可得到1000以上的Qf值。
该低温烧结陶瓷材料较好是不含有Li2O或Na2O等碱金属氧化物。因为这些碱金属氧化物也和B2O3一样,在烧成时易于挥发,成为造成所得基板的组成不均匀的原因。还有,如果不含有这些碱金属氧化物,则可以提高对高温、高湿等环境条件的耐受性,还可以提高抑制向镀液的溶出这样的耐化学品性。
在该低温烧结陶瓷材料中,较好是作为副成分陶瓷材料,相对于100重量份的主成分陶瓷材料,还含有换算成MgO为0.1~5重量份的Mg。如果含有Mg(特别是MgO),则烧成时的低温烧结陶瓷材料的结晶化得到促进。其结果为,可以减少导致基板强度下降的液相部分的体积量,并可以使得到的烧结体的弯曲强度进一步提升。
另外,在该低温烧结陶瓷材料中,作为副成分陶瓷材料,相对于100重量份的主成分陶瓷材料,较好是还含有分别换算成Nb2O5、CeO2、ZrO2、ZnO为0.1~6重量份的选自Nb、Ce、Zr及Zn的至少一种。如果含有选自Nb、Ce、Zr和Zn的至少一种(特别是选自Nb2O5、CeO2、ZrO2、ZnO的至少一种氧化物),则可减少作为非晶质成分易残存的Mn(特别是MnO)的添加量。其结果为,可以减少导致基板强度下降的液相部分的体积量,并可以使得到的多层陶瓷基板的弯曲强度进一步提升。
另外,该低温烧结陶瓷材料中作为副成分陶瓷材料,相对于100重量份的主成分陶瓷材料,还可以含有分别换算成CoO和V2O5为0.1~5.0重量份的Co和/或V。这些成分可进一步提高得到的多层陶瓷基板的弯曲强度,同时还起到染料的作用。
本发明的低温烧结陶瓷烧结体可以通过以下方法制造:将MnCO3陶瓷粉末、以及TiO2和Fe2O3的至少一方的陶瓷粉末添加到SiO2、BaCO3和Al2O3的各种陶瓷粉末中并混合,将混合后的低温烧结陶瓷材料成形为规定的形状,进一步将该成形体烧成。较好是经过以下工序制造:将TiO2和Fe2O3的至少一方的陶瓷粉末添加到SiO2、BaCO3和Al2O3的各种陶瓷粉末中,对于所形成的混合物焙烧而制得焙烧粉的工序;和在所述焙烧粉中添加未经焙烧的MnCO3陶瓷粉末的工序。
因而,含有上述低温烧结陶瓷材料的陶瓷生片较好是经过以下工序制造:将TiO2和Fe2O3的至少一方的陶瓷粉末添加到SiO2、BaCO3和Al2O3的各种陶瓷粉末中,对于所形成的混合物焙烧而制得焙烧粉的工序;在所述焙烧粉中添加未经焙烧的MnCO3陶瓷粉末的同时添加粘合剂而制得陶瓷浆料的工序;将陶瓷浆料成形而制得陶瓷生片的工序。
如上所述,在制造低温烧结陶瓷材料或陶瓷生片时,将Si成分、Ba成分、Al成分和Ti/Fe成分焙烧而得到焙烧粉后,如果将未经焙烧的Mn成分添加到焙烧粉中,则可抑制焙烧时的焙烧合成反应,由此可以使焙烧粉的粒径微小化。因而,在可以简化焙烧粉的粉碎工序的同时,易于实现用其制成的陶瓷生片的薄层化。并且可以防止焙烧粉的颜色变成焦茶色,因而,特别是在印刷以铜为主成分的导电糊时,可以提高使用这种焙烧粉制成的陶瓷生片的图像识别性。
下面,基于图示的实施方式,对使用本发明的低温烧结陶瓷材料构成的多层陶瓷基板及其制造方法进行说明。
图1是使用本发明的低温烧结陶瓷烧结体构成的多层陶瓷基板1的图解剖视图。
多层陶瓷基板1具备层叠体3,该层叠体3由层叠的多个陶瓷层2构成。层叠体3具备的陶瓷层2是由本发明的低温烧结陶瓷烧结体构成的。在该层叠体3中,在陶瓷层2的特定部分设置有各种相关的导体图形。
作为上述导体图形,包括在层叠体3的层叠方向的端面上形成的数个外部导体膜4和5,沿着陶瓷层2间的特定界面形成的数个内部导体膜6,以及贯穿陶瓷层2的特定部分而形成的作为层间连接导体的通孔导体7等。
设置于层叠体3表面的外部导体膜4用于连接将要安装在层叠体3的外表面上的电子零部件8和9。在图1中,图示了如半导体器件那样具有凸端电极10的电子零部件8,以及如芯片电容器那样具有平面状端子电极11的电子零部件9。另外,在层叠体3的背面设置的外部导体膜5用于连接安装该多层陶瓷基板1的主板(未图示)。
该多层陶瓷基板1所具备的层叠体3可通过将未烧成层叠体烧成而制得。该未烧成层叠体具有成为陶瓷层2的多个层叠的陶瓷生片层,和由导电糊形成的内部导体膜6和通孔导体7,根据情况还可具有由导电糊形成的外部导体膜4和5。
上述未烧成层叠体中的陶瓷生片层的叠层构造典型的是通过将陶瓷浆料成形得到的多枚陶瓷生片层叠而得到。在层叠前的陶瓷生片上设置导体图形,特别是内部的导体图形。
陶瓷浆料可以通过以下方法制得:将聚乙烯醇缩丁醛等有机粘合剂、甲苯及异丙醇等溶剂、邻苯二甲酸二正丁酯等增塑剂以及根据需要使用的分散剂等添加剂加入到上述的低温烧结陶瓷材料中进行浆料化。
在使用陶瓷浆料进行陶瓷生片的成形时,例如可通过以下方法实施:在由聚对苯二甲酸乙二醇酯等有机树脂形成的底膜上,采用刮刀法(日文:ドクタ一ブレ一ド法)将陶瓷浆料成形为片状。
在陶瓷生片上设置导体图形时,使用含有金、银或铜等低熔点金属材料作为导电成分的主成分的导电糊,在陶瓷生片上设置用于通孔导体7的贯通孔,用导电糊填充贯通孔的同时,通过例如丝网印刷法将用于内部导体膜6的导电糊膜、以及用于外部导体膜4和5的导电糊膜成形。另外,在金、银或铜的低熔点金属材料中,特别是以铜为主成分的导电糊与本发明的低温烧结陶瓷烧结体具有良好的共烧结性。
将这样的陶瓷生片按照规定的顺序层叠,在层叠方向上通过施加例如1000~1500kgf/cm2的压力进行压接,藉此得到未烧成层叠体。在该未烧成层叠体上,虽然没有图示,也可以设置用于收纳其他电子零部件的空穴,或设置用于固定覆盖电子零部件8和9等的盖子的接合部分。
未烧成层叠体通过以下方法烧成:在能够烧结陶瓷生片层含有的陶瓷材料的温度以上,例如在850℃以上,导体图形中含有的金属的熔点以下,如果是铜的情况下,在1050℃以下的温度范围内烧成。由此,在陶瓷生片层烧结的同时导电糊也烧结,由烧结后的导体膜形成电路图形。
另外,特别是导体图形中含有的主成分金属是铜的情况下,烧成在氮气氛等非氧化性气氛中进行,例如在900℃以下的温度完成脱粘合剂;还有,在降温时,使氧分压降低,让烧成完成时的铜没有实质性氧化。另外,烧成温度例如在980℃以上时,作为导体图形中包含的金属,银将难以使用,如果是钯含量为20重量%以上的Ag-Pd系合金,则可以使用。这种情况下,烧成可以在空气中进行。烧成温度如果在950℃以下时,则银可以作为导体图形中含有的金属使用。
如上所述,烧成工序结束时,可以得到图1所示的层叠体3。
之后,表面安装电子零部件8和9,由此,图1所示的多层陶瓷基板1就完成了。
上述多层陶瓷基板1中的陶瓷层2,如前所述,其起始原料不含有玻璃,但由于在其烧成循环中会生成作为非晶质成分的玻璃,所以在烧成后的陶瓷层2中含有玻璃。因而,不需要使用高价的玻璃,也可以稳定地制作多层陶瓷基板1。
另外,本发明的低温烧结陶瓷烧结体较好是用于包含具备所述层叠构造的层叠体的多层陶瓷基板,但也可用于只有一个陶瓷层的单层构造的陶瓷基板。此外,本发明的低温烧结陶瓷烧结体还适用于复合型的多层陶瓷基板,该复合型的多层陶瓷基板具备由该低温烧结陶瓷烧结体形成的低介电常数陶瓷层和介电常数εr较高的(例如εr为15以上的)其他低温烧结陶瓷烧结体形成的高介电常数陶瓷层。
[实验例]
接着,对为了确认本发明带来的效果而实施的实验例进行说明。
首先,作为起始原料,准备了粒径均在2.0μm以下的SiO2、BaCO3、Al2O3、MnCO3、TiO2和Mg(OH)2的各种陶瓷粉末。然后,按照可以在烧成后形成表1所示的组成比例的条件称量这些起始原料粉末,经湿式混合粉碎后干燥,将得到的混合物在750~1000℃下焙烧1~3小时,得到原料粉末。上述BaCO3烧成后变为BaO、上述MnCO3烧成后变为MnO、上述Mg(OH)2烧成后变为MgO。
此外,在表1中,主成分陶瓷材料SiO2、BaO和Al2O3以重量%(wt%)为单位表示,这些材料合计为100重量%。另一方面,副成分陶瓷材料MnO、TiO2和MgO的相对于主成分陶瓷材料100重量份的比例以重量份为单位表示。
[表1]
接着,往上述的各试料的原料粉末中添加适量的有机粘合剂、分散剂以及增塑剂,制成陶瓷浆料。然后,将浆料中的原料粉末混合粉碎至平均粒径(D50)为1.5μm以下。
接着,使用刮刀法将陶瓷浆料成形为片状,干燥,切割成合适的大小,得到厚度为50μm的陶瓷生片。
接着,在规定的陶瓷生片上通过丝网印刷法印刷以铜为主成分的导电糊,形成作为外部导体膜的导体图形。
接着,将得到的陶瓷生片切割成规定的大小后,将多枚层叠,然后在温度为60~80℃、压力为1000~1500kgf/cm2的条件下进行热压接,得到未烧成层叠体。
接着,将未烧成层叠体在氮气—氢气的非氧化性气氛中于900~1050℃的温度下烧成,可得到陶瓷生片和导体图形共烧结而形成的板状的陶瓷烧结体试料。
接着,对于得到的试料,使用维氏压头在500gf×15秒的条件下在其表面施加压痕,根据其大小和龟裂的长度算出破坏韧性值KIC。此外,对于得到的试料,在其表面的一边为2mm的方形电极上焊接L字状的引线,通过相对于试料表面的垂直方向上的拉伸试验测定试料与电极的接合强度(电极剥离强度)。此外,将试料粉末化,通过X射线衍射光谱鉴定析出的结晶,同时根据衍射峰强度算出硅钛钡石结晶相的重量比率(析出量)。此外,通过扫描型显微镜和透射型显微镜算出硅钛钡石结晶相的平均粒径。此外,通过微扰法测定在3GHz下的介电常数εr。
以上的结果示于表2中。
[表2]
*1:Q:石英 A:氧化铝 S:硅钡石 C:钡长石 F:硅钛钡石
从试料No.1~4和6可以看出,当陶瓷烧结体中有石英、氧化铝和硅钛钡石的各结晶相析出时,会得到电极剥离强度超过20N/2mm2、破坏韧性值KIC超过1.2Pa·m1/2、介电常数εr在10以下的烧结体。
此外,从试料No.1~4间的比较可以看出,通过使TiO2的量增加,烧结体中硅钛钡石结晶相的相对析出量会变多,任何一个的破坏韧性值KIC都超过了1.3Pa·m1/2。即,在这些试料中,龟裂的扩展不易发生,基板的强度优良。还有,从结果可以了解到,在电极接合界面的龟裂不易发生、裂纹的扩展也不易发生、耐冲击性得到提高。
另一方面,如试料No.5所示,在没有硅钛钡石结晶相产生的情况时,破坏韧性值KIC低、电极剥离强度也低。
另外,如试料No.6所示,低温烧结陶瓷材料中,如果相对于100重量份的主成分陶瓷材料的TiO2的比例超过10重量份,则硅钛钡石结晶相的析出会增加,相对地硅钡石或钡长石等其他的结晶相的析出量就会减少,结晶构造倾向于均质化。这种情况下,就会有阻碍龟裂扩展的应力分布减少、破坏韧性值KIC降低的倾向。此外,硅钛钡石结晶相的平均粒径变大也被认为是晶界减少、破坏韧性值KIC降低的原因。
符号的说明
1多层陶瓷基板
2陶瓷层
3层叠体
4、5外部导体膜
6内部导体膜
7通孔导体
Claims (6)
1.一种低温烧结陶瓷烧结体,由非玻璃系的低温烧结陶瓷材料烧结形成,并析出了石英、氧化铝和硅钛钡石的各结晶相。
2.如权利要求1所述的低温烧结陶瓷烧结体,其中,还析出了硅钡石和钡长石中的至少一种结晶相。
3.如权利要求1或2所述的低温烧结陶瓷烧结体,其中,所述硅钛钡石结晶相的含有比例为1~20重量%。
4.如权利要求1~3中任一项所述的低温烧结陶瓷烧结体,其中,所述硅钛钡石结晶相的平均结晶粒径为5μm以下。
5.如权利要求1~4中任一项所述的低温烧结陶瓷烧结体,所述非玻璃系的低温烧结陶瓷材料含有主成分陶瓷材料和副成分陶瓷材料,实质上不含有Cr氧化物和B氧化物中的任何一种,其中,所述主成分陶瓷材料含有Si氧化物、Ba氧化物和Al氧化物,所述副成分陶瓷材料含有Mn氧化物和Ti氧化物。
6.一种多层陶瓷基板,具备由多个陶瓷层层叠而形成的层叠体和设置在所述层叠体的表层和内层的以金、银或铜为主成分的导体图形,其中,所述陶瓷层由低温烧结陶瓷烧结体构成,所述低温烧结陶瓷烧结体由非玻璃系的低温烧结陶瓷材料烧结形成,并析出了石英、氧化铝和硅钛钡石的各结晶相。
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