CN105453201B - 电介质膜、膜电容器以及电子设备 - Google Patents
电介质膜、膜电容器以及电子设备 Download PDFInfo
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- CN105453201B CN105453201B CN201480042252.9A CN201480042252A CN105453201B CN 105453201 B CN105453201 B CN 105453201B CN 201480042252 A CN201480042252 A CN 201480042252A CN 105453201 B CN105453201 B CN 105453201B
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- dielectric film
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- membrane capacitance
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Classifications
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Abstract
本发明提供可以提高比介电常数且不会降低击穿电场强度的电介质膜、膜电容器以及电子设备。一种电介质膜,其在有机树脂5中含有陶瓷粒子3,陶瓷粒子3具有形成通过a、b和c的3个轴所形成的晶格并且轴比c/a不同的2种以上的晶相3a、3b。由于晶格形状(尺寸)的差异,因此各晶相3a、3b的介电极化的程度不同,因此陶瓷粒子3具有介电常数不同的区域,可以提高比介电常数且不会降低击穿电场强度。
Description
技术领域
本发明涉及电介质膜、膜电容器以及电子设备。
背景技术
膜电容器例如具有在将聚丙烯树脂膜化而成的电介质膜的表面上通过蒸镀所形成的金属膜作为电极。通过这样的构成,膜电容器具有如下优点:即使在电介质膜的绝缘缺陷部产生短路的情况下,缺陷部周边的金属膜因短路的能量而蒸发、飞散,产生绝缘化,从而可以防止膜电容器的绝缘击穿(例如,参见专利文献1)。
因此,膜电容器在可以防止电路短路时的燃烧、触电这一点受到关注,近年来其首先应用于LED(Light Emitting Diode)照明等的电源电路,并且用途正不断扩大(例如,参见专利文献2)。
但是,在安装了各种电子部件的基板上,膜电容器与陶瓷电容器等其他电子部件相比,尺寸仍然较大,因此妨碍了该基板的低高度化以及安装密度的提高,因此正在对膜电容器的小型化进行研究。
这时,为了实现膜电容器的小型化而使作为电介质的膜薄化或者减少膜的层叠数、卷绕数,因此需要提高膜的比介电常数和击穿电场强度。
例如,在专利文献3中,提出了使用在具有环氧基的有机树脂中分散陶瓷填料而成的电介质膜作为膜。
现有技术文献
专利文献
专利文献1:日本特开平9-129475号公报
专利文献2:日本特开2010-178571号公报
专利文献3:日本特开2006-225484号公报
发明内容
发明要解决的问题
然而,上述电介质膜中,即使在陶瓷粒子的体积比率较高时,在比介电常数高的陶瓷粒子侧也难以产生起因于所施加的电场的电场能量(εr×E^2/2)的集中,因此比介电常数并没怎么提高。另外,另一方面,由于在陶瓷粒子周围的有机树脂侧电场强度增加,因此还具有作为电介质膜整体而击穿电场强度下降的问题。
本发明是为了解决上述问题而完成的,其目的在于提供可以提高比介电常数且不会降低击穿电场强度的电介质膜、膜电容器以及电子设备。
解决问题的方法
本发明的电介质膜,其特征在于,具有有机树脂和包含在该有机树脂中的陶瓷粒子,所述陶瓷粒子包含具有通过a、b和c的3个轴所形成的晶格并且轴比c/a不同的2种以上的晶相。
本发明的膜电容器,其特征在于,具有上述电介质膜和设置于该电介质膜上的电极层。
本发明的电子设备,其特征在于,上述膜电容器与电路中所具备的导体连接。
发明效果
根据本发明,可以提高电介质膜的比介电常数而不会降低击穿电场强度。另外,使用该电介质膜的膜电容器,其击穿电场强度高,并且能够在小型的情况下得到高静电容量。此外,使用该膜电容器的电子设备小型并且安装密度高,成为发挥优异整流作用的电子设备。
附图说明
图1是部分地表示本发明的电介质膜的一种实施方式的剖面模式图。
图2是部分地表示以往的电介质膜的剖面模式图。
图3是表示在图1所示的电介质膜中存在陶瓷粒子时的陶瓷粒子和有机树脂界面处的比介电常数和电场强度的变化的模式图。
图4是表示图2中所示的以往电介质膜,以及在该电介质膜中存在陶瓷粒子时的、陶瓷粒子和有机树脂界面处的比介电常数和电场强度的变化的模式图。
图5(a)是模式地表示在电介质膜的两面上具有电极层的结构的剖面图,图5(b)是表示本发明的膜电容器的一种实施方式的外观剖视图。
图6是表示使用本发明的膜电容器的电路的一例的图。
具体实施方式
图1是部分地表示本发明的电介质膜的一种实施方式的剖面模式图。图2是部分地表示以往的电介质膜的剖面模式图。图3是表示在图1所示的电介质膜中存在陶瓷粒子时的陶瓷粒子和有机树脂界面处的比介电常数和电场强度的变化的模式图。图4是表示图2中所示的以往电介质膜,以及在该电介质膜中存在陶瓷粒子时的、陶瓷粒子和有机树脂界面处的比介电常数和电场强度的变化的模式图。
本实施方式的电介质膜1通过陶瓷粒子3和有机树脂5的复合电介质而构成。此处,构成本实施方式的电介质膜1的陶瓷粒子3利用2种以上的晶相构成,所述晶相具有通过a、b和c的3个轴所形成的晶格,并且轴比c/a不同(在图1、图3中,示出了由2种晶相3a、3b形成的陶瓷粒子。)。
根据本实施方式的电介质膜1,电介质膜1中含有陶瓷粒子3,因此起因于施加电场的电场能量的集中容易在比介电常数高的陶瓷粒子3侧产生,由此,可以提高电介质膜1的比介电常数。
构成该电介质膜1的陶瓷粒子3,例如,如图1和图3所示,具有轴比c/a不同的2种以上的晶相3a、3b,因此由于晶格形状(尺寸)的差异,各晶相3a、3b的介电极化的程度不同,陶瓷粒子3具有介电常数不同的区域。
根据电介质膜1,在陶瓷粒子3的内部(在图3中表示为3a)、陶瓷粒子3的表面附近(在图3中表示为3b)、和有机树脂5的各区域中,存在不同介电常数的相,因此能够抑制陶瓷粒子3和有机树脂5之间的局部电场强度的增加。如此,可以较高地维持电介质膜1的击穿电场强度,能够提高比介电常数且不会降低击穿电场强度。
即,在本实施方式的电介质膜1中,由于陶瓷粒子3和有机树脂5之间的介电常数的变化较小,因此可以抑制陶瓷粒子3和有机树脂5之间的介电常数变化所导致的局部的电场强度的增加。由此,可以将电介质膜1的击穿电场强度提高至接近有机树脂5本身所具有的值。
相对于此,在如图2和图4所示的含有由单一晶相13a所构成的陶瓷粒子13的以往的电介质膜11的情况下,在陶瓷粒子13和有机树脂15之间,容易产生介电常数的急剧变化。因此,陶瓷粒子13和有机树脂15之间的介电常数的变化所导致的局部的电场强度容易变高,因此电介质膜11的击穿电场强度变低。
此处,在陶瓷粒子3中存在轴比c/a不同的晶相3a、3b的状态可由如下差异来确认:在X射线衍射图中,例如,在晶面指数(400)、(004)和(040)的衍射峰中,至少2个分开,或者这些晶面指数(400)、(004)和(040)的衍射峰在相同的2θ角度中处于重合的状态。此处,晶格的轴比c/a不同,是指c/a值具有0.002(2/1000)以上的差值。陶瓷粒子3的轴比c/a通过X射线衍射法求出。
作为能够通过X射线衍射法更明确地看出晶相3a、3b的存在的陶瓷粒子3,优选仅含有2种轴比c/a不同的晶相。
在可以减小陶瓷粒子3和有机树脂5之间的介电常数的急剧变化这一点上,较好的是陶瓷粒子3具有轴比c/a不同的多个晶相,但是在陶瓷粒子3含有较多的轴比c/a不同的晶相时,由于高介电常数的晶相的比例可能会变小,因此在陶瓷粒子3中优选仅存在2种具有轴比c/a差的晶相3a、3b。
此处,所谓陶瓷粒子3具有轴比c/a不同的2种晶相的状态,例如是指:如在晶面指数(400)、(004)和(040)的衍射峰中所观察到的那样,晶体结构基本相同,可以由X射线衍射图分离出基于各晶相3a、3b的衍射峰。因此,基本的晶体结构不同的晶相除外。
如果陶瓷粒子3中存在的具有轴比c/a差的晶相3a、3b仅为2种,则在陶瓷粒子3和有机树脂5之间,陶瓷粒子3显示出2种不同的介电常数,另一方面,有机树脂5显示出1种介电常数。因此,从陶瓷粒子3到有机树脂5,容易形成介电常数逐渐变化的区域。如此,在电介质膜1中,可以减少局部电场强度增加的位置的数量,能够在较高地维持击穿电场强度的状态下实现高介电常数化。
作为这种陶瓷粒子3,如图3所示,优选以构成陶瓷粒子3的2种晶相形成核壳结构的方式进行配置。此处,所谓核壳结构,是指由核部以及设置在该核部周围的壳部形成,核部由2种晶相中的一种晶相形成,壳部由2种晶相中的另一种晶相形成的构成。
如果是以构成陶瓷粒子3的2种晶相形成核壳结构的形式进行配置的陶瓷粒子,则在陶瓷粒子3的中心区域(核部:3a)和有机树脂5之间隔着陶瓷粒子3的表面区域(壳部:3b),因此,陶瓷粒子3的表面区域(壳部:3b)在陶瓷粒子3的中心区域(核部:3a)和有机树脂5之间成为显示出中间的介电常数的区域。因此,可以形成从陶瓷粒子3的中心区域(核部:3a)到有机树脂5,介电常数阶段性变化的陶瓷粒子3。因此,可以减小陶瓷粒子3和有机树脂5的界面处的急剧的电场强度的变化。结果可以得到高介电常数、击穿电场强度高、并且绝缘可靠性高的电介质膜1。
此外,在以构成陶瓷粒子3的2种晶相形成核壳结构的方式进行配置时,如图3所示,优选轴比c/a小的晶相配置在轴比c/a大的晶相的外侧。即,优选构成壳部的晶相的轴比c/a比构成核部的晶相小。
作为这种具有核壳结构的陶瓷粒子3,优选使用具有钙钛矿结构的陶瓷材料。其原因在于,如果陶瓷粒子3具有钙钛矿结构,则例如能够通过组成的变化、成分固溶度的差异而改变轴比c/a,另外,高介电常数化也变得容易。
作为具有钙钛矿结构的陶瓷材料,可以列举钛酸钡系陶瓷作为适当材料。
此处,所谓钛酸钡系陶瓷,不只是化学式BaTiO3表示的化学计量比的组成式所表示的复合氧化物,只要是可以维持钙钛矿结构的程度,则也可以是改变了Ba:Ti的组成比和氧含量的材料,还可以是Ca置换到Ba的位点,使Ca固溶于陶瓷粒子3的几乎整体的材料。
另外,还可以使用使Ba、Ca和Ti以外的成分固溶而成的材料。这时,作为Ba、Ca和Ti以外的成分,优选Mg、Sr、Zr和Sn。对于这些元素,在与陶瓷粒子3中的核部3a进行比较时,在表面附近(距离陶瓷粒子3表面的深度为直径的1/3以下的区域)以高浓度含有的元素以一种为宜。另外,在提高介电常数(ε)和绝缘击穿电压(E)的乘积(ε×E)这一点上,优选核部3a为BaTiO3、且壳部3b含有Mg的构成。换句话说,优选为陶瓷粒子3含有镁、并且与核部相比而在壳部中以高浓度含有该镁。此处,对于陶瓷粒子3具有核壳结构的状态而言,在将特定成分(例如,Mg、Sr、Zr和Sn中的任一种)的表层附近的浓度设为1时,将这些成分的浓度为1/10以下的区域判定为核部。这时,在含有壳部3b的陶瓷粒子3中,以不含有稀土类元素和锰为宜。在陶瓷粒子3中含有Mg、Sr、Zr和Sn以外的元素(例如,稀土类元素、锰)时,由于在陶瓷粒子3中形成多个浓度梯度,因此难以区分核部和壳部。结果难以形成图3所示的具有介电常数的变化的电介质膜1。
在本实施方式的电介质膜1中,所含有的陶瓷粒子3的体积比率为2~30体积%,优选为3~20体积%,更优选为10~15体积%。
从可以形成轴比c/a不同的晶相3a、3b,实现高介电常数化的理由出发,陶瓷粒子3的平均粒径优选为50~500nm、50~300nm,特别优选为50~90nm。
构成电介质膜1的陶瓷粒子3的体积比率,在剖面观察电介质膜1时,由划分为矩形的照片内所存在的陶瓷粒子3和有机树脂5各自的比例求出。
电介质膜1的比介电常数(ε),由在从膜电容器切下的电介质膜1的两面上以规定面积形成电极层的试样求出。
在进行特性评价时,使用LCR测量器测定静电容量,由测定的静电容量、电极层的有效面积(在电介质膜的两面上重叠有电极层的面积)和电介质膜的厚度算出比介电常数。
电介质膜1的击穿电场强度(E)使用测定静电容量的试样,在电介质膜1的电极间以商用频率60Hz、每秒100V的升压速度施加电压,并由漏电流值超过1.0mA的瞬间的电压值求出。
构成本实施方式的膜电容器的电介质膜1的厚度,从高容量化的观点考虑,优选为10μm以下,特别优选为5μm以下,另一方面,从确保电介质膜1的击穿电场强度(E)、可以稳定化的理由出发,优选为1μm以上。
图5(a)是模式地表示在电介质膜的两面上具有电极层的结构的剖面图,图5(b)是模式地表示本发明的膜电容器的一种实施方式的外观剖视图。
具备上述电介质膜1的本实施方式的膜电容器由本体部23构成,所述本体部23以在电介质膜1的两面具备电极层21的构成为基本结构。由此,可以得到能够提高比介电常数且不会降低击穿电场强度的膜电容器。
需要说明的是,关于本体部23,除了将矩形的电介质膜1和电极层21交替层叠的层叠型的膜电容器以外,还可以应用于将长条状的电介质膜1和电极层21卷绕而成的结构的卷绕型的膜电容器。这些膜电容器还可以在外部电极24上具有作为端子的引线25,但是从膜电容器小型化的观点考虑,优选不具有引线25的结构。另外,从绝缘性和耐环境的观点考虑,本体部23、外部电极24和引线25的一部分可以被外装部件26覆盖。
而且,这种构成的膜电容器,通过与电路中具备的导体连接,可以形成发挥优异的整流作用的电路,可以得到安装密度高、小型的电子设备。图6中示出了将以去耦为目的的电路(膜电容器为图6中箭头所表示的位置)作为基本电路、而使用本发明的膜电容器的电子设备的例子,但本实施方式的膜电容器并不限于此,除了去耦以外,还可以同样地用于噪声除去、耦合、电压的平滑化和直流/交流转换等电路。
接着,本实施方式的电介质膜例如可以通过以下所示的制造方法得到。首先,准备用作电介质膜1母材的有机树脂。
作为有机树脂,聚对苯二甲酸乙二醇酯(PET)、聚丙烯(PP)、聚苯硫醚(PPS)、聚萘二甲酸乙二醇酯(PEN)、环烯烃聚合物(COP)、聚醚砜(PES)、聚芳酯(PAR)、聚苯醚(PPE)和聚醚酰亚胺(PEI)等是适合的。
关于这些有机树脂在室温(约25℃)下的比介电常数(ε),例如,聚对苯二甲酸乙二醇酯(PET)为3.3,聚丙烯(PP)为2.3,聚苯硫醚(PPS)为3.0,环烯烃聚合物(COP)为2.2~3.0,聚醚砜(PES)为3.4~3.7,聚芳酯(PAR)为3.1~3.4,聚苯醚(PPE)为2.5~2.7,聚醚酰亚胺(PEI)为3.1~3.3。
另外,关于这些有机树脂在室温(约25℃)下的施加交流电压(频率为60Hz)时的击穿电场强度(E),例如,聚对苯二甲酸乙二醇酯(PET)为310(V/μm),聚丙烯(PP)为380(V/μm),聚苯硫醚(PPS)为210(V/μm),环烯烃聚合物(COP)为370~510(V/μm),聚醚砜(PES)为280(V/μm),聚芳酯(PAR)为300(V/μm),聚苯醚(PPE)为420(V/μm),聚醚酰亚胺(PEI)为210(V/μm)。
作为陶瓷粒子3,具有钙钛矿结构的陶瓷粒子3是适合的,例如,使用钛酸钡系陶瓷为宜。这时,在提高陶瓷粒子3和有机树脂5的相容性方面,可以对陶瓷粒子3进行硅烷偶联处理、钛酸酯偶联处理等表面处理。
具有轴比c/a不同的2种以上的晶相的钛酸钡系陶瓷,例如,可以通过以下方式得到:使MgO等可以相对于钛酸钡固溶的、Ba、Ca和Ti以外的多种元素,部分地附着在钛酸钡粉末的表面,并对其进行加热使其在钛酸钡粉末的表面附近部分固溶。
对于具有轴比c/a不同的2种晶相的钛酸钡系陶瓷,只要使固溶的元素为1种即可。
为了得到以2种晶相形成核壳结构的方式进行配置的陶瓷粒子3,可以通过使用于固溶的元素附着于钛酸钡粉末的表面的几乎整个面,并对其进行加热而得到。这种情况下,如果用于固溶的元素为1种,则可以得到以轴比c/a不同的2种晶相形成核壳结构的方式配置、并且轴比c/a小的晶相被配置在轴比c/a大的晶相外侧的结构的陶瓷粒子3。
电介质膜1,例如,可以通过应用PET制的膜作为基材,并在其表面上形成含有陶瓷粒子3的有机树脂5的膜而得到。
作为用于成膜的溶剂,例如,可以使用甲醇、异丙醇、正丁醇、乙二醇、乙二醇单丙醚、甲乙酮、甲基异丁酮、二甲苯、丙二醇单甲醚、丙二醇单甲醚乙酸酯、二甲基乙酰胺、环己烷、或含有选自其中的2种以上的混合物的有机溶剂。
接着,通过在电介质膜1的表面蒸镀Al(铝)等金属成分而形成电极层21,接下来,卷绕形成了电极层21的电介质膜1,得到膜电容器的本体部23。
接着,在本体部23的露出电极层21的端面上形成外部电极24。对于外部电极24的形成,例如,金属的热喷涂、溅射法、镀覆法等是适合的。另外,此处还可以在外部电极24上形成引线25。接下来,在形成了外部电极24(包括引线15)的本体部23的表面形成外装树脂26,由此可以得到本实施方式的膜电容器。
实施例
选择具体的材料,制作电介质膜。首先,作为陶瓷粒子,准备表1所示的复合氧化物的陶瓷粒子。该陶瓷粒子是,将以钛酸钡为主成分的电介质材料作为核,并在其表面的整个面上使Mg、Sr、Zr和Sn作为氧化物固溶而得到的材料。需要说明的是,陶瓷粒子作为瓷器进行评价的比介电常数为1500~2500。
作为有机树脂,准备聚环烯烃聚合物(分子量:Mw=20000,比介电常数为2.2)。为了提高与有机树脂的相容性,对陶瓷粒子进行硅烷偶联处理。
接着,将上述陶瓷粒子分散在环烯烃聚合物中调制浆料。这时,加入环己烷作为稀释剂。
然后,使用涂布机将上述浆料涂布在聚对苯二甲酸乙二醇酯(PET)膜上,成形为片状。
接着,通过真空蒸镀法在电介质膜的两面上形成平均厚度为75nm的Al电极层。
接着,对于得到的电介质膜,进行以下评价。
绝缘击穿电压是在电介质膜的电极层间以商用频率(60Hz)、每秒10V的升压速度施加电压,并由漏电流值超过1.0mA的瞬间的电压值求出。
比介电常数和介电损耗角正切使用LCR测量器进行测定。具体而言,确认制作的电介质膜的电极层间有无短路后,使用LCR测量器在频率1KHz、输入信号电平为1.0Vrms的测定条件下测定电介质膜的静电容量和介电损耗。然后,由静电容量、电极层的有效面积(在电介质膜的两面上重叠有电极层的面积)和电介质膜的厚度算出比介电常数。
另外,由测定得到介电常数(ε)和绝缘击穿电压(E)求出静电能量密度(ε×E2)。
陶瓷粒子是否成为具有轴比c/a不同的2种以上的晶相的结构的判定,是将电介质膜溶解于溶剂,对提取出的陶瓷粒子实施X射线衍射,进行晶相的鉴定(选择晶面指数(400)),然后对于各个晶相而由晶格常数求出。
另外,关于电介质膜中含有的陶瓷粒子的体积比例,是将电介质膜埋入到树脂中后进行研磨,制作露出剖面的试样,并使用利用扫描型电子显微镜(SEM)拍摄的照片进行测定。测定结果与配合时的比例一致。
另外,制作应用了下述陶瓷粒子的试样(陶瓷粒子的体积百分率为10%),进行同样的评价,所述陶瓷粒子是:将用于固溶的元素(Mg)的添加量设为表1所示试样的约1/2,在陶瓷粒子的表面上,部分地形成c/a与核不同的晶相的陶瓷粒子;以及在钛酸钡粉末的表面上部分地附着2种(MgO、Y2O3),而具有轴比c/a不同的2种以上的晶相的陶瓷粒子。
[表1]
由表1的结果可知,对于包含如下陶瓷粒子的电介质膜的试样(试样No.2~13)而言,其介电常数为3以上,同时绝缘击穿电压为1440V以上,所述陶瓷粒子具有轴比c/a不同的2种晶相、并且这些晶相以形成核壳结构的方式配置。
另外,对于应用了在陶瓷粒子的表面上、部分地形成c/a与核不同的晶相的陶瓷粒子的试样而言,其介电常数为3.3,绝缘击穿电压为1250V。
另外,对于应用了在钛酸钡粉末的表面上部分地附着2种(MgO、Y2O3)、具有轴比c/a不同的2种以上的晶相的陶瓷粒子的试样而言,其介电常数为3.1,绝缘击穿电压为1320V。
在这些试样中,以钛酸钡为核部、并且将固溶于壳部的元素设为Mg的试样(试样No.2~7),其静电能量密度(ε×E2)为7,879,680以上,与使Sr、Zr和Sn中的任一种元素固溶于壳部的试样(试样No.8~13)相比,显示出高静电能量密度。
相对于此,在应用仅显示出单一轴比c/a的陶瓷粒子的试样(No.1)的情况下,介电常数为3.3,绝缘击穿电压为860V。
符号说明
1、11 电介质膜
3、13 陶瓷粒子
3a 核
3b 壳
5 有机树脂
13a 晶相
21 电极层
23 本体部
24 外部电极
25 引线
26 外装部件
Claims (6)
1.一种电介质膜,其特征在于,具有有机树脂和包含在该有机树脂中的陶瓷粒子,所述陶瓷粒子仅包含具有通过a、b和c的3个轴所形成的晶格并且轴比c/a不同的2种晶相,所述陶瓷粒子具有由核部以及设置在该核部周围的壳部而形成的核壳结构,所述核部由所述2种晶相中的一种晶相形成,所述壳部由所述2种晶相中的另一种晶相形成,所述核部为钛酸钡或含Ca钛酸钡,所述壳部在构成所述核部的材料中固溶有Mg、Sr、Zr、Sn中的任一种元素,电介质膜的静电能量密度为6220800以上。
2.根据权利要求1所述的电介质膜,其特征在于,构成所述壳部的晶相的轴比c/a小于构成所述核部的晶相。
3.根据权利要求2所述的电介质膜,其特征在于,所述陶瓷粒子是具有钙钛矿结构的陶瓷粒子。
4.根据权利要求1所述的电介质膜,其特征在于,所述陶瓷粒子含有镁,并且在所述壳部中以高于所述核部的浓度含有该镁。
5.一种膜电容器,其特征在于,具有权利要求1至4中任一项所述的电介质膜,和设置在该电介质膜上的电极层。
6.一种电子设备,其特征在于,权利要求5所述的膜电容器与电路中具备的导体连接。
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