CN1336347A - 压电陶瓷块和压电陶瓷器件 - Google Patents

压电陶瓷块和压电陶瓷器件 Download PDF

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CN1336347A
CN1336347A CN01117270A CN01117270A CN1336347A CN 1336347 A CN1336347 A CN 1336347A CN 01117270 A CN01117270 A CN 01117270A CN 01117270 A CN01117270 A CN 01117270A CN 1336347 A CN1336347 A CN 1336347A
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piezoelectric ceramics
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CN1149181C (zh
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木村雅彦
泽田拓也
安藤阳
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Murata Manufacturing Co Ltd
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Abstract

提供一种作为制造压电陶瓷器件等有效材料的压电陶瓷块,包含SrBi2Nb2O9作为主要组分,不含或只含少量的铅或铅化合物,具有提高到适合实际使用水平的最大值Qmax。它包含由Sr、Bi、Nb和氧组成的层状铋化合物作为主要组分,所含作为层状铋化合物主要组分的Sr、Bi和Nb的摩尔比值以a∶b∶c表示,保持着0.275≤a/c<0.5和4≤(2a+3b)/c≤4.5的关系。

Description

压电陶瓷块和压电陶瓷器件
本发明涉及压电陶瓷以及使用该压电陶瓷的压电陶瓷器件。具体而言，本发明涉及可用作制造压电陶瓷器件如压电陶瓷滤波器、压电陶瓷振荡器和压电陶瓷谐振器有效材料的压电陶瓷块，还涉及使用该压电陶瓷的压电陶瓷器件。
主要包含钛锆酸铅(Pb(TixZr1-x)O3)或钛酸铅(PbTiO3)的压电陶瓷块常规地用于压电陶瓷器件如压电陶瓷滤波器、压电陶瓷振荡器和压电陶瓷谐振器。然而，这类主要包含钛锆酸铅或钛酸铅的压电陶瓷块，在组成上含有大量铅组分，氧化铅在制备步骤中会由于蒸发，而影响所制器件性能均匀性的问题。为避免这个问题，优选使用不含或含少量铅的压电陶瓷块。
主要包含层状铋化合物如SrBi2Nb2O9的压电陶瓷块，因其组成中不含氧化铅，不会有上述问题。
一般用于压电陶瓷器件，尤其是压电陶瓷振荡器等的材料，在从谐振频率到反谐振频率范围的带宽上，其电品质因素Q(1/tanδ)一般宜具有最大值Qmax。然而，主要包含层状铋化合物如SrBi2Nb2O9的压电陶瓷块，存在的问题是不可能获得足供实际应用的最大值Qmax。
因此，本发明的一个主要目的是提供一种压电陶瓷块，可作为制造压电陶瓷器件的有效材料，它主要包含SrBi2Nb2O9，不含或含少量铅化合物，其最大值Qmax提高到适合实际使用的水平。另外，本发明提供使用上述压电陶瓷块的压电陶瓷器件。
根据本发明，在主要包含由Sr、Bi、Nb和氧组成的层状秘化合物的压电陶瓷块中，当作为主要组分的层状铋化合物所含Sr、Bi和Nb摩尔比值，用a∶b∶c表示时保持着0.275≤a/c＜0.5和4≤(2a＋3b)/c≤4.5的关系。
本发明的压电陶瓷块还可包含一种Sr之外的二价金属或一种除Bi之外的三价金属，其含量为，相对于1摩尔主要组分之一的Nb，在大于0至0.1摩尔范围。这种情况下，压电陶瓷块所含Sr之外的二价金属元素较好的是至少一种选自Mg、Ca、Ba或Pb的元素；另外，压电陶瓷块所含除Bi之外的三价金属元素较好的是至少一种选自Sc、Y、La、Ce、Pr、Nd、Sm、Gd、Dy、Er或Yb的金属。
本发明的压电陶瓷块还包含Ta，相对于1摩尔主要组分之一的Nb，其含量为大于0至0.25摩尔。
另外，本发明的压电陶瓷块还包含锰，按MnCO3计，其含量为大于0％(重量)至1.5％(重量)。
本发明的压电陶瓷器件包括本发明的压电陶瓷块和为压电陶瓷块供给的电极。
在这方面，本发明的压电陶瓷块是一种对压电陶瓷块的原料组合物进行烧结形成的烧结材料；然而，观察到在烧结前后，上述组成比几乎没有什么变化。
根据本发明，在主要包含由Sr、Bi、Nb和氧组成的层状秘化合物的压电陶瓷块中，当作为主要组分的层状铋化合物所含Sr、Bi和Nb摩尔比值用a∶b∶c表示时，保持着0.275≤a/c＜0.5和4≤(2a＋3b)/c≤4.5的关系。其原因是当组成超出上述关系范围时，不能获得足供实际应用的Qmax。
另外，当本发明的压电陶瓷块还包含一种Sr之外的二价金属或一种除Bi之外的三价金属，其含量为相对于1摩尔主要组分之一的Nb，在大于0至0.1摩尔范围时，本发明的优点更为显著。压电陶瓷块包含相对于1摩尔Nb大于0至0.1摩尔一种除Sr外的二价金属或除Bi外的三价金属，其原因是，当它们的含量超出上述范围时，与不含这些金属元素的情况相比，Qmax反而较小。
另外，当本发明的压电陶瓷块还包含相对于1摩尔主要组分之一的Nb，在大于0至小于0.25摩尔范围的Ta时，本发明的优点更为明显。压电陶瓷块包含的Ta在上述范围的原因是当其含量超出上述范围时，与不含Ta的情况相比，Qmax反而较小。
而且，当本发明的压电陶瓷块还包含按MnCO3计在大于0至1.5％(重量)范围的Mn时，本发明的优点更为明显。压电陶瓷块包含的Mn在上述范围的原因是当该含量超出上述范围时，与不含Mn的情况相比，Qmax反而较小。
由下面对实施方案的详细描述，能更好地理解本发明上述目的、另一些目的、特征和优点。
图1是本发明一个压电陶瓷谐振器例子的透视图；
图2是图1所示压电陶瓷谐振器的剖面图。
实施例
作为原料，制备SrCO3、Bi2O3、Nb2O5、CaCO3、BaCO3、La2O3、Nd2O3、Ta2O5和MnCO3，然后按SraBibNbcO9＋x摩尔Me＋y摩尔Ta＋z重量％MnCO3表示的组成称量配料，上式中Me指Ca、Ba、Nd或La；a、b、c、x、y和z的值示于表1和表2。所得组成的配料在球磨机中湿混约4小时，获得一混合物。进行干燥后，在700-900℃煅烧该混合物，制得煅烧产物。将煅烧产物粗粉碎，在粗粉碎产物中加入适量有机粘合剂，在球磨机中湿磨4小时。将湿磨产物通过一个40目筛，控制粉末的粒度。然后在1000kg/cm2压力下将粉末压制成直径12.5mm，厚2mm的圆片，然后在1000-1300℃，进行空气烧结，获得陶瓷圆片。以常规方式，在陶瓷圆片表面(两个主平面)上施加银浆然后进行烘焙，形成银电极。最后将陶瓷圆片在150-200℃绝缘油中，施加5-10kv/mm直流电压10-30分钟，进行极化处理，制得一压电陶瓷片(样品)。
测定上述样品即圆片谐振器以厚度延伸振动模式为基波时的Qmax。结果列于表1和表2。
                                    表1
   样品No.    a    b    c    Me    x   y     z    烧结温度(℃)    Qmax
1＊ 0.5 2.5 2.0    -    0   0     0      1100     8.3
2＊ 0.55 2.2 2.0    -    0   0     0      1200     9.2
3 0.55 2.3 2.0    -    0   0     0      1150    15.2
4 0.55 2.6 2.0    -    0   0     0      1050    16.6
5＊ 0.55 2.7 2.0    -    0   0     0      1050     9.4
6＊ 0.6 2.2 2.0    -    0   0     0      1200     8.7
7 0.6 2.3 2.0    -    0   0     0      1150    16.2
8 0.6 2.6 2.0    -    0   0     0      1050    16.7
9＊ 0.6 2.7 2.0    -    0   0     0      1050     9.2
10＊ 0.8 2.1 2.0    -    0   0     0      1150     9.5
11 0.8 2.2 2.0    -    0   0     0      1100    18.8
12 0.8 2.4 2.0    -    0   0     0      1050    19.1
13＊ 0.8 2.5 2.0    -    0   0     0      1050     9.5
14＊ 1.0 2.0 2.0    -    0   0     0      1250     9.8
15＊ 0.8 2.1 2.0   Nd    0.1   0     0      1150     9.7
16 0.8 2.2 2.0   Nd    0.1   0     0      1100    22.2
17 0.8 2.4 2.0   Nd    0.1   0     0      1050    23.1
18＊ 0.8 2.5 2.0   Nd    0.1   0     0      1050     9.8
19＊ 0.8 2.1 2.0   Nd    0.2   0     0      1150     9.4
20 0.8 2.2 2.0   Nd    0.2   0     0      1100    20.3
21 0.8 2.4 2.0   Nd    0.2   0     0      1050    20.6
22＊ 0.8 2.5 2.0   Nd    0.2   0     0      1050     9.6
23＊ 0.8 2.4 2.0   Nd    0.25   0     0      1200     7.8
24＊ 0.8 2.1 2.0   Ba    0.1   0     0      1050     9.6
25 0.8 2.2 2.0   Ba    0.1   0     0      1150    22.0
26 0.8 2.4 2.0   Ba    0.1   0     0      1050    22.6
27＊ 0.8 2.5 2.0   Ba    0.1   0     0      1200     9.5
28＊ 0.8 2.1 2.0   Ba    0.2   0     0      1150     9.1
29 0.8 2.2 2.0   Ba    0.2   0     0      1050    19.4
30 0.8 2.4 2.0   Ba    0.2   0     0      1050    20.1
                                    表2
   样品No. a b c Me x y z    烧结温度(℃) Qmax
31＊ 0.8 2.5 2.0   Ba 0.2  0 0     1050     9.3
32＊ 0.8 2.4 2.0   Ba 0.25  0 0     1200     7.2
33 0.8 2.4 2.0   Ca 0.1  0 0     1050     18.6
34 0.8 2.4 2.0   Ca 0.2  0 0     1050     18.1
35＊ 0.8 2.4 2.0   Ca 0.25  0 0     1050     8.9
36 0.8 2.4 2.0   La 0.1  0 0     1050     20.5
37＊ 0.8 2.1 2.0   - 0  0.1 0     1150     9.3
38 0.8 2.2 2.0   - 0  0.1 0     1100     21.2
39 0.8 2.4 2.0   - 0  0.1 0     1050     20.7
40＊ 0.8 2.5 2.0   - 0  0.1 0     1050     9.8
41＊ 0.8 2.1 2.0   - 0  0.2 0     1050     9.1
42 0.8 2.2 2.0   - 0  0.2 0     1150     20.1
43 0.8 2.4 2.0   - 0  0.2 0     1050     19.4
44＊ 0.8 2.5 2.0   - 0  0.2 0     1200     9.3
45＊ 0.8 2.4 2.0   - 0  0.25 0     1050     6.7
46＊ 0.8 2.1 2.0   - 0  0 1     1200     9.9
47 0.8 2.2 2.0   - 0  0 1     1100     19.7
48 0.8 2.4 2.0   - 0  0 1     1050     20.1
49＊ 0.8 2.5 2.0   - 0  0 1     1050     9.5
50＊ 0.8 2.1 2.0   - 0  0 1.5     1200     9.5
51 0.8 2.2 2.0   - 0  0 1.5     1050     18.2
52 0.8 2.4 2.0   - 0  0 1.5     1050     18.8
53＊ 0.8 2.5 2.0   - 0  0 1.5     1150     9.6
54＊ 0.8 2.1 2.0   - 0  0 1.6     1100     8.8
注：在样品一栏中的*指超出本发明范围的样品。
表1和表2中，Qmax是同样组成的样品在不同条件(原料混合物的煅烧温度、烧结温度、进行极化的绝缘油温度和DC电压)下所能获得的最大Qmax的值。另外，尽管Qmax随样品形状、振动模式、电极类型等变化，当在此实施方案条件下实施本发明获得的Qmax为10或更大时，可认为该样品适合于实际应用。
由表1和表2可知，本发明这一实施例的所有样品的Qmax均为10或更大，因此，可清楚地理解，这些样品是制造压电陶瓷器件，尤其是压电陶瓷振荡器等的有效材料。
另外，本发明这一实施例的样品，由于是在比SrBi2Nb2O9压电陶瓷低的烧结温度下获得各样品最大Qmax的，可以确认降低烧结温度的辅助性优点。因为降低了烧结温度，可以获得降低烧结所需的能量例如电能，可以延长烧结时装压电陶瓷的坩埚等容器的寿命，从而能降低制造成本。
另外，本发明的压电陶瓷块不限于上述实施例的组成，可使用在本发明组成范围的任何类型的压电陶瓷块。
另外，在上述实施例中，以举例方式报导了圆片谐振器在厚度延伸振动模式中的Qmax；然而，本发明的优点不限于这些，除了厚度延伸振动情况外，本发明可有效应用于压电陶瓷器件尤其是压电陶瓷振荡器用的其它振动模式，如切变振动或厚度延伸振动谐波。
例如，T.Atsuki等人在Jpn.J.Appl.Pys.，Vol.34，Part 1，9B，pp5096-5099，关于用于铁电存储器薄膜材料的层状铋化合物SrBi2Ta2O9一文中，报道了当该层状铋化合物组成调整为Sr0.7Bi2.4Ta2O9等时，残余极化获得改善。然而，本发明的组成不同于上述文献所公开的组成。而且，本发明的目的是提供制造压电陶瓷器件材料用的有效压电陶瓷块，因此，本发明的应用范围不同于上述化合物的应用范围。而且，用于制造铁电存储器的材料所要求的性能不同于制造压电陶瓷器件用材料的性能，因此，由T Atsuki等进行的研究难以推想出本发明。
图1是本发明压电陶瓷振荡器一个例子的透视图，图2是其剖面图。图1和图2所示的压电陶瓷振荡器10包括一个形状例如为长方体形的压电陶瓷块12。压电陶瓷块12包括两层压电陶瓷层12a和12b。它们由本发明上述的压电陶瓷片制造，通过相互层叠为一整体。此外，压电陶瓷层12a和12b按照图2中箭头所示的同一厚度方向进行了极化。
在压电陶瓷层12a和12b之间的中心，在压电陶瓷块12的中心位置提供了一个例如圆片形的振动电极14a，并由其形成一个T形的引导电极16a，它从振动电极14a伸出到压电陶瓷块12的一个端面。另外，在压电陶瓷层12a表面的中心，形成例如一个圆片形的振动电极14b，并形成一个T形的引导电极16b，从振动电极14b伸出到压电陶瓷块12的另一个端面。而且在压电陶瓷层12b表面的中心，形成一个例如圆片形的振动电极14c，并形成一个T形的引导电极16c，从振动电极14c伸出到压电陶瓷块12的另一个端面。
一个外接头20a通过引线18a连接到引导电极16a，另一个外接头20b通过另一根导线18b连接到引导电极16b和16c。
在这方面，本发明不仅可应用于上述压电陶瓷振荡器10所示的元件结构和其中所激发的振动模式，还可以应用于使用其它器件结构和振动模式(例如切变振动和厚度延伸第三谐波)的其它压电陶瓷器件，例如压电陶瓷振荡器、压电陶瓷滤波器、压电陶瓷谐振器。
根据本发明制造的压电陶瓷块可作为制造压电陶瓷器件等的有效材料，它主要包含SrBi2Nb2O9，不含或只含少量的铅或铅化合物，具有提高到适合实际使用水平的最大值Qmax。

Claims (7)

1.一种压电陶瓷块，主要包括含Sr、Bi、Nb和氧的层状铋化合物，作为主要组分的层状铋化合物所含Sr、Bi和Nb的摩尔比值用a∶b∶c表示，保持着0.275≤a/c＜0.5和4≤(2a＋3b)/c≤4.5的关系。
2.如权利要求1所述的压电陶瓷块，其特征在于所述的压电陶瓷块还包含一种Sr之外的二价金属元素和一种除Bi之外的三价金属元素，其含量为，相对于1摩尔的Nb，在大于0至0.1摩尔的范围。
3.如权利要求2所述的压电陶瓷块，其特征在于所述除Sr之外的二价金属元素是至少一种选自Mg、Ca、Ba和Pb的元素。
4.如权利要求2所述的压电陶瓷块，其特征在于所述除Bi之外的三价金属元素是至少一种选自Sc、Y、La、Ce、Pr、Nd、Sm、Gd、Dy、Er和Yb的元素。
5.如权利要求1所述的压电陶瓷块，其特征在于所述压电陶瓷块还包含Ta，其含量为，相对于1摩尔Nb，在大于0至小于0.25摩尔的范围。
6.如权利要求1所述的压电陶瓷块，其特征在于所述压电陶瓷块还包含Mn，按照MnCO3计，其重量百分数在大于0至1.5％的范围。
7.一种压电陶瓷器件，包括如权利要求1-6中任一权利要求所述的压电陶瓷块和为该压电陶瓷块提供的电极。
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CN100522873C (zh) * 2005-12-30 2009-08-05 中国科学院上海硅酸盐研究所 一种铋层状结构弛豫铁电陶瓷材料及其制备方法

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CN100522873C (zh) * 2005-12-30 2009-08-05 中国科学院上海硅酸盐研究所 一种铋层状结构弛豫铁电陶瓷材料及其制备方法

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