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CN1568295A - 含有稀土、钇或铋元素的钛酸铜钠组合物 - Google Patents

含有稀土、钇或铋元素的钛酸铜钠组合物 Download PDF

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CN1568295A
CN1568295A CNA028202465A CN02820246A CN1568295A CN 1568295 A CN1568295 A CN 1568295A CN A028202465 A CNA028202465 A CN A028202465A CN 02820246 A CN02820246 A CN 02820246A CN 1568295 A CN1568295 A CN 1568295A
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dielectric substance
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M·A·苏布拉马尼安
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EIDP Inc
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Abstract

本发明提供分子式为Na0.5M0.5Cu3Ti4O12的组合物，其中M是La－Lu、Y、Bi或它们的混合物。本发明的组合物在大约1kHz到1MHz的频率范围内具有高介电常数和低介质损耗。

Description

含有稀土、钇或铋元素的钛酸铜钠组合物
本申请要求美国临时申请No.60/328,758的优先权，该临时申请于2001年10月12日提交。
技术领域
本发明涉及分子式为Na0.5M0.5Cu3Ti4O12的新组合物，其中M是La-Lu、Y、Bi或它们的混合物。
背景技术
用电介质材料提高电容器容量的方法是众所周知的并已长期使用。已知的电介质材料归于两大类。一类电介质的介电常数与温度相对无关，但其介电常数很低，例如在5-10。诸如普通电瓷和云母的材料都属于这一大类。另一大类电介质具有非常高的介电常数，如1000或1000以上，但其介电常数大小与频率有关。其中一个例子是钛酸钡(BaTiO3)。
由于电容量与介电常数成正比，所以希望材料有高的介电常数。为了满足电路应用的要求，电介质的介电常数与频率之间必须呈小的相关性。同时也希望材料有尽可能小的介质损耗或损耗因数。本发明材料满足这些需求。
发明内容
本发明提供分子式为Na0.5M0.5Cu3Ti4O12的组合物，其中M是La-Lu、Y、Bi或它们的混合物。这些组合物在1KHz-1MHZ频率范围内有高介电常数和低的介质损耗，在下列电子装置的电容器中特别有用：如移相器、网络匹配器、振荡器、滤波器、谐振器，以及包含有插指电极、三层电容、共平面型波导和微带的天线装置。
插图说明
图1表示实施例2、4、6和7的组合物的介电常数和介质损耗的变化。
具体实施方式
本发明的组合物Na0.5M0.5Cu3Ti4O12，其中M是La-Lu、Y、Bi或它们的混合物，具有电介质特性，在需要具有低频率相关性的高介电常数及低介质损耗的电子装置中具有优势。“La-Lu”在此定义为原子序数从57到71的所有镧系元素(稀土元素)。
本发明组合物可通过下列工艺合成。将按照化学计量比的原料完全混合。原料优选的是M2O3(M是La-Lu、Y、Bi或它们的混合物)、CuO、TiO2和Na2CO3。混合后的原料粉末在约900℃煅烧12小时。煅烧后粉末重新研磨后压制成直径约12.7mm，厚度1-2mm的圆片。圆片于空气中在950℃左右烧结24小时。在煅烧和烧成阶段，从室温(20-25℃)开始升温的速度都大约是每小时200℃，降温速度都大约是每小时150℃降至室温。
本发明的Na0.5M0.5Cu3Ti4O12晶相都属立方类钙钛矿Im3结构。
圆片试样可进行介电性能的测量。圆片型试样的表面先用细玻璃砂或砂纸打磨，然后在表面涂覆银电极并在70-100℃干燥。通过两端接线法用Hewlett-Packard4275A和4284A LCR电桥在25℃下测试电容和介电损耗，测量频率从约1K到约1MHz。电容(C)和介质损耗可从电桥直接读出。介电常数(K)通过测量的电容(C)皮法值按下式计算：
K＝(100*C*t)/(8.854*A)，式中t是圆片成型样品的厚度cm，A是电极的面积，单位是cm2，*指乘号。
本发明的优越性能通过下列实施例得到了验证。基于本发明的实施方案仅是举例说明，而不限制本发明的范围。
实施例1-7
实施例1-7的Na0.5M0.5Cu3Ti4O12组合物中M分别是La、Sm、Gd、Dy、Yb、Bi和Y，所述组合物通过如下工艺工程进行制备。将按化学计量比称量的Na2CO3、M2O3、CuO、TiO2原料在玛瑙研钵中充分混合。所需起始原料的克数如表1所示。
                                          表1
实施例   组成   Na2CO3     M2O3   CuO   TiO2
  1   Na0.5La0.5Cu3Ti4O12   0.0647   0.1989(La2O3)   0.5828   0.7803
  2   Na0.5Sm0.5Cu3Ti4O12   0.0641   0.2110(Sm2O3)   0.5777   0.7736
  3   Na0.5Gd0.5Cu3Ti4O12   0.0638   0.2182(Gd2O3)   0.5747   0.7696
  4   Na0.5Dy0.5Cu3Ti4O12   0.0635   0.2237(Dy2O3)   0.5725   0.7665
  5   Na0.5Yb0.5Cu3Ti4O12   0.0630   0.2345(Yb2O3)   0.5680   0.7605
  6   Na0.5Bi0.5Cu3Ti4O12   0.0614   0.2700(Bi2O3)   0.5532   0.7407
  7   Na0.5Y0.5Cu3Ti4O12   0.0672   0.1433(Y2O3)   0.6059   0.8113
在每个实施例中，混合粉末在约900℃煅烧12小时。煅烧后粉末重新研磨后压制成直径约12.7mm、厚度1-2mm的圆片。圆片于空气中在约950℃烧成24小时。在煅烧和烧成阶段，从室温开始的升温速率都是每小时约200℃，降温速率都是每小时约150℃降至室温。
通过Simens D5000衍射仪得到x射线粉末衍射图。数据表明所有样品都结晶为立方类钙钛矿Im3结构。所测量的晶格参数见表2。
                         表2
实施例   组成    晶格参数(纳米)     介电常数(105Hz在298K下)  介质损耗tanδ(105Hz)在298K下
  1   Na0.5La0.5Cu3Ti4O12     0.7420(1)     3560     0.074
  2   Na0.5Sm0.5Cu3Ti4O12     0.7395(1)     2263     0.047
  3   Na0.5Gd0.5Cu3Ti4O12     0.7388(1)     2645     0.054
  4   Na0.5Dy0.5Cu3Ti4O12     0.7379(1)     2049     0.035
  5   Na0.5Yb0.5Cu3Ti4O12     0.7361(1)     2048     0.059
  6   Na0.5Bi0.5Cu3Ti4O12     0.7412(1)     2952     0.065
  7   Na0.5Y0.5Cu3Ti4O12     0.7385(1)     2375     0.048
将圆片试样抛光以使表面平整均匀，然后被覆银电极，并在70-100℃干燥一夜。用Hewlett-Packafd 4284A LCR仪器在室温下测试电容和损耗角正切值，测量频率从1K到1MHz。25℃(298K)、约105Hz条件下测得的介电常数和损耗因数参见表2。各试样具有高介电常数和低的介质损耗。在大约103Hz到106Hz频率范围内，实施例2、4、6和7样品的介电常数和损耗因数的变化见图1所示。介电常数和介质损耗在3个量级以上频率范围内具有很小的频率相关性。

Claims (22)

1.一种组合物，其分子式为Na0.5M0.5Cu3Ti4O12，其中M是La-Lu、Y、Bi或它们的混合物。
2.一种组合物，其分子式为Na0.5M0.5Cu3Ti4O12，其中M是La-Lu。
3.一种组合物，其分子式为Na0.5M0.5Cu3Ti4O12，其中M是Y。
4.一种组合物，其分子式为Na0.5M0.5Cu3Ti4O12，其中M是Bi。
5.按照权利要求1的组合物，其中M是La、Sm、Gd、Dy、Yb、Y或Bi。
6.按照权利要求1的组合物，其中M是La。
7.按照权利要求1的组合物，其中M是Sm。
8.按照权利要求1的组合物，其中M是Gd。
9.按照权利要求1的的组合物，其中M是Dy。
10.按照权利要求1的的组合物，其中M是Yb。
11.一种提供电介质的方法，包括提供分子式为Na0.5M0.5Cu3Ti4O12的组合物，其中M是La-Lu、Y、Bi或它们的混合物。
12.按照权利要求11的的方法，其中M是Y或Bi。
13.一种含有电介质材料电容器的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是La-Lu、Y、Bi或它们的混合物。
14.一种含有电介质材料电容器的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是La-Lu。
15.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是La、Sm、Gd、Dy、Yb、Y或Bi。
16.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是La。
17.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是Sm。
18.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是Gd。
19.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是Dy。
20.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是Yb。
21.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是Y。
22.按照权利要求13的电子装置，其中所述电介质材料由分子式为Na0.5M0.5Cu3Ti4O12的组合物构成，其中M是Bi。
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CN101671178B (zh) * 2009-09-24 2012-05-30 华中科技大学 一种Bi0.5Na0.5Cu3Ti4O12巨介电非线性压敏陶瓷的制备方法
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CN101955354A (zh) * 2010-10-21 2011-01-26 华中科技大学 一种巨介电-非线性低压压敏双功能陶瓷材料及其制备方法
CN101955354B (zh) * 2010-10-21 2012-12-19 华中科技大学 一种巨介电--非线性低压压敏双功能陶瓷材料及其制备方法
CN102219508A (zh) * 2011-03-16 2011-10-19 陕西师范大学 镧取代钛酸铜铋钠巨介电陶瓷材料及其制备方法
CN102219508B (zh) * 2011-03-16 2013-04-17 陕西师范大学 镧取代钛酸铜铋钠巨介电陶瓷材料及其制备方法
CN103011814A (zh) * 2012-10-13 2013-04-03 中国计量学院 微波介质陶瓷及其制备工艺
CN103011814B (zh) * 2012-10-13 2014-05-21 中国计量学院 微波介质陶瓷及其制备工艺
CN103253933A (zh) * 2013-05-09 2013-08-21 陕西师范大学 锂取代钛酸铜镉巨介电陶瓷材料及其制备方法
CN103253933B (zh) * 2013-05-09 2015-03-25 陕西师范大学 锂取代钛酸铜镉巨介电陶瓷材料及其制备方法
CN108751977A (zh) * 2018-07-02 2018-11-06 渭南师范学院 一种低介电损耗的钛酸铜钐锂钠巨介电陶瓷材料及其制备方法
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