TWI248923B - Dielectric ceramic composition and ceramic electronic component - Google Patents

Dielectric ceramic composition and ceramic electronic component Download PDF

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Publication number
TWI248923B
TWI248923B TW093117067A TW93117067A TWI248923B TW I248923 B TWI248923 B TW I248923B TW 093117067 A TW093117067 A TW 093117067A TW 93117067 A TW93117067 A TW 93117067A TW I248923 B TWI248923 B TW I248923B
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Taiwan
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ceramic
composition
sintered compact
dielectric
weight
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TW093117067A
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English (en)
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TW200512172A (en
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Koichi Banno
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Murata Manufacturing Co
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    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
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Description

1248923 九、發明說明： 【發明所屬之技術領域】 本發明係關於介電陶究組合物，並且具體而言，係關於 一種展示高介電常數之介電陶竟組合物。其亦係關於一種 用该介電陶瓷組合物製成之陶瓷電子元件。 【先前技摘
BaTi〇3陶竟被廣泛用作高介電常數之陶竟組合物。缺 而，3爪〇3_在高頻率，即1MH_以上時展示低q值。 為了克服此問題’日本未審查專射請公開仏巧遍中教 示 了-種 SrTi〇3-MgTi〇3_CaTi〇3_Bi2〇3_Ti〇2_Cu〇 Mn〇_
Ce02陶兗組合物”盡管該組合物具有高介電常數以… MHz或以上之頻率時的高Q，且展示了介電常數相對於溫度 變化的微小變化，但體積電阻率僅為1〇12至ι〇η歐姆公分， 其不夠面。 【發明内容】 本發明之-目的係提供具有高介電常數ε及在】顧2或以 上頻率時Q值至少約為i’OOO之介電陶究組合物，其介電常 數相對於溫度變化經受微小的變化且展示高體積電阻率。 本發明之另一目的係提供一種用該介電陶究組合物製成之 陶瓷電子元件。 本發明之第一態樣係提供一種介電陶竟組合物，該組4 物包含100重量份之由通式a[(SrbCa〗 b)Ti〇n| [Βι^.ηΤ^]表示之主要組份，其中咖為各自之莫耳量J η為Ti〇2與Bi2〇3之莫耳比；w重量份（MgTi〇^ X重量^ 93616.doc 1248923
Si〇2; y重量份之Mn0m(MnC03當量）；及2重量份2Ln〇k， 其中m為1至2 ; Ln為鑭、鈽、镨、鉞、釤、銪、釓、鏑、 鈥與铒中之至少—種；且“丨.…，以便Ln〇k成為電中性 的，且其中a、b、η、w、X、y與z滿足以下條件： 0-90 S a 幺 〇·95， 0.90 < b < 0.95 ^ 18 幺 η < 3.0， 5.0 < w < lo.o , °·! ^ X < 1.0 ^ 0.1 < y < 0.3 ，及 1〇 < z < 5.0 〇 本發明之第二個態樣係提供一種包含由上述之介電陶瓷 組合物組成之陶瓷燒結壓塊的陶瓷電子元件；及在陶瓷燒 結壓塊之表面上形成的電極。 【實施方式】 現將詳細描述本發明之較佳實施例。圖1為一單電容器， 即根據本發明之一個實施例之陶瓷電子元件的部分剖面正 視圖。此單電容器係用本發明之介電陶瓷組合物製成的。 單電容器包括由本發明之介電陶瓷組合物組成之燒結壓 塊1，在燒結壓塊1之兩面形成之電極2，通過焊料3與電極2 電連接之引線4a與4b，及覆蓋燒結壓塊i之樹脂外殼5。 在此實施例中，介電陶瓷組合物包含由通式 + 表示之主要組份。介電 陶瓷組合物亦包含：相對於1 〇〇重量份之主要組份，w重量 93616.doc -6 - J248923 •份之MgTi〇3; 乂重量份之Si〇2; y重量份之 ΐ)及z重罝份之Ln〇k。在通式中，&與]3為各自之莫耳量； 及η為Ti〇2與Bi2〇3之莫耳比；至2; ^為鋼、飾、譜、 鈥、釤、銪、釓、鏑、鈥與铒中之至少一種；且415至2， 以便LnOk成為電中性的。 體而σ，氧之化合價為，鑭、镨、鈥、釤、銪、釓、 鏑、鈥與铒之化合價為+3，及鈽之化合價為+4。因此，當 Ln為選自+3化合價之元素中之至少一種日夺，U 15。當！1 為+4化合價之元素時，k為2。當Ln包括+3化合價與+4化合 價之兩種元素時，根據此等元素之比例確定k。 士此製備組合物，以便a、b、n、w、χ、y與z滿足以下條 件·· ' 0.90 < a < 0.95 ， 0.90 < b < 0.95 ^ 1.8 < n < 3.0 ^ 5.0 < w < 10.0 , 0-1 < x < 1.0 ^ 〇.1 < y < 0.3 ，及 1·〇 幺 z 幺 5.0 。 用此介電陶究組合物製成之電容器可以展示高介電常 數，即介電常數ε至少為5〇〇，在i 或以上頻率時卩值至 少約為1，000，溫度係數為_2,〇〇〇 ppm/C>c或以下，及體積電 阻率為1014歐姆·公分或以上。 現將描述製備單電容器之方法。 936l6.doc 1248923 4首先t備，，電陶究組合物。具體而言，按照上述條件 ^ 取 SrC03、CaC03、Bi2〇3、Ti〇2、吨⑽、、施叫 舁[叫並混合。將混合物及研磨介質例如氧化鍅放置罐 中，並藉由濕式遇合預定長之時間將混合物磨碎。藉由蒸 發作用乾燥磨碎之混合物，放置氧化錯外殼中，纟在約· 。至!，〇〇〇°C煅燒約2小時。然後，將煅燒過的混合物與黏 合劑例如聚乙稀醇，放置罐中並濕式混合預定長之時間。 通過脫水作用乾燥所得到的混合物，分級，並壓製形成為 預定的圓盤形的壓坦。將麼堪在約！，⑽。〇至供培2 小時以製備燒結壓塊1。 將主要由銀等組成之導電膏塗布燒結壓塊丨之兩面，並烘 焙形成電極2。藉由焊料3將引線乜及仆與電極2連接。隨 後’藉由樹脂模塑形成外殼5，以製備該電容器。 根據此方法，可以很容易製造此單電容器，該單電容器 具有高介電常數ε及在1 MHz或以上之頻率時至少約為 ，00之Q值，其介電常數相對於溫度變化經受微小之變 化’且展示高體積電阻率。 本發明不限制於以上所描述之實施例。例如，介電陶究 組合物之原料可以是鈦酸鹽化合物，例如SrTi〇3或 CaTi03，代替丁丨〇2與碳酸鹽，例如srC〇34CaC〇3。 介電陶瓷組合物可以用於製造其它之陶瓷電子元件，例 如微調電容器及單片陶瓷電容器。所得之元件亦將展示高 介電常數，高Q值，優越之溫度特性及高體積電阻率。 實例 93616.doc 1248923 準備 SrC03、CaC03、Bi2〇3、Ti02、MgTi03、Si〇2、MnC03、
Ce02、La2〇3、Pr2〇3、Nd2〇3、Sm2〇3、E112O3、Gd2〇3、Dy2〇3、
Ho203、Er203、Yb2〇3及CuO作為主要與辅助組份之原料。 根據表1分別稱重原料並混合以製備樣品混合物。如表2 所示’樣品41至43中包含預定量之Cu〇。將每一種混合物 放置於含有氧化鍅球之聚乙烯罐中，並藉由濕式混合16小 π進行磨卒藉由蒸發作用乾燥所得之磨碎之混合物，將 其放置氧化錯外殼中，並在950t锻燒2小時。 樣品號 2 a -8-9 o.o.l 89 b 0.0. η
表 W 助 I辅 一份 3 * 6 9 ο· 4 氺 8 * 9 氺
ο 1X
1X 1X
2 1X 4 1i 1X | 氺* 1_ 112 2 2 2 氺氺氺 2氺氺氺 11312 2 4 9 9 9 9 9 0·0·0·0·0. 2 2 5 9 9 9 0·0·0· ο· 0·0.0·0· 0.0·0·0·0·0·0· 222224222321 999999999999 0·0·0_0·0· 5 5 5 8 0 2 5 9 9 9 8 9 9 9 8 9 ο· 5 0 9 9 ο· ο· 5 9 ο· 254535255535 999999999999 oooooooooooo 2 X.2.2 y 000000580502500000000 1.2-2
L c C η
Z .2I.4I.3I.3I.3 ο ο 3 0. .31.3 ο 3 ο .2.2.2 .2.2 2 20-0. 2 ο
c c C
c C
C
c C 3 4 5 0 1015.19.14.18.10127.8:9:9:9:1 .5.3T.3.3.3.3.0TT.5 3 ο .3.11.21.23.11.21.21.21.2 ο ο ο
C
c c c c c c c c c c C
C 93616.doc 1248923
成電極，以製備電容器樣品。 根據以下之條件與方法確定每一種樣品之特性： 介電常數：1 MHz，1 Vrms，20°C ; Q值：1 MHz，1 Vrms，在20°C介電損失之倒數；及 溫度係數：基於+20°C之介電常數，介電常數在-25°C至 93616.doc -10- 1248923 85°C之最大變化率。 結果展示於表3與表4中。 表3 樣品 號 介電常數ε Q值 溫度係數 體積電阻 率P [ppm/°C ] [歐姆·公 分] *1 650 847 -1750 4.5xl014 2 544 1140 -1990 3.8xl014 *3 435 2540 -2330 8.7xl014 *4 568 875 -1540 5·2χ1014 5 574 1050 -1760 1·4χ10】4 6 532 1210 -1790 2.5χ1014 7 572 1080 -1960 3.5χ1014 *8 578 1260 -2080 7.2χ1014 *9 486 1450 -1990 3·6χ1014 10 514 1380 -1880 5·2χ1014 11 524 1250 -1850 4·8χ1014 12 536 1150 -1800 2·8χ1014 13 558 1030 -1710 7.5χ1014 *14 565 935 -1660 8·9χ1014 *15 542 3520 -2160 4.2χ1014 16 564 1450 -1990 2.8χ1014 *17 535 761 1850 5·6χ1014 *18 514 518 -1760 4·5χ1014 *19 576 1060 -2070 8·5χ1014 20 584 1040 -1850 4.2χ1014 *21 543 985 -1750 3·8χ1014 *22 557 854 -1670 8·2χ1014 *23 587 1060 -2110 6·5χ1014 24 542 1100 -1950 5·4χ1014 *25 486 1120 -1870 2·6χ1014 *26 452 1150 •1850 7·8χ1014 *27 752 587 -2050 2.5χ1014 28 587 1060 -1850 5·8χ1014 *29 485 1330 -1680 7·1χ1014 93616.doc -11 - 1248923
*30 389 1560 -1460 3 6y 1 0 14 3 I 602 1420 -1480 4 7 y 1 014 32 Ο 〇 584 1510 -1450 2 5v 1 014 33 Ο A 578 1520 -1470 7 8 v 1 014 34 35 564 1510 1 c 70 -1430 2.8x1014 "—-______--s--- 36 550 1 / u 1530 -1420 -1430 ^uTo 3.6X101 4.8x1014 37 538 1570 38 542 1540 O.OXlt/ 1.5xl014 ------m-- 5 6v10 4 39 ik Λ Γ\ 1550 495 1520 -1430 4 8 v 1 014 ------- 表 4 樣品 號 介電常數ε Q值 溫度係數 體積電阻 ο [ppm/°C ] —_tJI [歐姆·公 公Ί *41 538 1250 -1980 __刀J 5 2y 1 013 *42 557 1100 -1840 J · Z X 1* V*/ _4.2xl013 4.8x1013 *43 565 1180 ~~^1940 在表1至4中，加星號之樣品不在本發明範圍之内，及無 星號之樣品在本發明範圍之内。具體而言，表2與4之樣品 包含CuO且不在本發明範圍内。自表⑴清楚地看出，基 於以下原因，限制了本發明之組合物： Q值變得小於約1，000(樣品 ，介電常數變得小於500且 (1)在Bi2〇3含量！_a超出〇1時， 1)。在叫〇3含量小於〇 〇5時 溫度係數變得小於_2,000 ppm/t (樣品3)。 ⑺在SrTi〇3含量b小於0.9時，Q值變得小於約！，_(補 4)。在抓〇3含量b超纽％時，溫度係數變得小於_2，( ppm/°C (樣品 8)。 ’ (3)當Ti02與Bi2〇3之莫耳 比η小於1 · 8時 介電常數變得小 93616.doc -12- 1248923 於500(樣品9)。當11超過3時，（^值變得小於約1，〇〇〇(樣品14)。 (4) 在MgTi〇3含量W小於5時，溫度係數變得低於_2,〇〇〇 ppmrc (樣品15)。在w超過10時，q值變得小於約（樣 品17與18)。 (5) 在Si〇2含篁X小於〇·ι時，溫度係數變得低於_2,〇〇〇 ppm/°C (樣品19)。在X超過h0時，q值變得小於約（樣 品21與22)。 (6) 當Mn〇m含量_=1至2，等量的MnC〇3)小於〇1時溫 度係數變得低於-2,000 ppm/t(樣品23)。當7超過〇·3時，介 電常數變得小於500(樣品25與26)。 (7) 在LnOk含量ζ小於丨.〇時，q值變得小於約以⑼，且溫 度係數變得低於-2,〇00卯111/。(：（樣品27)。在2超過5〇時，介 電常數變得小於500(樣品29與30)。 (8) 當Ln為不同於上述之元素時，介電常數變得小於 (樣品40)。 (9) 含有Cu〇之樣品之體積電阻率低於1〇M歐姆.公分（樣 品41至43)。 【圖式簡單說明】 圖1為一單電容器’即用㈣本發明之一個實施例之介電 陶瓷組合物製成之陶瓷電子元件的部分剖面正視圖。 【主要元件符號說明】 1 燒結壓塊 2 電極 3 焊料 93616.doc 1248923 4a 、 4b 引線 5 外殼
93616.doc -14-

Claims (1)

1248923 L 十、申請專利範圍： i 一種介電陶瓷組合物，其包含： 100 重量份之由通式 a[(Srbcai_b)Ti03；Kl-a)[Bi203.nTi02]表示 之主要組份，其中a與b為各自之莫耳量，及11為Ti〇2與 出2〇3之莫耳比； w重量份之MgTi03 ; x重量份之Si02 ; y重置份之MnOm(^f算出作為％11(：：〇3當量）；及 z重量份之Ln〇k， 釤、銪、乱、 以便LnOk為電 其中Π1為1至2; Ln為鑭、鈽、镨、敍 鏑、欽與錦中之至少一種；且鸸15至2 中性的， 其中a、b、n、w、x °·9〇 ^ a < 0.95 ^ °·9〇 ^ b < 0.95 , i·8 幺 η 幺 3.0 ， 5·0 ^ w < ι〇β〇 , °·1 ^ X ^ 1.0 , 0·1 $ y $ 0.3 ，及 h〇 S z 幺 5.0。 y與z滿足以下條件： 2· τ 項1之介電陶瓷組合物 0,91 ^ ^ < 0.95 , 〇·92 …0.95， 1,8 ^ η ^ 2.5 ， 93616.doc 1248923 7.0 < w < 9.5 » 0.2 < x < 0.5 ^ ^ 2.0 < z < 3.0 。 3·如請求項2之介電陶瓷組合物，其中該Ln為鈽。 4·如請求項2之介電陶瓷組合物，其中該組合物不包含Cu。 5.如請求項2之介電陶瓷組合物，其中〇·92< 0.95。 6·如請求項1之介電陶瓷組合物，其中該。為鈽。 7· 一種陶瓷電子元件，其包括： 一包含如請求項6之介電陶瓷組合物之陶瓷燒結壓 塊；及 一在該陶瓷燒結壓塊表面上之電極。 8· 一種陶瓷電子元件，其包括·· 一包含如請求項5之介電陶瓷組合物之陶瓷燒結壓 塊；及 一在該陶瓷燒結壓塊表面上之電極。 9· 一種陶瓷電子元件，其包括·· 一包含如請求項4之介電陶瓷組合物之陶瓷燒結壓 塊；及 一在該陶瓷燒結壓塊表面上之電極。 ίο. —種陶瓷電子元件，其包括： 包含如請求項3之介電陶瓷組合物之陶瓷燒結壓 塊；及 —在該陶瓷燒結壓塊表面上的電極。 U.—種陶瓷電子元件，其包括： 93616.doc 1248923 一包含如請求項2之介電陶瓷組合物之陶瓷燒結壓 塊；及 一在該陶瓷燒結壓塊表面上之電極。 12. —種陶瓷電子元件，其包括： 一包含如請求項1之介電陶瓷組合物之陶瓷燒結壓 塊，及 一在該陶瓷燒結壓塊表面上及電極。
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