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TWI235141B - Microwave dielectric ceramic composition - Google Patents

Microwave dielectric ceramic composition Download PDF

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TWI235141B
TWI235141B TW090126690A TW90126690A TWI235141B TW I235141 B TWI235141 B TW I235141B TW 090126690 A TW090126690 A TW 090126690A TW 90126690 A TW90126690 A TW 90126690A TW I235141 B TWI235141 B TW I235141B
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dielectric
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Tomoki Fukagawa
Kazuhiro Nishikawa
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Sumitomo Spec Metals
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Description

1235141
拮術領域 口 關於數GHZ帶之微波領域中所用之共振器材料 或電合為材料等所使用的微波用介電質磁器 背景技名好 、、、取 近年，於利用數GHZ帶之微波之衛星通信播送或移 識別裝置等之送受信機所用之共振器、濾光/ a
乃使用介電質。 ％ a的T 此種”電質磁器材料例如已提案以卜丁^一^^仏一以以系 組成物（特開昭6 1 -8806號公報）。前述組成物為介電率之 為no左右’構成介電質共振ι§或電容器時，因為使 用介電率之愈大之材料，則共振器之尺寸可愈縮小，故期 望具有更大介電率^之材料。 以往，介電率ε大之材料例如為S r T i 03、C a T i 〇3等，其介 電率之雖非常大至3 0 0及1 8 0，但因共振周波數之溫度係數 !^為非常大至+ 17〇〇13_/^：及+ 8 0 0??111/。(：，故無法使 用〇 因此’令介電質磁器組成物之溫度係數r f下降之方法 為將儘可能令介電率ε為大，且溫度係數τ f為負值之材 料予以組合之方法，若根據此方法，則經由適當之組合則 了取彳于介電率£為大，且共振周波數之溫度係數^ f小之 磁裔組成物。 例如，於特開平5 - 2 1 1 0 0 9號公報中，介電率£為大、且 概度係數r f為負值之材料乃提案經由組合組成式為以 (Al+1/2、B3+1/2)Ti03 表示，且ΑΓ 為Li1+、B3+ Nd3+、Sm3+、Co3+
1235141 五、發明說明（2) 次h之材料’取得介雷至 ^ , 係數μ為接近〇之磁器物為大、且共振周波數之溫度· 迫:】是並於携帶型電子終端機器之小型化的要求 器：介ίΐΓ:類裝置所使用之共振器、遽光片、電容 中，強烈要求使用具有更高介…之材料。 本發明為鏗於微波用介電皙 經由在共振周波數之、、…:：磁：且成物所要未之特性’ 中度係數T f為負侧大之磁器組成物 大二口 口 T f於正側大之磁器組成物，取得介電率ε 以振周波數之溫度係數rf為接近。、且〇值大：：； '磁态組成物為其目的。 數Λ者接等二’於。取得介電率ε A、共振周波數之溫度係 f為接近〇、且Q值大之介電質磁器組成物之目的中， R ηΥ 案組成式為以Li2〇~Na2〇_Bi2〇3~R2〇3_Ti02 表示，且 ^為含人有u:〇3、、^d2〇3、、Sm2〇3、c〇2〇3或叫之一種或二種 之"電質磁器組成物（特願2〇〇〇 —337141號）。 又，本發明者等人提案組成式為以 =2〇-Bi2〇3-R2〇3-SrTi〇3U，且㈣為含有U2〇3 ,2〇3、 2 3、C〇2〇3或Ρι·2〇3之一種或二種以上之介電質磁器组成 物（特願 2 0 0 0 - 3 4 0 1 0 4 號）。 〆發明者等人為再進行致力檢討，結果發現Li2〇〜—Ti〇 糸組成物且R為La、Nd、Pr、sm中之一種或二種以上3，且2 共同具有特定量之BiA、N^O及M〇(M:Ca、Sr之一種或二 種），則可安定取得優良之介電特性。 \\312\2d-code\91-01\90126690.ptd 第5頁 1235141
五、發明說明（3) 經I丄ί發2者等人為發現MLi2〇-R2〇3-Ti〇2系組成物中， 量之m3〇H定1之Bi_l〇3，提高介電率ε ，且經由含有特定 側 、， Sr之一種或一種），不僅可令r f移動至正 側，亚且取得Qf之大幅的改善效果。 正 於ί i卜並經由含有肋，貝…變得過大’難將Qf保持 二種）丑F1人7 Τ ^接近〇，故經由令㈣⑼：以、Sr之一種或 中，/、5 B有特定量之Na2〇，則特別於ε r >150之材料 成本：為高值，並且可將rf控制於0附近，因而完 即，本發明為組成式為以 =、l2〇:bNa2〇 —cR2〇3 —dBi2〇3 —eM〇 —fTi〇2(a + b + c + d + e + f = 1〇〇， P (： (1、6、€為莫耳％)表示，且1?為含有“、3111、 二猫La中之一種或二種以上，M為含有ca、^中之一種 :’ 8、1"、（：、（1、6、1?為滿足5<8<15、0<13<1〇、3 波 <d <15、1 <e <30、40 <f <75 為其特徵之微 最佳f祐.揪能 於本發明中L“。-Na2Q_RL_MQ_Tm成物⑺： n一d ^、Pr、La之一種或二種以上，MACa、計之一種或 = )Ά20未滿5莫耳％則介電率低，且"於正侧變得 f15^%mi2()為低溶點，燒結時磁器組成 =為與敷板和敷粉反應而具有溶枯之問題，故為不佳。因 此’ Ll20(a)為以5 <a <15莫耳％之範圍。 又’Na2〇若超過10莫耳％則“於正侧變得過大，並且具
\\312\2d-code\91-01\90126690.ptd 第6頁 1235141 五、發明說明（4) 有令Qf降低之問題，故為不佳。因〇( 10莫耳％之範圍。 2…為以0<b< . R2〇3 (R3+ 為 Nd3+、Sm3+、pr3+、La3+ 中之一種戍二藉 未滿3莫耳％則介電率低，且q亦變差，ϋ )為 …效果，且費用變高，故為不佳。因此' <15莫耳％之範圍。 2U3U)為以3<c =〇3為具有令—介電率ε提高之效果，必須至少含扪莫 〇 ，因低熔點故若超過1 5莫耳％，則恐於燒&時磁 -J ^ γ a a ^ ^ ^ 〇 -；；", ^
Ki2〇3(d)為以1 <d <15莫耳％之範圍。 J产ί Γ〇!Μ: 'a广之一種或二種)則具有提高Qf及提 :μ度係數r f之效果，但未滿！莫耳％，則Qf之提 ;\度:數提高效果少，若超過30莫耳%則溫度係數r 30莫耳過大，故為不佳。因此，M〇(e)為以1 <e< 3 U莫耳％之範圍。 i且’Ti〇2未滿40莫耳％則無法取得所要的結晶相，且 ”，得所要的介電特性，若超過75莫耳%則出 之 早體相，具有Qf顯著降低之問題，故為不佳。因此， Ti〇2(f)為以40 <f <75莫耳％之範圍。 實施例 以取得組成式為aLi20-bNa2〇-cR2〇3-dBi2〇3 — eM〇-fTi U + b + C + d + e + f = 1〇〇’a、b、c、d、e、u^w，R^d、
Sm、Pr、La中之一種或二種以上，M為。、&中之一種或 二種）之混合物地，於原料中將Ti〇2、BiA、Li^、 1235141 五、發明說明（5)
Nd2 03 Sm2 03、、La2 03、Na2C03、cac〇3、src〇3 之高純- 度粉末以所需之莫耳分率如表1〜表2秤量、配合，並以球 磨混合5〜2 0小時。 前述混合後，於70 0它〜lOOfTC進行i小時〜5小時俨 燒。其後再粉碎2〜50小時，並於前述粉碎粉中加入^ 钻合劑且造粒、分級後，以2〜3 T / cm2之壓力成形為斤 1 0 mm、厚度6 mm之圓板狀。將前述成形體於丨2 〇 〇它二 杈 °C燒結1〜5小時後，將燒結體之厚度兩面研磨成〜1 1 / 2，作成測定試料。 彳泛之 波數 。表
所得之測定試料使用H a c k & c 〇 r m a η η法，以測定 3GHZ測定介電率ε、Q值及共振周波數之溫度係數 3示出測定試料之介電特性之測定結果。
\\312\2d-code\91-01\90126690.ptd
1235141 五、發明說明（6) 表1
Li2〇 Na2〇 R2〇3(R = Na，Sm，Pr，La) (a) (b) (c) 本 發 明 例 1 9.50 3.97 Sm3 + 8.77 2 10.58 4.31 9.03 3 10.00 5.02 9.57 4 9.70 5.56 9.98 5 10.50 0.38 Nd3 + 7.97 6 10.75 0.69 8.24 7 9.80 0.93 8.44 8 10.70 1.24 8.72 9 8.00 4.01 Pr3+ 〇.5 + Nd3 + 〇.5 5.86 10 9.40 4.35 6.06 11 7.00 5.03 6.45 12 8.00 5.38 6.65 13 9.00 0.30 Pr3 + 6.60 14 9.00 0.60 6.86 15 7.00 0.90 7.11 16 7.00 1.20 7.37 17 8.00 4.14 La3 + 〇.5 + Nd3 + 〇.5 6.85 18 9.00 4.49 7.05 19 9.50 5.19 7.47 20 7.00 5.56 7.68 比 較 例 1 10.50 0 Nd3 + 7.64 2 9.00 0 pr3 + 6.35 3 8.82 0 La3 + 4.41 4 9.50 4.14 Sm3 + 13.69 5 10.50 0.30 Nd3 + 10.98 6 9.00 0.30 pr3 + 9.17 7 8.00 8.33 Pr3 + 〇.5 + Nd3 + 〇.5 8.33 8 9.00 6.67 Pr3 + 12.00 9 8.00 6.67 La3 + 〇.5 + Nd3 + 〇.5 8.33 C:\2D-CODE\91-01\90126690.ptd 第9頁 1235141 五、發明說明（7)表2
Bl2〇3 MO Ti〇2 (d) CaO(e) SrO(e) (f) 本 發 明 例 1 4.72 0.00 9.52 63.52 2 4.86 0.00 8.31 62.90 3 5.15 0.00 5.83 64.43 4 5.38 0.00 3.92 65.46 5 3.10 16.79 0.00 61.26 6 3.20 15.67 0.00 61.44 7 3.28 14.81 0.00 62.73 8 3.39 13.66 0.00 62.28 9 5.86 14.81 0.00 61.44 10 6.06 13.66 0.00 60.48 11 6.45 11.32 0.00 63.75 12 6.65 10.13 0.00 63.20 13 2.57 22.49 0.00 59.05 14 2.67 21.43 0.00 59.45 15 2.77 20.36 0.00 61.86 16 2.87 19.28 0.00 62.28 17 6.85 8.92 0.00 65.25 18 7.05 7.69 0.00 64.72 19 7.47 5.19 0.00 65.18 20 7.68 3.92 0.00 68.16 比 較 例 1 2.97 18.18 0.00 60.71 2 2.47 23.53 0.00 58.85 3 4.41 23.53 0.00 58.82 4 0 0.00 8.92 63.75 5 0 17.07 0.00 61.15 6 0 22.49 0.00 58.05 7 8.33 0.00 0.00 67.00 8 4.67 0.00 0.00 67.67 9 8.33 0.00 0.00 68.67 〇
C:\2D-C0DE\91-01\90126690.ptd 第10頁 1235141 五、發明說明（8)表3 介電特性 er Qf(GHz) xf(ppm/°C) 本 發 明 例 1 131 3202 17 2 133 3134 8 3 135 3198 -2 4 137 3157 -6 5 151 2132 10 6 153 2107 3 7 155 2064 -5 8 157 1987 -12 9 167 1767 22 10 170 1723 14 11 173 1702 0 12 175 1678 -8 13 179 1545 14 14 182 1512 2 15 185 1448 -4 16 188 1398 18 17 198 1312 23 18 202 1280 10 19 208 1223 1 20 217 1187 -5 比 例 1 151 2209 41 2 180 1533 86 3 205 1109 143 4 111 3256 35 5 129 2389 68 6 142 1644 123 7 165 978 4 8 177 745 -5 9 195 465 2
C: \2D-CODE\91 -01 \90126690. ptd 第11頁 1235141 五、發明說明（9) 產業上之可利用性 丨 於Li2〇 -R2O3 — Ti〇2系組成物中，含有特定量之提南 介電率ε ，並經由含有特定量之MO(M:Ca、Sr之一種或二 種），令τ f移動至正側，大幅改善Q f，再經由含有 Μ 0 (M : C a、S r之一種或二種）和特定量之N a2 0，特別於ε r > 150之材料中，可保持Qf為高值，並且將7： f控制於0附 近。 根據本發明之介電質磁器組成物，如實施例所闡明般， 介電率ε為大、共振周波數之溫度係數r f為接近0，取得 大的Q值，最適於利用數GHZ帶之微波之衛星通信放送或移 0 動體識別裝置等之送受信機中所用之共振器、濾光片、電 容器的介電質。
\\312\2d-code\91-01\90126690.ptd 第12頁 1235141 圖式簡單說明 Φ C:\2D-CODE\91-01\90126690.ptd 第13頁

Claims (1)

1235141 六、申請專利範圍 1. 一種微波用介電質磁器組成物，其為以組成式為 aLi20 - bNa〗。- cR2〇3 - dBi2〇3~eMO - fT i〇2 (a + b + c + d + e + f 二 1 00，a 、b、c、d、e、f為莫耳％)表示，且R為含有Nd、Sm、Pr、 La中之一種或二種以上，且M為含有Ca、Sr中之一種或二 種，a、b、c、d、e、f為滿足下述值 5 < a < 1 5、0<b<10、3<c<15、 1 <d < 15 、l<e<30 、40< f <75 。
C:\2D-CODE\91-01\90126690.ptd 第14頁 申請曰 ^ 案號：90126690 年r! 類別：1 »·». IJ« III· 1. ·*. * ......... ··,, (以上各欄由本局填註） 發明專利說明書 、 發明名稱 中文 微波用介電質磁器組成物 英文 發明人 姓名 (中文） 1. 深川智機 2. 西川和裕 姓名 (英文） 1. 2. 國籍 1.日本2.日本 住、居所 1. 日本國兵庫縣尼崎市南塚口町6丁目9-13-301 2. 曰本國京都府長岡京市勝龍寺16-20 二 申請人 姓名 (名稱） (中文） 1.新王磁材股份有限公司 姓名 (名稱） (英文） 1.株式会社NEOMAX 國籍 1.日本 住、居所 (事務所） 1.日本國大阪府大阪市中央區北浜4丁目7番19號 代表人 姓名 (中文） 1.戶井詰哲郎 代表人 姓名 (英文） 1.
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