WO2005124791A1 - Composition de ceramique dielectrique, substrat produit a partir de cette composition et procede de production dudit substrat - Google Patents

Composition de ceramique dielectrique, substrat produit a partir de cette composition et procede de production dudit substrat Download PDF

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Publication number
WO2005124791A1
WO2005124791A1 PCT/IB2005/051980 IB2005051980W WO2005124791A1 WO 2005124791 A1 WO2005124791 A1 WO 2005124791A1 IB 2005051980 W IB2005051980 W IB 2005051980W WO 2005124791 A1 WO2005124791 A1 WO 2005124791A1
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WO
WIPO (PCT)
Prior art keywords
dielectric ceramic
ceramic composition
composition according
dielectric
electrodes
Prior art date
Application number
PCT/IB2005/051980
Other languages
English (en)
Inventor
Uwe Mackens
Detlev Hennings
Nicole Hilbrandt
Baby Seriyati Schreinemacher
Original Assignee
Philips Intellectual Property & Standards Gmbh
Koninklijke Philips Electronics N. V.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Philips Intellectual Property & Standards Gmbh, Koninklijke Philips Electronics N. V. filed Critical Philips Intellectual Property & Standards Gmbh
Publication of WO2005124791A1 publication Critical patent/WO2005124791A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/46—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates
    • C04B35/462—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates
    • C04B35/465—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates
    • C04B35/468—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates based on barium titanates
    • C04B35/4682—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates based on barium titanates based on BaTiO3 perovskite phase

Definitions

  • Dielectric ceramic composition substrate made from the same and method of manufacturing the substrate
  • the present invention relates to a dielectric ceramic composition, a
  • LTCC Low Temperature Cofired Ceramics
  • Dielectric ceramics based on (Ba,Sr,Ca)-titanates show a high dielectric constant (K ⁇ 70-90) at high frequencies, high temperature stability of K ( ⁇ K/K ⁇ 50*10 "6 /°C) and low dissipation losses (tan ⁇ ⁇ 10 "2 ).
  • a well-known dielectric composition consists of (Bao. 3 ⁇ Sro.o 2 Ca 0 .o5Gdo.i96Ndo. 27 o)TiO 3 and is commercially available as temperature- stable dielectric substance with K ⁇ 85 (FERRO, Uden, NL).
  • the ceramic material is suitable for the manufacturing of multilayer capacitors with inner electrodes containing Ag-Pd at sintering temperatures higher than 1100°C.
  • Sintering with strictlyBase Metal Electrodes (BME)" e.g. containing Cu, Ni in sintering atmosphere is not possible, because (Ba,Sr,Ca, RE)-titanates wherein RE is a rare earth element like Gd, Nd etc. in reducing or low oxygen atmosphere would be semi-conductive.
  • BME Base Metal Electrodes
  • a dielectric composition which contains a mixture of a ceramic composition containing Ba a RE b Ti c O 3 , wherein RE represents a rare earth element and a, b, c satisfy certain relations, a glass composition and a metal oxide.
  • the dielectric composition can be sintered in the presence of Cu electrodes and at a temperature below the melting point of Cu so as to manufacture an electronic device such as a ceramic multilayer element. After sintering, the dielectric composition has a relative dielectric constant of at least 55.
  • US 6,631,070 B2 there is disclosed a ceramic capacitor having at least two electrodes and a ceramic dielectric preparation which is essentially composed of an oxide-ceramic dielectric substance and a sintering agent including zinc borate
  • the sintering aid may additionally comprise a compound like CuO, SiO 2 , ZnSiTiOs.
  • the ceramic capacitor can be sintered at low temperatures and is characterized by reproducible dielectric properties.
  • the dielectric ceramic preparation may be used for LTCC substrates in integrated micromodules.
  • For the outer electrodes use is made of a vapour-deposited CrNi layer coated with Au.
  • a multilayer structure of conductive layers is separated by insulating ceramic dielectric layers, which contain BaTiO 3 , zinc barium borate frit and Bi 2 O 3 in certain compositions.
  • the electrodes contain silver to provide the advantages of low cost and high conductivity.
  • US 6,407,024 Bl, US 6,458,734 Bl and US 6,556,423 B2 each describe a dielectric ceramic composition containing components selected from the group of calcium titanate, strontium titanate and barium titanate in certain molar ratios.
  • Sintering aids like SiO , MgO, ZnO, Al 2 O 3 , Li 2 O are provided, too.
  • An object of the present invention is to provide a dielectric material based on the composition (Bao. 23 ⁇ Sro.o 2 Cao . o 5 Gd 0 .i 96 Ndo. 27 o)TiO 3 , which is prevented from reduction by suitable additives and can be sintered in LTCC substrates together with Cu electrodes at temperatures below 1000°C. Lowering of the sintering temperature of (Ba Sr,RE)-titanates is made possible by additives like for example B 2 O 3 , ZnO, Li 2 CO 3 , Bi 2 O 3 , CuO and SiO 2 . SiO 2 and Bi 2 O 3 usually form low melting glasses which provide the basis of a pressing of the dielectric ceramic at temperatures below 1000°C.
  • double oxides like Zn B 6 O] 3 and ZnSiTiOs are produced according to the well-know solid state method by intensive mixing of the several oxides SiO 2 , TiO 2 , B 2 O 3 , ZnO und calcining them at 1000°C, see Table 1.
  • composition (Bao. 23 ⁇ Sr 0 .o 2 Cao.o 5 Gdo.i 96 Ndo .27 o)TiO 3
  • Table 2 shows different mixtures made from the basic material (Bao. 231 Sro.o 2 Cao.o 5 Gdo.i 9 6Ndo.27o)TiO 3 with different sinter additives .
  • Table 2 Flux variation Sample . additives Zr BeO ⁇ ZnSiTiO 5 CuO SiO 2 Li 2 CO 3 Bi 2 O 3
  • Table 5 Insulation resistance on air at 900°C and 980°C of sintered samples sample IR 25°C 150°C 900°C DC voltage ZBCSBL 200V 8.69E+12 1.25E+13 ZBCSBLJ .” lOOOV 7.03E+12 1.26E+13 ZBCSBL_3 200V 5.09E+11 1.32E+13 ZBCSBL 3 lo ov 3.30E+U ', 1.23E+13 ZBCSBL_6 200V 4.61E+12 6.02E+12 ZBCSBL_6 1000V 5.77E+12 5.92E+12 ZBCSBL_8 200V 2.00E+13 6.45E+12 ZBCSBL_8' 1000V 2.70E+13 6.41E+12 980°C * ⁇ ZBCSBL_1 200V 2E+13 6.06E+12 ZBCSBLJL 1000V TM 9.99E+13 6.09E+12 ZBCSBL_3 200V 2E+13 8.06E+12 ZBCSBL_3 1000
  • High insulating dielectric ceramics with good dielectric properties could be sintered with Cu-electrodes in certain temperature intervals and atmospheres.
  • a schematic feature of an LTCC multilayer module with sintered electrodes is shown in the Figure.
  • Ceramic tapes with a thickness of ⁇ 20 ⁇ m were manufactured from sample 6 with aid of a binder from polyvinylalcohol (PVA) according to the well- known doctor blade method. After printing of conductive lines and electrodes with a Cu-paste (Shoei, Japan) the foils were aligned, stacked and laminated (1 to 3 active ceramic tapes). The inner electrodes were contacted from the outside with vias of diameter ⁇ 200 ⁇ m, which were punched through the tape and filled with Cu paste. Sintering was performed in different atmospheres at temperatures in the range between 900° and 1000°C. The results are shown in table 6.
  • Table 6 Results in LTCC-substrates, sample 6 top_temp atmosphere Ag electrodes, Cu electrodes T°C K tan ⁇ [%] IR [ ⁇ ] K tan ⁇ [%] IR [ ⁇ ] 9,00 "" . N 2 et 20°C J. J ⁇ ./. i 30 2.Q. 2*10 10 950 ⁇ N 2 * wet20°C ./. J ⁇ ./. 50 0.3 >10 12 975 N 2 wet 20°C ./. J. ./. 6 ⁇ I 0.5 >10 12 1000 ;N 2 wet 20°C Bitcoin 1 J • ' j. 63.
  • the sintering atmosphere exerciset 20°C is optimal and means a water vapour-saturated N 2 -atmosphere with ⁇ 50 ppm O 2 at 20°C.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Ceramic Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Structural Engineering (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Oxide Ceramics (AREA)
  • Inorganic Insulating Materials (AREA)

Abstract

L'invention concerne des céramiques diélectriques à base de (Ba, Sr, Ca, Gd, Nd)-titanate connues pour leurs faibles pertes de dissipation (tanδ < 10-2) à une constante diélectrique (K ~ 70-90) relativement élevée et à une stabilité de température (ΔK/K < 50*10-6/°C) élevée. Ces matériaux sont cependant communément utilisés pour préparer des condensateurs à température stable. Ils sont habituellement soumis à une cocuisson à l'aide d'électrodes Ag-Pd chères. Les électrodes en métaux nobles peuvent être remplacées par Cu très conducteur et bon marché, lorsque le frittage est exécuté dans une atmosphère de réduction. Lorsqu'on leur ajoute, de manière appropriée, ZnO, Bi203, B203, Si02, CuO et Li203, les matériaux de céramique précités peuvent être cuits à 950 °C à l'aide d'électrodes Cu dans une atmosphère de N2 humide. Les matériaux cuits possèdent des constantes diélectriques de K ~ 50-60, tanδ < 0,5 %, une résistance à l'isolation IR > 1012 O et des coefficients de température TCC <50ppm/ °C.
PCT/IB2005/051980 2004-06-17 2005-06-15 Composition de ceramique dielectrique, substrat produit a partir de cette composition et procede de production dudit substrat WO2005124791A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
EP04102778.0 2004-06-17
EP04102778 2004-06-17

Publications (1)

Publication Number Publication Date
WO2005124791A1 true WO2005124791A1 (fr) 2005-12-29

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104845617A (zh) * 2015-04-30 2015-08-19 陕西师范大学 一种Zn4B6O13:Eu3+发光材料的简易制备方法

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0960868A1 (fr) * 1998-05-27 1999-12-01 Koninklijke Philips Electronics N.V. Composition céramique diélectrique
JP2000251537A (ja) * 1999-02-26 2000-09-14 Philips Japan Ltd 誘電体磁器組成物
US20020093782A1 (en) * 2000-08-08 2002-07-18 Ronald Mikkenie Dielectric composition, method of manufacturing a ceramic multilayer element, and electronic device
US20030002239A1 (en) * 2000-11-04 2003-01-02 Peter Schmidt Ceramic capacitor with czt dielectric
DE10155593A1 (de) * 2001-11-13 2003-05-22 Philips Corp Intellectual Pty Dielektrische keramische Zusammensetzung
WO2003100799A1 (fr) * 2002-05-24 2003-12-04 Philips Intellectual Property & Standards Gmbh Dispositif electronique hybride comprenant une bande ceramique cocuite a basse temperature

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0960868A1 (fr) * 1998-05-27 1999-12-01 Koninklijke Philips Electronics N.V. Composition céramique diélectrique
JP2000251537A (ja) * 1999-02-26 2000-09-14 Philips Japan Ltd 誘電体磁器組成物
US20020093782A1 (en) * 2000-08-08 2002-07-18 Ronald Mikkenie Dielectric composition, method of manufacturing a ceramic multilayer element, and electronic device
US20030002239A1 (en) * 2000-11-04 2003-01-02 Peter Schmidt Ceramic capacitor with czt dielectric
DE10155593A1 (de) * 2001-11-13 2003-05-22 Philips Corp Intellectual Pty Dielektrische keramische Zusammensetzung
WO2003100799A1 (fr) * 2002-05-24 2003-12-04 Philips Intellectual Property & Standards Gmbh Dispositif electronique hybride comprenant une bande ceramique cocuite a basse temperature

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
PATENT ABSTRACTS OF JAPAN vol. 2000, no. 12 3 January 2001 (2001-01-03) *

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104845617A (zh) * 2015-04-30 2015-08-19 陕西师范大学 一种Zn4B6O13:Eu3+发光材料的简易制备方法

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