WO2004085339A1 - 希土類硫化物の焼結体からなる高誘電材料 - Google Patents
希土類硫化物の焼結体からなる高誘電材料 Download PDFInfo
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- WO2004085339A1 WO2004085339A1 PCT/JP2004/003883 JP2004003883W WO2004085339A1 WO 2004085339 A1 WO2004085339 A1 WO 2004085339A1 JP 2004003883 W JP2004003883 W JP 2004003883W WO 2004085339 A1 WO2004085339 A1 WO 2004085339A1
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- rare earth
- dielectric material
- high dielectric
- dielectric constant
- sintered body
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- 239000003989 dielectric material Substances 0.000 title claims abstract description 22
- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 20
- -1 rare earth sulfide Chemical class 0.000 title claims abstract description 15
- 239000003990 capacitor Substances 0.000 claims abstract description 22
- 239000013078 crystal Substances 0.000 claims abstract description 11
- RKTYLMNFRDHKIL-UHFFFAOYSA-N copper;5,10,15,20-tetraphenylporphyrin-22,24-diide Chemical compound [Cu+2].C1=CC(C(=C2C=CC([N-]2)=C(C=2C=CC=CC=2)C=2C=CC(N=2)=C(C=2C=CC=CC=2)C2=CC=C3[N-]2)C=2C=CC=CC=2)=NC1=C3C1=CC=CC=C1 RKTYLMNFRDHKIL-UHFFFAOYSA-N 0.000 claims abstract description 9
- 239000000203 mixture Substances 0.000 claims abstract description 5
- 150000002910 rare earth metals Chemical class 0.000 claims abstract description 5
- 239000000126 substance Substances 0.000 claims abstract description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 11
- 229910052684 Cerium Inorganic materials 0.000 claims description 4
- 229910052779 Neodymium Inorganic materials 0.000 claims description 4
- 229910052777 Praseodymium Inorganic materials 0.000 claims description 4
- 229910052746 lanthanum Inorganic materials 0.000 claims description 4
- 229910052697 platinum Inorganic materials 0.000 claims description 4
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 3
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 claims description 3
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 claims description 3
- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 0.000 claims description 3
- 239000000463 material Substances 0.000 abstract description 7
- 238000000034 method Methods 0.000 description 11
- 238000005245 sintering Methods 0.000 description 9
- YTYSNXOWNOTGMY-UHFFFAOYSA-N lanthanum(3+);trisulfide Chemical compound [S-2].[S-2].[S-2].[La+3].[La+3] YTYSNXOWNOTGMY-UHFFFAOYSA-N 0.000 description 8
- 239000000843 powder Substances 0.000 description 7
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 5
- 229910052760 oxygen Inorganic materials 0.000 description 5
- 239000001301 oxygen Substances 0.000 description 5
- 230000007704 transition Effects 0.000 description 5
- 239000002994 raw material Substances 0.000 description 4
- 238000005259 measurement Methods 0.000 description 3
- 239000004065 semiconductor Substances 0.000 description 3
- 239000012535 impurity Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000000465 moulding Methods 0.000 description 2
- 239000010955 niobium Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- KKZKWPQFAZAUSB-UHFFFAOYSA-N samarium(iii) sulfide Chemical compound [S-2].[S-2].[S-2].[Sm+3].[Sm+3] KKZKWPQFAZAUSB-UHFFFAOYSA-N 0.000 description 2
- 229910052692 Dysprosium Inorganic materials 0.000 description 1
- 229910052691 Erbium Inorganic materials 0.000 description 1
- 229910052693 Europium Inorganic materials 0.000 description 1
- 229910052688 Gadolinium Inorganic materials 0.000 description 1
- 229910052689 Holmium Inorganic materials 0.000 description 1
- 229910052765 Lutetium Inorganic materials 0.000 description 1
- 229910052772 Samarium Inorganic materials 0.000 description 1
- 229910052771 Terbium Inorganic materials 0.000 description 1
- 229910052775 Thulium Inorganic materials 0.000 description 1
- 229910052769 Ytterbium Inorganic materials 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 229910052789 astatine Inorganic materials 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 1
- 229910002113 barium titanate Inorganic materials 0.000 description 1
- 239000003985 ceramic capacitor Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 238000007731 hot pressing Methods 0.000 description 1
- 229910052747 lanthanoid Inorganic materials 0.000 description 1
- 150000002602 lanthanoids Chemical class 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- VUXGXCBXGJZHNB-UHFFFAOYSA-N praseodymium(3+);trisulfide Chemical compound [S-2].[S-2].[S-2].[Pr+3].[Pr+3] VUXGXCBXGJZHNB-UHFFFAOYSA-N 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- VEALVRVVWBQVSL-UHFFFAOYSA-N strontium titanate Chemical compound [Sr+2].[O-][Ti]([O-])=O VEALVRVVWBQVSL-UHFFFAOYSA-N 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/547—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on sulfides or selenides or tellurides
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- C04B35/64—Burning or sintering processes
- C04B35/645—Pressure sintering
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G4/00—Fixed capacitors; Processes of their manufacture
- H01G4/002—Details
- H01G4/018—Dielectrics
- H01G4/06—Solid dielectrics
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- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
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- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
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Definitions
- High dielectric material consisting of sintered rare earth sulfide
- the present invention is particularly useful for large-capacity capacitor materials that have a large dielectric constant.
- the present invention relates to a high dielectric material comprising a rare earth sulfide sintered body.
- BACKGROUND ART Searching for substances having a large dielectric constant has been carried out for some time.
- ferroelectrics with a perovskite structure called a relaxor which has a diffused phase containing lead (Pb), zinc (Zn), and niobium (Nb)
- Non-Patent Documents 1 and 2 ferroelectrics with a perovskite structure called a relaxor, which has a diffused phase containing lead (Pb), zinc (Zn), and niobium (Nb)
- Non-Patent Documents 1 and 2 and semiconductors
- a sintered body Non-Patent Document 3 or the like in which the apparent dielectric constant is increased by using a very thin insulating boundary layer using barium or strontium titanate as a base material.
- Non-Patent Document 1 SE Park, ML Mulvihill, G.
- Non-Patent Document 2 “Characteristics and Measurement of Dielectric Materials' Evaluation and Application Technology”, Technical Information Association, 2001, p. 292
- Non-patent Document 3 M. Fujimoto and WD Kingery, "kiicrostruc” ture of SrTi03 ⁇ nternal Boundary Layer Capacitors During and After Processing and Resultant Electrical Properties J, J. Am. Cerm. Soc., 68 (1985) 169-173 Disclosure of the invention
- the thickness of the boundary layer is extremely thin and lacks uniformity, so that there is a problem in withstand voltage or resistance to electric shock.
- the capacitance F of a disk capacitor is expressed as F oc £ ⁇ S / d, where ⁇ is the dielectric constant of the dielectric, d is the thickness in the electrode direction, and S is the electrode area.
- ⁇ is the dielectric constant of the dielectric
- d is the thickness in the electrode direction
- S is the electrode area.
- electrodes and dielectrics are alternately stacked, and S is increased and d is decreased, enabling a capacitor with a large F.
- the dielectric material used in multilayer capacitors is mainly barium titanate, which has a large dielectric constant. Temperature, which is around 120 ° C for pure crystals. In order to use a capacitor with a large capacity at room temperature, the transition temperature is lowered by various processes such as adding other elements to this titanium titanate, so that the temperature stability and aging change Etc. has a problem.
- thermoelectric properties a lanthanum sulfide-based sintered body has excellent thermoelectric properties (see the following document).
- Shinji Hirai et al. Synthesis and thermoelectric properties of ⁇ -La2S3”, according to the Abstract of the 125th Annual Meeting of the Japan Institute of Metals, November 1999, p317
- the present invention provides (1) a crystal structure of tetragonal type 3 and a chemical composition of L n
- the present invention also provides (2) the high dielectric constant of (1), wherein the rare earth is at least one of lanthanum (La), praseodymium (Pr), cerium (Ce), and neodymium (Nd). Material. Also, the present invention provides the above (1) or (2), wherein platinum that inhibits the crystal structure of the (3) type tridisulfide from being converted to the ⁇ type at a high temperature is added. It is a high dielectric material.
- the present invention provides (4) a capacitor characterized by using any one of the high dielectric materials according to (1) to (3).
- the dielectric material having the mold structure of the present invention has a dielectric constant at room temperature of more than 100,000 to 1,000,0000, and a frequency range of 0.5 kHz to 1,000. In kHz, the change in the value can be limited to about one digit, and the value of tan ⁇ is between 0 and 2. In addition, the temperature dependence of the dielectric constant of the dielectric material increases with temperature in the range of about 200 K to about 370 K when the frequency is 1 kHz, but can be kept within one digit. .
- a rare earth sulfide having a large dielectric constant can be provided as a Balta-shaped molded body, it is possible to produce a capacitor having an arbitrary shape and a large capacity excellent in mechanical strength. Also, no special processing such as addition of impurities is required to obtain a dielectric having a large dielectric constant. Therefore, if a dielectric having a large dielectric constant is used in the production of a multilayer capacitor, it is possible to produce a capacitor with even higher capacitance and better stability.
- FIG. 1 is a graph showing the relationship between the applied frequency and the relative permittivity of a lanthanum sulfide (LasSs) sintered body produced by the plasma sintering method of Example 1.
- Figure 2 shows the applied frequency of the platinum-added lanthanum sulfide (La 2 S 3 ) sintered body produced by the hot press method of Example 2.
- 5 is a graph showing the relationship between the number and the relative permittivity.
- FIG. 3 is a graph showing the relationship between the specific dielectric constant at an applied frequency of 1 kHz and the measurement temperature of a platinum-added lanthanum sulfide (La 2 S3) sintered body produced by the hot pressing method of Example 2. .
- the present invention is a high-dielectric material having the above-mentioned constitution, which is made of rare earth sulfide (Ln 2 S 3 ) powder as a raw material, and is subjected to a normal pressure sintering method, a hot press method, and a plasma sintering method. And so on.
- Ln 2 S 3 rare earth sulfide
- the structure of the sintered body becomes a mold structure.
- the rare earth elements composing the rare earth sulfide at least one of lanthanum (La), praseodymium (Pr), cerium (Ce), and neodymium (Nd) is preferable because they are electrically insulating. This is because it has a certain tetragonal ⁇ -type structure and therefore a large dielectric constant.
- the following method is used to produce a sintered body using a starting material obtained by adding platinum to a rare earth sulfide raw material powder. 0 oxygen content as an impurity. 9 mass 0/0 above composition formula L ns S 3 (L n is, La, Ce, Pr, Nd , Sm, Eu, Gd, Tb, Dy, Ho, At least one selected from the group consisting of Er, Tm, Yb, and Lu) / 3 type lanthanoid Mix platinum powder with tridisulfide powder, and after molding or simultaneously with molding, from 1300 ° C to 1700 ° Sinter in the temperature range of C. Platinum powder has an average particle size of 50 // m or less, and the mixing amount is 1.5 mass. / 0 or less is preferable.
- a capacitor using the above dielectric material it is necessary to form the capacitor into a disk shape and sandwich the upper and lower sides of the disk with metal electrodes.
- the type of metal or the like as the electrode is not particularly limited.
- a multilayer capacitor is used in which electrodes and dielectric materials are alternately stacked.
- lanthanum sulfide (La 2 S 3 ) powder manufactured by Kojundo Chemical Co., Ltd., oxygen concentration 1% by weight, particle size is about 0.1 to 10 Oi ra, used amount is about 4 g
- the obtained sample was a disk, a disk capacitor with a diameter of 15. Omra and a thickness of 4.24 mm.
- the electrode used was a gold vapor-deposited film having a diameter of 10.0 mm.
- the capacitance of this sample as a capacitor was several tens to several tens OnF.
- the crystal structure of this sample is a tetragonal type, and its relative dielectric constant ( ⁇ ) at room temperature is about 1,000,000,000 at lk Hz, as shown in Fig. 1. Was about 1.6.
- a sample obtained by adding 1.5 wt ° / 0 platinum powder to lanthanum sulfide (La 2 S 3 ) powder was sintered by a hot press method in which the sample was held at 1500 ° C and 2 OMPa for 10 minutes.
- the shape of the obtained sample was a disk with a diameter of 15.0 mm and a thickness of about 4 mm.
- the structure of this sample was typical of tetragonal.
- the relative dielectric constant ( ⁇ ) of this sample at room temperature is about 40,000 at 1 kHz, and decreases with increasing frequency. , 0000.
- Figure 3 shows the relationship between the relative dielectric constant ( ⁇ ) at an applied frequency of 1 kHz and the measurement temperature ( ⁇ ).
- the value of the relative permittivity increased with increasing temperature from about 50,000 at about 160 ° to 34,000 at about 370 °.
- the powder of praseodymium sulfide (Pr 2 S 3 ) was reduced to 150,000. C, it was sintered by holding at 3 O MPa for 10 minutes. The obtained sample had a tetragonal crystal structure. The dielectric constant of this sample was about 140,000 at room temperature and a frequency of 70 kHz.
- the samarium sulfide (S1112S3) powder was sintered by plasma sintering at 125 ° C. and 30 MPa for 10 minutes by the plasma sintering method.
- the obtained sample was of the ⁇ -type with a cubic crystal structure.
- the dielectric constant of this sample was about 40 at room temperature in the frequency range of 1 kHz to 10 MHz.
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Abstract
Description
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Priority Applications (3)
Application Number | Priority Date | Filing Date | Title |
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JP2005504044A JP4551987B2 (ja) | 2003-03-27 | 2004-03-22 | 希土類硫化物の焼結体からなる誘電体材料 |
CA002520699A CA2520699A1 (en) | 2003-03-27 | 2004-03-22 | High dielectric material composed of sintered body of rare earth sulfide |
US10/550,625 US20070040206A1 (en) | 2003-03-27 | 2004-03-22 | High dielectric material composed of sintered body of rare earth sulfide |
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JP2003086830 | 2003-03-27 | ||
JP2003-086830 | 2003-03-27 |
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WO2004085339A1 true WO2004085339A1 (ja) | 2004-10-07 |
WO2004085339A8 WO2004085339A8 (ja) | 2005-07-28 |
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US (1) | US20070040206A1 (ja) |
JP (1) | JP4551987B2 (ja) |
CA (1) | CA2520699A1 (ja) |
WO (1) | WO2004085339A1 (ja) |
Cited By (3)
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JP2019110181A (ja) * | 2017-12-18 | 2019-07-04 | 国立大学法人室蘭工業大学 | 電磁波吸収粉末、電磁波吸収組成物、電磁波吸収体および塗料 |
WO2022230786A1 (ja) * | 2021-04-28 | 2022-11-03 | パナソニックIpマネジメント株式会社 | キャパシタ、キャパシタの製造方法、電気回路、回路基板、及び機器 |
WO2022230787A1 (ja) * | 2021-04-26 | 2022-11-03 | パナソニックIpマネジメント株式会社 | キャパシタ、電気回路、回路基板、及び機器 |
Citations (1)
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JP2001335367A (ja) * | 2000-05-19 | 2001-12-04 | Japan Science & Technology Corp | 硫化ランタンまたは硫化セリウム焼結体およびその製造方法 |
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US6531354B2 (en) * | 2000-01-19 | 2003-03-11 | North Carolina State University | Lanthanum oxide-based gate dielectrics for integrated circuit field effect transistors |
WO2006097503A2 (en) * | 2005-03-18 | 2006-09-21 | Cinvention Ag | Process for the preparation of porous sintered metal materials |
-
2004
- 2004-03-22 US US10/550,625 patent/US20070040206A1/en not_active Abandoned
- 2004-03-22 CA CA002520699A patent/CA2520699A1/en not_active Abandoned
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JP2001335367A (ja) * | 2000-05-19 | 2001-12-04 | Japan Science & Technology Corp | 硫化ランタンまたは硫化セリウム焼結体およびその製造方法 |
Non-Patent Citations (2)
Title |
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GUBKIN A.N. ET AL.: "Synthesis and dielectric properties of lanthanum sulfide", IZVESTIYA AKADEMII NAUK SSSR, NEORGANCHESKIE MATERIALY, vol. 9, no. 9, 1973, pages 1511 - 1515, XP002982740 * |
UEMURA YOICHIRO ET AL.: "Pd o tenka shita La2S3 joatsu shokettai no netsuden tokusei", THE PHYSICAL OCIETY OF JAPAN KOEN GAIYOSHU, vol. 56, no. 2, 3 September 2002 (2002-09-03), pages 530, XP002982739 * |
Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
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JP2019110181A (ja) * | 2017-12-18 | 2019-07-04 | 国立大学法人室蘭工業大学 | 電磁波吸収粉末、電磁波吸収組成物、電磁波吸収体および塗料 |
WO2022230787A1 (ja) * | 2021-04-26 | 2022-11-03 | パナソニックIpマネジメント株式会社 | キャパシタ、電気回路、回路基板、及び機器 |
WO2022230786A1 (ja) * | 2021-04-28 | 2022-11-03 | パナソニックIpマネジメント株式会社 | キャパシタ、キャパシタの製造方法、電気回路、回路基板、及び機器 |
Also Published As
Publication number | Publication date |
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WO2004085339A8 (ja) | 2005-07-28 |
JPWO2004085339A1 (ja) | 2006-06-29 |
US20070040206A1 (en) | 2007-02-22 |
JP4551987B2 (ja) | 2010-09-29 |
CA2520699A1 (en) | 2004-10-07 |
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