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CN113800908A - Medium dielectric constant double perovskite microwave dielectric ceramic material and preparation method thereof - Google Patents

Medium dielectric constant double perovskite microwave dielectric ceramic material and preparation method thereof Download PDF

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CN113800908A
CN113800908A CN202110989647.1A CN202110989647A CN113800908A CN 113800908 A CN113800908 A CN 113800908A CN 202110989647 A CN202110989647 A CN 202110989647A CN 113800908 A CN113800908 A CN 113800908A
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杨利
杨小燕
匡小军
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Guilin University of Technology
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Abstract

The invention discloses a dielectric constant epsilon between 20 and 27, a product (Qxf) of a quality factor and a resonant frequency between 17,000 and 29,000GHz, and a temperature coefficient (tau) of the resonant frequencyf) A novel double perovskite structure microwave dielectric ceramic at-77 to-79 ppm/DEG C and a preparation method thereof, belonging to the technical field of microwave dielectric ceramic preparation, wherein the chemical composition of the microwave dielectric ceramic is La3Mg2MO9(M ═ Nb, Sb, Ta). The microwave dielectric ceramic with the double perovskite structure disclosed by the invention is simple in chemical composition and preparation process, and can be applied to the manufacture of microwave devices such as dielectric resonators, microwave integrated circuit substrates and the like.

Description

Medium dielectric constant double perovskite microwave dielectric ceramic material and preparation method thereof
Technical Field
The invention relates to a dielectric ceramic material of microwave components such as a dielectric substrate, a resonator, a waveguide loop and the like used at microwave frequency and a preparation method thereof.
Background
With the rapid development of modern communications such as 5G communications technology, communications network technology and satellite communications, the demands for miniaturization, low loss, low cost and high stability of modern communications technology materials are further increased. The microwave dielectric ceramic is used as a core component of modern communication technology, and is widely applied to mobile communication, satellite communication, global health and the like as microwave electronic components such as a dielectric resonator/filter, a dielectric antenna, a dielectric guided wave loop and the like due to excellent dielectric constant, high quality factor and low resonant frequency temperature coefficientIn microwave communication systems such as a satellite positioning system, Bluetooth equipment, a wireless local area network and the like, designing and exploring a novel microwave dielectric ceramic material with excellent microwave dielectric properties is a key for the development of modern communication technology. A has been reported so far3MM'2O9(A ═ Ca, Sr, Ba; M ═ Ni, Mg, Zn, Co; M ═ Nb, Ta, etc.) perovskite structure oxide ceramics exhibit excellent microwave dielectric properties, with hexagonal phase Ba3ZnTa2O9Most typically, the dielectric constant is-30, the temperature coefficient of the resonant frequency is 0 + -0.5 ppm/deg.C, and the quality factor Qxf is-168,000 GHz. Furthermore, in the double perovskite structure La3M2M'O9(M ═ Mg, Ni, Co; M ═ Nb, Ta, Sb) oxides, only La3Mg2TaO9The composition is studied about the dielectric constant and the electrical properties at a frequency of 100KHz, the dielectric constant is 22.7, the dielectric loss is 0.004, and the temperature coefficient of the resonance frequency is 98 +/-1 ppm/DEG C. Currently, La is lacking for double perovskite3M2M'O9The microwave dielectric properties of (M ═ Mg, Ni, Co; M ═ Nb, Ta, Sb) in the microwave band (300MHz to 300 GHz) were investigated.
Disclosure of Invention
The invention aims to provide a novel medium-dielectric-constant double perovskite microwave dielectric ceramic material and a preparation method thereof.
The invention relates to a medium dielectric constant double perovskite microwave dielectric ceramic material which comprises the following chemical components: la3Mg2MO9Where M ═ Nb, Sb, Ta.
The microwave dielectric ceramic with the double perovskite structure is prepared by the following steps:
(1) la with the purity of 99.99 percent2O3Pre-burning the MgO raw material for 3 hours at 1000 ℃ in an atmosphere to remove water and carbon dioxide;
(2) la with the purity of 99.99 percent2O3,MgC2O4·2H2O or MgO, Nb2O5,Sb2O5,Ta2O5Dried powder according to La3Mg2MO9Weighing and batching the chemical formula (M ═ Nb, Sb and Ta);
(3) mixing the raw materials in the step (2), wet-type hand-milling for 1-2 hours by using absolute ethyl alcohol as a solvent, drying, and presintering for 10 hours at 1450 ℃ in an atmosphere;
(4) adding a binder into the powder prepared in the step (3), mixing, then pressing and forming, and finally sintering for 10 hours at 1530-1580 ℃ in an atmospheric atmosphere; the binder adopts a polyvinyl alcohol solution with the mass concentration of 5%, and the dosage of the binder accounts for 2% of the total mass of the powder.
The microwave dielectric ceramic with the double perovskite structure prepared by the invention has simple preparation process, high quality factor (Q multiplied by f-17,000-29,000 GHz) and medium dielectric constant (29-35), and the temperature coefficient of resonance frequency is-77 to-79 ppm/DEG C, so that the microwave dielectric ceramic can meet the application requirements of communication electronic elements such as medium dielectric constant type dielectric resonators, filters and the like.
Detailed Description
Table 1 shows 3 specific examples of the invention and their microwave dielectric properties. The preparation method is as described above, phase analysis is carried out on the sintered ceramic sample by the powder X-ray diffraction method, FIG. 1 is the X-ray diffraction patterns of examples 1, 2 and 3, which show that a single double perovskite structure phase is formed, and FIG. 2 is a schematic diagram of the crystal structure of examples 1, 2 and 3 projected along the [010] direction, which shows that two octahedrons in the structure are connected together at the same vertex, and lanthanum atoms are in the octahedral framework channel. The dielectric properties of the microwaves were evaluated by the cylindrical dielectric resonator method.
The present invention is by no means limited to the above embodiments. The composition, the upper limit and the lower limit of the sintering temperature and the range value can realize the invention, and the embodiments are not listed.
The invention can be widely used for manufacturing microwave devices such as various dielectric substrates, resonators/filters and the like, and can meet the technical requirements of systems such as mobile communication, satellite communication, global satellite positioning systems, Bluetooth equipment, wireless local area networks and the like.
Table 1:
Figure BDA0003232040470000031
drawings
FIG. 1 is an X-ray diffraction pattern of 3 examples of the present invention
FIG. 2 is a schematic diagram of the crystal structure projected along [010] direction of 3 embodiments of the present invention.

Claims (2)

1. The invention discloses a dielectric constant epsilon between 20 and 27, a product (Qxf) of a quality factor and a resonant frequency between 17,000 and 29,000GHz, and a temperature coefficient (tau) of the resonant frequencyf) A novel double perovskite structure microwave dielectric ceramic at-77 to-79 ppm/DEG C and a preparation method thereof, belonging to the technical field of microwave dielectric ceramic preparation, wherein the chemical composition of the microwave dielectric ceramic is La3Mg2MO9(M=Nb,Sb,Ta)。
2. The microwave dielectric ceramic of claim 1 prepared by the steps of:
(1) la with the purity of 99.99 percent2O3Pre-burning the MgO raw material for 3 hours at 1000 ℃ in an atmosphere to remove water and carbon dioxide;
(2) la with the purity of 99.99 percent2O3,MgC2O4·2H2O or MgO, Nb2O5,Sb2O5,Ta2O5Dry powder according to La3Mg2MO9Weighing and batching the chemical formula (M ═ Nb, Sb and Ta);
(3) mixing the raw materials in the step (2), wet-type hand-milling for 1-2 hours by using absolute ethyl alcohol as a solvent, drying, and presintering for 10 hours at 1450 ℃ in an atmosphere;
(4) adding a binder into the powder prepared in the step (3), mixing, then pressing and forming, and finally sintering for 10 hours at 1530-1580 ℃ in an atmospheric atmosphere; the binder adopts a polyvinyl alcohol solution with the mass concentration of 5%, and the dosage of the binder accounts for 2% of the total mass of the powder.
CN202110989647.1A 2021-08-26 2021-08-26 Medium dielectric constant double perovskite microwave dielectric ceramic material and preparation method thereof Pending CN113800908A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115849895A (en) * 2022-12-23 2023-03-28 吉林大学 Tantalum-magnesium-lanthanum-modified bismuth ferrite-based dielectric energy storage material and preparation method thereof

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US5788876A (en) * 1994-11-30 1998-08-04 U.S. Philips Corporation Complex substituted lanthanum-lead-zirconium-titanium perovskite, ceramic composition and actuator
JPH1171173A (en) * 1996-10-25 1999-03-16 Ngk Spark Plug Co Ltd Dielectric material and method of manufacturing the same
CN1524792A (en) * 2003-02-28 2004-09-01 新加坡纳米材料科技有限公司 A method for preparing various crystalline perovskite compound powders
CN1672284A (en) * 2002-08-01 2005-09-21 圣安德鲁斯大学董事会 Perovskite-based fuel cell electrodes and thin films
CN106830923A (en) * 2017-03-24 2017-06-13 桂林理工大学 High quality factor microwave dielectric ceramic Bi3Y2Ga3O12
CN113292997A (en) * 2021-05-25 2021-08-24 常熟理工学院 Double-ordered composite perovskite red fluorescent powder and preparation method thereof

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5788876A (en) * 1994-11-30 1998-08-04 U.S. Philips Corporation Complex substituted lanthanum-lead-zirconium-titanium perovskite, ceramic composition and actuator
JPH1171173A (en) * 1996-10-25 1999-03-16 Ngk Spark Plug Co Ltd Dielectric material and method of manufacturing the same
CN1672284A (en) * 2002-08-01 2005-09-21 圣安德鲁斯大学董事会 Perovskite-based fuel cell electrodes and thin films
CN1524792A (en) * 2003-02-28 2004-09-01 新加坡纳米材料科技有限公司 A method for preparing various crystalline perovskite compound powders
CN106830923A (en) * 2017-03-24 2017-06-13 桂林理工大学 High quality factor microwave dielectric ceramic Bi3Y2Ga3O12
CN113292997A (en) * 2021-05-25 2021-08-24 常熟理工学院 Double-ordered composite perovskite red fluorescent powder and preparation method thereof

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Title
AKBAS MEHMET A. ET AL.: "Structure and dielectric properties of the Ba(Mg1/3 Nb2/3 )O3 –La(Mg2/3 Nb1/3 )O3 System", 《 J AM CERAM. SOC》 *

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115849895A (en) * 2022-12-23 2023-03-28 吉林大学 Tantalum-magnesium-lanthanum-modified bismuth ferrite-based dielectric energy storage material and preparation method thereof
CN115849895B (en) * 2022-12-23 2023-09-29 吉林大学 Tantalum-magnesium-lanthanum modified bismuth ferrite-based dielectric energy storage material and preparation method thereof

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Application publication date: 20211217