CN105777078A - Low-loss temperature-stable type ultralow dielectric constant microwave dielectric ceramic Mg3Y2Ge3O12 - Google Patents

Low-loss temperature-stable type ultralow dielectric constant microwave dielectric ceramic Mg3Y2Ge3O12 Download PDF

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CN105777078A
CN105777078A CN201610344296.8A CN201610344296A CN105777078A CN 105777078 A CN105777078 A CN 105777078A CN 201610344296 A CN201610344296 A CN 201610344296A CN 105777078 A CN105777078 A CN 105777078A
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ceramic
temperature
dielectric constant
binding agent
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徐敏育
方亮
唐莹
邓酩
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Guilin University of Technology
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Guilin University of Technology
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Abstract

The invention discloses application of a compound oxide Mg3Y2Ge3O12 as a low-loss temperature-stable type ultralow dielectric constant microwave dielectric ceramic and a preparation method of the compound oxide. The preparation method comprises the following steps of: (1) weighing and burdening MgO, Y2O3 and GeO2 original powders with the purity more than 99.9% (percentage by weight) according to composition of Mg3Y2GeO12; (2) carrying out wetted ball grinding and mixing on the raw materials in the step (1) for 12 hours, wherein ball grinding medium is absolute ethyl alcohol, drying, and then presintering for 6 hours in the air atmosphere at the temperature of 1350 DEG C; and (3) adding a binding agent into the powder obtained in the step (2), granulating, then carrying out compression moulding, and finally sintering for 4 hours in the air atmosphere at the temperature of 1400-1450 DEG C, wherein the binding agent adopts polyvinyl alcohol solution with the mass concentration of 5%, and addition amount of polyvinyl alcohol accounts for 3% of the total mass of the powder. The prepared ceramic is well sintered, dielectric constant reaches 10.9-11.8, quality factor Qf value of the ceramic reaches up to 113000-153000GHz, temperature coefficient of resonance frequency is small, and the ceramic has great application value in the industry.

Description

Low-loss temperature-stabilized ultralow dielectric microwave dielectric ceramic Mg3Y2Ge3O12
Technical field
The present invention relates to dielectric ceramic material, particularly relate to for manufacturing ceramic substrate, the resonance that microwave frequency uses Dielectric ceramic materials of microwave device such as device and wave filter and preparation method thereof.
Background technology
Microwave dielectric ceramic refers to be applied in microwave frequency band (mainly UHF and SHF frequency range) circuit as dielectric material And complete the pottery of one or more functions, modern communication is widely used as resonator, wave filter, dielectric substrate and medium The components and parts such as wave circuit, are the key foundation materials of modern communication technology, in portable mobile phone, automobile telephone, nothing The aspect such as rope phone, television satellite accepter and military radar has highly important application, small-sized at modern communication instrument Change, integrated during just playing increasing effect.
It is applied to the dielectric ceramic of microwave frequency band, should meet the requirement of following dielectric property: (1) seriation DIELECTRIC CONSTANT εr To adapt to different frequency and the requirement of different application occasion;(2) high quality factor q value or low dielectric loss tan δ are to reduce Noise, typically requires Qf >=3000 GHz;(3) the temperature coefficient τ of resonant frequencyƒThe least to ensure what device had had Heat stability, general requirement-10 ppm/DEG C≤τƒ≤+10 ppm/℃.Just have tried to from late 1930s in the world Dielectric substance is applied to microwave technology, and prepares TiO2Microwave dielectric filter, but its temperature coefficient of resonance frequency τƒ Too greatly cannot be practical.Since the seventies in last century, the large-scale development to medium ceramic material, root are started According to relative dielectric constant εrSize from use frequency range different, generally can will have been developed that and developing microwave-medium pottery Porcelain is divided into 4 classes.
(1) ultralow dielectric microwave dielectric ceramic, main representative is Al2O3-TiO2、Y2BaCuO5、MgAl2O4With Mg2SiO4Deng, its εr≤ 20, quality factor q × f >=50000GHz, τƒ≤10 ppm/°C.It is mainly used in microwave base plate and height End microwave device.
(2) low εrWith the microwave dielectric ceramic of high q-factor, mainly BaO-MgO-Ta2O5, BaO-ZnO-Ta2O5Or BaO- MgO-Nb2O5,BaO-ZnO-Nb2O5System or the hybrid system MWDC material between them.Its εr=20~35, Q=(1~2) × 104(under the GHz of f >=10), τƒ≈0.As medium in the microwave communication equipments such as the direct broadcasting satellite being mainly used in f >=8 GHz Resonating device.
(3) medium εrWith the microwave dielectric ceramic of Q-value, it is mainly with BaTi4O9、Ba2Ti9O20(Zr, Sn) TiO4Etc. for The MWDC material of base, its εr=35 ~ 45, Q=(6~9) × 103(under f=3~-4GHz), τƒ≤5 ppm/°C.It is mainly used in 4 ~8 in microwave military radar in GHz frequency range and communication system as dielectric resonance device.
(4) high εrAnd the microwave dielectric ceramic that Q-value is relatively low, in being mainly used in 0.8~4GHz frequency range, civilian movement is led to News system, this is also the emphasis of microwave dielectric ceramic research.Since the eighties, Kolar, Kato et al. in succession find and have studied Perovskite-like tungsten bronze type BaO Ln2O3—TiO2Series (Ln=La, Sm, Nd or Pr etc. are called for short BLT system), composite perofskite Structure C aO Li2O—Ln2O3—TiO2Series, lead base series material, Ca1-xLn2x/3TiO3It is contour εrMicrowave dielectric ceramic, The wherein BaO Nd of BLT system2O3—TiO2Material dielectric constant reaches 90, lead base series (Pb, Ca) ZrO3Dielectric constant reaches To 105.
Three performance indications (ε due to microwave dielectric ceramicrWith Q f and τƒBetween) be mutually restriction relation (see Document: the restricting relation between microwave dielectric ceramic materials dielectric properties, Zhu Jianhua, Liang Fei, Wang little Hong, Lv Wenzhong, electronics unit Part and material, phase March the 3rd in 2005), the single-phase microwave-medium ceramics meeting three performance requirements is considerably less, is mainly them Temperature coefficient of resonance frequency the most excessive or quality factor are on the low side and cannot application request.At present microwave-medium is made pottery The research major part of porcelain is the summary of experience drawn by great many of experiments, but do not have complete theory to illustrate microstructure with The relation of dielectric properties, therefore, the most also cannot predict its resonant frequency temperature system from the composition of compound and structure Number and the microwave dielectric property such as quality factor, explore and develop near-zero resonance frequency temperature coefficient (-10 ppm/DEG C≤τƒ≤+ 10 ppm/ DEG C) it is that those skilled in the art are the most thirsty with the serial differing dielectric constant microwave dielectric ceramic of higher figure of merit Hope solution but be difficult to the difficult problem succeeded all the time, which greatly limits the development of microwave dielectric ceramic and device. We are to composition Mg3Y2Ge3O12、Mg3Sm2Ge3O12、Mg3La2Ge3O12Series compound carried out grinding of microwave dielectric property Study carefully, wherein Mg3Sm2Ge3O12And Mg3La2Ge3O12(respectively-102 ppm/ DEG C and-76 bigger than normal of temperature coefficient of resonance frequency Ppm/ DEG C) and cannot be as practical microwave-medium ceramics.
Summary of the invention
It is an object of the invention to provide one and there is good thermal stability and low-loss ultralow dielectric micro-wave dielectric Ceramic material and preparation method thereof.
The chemical composition of the microwave dielectric ceramic material of the present invention is Mg3Y2Ge3O12
The preparation method step of this microwave dielectric ceramic material is:
(1) be 99.9%(percentage by weight by purity) more than MgO, Y2O3And GeO2Starting powder press Mg3Y2Ge3O12Group Become to weigh dispensing.
(2) being mixed 12 hours by step (1) raw material wet ball-milling, ball-milling medium is dehydrated alcohol, at 1350 DEG C after drying Pre-burning 6 hours in air atmosphere.
(3), after adding binding agent pelletize in the powder that step (2) prepares, re-compacted molding, finally 1400 ~ 1450 DEG C air atmosphere sinters 4 hours;Described binding agent uses mass concentration to be the poly-vinyl alcohol solution of 5%, adding of polyvinyl alcohol Dosage accounts for the 3% of powder gross mass.
Advantages of the present invention: Mg3Y2Ge3O12Pottery less than 1450 DEG C sintering well, dielectric constant reach 10.9~ The temperature coefficient τ of 11.8, especially resonant frequencyƒLittle, temperature stability is good;Quality factor q f value is up to 113000- 153000GHz, can be widely used for the manufacture of the microwave devices such as various medium substrate, resonator and wave filter, can meet low temperature altogether The technology of burning technology and microwave multilayer device needs, and industrially has great using value.
Detailed description of the invention
Embodiment:
Table 1 shows 3 specific embodiments and the microwave dielectric property thereof of the different sintering temperatures constituting the present invention.Its preparation side Method as it has been described above, carry out the evaluation of microwave dielectric property by cylindrical dielectric resonator method.
This pottery can be widely used for the manufacture of the microwave devices such as various medium substrate, resonator and wave filter, can meet shifting The technology of the systems such as dynamic communication and satellite communication needs.
Table 1:

Claims (1)

1. composite oxides are as an application for low-loss temperature-stabilized ultralow dielectric microwave dielectric ceramic, its feature The chemical composition being described composite oxides is: Mg3Y2Ge3O12
The preparation method step of described composite oxides is:
(1) be 99.9%(percentage by weight by purity) more than MgO, Y2O3And GeO2Starting powder press Mg3Y2Ge3O12Group Become to weigh dispensing;
(2) being mixed 12 hours by step (1) raw material wet ball-milling, ball-milling medium is dehydrated alcohol, at 1350 DEG C of air after drying Pre-burning 6 hours in atmosphere;
(3) after adding binding agent pelletize in the powder that step (2) prepares, re-compacted molding is finally big at 1400 ~ 1450 DEG C Gas atmosphere sinters 4 hours;Described binding agent uses mass concentration to be the poly-vinyl alcohol solution of 5%, the addition of polyvinyl alcohol Account for the 3% of powder gross mass.
CN201610344296.8A 2016-05-23 2016-05-23 Low-loss temperature-stable type ultralow dielectric constant microwave dielectric ceramic Mg3Y2Ge3O12 Pending CN105777078A (en)

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110627480A (en) * 2019-09-01 2019-12-31 桂林理工大学 MgO-Al2O3-GeO2Preparation method of ternary system microwave dielectric material
CN111517789A (en) * 2020-04-29 2020-08-11 桂林理工大学 Low-dielectric microwave dielectric ceramic material and preparation method thereof
CN116143508A (en) * 2022-12-20 2023-05-23 无锡鑫圣慧龙纳米陶瓷技术有限公司 Low-dielectric-constant high-temperature stable microwave dielectric ceramic and preparation method thereof

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1524792A (en) * 2003-02-28 2004-09-01 新加坡纳米材料科技有限公司 Method for preparing crystalline state perovskite compounds powder
CN101891465A (en) * 2010-07-08 2010-11-24 桂林理工大学 Barium-strontium stannate titanate lead-free piezoelectric ceramics with high piezoelectric constant
CN105330261A (en) * 2015-11-30 2016-02-17 桂林理工大学 Temperature-stable microwave dielectric ceramic Li2MgGeO4 with high quality factor and preparation method thereof

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1524792A (en) * 2003-02-28 2004-09-01 新加坡纳米材料科技有限公司 Method for preparing crystalline state perovskite compounds powder
CN101891465A (en) * 2010-07-08 2010-11-24 桂林理工大学 Barium-strontium stannate titanate lead-free piezoelectric ceramics with high piezoelectric constant
CN105330261A (en) * 2015-11-30 2016-02-17 桂林理工大学 Temperature-stable microwave dielectric ceramic Li2MgGeO4 with high quality factor and preparation method thereof

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110627480A (en) * 2019-09-01 2019-12-31 桂林理工大学 MgO-Al2O3-GeO2Preparation method of ternary system microwave dielectric material
CN111517789A (en) * 2020-04-29 2020-08-11 桂林理工大学 Low-dielectric microwave dielectric ceramic material and preparation method thereof
CN111517789B (en) * 2020-04-29 2022-06-14 桂林理工大学 Low-dielectric microwave dielectric ceramic material and preparation method thereof
CN116143508A (en) * 2022-12-20 2023-05-23 无锡鑫圣慧龙纳米陶瓷技术有限公司 Low-dielectric-constant high-temperature stable microwave dielectric ceramic and preparation method thereof

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Application publication date: 20160720