CN103496979A

CN103496979A - Low-temperature sintering microwave dielectric ceramic La3Cu2VO9 and preparation method thereof

Info

Publication number: CN103496979A
Application number: CN201310434743.5A
Authority: CN
Inventors: 苏聪学; 李洁; 方亮
Original assignee: Guilin University of Technology
Current assignee: YANCHENG LIYAN NEW MATERIAL Co.,Ltd.
Priority date: 2013-09-23
Filing date: 2013-09-23
Publication date: 2014-01-08
Anticipated expiration: 2033-09-23
Also published as: CN103496979B

Abstract

The invention discloses a low-temperature sintering microwave dielectric ceramic La3Cu2VO9 and a preparation method thereof. The chemical composition formula of the low-temperature sintering microwave dielectric ceramic is La3Cu2VO9. The preparation method comprises the steps of (1) weighing and batching original powder of La2O3, CuO and V2O5 with the purity being over 99.9% according to the chemical formula La3Cu2VO9; (2) carrying out mixing and wet ball-milling on raw materials obtained in the step (1) for 12 hours, taking distilled water as a solvent, drying, and then, pre-sintering in an air atmosphere for 6 hours at the temperature of 800 DEG C; (3) adding a binder into powder prepared in the step (2), granulating, then, carrying out compression molding, and finally, sintering in the air atmosphere for 4 hours at the temperature of 900-950 DEG C, wherein a polyvinyl alcohol solution with the mass concentration of 5% is adopted as the binder, and the dosage of the binder accounts for 3% of the total mass of the powder. According to the ceramic prepared by the preparation method, the sintering at the temperature of 900-950 DEG C is good, the dielectric constant reaches 19-20, the quality factor (Qf) reaches up to 77,000-86,000GHz, and the temperature coefficient of resonance frequency is small, so that the ceramic has a great application value in industries.

Description

Low temperature sintering microwave dielectric ceramic La 3cu 2vO 9and preparation method thereof

Technical field

The present invention relates to dielectric ceramic material, particularly relate to microwave dielectric ceramic material of the microwave devices such as medium substrate, resonator and wave filter that use in microwave frequency and preparation method thereof.

Background technology

Microwave dielectric ceramic refers to and is applied in microwave frequency band (being mainly UHF, SHF frequency range) circuit as dielectric material and completes the pottery of one or more functions, be widely used as the components and parts such as resonator, wave filter, dielectric substrate and medium guided wave loop in modern communication, it is the key foundation material of modern communication technology, at aspects such as portable mobile phone, automobile telephone, cordless telephone, telestar susceptor and military radars, very important application is arranged, in the miniaturization of modern communication instrument, integrated process, just bringing into play increasing effect.

Be applied to the dielectric ceramic of microwave frequency band, should meet the requirement of following dielectric characteristics: (1) seriation DIELECTRIC CONSTANT ε _rto adapt to the requirement of different frequency and different application occasion; (2) high quality factor q value or dielectric loss tan δ are to reduce noise, general requirement Qf>=3000 GHz; (3) the temperature factor τ of resonant frequency _?the as far as possible little thermostability to guarantee that device has had, general requirement-10/ ℃≤τ _?≤+10 ppm/ ℃.From late 1930s, just someone attempts dielectric substance is applied to microwave technology in the world.

According to relative permittivity ε _rsize from use the different of frequency range, usually the microwave dielectric ceramic be developed He developing can be divided into to 4 classes.

(1) ultralow dielectric microwave dielectric ceramic, main representative is Al ₂o ₃-TiO ₂, Y ₂baCuO ₅, MgAl ₂o ₄and Mg ₂siO ₄deng, its ε _r≤ 20, quality factor q * f>=50000GHz, τ _?≤ 10 ppm/ ° C.Be mainly used in microwave base plate and high-end microwave device.

(2) low ε _rwith the microwave dielectric ceramic of high Q value, be mainly BaO-MgO-Ta ₂o ₅, BaO-ZnO-Ta ₂o ₅or BaO-MgO-Nb ₂o ₅, BaO-ZnO-Nb ₂o ₅system or the composite system MWDC material between them.Its ε _r=25～30, Q=(1～2) * 10 ⁴(under f>=10 GHz), τ _?≈ 0.Be mainly used in the microwave communication equipments such as direct broadcasting satellite of f >=8 GHz as the dielectric resonance device.

(3) medium ε _rwith the microwave dielectric ceramic of Q value, be mainly with BaTi ₄o ₉, Ba ₂ti ₉o ₂₀(Zr, Sn) TiO ₄deng the MWDC material that is base, its ε _r=35 ~ 40, Q=(6～9) * 10 ³(f=3～-4GHz under), τ _?≤ 5 ppm/ ° C.Be mainly used in the interior microwave military radar of 4～8 GHz range of frequency and communication system as the dielectric resonance device.

(4) high ε _rand the lower microwave dielectric ceramic of Q value is mainly used in civilian mobile communcations system in 0.8～4GHz range of frequency, this is also the emphasis of microwave dielectric ceramic research.Since the eighties, the people such as Kolar, Kato find and have studied perovskite-like tungsten bronze type BaO-Ln in succession ₂o ₃-TiO ₂series (Ln=La, Sm, Nd or Pr etc. are called for short BLT system), complex perovskite structure CaO-Li ₂o-Ln ₂o ₃-TiO ₂series, lead base series material, Ca _1-xln _2x/3tiO ₃be contour ε _rmicrowave dielectric ceramic, the wherein BaO-Nd of BLT system ₂o ₃-TiO ₂material dielectric constant reaches 90, lead base series (Pb, Ca) ZrO ₃specific inductivity reaches 105.

The sintering temperature of above these material systems is generally higher than 1300 ° of C, can not be directly and the low melting point metals such as Ag and Cu burn altogether the formation laminated ceramic capacitor.In recent years, along with LTCC Technology (Low Temperature Co-fired Ceramics, the requirement of development LTCC) and the development of microwave multilayer device, researchist both domestic and external has carried out exploring widely and studying to some low fever's system materials, mainly to adopt devitrified glass or glass-ceramic composite system, because low melting glass has relatively high dielectric loss mutually, the existence of glassy phase has improved the dielectric loss of material greatly.Therefore development is the emphasis of current research without the low temperature sintering microwave-medium ceramics of glassy phase.We are to consisting of La ₃cu ₂vO ₉the vanadate pottery carried out sintering characteristic and Study on microwave dielectric property, found that such pottery have excellent comprehensive microwave dielectric property simultaneously sintering temperature lower than 950 °c, can be widely used in the manufacture of the microwave devices such as various resonators and wave filter, can meet the needs of low temperature co-fired technology and microwave multilayer device.

Summary of the invention

The purpose of this invention is to provide a kind of have low-loss and good thermostability, simultaneously the low microwave dielectric ceramic of sintering temperature.

The chemical constitution formula of microwave dielectric ceramic of the present invention is: La ₃cu ₂vO ₉.

Preparation method's concrete steps of described microwave dielectric ceramic are:

(1) by purity, be the La more than 99.9% ₂o ₃, CuO and V ₂o ₅starting powder press La ₃cu ₂vO ₉the chemical formula weigh batching.

(2) by step (1) raw material mixing wet ball-milling 12 hours, solvent was distilled water, pre-burning 6 hours in 800 ℃ of air atmosphere after oven dry.

(3) after adding binding agent granulation in the powder made in step (2), then compression moulding, last sintering 4 hours in 900 ~ 950 ℃ of air atmosphere; Described binding agent adopts the polyvinyl alcohol solution that mass concentration is 5%, and dosage accounts for 3% of powder total mass.

Therefore pottery prepared by the present invention is good at 900-950 ℃ of sintering, and its specific inductivity reaches 19～20, and quality factor q f value is up to 77000-86000GHz, and temperature coefficient of resonance frequency is little, industrial great using value is arranged.

Embodiment

Embodiment:

Table 1 shows 4 specific embodiments and the microwave dielectric property thereof that forms different sintering temperatures of the present invention.Its preparation method as mentioned above, carries out the evaluation of microwave dielectric property by the cylindrical dielectric resonator method; By La ₃cu ₂vO ₉powder mixes with the Ag powder that accounts for powder quality 20%, after compression moulding, 950 ℃ of lower sintering 4 hours; X ray diffraction material phase analysis and scanning electron microscopic observation all show La ₃cu ₂vO ₉with Ag, chemical reaction, i.e. La do not occur ₃cu ₂vO ₉can be low temperature co-fired with the Ag electrode.

The present invention never is limited to above embodiment.The bound of sintering temperature, interval value can realize the present invention, at this, do not enumerate embodiment.

This pottery can be widely used in the manufacture of the microwave devices such as various medium substrates, resonator and wave filter, can meet the Technology Need of the systems such as mobile communication, satellite communications.

Table 1:

Claims

1. a vanadate, as the application of low temperature sintering microwave dielectric ceramic, is characterized in that the chemical constitution of described vanadate is: La ₃cu ₂vO ₉;

Preparation method's concrete steps of described vanadate are:

(1) by purity, be the La more than 99.9% ₂o ₃, CuO and V ₂o ₅starting powder press La ₃cu ₂vO ₉the chemical formula weigh batching;

(2) by step (1) raw material mixing wet ball-milling 12 hours, solvent was distilled water, pre-burning 6 hours in 800 ℃ of air atmosphere after oven dry;