CN104230328B - Low dielectric microwave medium ceramic material of a kind of intermediate sintering temperature and preparation method thereof - Google Patents

Low dielectric microwave medium ceramic material of a kind of intermediate sintering temperature and preparation method thereof Download PDF

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CN104230328B
CN104230328B CN201410409636.1A CN201410409636A CN104230328B CN 104230328 B CN104230328 B CN 104230328B CN 201410409636 A CN201410409636 A CN 201410409636A CN 104230328 B CN104230328 B CN 104230328B
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sintering temperature
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microwave medium
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CN104230328A (en
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张启龙
周珏辉
刘进壮
杨辉
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Zhejiang University ZJU
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Abstract

The invention belongs to material science, aim to provide low dielectric microwave medium ceramic material of a kind of intermediate sintering temperature and preparation method thereof.The chemical expression of the low dielectric microwave medium ceramic material of intermediate sintering temperature of the present invention is (1-x) Mg 2snO 4– xLFV, wherein: complex sintering aids LFV is LiF-Fe 2o 3-V 2o 5, x=2 ~ 5wt%, described LiF-Fe 2o 3-V 2o 5in be by raw material Li F, Fe 2o 3and V 2o 5mass content ratio be 4: 1: 2 composition.The invention has the beneficial effects as follows: add complex sintering aids LFV, aid melts in ceramic post sintering process, form liquid phase, Fe ion enters Mg simultaneously 2snO 4lattice, common acceleration of sintering mass transfer process, significantly reduces Mg 2snO 4the sintering temperature of stupalith, can at 1025-1075 DEG C dense sintering.

Description

Low dielectric microwave medium ceramic material of a kind of intermediate sintering temperature and preparation method thereof
Technical field
The invention belongs to material science, be specifically related to low dielectric microwave medium ceramic material of a kind of intermediate sintering temperature and preparation method thereof.
Background technology
In recent years, along with developing rapidly of mobile communication technology, growing to the requirement of the microwave devices such as dielectric capacitance, resonator and wave filter microwave dielectric ceramic materials used.Microwave frequency band resource-constrained, operating frequency, gradually to the expansion of high frequency millimeter ripple, needs components and parts to use and has low-k (ε r<10) microwave dielectric ceramic materials, reduces cross-coupling effect to reach, reduces the objects such as signal delay.
Mg 2snO 4stupalith has low-k (ε r=8.41), (quality factor and Q × f value are up to 5 × 10 for low-dielectric loss 4the superior dielectric characteristic such as GHz), has broad prospect of application as microwave device dielectric material.Mainly concentrate at present modification doping research, if ChenYC etc. is at " MaterialsChemistryandPhysics " 133 phase in 2012 829 pages of " EnhancementmicrowavedielectricpropertiesofMg delivered 2snO 4ceramicsbysubstitutingMg 2+withNi 2+" in a literary composition, use the method for Ni doping to improve Mg 2snO 4the quality factor of pottery, reduces dielectric loss.ZhouJ etc. are at " JournalofMaterialsScience: MaterialsinElectronics " the 25th volume the 1st phase in 2014 500 pages of " Enhancedeffectofnon-stoichiometryonthesinterabilityandmi crowavedielectricpropertiesofMg delivered 2+xsnO 4ceramics " in a literary composition, the method that have employed Mg position non-stoichiometric improves Mg 2snO 4ceramic sintering character also reduces its dielectric loss.
But the Mg of research at present 2snO 4microwave ceramics is hard-to-sinter comparatively, and sintering temperature, all higher than 1550 DEG C, cannot meet the processing requirement of burning altogether with low cost metal electrode in microwave device manufacturing process, the industrial application of obstructing body system.The present invention is at Mg 2snO 4lFV (LiF-Fe is introduced in stupalith 2o 3-V 2o 5) complex sintering aids, overcome the deficiencies in the prior art, develop a kind of low dielectric microwave medium ceramic material of the intermediate sintering temperature that can burn altogether with 70Ag/30Pd electrode.
Summary of the invention
The technical problem to be solved in the present invention is, overcomes deficiency of the prior art, provides low dielectric microwave medium ceramic material of a kind of intermediate sintering temperature and preparation method thereof.
For technical solution problem, solution of the present invention is:
There is provided a kind of intermediate sintering temperature low dielectric microwave medium ceramic material, the chemical expression of the low dielectric microwave medium ceramic material of described intermediate sintering temperature is (1-x) Mg 2snO 4– xLFV, wherein: complex sintering aids LFV is LiF-Fe 2o 3-V 2o 5, x=2 ~ 5wt%, described LiF-Fe 2o 3-V 2o 5in be by raw material Li F, Fe 2o 3and V 2o 5mass content ratio be 4: 1: 2 composition.
In the present invention, the preparation method of the low dielectric microwave medium ceramic material of a kind of described intermediate sintering temperature is also provided, comprises the steps:
Step (1): SnO in molar ratio 2: MgO=1: 2 take raw material SnO 2and MgO, carry out ball mill mixing 4h, then put into alumina crucible and fire with 1200 DEG C, then ball milling obtains Mg 2snO 4powder;
Step (2): compare for LiF: Fe by mass content 2o 3: V 2o 5take raw material Li F, Fe at=4: 1: 2 2o 3and V 2o 5mix, obtain complex sintering aids LFV;
Step (3): compare Mg by mass content 2snO 4: LFV=(1-x): x takes the obtained Mg of step (1) 2snO 4, obtained complex sintering aids LFV, wherein x=2 ~ 5wt% in step (2), ball milling mixing 4h;
Step (4): add 5% polyvinyl alcohol water solution and carry out granulation in the obtained mixed powder of step (3), suppress under 150MPa pressure, prepare the cylindric base substrate of diameter 18mm, thickness 9mm;
Step (5): base substrate obtained in step (4) is warmed up to 550 DEG C of insulation 1h with 2 DEG C/min, is then warmed up to 1025 ~ 1075 DEG C of heat preservation sintering 4h with 5 DEG C/min, be i.e. the obtained described low dielectric microwave medium ceramic material of intermediate sintering temperature.
Compared with prior art, the invention has the beneficial effects as follows:
Add complex sintering aids LFV, aid melts in ceramic post sintering process, form liquid phase, Fe ion enters Mg simultaneously 2snO 4lattice, common acceleration of sintering mass transfer process, significantly reduces Mg 2snO 4the sintering temperature of stupalith, can at 1025-1075 DEG C dense sintering.In addition, (1-x) Mg obtained 2snO 4-xLFV pottery (x=2 ~ 5wt%) maintains good dielectric properties: specific inductivity (ε r) be 7.72-7.97, quality factor q × f is 19600 ~ 41400GHz.Pottery and 70Ag/30Pd electrode burn in the scanning electron microscope (SEM) photograph of sample section and power spectrum line sweep result altogether can be found out, stupalith and 70Ag/30Pd electrode do not react and obviously spread, meet pottery-electrode co-firing technology requirement, single or multiple lift microwave devices such as preparing electrical condenser, antenna, wave filter can be applied to.
Accompanying drawing explanation
Fig. 1 is scanning electron microscope (SEM) photograph and the power spectrum line sweep result that the low dielectric microwave medium ceramic material of intermediate sintering temperature prepared by the present invention and 70Ag/30Pd electrode burn sample section altogether.
Embodiment
Following embodiment can make the technician of this professional skill field more fully understand the present invention, but does not limit the present invention in any way:
Embodiment 1:
The chemical expression of the low dielectric microwave medium ceramic material of described intermediate sintering temperature is (1-x) Mg 2snO 4– xLFV, wherein complex sintering aids LFV is LiF-Fe 2o 3-V 2o 5, x=2wt%, described LiF-Fe 2o 3-V 2o 5in be by raw material Li F, Fe 2o 3and V 2o 5mass content ratio be 4: 1: 2 composition.
The preparation method of the low dielectric microwave medium ceramic material of described intermediate sintering temperature, carries out according to the following steps:
Step 1): SnO in molar ratio 2: MgO=1: 2 raw materials weighing SnO 2and MgO, ball mill mixing 4h, then put into alumina crucible and fire at 1200 DEG C, ball milling prepares Mg 2snO 4powder.
Step 2): 4: 1: 2 difference raw materials weighing LiF, Fe in mass ratio 2o 3and V 2o 5obtain complex sintering aids LFV; And weigh step 1) obtained Mg 2snO 4powder, makes the mass content of itself and complex sintering aids LFV be respectively 98%, 2%, ball milling mixing 4h.
Step 3): weigh step 2) mixing gained powder, add the polyvinyl alcohol water solution of 5%, granulation; Be pressed into the green body cylinders of diameter 18mm, thickness 9mm with 150MPa pressure under tabletting machine.
Step 4): by step 3) in the base substrate of preparation be warmed up to 550 DEG C of insulation 1h with 2 DEG C/min, be then warmed up to 1075 DEG C of heat preservation sintering 4h with 5 DEG C/min, i.e. the obtained low dielectric microwave medium ceramic material of intermediate sintering temperature of the present invention.
According to the low dielectric microwave medium ceramic material of intermediate sintering temperature that aforementioned formula and step obtain, property indices is: sintering temperature 1075 DEG C, density 4.48g/cm 3, DIELECTRIC CONSTANT ε r=7.72, quality factor q × f=19600GHz.
Embodiment 2:
The chemical expression of the low dielectric microwave medium ceramic material of described intermediate sintering temperature is (1-x) Mg 2snO 4– xLFV, wherein complex sintering aids LFV is LiF-Fe 2o 3-V 2o 5, x=3wt%, described LiF-Fe 2o 3-V 2o 5in be with raw material Li F: Fe 2o 3: V 2o 5mass content ratio be 4: 1: 2 composition.
The preparation method of the low dielectric microwave medium ceramic material of described intermediate sintering temperature, carries out according to the following steps:
Step 1): SnO in molar ratio 2: MgO=1: 2 raw materials weighing SnO 2and MgO, ball mill mixing 4h, then put into alumina crucible and fire at 1200 DEG C, ball milling prepares Mg 2snO 4powder.
Step 2): 4: 1: 2 difference raw materials weighing LiF, Fe in mass ratio 2o 3and V 2o 5obtain complex sintering aids LFV; And weigh step 1) obtained Mg 2snO 4powder, makes the mass content of itself and complex sintering aids LFV be respectively 97%, 3%, ball milling mixing 4h.
Step 3): weigh step 2) mixing gained powder, add the polyvinyl alcohol water solution of 5%, granulation; Be pressed into the green body cylinders of diameter 18mm, thickness 9mm with 150MPa pressure under tabletting machine.
Step 4): by step 3) in the base substrate of preparation be warmed up to 550 DEG C of insulation 1h with 2 DEG C/min, be then warmed up to 1075 DEG C of heat preservation sintering 4h with 5 DEG C/min, i.e. the obtained low dielectric microwave medium ceramic material of intermediate sintering temperature of the present invention.
According to the low dielectric microwave medium ceramic material of intermediate sintering temperature that aforementioned formula and step obtain, property indices is: sintering temperature 1075 DEG C, density 4.60g/cm 3, DIELECTRIC CONSTANT ε r=7.97, quality factor q × f=21400GHz.
Embodiment 3:
The chemical expression of the low dielectric microwave medium ceramic material of described intermediate sintering temperature is (1-x) Mg 2snO 4– xLFV, wherein complex sintering aids LFV is LiF-Fe 2o 3-V 2o 5, x=4wt%, described LiF-Fe 2o 3-V 2o 5in be with raw material Li F: Fe 2o 3: V 2o 5mass content ratio be 4: 1: 2 composition.
The preparation method of the low dielectric microwave medium ceramic material of described intermediate sintering temperature, carries out according to the following steps:
Step 1): SnO in molar ratio 2: MgO=1: 2 raw materials weighing SnO 2and MgO, ball mill mixing 4h, then put into alumina crucible and fire at 1200 DEG C, ball milling prepares Mg 2snO 4powder.
Step 2): 4: 1: 2 difference raw materials weighing LiF, Fe in mass ratio 2o 3and V 2o 5obtain complex sintering aids LFV; And weigh step 1) obtained Mg 2snO 4powder, makes the mass content of itself and complex sintering aids LFV be respectively 96%, 4%, ball milling mixing 4h.
Step 3): weigh step 2) mixing gained powder, add the polyvinyl alcohol water solution of 5%, granulation; Be pressed into the green body cylinders of diameter 18mm, thickness 9mm with 150MPa pressure under tabletting machine.
Step 4): by step 3) in the base substrate of preparation be warmed up to 550 DEG C of insulation 1h with 2 DEG C/min, be then warmed up to 1050 DEG C of heat preservation sintering 4h with 5 DEG C/min, i.e. the obtained low dielectric microwave medium ceramic material of intermediate sintering temperature of the present invention.
According to the low dielectric microwave medium ceramic material of intermediate sintering temperature that aforementioned formula and step obtain, property indices is: sintering temperature 1050 DEG C, density 4.59g/cm 3, DIELECTRIC CONSTANT ε r=7.90, quality factor q × f=41400GHz.
Embodiment 4:
The chemical expression of the low dielectric microwave medium ceramic material of described intermediate sintering temperature is (1-x) Mg 2snO 4– xLFV, wherein complex sintering aids LFV is LiF-Fe 2o 3-V 2o 5, x=5wt%, described LiF-Fe 2o 3-V 2o 5in be with raw material Li F: Fe 2o 3: V 2o 5mass content ratio be 4: 1: 2 composition.
The preparation method of the low dielectric microwave medium ceramic material of described intermediate sintering temperature, carries out according to the following steps:
Step 1): SnO in molar ratio 2: MgO=1: 2 raw materials weighing SnO 2and MgO, ball mill mixing 4h, then put into alumina crucible and fire at 1200 DEG C, ball milling prepares Mg 2snO 4powder.
Step 2): 4: 1: 2 difference raw materials weighing LiF, Fe in mass ratio 2o 3and V 2o 5obtain complex sintering aids LFV, and weigh step 1) obtained Mg 2snO 4powder, makes the mass content of itself and complex sintering aids LFV be respectively 95%, 5%, ball milling mixing 4h.
Step 3): weigh step 2) mixing gained powder, add the polyvinyl alcohol water solution of 5%, granulation; Be pressed into the green body cylinders of diameter 18mm, thickness 9mm with 150MPa pressure under tabletting machine.
Step 4): by step 3) in the base substrate of preparation be warmed up to 550 DEG C of insulation 1h with 2 DEG C/min, be then warmed up to 1025 DEG C of heat preservation sintering 4h with 5 DEG C/min, i.e. the obtained low dielectric microwave medium ceramic material of intermediate sintering temperature of the present invention.
According to the low dielectric microwave medium ceramic material of intermediate sintering temperature that aforementioned formula and step obtain, property indices is: sintering temperature 1025 DEG C, density 4.56g/cm 3, DIELECTRIC CONSTANT ε r=7.93, quality factor q × f=28700GHz.
Scanning electron microscope (SEM) photograph and the power spectrum line sweep result that intermediate sintering temperature low dielectric microwave medium ceramic material that in the present invention prepared by each embodiment above-mentioned and 70Ag/30Pd electrode burn sample section altogether according to Fig. 1: this curve represents the content of each element of sweep test, can find out electrode and stupalith interface clear, the rough sledding almost not having generating electrodes to diffuse into pottery, separate out in pottery or react with stupalith.
Therefore, actual range of the present invention not only comprises the disclosed embodiments, be also included under claims implement or perform all equivalents of the present invention.

Claims (1)

1. the low dielectric microwave medium ceramic material of intermediate sintering temperature, is characterized in that, the chemical expression of the low dielectric microwave medium ceramic material of described intermediate sintering temperature is (1-x) Mg 2snO 4– xLFV, wherein: complex sintering aids LFV is LiF-Fe 2o 3-V 2o 5, x=2 ~ 5wt%, described LiF-Fe 2o 3-V 2o 5in be by raw material Li F, Fe 2o 3and V 2o 5mass content ratio be 4: 1: 2 composition;
The preparation method of the low dielectric microwave medium ceramic material of described intermediate sintering temperature comprises the steps:
Step (1): SnO in molar ratio 2: MgO=1: 2 take raw material SnO 2and MgO, carry out ball mill mixing 4h, then put into alumina crucible and fire with 1200 DEG C, then ball milling obtains Mg 2snO 4powder;
Step (2): compare for LiF: Fe by mass content 2o 3: V 2o 5take raw material Li F, Fe at=4: 1: 2 2o 3and V 2o 5mix, obtain complex sintering aids LFV;
Step (3): compare Mg by mass content 2snO 4: LFV=(1-x): x takes the obtained Mg of step (1) 2snO 4, obtained complex sintering aids LFV, wherein x=2 ~ 5wt% in step (2), ball milling mixing 4h;
Step (4): carry out granulation by adding 5% polyvinyl alcohol water solution in obtained for step (3) mixed powder, and suppress under 150MPa pressure, prepare the cylindric base substrate of diameter 18mm, thickness 9mm;
Step (5): base substrate obtained for step (4) is warmed up to 550 DEG C of insulation 1h with 2 DEG C/min, is then warmed up to 1025 ~ 1075 DEG C of heat preservation sintering 4h with 5 DEG C/min, be i.e. the obtained low dielectric microwave medium ceramic material of described intermediate sintering temperature.
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CN103193478A (en) * 2013-04-15 2013-07-10 陕西师范大学 Magnesium titanate based composite ceramic sintered at low temperature and preparation method thereof

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CN103193478A (en) * 2013-04-15 2013-07-10 陕西师范大学 Magnesium titanate based composite ceramic sintered at low temperature and preparation method thereof

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