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CN114634353A - Low-dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material and preparation method thereof - Google Patents

Low-dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material and preparation method thereof Download PDF

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CN114634353A
CN114634353A CN202011487765.4A CN202011487765A CN114634353A CN 114634353 A CN114634353 A CN 114634353A CN 202011487765 A CN202011487765 A CN 202011487765A CN 114634353 A CN114634353 A CN 114634353A
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low
temperature
fired ceramic
ceramic material
dielectric
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宋锡滨
闫鑫升
朱恒
刘振锋
奚洪亮
艾辽东
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Maxtor Technology Innovation Shandong Co ltd
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Shandong Sinocera Functional Material Co Ltd
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Abstract

The invention relates to an electronic ceramic material and the manufacturing technical field thereof, in particular to a low-temperature co-fired ceramic material with low dielectric loss and near-zero temperature drift performance, and further discloses a preparation method thereof. The low dielectric low loss near zero temperature drift low temperature co-fired ceramic material is prepared from ZnO-SiO2‑Al2O3Glass, Al2O3Prepared from rare earth oxide, with dielectric constant of 7 + -0.5 and dielectric loss of less than 2 × 10 at room temperature and test frequency of 20GHz by SPDR test method‑3(ii) a The temperature drift is within +/-3 ppm/DEG C within the temperature range of-40-110 ℃ and the test frequency of 20 GHz; in addition, of low temperature co-fired ceramic materialsBending strength is more than 150MPa, and the antenna can be applied to a 5G communication millimeter wave antenna module.

Description

Low-dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material and preparation method thereof
Technical Field
The invention relates to an electronic ceramic material and the manufacturing technical field thereof, in particular to a low-temperature co-fired ceramic material with low dielectric loss and near-zero temperature drift performance, and further discloses a preparation method thereof.
Background
In recent years, with the rapid development of semiconductor technology, electronic components have been increasingly miniaturized, integrated, and high-frequency. The selection of proper ceramics capable of co-firing with conductive materials such as silver at low temperature not higher than 900 ℃ to manufacture multilayer components or embed passive devices in multilayer circuit substrates is an inevitable requirement of the above trend, and low temperature co-fired ceramics as the main dielectric material of passive integrated components is an important development trend.
Low Temperature cofired Ceramic LTCC (Low Temperature cofired Ceramic) materials are mainly prepared by introducing an appropriate amount of sintering aid, typically a Low melting point oxide or a Low melting point glass, for example, CaO-B, into a dielectric Ceramic system, and then promoting densification of the material by a liquid phase sintering mechanism2O3Adding B into the system2O3、Bi2O3Etc. can reduce the sintering temperature to 950 deg.c. The low-temperature co-fired ceramic technology has the advantages of controllable impedance, low transmission loss, high packaging density, rich functional modules and the like, and is an indispensable key technology for realizing miniaturization, multiple functions, high reliability and low cost of the microwave/millimeter wave circuit assembly.
Research shows that the development of the high-frequency low-dielectric low-loss LTCC substrate material is the key for the successful application of the LTCC technology in the microwave/millimeter wave field. At present, LTCC substrate materials widely applied at home and abroad are mainly divided into two categories: glass/ceramic systems and microcrystalline glass systems. The physical and chemical properties of the glass/ceramic system are mainly determined by the added ceramic phase, and the glass/ceramic system has the advantages of stable performance, good process adaptability and the like; however, the composition contains nearly 50% of glass phase, which causes large high-frequency dielectric loss of the substrate and limits the high-frequency application, for example, the application frequency of the borosilicate lead glass/alumina system is generally below 8 GHz. The physical and chemical properties of the microcrystalline glass system are controlled by the type and quantity of the precipitated crystals, and the substrate material is prepared by the methodThe sintered material has very little residual glass phase and thus has excellent high-frequency properties, such as CaO-B2O3-SiO2The application frequency of the microcrystalline glass can reach 100 GHz; however, the crystallization behavior of the microcrystalline glass system is extremely sensitive to the sintering process, which results in high difficulty in controlling the product process and poor stability of the product performance.
Lead-free La with low softening point for Chenxingyu and the like of national defense science and technology university2O3-B2O3-Al2O3(LBA) glass ceramics and Al2O3Preparing the novel microcrystalline glass/ceramic composite material and sintering the 60-LBA glass and 40-Al at 900 DEG C2O3A composite material having a dielectric constant of 7.91 and a dielectric loss of 2.12X 10 at 8.1GHz-3. Also as in the solution of Chinese patent CN109608050A, it is treated with 60% MO-BAS (alkaline earth metal oxide-BaO-Al)2O3-SiO2) Microcrystalline glass with 40% Al2O3After the microcrystalline glass/ceramic LTCC substrate material prepared by compounding is sintered for 3.5 hours at 875 ℃, the dielectric constant of the obtained material is 5.82 at 9-11GHz, and the dielectric loss is 7.52 multiplied by 10-3The bending strength was 102.7 MPa. Although the sintering temperature of the material reaches the use requirement, the dielectric loss is still large, and the material is not suitable for the 5G communication fields such as millimeter wave antenna modules.
Disclosure of Invention
Therefore, the technical problem to be solved by the invention is to provide a low-dielectric low-loss near-zero temperature-drift low-temperature co-fired ceramic material to meet the performance requirements of a millimeter wave antenna module in 5G communication;
the second technical problem to be solved by the invention is to provide a preparation method of the low dielectric low-loss near-zero temperature-drift low-temperature co-fired ceramic material.
In order to solve the technical problems, the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material comprises the following components in percentage by mass based on the total amount of the material:
ZnO-SiO2-Al2O345-65 wt% of glass;
Al2O3 35-50wt%;
0-15 wt% of rare earth oxide.
Specifically, the ZnO-SiO2-Al2O3The glass comprises the following raw material components in percentage by mass:
Figure BDA0002839828940000021
Figure BDA0002839828940000031
wherein x is 1 or 2, y is 1, 2, 3 or 5;
the R element is at least one selected from Zr element, Ba element, Sb element, Cu element or Ti element.
Specifically, the rare earth oxide comprises CeO2、Pr6O11、La2O3、Nb2O5At least one of (1).
Specifically, in the low-temperature co-fired ceramic material, the Al is controlled2O3Content of the components and Al in the glass2O3The sum of the contents of the components accounts for 43 to 63 weight percent of the total weight of the low-temperature co-fired ceramic material.
Specifically, in the low-temperature co-fired ceramic material, ZnO and SiO in the glass powder are controlled2、RxOyRespectively account for 26.55-39.55%, 8.55-13.65% and 0.045-0.65% of the total amount of the low-temperature co-fired ceramic material.
Specifically, the low-temperature co-fired ceramic material uses an SPDR test method, and has a dielectric constant of 7 +/-0.5, a dielectric loss of less than 2 x 10 < -3 >, a temperature drift (temperature coefficient of resonance frequency) within +/-3 and a strength of more than 150MPa at room temperature and a test frequency of 20 GHz.
Specifically, the preparation method of the low-temperature co-fired ceramic material comprises the step of taking the ZnO-SiO according to the selected content proportion2-Al2O3Glass, alumina and selected rare earth oxidesAnd mixing, further performing ball milling, drying and sieving treatment to obtain formula powder.
The invention also discloses low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic slurry, which comprises the low-temperature co-fired ceramic material and an organic carrier, wherein the low-temperature co-fired ceramic material accounts for 37-48 wt% of the slurry.
Specifically, the preparation method of the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic slurry comprises the step of fully mixing the low-temperature co-fired ceramic material and the organic carrier.
Specifically, the organic carrier comprises a binder, a plasticizer and a dissolving agent, and further comprises a dispersing agent and a defoaming agent.
Specifically, the binder comprises one of PVA, PVB, polymethyl acrylate, ethyl cellulose, acrylic emulsion and ammonium polyacrylate salt;
the plasticizer comprises one of polyethylene glycol, phthalate and glycol;
the dissolving agent comprises one of water, ethanol, methyl ethyl ketone, trichloroethylene, toluene and xylene;
the dispersing agent comprises one of ammonium polyacrylate, phosphate ester, ethoxy compound and fresh fish oil;
the defoaming agent comprises emulsified silicone oil, a high-alcohol fatty acid ester compound, polyoxyethylene polyoxypropylene pentaerythritol ether, polyoxyethylene polyoxypropylene amine ether, polyoxypropylene glycerol ether and polyoxypropylene.
The invention also discloses a low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic green tape which is prepared from the low-temperature co-fired ceramic slurry.
Specifically, the preparation method of the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic green tape comprises the step of preparing the required green tape by the low-temperature co-fired ceramic material based on a tape casting method.
The invention discloses a low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic substrate which is prepared from a low-temperature co-fired ceramic material.
The invention also discloses a low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic substrate which is prepared by sintering the low-temperature co-fired ceramic green ceramic tape.
Specifically, the invention also discloses a method for preparing the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic substrate, which comprises the following steps:
(1) taking the ZnO-SiO according to the selected content proportion2-Al2O3Mixing glass, alumina and selected rare earth oxide, and performing ball milling, drying and sieving treatment to obtain formula powder for later use;
(2) and preparing the formula powder into a raw ceramic tape, and sintering to obtain the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic substrate.
Specifically, in the step (1), in the ball milling step, the mass ratio of the raw material, water and zirconia balls is controlled to be 1: 1.2-1.5: 2.4-3;
the diameter of the zirconia ball is controlled to be 1.5mm, the ball milling rotating speed is controlled to be 300-350r/min, and the ball milling time is controlled to be 2-5 h.
Controlling the temperature of the drying step to be 80-180 ℃ and the drying time to be 3-12 h.
The screen mesh of the sieving step was controlled to 80 mesh.
Specifically, in the step (2), the sintering step includes: the raw porcelain band is controlled to be heated from room temperature to 230-270 ℃ under the oxygen-containing atmosphere, then heated from 230-270 ℃ to 330-370 ℃, and finally heated from 330-370 ℃ to 840-890 ℃.
Specifically, the temperature rise rate of each gradient temperature stage is controlled to be 1-5 ℃/min independently.
Preferably, the heat preservation sintering time of the sintering step is controlled to be 2-4 h.
In the step (2), the step of preparing the green tape comprises a tape casting method, and specifically comprises the step of preparing the formula powder into the required low-temperature co-fired ceramic slurry.
Specifically, the preparation method of the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material, the slurry, the green ceramic tape and the substrate further comprises the steps of preparing selected components andcontent of the ZnO-SiO2-Al2O3The glass preparation process includes mixing the materials, high temperature melting to form molten glass slurry, cooling to form sheet glass, ceramic rolling to form coarse glass, dry crushing and airflow crushing to form the coarse glass into required ZnO-SiO2-Al2O3And (3) glass.
The invention also discloses application of the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material in preparation of LTCC devices.
The low dielectric low loss near zero temperature drift low temperature co-fired ceramic material comprises ZnO-SiO2-Al2O3Glass, Al2O3And rare earth oxide. ZnO-SiO used in the invention2-Al2O3Glass in which Zn is present in ZnO2+Belongs to a transition metal ion structure, the outer layer has 18 electrons, the electron cloud is easy to deform, the covalent component of the electron cloud can be increased through polarization, the capability of competing for oxygen ions with glass network forming body ions is stronger, and the electron cloud is easy to cause [ SiO4 ]]Depolymerization of the tetrahedral conglomerate structure, thereby reducing the viscosity of the glass melt and enhancing the glass melting effect; and SiO2And Al2O3The glass belongs to a formed body and an intermediate of a glass network, has high binding energy, and is not easy to generate polarization under the action of an external electric field, so that the glass can show lower dielectric constant and dielectric loss, and can inhibit crystallization of the glass; rxOyThe addition of (A) mainly plays a role in improving the thermal stability, chemical stability and mechanical strength of the glass. In addition, the rare earth oxide added into the ceramic material can form a solid solution with alumina, different tolerance factors are obtained due to different ionic radii, and oxygen octahedron distortion of different degrees is caused, so that the effect of reducing temperature drift is achieved.
The low dielectric loss and near-zero temperature drift low-temperature co-fired ceramic material uses an SPDR test method, the dielectric constant is 7 +/-0.5 at room temperature and test frequency, and the dielectric loss<2×10-3Temperature drift (resonance) in the temperature range of-40 ℃ to 110 ℃ and at the test frequency of 20GHzFrequency temperature coefficient) is within ± 3; furthermore, the strength of the low temperature co-fired ceramic material>150 MPa. The low-temperature co-fired ceramic material can be applied to a 5G communication millimeter wave antenna module.
Detailed Description
Preparation examples 1 to 5
The preparation method comprises the steps of respectively mixing the selected raw materials according to the mass percentage recorded in the following table 1, preparing glass melt slurry through high-temperature melting, cooling and rolling the glass into sheet glass through a pair of rollers, preparing crude glass through a pair of ceramic rollers, and preparing the crude glass into ZnO-SiO with required components through dry crushing and airflow crushing2-Al2O3And (3) glass.
ZnO-SiO Table 1 shows2-Al2O3Glass ingredient batching table (wt%)
Figure BDA0002839828940000061
Figure BDA0002839828940000071
Example 1
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate comprises the following steps:
(1) the ingredients were blended according to the compositions and mass percentages described in Table 2 below, and the ZnO-SiO obtained in preparation example 1 was taken2-Al2O3Glass, Al2O3And selecting rare earth oxide for mixing, and preparing raw material materials: water: the mass ratio of the zirconia balls is 1: 1.4: 2.8, adding water and zirconia balls according to the proportion, controlling the diameter of the zirconia balls to be 1.5mm, controlling the ball milling rotation speed to be 300r/min, carrying out ball milling for 5h, then drying for 3h at 180 ℃ until the materials are completely dried, and sieving by using a 80-mesh sieve to obtain formula powder for later use;
(2) and rolling/casting the obtained formula powder to prepare a film/raw ceramic tape from the sieved formula powder, controlling the heating rate of the raw ceramic tape to be 3 ℃/min in the air atmosphere, heating from room temperature to 250 ℃, controlling the heating rate to be 1 ℃/min, heating from 250 ℃ to 350 ℃, finally controlling the heating rate to be 4 ℃/min, heating from 350 ℃ to 840 ℃, carrying out heat preservation sintering for 4h, and preparing the raw ceramic tape into a substrate after sintering treatment, thus obtaining the required low-temperature co-fired ceramic substrate.
Example 2
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate comprises the following steps:
(1) the ingredients are mixed according to the components and mass percentage content described in the following table 2, and the ZnO-SiO obtained in the preparation example 2 is taken2-Al2O3Glass, Al2O3And selecting rare earth oxide for mixing, and preparing raw material materials: water: the mass ratio of the zirconia balls is 1: 1.5: 3, adding water and zirconia balls according to the proportion, controlling the diameter of the zirconia balls to be 1.5mm, controlling the ball milling rotation speed to be 320r/min, carrying out ball milling for 4h, then drying for 6h at 150 ℃ until the zirconia balls are completely dried, and sieving by using a 80-mesh sieve to obtain formula powder for later use;
(2) and (3) rolling/casting the obtained formula powder to prepare the sieved formula powder into a diaphragm/raw ceramic tape, controlling the heating rate of the raw ceramic tape to be 3 ℃/min under the air atmosphere, heating the raw ceramic tape from room temperature to 250 ℃, then controlling the heating rate to be 1 ℃/min, heating the raw ceramic tape from 250 ℃ to 350 ℃, finally controlling the heating rate to be 4 ℃/min, heating the raw ceramic tape from 350 ℃ to 850 ℃ and carrying out heat preservation sintering for 3h, and preparing the raw ceramic tape into a substrate after sintering treatment to obtain the required low-temperature co-fired ceramic substrate.
Example 3
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate comprises the following steps:
(1) the ingredients are mixed according to the components and mass percentage content described in the following table 2, and the ZnO-SiO obtained in the preparation example 3 is taken2-Al2O3Glass, Al2O3And selecting rare earth oxide for mixing, and preparing raw material materials: water: the mass ratio of the zirconia balls is 1: 1.2: 2.4 adding water and zirconia balls in the ratio to control oxidationThe diameter of a zirconium ball is 1.5mm, the ball milling rotation speed is controlled to be 340r/min, ball milling is carried out for 4h, then drying is carried out for 10h at 120 ℃ until complete drying is achieved, and sieving is carried out by using a 80-mesh sieve to obtain formula powder for later use;
(2) and (3) rolling/casting the obtained formula powder to prepare the sieved formula powder into a diaphragm/raw ceramic tape, controlling the heating rate of the raw ceramic tape to be 3 ℃/min under the air atmosphere, heating the raw ceramic tape from room temperature to 250 ℃, then controlling the heating rate to be 1 ℃/min, heating the raw ceramic tape from 250 ℃ to 350 ℃, finally controlling the heating rate to be 4 ℃/min, heating the raw ceramic tape from 350 ℃ to 870 ℃, carrying out heat preservation sintering for 3h, and preparing the raw ceramic tape into a substrate after sintering treatment to obtain the required low-temperature co-fired ceramic substrate.
Example 4
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate comprises the following steps:
(1) the ingredients and mass percentage contents described in the following table 2 were mixed, and the ZnO-SiO obtained in preparation example 4 was taken2-Al2O3Glass, Al2O3And selecting rare earth oxide for mixing, and preparing raw material materials: water: the mass ratio of the zirconia balls is 1: 1.3: 2.6, adding water and zirconia balls according to the proportion, controlling the diameter of the zirconia balls to be 1.5mm, controlling the ball milling rotation speed to be 350r/min, carrying out ball milling for 2.5h, then drying for 12h at 80 ℃ until the mixture is completely dried, and sieving by using a 80-mesh sieve to obtain formula powder for later use;
(2) and (3) rolling/casting the obtained formula powder to prepare the sieved formula powder into a diaphragm/raw ceramic tape, controlling the heating rate of the raw ceramic tape to be 3 ℃/min under the air atmosphere, heating the raw ceramic tape from room temperature to 250 ℃, then controlling the heating rate to be 1 ℃/min, heating the raw ceramic tape from 250 ℃ to 350 ℃, finally controlling the heating rate to be 4 ℃/min, heating the raw ceramic tape from 350 ℃ to 890 ℃, carrying out heat preservation sintering for 2.5h, and preparing the raw ceramic tape into a substrate after sintering treatment to obtain the required low-temperature co-fired ceramic substrate.
Example 5
The preparation method of the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic substrate of the embodiment is the same as that of embodiment 3, and is only different in that the addition amounts of the rare earth oxides in the formula powder are different, which is specifically shown in table 2.
Example 6
The preparation method of the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic substrate of the embodiment is the same as that of embodiment 3, and is only different in that the addition amounts of the rare earth oxides in the formula powder are different, which is specifically shown in table 2.
Example 7
The preparation method of the low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic substrate of the embodiment is the same as that of embodiment 3, and is only different in that the addition amounts of the rare earth oxides in the formula powder are different, which is specifically shown in table 2.
Example 8
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate of this embodiment is the same as that of embodiment 3, except that the ZnO-SiO prepared in preparation example 1 is adopted2-Al2O3And (3) glass.
Example 9
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate of this embodiment is the same as that of embodiment 3, except that the ZnO-SiO prepared in preparation example 2 is adopted2-Al2O3And (3) glass.
Example 10
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate of this embodiment is the same as that of embodiment 3, except that the ZnO-SiO prepared in preparation 4 is adopted2-Al2O3And (3) glass.
Example 11
The preparation method of the low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate of this embodiment is the same as that of embodiment 3, except that the ZnO-SiO prepared in preparation example 5 is adopted2-Al2O3And (3) glass.
Table 2 components and mass ratio (wt%) of the powders of the formulations described in the examples
Examples Glass powder Al2O3 La2O3 CeO2 Pr6O11 Nb2O5
1 60 40 - - - -
2 50 40 10 - - -
3 55 35 5 - 5 -
4 52.5 35 5 5 - 2.5
5 55 35 10 - - -
6 55 35 - 10 - -
7 55 35 - 5 - 5
8 55 35 5 - - -
9 55 35 5 - - -
10 55 35 5 - - -
11 45 50 5 - - -
Comparative example 1
The preparation of the low-temperature co-fired ceramic substrate of the comparative example is the same as that of example 3, except that the glass is boron-containing silicate glass powder and the component B2O3(67.5wt%)、SiO2(15.1wt%)、Al2O3(14.3wt%)、ZnO(2.7%)、CaO(0.4wt%)。
Examples of the experiments
The performance of the low-temperature co-fired ceramic substrates prepared in the above examples 1 to 11 and comparative example 1 was tested, and the test results are shown in table 3 below.
Testing the dielectric constant and the dielectric loss of the low-temperature co-fired ceramic material by using an SPDR test method at room temperature and a test frequency of 20 GHz; testing the temperature drift of the low-temperature co-fired ceramic material within the temperature range of room temperature-40-110 ℃ and the testing frequency of 20 GHz; and simultaneously, the bending strength of the low-temperature co-fired ceramic material is tested.
TABLE 3 Properties of sintered samples of the examples
Numbering Dielectric constant Loss tangent Temperature drift (ppm/. degree.C.) Bending strength (MPa)
Example 1 6.6 1.6×10-3 2.8 213
Example 2 7.4 8.3×10-4 1.2 179
Example 3 6.9 1.3×10-3 0.9 194
Example 4 7.2 1.1×10-3 0.7 188
Example 5 7.0 1.5×10-3 1.3 190
Example 6 7.1 1.6×10-3 2.5 185
Example 7 7.1 1.5×10-3 2.3 180
Example 8 6.6 1.1×10-3 1.0 195
Example 9 6.8 1.2×10-3 1.1 192
Example 10 7.2 1.7×10-3 0.9 186
Example 11 7.5 1.2×10-3 2.7 152
Comparative example 1 8.1 5.2×10-3 12 160
Therefore, the low-dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material has the dielectric constant of 7 +/-0.5 and the dielectric loss at room temperature and the test frequency of 20GHz<2×10-3(ii) a The temperature drift is within +/-3 ppm/DEG C within the temperature range of room temperature-40-110 ℃ and the test frequency of 20 GHz; in addition, the flexural strength of the low-temperature co-fired ceramic material>150MPa, can be applied to millimeter wave antenna module in 5G communication.
It should be understood that the above examples are only for clarity of illustration and are not intended to limit the embodiments. Other variations and modifications will be apparent to persons skilled in the art in light of the above description. This need not be, nor should it be exhaustive of all embodiments. And obvious variations or modifications therefrom are within the scope of the invention.

Claims (17)

1. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material is characterized by comprising the following components in percentage by mass based on the total amount of the material:
ZnO-SiO2-Al2O345-65 wt% of glass;
Al2O3 35-50wt%;
0-15 wt% of rare earth oxide.
2. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material of claim 1, wherein the ZnO-SiO is2-Al2O3The glass comprises the following raw material components in percentage by mass:
Figure FDA0002839828930000011
wherein x is 1 or 2, y is 1, 2, 3 or 5;
the R element is at least one selected from Zr element, Ba element, Sb element, Cu element or Ti element.
3. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material of claim 2, wherein the rare earth oxide comprises CeO2、Pr6O11、La2O3、Nb2O5At least one of (1).
4. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material according to any one of claims 1 to 3, wherein Al is controlled in the low-temperature co-fired ceramic material2O3Content of the components and Al in the glass2O3The sum of the contents of (A) and (B) accounts for the low-temperature co-firing43-63 wt% of the total amount of ceramic material.
5. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material according to any one of claims 1 to 4, wherein ZnO and SiO in the glass powder are controlled in the low-temperature co-fired ceramic material2、RxOyRespectively account for 26.55-39.55%, 8.55-13.65% and 0.045-0.65% of the total amount of the low-temperature co-fired ceramic material.
6. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material according to any one of claims 1 to 5, wherein the dielectric constant of the low-temperature co-fired ceramic material is 7 ± 0.5 at room temperature and a test frequency of 20 GHz.
7. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material according to any one of claims 1 to 5, wherein the low-temperature co-fired ceramic material has dielectric loss at room temperature and a test frequency of 20GHz<2×10-3
8. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material according to any one of claims 1 to 5, wherein the temperature drift of the low-temperature co-fired ceramic material is within ± 3ppm/° c at a test frequency of 20GHz in a temperature range of-40 ℃ to 110 ℃.
9. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic material according to any one of claims 1 to 5, wherein the bending strength of the low-temperature co-fired ceramic material is >150 MPa.
10. A low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic slurry, which is characterized by comprising the low-temperature co-fired ceramic material as claimed in any one of claims 1 to 9 and an organic carrier, wherein the low-temperature co-fired ceramic material accounts for 37 to 48 wt% of the slurry.
11. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic slurry of claim 10, wherein the organic vehicle comprises a binder, a plasticizer, and a dissolving agent.
12. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic slurry of claim 11, wherein the organic vehicle further comprises a dispersant and a defoamer.
13. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic slurry of claim 11, wherein:
the binder comprises one of PVA, PVB, polymethyl acrylate, ethyl cellulose, acrylic emulsion and ammonium polyacrylate salt;
the plasticizer comprises one of polyethylene glycol, phthalate and glycol;
the dissolving agent comprises one of water, ethanol, methyl ethyl ketone, trichloroethylene, toluene and xylene.
14. The low dielectric low-loss near-zero temperature drift low-temperature co-fired ceramic slurry of claim 12, wherein:
the dispersing agent comprises one of ammonium polyacrylate, phosphate ester, ethoxy compound and fresh fish oil;
the defoaming agent comprises emulsified silicone oil, a high-alcohol fatty acid ester compound, polyoxyethylene polyoxypropylene pentaerythritol ether, polyoxyethylene polyoxypropylene amine ether, polyoxypropylene glycerol ether and polyoxypropylene.
15. A low dielectric loss and near zero temperature drift low temperature co-fired ceramic green tape, which is characterized by being prepared from the low temperature co-fired ceramic slurry of any one of claims 10 to 14.
16. A low dielectric low loss near zero temperature drift low temperature co-fired ceramic substrate, characterized in that it is made of the low temperature co-fired ceramic material according to any one of claims 1 to 9.
17. A low dielectric loss and near zero temperature drift low temperature co-fired ceramic substrate, which is characterized in that the low temperature co-fired ceramic green tape of claim 15 is prepared by sintering.
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