CN113999002A - Low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material and preparation method thereof - Google Patents
Low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material and preparation method thereof Download PDFInfo
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Abstract
The invention belongs to the technical field of ceramic materials, and discloses a low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material and a preparation method thereof, wherein the chemical formula is Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO‑(y)B2O3](ii) a Wherein the mass ratio of x to y is 1.0: 1.2-1.4: 1.0; dielectric constant εr21.3 to 24.5, a quality factor Qf of 20,496 to 61,801GHz, and a temperature coefficient of resonance frequency τfIs 19.0 to 29.0 ppm/DEG C. The invention adopts the traditional solid phase synthesis method to successfully prepare the high Q microwave dielectric material for LTCC, and utilizes low melting point oxides CuO and B2O3The sintering characteristics of the matrix are adjusted together, the introduction of the two utilizes a liquid phase mass transfer mechanism to accelerate the sintering mass transfer process, thereby not only reducing the sintering temperature of the matrix, but also promoting the material densification process to be lowerThe dielectric constant can be improved to a certain extent by completing the reaction at the temperature.
Description
Technical Field
The invention belongs to the technical field of ceramic materials, and particularly relates to a ceramic composition characterized by components and a preparation method thereof.
Technical Field
In recent years, the development of 5G communication technology has made integration and miniaturization of communication systems urgent. The low temperature co-fired ceramic (LTCC) technology is adapted to the above development, and can embed a passive device in a multilayer ceramic substrate to prepare a high-integration microwave module/assembly, which is an important packaging technology for realizing high performance, miniaturization and high reliability of an electronic system, and many passive devices manufactured based on the LTCC technology, such as dielectric antennas, filters, millimeter wave radars, and the like, have been widely applied to wireless communication. In addition, LTCC technology generally requires that microwave dielectric ceramics can be sintered at temperatures below 961 ℃ (the melting point of Ag, the melting point of Cu is 1064 ℃) or lower to ensure that the interlayer electrode can be co-sintered with the ceramic layer.
Among various microwave dielectric materials, Li2TiO3The microwave dielectric ceramic is a lithium-based rock salt material, has low volume density, is made into a filter with the same volume, and has light weight; the raw materials are relatively cheap; has moderate dielectric constant (epsilon) in millimeter wave bandr22) belonging to the K20 series microwave dielectric material, ensures the miniaturization of the filter and keeps low transmission loss, and is the preferable material for 5G base station filters and future wearable devices. However, in LTCC applications, the sintering temperature (T) is highs1220 ℃ C.). The main methods for reducing the sintering temperature of the microwave dielectric ceramic at present comprise (1) a wet chemical preparation method; (2) performing reaction by using superfine nano powder; (3) by addition of low-melting oxidationThe material is used as sintering aid; (4) adding a glass phase and cooling in a liquid phase sintering mode. The wet chemical method has complex preparation flow and expensive price of the superfine nano powder, and the dielectric property of the dielectric ceramic material is greatly reduced after the glass phase is added, so the addition of a proper amount of low-melting-point oxide becomes the most popular method for reducing the sintering temperature of the dielectric material.
Disclosure of Invention
The present invention is directed to existing Li2TiO3The sintering temperature (T) of the base microwave dielectric material is too highsThe temperature of minus 1220 ℃) can not meet the technical problem of LTCC application, provides a low-temperature sintering high-Q lithium titanate-based microwave dielectric ceramic material and a preparation method thereof, and effectively improves Li by adding low-melting-point oxide2TiO3The sintering characteristic of the microwave dielectric ceramic enables the sintering temperature to be reduced to a lower level on the basis of ensuring a high Q value.
The invention is realized by the following technical scheme:
according to one aspect of the invention, a low-temperature sintering high-Q lithium titanate-based microwave dielectric ceramic material is provided, and the chemical formula is Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3](ii) a Wherein the mass ratio of x to y is 1.0: 1.2-1.4: 1.0.
Further, a dielectric constant εr21.3 to 24.5, a quality factor Qf of 20,496 to 61,801GHz, and a temperature coefficient of resonance frequency τfIs 19.0 to 29.0 ppm/DEG C.
Further, when x: y is 1.4:1.0, the dielectric constant is 21.3 to 24.5.
Further, when x: y is 1.0:1.2, the temperature coefficient of resonance frequency is 19.0-19.4 ppm/DEG C; the temperature coefficient of the resonance frequency is 23.8 to 24.2 corresponding to the dielectric constant, Qf is 33,900 to 41,400 GHz.
Further, when x is 1.0:1.0, the sintering temperature is 750 ℃, the Qf value is 51,500 to 51,636GHz, and the dielectric constant is 23.5 to 23.7.
According to another aspect of the invention, a preparation method of the low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material is provided, and the method is carried out according to the following steps:
(1) according to Li2Ti0.98Mg0.02O2.96F0.04The chemical formula of (1) respectively preparing raw materials of lithium carbonate, titanium dioxide and magnesium fluoride; putting the raw materials into a ball milling tank, performing ball milling, and drying in an air atmosphere;
(2) pre-synthesizing the dried powder obtained in the step (1);
(3) filling the pre-synthesized powder obtained in the step (2) into a ball milling tank, and adding 1 w.t.% of Nb2O5And 1 w.t.% [ (x) CuO- (y) B ]2O3]Drying in air atmosphere after ball milling; wherein the mass ratio of x to y is 1.0: 1.2-1.4: 1.0; wherein 1 w.t.% is Nb2O5Or [ (x) CuO- (y) B2O3]Occupy Li2Ti0.98Mg0.02O2.96F0.04The mass percentage of (A);
(4) granulating the dried powder obtained in the step (3) and forming a blank;
(5) sintering the blank formed in the step (4) at 750-850 ℃ in air atmosphere and preserving heat to obtain Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3]A ceramic material.
Further, the ball milling time of the step (1) and the step (3) is 12 h.
Further, the ball milling agent adopted in the ball milling in the step (1) and the step (3) is absolute ethyl alcohol.
Preferably, the temperature of the pre-synthesis in the step (2) is 800 ℃ and the holding time is 4 h.
Preferably, the sintering temperature in step (5) is 790 ℃, and the holding time is 4 h.
The invention has the beneficial effects that:
the invention adopts the traditional solid phase synthesis method to successfully prepare the high Q microwave dielectric material for LTCC, and utilizes low melting point oxides CuO and B2O3Co-regulation of Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5The sintering characteristic of the matrix and the introduction of the two utilize a liquid phase mass transfer mechanism, the sintering mass transfer process is accelerated, the sintering temperature of the matrix is reduced, the material densification process is promoted to be completed at a lower temperature, and the dielectric constant can be improved to a certain extent. The maximum dielectric constant of the high-Q microwave dielectric material for the lithium titanate-based LTCC technology is 24.5, the maximum Qf value is 61,801GHz, and the temperature coefficient of the resonant frequency is 19.4 ppm/DEG C at the lowest.
Drawings
FIG. 1 is a graph showing the Qf changes of low-temperature sintered lithium titanate-based high Q microwave dielectric ceramics obtained in examples 1 to 16;
FIG. 2 shows the dielectric constants (. epsilon.) of low-temperature sintered lithium titanate-based high Q microwave dielectric ceramics obtained in examples 1 to 16r) And (5) a variation graph.
FIG. 3 shows the temperature coefficient of resonance frequency (. tau.) of low-temperature sintered lithium titanate-based high Q microwave dielectric ceramics obtained in examples 6, 7, 9 and 16f) And (5) a variation graph.
Detailed Description
The present invention is further described in detail below by way of specific examples, which will enable one skilled in the art to more fully understand the present invention, but which are not intended to limit the invention in any way.
Example 1
(1) According to Li2Ti0.98Mg0.02O2.96F0.04The chemical formula of the method comprises the following steps of respectively preparing raw materials of lithium carbonate, titanium dioxide and magnesium fluoride, putting the raw materials into a ball milling tank, ball milling for 12 hours by using absolute ethyl alcohol as a ball milling agent, and then putting slurry into a 120 ℃ drying oven to dry for 4-5 hours in an air atmosphere;
(2) pre-synthesizing the dried powder obtained in the step (1) at 800 ℃ after passing through a 40-mesh sieve, and preserving heat for 4 hours;
(3) sieving the pre-synthesized raw material obtained in the step (2), and adding Nb2O5And [ (x) CuO- (y) B2O3](x is 1.0, y is 1.2) is put into a ball milling pot, absolute ethyl alcohol is used as a ball milling agent, ball milling is carried out for 12h, and thenDrying the slurry in an oven in an air atmosphere;
(4) granulating the dried powder obtained in the step (3) by using paraffin, and forming a blank;
(5) and (4) sintering the blank formed in the step (4) at 750 ℃ in an air atmosphere, and preserving heat for 4 hours to obtain the low-temperature sintered lithium titanate-based high-Q microwave dielectric ceramic.
Example 2
A lithium titanate-based microwave dielectric ceramic was prepared using the method of example 1, except that x was 1.0 and y was 1.0.
Example 3
A lithium titanate-based microwave dielectric ceramic was prepared using the method of example 1, except that x was 1.2 and y was 1.0.
Example 4
A lithium titanate-based microwave dielectric ceramic was prepared using the method of example 1, except that x was 1.4 and y was 1.0.
Example 5
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 1, except that the sintering temperature in step (5) was 790 ℃.
Example 6
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 2, except that the sintering temperature in step (5) was 790 ℃.
Example 7
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 3, except that the sintering temperature in step (5) was 790 ℃.
Example 8
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 4, except that the sintering temperature in step (5) was 790 ℃.
Example 9
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 1, except that the sintering temperature in step (5) was 800 ℃.
Example 10
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 2, except that the sintering temperature in step (5) was 800 ℃.
Example 11
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 3, except that the sintering temperature in step (5) was 800 ℃.
Example 12
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 4, except that the sintering temperature in step (5) was 800 ℃.
Example 13
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 1, except that the sintering temperature in step (5) was 850 ℃.
Example 14
The lithium titanate-based microwave dielectric ceramic was prepared by the method of example 2 except that the sintering temperature in step (5) was 850 ℃.
Example 15
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 3, except that the sintering temperature in step (5) was 850 ℃.
Example 16
A lithium titanate-based microwave dielectric ceramic was prepared by the method of example 4, except that the sintering temperature in step (5) was 850 ℃.
For samples of the lithium titanate-based microwave dielectric ceramics prepared in examples 1 to 16, a dielectric loss test was performed with an Agilent 8720ES network analyzer and a metal closed chamber to obtain fig. 1. For samples of the lithium titanate-based microwave dielectric ceramics prepared in examples 1 to 16, a dielectric constant test was performed with the aid of an Agilent 8720ES network analyzer and a parallel plate open cavity to obtain fig. 2. For samples of the lithium titanate-based microwave dielectric ceramics obtained in example 6, example 9, example 11 and example 12, the resonance frequency temperature coefficient test was performed by means of an Agilent 8720ES network analyzer and a metal closed cavity, and fig. 3 was obtained.
FIG. 1 is a graph showing the Qf changes of the lithium titanate-based microwave dielectric ceramics prepared in examples 1 to 16. As can be seen from FIG. 1, when the sintering temperature is lowered to 750 ℃, the Qf value gradually increases with increasing x: y ratio to 1.0:1.0When the doping ratio is more than 1.0:1.0, the Qf value shows a decreasing tendency, reaches the lowest value at a ratio of 1.4:1, and shows the same tendency of change for the sample sintered at 790 ℃. This shows that CuO and B are controlled during sintering at 750 ℃ and 790 DEG C2O3The optimum Qf value can be obtained by the doping amount ratio of (2). When the sintering temperatures were 800 ℃ and 850 ℃, it was observed that the Qf values varied with CuO and B2O3The increase in the doping amount ratio indicates that when the sintering temperature reaches a certain level, the increase in the doping amount ratio effectively promotes Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3]The Qf value of the ceramic is increased. Sintering temperature (T) with existing lithium titanate-based ceramicssAs compared with Qf value (20,000-50,000 GHz), 1220 deg.C of sintering temp. is reduced by 470 deg.C, and Qf value is raised by-23%.
When CuO and B are added in the secondary ball milling2O3The mass ratio was 1.4:1.0 (i.e., x: y ═ 1.4:1.0), and the Qf value of the system was highest at 61,801GHz at a sintering temperature of 850 ℃. Shows a chemical formula of Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3]The lithium titanate-based microwave dielectric ceramic (x ═ 1.4, y ═ 1.0) has good Qf.
FIG. 2 is a graph showing dielectric constants (. epsilon.) of the lithium titanate-based microwave dielectric ceramics prepared in examples 1 to 16r) And (5) a variation graph. As can be seen from FIG. 2, the dielectric constants of the ceramic samples obtained in examples 1 to 16 were all 21 to 25, indicating that the chemical formula is Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3]The lithium titanate-based microwave dielectric ceramic (the mass ratio of x to y is 1.0: 1.2-1.4: 1.0) belongs to K20 series microwave dielectric materials, not only meets the requirement of low-temperature sintering of LTCC technology, but also can further miniaturize microwave assemblies and keep lower transmission loss.
FIG. 3 shows examples 6, 7, 9 and examples of the present inventionGraph of temperature coefficient of resonance frequency of the lithium titanate-based microwave dielectric ceramic prepared in example 16. As can be seen from FIG. 3, the temperature coefficient of resonance frequency τ is for the sample sintered at the optimum sintering temperature (highest Qf value)fThe pure phase lithium titanate is improved to a certain extent, and the numerical value is reduced by 24 percent. This indicates that CuO and B2O3The introduction of the additive not only reduces the sintering temperature, but also optimizes Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5Temperature stability of the matrix.
For Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3]The temperature coefficient of resonance frequency was minimized (19.4 ppm/deg.C) at x: y of 1.0:1.2 and a sintering temperature of 800 deg.C. Compare Li2TiO3Temperature coefficient of resonance frequency (τ)f+38.5 ppm/. degree.C.). Shows that the sintering temperature can be reduced and the Li can be increased simultaneously in the invention2TiO3Temperature stability of (3).
Although the preferred embodiments of the present invention have been described, the present invention is not limited to the above-mentioned embodiments, which are only illustrative and not restrictive, and those skilled in the art can make various modifications without departing from the spirit and scope of the present invention, which falls within the protection scope of the present invention.
Claims (10)
1. A low-temperature sintering high-Q lithium titanate-based microwave dielectric ceramic material is characterized in that the chemical formula is Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3](ii) a Wherein the mass ratio of x to y is 1.0: 1.2-1.4: 1.0.
2. The low temperature sintered high Q lithium titanate-based microwave of claim 1Dielectric ceramic material characterized by a dielectric constant εr21.3 to 24.5, a quality factor Qf of 20,496 to 61,801GHz, and a temperature coefficient of resonance frequency τfIs 19.0 to 29.0 ppm/DEG C.
3. The low-temperature sintering high-Q lithium titanate-based microwave dielectric ceramic material as claimed in claim 1, wherein when x: y is 1.4:1.0, the dielectric constant is 21.3-24.5.
4. The low-temperature sintering high-Q lithium titanate-based microwave dielectric ceramic material of claim 1, wherein when x: y is 1.0:1.2, the temperature coefficient of resonance frequency is 19.0-19.4 ppm/° C; the temperature coefficient of the resonance frequency is 23.8 to 24.2 corresponding to the dielectric constant, Qf is 33,900 to 41,400 GHz.
5. The low-temperature sintering high-Q lithium titanate-based microwave dielectric ceramic material as claimed in claim 1, wherein when x is 1.0:1.0, the sintering temperature is 750 ℃, the Qf value is 51,500-51,636 GHz, and the dielectric constant is 23.5-23.7.
6. A method for preparing a low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material as claimed in claims 1 to 5, which comprises the following steps:
(1) according to Li2Ti0.98Mg0.02O2.96F0.04The chemical formula of (1) respectively preparing raw materials of lithium carbonate, titanium dioxide and magnesium fluoride; putting the raw materials into a ball milling tank, performing ball milling, and drying in an air atmosphere;
(2) pre-synthesizing the dried powder obtained in the step (1);
(3) filling the pre-synthesized powder obtained in the step (2) into a ball milling tank, and adding 1 w.t.% of Nb2O5And 1 w.t.% [ (x) CuO- (y) B ]2O3]Drying in air atmosphere after ball milling; wherein the mass ratio of x to y is 1.0: 1.2-1.4: 1.0; wherein 1 w.t.% is Nb2O5Or [ (x) CuO- (y) B2O3]Occupy Li2Ti0.98Mg0.02O2.96F0.04The mass percentage of (A);
(4) granulating the dried powder obtained in the step (3) and forming a blank;
(5) sintering the blank formed in the step (4) at 750-850 ℃ in air atmosphere and preserving heat to obtain Li2Ti0.98Mg0.02O2.96F0.04+1w.t.％Nb2O5+1w.t.％[(x)CuO-(y)B2O3]A ceramic material.
7. The preparation method of the low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material as claimed in claim 6, wherein the ball milling time of step (1) and step (3) is 12 h.
8. The preparation method of the low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material as claimed in claim 6, wherein the ball milling agent used in the ball milling in the steps (1) and (3) is absolute ethyl alcohol.
9. The preparation method of the low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material as claimed in claim 6, wherein the pre-synthesis temperature in the step (2) is 800 ℃, and the holding time is 4 h.
10. The preparation method of the low-temperature sintered high-Q lithium titanate-based microwave dielectric ceramic material as claimed in claim 6, wherein the sintering temperature in the step (5) is 790 ℃, and the holding time is 4 h.
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101362647A (en) * | 2008-09-05 | 2009-02-11 | 西安交通大学 | Low temperature sintering lithium-base microwave dielectric ceramic material and preparation thereof |
| WO2018010633A1 (en) * | 2016-07-12 | 2018-01-18 | 深圳顺络电子股份有限公司 | Cbs-class ltcc material and manufacturing method thereof |
| CN108191426A (en) * | 2018-01-17 | 2018-06-22 | 天津大学 | A kind of intermediate sintering temperature high q-factor microwave dielectric material |
| CN111606705A (en) * | 2020-04-16 | 2020-09-01 | 天津大学 | high-Q light microwave dielectric material for 5G base station ceramic filter |
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2021
- 2021-12-09 CN CN202111501140.3A patent/CN113999002A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101362647A (en) * | 2008-09-05 | 2009-02-11 | 西安交通大学 | Low temperature sintering lithium-base microwave dielectric ceramic material and preparation thereof |
| WO2018010633A1 (en) * | 2016-07-12 | 2018-01-18 | 深圳顺络电子股份有限公司 | Cbs-class ltcc material and manufacturing method thereof |
| CN108191426A (en) * | 2018-01-17 | 2018-06-22 | 天津大学 | A kind of intermediate sintering temperature high q-factor microwave dielectric material |
| CN111606705A (en) * | 2020-04-16 | 2020-09-01 | 天津大学 | high-Q light microwave dielectric material for 5G base station ceramic filter |
Non-Patent Citations (2)
| Title |
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| DONG WANG ET AL.: "A low-sintering temperature microwave dielectric ceramic for 5G LTCC applications with ultralow loss", 《CERAMICS INTERNATIONAL》 * |
| JONG-BONG LIM ET AL.: "Effect of B2O3 and CuO additives on the sintering temperature and microwave dielectric properties of Ba(Mg1/3Nb2/3)O3 ceramics", 《MATERIALS RESEARCH BULLETIN》 * |
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