Multilayer ceramic electrical card material and method for manufacturing the same

Abstract

The application belongs to the field of electric calorimetric refrigeration, and particularly relates to a multilayer ceramic electric calorimetric material and a preparation method thereof. x Ti 1‑x O3-Li2CO3; wherein 0.15<=x<=0.3, 1%<=Li2CO3<=10%. The application mainly controls the electric calorimetric effect, sintering temperature and sintering density of the pre-sintered ceramic powder by changing the zirconium-titanium ratio and the content of the sintering aid. The pre-sintered ceramic powder after the component regulation of the application successfully passes the flow casting process to form the MLCs device, and the MLCs device has large electric calorimetric effect and low manufacturing cost.

Description

TECHNICAL FIELD

[0001] The present application belongs to the field of electrocaloric refrigeration, and more particularly, to a sheet-type multilayer ceramic (MLCs) electrocaloric material and a preparation method thereof. BACKGROUND

[0002] Refrigeration technology is widely used in military, industrial, medical and daily life fields. At present, the realization of refrigeration still relies on vapor compression refrigeration technology. However, this refrigeration technology is low in efficiency, and the fluorine-containing refrigerant used thereby can cause destruction of the ozone layer and bring serious environmental pollution. The electrocaloric effect refers to phase transition and dipole orientation of ferroelectric materials under the induction of an electric field, thereby causing entropy change and temperature change of the materials, realizing heat transport and refrigeration. The electrocaloric effect of the electrocaloric material does not need to use a compressor and fluorinated refrigerant to realize, and thus has the characteristics of small size and environmental friendliness, and has high refrigeration efficiency.

[0003] At present, the electrocaloric materials mainly focus on organic ferroelectric polymer electrocaloric materials and inorganic ferroelectric ceramic materials. Compared with the organic ferroelectric polymer electrocaloric materials, the inorganic ferroelectric ceramic has high polarization rate, large electrocaloric strength, rich phase structure and various regulation methods, and thus is concerned in the research of the electrocaloric effect. So far, a series of inorganic ferroelectric ceramic electrocaloric materials with application potential have been developed, mainly including BaTiO3-based, Bi 0.5 Na 0.5 TiO3-based, K 0.5 Na 0.5 NbO3-based and PbTiO3-based ceramics. Due to the harm of lead-containing materials to human body and environment, at present, the research of the ferroelectric ceramic electrocaloric material mainly focuses on BaTiO3-based lead-free ceramics. Compared with ceramic bulk and ceramic thin film, ceramic thick film has large heat capacity and large breakdown field strength. Further, the MLCs electrocaloric material based on the ceramic thick film can further improve the heat capacity of the electrocaloric ceramic, and has larger breakdown field strength, and thus can obtain larger field-induced temperature change.

[0004] At present, the production equipment and preparation process of the BaTiO3-based MLCs material are relatively mature, which lays a foundation for the BaTiO3-based sheet-type multilayer ceramic electrocaloric material to be practical, but the electrocaloric effect still needs to be further enhanced.

[0005] In the past few years, researchers still mainly use pure BaTiO3 as the matrix material of the MLCs. In 2010, Kar-Narayan et al. developed a BaTiO3-based MLCs, which has a single layer thickness of 6.5 μm and a total of 200 layers, and has a maximum temperature change of 2.5 K at 300 kV cm -1only 0.55 K under electric field (Appl. Phys. Lett. 96, 192902 (2010).). Liu et al. developed BaTiO3 ceramic MLCs (single layer thickness of 11 microns, 150 layers) in 2016, which had a temperature change of only 0.6 K at 182 kV cm -1 under electric field (Appl. Phys. Lett. 109, 212902 (2016).). Kar-Narayan and Faye et al. also studied BaTiO3 ceramic, but failed to improve the electric caloric effect of MLCs to more than 0.8 K (Appl. Phys. Lett. 102, 032903 (2013).; J. Phys. D Appl. Phys. 50, 464002 (2017).). In addition, in 2021, researchers tested the electric caloric performance of BaTiO3-based Y5V type commercial MLCs, and the temperature change was only 0.46 K at 300 kV cm -1 Therefore, although MLCs can endow the ceramic body with a higher working electric field, due to the low electric caloric strength of most BaTiO3-based MLC ceramic bodies, it is still difficult for MLCs to break through the temperature change of 0.8 K.

[0006] On the other hand, the sintering temperature of BaTiO3-based MLC ceramic body is usually around 1500℃, and due to the high sintering temperature, only precious metal electrodes with high price can withstand the sintering of electrodes and ceramic body together, which is not conducive to its popularization and use. Therefore, it is urgent to develop a BaTiO3-based MLC electric caloric material with high giant electric caloric temperature change, low material cost and low sintering temperature. SUMMARY

[0007] In order to solve the above problems, the present application provides a sheet type multilayer ceramic material with giant electric caloric effect and a preparation method thereof. The present application changes the BaZr x Ti 1-xThe zirconium-to-titanium ratio in O3, the final sintering temperature, and the proportion of sintering aids are all used to regulate the enhancement of the electrocaloric effect. Firstly, adjusting the zirconium-to-titanium ratio aims to achieve multiphase coexistence in the material, increasing the number of polarized states within the material in its initial, unfielded state, thus increasing the entropy and consequently the temperature change. Secondly, adjusting the sintering temperature controls the grain size. A suitable grain size is beneficial for the breakdown of MLCs and also helps release internal stress, inducing highly polarized phases and enhancing the electrocaloric strength of the material. Furthermore, lithium carbonate, a commonly used sintering aid, effectively lowers the sintering temperature and improves the density during sintering. Lowering the sintering temperature allows for the use of cheaper metals as internal electrodes, reducing costs, and also enhances the electrocaloric temperature change of MLCs.

[0008] To achieve the above objectives, according to one aspect of the present invention, the present invention first provides a method for preparing a barium titanate-based multilayer ceramic material, comprising:

[0009] Step 1: According to the chemical formula BaZr x Ti 1-x The stoichiometric ratio of Ba, Zr, and Ti atoms in O3 was determined by weighing BaCO3, TiO2, and ZrO2 raw materials and ball milling the raw materials, wherein 0.15 ≤ x ≤ 0.3;

[0010] Step 2: The ceramic powder is subjected to a first sintering to obtain BaZr. x Ti 1-x O3 powder;

[0011] Step 3: Mix Li2CO3 with BaZr x Ti 1-x O3 powder was mixed and ball-milled a second time to obtain BaZr. x Ti 1-x O3-Li2CO3 ceramic powder;

[0012] Step 4: The ceramic powder is sintered a second time to obtain pre-fired powder;

[0013] Step 5: Grind the pre-calcined powder; mix the ground pre-calcined powder with solvent, dispersant, plasticizer and binder and ball mill to obtain cast colloid;

[0014] Step 6: Filter and vacuum process the cast colloid to eliminate coagulated colloid and air bubbles;

[0015] Step 7: Cast the colloid to obtain a film tape;

[0016] Step 8: Deposit electrodes onto the adhesive film strip and stack the adhesive film strips with electrodes to form a multilayer adhesive film strip;

[0017] Step 9: performing final sintering on the multilayer adhesive film to obtain a multilayer ceramic electrical capacitor material.

[0018] Further, the Li2CO3 in step 3 is mixed with the BaZr x Ti 1-x The mass fraction of the Li2CO3 in the BaZr

[0019] Further, the ball milling conditions in steps 1, 3 and 5 are as follows: the mass ratio of the ball milling medium, the ball milling solvent and the ball milling raw material is (3-4):(0.7-1):1; and the ball milling time is 1-24 hours.

[0020] Further, the first sintering and the second sintering in steps 2 and 4 are performed at a temperature rising rate of 0.1-50℃ / min to 900-1100℃ and for 1-3 hours.

[0021] Further, the mass ratio of the pre-sintered powder, the solvent, the dispersant, the plasticizer and the binder in step 5 is 1:0.6:(0.001-0.012):(0.001-0.012):(0.1-0.5), preferably 1:0.6:0.006:0.006:0.3.

[0022] Further, the solvent in step 5 is preferably a mixed solution of ethanol and toluene; the dispersant in step 5 is preferably polyethylene glycol; the plasticizer in step 5 is preferably butyl benzyl phthalate; and the binder in step 5 is preferably a mixed colloid of polyvinyl butyral and ethanol.

[0023] Further, the electrode in step 8 is a noble metal electrode, and the noble metal is one or a combination of Ag, Pt, Pd, Au and Ru.

[0024] Further, the noble metal electrode in step 8 is an Ag / Pd composite electrode, and the mass fraction of Ag in the Ag / Pd composite electrode is 50%-70%.

[0025] Further, the final sintering in step 9 is performed at a temperature rising rate of 5-50℃ / min to 1150-1300℃ and for 1-3 hours.

[0026] According to another aspect of the present application, the present application also provides a BaTiO3-based multilayer ceramic material prepared by the above method.

[0027] In general, the above technical solution conceived by the present application can achieve the following beneficial effects:

[0028] (1) The present application can improve the BaZr xTi 1-x O3-Li2CO3, the preparation process is simple, and the temperature change of the electric calorimetric material is increased.

[0029] (2) The sintering temperature of the ceramic material is effectively reduced, the density in the sintering process is improved, and the electric calorimetric temperature change of the material is improved by introducing the sintering aid Li2CO3 in a preferred proportion.

[0030] (3) The self-density and breakdown field strength of the ceramic adhesive film belt to be sintered are improved by adjusting the component ratio of the flow casting adhesive, and the temperature change performance of the sheet type multilayer ceramic is indirectly improved.

[0031] (4) The preferred electrode type can further reduce the final sintering temperature of the ceramic adhesive film belt to be sintered, and reduce the energy consumption in the preparation process. BRIEF DESCRIPTION OF DRAWINGS

[0032] Figure 1 is BaZr x Ti 1-x O3-Li2CO3 sheet type multilayer ceramic.

[0033] Figure 2 is BaZr x Ti 1-x O3-Li2CO3 sheet type multilayer ceramic under a constant electric field of 250 kV / cm. DETAILED DESCRIPTION

[0034] In order to make the purpose, technical scheme and advantages of the present application clearer, the present application will be further described in detail below in combination with the drawings and examples. It should be understood that the specific examples described herein are only used to explain the present application and are not used to limit the present application. In addition, the technical features involved in each embodiment of the present application described below can be combined with each other as long as they do not conflict with each other.

[0035] Example 1:

[0036] Preparation of BaZr 0.3 Ti 0.7 O3 sheet type multilayer ceramic electric calorimetric material (x=0.3), comprising the following steps:

[0037] Step 1: According to the stoichiometric ratio of Ba, Zr and Ti in the BaZr 0.3 Ti 0.7 O3 chemical formula, BaCO3, TiO2 and ZrO2 raw materials are weighed, and the raw materials are mixed and ball milled to obtain ceramic powder;

[0038] Step 2: sintering the ceramic powder to obtain BaZr 0.3 Ti 0.7 O3 pre-sintered powder, the pre-sintering temperature is 1100℃, the heating rate is 3℃ / min, and the holding time is 3h;

[0039] Step 3: weighing Li2CO3 according to the mass ratio of BaZr 0.3 Ti 0.7 O3-2wt.% Li2CO3 and mixing with BaZr 0.3 Ti 0.7 O3 pre-sintered powder to obtain BaZr 0.3 Ti 0.7 O3-2wt.% Li2CO3 ceramic powder; the ball milling process is wet ball milling, the mass ratio of ball milling medium, solvent and ball milling material is 4:0.7:1, and the ball milling time is 1 hour.

[0040] Step 4: sintering the BaZr 0.3 Ti 0.7 O3-2wt.% Li2CO3 ceramic powder to obtain pre-sintered powder;

[0041] Step 5: grinding the pre-sintered powder; weighing the ground pre-sintered powder, solvent, dispersant, plasticizer and binder in a ratio of 1:0.6:0.006:0.006:0.3 and mixing ball milling to obtain a casting gel; wherein the solvent is a mixed solution of ethanol and toluene; the dispersant is polyethylene glycol; the plasticizer is butyl benzyl phthalate; and the binder is a mixed gel of polyvinyl butyl and ethanol (the weight ratio of polyvinyl butyl and ethanol is 1:5);

[0042] Step 6: filtering and vacuuming the casting gel to eliminate condensed gel and bubbles;

[0043] Step 7: casting the casting gel to obtain a gel film strip;

[0044] Step 8: plating Pt electrode on the gel film strip and stacking the gel film strip with Pt electrode to form a multi-layer ceramic green body;

[0045] Step 9: sintering the multi-layer ceramic green body: heating to 1180℃ at a rate of 5℃ / min and holding for 3 hours, and then reducing to room temperature in the furnace to obtain a sheet type multi-layer ceramic electrical card material, the electrical card temperature change of the obtained sheet type multi-layer ceramic under an electric field of 323K and 250kV / cm is 0.85K.

[0046] Example 2:

[0047] Preparation of BaZr 0.2 Ti 0.8O3 sheet-type multilayer ceramic electrical card material (x=0.2), including the following steps:

[0048] Step 1: According to BaZr 0.2 Ti 0.8 The stoichiometric ratio of Ba, Zr, and Ti in the chemical formula of O3 is used to weigh out raw materials BaCO3, TiO2, and ZrO2, and the raw materials are mixed and ball-milled to obtain ceramic powder;

[0049] Step 2: Sinter the ceramic powder to obtain BaZr. 0.2 Ti 0.8 O3 pre-calcined powder, pre-calcination temperature is 1100℃, heating rate is 5℃ / min, holding time is 3h;

[0050] Step 3: Prepare Li2CO3 according to BaZr 0.2 Ti 0.8 Weigh out O3-2 wt.% Li2CO3 and mix with BaZr. 0.2 Ti 0.8 O3 pre-calcined powder was mixed and ball-milled a second time to obtain BaZr. 0.2 Ti 0.8 O3-2wt.%Li2CO3 powder; the ball milling process is wet ball milling, the mass ratio of ball milling media, solvent and ball milling material is 3:0.7:1, and the ball milling time is 24 hours.

[0051] Step 4: Prepare BaZr according to steps 4-9 in Example 1. 0.2 Ti 0.8 O3-2wt.%Li2CO3 sheet-type multilayer ceramic green body;

[0052] Step 5: Sinter the multilayer ceramic green body: heat to 1180℃ at 25℃ / min and hold for 3 hours, then cool to room temperature in the furnace to obtain MLCs electrical card material.

[0053] like Figure 1 As shown, this is the BaZr in Embodiment 2. 0.2 Ti 0.8 SEM image of the cross-section of the O3-2 wt.% Li2CO3 sheet-like multilayer ceramic electrode. The obtained sheet-like multilayer ceramic electrode is continuous and has no obvious pores inside.

[0054] like Figure 2 As shown, this is the BaZr in Embodiment 2. 0.2 Ti 0.8 The electrocaloric temperature change curve of O3-2 wt.%Li2CO3 multilayer ceramic plates under a constant electric field of 250kV / cm is given as a function of temperature. The obtained electrocaloric temperature change of the multilayer ceramic plates under an electric field of 323K and 250kV / cm is 1.2K.

[0055] Example 3

[0056] Preparation of BaZr 0.15 Ti 0.85 O3 multilayer ceramic material (x = 0.15) comprising the following steps:

[0057] Step 1 : The required BaCO3, TiO2 and ZrO2 raw materials were weighed according to the stoichiometric ratio of BaZr 0.15 Ti 0.85 O3 and ball-milled to obtain ceramic powder;

[0058] Step 2: The ceramic powder was sintered to obtain BaZr 0.15 Ti 0.85 O3 pre-sintered powder, the pre-sintering temperature was 900°C, the heating rate was 5°C / min, and the holding time was 3h;

[0059] Step 3: Li2CO3 was weighed according to the mass ratio of BaZr 0.15 Ti 0.85 O3-2 wt.% Li2CO3 and mixed with BaZr 0.15 Ti 0.85 O3 pre-sintered powder for secondary ball-milling; the ball-milling process was wet ball-milling, the mass ratio of ball-milling medium, solvent and ball-milling material was 3:1:1, and the ball-milling time was 24 hours.

[0060] Step 4: BaZr 0.15 Ti 0.85 O3-2 wt.% Li2CO3 multilayer ceramic green body was prepared according to steps 4-9 in Example 1;

[0061] Step 5: The multilayer glue green body was sintered: heated to 1180°C at a rate of 50°C / min and held for 3 hours, then cooled to room temperature in the furnace to obtain MLCs electric card material. The sheet multilayer ceramic obtained has an electric card temperature change of 1.05K under an electric field of 323K, 250kV / cm.

[0062] Example 4

[0063] BaZr 0.2 Ti 0.8 O3 multilayer ceramic electric card material was prepared according to the manner of Example 2, wherein the mass fraction of Li2CO3 in step (3) was changed to 0.1 wt.%, 1 wt.%, 5 wt.%, 10 wt.% and 15 wt.% respectively, and the electric card temperature change of the sheet multilayer ceramic obtained under an electric field of 323K, 250kV / cm and the final sintering temperature are shown in Table 1.

[0064] Table 1 Electric card properties of sheet multilayer ceramics prepared with different Li2CO3 additive contents

[0065]

[0066] Example 5

[0067] BaZr was prepared according to Example 1. 0.3 Ti 0.7 O3 sheet-type multilayer ceramic electric card material (x=0.3), with different component ratios in the cast colloid, the volume density, limiting working electric field and electric card temperature change performance of different cast colloids are shown in Table 2.

[0068] Table 2. Bulk density and limiting electric field of sheet-like multilayer ceramics prepared under different casting colloidal composition ratios.

[0069]

[0070]

[0071] Example 6

[0072] BaZr was prepared according to the method in Example 4. 0.2 Ti 0.8 O3 sheet-type multilayer ceramic electrical card material (x=0.2), including the following steps:

[0073] Step 1: According to BaZr 0.3 Ti 0.7 The chemical formula of O3 is obtained by weighing out the required proportions of BaCO3, TiO2 and ZrO2 raw materials, mixing and ball milling them to obtain ceramic powder;

[0074] Step 2: Sinter the dried ceramic powder to obtain BaZr. 0.2 Ti 0.8 O3 pre-calcined powder, pre-calcination temperature is 1100℃, heating rate is 3℃ / min, holding time is 3h;

[0075] Step 3: Prepare Li2CO3 according to BaZr 0.2 Ti 0.8 Weigh out O3-1wt.%Li2CO3 by mass ratio and mix with BaZr. 0.2 Ti 0.8 O3 pre-calcined powder is mixed and then ball-milled a second time; the ball milling process is wet ball milling, the mass ratio of ball milling media, solvent and ball milling material is 3:0.7:1, and the ball milling time is 24 hours.

[0076] Step 4: The BaZr after secondary ball milling... 0.2 Ti 0.8 Pre-sintered powder was obtained by sintering O3-1wt.%Li2CO3 ceramic powder;

[0077] Step 5: grinding the pre-sintered powder; taking the pre-sintered powder, solvent, dispersant, plasticizer and binder after grinding according to the ratio of 1:0.6:0.006:0.006:0.3 to mix and ball mill to obtain a tape casting colloid; wherein the solvent is a mixed solution of ethanol and toluene; the dispersant is polyethylene glycol; the plasticizer is butyl benzyl phthalate; the binder is a mixed colloid of polyvinyl butyl and ethanol (the weight ratio of polyvinyl butyl and ethanol is 1:5);

[0078] Step 6: filtering and vacuumizing the tape casting colloid to eliminate condensed colloid and bubbles;

[0079] Step 7: tape casting the tape casting colloid to obtain a film strip;

[0080] Step 8: plating Ag / Pd composite electrode on the film strip and stacking the film strip with the composite electrode to form a multi-layer ceramic green body;

[0081] Step 9: sintering the multi-layer ceramic green body: heating to 1300℃ at a rate of 5℃ / min and keeping for 3 hours, and then cooling to room temperature in the furnace to obtain a sheet multi-layer ceramic electric calorimetric material.

[0082] Wherein, the influence of different Ag / Pd mass ratios on the performance of the multi-layer ceramic electric calorimetric material is shown in Table 3:

[0083] Table 3 Performance table of multi-layer ceramic electric calorimetric material obtained under different Ag / Pd mass ratios (under an electric field of 323K, 250kV / cm)

[0084] Ag / Pd mass ratio Final sintering temperature Temperature change Electrode cost (relative to pure Pt) 50:50 1250℃ 0.8K -269.6 yuan / g 60:40 1220℃ 0.85K -294.1 yuan / g 70:30 1160℃ 0.86K -318.7 yuan / g 80:20 1130℃ 0.6K -343.2 yuan / g 20:80 1340℃ 0.75K -196.1 yuan / g 10:90 1370℃ 0.75K -171.5 yuan / g Pure Pd 1445℃ 0.7K -147 yuan / g

[0085] Comparative Example 1

[0086] Preparation of BaZr 0.4 Ti 0.6 O3-2 wt.%Li2CO3 sheet multi-layer ceramic electric calorimetric material (x=0.4), comprising the following steps:

[0087] Step 1: taking the required BaCO3, TiO2 and ZrO2 raw materials according to the stoichiometric ratio of BaZr 0.4 Ti 0.6 O3 to mix and ball mill to obtain ceramic powder;

[0088] Step 2: sintering the dried ceramic powder to obtain BaZr 0.4 Ti 0.6 O3 pre-sintered powder, the pre-sintering temperature is 1100℃, the heating rate is 5℃ / min, and the holding time is 3h;

[0089] Step 3: taking Li2CO3 according to BaZr 0.4 Ti0.6 O3-2 wt. % Li2CO3 mass ratio and mixed with BaZr 0.4 Ti 0.6 O3 presintered powder mixture was secondarily ball-milled;

[0090] Step 4: BaZr 0.4 Ti 0.6 O3 sheet multilayer ceramic green compact was prepared;

[0091] Step 5: the multilayer ceramic green compact was sintered: heated to 1180°C at a rate of 5°C / min, kept for 3 hours, and then cooled down to room temperature to obtain an MLCs electric card material. The electric card temperature variation of the obtained electric card material under an electric field of 323K and 250kV / cm was 0.77K.

[0092] Comparative Example 2

[0093] BaZr 0.1 Ti 0.9 O3-2 wt. % Li2CO3 sheet multilayer ceramic electric card material (x = 0.1) comprising the following steps:

[0094] Step 1: BaZr 0.1 Ti 0.9 O3 stoichiometric ratio of the required BaCO3, TiO2 and ZrO2 raw materials were weighed and ball-milled to obtain ceramic powder;

[0095] Step 2: the dried ceramic powder was sintered to obtain BaZr 0.1 Ti 0.9 O3 presintered powder, the presintering temperature was 1100°C, the heating rate was 5°C / min, and the holding time was 3h;

[0096] Step 3: Li2CO3 was weighed according to BaZr 0.1 Ti 0.9 O3-2 wt. % Li2CO3 mass ratio and mixed with BaZr 0.1 Ti 0.9 O3 presintered powder mixture was secondarily ball-milled;

[0097] Step 4: BaZr 0.1 Ti 0.9 O3 sheet multilayer ceramic green compact was prepared;

[0098] Step 5: the multilayer ceramic green compact was sintered: heated to 1180°C at a rate of 5°C / min, kept for 4 hours, and then cooled down to room temperature to obtain an MLCs electric card material. The electric card temperature variation of the obtained electric card material under an electric field of 323K and 250kV / cm was 0.72K.

[0099] It is to be understood that the above description is intended to be illustrative and not restrictive. Many other embodiments will be apparent to those of skill in the art upon reading and understanding the above description. The scope of the application should, therefore, be determined with reference to the appended claims, along with the full scope of equivalents to which such claims are entitled.

Claims

1. A method of producing a barium titanate-based multilayer ceramic material, characterized by, The application comprises the following steps: Step 1 : BaZr x Ti 1-x The stoichiometric ratio of Ba, Zr, Ti in BaTiO3is taken as BaCO3, TiO2and ZrO2raw materials and the ceramic powder is obtained by ball milling the raw materials, wherein 0.15≤x≤0.3; Step 2: The ceramic powder is sintered for the first time to obtain BaZr x Ti 1-x O3 powder; Step 3: Li2CO3 and BaZrxTi 1-x O3 powder were mixed and ball-milled for 2 hours to obtain BaZr x Ti 1-x O3 - Li2CO3 ceramic powder; the mass fraction of Li2CO3 in the BaZrxTi 1-x O3 - Li2CO3 ceramic powder is 2-5 wt.%. Step 4: The BaZr x Ti 1-x sintering the pre-sintered powder at 0.1~50℃ / min to 900~1100℃ and keeping for 1~3 hours. Step 5: grinding the pre-sintered powder; weighing the pre-sintered powder, solvent, dispersant, plasticizer and binder, mixing and ball-milling to obtain a casting gel, the mass ratio of the pre-sintered powder, solvent, dispersant, plasticizer and binder being 1:0.6:(0.004-0.006):(0.001-0.006):(0.3-0.5); the solvent is a mixture of ethanol and toluene; the dispersant is polyethylene glycol; the plasticizer is butyl benzyl phthalate; and the binder is a mixture of polyvinyl butyral and ethanol; Step 6: filtering and vacuumizing the casting gel to remove condensed gel and air bubbles; Step 7: casting the casting gel to obtain a gel film strip; Step 8: plating an electrode on the gel film strip and stacking the gel film strip with the electrode to form a multi-layer gel film strip; Step 9: final sintering the multi-layer gel film strip to obtain a multi-layer ceramic electrical card material; the final sintering conditions are as follows: heating at 5-50℃ / min to 1150-1180℃ and keeping the temperature for 1-3 hours.

2. The production method according to claim 1, characterized by, The ball-milling conditions in steps 1, 3 and 5 are as follows: the mass ratio of the ball-milling medium, ball-milling solvent and ball-milling raw material being (3-4):(0.7-1):1; and the ball-milling time being 1-24 hours.

3. The preparation method according to claim 1, characterized in that, In step 5, the mass ratio of the pre-sintered powder, solvent, dispersant, plasticizer and binder is 1:0.6:0.006:0.006:0.

3.

4. The preparation method according to claim 1, characterized in that, The electrode in step 8 is a noble metal electrode, and the noble metal is one or a combination of Ag, Pt, Pd, Au and Ru.

5. The preparation method according to claim 1, characterized in that, The noble metal electrode in step 8 is an Ag / Pd composite electrode, and the mass fraction of Ag in the Ag / Pd composite electrode is 50%-70%.

6. A barium titanate-based multi-layer ceramic material prepared by the method of any one of claims 1-5.

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