KR20160135462A - Multi-junction pellet of thermal battery for preventing crack and manufacturing method theref - Google Patents

Multi-junction pellet of thermal battery for preventing crack and manufacturing method theref Download PDF

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Publication number
KR20160135462A
KR20160135462A KR1020150068772A KR20150068772A KR20160135462A KR 20160135462 A KR20160135462 A KR 20160135462A KR 1020150068772 A KR1020150068772 A KR 1020150068772A KR 20150068772 A KR20150068772 A KR 20150068772A KR 20160135462 A KR20160135462 A KR 20160135462A
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South Korea
Prior art keywords
electrolyte
powder
pellet
lif
junction
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KR1020150068772A
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Korean (ko)
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KR101736903B1 (en
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하상현
김기열
조성백
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국방과학연구소
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/30—Deferred-action cells
    • H01M6/36—Deferred-action cells containing electrolyte and made operational by physical means, e.g. thermal cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/14—Cells with non-aqueous electrolyte
    • H01M6/18—Cells with non-aqueous electrolyte with solid electrolyte
    • H01M6/182—Cells with non-aqueous electrolyte with solid electrolyte with halogenide as solid electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/42—Grouping of primary cells into batteries
    • H01M6/46—Grouping of primary cells into batteries of flat cells

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The present invention relates to a method for manufacturing a multi-junction pallet for preventing crack of the pallet which is easily manufactured comparing to a process for manufacturing a single pallet of a thermal battery. The present invention can be manufactured as one pallet in which a cathode, an anode, and an electrolyte pallet are stacked on one another. The multi-junction pallet can reduce the defect ratio of the battery by reducing a breaking phenomenon of the pallet during a stacking manufacturing process of the battery, and reduce manufacturing costs of the battery since the overall multi-layered number is simplified.

Description

TECHNICAL FIELD [0001] The present invention relates to a multi-junction pellet for preventing cracking of a thermal cell pellet,

The present invention relates to a method for producing a multiple junction pellet for preventing breakage of pellets which can be used in a thermocouple, which is a type of military or industrial non-accumulator battery, and more particularly to a method for producing a multiple junction pellet by pelletizing a cathode, an electrolyte and a cathode pellet ≪ / RTI >

The inside of a thermal battery is constituted by laminating parts such as an anode, a cathode, an electrolyte, a heat source, and a current collector, and one set of three pellets of an anode, a cathode and an electrolyte constitutes a unit cell.

2. Description of the Related Art Generally, an anode, a cathode, and an electrolyte in a thermocouple are separately manufactured in the form of pellets or discs by using a method of pressing a raw material powder uniaxial as a porous material.

However, it is difficult to form pellets having high strength due to a small contact area between the raw powder particles, and the thickness of each pellet is as thin as about 0.3 mm, which is not easy to handle in the production of electrodes, A variety of techniques are being explored to increase gender.

Japanese Patent Laid-Open No. 2009-152094 (2009.07.09) U.S. Patent No. 4,013,818 (issued Mar. 23, 1977)

In order to increase the bonding force between raw powder particles in the production of a pellet for a thermal battery, a method of mixing with a eutectic salt powder having excellent ductility and compression molding has been performed. However, even when this method is applied, it is possible to observe a phenomenon in which pellets are cracked or broken during pellet production. In order to form an anode having excellent strength, a press having high pressurizing ability is required. As a result, It became a cause.

Accordingly, an object of the present invention is to provide a method for producing a multiple junction pellet in which an anode, a cathode, and an electrolyte are bonded to each other instead of a method in which pellets of an anode, a cathode, and an electrolyte are formed by compression in a multi- It is another object of the present invention to provide a multi-junction pellet for preventing breakage of a pellet for a thermal cell produced by the same manufacturing method.

In order to achieve the above object, a method of manufacturing a multiple bonded pellet for preventing breakage of a pellet for a thermal battery according to the present invention is characterized in that a positive electrode powder is placed in a press mold, and one side of the positive electrode powder is pressed with a first pressure by a hydraulic press to form a positive electrode An anode compression step, an electrolyte compression step in which an electrolyte powder is placed on the anode, and an electrolyte is formed by pressurizing one side of the electrolyte powder with a hydraulic press with a hydraulic press, and a negative electrode powder is placed on the electrolyte formed in the electrolyte compression step, A negative electrode pressing step of pressing one side of the powder to a third pressure to form a negative electrode, and forming a multi-junction pellet having a structure in which the positive electrode, the electrolyte and the negative electrode are multi-bonded.

The first pressure is applied by applying 50% of a preset reference pressing force.

The second pressure is compressed by applying 80% of a predetermined reference pressing force, and then the pressing is stopped for 10 seconds after being compressed.

The second pressure is applied by applying 100% of a preset reference pressing force.

And selected from the positive electrode powder is a Li-Si, the cathode powder is FeS 2, In addition, the electrolyte powder is LiCl-KCl, LiCl-LiF, LiF-LiCl-LiBr, LiF-CaF 2, LiF-KF and LiF-NaF May be used.

The multiple junction pellet according to the present invention comprises a cathode layer composed of anode powder, a cathode layer composed of cathode powder, and an electrolyte layer bonded between the anode layer and the cathode layer and composed of electrolyte powder.

The positive electrode powder is a Li-Si, the cathode powder is FeS 2, the electrolyte powder as is selected from the group consisting of LiCl-KCl, LiCl-LiF, LiF-LiCl-LiBr, LiF-CaF 2, LiF-KF and LiF-NaF And may include any one or more of them.

The method for producing a multiple junction pellet for preventing breakage of a pellet for a thermal cell according to the present invention can produce one multiple pellet having a thickness of about 1 mm in which a cathode, an anode and an electrolyte pellet each having a thickness of about 0.3 mm are laminated to each other have.

In the multi-junction pellet thus produced, the total number of stacked layers is simplified, the strength of the pellet is improved, and the cracking of the pellet is reduced in the manufacturing process of the battery in which the respective pellets are stacked, thereby facilitating handling and reducing the defective ratio of the battery. The manufacturing cost of the battery also decreases.

In addition, the multi-junction pellet of the present invention has an effect of improving the performance of the battery because it not only prevents breakage but also reduces the internal resistance by reducing the contact resistance of each pellet.

FIG. 1A is a process diagram of an anode compression step in a method of manufacturing a multiple junction pellet for preventing breakage of a pellet for a thermal cell of the present invention. FIG.
FIG. 1B is a process diagram of a step of pressing an electrolyte in a method of manufacturing a multiple junction pellet for preventing breakage of a pellet for a thermal cell of the present invention.
1C is a process diagram of a negative electrode compacting step in a method of manufacturing a multiple junction pellet for preventing cracking of a pellet for a thermal cell of the present invention.
2 shows a top or bottom view of the inventive multi-junction pellet.
3 shows a side view of the inventive multi-junction pellet.
4 is a conceptual view of a multiple junction pellet including an anode, a cathode, and an electrolyte.
Figure 5 is a multiple-junction pellet made through one embodiment of the present invention.
6 shows the results of a comparison of the battery discharge test between the multi-junction pellet and the single pellet.

Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the accompanying drawings. It is to be understood, however, that the invention is not intended to be limited to the particular forms disclosed, but on the contrary, is intended to cover all modifications, equivalents, and alternatives falling within the spirit and scope of the invention. The terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention.

A method for manufacturing a multi-junction pellet formed by multi-junctioning an anode, an electrolyte and an anode includes the steps of: preparing a positive electrode by placing a positive electrode powder in a press mold and pressing one side of the positive electrode powder with a hydraulic press to form a positive electrode; And a negative electrode pressing step of pressing the negative electrode powder on the electrolyte formed in the electrolyte pressing step and pressing the positive electrode, the electrolyte, and the negative electrode to form a multi-junction structure in which the positive electrode, Molding is performed in a pellet form.

At this time, in the negative electrode material powder has an Li-Si, as in the positive electrode material powder can be used for FeS 2 (Pyrite), In addition, the electrolyte powder is LiCl-KCl, LiCl-LiF, LiF-LiCl-LiBr, of the LiF-CaF 2, LiF-KF-NaF and LiF can be used at least either one.

FIG. 1A is a process diagram of an anode compression step in a method of manufacturing a multiple junction pellet for preventing thermal pellet breakage according to an embodiment. FIG.

As shown in FIG. 1A, in the anodic pressing step, about 0.53 g of the positive electrode powder is put into a press mold, and the upper surface of the positive electrode powder is made uniform, and then the press mold is raised to about 10 mm so that the electrolyte can be supplied. Then, when the positive electrode powder is pressurized to one side by the hydraulic pressure by the hydraulic press, and the preset pressure is 1600 psi (Pound per square inch) used in the conventional single pellet pressing, About 800 psi, which is 50% of the pressure, the first pressure is applied and the press is released after pressing.

FIG. 1B is a view illustrating a process of a step of pressing an electrolyte in a method of manufacturing a multiple junction pellet for preventing breakage of a pellet for a thermal battery according to an embodiment.

As shown in Fig. 1B, the electrolyte pressing step supplies 0.62 g of the electrolytic powder directly to the squeezed anode. The one end of the supplied electrolyte powder is pressurized to a second pressure using a hydraulic press, wherein the second pressure is about 1300 psi which is 80% of the predetermined reference pressure of 1600 psi, The positive electrode is pressed together with the positive electrode. At this time, in order to increase the pressing force between the anode and the electrolyte, the press is stopped for about 10 seconds after the pressing. After stopping, the press mold is again raised about 10 mm to secure a space for supplying the cathode powder.

FIG. 1C is a view illustrating a process of a negative electrode pressing step in a method of manufacturing a multiple junction pellet for preventing breakage of a pellet for a thermal battery according to an embodiment.

Specifically, in the negative electrode pressing step, 0.34 g of the negative electrode powder is supplied, and one side of the negative electrode powder is pressurized to the third pressure using a hydraulic press. The third pressure compresses the anode, the electrolyte and the cathode together at 1600 psi, which is 100% of the preset reference pressure.

The pellet may be broken due to a spring back phenomenon in which the thickness of the pellet is restored to its original value by residual stress due to the residual stress in the pellet formed in the formed pellet. To press down the side of the press mold that encloses the pellet so that the pellet is not broken.

The multiple bonded pellets formed by the manufacturing method of the above embodiment are formed in the form of a multi-junction in which respective layers of the anode layer 10, the electrolyte layer 20 and the cathode layer 30 are bonded to each other, and the anode layer 10, It can be seen that the electrolyte layer 20 and the negative electrode layer 30 have a multilayer pellet having a thickness of about 0.3 mm and a total thickness of the pellet of about 1 mm. 2 to Fig. 5.

As a comparative example for comparing the amount of active material with the multiple junction pellets according to an embodiment of the present invention, a cathode, an electrolyte and a cathode which are single pellets are produced. At this time, 0.34 g of the negative electrode powder, 0.62 g of the electrolyte powder and 0.53 g of the positive electrode powder were made equal to the amount of the multiple pellets according to one embodiment, and all the pellets were produced at a pressure of 1600 psi.

The multi-junction pellet is manufactured in the same manner as in the above embodiment. For comparison with the above-described comparative example, the same amount of current is experimentally measured when the battery discharge test is performed.

As shown in FIG. 6, in the discharge test of the battery, the multi-junction pellet showed a voltage (V) higher than that of the single pellet by about 5%, which is because the contact resistance of the multiple pellets was smaller than that of the single pellet, This reduction in internal resistance leads to an increase in battery performance. Therefore, it can be seen that the performance of the multi-junction pellet is about 5% higher than that of the single pellet.

While the present invention has been described with reference to exemplary embodiments, it is to be understood that the invention is not limited to the disclosed exemplary embodiments, but, on the contrary, is intended to cover various modifications and equivalent arrangements included within the spirit and scope of the invention. It will be understood that various modifications and changes may be made in the present invention.

Claims (12)

Pressing a positive electrode powder into a press mold and pressing one side of the positive electrode powder to a first pressure with a hydraulic press to form a positive electrode;
An electrolyte compression step of putting an electrolyte powder on the anode and pressurizing one side of the electrolyte powder with a second pressure with a hydraulic press to form an electrolyte; And
And a negative electrode pressing step of placing a negative electrode powder on the electrolyte formed in the electrolyte pressing step and pressurizing one side of the negative electrode powder with a third pressure with a hydraulic press to form a negative electrode, wherein the positive electrode, the electrolyte and the negative electrode are multi- A method for producing multiple bonded pellets.
The method of claim 1, wherein the first pressure is applied by applying 50% of a predetermined reference pressure.
2. The method of claim 1, wherein the second pressure is applied by applying 80% of a preset reference pressure.
The method of claim 1, wherein the third pressure is 100% of a predetermined reference pressing force.
The method of any one of claims 2 to 4, wherein the reference pressing force is 1600 psi.
The method of claim 1, wherein the positive electrode powder is Li-Si.
The method of claim 1, wherein the negative electrode powder is FeS 2 .
The electrolyte according to claim 1, wherein the electrolyte powder is selected from the group consisting of LiCl-KCl, LiCl-LiF, LiCl-KCl, LiF-LiCl-LiBr, LiF-CaF2, LiF- / RTI >
A positive electrode layer composed of positive electrode powder;
A negative electrode layer composed of a negative electrode powder; And
And an electrolyte layer joined between the anode layer and the cathode layer and composed of an electrolyte powder.
The multi-junction pellet according to claim 9, wherein the positive electrode powder is Li-Si.
The multi-junction pellet according to claim 9, wherein the negative electrode powder is FeS 2 .
The electrolyte according to claim 9, wherein the electrolyte powder is selected from the group consisting of LiCl-KCl, LiCl-LiF, LiCl-KCl, LiF-LiCl-LiBr, LiF-CaF2, LiF- Multiple junction pellets to prevent breakage of pellets for thermal cells.
KR1020150068772A 2015-05-18 2015-05-18 Method for manufacturing of multi-junction pellet of thermal battery for preventing crack KR101736903B1 (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR102140804B1 (en) * 2020-01-31 2020-08-03 국방과학연구소 Thermo battery electrode production apparatus and Thermo battery electrode production method
KR20200139487A (en) * 2019-06-04 2020-12-14 국방과학연구소 Current collector comprising heat source, thermal battery and method for producing thereof

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8394520B2 (en) 2009-04-06 2013-03-12 Eaglepicher Technologies, Llc Thermal battery electrolyte materials, electrode-electrolyte composites, and batteries including same

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20200139487A (en) * 2019-06-04 2020-12-14 국방과학연구소 Current collector comprising heat source, thermal battery and method for producing thereof
KR102140804B1 (en) * 2020-01-31 2020-08-03 국방과학연구소 Thermo battery electrode production apparatus and Thermo battery electrode production method

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