JPH04264369A - Manufacture of full solid voltage memorizing element - Google Patents

Abstract

PURPOSE:To offer the manufacture of a full solid voltage memorizing element; in which short circuit occurrence, due to soil on a solid electrolyte layer side surface caused by the use of a forming die, is prevented, and having a simplified manufacturing process and an excellent characteristic; in the manufacture of the full solid voltage memorizing element. CONSTITUTION:A full solid voltage memorizing element is composed by forming a solid electrolyte layer 2 with solid electrolyte powder pressurized in a resin- made cylinder 1, inserting electrode material powder from the upper and lower sides of the solid electrolyte layer 2, forming an electrode layer 3 by pressurization forming, moreover joining a copper wire 4 with conductive carbon paste 5, and applying the upper and lower parts with an epoxyresin system powder paint 6. The unnecessariness of taking out a full solid voltage memorizing element main body to outside from a die, can prevent soiling the side surface of the solid electrolyte layer due to the electrode material powder adhering to a forming die inner wall, also a short circuit between both electrode layers, and also can omit a process for grinding the main body side surface of the full solid voltage memorizing element.

Description

[Detailed description of the invention]

0001

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for manufacturing an all-solid-state voltage storage element using a solid electrolyte.

0002

[Prior Art] All-solid-state voltage memory elements mainly consist of electrode layers/
It consists of three layers: a solid electrolyte layer/an electrode layer, and conventionally, all-solid-state voltage storage elements have been manufactured by laminating and pressing these three layers together using the same molding die. Specifically, a solid electrolyte is pressure-molded in a mold, electrode materials are placed on the top and bottom of this mold, and the electrode layer/solid is removed from the mold by integral pressure molding. Forming the main body of the voltage storage element consisting of an electrolyte layer/electrode layer,
After that, in order to remove the electrode material attached to the side surface of the solid electrolyte layer of the main body, the side surface of this solid electrolyte layer is scraped, the lead terminal is bonded using carbon paste, and further,
In order to prevent damage to the element and peeling of lead terminals, all-solid-state voltage memory elements were manufactured by sealing with resin.

0003

However, in the conventional manufacturing method described above, after the main body of the all-solid-state voltage memory element is molded, when the main body of the voltage memory element is taken out from the molding mold,
The side surfaces of the solid electrolyte layer are often contaminated by electrode material adhering to the inner wall of the mold, resulting in a short circuit between the two electrodes. Therefore, it is necessary to shave the side surface of the molded body, which takes a lot of time to manufacture, and there is a problem that the body is damaged in the process of scraping the side surface of the body.

[0004] The present invention solves the above problems,
The object of the present invention is to provide a manufacturing method capable of manufacturing an all-solid-state voltage memory element with excellent reliability using a simplified process.

[0005]

[Means for Solving the Problems] In order to achieve the above object, the present invention involves pressure-molding a solid electrolyte layer and a pair of electrode layers sandwiching the solid electrolyte layer in a resin cylinder.

[0006]

[Operation] Therefore, according to the present invention, since pressure molding is performed in a resin cylinder and the main body of the all-solid-state voltage memory element is not taken out, the electrode material adhered to the inner wall of the molding die. Powder does not adhere to the side surfaces of the solid electrolyte layer, preventing short circuits between the two electrodes arranged above and below through the solid electrolyte layer, and eliminating the step of scraping the side surfaces of the solid electrolyte layer. , the manufacturing method can be simplified.

[0007]

Embodiment A method of manufacturing an all-solid-state voltage memory element according to an embodiment of the present invention will be described below with reference to the drawings.

[0008] First, AgI, Ag2O, and WO3 are weighed out in a molar ratio of 4:1:1 and mixed in an alumina mortar. This mixture was pressure-molded to form a molded body, which was then sealed in a Pyrex tube under reduced pressure and allowed to melt and react at a temperature of 400° C. for 17 hours. The reaction product was wet-pulverized in a ball mill and classified into 4AgI/Ag2WO of 200 mesh or less.
A silver ion conductive solid electrolyte powder represented by 4 was obtained.

[0009] Next, vanadium oxide represented by V2O5 and metal silver powder are weighed so that the molar ratio is 1:0.7, and mixed in a mortar. The mixture was pressure-molded to form a molded body, then sealed in a quartz tube under reduced pressure and heated to 600℃ for 4 hours.
Allow to react for 8 hours. The reaction product was crushed in a mortar and classified to obtain an electrode active material powder made of silver vanadium oxide represented by Ag0.7V2O5 with a size of 200 mesh or less.

FIG. 1 shows a cross section of an all-solid-state voltage memory element for explaining the manufacturing method in one embodiment of the present invention, and shows the solid electrolyte powder and electrode active material powder obtained in the above-mentioned preparatory stage. Using this method, an all-solid-state voltage memory element was fabricated. First, an electrode material was prepared by mixing a solid electrolyte powder and an electrode active material powder so that the content of the electrode active material in the electrode layer was 30%. First, add 30% of the above solid electrolyte powder.
By weighing 0 mg and pressurizing it at a pressure of 2 ton/cm2 in a resin cylinder 1 made of epoxy resin or the like,
A solid electrolyte layer 2 is formed. Next, add 20 mg of electrode material to 2
The solid electrolyte layer 2 is placed between the top and bottom of a resin cylinder 1 and pressurized at a pressure of 4 ton/cm 2 to form two electrode layers 3 . Next, tin-plated copper wires 4 are bonded to these two electrode layers 3 with conductive carbon paste 5, and the gaps between the two electrode layers 3 and the upper and lower open ends of the resin cylinder 1 are filled with epoxy resin. powder coating 6
was filled at a temperature of 150°C.

Next, as a comparative example, an all-solid-state voltage memory element was manufactured using a conventional manufacturing method. First, an electrode material was prepared by mixing the solid electrolyte powder obtained by the method shown in the above example and the electrode active material powder so that the electrode layer contained 30% of the electrode active material. Next, 300 mg of solid electrolyte powder was weighed and pressure-molded at 2 tons/cm2. Next, two parts of 30 mg of the electrode material were weighed out, inserted into the mold in which the solid electrolyte layer had been formed from above and below, and integrally press-molded at 4 ton/cm2. This molded body is removed from the mold, tin-plated copper wires are bonded to the upper and lower electrode layers of the molded body using conductive carbon paste, and the entire body is coated with epoxy resin powder paint at a temperature of 150°C. It was sealed with.

[0012] 100 samples of all-solid-state voltage storage elements were prepared using the above-described embodiment of the present invention and the conventional manufacturing method.
In order to make a prototype and check for short circuits at the end of the element, we
The battery was charged at a constant voltage of 100 mV for 2 hours, and the holding voltage (memory voltage) was examined 2 hours later. The measurement results are shown in FIG. As is clear from FIG. 2, in the comparative example manufactured by the conventional manufacturing method, the storage voltage rapidly decreases due to a short circuit on the side surface of the solid electrolyte layer. On the other hand, it can be seen that in the sample manufactured by the manufacturing method of the example, no short circuit occurs on the side surface of the solid electrolyte layer 2, so that the decrease in storage voltage is extremely small.

Although epoxy resin was used as the resin material for the resin cylinder 1 in this embodiment, it is not limited to epoxy resin, but may also be used such as phenol resin, urea resin, vinyl chloride resin,
It goes without saying that the same effect can be obtained using silicone resin. It goes without saying that the same effect can be obtained even if the cross-sectional shape of the resin cylinder 1 is polygonal, such as a triangle or a quadrangle, in addition to a circle.

According to the above embodiment, since the electrode layer 3 and the solid electrolyte layer 2 are integrally pressure-molded in the resin cylinder 1, a short circuit occurs between the two electrode layers 3. Therefore, the effect that the holding voltage does not drop rapidly can be obtained.

[0015]

[Effects of the Invention] As is clear from the above examples, the present invention provides a method for manufacturing an all-solid-state voltage memory element having a solid electrolyte layer and electrode layers above and below the solid electrolyte layer. Because the solid electrolyte layer and the two electrode layers sandwiching it are pressure-molded inside the cylinder, it is possible to eliminate short circuits on the sides of the main body of the all-solid-state voltage memory element. Not only can the process of scraping the side surface be omitted, but also the process of sealing the entire body with powder coating is not required, and an all-solid-state voltage memory element with excellent reliability can be manufactured.

[Brief explanation of the drawing]

FIG. 1 is a cross-sectional view showing the structure of an all-solid-state voltage storage element manufactured according to an embodiment of the present invention.

FIG. 2 is a characteristic diagram comparing the storage voltage retention characteristics of an all-solid-state voltage storage element manufactured by an embodiment of the present invention and a conventional manufacturing method.

[Explanation of symbols]

1. Resin cylinder 2 Solid electrolyte layer 3 Electrode layer

Claims (1)

[Claims] 1. A method for manufacturing an all-solid-state voltage memory element comprising an ion-conductive solid electrolyte layer and a pair of electrode layers sandwiching the solid electrolyte layer, wherein the A method for manufacturing an all-solid-state voltage memory element, which comprises press-molding a solid electrolyte layer and an electrode layer.