JPS59127375A - Manufacture of solid electrolyte battery - Google Patents
Manufacture of solid electrolyte batteryInfo
- Publication number
- JPS59127375A JPS59127375A JP13283A JP13283A JPS59127375A JP S59127375 A JPS59127375 A JP S59127375A JP 13283 A JP13283 A JP 13283A JP 13283 A JP13283 A JP 13283A JP S59127375 A JPS59127375 A JP S59127375A
- Authority
- JP
- Japan
- Prior art keywords
- solid electrolyte
- mold
- negative electrode
- electrolyte layer
- electrolyte battery
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Classifications
-
- 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
Landscapes
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Primary Cells (AREA)
Abstract
Description
【発明の詳細な説明】
末完８Ａはリチウムなどのアルカリ金属を負極活物質と
する固体電解質電池の製造法の改良（で係り、負極と固
体電解質層との圧着を容易にし、かつ負極と固体電解質
層との密着性を高めて放電性能の良好な固体電解質電池
を提供することを目的とする。[Detailed Description of the Invention] Shukan 8A is an improvement in the manufacturing method of a solid electrolyte battery using an alkali metal such as lithium as a negative electrode active material. It is an object of the present invention to provide a solid electrolyte battery with good discharge performance by increasing adhesion with an electrolyte layer.
一般に固体電解質電池では正峨、固体電解質および負極
を層状に積み重ねた構造を採用しているが、負極を構成
するリチウムなどのアルカリ金属が金型への粘着性が強
く、金型に残留して短絡発生の原因になるため、従来は
負極と固体電ＩｖＩ！質層との圧着は金型によらず、負
極の一方の面に集電板を当接した状態で負極の他方の面
を固体市解質層に押し付けることによって行なわれてい
た。そのため負極と固体電解質層との界面の充分な密着
性が得られず、負極の放電利用率が低下するとともに、
抑圧により負極の周縁部が固体電解質層を越えて正、５
ｔ＜１１１１１・＼流出して短絡が生じるのを防止する
ために、負１赦は電解質径より若干小さくしなければな
らず、そのため負極の充填量自体も低下して、実質的な
放電界かが非常に低下するきいう欠点があった。Generally, solid electrolyte batteries employ a structure in which a positive electrode, a solid electrolyte, and a negative electrode are stacked in layers, but the alkali metals such as lithium that make up the negative electrode have strong adhesion to the mold and may remain on the mold. Conventionally, the negative electrode and solid-state electrode IvI! Pressure bonding with the solute layer was carried out without using a mold, by pressing the other side of the negative electrode against the solid solute layer with a current collector plate in contact with one side of the negative electrode. Therefore, sufficient adhesion at the interface between the negative electrode and the solid electrolyte layer cannot be obtained, and the discharge utilization rate of the negative electrode decreases.
Due to suppression, the periphery of the negative electrode crosses the solid electrolyte layer and becomes positive, 5
t<11111・＼In order to prevent leakage and short circuit, the negative electrode must be made slightly smaller than the electrolyte diameter, so the filling amount of the negative electrode itself decreases and the actual discharge field becomes smaller. There was a drawback that the value decreased significantly.
本発明者らはそのような事情に鑑み、負極と固体電解質
の圧着を金型で行なうことができるようにすべく種々研
究を喧ねた結果、負極と固体電解質層との圧着ＶＣ捺し
、金型と負極との接面にステアリン酸などの高級脂肪酸
またはその塩を介在させるさきは、前述の目的が容易に
達成され、負礒七固体電解質層との密着性を高めること
ができ、かつ負櫃径を固体電解質層と同径にすることが
できることを見出し、本発明を完成するにいたった。In view of such circumstances, the inventors of the present invention have carried out various studies in order to make it possible to press-bond the negative electrode and solid electrolyte layer with a mold. By interposing a higher fatty acid such as stearic acid or a salt thereof on the contact surface between the mold and the negative electrode, the above-mentioned purpose can be easily achieved, and the adhesion with the negative solid electrolyte layer can be improved. It was discovered that the diameter of the tube can be made the same as that of the solid electrolyte layer, and the present invention was completed.
かかる本発明によれば、正極と固体７し解質層との圧着
および固体電解質層と負極との圧着を同一の金型で連続
的に行なうことができ、しかも電池としての機能を有す
る正極、固体電解質層および負極からなる発電要素の形
で金型から取り出すことができるので、固体電解質と正
極との２層成形体を金型から取り出し負極との圧着を別
工程で行なわざるを得なかった従来法に比べて工程面で
も簡略化できて有利であり、しかも負極と固体電解質層
との密着度を高くすることができるので、従来法だ比べ
て放電性能が著しく向上する。According to the present invention, the positive electrode and the solid electrolyte layer and the solid electrolyte layer and the negative electrode can be continuously pressed together using the same mold, and the positive electrode has the function of a battery. Since it can be taken out of the mold in the form of a power generation element consisting of a solid electrolyte layer and a negative electrode, it was necessary to take out the two-layer molded body of the solid electrolyte and positive electrode from the mold and perform crimping with the negative electrode in a separate process. Compared to the conventional method, this method is advantageous in that it can be simplified in terms of process, and since the degree of adhesion between the negative electrode and the solid electrolyte layer can be increased, the discharge performance is significantly improved compared to the conventional method.
高級脂肪酸としては例えばパルミチン酸、ステアリン酸
、オレイン酸、リノール酸、リルン酸などが用いられ、
高級脂肪酸塩としてはそれらの高級脂肪酸とバリウム、
ナトリウム、リチウム、カルシウム、鉛、亜鉛などとの
塩が用いられる。Examples of higher fatty acids used include palmitic acid, stearic acid, oleic acid, linoleic acid, and lylunic acid.
As higher fatty acid salts, these higher fatty acids and barium,
Salts with sodium, lithium, calcium, lead, zinc, etc. are used.
それらの中でも特にステアリン酸バリウムおよびステア
リン酸カルシクムが好ましい。Among them, barium stearate and calcium stearate are particularly preferred.
つぎに本発明の実施例を図面とともに説明する。Next, embodiments of the present invention will be described with reference to the drawings.
実施例１
下型（Ｊ］）、側型（６）および上型α４からなる金型
の下型αＤと側型曹をセットし、側型（２）の内周面に
ステアリン酸バリウム（１４ａ）を塗布した（′ＭＩｊ
１図）。Example 1 A lower mold αD and a side mold carbon are set in a mold consisting of a lower mold (J]), a side mold (6), and an upper mold α4, and barium stearate (14a ) was applied (′MIj
Figure 1).
Ｌｉ５Ｎ−Ｌｉｌ粉末を下型（１１）と側型＠で形成さ
れるキャビディ内に入れ、上型ａ４を降下させて０．５
ｔ々２（Ｄ圧力テＬｉ５ Ｎ Ｌｉ Ｉを直径６ＷＩ
Ｉ！、厚さ０．２ｍに加圧成）［モ１−て固体電解を層
（１）を形成した（第２図）。Put the Li5N-Lil powder into the cavity formed by the lower mold (11) and the side mold @, and lower the upper mold a4 to 0.5
t2 (D pressure te Li5 N Li I to diameter 6WI
I! A layer (1) of solid electrolyte was formed by pressurizing to a thickness of 0.2 m (Fig. 2).
上型Ｑを引きあげ（第３図）、上記固体電解質（１）上
にヨウ化鉛４部（体積部、以下同様）とカルボニルニッ
ケル１都とからなる混合粉末５０Ｍｖを入れ、■、５ｔ
／ｃＩＭ２の圧力で加圧成形して正＋６ （２）および
固体心解−ＩＭ′層（１）からなる２層ペレットとした
（第４図）。Lift up the upper mold Q (Fig. 3), put 50Mv of a mixed powder consisting of 4 parts of lead iodide (parts by volume, hereinafter the same) and 1 part of carbonyl nickel on the solid electrolyte (1), and
The pellet was press-molded at a pressure of /cIM2 to obtain a two-layer pellet consisting of a positive +6 layer (2) and a solid-core core-IM' layer (1) (FIG. 4).
つぎに、下型Ｃυを下峰させ（なお下型；１］）を取り
除いても固体電解質層（１）および正極（２）は径方向
外方へ広がろうとするスプリングバック現象により金型
から落下しない）、側型（６）の内周面および下型Ｕυ
の凸部（ｌｌａ）上面にステアリン酸バリウム（１４ｂ
）を塗布しく第５図）、固体電解質層（１１に厚さＱ、
２Ｍｍｍ、直径５屑のリチウム板を押しっけ、下型αυ
を上昇させて１．５ ｔ／ｃＩＮ２の圧力でリチウム板
を固体電解質層（１）に圧着して負極（３）とした（第
６図）。Next, even if the lower mold Cυ is lowered (the lower mold; 1]) is removed, the solid electrolyte layer (1) and the positive electrode (2) are released from the mold due to the springback phenomenon in which they try to spread outward in the radial direction. (not fall), inner peripheral surface of side mold (6) and lower mold Uυ
barium stearate (14b) on the upper surface of the convex part (lla)
) is applied (Fig. 5), solid electrolyte layer (thickness Q at 11,
Push the lithium plate of 2 mm diameter and 5 pieces into the lower mold αυ
The lithium plate was pressed onto the solid electrolyte layer (1) at a pressure of 1.5 t/cIN2 to form a negative electrode (3) (FIG. 6).
上記のようにして作製した発電要素を、周縁部にセラミ
ック製リング（４）を溶着した集電板（５）のセラミッ
ク製リング（４）内に負極（３）側から入れ、正極（２
）上を他方の集電板（６）で覆い、該集電板（６）の周
縁部とセラミック製リング（４）を溶着して封口し第７
図に示すような固体′鐵解質電池を組み立てた。なお第
７図において、（７）は集電＆（５）、（６）とセラミ
ラミ特性を第８図に曲線Ａで示す。The power generation element produced as described above is placed from the negative electrode (3) side into the ceramic ring (4) of the current collector plate (5), which has a ceramic ring (4) welded to the periphery.
) is covered with the other current collector plate (6), and the peripheral edge of the current collector plate (6) and the ceramic ring (4) are welded to seal the seventh
A solid-state iron electrolyte battery as shown in the figure was assembled. In addition, in FIG. 7, (7) is current collection & (5), (6), and the ceramic ceramic characteristics are shown by curve A in FIG.
比較例１
ステアリン酸バリウムを用力なかった点を除いては実施
例１と同様にして金型で固体電解質層と正極とを圧着し
て２層構造のペレットとしたのち金型から取り出した。Comparative Example 1 The solid electrolyte layer and the positive electrode were pressed together in a mold to form a pellet with a two-layer structure in the same manner as in Example 1, except that barium stearate was not used, and the resulting pellet was taken out from the mold.
つぎに、一方の面に集電板を押し付けた直径５羽、厚さ
０．２Ｍｍのリチウム板を前記２層構造のベレットの固
体電解質側に約５０ｋｇ／ｃｍ２ （ＩＪチクム板が変
形しない程度の圧力）で押し付けて発電要素を作製し、
実施例１と同型の電池を組み立てた。Next, a lithium plate with a diameter of 5 blades and a thickness of 0.2 mm, with a current collector plate pressed against one side, was placed on the solid electrolyte side of the two-layer structure pellet at a weight of about 50 kg/cm2 (at a weight of about 50 kg/cm2 (just enough to prevent the IJ Chikum plate from deforming). pressure) to create a power generation element,
A battery of the same type as in Example 1 was assembled.
この電池を２０°Ｃ，１０μＡの定′屯流で放電させた
ときの放電特性を第８図に曲線Ｂで示す。The discharge characteristics of this battery when it was discharged at 20 DEG C. and a constant current of 10 .mu.A are shown by curve B in FIG.
第８図に示すように、本発明による場合は従来法による
場合に比べて放電容量が大きい。これは負極と固体電解
質との密着度が高いことに基づくものと考えられる。As shown in FIG. 8, the discharge capacity according to the present invention is larger than that according to the conventional method. This is considered to be due to the high degree of adhesion between the negative electrode and the solid electrolyte.
なお￥雄側においては、側型（２）内周面のリチウムと
の接触しない面にもステアリン酸バリウムを塗布したが
、これはステアリン酸バリウムの塗布により側型＠内周
面への固体電解質粉末や正極粉末の付着ならびに上型（
１３の降下、上昇に伴なう摩擦による金型の損傷を防止
しうるからである。ただし、これらの部位へのステアリ
ン酸バリウムの塗布は必ず必要とされるものではなく、
負極と金型とが接触する部位にステアリン酸バリウムが
塗布されていれば目的が達成される。なお、負極と固体
電解質層との界面、固体電解質層と正極との界面（では
ステアリン酸バリウムが付着しないようにするのが好寸
しＡｏ
′Ｘ施雄側
ステアリン酸バリウムに代えてステアリン酸カルシクム
を用いたほかは実施例１と同様にして固体電解質電池を
製造した。放電特性は実施例１の電池と同様であった。On the male side, barium stearate was also applied to the inner peripheral surface of the side mold (2) that did not come in contact with lithium; Adhesion of powder and cathode powder and upper mold (
This is because damage to the mold due to friction caused by the lowering and raising of the mold 13 can be prevented. However, application of barium stearate to these areas is not always necessary;
The purpose can be achieved if barium stearate is applied to the area where the negative electrode and the mold come into contact. Note that it is best to prevent barium stearate from adhering to the interface between the negative electrode and the solid electrolyte layer, and the interface between the solid electrolyte layer and the positive electrode. A solid electrolyte battery was manufactured in the same manner as in Example 1 except that the battery was used.The discharge characteristics were the same as those of the battery in Example 1.
実施例３
ステアリン酸バリウムに代えてパルミチン酸カルシクム
を用いたほかは実施例１と同様にして固体電解質電池を
製造した。放電特性は実施例１の電池と同様であった。Example 3 A solid electrolyte battery was manufactured in the same manner as in Example 1 except that calcium palmitate was used in place of barium stearate. The discharge characteristics were similar to the battery of Example 1.
実施例４
負極としてリチウム板に代えてリチウム粉末とＬ ｌ
３ Ｎ Ｌ ｒ Ｉ粉末との混合物を用いたほかは実
施例１と同様にして固体電解質電池を製造した。金型へ
のリチウムの付着はなかった。なお、この実施例４では
負極構成材であるリチウムとＬｉ５Ｎ−ＬｉＩとを粉末
状で金型に供給する関係上、正極と固体電解質層との圧
着後、金型の上下を反転させた。Example 4 Lithium powder and lithium instead of lithium plate as negative electrode
A solid electrolyte battery was manufactured in the same manner as in Example 1 except that the mixture with 3N L r I powder was used. There was no adhesion of lithium to the mold. In this Example 4, since lithium and Li5N-LiI, which are negative electrode constituent materials, were supplied to the mold in powder form, the mold was turned upside down after the positive electrode and the solid electrolyte layer were pressed together.
第１〜６図は本発明の方法により固体電解質電池を製造
するときの主要工狸を模式的に示す断面図、弛１図は木
発明に係る固体電解質電池の一例を示す断面図、第８図
は木発明の方法により製造された固体電解質電池と従来
法により製造された固体電解質電池の放電特性図である
。
（１）・・・固体電解質層、 （２）・・・正極、 （
３）・・・負極、（１１）・・・下型、 ｔ１２・・・
側型、 （埒・・・上型、（１４ａ）、（１４ｂ）・・
・ステアリン酸パリクム特許出頒人 日立マクセル株式
会社
芳５図 ７６図
″７ｔ７図Figures 1 to 6 are cross-sectional views schematically showing the main components when producing a solid electrolyte battery by the method of the present invention, Figure 1 is a cross-sectional view showing an example of the solid electrolyte battery according to the invention, and Figure 8 The figure is a discharge characteristic diagram of a solid electrolyte battery manufactured by the method of the Wood invention and a solid electrolyte battery manufactured by the conventional method. (1)...Solid electrolyte layer, (2)...Positive electrode, (
3)...Negative electrode, (11)...Lower mold, t12...
Side mold, (埒...upper mold, (14a), (14b)...
・Paricum Stearate Patent Distributor Hitachi Maxell Co., Ltd. Yoshi 5 Figure 76''7t7 Figure
Claims (1)
質とを圧着する工程を経る固体電解質電池の製造におい
て、負極と金型との接面に高級脂肪酸または高級脂肪酸
塩を介在させて固体電＋ｌ＋（ｄ 質と負極とを圧着す
ることを特徴とする固体電解質電池の製造法。 ２、 アルカリ金属がリチウムである特許請求の範囲第
１項記）戒の固体電解質電池の製造法。 ３、高級脂肪酸がパルミチン酸、ステアリン酸、オレイ
ン酸、リノール酸捷たはリルン酸である特許請求の範囲
第１項または第２項記載の固体電解質電池の製造法。 ４ 高級脂肪酸塩が高級脂肪酸とパリクム、ナトリウム
、リチウム、カルシタム、細首たは亜鉛との塩である特
許請求の範囲第１項または第２項記載の固体電解質電池
め製造法。 ５、 高級脂肪酸塩がステアリン酸バリウムである特許
請求の範囲第１項または第２項記載の固体電解質電池の
製造法。 ６、 高級脂肪酸塩がステアリン酸カルシウムである特
許請求の範囲第１項または第２項記載の固体電解質電池
の製造法。[Claims] 1. In the production of a solid electrolyte battery through the process of press-bonding a negative electrode containing an alkali metal as a negative electrode active material and a solid electrolyte, higher fatty acids or higher fatty acid salts are added to the contact surface between the negative electrode and the mold. 2. A method for manufacturing a solid electrolyte battery characterized by compressing a solid electrode and a negative electrode by interposing the solid electrolyte battery. Manufacturing method. 3. The method for producing a solid electrolyte battery according to claim 1 or 2, wherein the higher fatty acid is palmitic acid, stearic acid, oleic acid, linoleic acid, or lylunic acid. 4. The method for producing a solid electrolyte battery according to claim 1 or 2, wherein the higher fatty acid salt is a salt of a higher fatty acid and palicum, sodium, lithium, calcitam, fine neck, or zinc. 5. The method for producing a solid electrolyte battery according to claim 1 or 2, wherein the higher fatty acid salt is barium stearate. 6. The method for producing a solid electrolyte battery according to claim 1 or 2, wherein the higher fatty acid salt is calcium stearate.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP13283A JPS59127375A (en) | 1983-01-04 | 1983-01-04 | Manufacture of solid electrolyte battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP13283A JPS59127375A (en) | 1983-01-04 | 1983-01-04 | Manufacture of solid electrolyte battery |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS59127375A true JPS59127375A (en) | 1984-07-23 |
Family
ID=11465500
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP13283A Pending JPS59127375A (en) | 1983-01-04 | 1983-01-04 | Manufacture of solid electrolyte battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS59127375A (en) |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5482628A (en) * | 1977-11-25 | 1979-07-02 | Mallory & Co Inc P R | Solid cell and method of producing same |
-
1983
- 1983-01-04 JP JP13283A patent/JPS59127375A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5482628A (en) * | 1977-11-25 | 1979-07-02 | Mallory & Co Inc P R | Solid cell and method of producing same |
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