JPH0534787B2 - - Google Patents
Info
- Publication number
- JPH0534787B2 JPH0534787B2 JP58158340A JP15834083A JPH0534787B2 JP H0534787 B2 JPH0534787 B2 JP H0534787B2 JP 58158340 A JP58158340 A JP 58158340A JP 15834083 A JP15834083 A JP 15834083A JP H0534787 B2 JPH0534787 B2 JP H0534787B2
- Authority
- JP
- Japan
- Prior art keywords
- negative electrode
- alkali metal
- battery
- metal ions
- lithium
- 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.)
- Expired - Lifetime
Links
- 239000007773 negative electrode material Substances 0.000 claims description 11
- 229910001413 alkali metal ion Inorganic materials 0.000 claims description 8
- 238000004519 manufacturing process Methods 0.000 claims description 7
- 239000011255 nonaqueous electrolyte Substances 0.000 claims description 7
- 239000003792 electrolyte Substances 0.000 claims description 5
- 239000000463 material Substances 0.000 claims description 3
- 238000000034 method Methods 0.000 claims description 2
- 238000007789 sealing Methods 0.000 claims 1
- 238000007599 discharging Methods 0.000 description 11
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 10
- 229910052744 lithium Inorganic materials 0.000 description 10
- 229910052751 metal Inorganic materials 0.000 description 9
- 239000002184 metal Substances 0.000 description 9
- 229910000925 Cd alloy Inorganic materials 0.000 description 6
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 6
- 239000000956 alloy Substances 0.000 description 6
- 229910045601 alloy Inorganic materials 0.000 description 6
- 229910052783 alkali metal Inorganic materials 0.000 description 5
- 150000001340 alkali metals Chemical class 0.000 description 5
- 210000004027 cell Anatomy 0.000 description 4
- 239000011521 glass Substances 0.000 description 4
- 229910052793 cadmium Inorganic materials 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 2
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 238000005275 alloying Methods 0.000 description 2
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000007872 degassing Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- -1 lithium Chemical class 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- 229910001416 lithium ion Inorganic materials 0.000 description 2
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 2
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 230000001186 cumulative effect Effects 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 230000002250 progressing effect Effects 0.000 description 1
- 238000005096 rolling process Methods 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Landscapes
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Description
【発明の詳細な説明】
産業上の利用分野
本発明は、負極を改良した非水電解質二次電池
の製造法に関する。DETAILED DESCRIPTION OF THE INVENTION Field of Industrial Application The present invention relates to a method for manufacturing a non-aqueous electrolyte secondary battery with an improved negative electrode.
従来例の構成とその問題点
現在まで、リチウム、ナトリウム等のアルカリ
金属を負極活物質材料として用い、γ−ブチロラ
クトン、テトラヒドロフラン、プロピレンカーボ
ネート、ジメトキシエタン等の溶媒中に、溶質と
して過塩素酸リチウム、ホウ弗化リチウム、塩化
リチウム等を溶解した、いわゆる非水電解質二次
電池の開発が進められてきた。Structure of conventional examples and their problems Until now, alkali metals such as lithium and sodium have been used as negative electrode active materials, and lithium perchlorate has been used as a solute in solvents such as γ-butyrolactone, tetrahydrofuran, propylene carbonate, dimethoxyethane, etc. Development of so-called non-aqueous electrolyte secondary batteries in which lithium borofluoride, lithium chloride, etc. are dissolved has been progressing.
しかし、この種の二次電池は、まだ実用化され
ていない。その理由は、充放電回数の寿命が短
く、また、充放電に際しての充放電効率が低いた
めである。 However, this type of secondary battery has not yet been put into practical use. The reason for this is that the life span of the number of times of charging and discharging is short, and the charging and discharging efficiency during charging and discharging is low.
このような欠点を改良するために、リチウム等
のアルカリ金属との合金を負極に用いることが従
来から提案されてきた。たとえば、アルミニウム
との合金化、銀（特開昭56−73860）、又は水銀
（特開昭57−98978）、鉛（特開昭57−141869）と
の合金化が知られ、またウツド合金等の可融合金
との合金化も提案されている。 In order to improve these drawbacks, it has been proposed to use an alloy with an alkali metal such as lithium for the negative electrode. For example, alloying with aluminum, silver (Japanese Unexamined Patent Publication No. 56-73860), mercury (Unexamined Japanese Unexamined Patent Application No. 57-98978), and lead (Unexamined Japanese Unexamined Patent Publication No. 57-141869) is known, and wood alloys etc. Alloying with fusible metals has also been proposed.
ところが、これらの金属又は合金を負極材料と
して用いる場合、すでにリチウム等のアルカリ金
属を吸蔵させていると、これらの負極材料は柔軟
性を失つているために、電池を製造する際に割れ
が発生し、電池の性能低下の原因となつている。 However, when these metals or alloys are used as negative electrode materials, if they have already occluded alkali metals such as lithium, these negative electrode materials lose their flexibility, which can lead to cracking during battery manufacturing. This causes a decline in battery performance.
したがつて、前記負極材料は、板状のアルカリ
金属と圧着一体化され、正極、セパレータと共に
電槽内に組み込み、電解質を注液し、アルカリ金
属を電気化学的に前記負極材料に吸蔵させる必要
があつた。 Therefore, it is necessary for the negative electrode material to be integrated with a plate-shaped alkali metal by pressure bonding, to be incorporated into a battery case together with the positive electrode and the separator, and to inject electrolyte to electrochemically occlude the alkali metal in the negative electrode material. It was hot.
しかし、注液後ただちに電槽を封口すると、前
記負極材料を溶融及び圧延したときに取り込まれ
るガスが、充放電を繰り返すうちに負極材料より
遊離し電槽内に蓄積するため、電池がふくらみ、
はなはなだしい場合には電池が破裂するという危
険があつた。 However, if the battery case is sealed immediately after injection, the gas introduced when the negative electrode material is melted and rolled is released from the negative electrode material during repeated charging and discharging and accumulates in the battery case, causing the battery to swell.
There was a risk that the battery could explode if the battery was too slow.
このような問題点を解決するため、前記負極材
料を真空下で溶融して脱気するということが提案
されているが、製造工程としては繁雑であり、圧
延する際に取り込まれるガスを除去することは困
難であつた。 In order to solve these problems, it has been proposed to melt the negative electrode material under vacuum and degas it, but this is a complicated manufacturing process, and it is difficult to remove the gas that is taken in during rolling. That was difficult.
発明の目的
本発明は、このような従来の欠点を除去するも
のであり、高エネルギー密度で、充放電の繰り返
しにおいてもガス発生のない信頼性の高い非水電
解質二次電池を提供することを目的とする。Purpose of the Invention The present invention aims to eliminate such conventional drawbacks, and provides a highly reliable non-aqueous electrolyte secondary battery that has high energy density and does not generate gas even after repeated charging and discharging. purpose.
発明の構成
本発明の非水電解質二次電池は、充電時にアル
カリ金属イオンを吸蔵し、放電時にアルカリ金属
イオンを放出する材料を用いた負極を構成要素と
するものであり、前記負極材料を電気化学的にア
ルカリ金属イオンを吸蔵した状態で脱気する工程
を有し、しかるのちに封口することを特徴とする
ものである。本発明によれば、充放電の繰り返し
においても負極からのガス発生がなく、電池形状
を保持し、また製造工程においても作業性が優れ
たものとなる。Structure of the Invention The non-aqueous electrolyte secondary battery of the present invention has a negative electrode made of a material that occludes alkali metal ions during charging and releases alkali metal ions during discharge, and the negative electrode material is electrically connected to the negative electrode. It is characterized in that it has a step of degassing in a state in which alkali metal ions are chemically occluded, and is then sealed. According to the present invention, no gas is generated from the negative electrode even during repeated charging and discharging, the battery shape is maintained, and workability is excellent in the manufacturing process.
実施例の説明 以下本発明の実施例について説明する。Description of examples Examples of the present invention will be described below.
充放電時におけるアルカリ金属イオンの吸蔵・
放出材料として、鉛（85重量％）・カドミウム
（15重量％）合金を用いた。 Absorption and absorption of alkali metal ions during charging and discharging
A lead (85% by weight)/cadmium (15% by weight) alloy was used as the release material.
上記組成の鉛・カドミウム合金をローラーによ
つて圧延し、厚さ0.2mmにしたあと、大きさ１cm
×２cmの寸法に切り出した。この圧延板を、大き
さ2.5cm×２cmに切り取つたニツケルエキスパン
ドメタルではさみ、加圧圧着したあと、鉛・カド
ミウム圧延板のついていない集電体にニツケルリ
ボンをスポツト溶接した。 A lead-cadmium alloy with the above composition is rolled with a roller to a thickness of 0.2 mm, and then rolled into a size of 1 cm.
It was cut out to a size of 2 cm. This rolled plate was sandwiched between nickel expanded metal pieces cut to a size of 2.5 cm x 2 cm, and the pieces were crimped together under pressure, and then a nickel ribbon was spot welded to the current collector to which the lead/cadmium rolled plate was not attached.
次にこの電極を、ニツケルエキスパンドメタル
に圧着した金属リチウム対極、及び、対極と同じ
構成の金属リチウム照合電極と共にガラスセルに
組み入れ、ゴム栓をした。 Next, this electrode was assembled into a glass cell together with a metallic lithium counter electrode crimped onto nickel expanded metal and a metallic lithium reference electrode having the same structure as the counter electrode, and a rubber stopper was attached.
電解液には、プロピレンカーボネートに１モ
ル／の割合で過塩素酸リチウムを溶解したもの
を用い、また、金属リチウム対極に発生するデン
ドライトによる内部短絡を防ぐため、セパレータ
にポリプロピレンの不織布を用い、鉛・カドミウ
ム合金極と金属リチウム対極との間隔を充分にあ
けた。 The electrolyte was prepared by dissolving lithium perchlorate in propylene carbonate at a ratio of 1 mol/mole, and in order to prevent internal short circuits caused by dendrites that occur at the metal lithium counter electrode, a polypropylene nonwoven fabric was used as the separator, and lead・Enough space was left between the cadmium alloy electrode and the metal lithium counter electrode.
このように構成した電池の鉛・カドミウム合金
と金属リチウム対極とを外部短絡させ、電気化学
的にリチウムイオンを合金極へ吸蔵させた。１日
後、外部短絡を中止し、ゴム栓をはずしたあと極
板を電解液中に沈めたまま脱気した。脱気のの
ち、この電池をガラスセルごと電解液を満たした
容器内で倒立させ、ガラスセル内部の気体を抜い
た。この電池をＡとする。 The lead-cadmium alloy of the battery constructed in this manner and the metallic lithium counter electrode were externally shorted, and lithium ions were electrochemically occluded into the alloy electrode. One day later, the external short circuit was discontinued, the rubber stopper was removed, and the electrode plate was degassed while submerged in the electrolyte. After degassing, the battery was inverted along with the glass cell in a container filled with electrolyte to remove the gas inside the glass cell. This battery is called A.
こののち、鉛・カドミウム合金極に対してリチ
ウムイオンの吸蔵・放出の繰り返しを２ｍＡの定
電流、金属リチウム照合極に対し0.05〜0.8Vの電
位の範囲で行い、発生するガスを捕集し体積を測
定した。この様子を第１図に示す。 After this, lithium ions are repeatedly inserted and released into the lead-cadmium alloy electrode at a constant current of 2 mA and a potential range of 0.05 to 0.8 V relative to the metal lithium reference electrode, and the gas generated is collected and the volume is was measured. This situation is shown in FIG.
比較のため、外部短絡させて脱気しない以外は
上記と同様の方法で作成した電池をＢとし、発生
するガス量を同様に測定した。 For comparison, a battery B was prepared in the same manner as above except that it was not degassed by external short-circuiting, and the amount of gas generated was measured in the same manner.
上記電池Ａ，Ｂの充放電の各サイクルにおいて
発生するガスの累積量の変化の様子を第２図に示
す。 FIG. 2 shows changes in the cumulative amount of gas generated during each cycle of charging and discharging the batteries A and B.
第２図より明らかなように、比較例の電池Ｂで
は、充放電に伴つてガス発生量が著しく多いのに
くらべ、本発明の電池Ａではガス発生がほとんど
見られないことがわかる。 As is clear from FIG. 2, in comparison with the battery B of the comparative example, which generated a significantly large amount of gas during charging and discharging, in the battery A of the present invention, almost no gas generation was observed.
なお、実施例では鉛・カドミウム合金を用いた
が、上記組成の鉛・カドミウム合金に限らず、
Sn、Bi、Pb、Cd、In、Hg、Sb、Zn、Agの中か
ら選ばれた１つの金属、あるいは２つ以上の金属
の組み合わせからなる合金を用いてもよい。 In addition, although a lead-cadmium alloy was used in the examples, it is not limited to lead-cadmium alloys having the above composition.
One metal selected from Sn, Bi, Pb, Cd, In, Hg, Sb, Zn, and Ag, or an alloy consisting of a combination of two or more metals may be used.
発明の効果
以上のように、本発明によれば、充放電を繰り
返した場合でも、ガス発生による電池のふくらみ
がなく形状を保持し、しかも製造工程においても
繁雑性がない。Effects of the Invention As described above, according to the present invention, even when charging and discharging are repeated, the battery does not bulge due to gas generation and retains its shape, and there is no complexity in the manufacturing process.
第１図は実施例に用いたガラスセルの構成を示
す図、第２図は本発明の実施例及び比較例の非水
電解質二次電池の充放電時のガス発生量を示す図
である。
FIG. 1 is a diagram showing the structure of the glass cell used in the example, and FIG. 2 is a diagram showing the amount of gas generated during charging and discharging of the nonaqueous electrolyte secondary batteries of the example and comparative example of the present invention.
Claims (1)
と、充電時にアルカリ金属イオンを吸蔵し、放電
時にアルカリ金属イオンを放出する材料を用いた
負極を構成要素とする非水電解質二次電池の製造
法であつて、前記負極材料を電気化学的にアルカ
リ金属イオンを吸蔵した状態で脱気する工程を有
し、その後に封口することを特徴とする非水電解
質二次電池の製造法。1. A method for producing a non-aqueous electrolyte secondary battery, the components of which are a positive electrode, an electrolyte conductive to alkali metal ions, and a negative electrode made of a material that stores alkali metal ions during charging and releases alkali metal ions during discharge. A method for manufacturing a non-aqueous electrolyte secondary battery, comprising the step of deaerating the negative electrode material in a state in which alkali metal ions are electrochemically occluded, and then sealing the negative electrode material.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP58158340A JPS6049576A (en) | 1983-08-29 | 1983-08-29 | Manufacture of nonaqueous secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP58158340A JPS6049576A (en) | 1983-08-29 | 1983-08-29 | Manufacture of nonaqueous secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS6049576A JPS6049576A (en) | 1985-03-18 |
| JPH0534787B2 true JPH0534787B2 (en) | 1993-05-24 |
Family
ID=15669495
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP58158340A Granted JPS6049576A (en) | 1983-08-29 | 1983-08-29 | Manufacture of nonaqueous secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS6049576A (en) |
-
1983
- 1983-08-29 JP JP58158340A patent/JPS6049576A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS6049576A (en) | 1985-03-18 |
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