JPH0526303B2 - - Google Patents
Info
- Publication number
- JPH0526303B2 JPH0526303B2 JP62251566A JP25156687A JPH0526303B2 JP H0526303 B2 JPH0526303 B2 JP H0526303B2 JP 62251566 A JP62251566 A JP 62251566A JP 25156687 A JP25156687 A JP 25156687A JP H0526303 B2 JPH0526303 B2 JP H0526303B2
- Authority
- JP
- Japan
- Prior art keywords
- bromine
- membrane
- electrical resistance
- separator
- paper
- 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 - Fee Related
Links
- 239000003365 glass fiber Substances 0.000 claims description 18
- 239000000835 fiber Substances 0.000 claims description 14
- -1 Polyethylene Polymers 0.000 claims description 13
- 239000004698 Polyethylene Substances 0.000 claims description 13
- 229920000573 polyethylene Polymers 0.000 claims description 13
- 229910052736 halogen Inorganic materials 0.000 claims description 6
- 150000002367 halogens Chemical class 0.000 claims description 6
- 239000002184 metal Substances 0.000 claims description 6
- 229910052751 metal Inorganic materials 0.000 claims description 6
- 239000012982 microporous membrane Substances 0.000 claims description 6
- 239000002657 fibrous material Substances 0.000 claims description 2
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 description 32
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 description 32
- 229910052794 bromium Inorganic materials 0.000 description 32
- 239000012528 membrane Substances 0.000 description 26
- 230000004888 barrier function Effects 0.000 description 24
- VNDYJBBGRKZCSX-UHFFFAOYSA-L zinc bromide Chemical compound Br[Zn]Br VNDYJBBGRKZCSX-UHFFFAOYSA-L 0.000 description 8
- 230000007423 decrease Effects 0.000 description 5
- 239000007864 aqueous solution Substances 0.000 description 4
- 229940102001 zinc bromide Drugs 0.000 description 4
- 230000000694 effects Effects 0.000 description 3
- 239000003792 electrolyte Substances 0.000 description 3
- ZRXYMHTYEQQBLN-UHFFFAOYSA-N [Br].[Zn] Chemical compound [Br].[Zn] ZRXYMHTYEQQBLN-UHFFFAOYSA-N 0.000 description 2
- 230000018044 dehydration Effects 0.000 description 2
- 238000006297 dehydration reaction Methods 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- 230000008094 contradictory effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000012212 insulator Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 229920013716 polyethylene resin Polymers 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Composite Materials (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Cell Separators (AREA)
Description
Ａ 産業上の利用分野
この発明は、金属ハロゲン電池において正極電
解液と負極電解液を隔離するために使用するセパ
レータに関するものである。
Ｂ 発明の概要
この発明は、ポリエチレン繊維とガラス繊維を
用いて、抄紙状微細多孔質膜をすることことによ
つて、膜の電気抵抗が低く、且つ、臭素バリアー
性の高い金属ハロゲン電池用セパレータを提供す
るものである。
Ｃ 従来の技術
金属ハロゲン電池の一例として、例えば、亜鉛
臭素電池においては、充電時に正極において臭素
が発生し、この臭素が負極に析出した亜鉛と反応
すると自己放電を引き起こすため、正極電解液と
負極電解液を隔離する臭素バリアー性の高いセパ
レータが必要不可欠である。
また、このセパレータは臭素バリアー性に優れ
るとともに、セパレータ自体の電気抵抗が低いこ
とが望まれるものである。
従来、このような亜鉛臭素電池のセパレータと
しては、各種の微細多孔質膜から適宜選択して用
いられているが、これらの微細多孔質膜は、素材
となる樹脂粉体に、各種無機微粉体および有機液
状体を加えて、混合、成形し、しかる後に空孔形
成成分である有機液状体を抽出することによつて
作られている。
Ｄ 発明が解決しようとする問題点
上記のような従来のセパレータにおいては、例
えば、絶縁物である素材樹脂の相対的な割合を低
下させると膜の電気抵抗は減少するが、臭素バリ
アー性は低下してしまうというように膜の電気抵
抗と臭素バリアー性とは相反する性質のものであ
つた。
すなわち、従来のセパレータにおいては、膜の
電気抵抗と臭素バリアー性は、膜の電気抵抗が比
較的低ければ臭素バリアー性が劣り、逆に臭素バ
リアー性に優れていれば膜の電気抵抗が高くなる
というように、反比例的な相関があり、求められ
る２つの特性の両立が困難であるという問題点が
あつた。
この発明は、係る問題点を解決し、電気抵抗が
低く、且つ、臭素バリアー性に優れた金属ハロゲ
ン電池用セパレータを提供することを目的とする
ものである。
Ｅ 問題点を解決するための手段
この発明においては、ポリエチレン繊維素材
に、直径が５〜0.5μmのガラス繊維を20〜50wt％
の含有量で分散させて実質的にポリエチレン繊維
とガラス繊維とのみからなる抄紙状微細多孔質膜
とすることにより、臭素バリアー性を低下させる
ことなく、膜の電気抵抗を引き下げて、上記の問
題を解決したものである。
Ｆ 作用
この発明において、ガラス繊維は、その添加に
より、膜の電気抵抗を引下げるとともに、素材で
あるポリエチレン繊維の間隙を充たして、適当な
微細孔を形成することにより、臭素バリアー性を
高める点においても有利に働くものである。
また、このガラス繊維は添加量が同じであれ
ば、その直径が小さいほうがより膜が緻密にな
り、臭素バリアー性がさらに向上する。
Ｇ 実施例
以下、実施例によつてこの考案をより詳細に説
明する。
実施例 １
直径約10〜15μm、長さ約１mmのポリエチレン
繊維と直径約10μmのガラス繊維を用いて、ポリ
エチレン繊維とガラス繊維の重量比を変化させ、
５種類の抄紙状微細多孔質膜（Ａ〜Ｅ）を作製し
た。
この内、膜Ａは、ポリエチレン繊維のみからな
る比較サンプルである。
また、抄紙状とする方法は、各繊維を所定の割
合に混合したものを、水に分散させ、この分散液
を抄紙機に入れて、紙層、脱水、乾燥の工程を経
て抄紙とするというものであるが、各繊維の結合
を強固なものにする上で、脱水後、抄紙を加熱加
圧することが望ましい。
この実施例においては、成形する際に、120℃
に昇温した２本ロールに通してヒートプレスする
ことによつて、ポリエチレン樹脂の密着を向上さ
せた。
以上のようにして作製した膜サンプルＡ〜Ｅに
ついて、膜の電気抵抗の測定と臭素バリアー性試
験を行つた。
膜の電気抵抗の測定はJIS Ｃ−2313に従つて行
い、その結果は、第１表および第１図に示される
ようであつた。
第１図から明らかなように、ポリエチレン繊維
のみからなる膜Ａに比べて、ガラス繊維を添加し
た膜（Ｂ〜Ｅ）は、いずれも膜の電気抵抗が著し
く低下している。
ここで、ガラス繊維の添加量が多い程、膜の電
気抵抗は低くなつているが、添加量が一定量に達
すると、それ以上添加量を増しても、膜の電気抵
抗の低下が少なくなるのは、膜がある程度の緻密
さに達するとそれ以上は膜の電気抵抗が低下しに
くくなるためと考えられる。
また、臭素バリアー性試験については、第４図
に示されるようなＵ字管２を用いて行い、微細多
孔質膜１を介して一方には3mol／ｌ臭化亜鉛水
溶液、他方に3mol／ｌ臭化亜鉛水溶液と
0.3mol／ｌ臭素の混合液を入れ、４時間後の臭
素透過量を測定した。
第１表及び第２図は臭素バリアー性試験の結果
を示すものであるが、ポリエチレン繊維のみから
なる膜Ａに比較して、ガラス繊維を添加した膜Ｂ
〜Ｅはいずれも臭素の透過量が大きく減少してお
り、ガラス繊維の添加量の多いもの程、臭素バリ
アー性の向上が著しい。
以上の結果は、ポリエチレン繊維にガラス繊維
を添加して、抄紙状の微細多孔質膜とすることが
膜の電気抵抗を低下させる上でも、臭素バリアー
性を向上させる上でも、非常に有効であることを
示している。
A. Industrial Application Field This invention relates to a separator used to separate a positive electrode electrolyte and a negative electrode electrolyte in a metal halogen battery. B. Summary of the Invention This invention provides a separator for metal halogen batteries that has low electrical resistance and high bromine barrier properties by forming a paper-like microporous membrane using polyethylene fibers and glass fibers. It provides: C. Prior Art As an example of a metal halogen battery, for example, in a zinc-bromine battery, bromine is generated at the positive electrode during charging, and when this bromine reacts with zinc deposited on the negative electrode, it causes self-discharge. A separator with high bromine barrier properties is essential to isolate the electrolyte. Further, it is desired that this separator has excellent bromine barrier properties and that the separator itself has low electrical resistance. Conventionally, separators for such zinc-bromine batteries have been used by appropriately selecting from various microporous membranes. and an organic liquid, mixed and shaped, and then the organic liquid, which is a pore-forming component, is extracted. D Problems to be Solved by the Invention In the conventional separators as described above, for example, if the relative proportion of the resin material, which is an insulator, is reduced, the electrical resistance of the film decreases, but the bromine barrier property decreases. The electrical resistance and bromine barrier properties of the membrane were contradictory in nature. In other words, in conventional separators, the electrical resistance and bromine barrier properties of the film are such that if the electrical resistance of the film is relatively low, the bromine barrier property is poor, and conversely, if the film has excellent bromine barrier property, the electrical resistance of the film is high. Thus, there was a problem that there was an inversely proportional correlation and it was difficult to achieve both of the required characteristics. The object of the present invention is to solve these problems and provide a separator for metal halogen batteries that has low electrical resistance and excellent bromine barrier properties. E Means for solving the problem In this invention, 20 to 50 wt% of glass fibers with a diameter of 5 to 0.5 μm are added to the polyethylene fiber material.
By dispersing the bromine fibers in a paper-like microporous membrane consisting essentially only of polyethylene fibers and glass fibers, the electrical resistance of the membrane can be lowered without reducing the bromine barrier properties, and the above problems can be solved. This is the solution. F Effect In this invention, the addition of glass fiber lowers the electrical resistance of the membrane, and also fills the gaps between the polyethylene fibers that are the raw material and forms appropriate micropores, thereby improving the bromine barrier properties. It also works advantageously. Furthermore, if the amount of glass fibers added is the same, the smaller the diameter, the denser the film, and the further improved the bromine barrier properties. G. Examples Hereinafter, this invention will be explained in more detail using examples. Example 1 Using polyethylene fibers with a diameter of about 10 to 15 μm and a length of about 1 mm and glass fibers with a diameter of about 10 μm, the weight ratio of the polyethylene fibers and glass fibers was changed,
Five types of paper-like microporous membranes (A to E) were produced. Among these, membrane A is a comparison sample consisting only of polyethylene fibers. In addition, the method of making paper is to mix each fiber in a predetermined ratio and disperse it in water, put this dispersion into a paper machine, and make paper through the steps of paper layering, dehydration, and drying. However, in order to strengthen the bonds between each fiber, it is desirable to heat and press the paper after dehydration. In this example, the temperature was 120°C during molding.
The adhesion of the polyethylene resin was improved by heat pressing it through two rolls heated to . Membrane samples A to E produced as described above were subjected to measurement of electrical resistance of the membrane and a bromine barrier property test. The electrical resistance of the film was measured according to JIS C-2313, and the results were as shown in Table 1 and FIG. As is clear from FIG. 1, the electrical resistance of the membranes to which glass fibers have been added (B to E) is significantly lower than that of membrane A consisting only of polyethylene fibers. Here, the electrical resistance of the membrane decreases as the amount of glass fiber added increases, but once the amount added reaches a certain level, even if the amount added is further increased, the decrease in the electrical resistance of the membrane becomes smaller. This is thought to be because once the film reaches a certain degree of density, the electrical resistance of the film becomes difficult to decrease beyond that point. In addition, the bromine barrier property test was conducted using a U-shaped tube 2 as shown in Figure 4, and a 3 mol/l zinc bromide aqueous solution was passed through the microporous membrane 1 to one side and 3 mol/l to the other. zinc bromide aqueous solution and
A mixed solution of 0.3 mol/l bromine was added, and the amount of bromine permeated after 4 hours was measured. Table 1 and Figure 2 show the results of the bromine barrier property test. Compared to membrane A consisting only of polyethylene fibers, membrane B containing glass fibers
- E, the amount of bromine permeation is greatly reduced, and the greater the amount of glass fiber added, the more remarkable the improvement in bromine barrier properties is. The above results demonstrate that adding glass fiber to polyethylene fibers to create paper-like microporous membranes is very effective in lowering the membrane's electrical resistance and improving its bromine barrier properties. It is shown that.
【表】
実施例 ２
実施例１で最も好ましい結果を得た膜サンプル
Ｅと同じ組成比で、ガラス繊維の直径を変化させ
て、抄紙状微細多孔質膜（Ｅ−１，Ｅ−２，Ｅ−
３，Ｅ−４）を作製し、実施例１と同様に膜の電
気抵抗を測定し、臭素バリアー性試験を行つた。
膜の電気抵抗については、第２表に示されるる
ように、ガラス繊維の直径によつて大差はなく、
いずれも0.0002Ω−cm2／枚前後であつた。
しかし、従来この種のセパレータとして用いら
れている微細多孔質膜の膜抵抗は、例えばポリオ
レフイン系のもので約0.005Ω−cm2／枚程度であ
るから、この発明に係るセパレータの電気抵抗は
従来のものの約20分の１以下と、極めて低いもの
である。
また、臭素バリアー性については、第２表およ
び第３図に示されるように、Ｅ−１＞Ｅ−２＞Ｅ
−３＞Ｅ−４とガラス繊維の直径が順に小さくな
る程、臭素透過量が少なく、臭素バリアー性が向
上していることが明確である。
これは、ガラス繊維の直径が小さくなることに
より、より膜の緻密化が図られているためと考え
られる。[Table] Example 2 Paper-like microporous membranes (E-1, E-2, E −
3, E-4) was prepared, and the electrical resistance of the film was measured in the same manner as in Example 1, and a bromine barrier property test was conducted. As shown in Table 2, the electrical resistance of the membrane does not vary greatly depending on the diameter of the glass fiber.
In all cases, the resistance was around 0.0002Ω-cm 2 /piece. However, since the membrane resistance of microporous membranes conventionally used as this type of separator, such as polyolefin-based membranes, is about 0.005Ω-cm 2 /sheet, the electrical resistance of the separator according to the present invention is lower than that of the conventional separator. This is extremely low, at less than one-twentieth of the average. Regarding the bromine barrier property, as shown in Table 2 and Figure 3, E-1>E-2>E
It is clear that the smaller the diameter of the glass fiber (-3>E-4), the smaller the amount of bromine permeation and the better the bromine barrier properties. This is thought to be because the membrane becomes more dense as the diameter of the glass fibers becomes smaller.
【表】
Ｈ 発明の効果
この発明は、以上説明したとおり、ポリエチレ
ン系繊維を素材として、ガラス繊維を分散させ
て、抄紙状微細多孔質膜をすることにより、膜の
臭素バリアー性を向上させつつ、且つ、膜の電気
抵抗も著しく低下させるという効果を有するもの
である。
係る特性を兼ね備えたセパレータは、金属ハロ
ゲン電池のセパレータとして、極めて優れたもの
である。[Table] H Effects of the Invention As explained above, this invention improves the bromine barrier properties of the membrane by forming a paper-like microporous membrane using polyethylene fibers as a material and dispersing glass fibers. , and has the effect of significantly lowering the electrical resistance of the film. A separator having such characteristics is extremely excellent as a separator for metal halogen batteries.
第１図は実施例における膜の電気抵抗を示すグ
ラフ、第２図は第１図と同じ実施例おける膜の臭
素バリアー性試験の結果を示すグラフ、第３図は
別の実施例における膜の臭素バリアー性試験の結
果を示すグラフ、第４図は臭素バリアー性試験に
用いた装置の模式図である。
１……微細多孔質膜、２……Ｕ字管、３……
3mol／ｌ臭化亜鉛水溶液、４……3mol／ｌ臭化
亜鉛水溶液と0.3mol／ｌ臭素の混合液。
Figure 1 is a graph showing the electrical resistance of the membrane in the example, Figure 2 is a graph showing the results of the bromine barrier test of the membrane in the same example as Figure 1, and Figure 3 is the graph of the membrane in another example. A graph showing the results of the bromine barrier property test, and FIG. 4 is a schematic diagram of the apparatus used in the bromine barrier property test. 1... Microporous membrane, 2... U-shaped tube, 3...
3 mol/l zinc bromide aqueous solution, 4... A mixed solution of 3 mol/l zinc bromide aqueous solution and 0.3 mol/l bromine.
Claims (1)
のガラス繊維を20〜50wt％の含有量で分散させ
て実質的にポリエチレン繊維とガラス繊維とのみ
からなる抄紙状微細多孔質膜としたことを特徴と
する金属ハロゲン電池用セパレータ。1 Polyethylene fiber material with a diameter of 5 to 0.5 μm
1. A separator for a metal halogen battery, characterized in that a paper-like microporous membrane consisting essentially of polyethylene fibers and glass fibers is obtained by dispersing glass fibers in a content of 20 to 50 wt%.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62251566A JPH0195466A (en) | 1987-10-07 | 1987-10-07 | Separator for metal halide battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62251566A JPH0195466A (en) | 1987-10-07 | 1987-10-07 | Separator for metal halide battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0195466A JPH0195466A (en) | 1989-04-13 |
| JPH0526303B2 true JPH0526303B2 (en) | 1993-04-15 |
Family
ID=17224721
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62251566A Granted JPH0195466A (en) | 1987-10-07 | 1987-10-07 | Separator for metal halide battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0195466A (en) |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5549868A (en) * | 1978-10-02 | 1980-04-10 | Asahi Chem Ind Co Ltd | Metal-halogen thin type battery |
| JPS58155651A (en) * | 1982-02-02 | 1983-09-16 | エムハート インダストリーズ インコーポレーテッド | Separator for battery |
-
1987
- 1987-10-07 JP JP62251566A patent/JPH0195466A/en active Granted
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5549868A (en) * | 1978-10-02 | 1980-04-10 | Asahi Chem Ind Co Ltd | Metal-halogen thin type battery |
| JPS58155651A (en) * | 1982-02-02 | 1983-09-16 | エムハート インダストリーズ インコーポレーテッド | Separator for battery |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0195466A (en) | 1989-04-13 |
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