JPH0421987B2 - - Google Patents
Info
- Publication number
- JPH0421987B2 JPH0421987B2 JP59164751A JP16475184A JPH0421987B2 JP H0421987 B2 JPH0421987 B2 JP H0421987B2 JP 59164751 A JP59164751 A JP 59164751A JP 16475184 A JP16475184 A JP 16475184A JP H0421987 B2 JPH0421987 B2 JP H0421987B2
- Authority
- JP
- Japan
- Prior art keywords
- electrode
- electrodes
- carbon
- porosity
- porous
- 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
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Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/96—Carbon-based electrodes
-
- 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
- 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
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Inert Electrodes (AREA)
- Hybrid Cells (AREA)
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は、亜鉛−臭素電池に使用される電極に
係り、特に経済性、電池効率、耐用寿命の面です
ぐれた性能を有する多孔性カーボンプラスチツク
電極の製造方法に関するものである。Detailed Description of the Invention [Field of Industrial Application] The present invention relates to an electrode used in a zinc-bromine battery, and in particular to a porous carbon electrode that has excellent performance in terms of economy, battery efficiency, and service life. This invention relates to a method for manufacturing plastic electrodes.
従来、亜鉛−臭素電池に使用されていた電極
は、貴金属（例えば白金）を用いた金属電極、ま
たはプラスチツク導電性を有する物質（例えばカ
ーボン）を混合し、これを混練・成形してなるプ
ラスチツク電極、もしくは炭素自体を利用した炭
素電極等であり、それぞれ次の問題があつた。
Conventionally, the electrodes used in zinc-bromine batteries are metal electrodes using noble metals (e.g. platinum), or plastic electrodes made by mixing conductive substances (e.g. carbon) and kneading and molding the mixture. or carbon electrodes using carbon itself, each of which had the following problems.
先づ、金属電極は、電池充電時に電極に発生す
る臭素による腐食を考慮すると貴金属に限定され
ることになる。貴金属は抵抗が非常に小さく、電
池の電圧効率も良好である。又放電時の放電時間
も長く、クーロン効率もすぐれている。しかしな
がら、貴金属であることから高価で、コストが高
く実用的でない。 First, metal electrodes are limited to noble metals, considering the corrosion caused by bromine that occurs in the electrodes during battery charging. Noble metals have very low resistance, and the voltage efficiency of batteries is also good. Furthermore, the discharge time during discharge is long and the coulombic efficiency is excellent. However, since it is a precious metal, it is expensive, and the cost is high, making it impractical.
次に、炭素電極は、前出の金属電極に続いて抵
抗値は低いが、機械的強度が低く、特に衝撃によ
るクラツク発生などその信頼性に問題があつた。
さらに一般的に炭素電極は多孔性のため電極に隔
離板としての機能を持たせるバイポラ型直列積層
電池システムには不適であつた。また、プラスチ
ツク電極は、耐用寿命の点では満足できるもの
の、抵抗値が高く、クーロン効率においても電極
表面の抵抗も当然高いので、活性物の電極反応抵
抗が大となる。そのため低い電池効率しか得られ
ないという問題があつた。 Next, although carbon electrodes have a low resistance value like the metal electrodes mentioned above, they have low mechanical strength and have problems with reliability, especially cracks caused by impact.
Furthermore, carbon electrodes are generally porous and therefore unsuitable for bipolar series stacked battery systems in which the electrodes function as separators. Furthermore, although plastic electrodes are satisfactory in terms of service life, they have a high resistance value, and naturally the resistance of the electrode surface is also high in terms of Coulombic efficiency, so the electrode reaction resistance of active substances becomes large. Therefore, there was a problem that only low battery efficiency could be obtained.
そこで、本発明は、亜鉛−臭素電池に従来用い
られていた電極がそれぞれ上述の通り経済性、耐
用寿命、電池効率の点において改善すべき問題を
有することに鑑み、これらの点を改善するために
なされたものである。
Therefore, in view of the fact that the electrodes conventionally used in zinc-bromine batteries have problems that should be improved in terms of economic efficiency, service life, and battery efficiency, the present invention aims to improve these points. This is what was done.
本発明においては、上記の問題点を解決するた
めに、電極表面の活物質としてのBr2との反応活
性面積を増加させ、電極電位特性のすぐれた臭素
極に最適な多孔性カーボンプラスチツク電極を製
造する方法を開発したものであり、具体的にはカ
ーボンプラスチツク部材の表面に導電性粉末及び
多孔化剤を含む合成樹脂層を静電塗装法で形成し
た後、多孔化処理を施すことを特徴とする方法で
ある。
In order to solve the above-mentioned problems, the present invention increases the active area for reaction with Br 2 as an active material on the electrode surface, and creates a porous carbon plastic electrode that is ideal for a bromine electrode and has excellent electrode potential characteristics. A manufacturing method has been developed, specifically, a synthetic resin layer containing conductive powder and a pore-forming agent is formed on the surface of a carbon plastic member using an electrostatic coating method, and then a porosity treatment is performed. This is the method to do so.
さらに一つの本発明は、カーボンプラスチツク
部材の表面に導電性粉末、多孔化処理剤、及びイ
オン交換繊維を含む合成樹脂層を静電塗装法で形
成した後、多孔化処理を施すことを特徴とする方
法である。 Another aspect of the present invention is that after forming a synthetic resin layer containing conductive powder, a pore-forming agent, and ion-exchange fibers on the surface of a carbon plastic member by electrostatic coating, a porosity-forming treatment is performed. This is the way to do it.
本発明において、導電性粉末として適用される
物質は、カーボンプラツク、活性炭、グラフアイ
ト又はPt、As等の貴金属粉、酸化アルミニウム、
酸化チタン、酸化ルチニウム等の金属酸化物であ
る。 In the present invention, substances applied as conductive powder include carbon plaque, activated carbon, graphite, noble metal powder such as Pt and As, aluminum oxide,
Metal oxides such as titanium oxide and rutinium oxide.
本発明において、多孔化剤として適用される物
質は、水溶性のポリビニルアルコール、KCl、
NaCl等である。 In the present invention, the substances applied as porosity agents include water-soluble polyvinyl alcohol, KCl,
NaCl etc.
本発明において、イオン交換繊維の添加は、特
に活物質として臭素を用いた電池のカーボンプラ
スチツク電極に有効であり、電極中にイオン交換
繊維を加えると、遊離臭素を電解液中で、しかも
電極と電解液との界面近傍に留め、電極の内部に
侵入することを阻止することができ、臭素の腐蝕
作用から電極を保護することができる。即ち、遊
離臭素は例えば、Br3 -形態で電解液中に存在し、
しかも腐蝕作用を有する。そのため陰イオン交換
繊維を電極に加えることにより、イオン交換繊維
のマイナスと臭素のマイナスが電気的に反発し、
臭素が電極内部に侵入することを防止することが
できる。 In the present invention, the addition of ion-exchange fibers is particularly effective for carbon plastic electrodes of batteries that use bromine as an active material.Adding ion-exchange fibers to the electrodes allows free bromine to be removed in the electrolyte and not only in the electrodes. It can be kept near the interface with the electrolytic solution and can be prevented from penetrating into the interior of the electrode, thereby protecting the electrode from the corrosive action of bromine. That is, free bromine is present in the electrolyte in the Br 3 -form , for example;
Moreover, it has a corrosive effect. Therefore, by adding anion exchange fiber to the electrode, the minus of the ion exchange fiber and the minus of bromine electrically repel,
Bromine can be prevented from entering inside the electrode.
しかして、上記導電性粉末、多孔化剤、活物質
トラツプ剤を上記カーボンプラスチツク部材の表
面に層着させるための合成樹脂バインダーとして
適用されるものは、バインダー効果と分散剤の効
果を併せ持つエポキシ樹脂、シリコン樹脂、フツ
ソ樹脂等であり、いずれもその溶剤により溶液と
されたものに前記の各混合物質を分散させるもの
とする。 Therefore, the synthetic resin binder used for layering the conductive powder, porosity agent, and active material trapping agent on the surface of the carbon plastic member is an epoxy resin that has both a binder effect and a dispersant effect. , silicone resin, fluorine resin, etc., each of which is made into a solution by its solvent, and the above-mentioned mixed substances are dispersed therein.
カーボンプラスチツク部材の表面への塗装方法
は、塗膜と該表面との結合力が刷毛塗り等の他の
手段に比べてすぐれており、かつカーボンプラス
チツクの持つている導電性を利用する有利さを活
かして静電塗装法により吹付け塗装をすることが
好ましい。 The method of coating the surface of carbon plastic members has the advantage of superior bonding strength between the coating film and the surface compared to other methods such as brush coating, and of utilizing the electrical conductivity of carbon plastic. It is preferable to spray paint using an electrostatic coating method.
また、多孔化処理は、上記の吹付け塗装後塗膜
層が安定してから温水処理し、前記多孔化剤を溶
出させるもので、塗膜面の凹凸のほかに多孔化剤
の溶出によつて生じたポーラス部分を有する多孔
層が形成されるものである。 In addition, in the porosity treatment, after the coating film layer is stabilized after spray painting, it is treated with hot water to elute the porosity agent. As a result, a porous layer having porous portions is formed.
本発明は、上記の構成を採用したことにより、
従来の電極にみられる物理的方法のみで得られた
表面凹凸より格別にすぐれた多孔性でかつ活物質
に対する化学的耐性においてもすぐれた電極を得
ることができた。
By adopting the above configuration, the present invention has the following features:
It was possible to obtain an electrode that has a porosity that is superior to the surface roughness obtained using only physical methods found in conventional electrodes, and is also excellent in chemical resistance to active materials.
次に、本発明の実施例を示す。 Next, examples of the present invention will be shown.
() 実施例 １
従来から用いられている密度0.96ｇ／cm2のポリ
エチレン：表面積1000m2／ｇのカーボンブラツク
比が100：50の組成の板状に成形されたカーボン
プラスチツク部材を静電塗装機の陰極に固定し、
電界をかけながら静電塗料表面積1000m2／ｇのカ
ーボンプラスチツクのケツチエンブラツクEC（ラ
イオン・アクゾ社製）、主成分がポリビニルアル
コールのソプロン（ニチビ社製）及びドータイト
のシンナー（藤倉化成社製ドータイト×C32）を
それぞれ100ｇ、50ｇ及び１の割合で混合した
溶液をスプレーガンで厚さ0.5〜1.0mmの範囲の一
様な厚さになるまで塗装した。次いで、この塗膜
層の形成されたカーボンプラスチツク部材を80〜
100℃の温水中に２時間浸漬し、塗膜層中の水溶
性成分であるポリビニルアルコールを溶出させ
た。() Example 1 A carbon plastic member formed into a plate shape with a composition of conventionally used polyethylene with a density of 0.96 g/cm 2 and a carbon black ratio of 100:50 with a surface area of 1000 m 2 /g was coated with an electrostatic coating machine. fixed on the cathode of
While applying an electric field, apply electrostatic paint to KETSUTIEN BLACK EC (manufactured by Lion Akzo Co., Ltd.) made of carbon plastic with a surface area of 1000 m 2 /g, Sopron (manufactured by Nichibi Co., Ltd.) whose main component is polyvinyl alcohol, and Dotite thinner (Dottite made by Fujikura Kasei Co., Ltd.). ×C32) were mixed in proportions of 100 g, 50 g, and 1, respectively, and the solution was coated with a spray gun to a uniform thickness in the range of 0.5 to 1.0 mm. Next, the carbon plastic member on which this coating layer was formed was heated to
It was immersed in warm water at 100°C for 2 hours to elute polyvinyl alcohol, which is a water-soluble component in the coating layer.
このようにして得られた本発明の多孔性カーボ
ンプラスチツク電極（以下ESP−CPという）と、
特願昭58−8635（昭和58年１月24日出願）に開示
してある従来の導電性フツ素シートバツキングカ
ーボンプラスチツク電極（以下FRI−CPに比べ
ても特に低Br2濃度範囲で特性が向上している。
これは既述したように従来の物理的処理にみられ
るような電極表面の凹凸化に加えて、化学的処理
で得られた多孔化のためであり、それらが電位特
性の向上に大きく貢献したものと考えられる。 The porous carbon plastic electrode of the present invention (hereinafter referred to as ESP-CP) thus obtained,
The conventional conductive fluorine sheet-backed carbon plastic electrode (hereinafter referred to as FR I -CP) disclosed in Japanese Patent Application No. 1986-8635 (filed on January 24, 1988) is particularly effective in the low Br 2 concentration range. Characteristics are improved.
As mentioned above, this is due to the unevenness of the electrode surface seen in conventional physical treatments, as well as the porosity created by chemical treatments, which greatly contributed to improving the potential characteristics. considered to be a thing.
() 実施例 ２
前記実施例１に示した温水処理による水溶性成
分（ポリビニルアルコール）の溶出による多孔化
効果を確めるために、実施例１と同一仕様・方法
でカーボンプラスチツク部材の表面に静電塗装を
行い、温水処理を施す前に一定の圧力（200Kg／
cm2）で塗装面を一様にプレスした。このようにし
て塗装面をフラツトな状態にした後この電極を２
枚に分割し、一方は実施例１と同様に温水処理を
行つて多孔化し、他方は温水処理を行わずに、そ
れぞれの放電電位特性を比較した。第２図は第１
図と同様に放電電流密度20ｍＡ／cm2における前記
２種類の電極の放電電位曲線を示すグラフであ
る。() Example 2 In order to confirm the porosity effect due to the elution of water-soluble components (polyvinyl alcohol) by the hot water treatment shown in Example 1, the surface of a carbon plastic member was coated with the same specifications and method as in Example 1. Electrostatic painting is carried out under a certain pressure (200Kg/
cm 2 ) to uniformly press the painted surface. After making the painted surface flat in this way, connect this electrode to the
It was divided into two sheets, one of which was treated with hot water to make it porous in the same manner as in Example 1, and the other with no hot water treatment, and the discharge potential characteristics of each sheet were compared. Figure 2 is the first
It is a graph showing discharge potential curves of the two types of electrodes at a discharge current density of 20 mA/cm 2 similarly to the figure.
第２図から明らかなように、温水処理を施して
多孔化したESP−CPプレス電極の方が、温水処
理を施さないESP−CPプレス電極よりもすぐれ
た特性を示し、多孔化による効果が現われてい
る。又温水処理を施して多孔化した方の電極の低
Br2濃度範囲のカーブをみると、先の実施例１に
おける第１図のESP−CPの低Br2濃度範囲での電
位向上には、この温水処理による多孔化が大きく
奇与していると考えられる。 As is clear from Figure 2, the ESP-CP press electrode that has been made porous by hot water treatment has better properties than the ESP-CP press electrode that has not been treated with hot water, and the effect of making the porous material appears. ing. Also, the electrodes that have been made porous by hot water treatment have a lower
Looking at the curve in the Br 2 concentration range, it can be seen that the porosity caused by the hot water treatment has a large effect on the potential improvement in the low Br 2 concentration range of the ESP-CP shown in Figure 1 in Example 1. Conceivable.
尚、第３図、第４図、第５図はそれぞれ実施例
１の本発明の電極即ちESP−CPの粒子構造を示
す走査型電子顕微鏡写真であり、第３図は100倍、
第４図は700倍、第５図は3000倍である。 Note that FIGS. 3, 4, and 5 are scanning electron micrographs showing the particle structure of the electrode of the present invention of Example 1, that is, ESP-CP, and FIG.
Figure 4 is 700 times larger, and Figure 5 is 3000 times larger.
これらの図から明らかなように、電極表面はほ
ぼフラツトな中に大小の空孔が現われており、多
孔化剤の溶出された後の状態がよく示されてい
る。 As is clear from these figures, the electrode surface is almost flat, with large and small pores appearing, which clearly shows the state after the porosity-forming agent has been eluted.
上記実施例の効果からも明らかなように、本発
明は次の効果を奏する。
As is clear from the effects of the above embodiments, the present invention has the following effects.
() カーボンプラスチツクの持つている導電性
を利用して静電塗装法により該カーボンプラス
チツク部材の表面に表面処理剤層を形成し、該
形成層中の水溶成分を温水処理によつて溶出さ
せることにより多孔化するので、経済性、電池
効率、耐用寿命のすべての面で向上がみられ
る。() Forming a surface treatment agent layer on the surface of the carbon plastic member by electrostatic coating using the conductivity of carbon plastic, and eluting water-soluble components in the formed layer by hot water treatment. This increases porosity, resulting in improvements in all aspects of economy, battery efficiency, and service life.
() 上記の構成になる電極は、臭素極としての
放電電位特性にすぐれ、亜鉛−臭素電池の陽極
として十分使用できる。特に低Br2濃度範囲に
おける電極表面活性の向上化が図られる。() The electrode having the above structure has excellent discharge potential characteristics as a bromine electrode, and can be used satisfactorily as an anode of a zinc-bromine battery. In particular, the electrode surface activity is improved in the low Br 2 concentration range.
第１図は電極電位と電解液中のBr2濃度の関係
を示したグラフ、第２図は電極電位と電解液中の
Br2濃度の関係を示すグラフ、第３図、第４図、
第５図は夫々本発明実施例電極の表面の粒子構造
を示す電子顕微鏡写真である。
Figure 1 is a graph showing the relationship between the electrode potential and the Br 2 concentration in the electrolyte, and Figure 2 is a graph showing the relationship between the electrode potential and the Br 2 concentration in the electrolyte.
Graphs showing the relationship between Br 2 concentration, Figures 3 and 4,
FIG. 5 is an electron micrograph showing the particle structure of the surface of each electrode according to an example of the present invention.
Claims (1)
末及び多孔化剤を含む合成樹脂層を静電塗装法で
形成した後、多孔化処理を施すことを特徴とする
多孔性カーボンプラスチツク電極の製造方法。 ２ カーボンプラスチツク部材の表面に導電性粉
末、多孔化処理剤、及びイオン交換繊維を含む合
成樹脂層を静電塗装法で形成した後、多孔化処理
を施すことを特徴とする多孔性カーボンプラスチ
ツク電極の製造方法。[Scope of Claims] 1. A porous carbon plastic electrode characterized in that a synthetic resin layer containing conductive powder and a porosity-forming agent is formed on the surface of a carbon plastic member by an electrostatic coating method and then subjected to a porosity treatment. manufacturing method. 2. A porous carbon plastic electrode characterized in that a synthetic resin layer containing conductive powder, a porous treatment agent, and ion exchange fibers is formed on the surface of a carbon plastic member by electrostatic coating, and then a porous treatment is performed. manufacturing method.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59164751A JPS6145567A (en) | 1984-08-08 | 1984-08-08 | Method for manufacturing porous carbon plastic electrodes |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59164751A JPS6145567A (en) | 1984-08-08 | 1984-08-08 | Method for manufacturing porous carbon plastic electrodes |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS6145567A JPS6145567A (en) | 1986-03-05 |
| JPH0421987B2 true JPH0421987B2 (en) | 1992-04-14 |
Family
ID=15799222
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59164751A Granted JPS6145567A (en) | 1984-08-08 | 1984-08-08 | Method for manufacturing porous carbon plastic electrodes |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS6145567A (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS63174279A (en) * | 1987-01-13 | 1988-07-18 | Meidensha Electric Mfg Co Ltd | Metal-halogen battery electrodes |
Family Cites Families (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CH554078A (en) * | 1971-08-31 | 1974-09-13 | Consiglio Nazionale Ricerche | ELECTRIC ACCUMULATOR. |
| DE2615779C3 (en) * | 1976-04-10 | 1980-04-03 | Daimler-Benz Ag, 7000 Stuttgart | Process for the production of sintered electrode bodies |
| JPS5438285A (en) * | 1977-08-31 | 1979-03-22 | Kanegafuchi Chem Ind Co Ltd | Cation exchange membrane and electrolysis method using the same |
| JPS5996662A (en) * | 1982-11-24 | 1984-06-04 | Meidensha Electric Mfg Co Ltd | Plastic electrodes for zinc-bromine batteries |
-
1984
- 1984-08-08 JP JP59164751A patent/JPS6145567A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS6145567A (en) | 1986-03-05 |
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| Date | Code | Title | Description |
|---|---|---|---|
| LAPS | Cancellation because of no payment of annual fees |