JPH07150380A - Electrolytic cell - Google Patents
Electrolytic cellInfo
- Publication number
- JPH07150380A JPH07150380A JP5323188A JP32318893A JPH07150380A JP H07150380 A JPH07150380 A JP H07150380A JP 5323188 A JP5323188 A JP 5323188A JP 32318893 A JP32318893 A JP 32318893A JP H07150380 A JPH07150380 A JP H07150380A
- Authority
- JP
- Japan
- Prior art keywords
- catalyst
- carbon sheet
- carbon
- slit
- electrolytic cell
- 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.)
- Granted
Links
Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は、隔膜電解法により水素
や塩素等のガスを製造する電解槽に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an electrolytic cell for producing a gas such as hydrogen or chlorine by a diaphragm electrolysis method.
【０００２】[0002]
【従来の技術】従来、この種の電解槽の一つとして、薄
膜状の隔膜の両面に、電解液が流通可能な空隙を備えた
炭素繊維からなる板状電極を密着配置したものが用いら
れているが、電解時の電力消費量低減のために、電極に
触媒を担持することにより活性化過電圧を低下させるこ
とが行なわれている。このようなものの担持形態として
は電解液が流通可能な前記板状電極に触媒を直接担持す
る方法、（特公昭６３−３５９１号公報）や薄板状のカ
ーボンシートに触媒を担持し、このシート状の触媒電極
を隔膜と板状電極との間に挾み込む方法 (特開昭６３−
５０４９０号公報）が知られている。2. Description of the Related Art Conventionally, as one of the electrolytic baths of this type, there has been used one in which a plate-like electrode made of carbon fiber having a void through which an electrolytic solution can flow is closely arranged on both sides of a thin membrane. However, in order to reduce the power consumption during electrolysis, a catalyst is carried on the electrodes to reduce the activation overvoltage. As a supporting form of such a material, a method of directly supporting a catalyst on the plate-shaped electrode through which an electrolytic solution can flow (Japanese Patent Publication No. 63-3591) or a catalyst on a thin carbon sheet, Method of sandwiching the catalyst electrode of the invention between the diaphragm and the plate electrode (Japanese Patent Laid-Open No. 63-
No. 50490) is known.
【０００３】[0003]
【発明が解決しようとする課題】しかしながら、従来の
電解槽で用いられる電極は、板状電極に直接触媒を担持
した場合には、フェルト状の電極の内側まで触媒が浸透
しているので、反応により発生したガスが電極内に留ま
り、発生したガスにより電解液の見かけの導電率が低下
し電解液での電圧降下が増大してしまった。この電圧降
下は板状電極の厚さ方向において、対極（つまり隔膜）
から遠ざかるほど大となり、電極反応は隔膜の近傍にお
いて集中的に起こり、隔膜から遠い部分では触媒が有効
に利用されていなかった。However, in the electrode used in the conventional electrolytic cell, when the catalyst is directly carried on the plate-shaped electrode, the catalyst penetrates to the inside of the felt-shaped electrode. The gas generated by the method remained in the electrode, and the generated gas decreased the apparent conductivity of the electrolytic solution and increased the voltage drop in the electrolytic solution. This voltage drop is the counter electrode (that is, the diaphragm) in the thickness direction of the plate electrode.
The electrode reaction was concentrated near the diaphragm, and the catalyst was not effectively used in the part far from the diaphragm.
【０００４】触媒として白金族金属等高価な触媒を用い
た場合、触媒が有効に利用されないのは大きな問題であ
るが、触媒を電極の隔膜に接する面近傍に選択的に担持
するのは煩雑な工程が必要となり製作費が大きくなると
いう問題があった。When an expensive catalyst such as a platinum group metal is used as the catalyst, it is a big problem that the catalyst is not effectively used, but it is complicated to selectively carry the catalyst in the vicinity of the surface of the electrode which contacts the diaphragm. There is a problem that the manufacturing cost is increased because the process is required.
【０００５】また隔膜と板状電極との間に触媒を担持し
たカーボンシートを挾み込む方法も、炭素繊維から構成
されるカーボンシート内部に発生したガスが滞留し、同
じように電解液による電圧降下の増大、すなわち電解電
圧が増大し電力消費量が増大するという問題が生じてい
た。そこで、本発明は電極内にガス留りのしにくい電極
を用いることにより電解電圧を低減し、さらに高価な触
媒を有効利用して触媒の使用量低減が可能な電解槽を提
供することを目的とする。Also, in the method of sandwiching a carbon sheet carrying a catalyst between the diaphragm and the plate electrode, the gas generated inside the carbon sheet composed of carbon fibers stays and the voltage caused by the electrolytic solution is similarly generated. There has been a problem that the drop is increased, that is, the electrolytic voltage is increased and the power consumption is increased. Therefore, the present invention aims to provide an electrolytic cell capable of reducing the electrolysis voltage by using an electrode in which gas retention is difficult, and effectively using an expensive catalyst to reduce the amount of the catalyst used. And
【０００６】[0006]
【課題を解決するための手段】前記課題を解決するた
め、本発明の電解槽は電解液が流通可能な空隙を備えた
炭素繊維からなる板状の電極をイオン交換膜の両面に密
着配置し、これらをエンドプレートで挟持してなる電解
槽において、前記イオン交換膜と電極との間の少なくと
も一方に電解液が流通可能な空隙を備えた、炭素繊維か
らなり、触媒を担持し、かつ上下方向の多数のスリット
を有するカーボンシートが介挿されていることを特徴と
する。炭素繊維から構成され、かつ微細な空隙を有する
カーボンシートとしては、カーボンフェルト及び炭素ク
ロスなども使用することができる。またスリットとして
は、直線状、下向き樹枝状、その他の形状のものが用い
られる。またイオン交換膜としてはアニオン交換膜ある
いはカチオン交換膜を反応の目的に応じて選択すること
ができる。なお、本発明の電解槽は一基単独で使用して
もよいし、直列に多数積層してフィルタープレス型の槽
を構成してもよいものである。In order to solve the above-mentioned problems, in the electrolytic cell of the present invention, plate-like electrodes made of carbon fiber provided with voids through which an electrolytic solution can flow are closely arranged on both sides of an ion exchange membrane. In an electrolytic cell in which these are sandwiched by end plates, at least one of the ion exchange membrane and the electrode is provided with a void through which an electrolytic solution can flow, is made of carbon fiber, carries a catalyst, and is vertically It is characterized in that a carbon sheet having a large number of slits in the direction is inserted. As the carbon sheet composed of carbon fibers and having fine voids, carbon felt and carbon cloth can also be used. Further, as the slit, linear slits, downward dendritic slits, and other slits are used. As the ion exchange membrane, an anion exchange membrane or a cation exchange membrane can be selected according to the purpose of the reaction. The electrolytic cell of the present invention may be used alone, or a plurality of cells may be laminated in series to form a filter press type cell.
【０００７】[0007]
【作用】上記手段においては、電極となるカーボンシー
トが反応層として機能し、かつ電解により発生するガス
が電極のスリットを介して放出されるため電解電圧を低
減することができ電解効率が向上するとともに、担持し
た触媒をすべて有効に利用することができる。In the above means, the carbon sheet that serves as an electrode functions as a reaction layer, and the gas generated by electrolysis is released through the slit of the electrode, so that the electrolysis voltage can be reduced and the electrolysis efficiency can be improved. At the same time, all the supported catalysts can be effectively used.
【０００８】[0008]
【実施例】以下、本発明の実施例について図面を参照し
て説明する。図１は本発明の電解槽の一実施例を示す断
面図である。この電解槽は、イオン交換膜（カチオン交
換膜）１の片面に、カーボンフェルト製陽極電極２を密
着配置すると共に、イオン交換膜（カチオン交換膜）１
の残る片面に、図２に示すように、上下方向の多数のス
リット３を有するカーボンシート４を介挿してカーボン
フェルト製陰極電極５を密着配置し、かつこれらを陽極
液入口、出口６ａ、６ｂを有する陽極側エンドプレート
６及び陰極液入口、出口７ａ、７ｂを有する陰極側エン
ドプレート７で挟持して構成されている。Embodiments of the present invention will be described below with reference to the drawings. FIG. 1 is a sectional view showing an embodiment of the electrolytic cell of the present invention. In this electrolytic cell, an anode electrode 2 made of carbon felt is closely arranged on one side of an ion exchange membrane (cation exchange membrane) 1 and an ion exchange membrane (cation exchange membrane) 1
As shown in FIG. 2, a carbon sheet 4 having a large number of slits 3 in the vertical direction is interposed on the remaining one side of the sheet to place a carbon felt cathode electrode 5 in close contact therewith. It is configured to be sandwiched between the anode side end plate 6 having the above and the cathode side end plate 7 having the cathode liquid inlet and outlets 7a and 7b.
【０００９】ここで、図２に示すように、縦 250mm、横
200mmのカーボンシート８の周辺縦10mm横９mmを除く範
囲に、幅２mm、長さ 230mmの16本のスリット９を等間隔
で開けたスリット有りで厚さ 0.3mmのカーボンシート１
（実施例）及び縦 250mm、横200mmのスリット無しで厚
さ 0.3mmのカーボンシート (比較例１）、のそれぞれ
に、触媒として白金 (Ｐｔ) を0.56mg/cm2担持させ、実
施例及び比較例１用の触媒付きカーボンシートを作製し
た。触媒の担持は、塩化白金酸液に有機溶剤の希釈液
(本実施例では２−プロパノールを純水で希釈した液）
を加えた塩化白金酸希釈液を、上記各カーボンシートに
含浸担持させた後、水素還元を施して行った。Here, as shown in FIG. 2, the length is 250 mm and the width is
A carbon sheet 1 with a thickness of 0.3 mm with 16 slits 9 with a width of 2 mm and a length of 230 mm opened at equal intervals in a range excluding a peripheral length of 10 mm and a width of 9 mm of a 200 mm carbon sheet 1
(Example) and a carbon sheet (comparative example 1) having a length of 250 mm and a width of 200 mm and a thickness of 0.3 mm (comparative example 1) were each loaded with 0.56 mg / cm 2 of platinum (Pt) as a catalyst. A carbon sheet with a catalyst for Example 1 was prepared. The catalyst is supported by a chloroplatinic acid solution diluted with an organic solvent.
(In this example, a solution obtained by diluting 2-propanol with pure water)
Each of the above carbon sheets was impregnated and supported with the dilute chloroplatinic acid diluted with, and then hydrogen reduction was performed.
【００１０】そして、触媒付きスリット有りカーボンシ
ート及びスリット無しカーボンシート（共に0.56mg/cm2
Ｐｔ担持) を先に述べた電解槽に使用し、下記条件で同
時に電解実験したところ、電解電圧の経時変化は、図４
に示すようになった。 （電解条件） 温度 ：60℃ 陽極液 ： 1.0mol/l ＦｅＳＯ4 、 0.5mol/l Ｈ2 ＳＯ
4 水溶液 陰極液 ： 0.5mol/l Ｈ2 ＳＯ4 水溶液 電解方法 ：定電流電解50、 100Ａ (100 、200mA/cm2
相当) 陽極及び陰極 ：厚さ５mmのカーボンフェルトA carbon sheet with a catalyst and a slit and a carbon sheet without a slit (both 0.56 mg / cm 2
Pt) was used in the electrolytic cell described above, and an electrolysis experiment was conducted simultaneously under the following conditions.
It came to be shown in. (Electrolysis conditions) Temperature: 60 ° C Anolyte: 1.0mol / l FeSO 4 , 0.5mol / l H 2 SO
4 aqueous solution Catholyte: 0.5 mol / l H 2 SO 4 aqueous solution Electrolysis method: constant current electrolysis 50, 100 A (100, 200 mA / cm 2
Equivalent) Anode and cathode: 5mm thick carbon felt
【００１１】図４より100mA/cm2 で電解したときは、電
解電圧にはほとんど差が認められなかったが、200mA/cm
2 の電流密度では、スリット有りカーボンシートの方が
スリット無しカーボンシートより電解電圧が0.07Ｖほど
低くなっている。これは本発明の電解槽では電極の近傍
に滞留するガスがスリットから有効に排出されるためで
あり、ガス発生の多い高電流密度において、その効果が
明らかである。From FIG. 4, when electrolyzing at 100 mA / cm 2 , there was almost no difference in electrolysis voltage, but 200 mA / cm
At the current density of 2, the electrolysis voltage of the carbon sheet with slits is about 0.07V lower than that of the carbon sheet without slits. This is because in the electrolytic cell of the present invention, the gas staying in the vicinity of the electrode is effectively discharged from the slit, and the effect is clear at high current density where much gas is generated.
【００１２】又、上記と同じ触媒付きスリット有りカー
ボンシート(0.56mg/cm2 Ｐｔ担持)（実施例）及び0.56m
g/cm2Ｐｔ担持（比較例２）と1.5mg/cm2 Ｐｔ担持（比
較例３）の触媒付きカーボンフェルトを電解槽に使用
し、上記と同じ条件（ただし電流密度は 100Ａ(200mA/c
m2相当) のみ）で電解したところ、電解電圧の経時変化
は図５に示すようになった。Also, the same carbon sheet with a slit as above (with 0.56 mg / cm 2 Pt supported) with catalyst (Example) and 0.56 m
The catalyst-supported carbon felt supporting g / cm 2 Pt (Comparative Example 2) and 1.5 mg / cm 2 Pt (Comparative Example 3) was used in the electrolytic cell under the same conditions as above (current density was 100 A (200 mA / c).
When electrolysis was performed using only (equivalent to m 2 )), the change with time of the electrolysis voltage became as shown in FIG.
【００１３】図５よりスリット有り触媒担持カーボンシ
ートを用いた本発明の電解槽では、触媒担持カーボンフ
ェルトを電極として用いた電解槽に比べ 1/3の白金量で
同等の性能が得られており、カーボンシートに担持した
触媒の白金が有効に利用されていることがわかる。As shown in FIG. 5, in the electrolytic cell of the present invention using the carbon sheet supporting the catalyst with slits, the same performance was obtained with an amount of platinum of 1/3 as compared with the electrolytic cell using the carbon felt supporting the catalyst as an electrode. It can be seen that the catalyst platinum supported on the carbon sheet is effectively used.
【００１４】次に図３に示すように、縦 250mm、横 200
mmのカーボンシート10の周辺20mmを除く範囲に直径５mm
の空孔（パンチ）11を10mm間隔で縦17列横22列合計 374
個開けた、実施例のスリット有りカーボンシートと同様
の触媒有効面積を有する、空孔有りカーボンシート10を
作製し、前述と同様の方法で白金（Ｐｔ）を0.56mg/cm2
担持した触媒電極を比較例４の電極として用意した。触
媒付きスリット有りカーボンシート(0.56mg/cm2 Ｐｔ担
持) （実施例）及び0.56mg/cm2Ｐｔ担持の触媒付き空孔
有りで厚さ 0.3mmのカーボンシート (比較例４）を電解
槽に使用し、上記と同じ条件（ただし電流密度は 100Ａ
(200mA/cm2相当) のみ）で同時に電解実験したところ、
電解電圧の経時変化は、図６に示すようになった。図６
からスリットの方が、空孔より0.04乃至0.07Ｖ電解電圧
が低くなっており、スリットを開けたカーボンシートを
持つ電解槽の方が効率のよい反応を得られることがわか
る。 これは、スリットは、ガスが上方へ抜け易いが、
空孔は、それぞれの孔の上方にガス留りが生じて抜け悪
いためと考えられる。Next, as shown in FIG. 3, length 250 mm, width 200
5mm diameter in the range excluding 20mm around the 10mm carbon sheet
Holes (punch) 11 of 10 rows with 17 rows and 22 rows in total 374
An open carbon sheet 10 having pores and having a catalytic effective area similar to that of the slit carbon sheet of the example was prepared, and platinum (Pt) was added at 0.56 mg / cm 2 by the same method as described above.
The supported catalyst electrode was prepared as the electrode of Comparative Example 4. A carbon sheet with a slit with a catalyst (0.56 mg / cm 2 Pt supported) (Example) and a carbon sheet with a hole with a catalyst of 0.56 mg / cm 2 Pt and a thickness of 0.3 mm (Comparative Example 4) used as an electrolytic cell. Use the same conditions as above (however, the current density is 100A
(Only 200mA / cm 2 ))
The change with time of the electrolytic voltage was as shown in FIG. Figure 6
From the results, it can be seen that the slits have a lower electrolytic voltage of 0.04 to 0.07 V than the holes, and that an electrolytic cell having a carbon sheet with slits can obtain a more efficient reaction. This is because the slit makes it easy for gas to escape upward,
It is considered that the voids are not easily removed because gas remains above each of the voids.
【００１５】以上のことから、本発明の電解槽は電極へ
の触媒担持量低減及び電力消費量低減の面でより効果的
であることがわかる。From the above, it can be seen that the electrolytic cell of the present invention is more effective in reducing the amount of catalyst supported on the electrodes and reducing the power consumption.
【００１６】なお、上記実施例においては、本発明の電
解槽に使用するカーボンシートへの担持触媒として白金
を使用する場合について述べたが、これに限定されるも
のではなく、例えば金、銀、パラジウム又はロジウム等
の単体や合金、酸化物等を触媒として使用してもよい。
又、スリットは、上下方向の直線状のものに限らず、下
向きの樹枝状、その他のガスの抜け易い形状のものとし
てもよい。In the above embodiments, the case where platinum is used as the catalyst supported on the carbon sheet used in the electrolytic cell of the present invention has been described, but the present invention is not limited to this, and for example, gold, silver, A simple substance such as palladium or rhodium, an alloy, an oxide or the like may be used as a catalyst.
Further, the slit is not limited to the straight line in the vertical direction, but may be a downward tree-like slit or any other shape that facilitates the escape of gas.
【００１７】[0017]
【発明の効果】以上説明したように、本発明の電解槽に
よれば、カーボンシートが反応層として機能し、かつ電
解により発生するガスがスリットを介して放出されるの
で、電極近傍でのガス滞留を低減することができ、従来
に比して触媒量を大幅に低減し、かつ低い電解電圧で電
気分解でき、ひいては電力消費量を低減させることがで
きる。特に本発明の電解槽を直列に多数積層した場合、
電解電圧の低下による効果はさらに大きくなり、電力消
費量低減へ多大な貢献をするものである。As described above, according to the electrolytic cell of the present invention, the carbon sheet functions as a reaction layer, and the gas generated by electrolysis is released through the slit. The retention can be reduced, the amount of the catalyst can be significantly reduced as compared with the conventional case, and the electrolysis can be performed at a low electrolysis voltage, which in turn can reduce the power consumption. Particularly when a large number of electrolytic cells of the present invention are stacked in series,
The effect of lowering the electrolysis voltage becomes even greater, and contributes greatly to reducing power consumption.
【図１】本発明の電解槽の一実施例を示す断面図であ
る。FIG. 1 is a sectional view showing an embodiment of an electrolytic cell of the present invention.
【図２】図１に示す電解槽に用いるスリット有りカーボ
ンシートの正面図である。FIG. 2 is a front view of a carbon sheet with slits used in the electrolytic cell shown in FIG.
【図３】比較例４に用いた空孔有りカーボンシートの正
面図である。FIG. 3 is a front view of a carbon sheet with holes used in Comparative Example 4.
【図４】触媒付きスリット有りとスリット無しのカーボ
ンシートを用いた電解槽による電解電圧の経時変化をを
示す説明図である。FIG. 4 is an explanatory diagram showing changes with time of electrolytic voltage in an electrolytic cell using a carbon sheet with and without a slit with a catalyst.
【図５】触媒付きスリット有りカーボンシートと従来の
触媒付きカーボンフェルトを用いた電解槽による電解電
圧の経時変化を示す説明図である。FIG. 5 is an explanatory diagram showing a change with time of an electrolysis voltage in an electrolytic cell using a carbon sheet with a slit with a catalyst and a conventional carbon felt with a catalyst.
【図６】触媒付きスリット有りカーボンシートと触媒付
き空孔有りカーボンシートを用いた電解槽による電解電
圧の経時変化を示す説明図である。FIG. 6 is an explanatory diagram showing a change with time of an electrolysis voltage in an electrolytic cell using a carbon sheet with a catalyst-attached slit and a carbon sheet with a catalyst-attached hole.
１ カチオン交換膜 ２ カーボンフェルト製陽極電極 ３ スリット ４ 触媒付き空孔有りカーボンシート ５ カーボンフェルト製陰極電極 1 Cation Exchange Membrane 2 Carbon Felt Anode Electrode 3 Slit 4 Porous Carbon Sheet with Catalyst 5 Carbon Felt Cathode Electrode
Claims (1)
維からなる板状の電極をイオン交換膜の両面に密着配置
し、これらをエンドプレートで挟持してなる電解槽にお
いて、前記イオン交換膜と電極との間の少なくとも一方
に、電解液が流通可能な空隙を備えた、炭素繊維からな
り、触媒を担持し、かつ上下方向の多数のスリットを有
するカーボンシートが介挿されていることを特徴とする
電解槽。1. An ion exchange in an electrolytic cell in which plate-like electrodes made of carbon fibers having voids through which an electrolytic solution can flow are closely arranged on both sides of an ion exchange membrane, and these are sandwiched by end plates. At least one of the membrane and the electrode is provided with a void through which an electrolytic solution can flow, a carbon sheet made of carbon fiber, carrying a catalyst, and having a large number of vertical slits is interposed. Electrolyzer characterized by
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP05323188A JP3092771B2 (en) | 1993-11-29 | 1993-11-29 | Electrolytic cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP05323188A JP3092771B2 (en) | 1993-11-29 | 1993-11-29 | Electrolytic cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH07150380A true JPH07150380A (en) | 1995-06-13 |
| JP3092771B2 JP3092771B2 (en) | 2000-09-25 |
Family
ID=18152054
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP05323188A Expired - Fee Related JP3092771B2 (en) | 1993-11-29 | 1993-11-29 | Electrolytic cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3092771B2 (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2006322053A (en) * | 2005-05-20 | 2006-11-30 | Yoichi Sano | Electrode for water electrolysis |
| JP2015124425A (en) * | 2013-12-27 | 2015-07-06 | 旭化成株式会社 | Manifold unit and cell |
| JP2020045512A (en) * | 2018-09-18 | 2020-03-26 | 株式会社東芝 | Hydrogen production device, and diaphragm |
| WO2021161598A1 (en) * | 2020-02-14 | 2021-08-19 | パナソニックＩｐマネジメント株式会社 | Electrolytic liquid generation device |
-
1993
- 1993-11-29 JP JP05323188A patent/JP3092771B2/en not_active Expired - Fee Related
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2006322053A (en) * | 2005-05-20 | 2006-11-30 | Yoichi Sano | Electrode for water electrolysis |
| JP2015124425A (en) * | 2013-12-27 | 2015-07-06 | 旭化成株式会社 | Manifold unit and cell |
| JP2020045512A (en) * | 2018-09-18 | 2020-03-26 | 株式会社東芝 | Hydrogen production device, and diaphragm |
| WO2021161598A1 (en) * | 2020-02-14 | 2021-08-19 | パナソニックＩｐマネジメント株式会社 | Electrolytic liquid generation device |
Also Published As
| Publication number | Publication date |
|---|---|
| JP3092771B2 (en) | 2000-09-25 |
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