JP2012233818A - Na+ CONCENTRATION MEASUREMENT SYSTEM USING pH METER - Google Patents
Na+ CONCENTRATION MEASUREMENT SYSTEM USING pH METER Download PDFInfo
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Abstract
Description
本発明は、ｐＨ計を用いたＮａ+濃度測定システムに関し、比較電極としてＫＣｌ溶液と液絡部を有する標準ｐＨ計と比較電極としてＮａ+選択性膜を有する差動式ｐＨ計を用い、測定液中のＮａ+濃度を測定可能としたＮａ+濃度測定システムに関するものである。 The present invention relates to a Na + concentration measurement system using a pH meter, and uses a standard pH meter having a KCl solution and a liquid junction as a reference electrode and a differential pH meter having a Na + selective membrane as a reference electrode. The present invention relates to a Na + concentration measurement system capable of measuring the Na + concentration in a liquid.
ｐＨの測定には種々の方法があるが、そのうちの主なものとして、指示薬を用いるもの、水素電極を用いるもの、キンヒドロンを用いるもの、アンチモンを用いるものなどがあるが、現在工業用としてはガラス電極を用いたものが広く用いられている。 There are various methods for measuring pH. Among them, the main ones are those using indicators, those using hydrogen electrodes, those using quinhydrone, and those using antimony. Those using electrodes are widely used.
ガラス電極法はガラス膜の両側に異なった２種の溶液を置いたとき、両方の溶液（内部液と測定液）のｐＨの差に比例した起電力がガラス膜の両面に発生することを利用するものである。
図２はガラス電極法によるｐＨ測定装置の測定原理を示すものである。
図２に示すように、薄いガラス膜１ａで作られたガラス電極１の中にｐＨのわかっている溶液（ｐＨ７）２を入れ、これを測定液３の中に浸すとガラス膜１ａの両側に起電力が生じる。４は生じた起電力を取出す内部極（Ａｇ／ＡｇＣｌ）である。
The glass electrode method utilizes the fact that when two different solutions are placed on both sides of a glass membrane, an electromotive force proportional to the pH difference between both solutions (internal solution and measurement solution) is generated on both sides of the glass membrane. To do.
FIG. 2 shows the measurement principle of the pH measuring device by the glass electrode method.
As shown in FIG. 2, when a solution (pH 7) 2 having a known pH is placed in a glass electrode 1 made of a thin glass film 1a and immersed in a measurement liquid 3, the glass electrode 1 is placed on both sides of the glass film 1a. An electromotive force is generated. 4 is an internal pole (Ag / AgCl) which takes out the generated electromotive force.
一方基準となる比較電極５は内部にＫＣｌ溶液（例えば３．３ＭＫＣｌ）６を満たし、この中に内部極７（Ａｇ／ＡｇＣｌ）を浸漬する。比較電極５側は測定液３が多孔質セラミック製液絡部８に接しており、比較電極の内部液であるＫＣｌ溶液が液絡部８を通して流出し測定液３と接することで、温度、圧力、流量など測定液の性状の変化に係りなく測定液との間に一定の基準電位を得ている。
この方式は広い測定範囲、短い測定時間、優れた再現性、簡便な操作性を有するという特徴がある。
On the other hand, the reference electrode 5 serving as a reference is filled with a KCl solution (for example, 3.3 MKCl) 6 and an inner electrode 7 (Ag / AgCl) is immersed therein. On the comparison electrode 5 side, the measurement liquid 3 is in contact with the liquid ceramic junction 8, and the KCl solution, which is the internal liquid of the comparison electrode, flows out through the junction 8 and comes into contact with the measurement liquid 3. Regardless of changes in the properties of the measuring solution such as the flow rate, a constant reference potential is obtained between the measuring solution and the measuring solution.
This method is characterized by having a wide measurement range, a short measurement time, excellent reproducibility, and simple operability.
図３はこのようなガラス電極法によるｐＨと起電力（ｍＶ）の関係を示すものである。 ガラス電極法においては、ｐＨガラス電極のスロープは−５９．１６ｍＶ／ｐＨ（理論値）であり、比較電極（Ａｇ／ＡｇＣｌ）の起電力はｐＨに依存せず一定の値（数ｍＶ）であり、ｐＨガラス電極の起電力と比較電極の起電力がそれぞれ出力されて変換器でｐＨガラス電極の演算が行われる。
図３において、破線：ｐＨガラス電極の起電力
点線：比較電極の起電力
である。本発明ではガラス電極１と液絡部８を有する比較電極５で構成されたｐＨ計を標準ｐＨ計という。
FIG. 3 shows the relationship between pH and electromotive force (mV) by such a glass electrode method. In the glass electrode method, the slope of the pH glass electrode is −59.16 mV / pH (theoretical value), and the electromotive force of the reference electrode (Ag / AgCl) is a constant value (several mV) independent of pH. Then, the electromotive force of the pH glass electrode and the electromotive force of the reference electrode are output, and the pH glass electrode is calculated by the converter.
In FIG. 3, broken line: electromotive force of pH glass electrode
Dotted line: electromotive force of the reference electrode. In the present invention, a pH meter composed of the glass electrode 1 and the comparison electrode 5 having the liquid junction 8 is referred to as a standard pH meter.
図４はＮａ+選択性膜を用いた比較電極（以下ｐＮａガラス電極という）を示す要部断面図である。
図４において、１０は内部液（ｐＨ７）１１が満たされた球状のｐＨ応答ガラス膜であり、上方に内部ガラス管１４が液密に接続されている。球状のｐＨ応答ガラス膜１０の中には塩化銀電極１２および温度センサ１３が浸漬されている。１２ａは塩化銀電極１２に接続されたリード線である。
FIG. 4 is a cross-sectional view of a principal part showing a comparative electrode (hereinafter referred to as a pNa glass electrode) using a Na + selective membrane.
In FIG. 4, 10 is a spherical pH-responsive glass membrane filled with an internal liquid (pH 7) 11, and an internal glass tube 14 is liquid-tightly connected to the upper side. A silver chloride electrode 12 and a temperature sensor 13 are immersed in the spherical pH-responsive glass film 10. A lead wire 12 a is connected to the silver chloride electrode 12.
１５はｐＨ応答ガラス膜１０の上方に内部ガラス管１４を覆って液密に形成された外部ガラス管で、ｐＨ応答ガラス膜１０に近い下部付近の外周にｐＮＡ応答ガラス膜１６が形成されている。１７はｐＮａ応答ガラス膜１６の上方に形成された白金電極で、この白金電極にはリード線１７ａが接続されている。１５ａは外部ガラス管１５の内面に貼付され白金電極部分を除いて一端が白金電極１７の下方まで延長されたシールド板である。 An external glass tube 15 is formed in a liquid-tight manner so as to cover the internal glass tube 14 above the pH-responsive glass film 10, and a pNA-responsive glass film 16 is formed on the outer periphery near the lower part near the pH-responsive glass film 10. . Reference numeral 17 denotes a platinum electrode formed above the pNa-responsive glass film 16, and a lead wire 17a is connected to the platinum electrode. Reference numeral 15 a denotes a shield plate attached to the inner surface of the external glass tube 15 and having one end extended to the lower side of the platinum electrode 17 except for the platinum electrode portion.
１８は外部ガラス管と内部ガラス管の間に配置された中部ガラス管で、一端はｐＮａ応答ガラス膜１６の上方と白金電極１７の間の外部ガラス管１５の内周に液密に接続されており、内部ガラス管１４と中部ガラス管１８の空間には1ＭＮａＣｌ内部液１９が満たされている。２０は内部ガラス管１４と中部ガラス管１８の間に配置されｐＮａ応答ガラス膜１６の近傍に配置された塩化銀電極、２０ａは塩化銀電極に接続されたリード線である。 18 is a middle glass tube disposed between the outer glass tube and the inner glass tube, and one end is liquid-tightly connected to the upper periphery of the pNa-responsive glass film 16 and the inner periphery of the outer glass tube 15 between the platinum electrodes 17. The space between the inner glass tube 14 and the middle glass tube 18 is filled with a 1M NaCl internal liquid 19. A silver chloride electrode 20 is disposed between the inner glass tube 14 and the middle glass tube 18 and is disposed in the vicinity of the pNa-responsive glass film 16, and 20a is a lead wire connected to the silver chloride electrode.
図５は図２に示した液絡部を有する比較電極５の替りに図４に示すｐＮａガラス電極１０を有する比較電極２１を用いた例を示す模式図である。
この比較電極２１における基準電位は内部極２２の電位とｐＮａガラス膜１０の電位で決まる。
ここで、
（1）内部極電位は温度、ＫＣｌ濃度で決まる一定の単極電位を発生する。
（２）ｐＮａガラス電極の電位はＮａ+濃度が変化しなければ比較電極として使用できる。
FIG. 5 is a schematic view showing an example in which the reference electrode 21 having the pNa glass electrode 10 shown in FIG. 4 is used instead of the reference electrode 5 having the liquid junction shown in FIG.
The reference potential in the comparison electrode 21 is determined by the potential of the internal electrode 22 and the potential of the pNa glass film 10.
here,
(1) The internal electrode potential generates a constant unipolar potential determined by temperature and KCl concentration.
(2) The potential of the pNa glass electrode can be used as a reference electrode if the Na + concentration does not change.
比較電極としてｐＮａガラス電極を用いた差動式ｐＨ計は標準ｐＨ計と同様にＨ+濃度に選択的なｐＨガラス電極を使用しているが、比較電極にはＫＣｌや液絡ではなく、Ｎａ+選択性膜を使用している。その結果、
１）ｐＨガラス電極の起電力と比較電極の起電力がそれぞれ出力されて変換器で演算（ｐＨガラス電極の起電力−比較電極の起電力）が行われる。
A differential pH meter using a pNa glass electrode as a reference electrode uses a pH glass electrode selective to H + concentration as in the standard pH meter, but the reference electrode is not KCl or liquid junction, but Na. + Selective membrane is used. as a result,
1) The electromotive force of the pH glass electrode and the electromotive force of the reference electrode are output, and the calculation (electromotive force of the pH glass electrode−electromotive force of the reference electrode) is performed by the converter.
２）ｐＮａガラス電極は、測定液中のＮａ+濃度に依存性を示す。
３）校正（二点校正は）は通常１ｍｏｌ／ｌＮａ+となるように調整したｐＨ標準液を使用する。次に、測定水のｐＨを標準のｐＨ検出器使って測定し、差動式ｐＨ計のｐＨ値標準ｐＨ値に合わせ込む（1点校正）。仮に測定液が１ｍｏｌ／ｌのＮａ+を含んでいれば、比較電極としてｐＮａガラス電極を用いたｐＨ計（差動式ｐＨ計）は標準ｐＨ計と同じｐＨ値を示し、1点校正の必要はない。
2) The pNa glass electrode shows dependence on the Na + concentration in the measurement solution.
3) For calibration (two-point calibration), a pH standard solution adjusted to 1 mol / l Na + is usually used. Next, the pH of the measurement water is measured using a standard pH detector, and adjusted to the standard pH value of the differential pH meter (one-point calibration). If the measurement solution contains 1 mol / l Na + , the pH meter (differential pH meter) using a pNa glass electrode as the reference electrode shows the same pH value as the standard pH meter, and one-point calibration is required. There is no.
ところで、差動式ｐＨ計は比較電極にｐＮａガラス電極を使用しているため、液絡部やＫＣｌ溶液を必要としない利点があるが、比較電極であるｐＮａガラス電極の起電力はＮａイオンの濃度に依存してしまう。 By the way, since the differential pH meter uses a pNa glass electrode as a reference electrode, there is an advantage that a liquid junction or a KCl solution is not required. However, the electromotive force of the pNa glass electrode as a reference electrode is Na ion. It depends on the concentration.
そのため、ｐＨ測定をするためには、測定液中のＮａ+濃度は一定でなければならないという制約がある。（仮にＨ+の濃度が一定でも、Ｎａ+濃度が変化してしまうと、変換器に出力されるｐＨは変化してしまう。）
例えば、測定液のＮａ+濃度が２０％増加（減少）すると、指示値は０．１ｐＨ高く（低く）表示される。という課題があった。
Therefore, in order to measure pH, there is a restriction that the Na + concentration in the measurement solution must be constant. (Even if the H + concentration is constant, if the Na + concentration changes, the pH output to the converter will change.)
For example, when the Na + concentration of the measurement solution increases (decreases) by 20%, the indicated value is displayed as 0.1 pH higher (lower). There was a problem.
従って本発明は、標準ｐＨ計と比較電極としてｐＮａガラス電極を用いた差動式ｐＨ計を用い、ｐＨの変化量からＮａ+濃度を算出することで、Ｎａ+濃度を測定することを可能としたＮａ+濃度測定システムを実現することを目的としている。 Accordingly, the present invention uses a differential equation pH meter using the pNa glass electrode as reference electrode and standard pH meter, by calculating the Na + concentration from the amount of change in pH, possible to measure the Na + concentration It aims at realizing the Na + concentration measuring system.
本発明は上記課題を解決するためになされたもので、請求項１に記載のｐＨ計を用いたＮａ+濃度測定システムにおいては、
標準ｐＨ計と、比較電極としてｐＮａガラス電極を用いた差動式のｐＨ計を用い、ｐＨの変化量からＮａ+濃度を算出することで、Ｎａ+濃度を測定することをことを特徴とする。
The present invention has been made to solve the above problems, and in the Na + concentration measurement system using the pH meter according to claim 1,
Using a standard pH meter and a differential pH meter using a pNa glass electrode as a reference electrode, the Na + concentration is measured by calculating the Na + concentration from the amount of change in pH. .
請求項２においては、請求項１に記載のｐＨ計を用いたＮａ+濃度測定システムにおいて、
Ｎａ+濃度の算出は前記標準ｐＨ計により得られたｐＨ値と前記差動式ｐＨ計により得られたｐＨ値の差から演算することを特徴とする。
In claim 2, in the Na + concentration measurement system using the pH meter according to claim 1,
The Na + concentration is calculated from the difference between the pH value obtained by the standard pH meter and the pH value obtained by the differential pH meter.
以上説明したことから明らかなように本発明によれば、
標準ｐＨ計と比較電極としてｐＮａガラス電極を用いた差動式ｐＨ計を併用するため、ｐＨの値を測定しながらＮａ+濃度を測定することができる。
As is clear from the above description, according to the present invention,
Since a standard pH meter and a differential pH meter using a pNa glass electrode as a reference electrode are used in combination, the Na + concentration can be measured while measuring the pH value.
図１（ａ〜ｃ）はＮａ+濃度を１ｍｏｌ/ｌ（ｐＮａ＝０）から増減させた場合のｐＨガラス電極、ｐＮａガラス電極の起電力およびｐＨガラス電極の起電力−ｐＮａガラス電極の起電力を示す図である。
図１（ｂ）は、Ｎａ+濃度を１ｍｏｌ/ｌ（ｐＮａ＝０）とした場合の出力の一例を示すもので、ｐＮａガラス電極の起電力は点線で示されるゼロであるためｐＨガラス電極の起電力−ｐＮａガラス電極の起電力は図３に示される標準ｐＨ計のｐＨガラス電極の起電力の出力と一致している。
1A to 1C show the pH glass electrode, the electromotive force of the pNa glass electrode, and the electromotive force of the pH glass electrode when the Na + concentration is increased or decreased from 1 mol / l (pNa = 0) —the electromotive force of the pNa glass electrode. FIG.
FIG. 1 (b) shows an example of the output when the Na + concentration is 1 mol / l (pNa = 0). Since the electromotive force of the pNa glass electrode is zero indicated by the dotted line, the pH glass electrode Electromotive force—The electromotive force of the pNa glass electrode coincides with the output of the electromotive force of the pH glass electrode of the standard pH meter shown in FIG.
図１（ａ）はＮａ+濃度が減少した場合の出力の一例を示すもので、Ｎａ+濃度が薄くなるとｐＮａガラス電極の起電力は減少し、その結果（ｐＨガラス電極の起電力−ｐＮａガラス電極の起電力は大きくなる。
る。
FIG. 1 (a) shows an example of the output when the Na + concentration decreases. When the Na + concentration decreases, the electromotive force of the pNa glass electrode decreases, and as a result (electromotive force of pH glass electrode-pNa glass). The electromotive force of the electrode increases.
The
図１（ｃ）はＮａ+濃度が増大した場合の出力の一例を示すもので、Ｎａ+濃度が濃くなるとｐＮａガラス電極の起電力は増加し、その結果、ｐＨガラス電極の起電力−ｐＮａガラス電極の起電力は小さくなる。 FIG. 1 (c) shows an example of the output when the Na + concentration increases. When the Na + concentration increases, the electromotive force of the pNa glass electrode increases, and as a result, the electromotive force of the pH glass electrode-pNa glass. The electromotive force of the electrode is reduced.
即ち、Ｎａ+濃度が１ｍｏｌ／ｌの場合は、差動式ｐＨ計におけるｐＮａガラス電極の起電力はほぼ０ｍＶで、出力されるｐＨは標準ｐＨ計とほとんど同じ挙動を示す。
Ｎａ+濃度が薄くなると、差動式ｐＨ計におけるｐＮａガラス電極の起電力は減少し、その結果ｐＨガラス電極の起電力−ｐＮａガラス電極の起電力は増加するため、結果として出力されるｐＨは小さくなる。Ｎａ+濃度が濃くなると、ｐＮａガラス電極の起電力は増加し、その結果ｐＨガラス電極の起電力−ｐＮａガラス電極の起電力は減少するため、結果として出力されるｐＨは大きくなる。
That is, when the Na + concentration is 1 mol / l, the electromotive force of the pNa glass electrode in the differential pH meter is almost 0 mV, and the output pH shows almost the same behavior as the standard pH meter.
When the Na + concentration decreases, the electromotive force of the pNa glass electrode in the differential pH meter decreases, and as a result, the electromotive force of the pH glass electrode−the electromotive force of the pNa glass electrode increases. Get smaller. As the Na + concentration increases, the electromotive force of the pNa glass electrode increases, and as a result, the electromotive force of the pH glass electrode minus the electromotive force of the pNa glass electrode decreases, resulting in an increase in the output pH.
次に計算方法について説明する。
比較電極としてｐＮａガラス電極を用いたｐＨ計と標準ｐＨ計を用いて測定液のｐＨを同時に測定する。
Next, the calculation method will be described.
The pH of the measurement solution is simultaneously measured using a pH meter using a pNa glass electrode as a reference electrode and a standard pH meter.
そして、標準ｐＨ計で測定した値がｐＨ＝８、比較電極としてｐＮａガラス電極を用いたｐＨ計がｐＨ５を示したとする。この場合、比較電極としてｐＮａガラス電極を用いたｐＨ計で測定した値が標準ｐＨ計で測定した値よりｐＨが３減少しているので、ｐＮａで測定した値は３増加していることなり、ｐＮａガラス電極を用いたＮａ濃度＝３（Ｎａ= １０-3ｍｏｌ／ｌ）であることが分かる。 The value measured with a standard pH meter is assumed to be pH = 8, and the pH meter using a pNa glass electrode as the reference electrode shows pH 5. In this case, since the pH measured by a pH meter using a pNa glass electrode as a reference electrode is 3 lower than the value measured by a standard pH meter, the value measured by pNa is increased by 3, It can be seen that Na concentration using a pNa glass electrode = 3 (Na = 10 −3 mol / l).
また、標準のｐＨの出力がｐＨ＝８、比較電極としてｐＮ+ガラス電極を用いた差動式ｐＨ計がｐＨ８．７５を示したとする。この場合、比較電極としてｐＮａガラス電極を用いた差動式ｐＨ計で測定した値が標準ｐＨ計で測定した値よりｐＨが０．７５増加しているので、ｐＮａで測定した値は０．７５減少していることなり、ｐＮａ＝−０．７５（Ｎａ=５．６２ｍｏｌ／ｌ）であることが分かる。 Further, it is assumed that a standard pH output is pH = 8, and a differential pH meter using a pN + glass electrode as a reference electrode shows pH 8.75. In this case, since the pH measured by the differential pH meter using a pNa glass electrode as the reference electrode is 0.75 higher than the value measured by the standard pH meter, the value measured by pNa is 0.75. It can be seen that pNa = −0.75 (Na = 5.62 mol / l).
なお、以上の説明は、本発明の説明および例示を目的として特定の好適な実施例を示したに過ぎない。
従って本発明は、上記実施例に限定されることなく、その本質から逸脱しない範囲で更に多くの変更、変形を含むものである。
The above description merely shows a specific preferred embodiment for the purpose of explanation and illustration of the present invention.
Therefore, the present invention is not limited to the above-described embodiments, and includes many changes and modifications without departing from the essence thereof.
１ ガラス電極
２ ｐＨ７の溶液
３ 測定液
４、７、１１ 内部極
５ 比較電極
６ ３ＭＫＣＬ溶液
８ 液絡部
１０ Ｎａ+選択性膜
１２、２０ 塩化銀電極
１２ａ、１７ａ、２０ａ リード線
１３ 温度センサ
１４ 内部ガラス管
１５ 外部ガラス管
１５ａ シールド板
１６ ｐＮａ応答ガラス膜
１７ 白金電極
１８ 中部ガラス膜
１９ １ＭＮａＣｌ内部液
DESCRIPTION OF SYMBOLS 1 Glass electrode 2 Solution of pH 7 3 Measuring solution 4, 7, 11 Inner electrode 5 Reference electrode 6 3MKCL solution 8 Liquid junction 10 Na + selective membrane 12, 20 Silver chloride electrode 12a, 17a, 20a Lead wire 13 Temperature sensor 14 Internal glass tube 15 External glass tube 15a Shield plate 16 pNa responsive glass film 17 Platinum electrode 18 Middle glass film 19 1M NaCl internal solution
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| JP2011103552A JP5790923B2 (en) | 2011-05-06 | 2011-05-06 | Na + concentration measurement system using pH meter |
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| JP2011103552A JP5790923B2 (en) | 2011-05-06 | 2011-05-06 | Na + concentration measurement system using pH meter |
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| JP2012233818A true JP2012233818A (en) | 2012-11-29 |
| JP5790923B2 JP5790923B2 (en) | 2015-10-07 |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2015190590A1 (en) * | 2014-06-12 | 2015-12-17 | 東亜ディーケーケー株式会社 | Electrode member, composite electrode, and method of manufacturing electrode member |
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| JPS61258160A (en) * | 1985-04-30 | 1986-11-15 | Sadaichi Murai | Precision type ph and ion concentration measuring instrument |
| JPH0213845A (en) * | 1988-06-30 | 1990-01-18 | Shimadzu Corp | Measurement of concentration of alkali metal component |
| JPH0465666A (en) * | 1990-07-05 | 1992-03-02 | Terumo Corp | Reference electrode |
| JPH06148134A (en) * | 1992-11-11 | 1994-05-27 | Japan Organo Co Ltd | Glass electrode type trace sodium ion measuring device |
| JPH06505559A (en) * | 1991-03-01 | 1994-06-23 | セラマテツク・インコーポレイテツド | sodium ion sensor |
| JPH09196883A (en) * | 1996-01-19 | 1997-07-31 | Hitachi Ltd | Ion sensor |
| JP2004117280A (en) * | 2002-09-27 | 2004-04-15 | Dkk Toa Corp | Electrochemical measurement method, comparison electrode, and combined electrode |
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2011
- 2011-05-06 JP JP2011103552A patent/JP5790923B2/en active Active
Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS61258160A (en) * | 1985-04-30 | 1986-11-15 | Sadaichi Murai | Precision type ph and ion concentration measuring instrument |
| JPH0213845A (en) * | 1988-06-30 | 1990-01-18 | Shimadzu Corp | Measurement of concentration of alkali metal component |
| JPH0465666A (en) * | 1990-07-05 | 1992-03-02 | Terumo Corp | Reference electrode |
| JPH06505559A (en) * | 1991-03-01 | 1994-06-23 | セラマテツク・インコーポレイテツド | sodium ion sensor |
| JPH06148134A (en) * | 1992-11-11 | 1994-05-27 | Japan Organo Co Ltd | Glass electrode type trace sodium ion measuring device |
| JPH09196883A (en) * | 1996-01-19 | 1997-07-31 | Hitachi Ltd | Ion sensor |
| JP2004117280A (en) * | 2002-09-27 | 2004-04-15 | Dkk Toa Corp | Electrochemical measurement method, comparison electrode, and combined electrode |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2015190590A1 (en) * | 2014-06-12 | 2015-12-17 | 東亜ディーケーケー株式会社 | Electrode member, composite electrode, and method of manufacturing electrode member |
| JP2016001163A (en) * | 2014-06-12 | 2016-01-07 | 東亜ディーケーケー株式会社 | Electrode member, composite electrode, and electrode member manufacturing method |
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| JP5790923B2 (en) | 2015-10-07 |
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