JPH0418621B2 - - Google Patents
Info
- Publication number
- JPH0418621B2 JPH0418621B2 JP59004305A JP430584A JPH0418621B2 JP H0418621 B2 JPH0418621 B2 JP H0418621B2 JP 59004305 A JP59004305 A JP 59004305A JP 430584 A JP430584 A JP 430584A JP H0418621 B2 JPH0418621 B2 JP H0418621B2
- Authority
- JP
- Japan
- Prior art keywords
- substrate
- measured
- immobilized enzyme
- electrode
- oxygen
- 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
- 239000000758 substrate Substances 0.000 claims description 48
- 108010093096 Immobilized Enzymes Proteins 0.000 claims description 36
- 239000012491 analyte Substances 0.000 claims description 8
- 239000007788 liquid Substances 0.000 claims description 5
- 238000009792 diffusion process Methods 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 3
- 230000003111 delayed effect Effects 0.000 claims 1
- 239000000126 substance Substances 0.000 claims 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 31
- 239000001301 oxygen Substances 0.000 description 31
- 229910052760 oxygen Inorganic materials 0.000 description 31
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 14
- 239000012528 membrane Substances 0.000 description 13
- 239000003054 catalyst Substances 0.000 description 7
- 230000007423 decrease Effects 0.000 description 7
- 238000005259 measurement Methods 0.000 description 6
- 238000010586 diagram Methods 0.000 description 4
- 238000000502 dialysis Methods 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000004809 Teflon Substances 0.000 description 3
- 229920006362 Teflon® Polymers 0.000 description 3
- HVYWMOMLDIMFJA-DPAQBDIFSA-N cholesterol Chemical group C1C=C2C[C@@H](O)CC[C@]2(C)[C@@H]2[C@@H]1[C@@H]1CC[C@H]([C@H](C)CCCC(C)C)[C@@]1(C)CC2 HVYWMOMLDIMFJA-DPAQBDIFSA-N 0.000 description 2
- 229910001882 dioxygen Inorganic materials 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 239000000696 magnetic material Substances 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 210000002966 serum Anatomy 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 description 1
- 235000012000 cholesterol Nutrition 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 239000008103 glucose Substances 0.000 description 1
- 150000002632 lipids Chemical class 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12Q—MEASURING OR TESTING PROCESSES INVOLVING ENZYMES, NUCLEIC ACIDS OR MICROORGANISMS; COMPOSITIONS OR TEST PAPERS THEREFOR; PROCESSES OF PREPARING SUCH COMPOSITIONS; CONDITION-RESPONSIVE CONTROL IN MICROBIOLOGICAL OR ENZYMOLOGICAL PROCESSES
- C12Q1/00—Measuring or testing processes involving enzymes, nucleic acids or microorganisms; Compositions therefor; Processes of preparing such compositions
- C12Q1/001—Enzyme electrodes
Description
【発明の詳細な説明】
本発明はセンサー電極に関し、特に、単一の電
極によつて複数基質の測定が可能なセンサー電極
に関する。DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a sensor electrode, and more particularly to a sensor electrode capable of measuring multiple substrates with a single electrode.
酸素電極、過酸化水素電極等のセンサー電極
は、被測定媒体中に溶け込んでいる酸素分子ある
いは過酸化水素を電解し、その時の電解電流を測
定することによつて酸素濃度あるいは過酸化水素
濃度を知り得るデバイスである。第１図は、従来
の酸素電極を示す図であり、１はガラス製の内
管、２は同じくガラス製の外管であり、該内管１
の底部には、白金製のカソード（第１電極）３が
設けられ、又、該外管２の底部には、酸素分子を
透過するテフロン膜４が取付けられている。該内
管１と該外管２との間には、内部液（30％
NaOH）５が入れられ、該内部液中には、鉛製
のアノード（第２電極）６が配置されている。該
カソード３、アノード６には夫々白金のリード線
１０を介して電流検出系に接続されている。該酸
素分子透過性のテフロン膜の外側には、中性脂質
等の測定対象の基質が透過できる透析膜７が設け
られ、その中には固定化酵素８が入れられてい
る。尚、９はＯリングである。 Sensor electrodes such as oxygen electrodes and hydrogen peroxide electrodes measure the oxygen concentration or hydrogen peroxide concentration by electrolyzing oxygen molecules or hydrogen peroxide dissolved in the medium to be measured and measuring the electrolytic current. It is a device that you can learn about. FIG. 1 is a diagram showing a conventional oxygen electrode, in which 1 is an inner tube made of glass, 2 is an outer tube also made of glass, and the inner tube 1
A cathode (first electrode) 3 made of platinum is provided at the bottom of the outer tube 2, and a Teflon membrane 4 that transmits oxygen molecules is attached to the bottom of the outer tube 2. Between the inner tube 1 and the outer tube 2, an internal liquid (30%
NaOH) 5 is placed in the internal liquid, and an anode (second electrode) 6 made of lead is placed in the internal liquid. The cathode 3 and anode 6 are connected to a current detection system via platinum lead wires 10, respectively. A dialysis membrane 7 through which a substrate to be measured such as a neutral lipid can permeate is provided on the outside of the oxygen molecule permeable Teflon membrane, and an immobilized enzyme 8 is placed therein. In addition, 9 is an O-ring.
このような酸素電極は、被測定基質が入れられ
た溶液中に浸される。その後、該固定化酵素８を
触媒として被測定基質は反応し、該反応によつて
溶液中の酸素分子濃度が低下する。この減少する
酸素分子の量を該電極間に流れる電流値に基づい
て測定し、結果として該被測定基質の濃度を測定
するようにしている。しかしながら、このような
酸素電極は単一の基質に対してのみその濃度を測
定することができ、他の基質を測定するために
は、種類の異なつた固定化酵素を備えた別の酸素
電極を用意しなければならない。 Such an oxygen electrode is immersed in a solution containing the substrate to be measured. Thereafter, the substrate to be measured reacts with the immobilized enzyme 8 as a catalyst, and the concentration of oxygen molecules in the solution decreases due to the reaction. This decreasing amount of oxygen molecules is measured based on the value of the current flowing between the electrodes, and as a result, the concentration of the substrate to be measured is measured. However, such an oxygen electrode can only measure the concentration of a single substrate; to measure other substrates, separate oxygen electrodes with different types of immobilized enzymes are required. Must be prepared.
本発明は上述した点に鑑みてなされたもので、
単一の電極によつて複数の基質を略同時に測定す
ることができるセンサー電極を提供することを目
的とする。 The present invention has been made in view of the above points, and
An object of the present invention is to provide a sensor electrode that can measure multiple substrates substantially simultaneously using a single electrode.
本発明に基づくセンサー電極は、内管と外管と
を有し、該内管の底部に配置された第１の電極
と、該内管と外管との間に入れられた内部液と、
該内部液中に配置された第２の電極と、該第１電
極に接近して配置された第１の被測定基質に感応
性の第１の固定化酵素と、第２の被測定基質に感
応性の第２の固定化酵素と、該第１と第２の固定
化酵素に近傍に配置された部材とを備え、該部材
により、該第１の固定化酵素への第１の被測定基
質の到達時刻と該第２の固定化酵素への第２の被
測定基質の到達時刻とに差が生じるように構成さ
れている。 The sensor electrode according to the present invention has an inner tube and an outer tube, a first electrode disposed at the bottom of the inner tube, and an internal liquid placed between the inner tube and the outer tube.
a second electrode disposed in the internal solution; a first immobilized enzyme sensitive to the first analyte substrate disposed close to the first electrode; and a first immobilized enzyme sensitive to the second analyte substrate. A sensitive second immobilized enzyme and a member disposed near the first and second immobilized enzymes, the member allows the first analyte to be measured to the first immobilized enzyme. The structure is such that a difference occurs between the arrival time of the substrate and the arrival time of the second measurement target substrate to the second immobilized enzyme.
以下本発明の一実施例を添付図面に基づき詳述
する。 An embodiment of the present invention will be described below in detail with reference to the accompanying drawings.
第２図は、本発明に基づく酸素電極を示してお
り、図中第１図の従来装置と同一部分は、同一番
号を付し、その詳細な説明を省略する。酸素ガス
透過性膜４と透析膜７との間の空間には、単一の
固定化酵素に代え、第１の被測定基質Ａに感応性
の第１の固定化酵素１１、第２の被測定基質Ｂに
感応性の第２の固定化酵素１２、中間膜１３が配
置されている。該中間膜１３としては、該基質Ａ
と基質Ｂとが共にその中を拡散できる材料であ
り、更に、その中の拡散速度が基質Ａと基質Ｂと
では相違するような材料が選ばれている。例え
ば、基質Ａがグルコースとし、基質Ｂがコレステ
ロールとすると、中間膜１３としては、透析膜が
使用される。 FIG. 2 shows an oxygen electrode according to the present invention. In the figure, the same parts as those of the conventional device shown in FIG. 1 are given the same numbers, and detailed explanation thereof will be omitted. In the space between the oxygen gas permeable membrane 4 and the dialysis membrane 7, instead of a single immobilized enzyme, a first immobilized enzyme 11 sensitive to the first analyte substrate A and a second immobilized enzyme are placed. A second immobilized enzyme 12 sensitive to the measurement substrate B and an intermediate film 13 are arranged. As the intermediate film 13, the substrate A
The material is selected such that both substrate A and substrate B can diffuse therein, and further, the diffusion rates in substrate A and substrate B are different. For example, if substrate A is glucose and substrate B is cholesterol, a dialysis membrane is used as the intermediate membrane 13.
第３図は、第２図に示した酸素電極２１を用い
た測定システムの一例を示している。該酸素電極
２１は、37℃に維持された水槽２２中に配置され
ているビーカ２３内に挿入される。該ビーカ２３
内の溶液中には、テフロン（登録商標）がコーテ
イングされた磁性体２４が入れられており、該ビ
ーカ２３の下部に設けられた回転磁場発生装置２
５による回転磁場により、該磁性体２４は回転
し、その結果、該ビーカ２３中の溶液は攪拌され
る。該酸素電極２１のカソード、アノード間に流
れた電流は、Ａ−Ｖ変換器２６によつて電圧信号
に変換され、演算回路２７に供給される。尚、２
８は測定試料をビーカ２３内に注入するためのマ
イクロシリンジである。 FIG. 3 shows an example of a measurement system using the oxygen electrode 21 shown in FIG. The oxygen electrode 21 is inserted into a beaker 23 placed in a water tank 22 maintained at 37°C. The beaker 23
A magnetic material 24 coated with Teflon (registered trademark) is placed in the solution in the beaker 23, and a rotating magnetic field generator 2 provided at the bottom of the beaker 23
5 rotates the magnetic body 24, and as a result, the solution in the beaker 23 is stirred. The current flowing between the cathode and anode of the oxygen electrode 21 is converted into a voltage signal by the AV converter 26 and supplied to the arithmetic circuit 27 . In addition, 2
8 is a microsyringe for injecting a measurement sample into the beaker 23.
上述した如き構成において、ビーカ２３内に酸
素電流２１を挿入し、磁性体２４を回転させて該
ビーカ内の溶液の攪拌を行う。該攪拌により、該
ビーカ２３内部の溶液中の酸素濃度はプラトーの
状態となり、その後、マイクロシリンジ２８より
血清が該溶液中に注入される。該血清中に含まれ
る第１の被測定基質Ａと第２の被測定基質Ｂは、
該酸素電極２１底部に設けられている中間膜１３
中を拡散して第１と第２の固定化酵素１１，１２
の部分に到達する。ここで、基質Ａの中間膜１３
中の拡散速度が基質Ｂのそれに比べて速い場合、
まず、基質Ａが第１の固定化酵素１１を触媒とし
て溶液中の酸素分子と反応し、過酸化水素等を生
成する。この結果、酸素電極底部のカソード３周
辺の酸素分子の量（濃度）は、該反応によつて少
くなり、該カソード３とアノード６との間に流れ
る電流は低くなる。第４図は時間経過に伴うこの
電流値変化を示した図であり、時刻t1で第１の固
定化酵素１１を触媒とした基質Ａの反応が開始さ
れ、該カソードとアノード間の電流値は徐々に減
少し、時刻t2で該電流値はプラトーの状態とな
る。この反応に寄与する酸素の量に比例した該電
流値の変化ａから該第１の被測定基質Ａの濃度を
測定することができる。更に、時刻t3になると、
第２の被測定基質Ｂが中間膜１３内を拡散して第
２の固定化酵素１２の部分に到達する。該第２の
被測定基質は、該第２の固定化酵素１２を触媒と
して溶液中の酸素分子と反応し、過酸化水素等を
生成する。この結果、酸素電極底部のカソード３
周辺の酸素分子の量（濃度）は、該反応によつて
少くなり、該カソード３とアノード６との間に流
れる電流は第４図に示す如く低くなる。時刻t4
に、該電流値はプラトーの状態となり、反応に寄
与する酸素の量に比例した該電流値の変化ｂを演
算回路２７で求めることによつて、該第２の被測
定基質Ｂの濃度を測定することができる。 In the above-described configuration, the oxygen current 21 is inserted into the beaker 23, and the magnetic body 24 is rotated to stir the solution in the beaker. Due to the stirring, the oxygen concentration in the solution inside the beaker 23 reaches a plateau state, and then serum is injected into the solution from the microsyringe 28. The first analyte substrate A and the second analyte substrate B contained in the serum are:
An intermediate film 13 provided at the bottom of the oxygen electrode 21
The first and second immobilized enzymes 11 and 12 are diffused inside.
reach the part. Here, the intermediate film 13 of substrate A
If the diffusion rate in substrate B is faster than that of substrate B,
First, the substrate A reacts with oxygen molecules in the solution using the first immobilized enzyme 11 as a catalyst to generate hydrogen peroxide and the like. As a result, the amount (concentration) of oxygen molecules around the cathode 3 at the bottom of the oxygen electrode decreases due to the reaction, and the current flowing between the cathode 3 and the anode 6 decreases. FIG. 4 is a diagram showing changes in this current value over time. At time t1 , the reaction of substrate A using the first immobilized enzyme 11 as a catalyst is started, and the current value between the cathode and the anode is gradually decreases, and the current value reaches a plateau at time t2 . The concentration of the first substrate A to be measured can be measured from the change a in the current value which is proportional to the amount of oxygen contributing to this reaction. Furthermore, at time t 3 ,
The second substrate to be measured B diffuses within the intermediate film 13 and reaches the second immobilized enzyme 12 portion. The second substrate to be measured reacts with oxygen molecules in the solution using the second immobilized enzyme 12 as a catalyst to generate hydrogen peroxide and the like. As a result, the cathode 3 at the bottom of the oxygen electrode
The amount (concentration) of surrounding oxygen molecules decreases due to this reaction, and the current flowing between the cathode 3 and anode 6 decreases as shown in FIG. time t 4
Then, the current value reaches a plateau state, and the concentration of the second substrate B to be measured is measured by determining the change b in the current value proportional to the amount of oxygen contributing to the reaction using the arithmetic circuit 27. can do.
第５図は、本発明の他の実施例を示しており、
第２図と同一部分は同一番号を付してある。この
実施例では、中間膜を第１と第２の固定化酵素膜
１１，１３の間に配置しており、被測定試料を注
入後、直ちに第１の固定化酵素を触媒とした第１
の被測定基質Ａの反応が開始され、測定電流値は
減少を始める。該反応がプラトーとなつた後に、
中間膜１３を拡散して第２の被測定基質SBが第
２の固定化酵素１２の部分に到達し、該第２の固
定化酵素を触媒とした基質Ｂの反応が開始され
る。この実施例でも、第４図に示した如き電流変
化が測定される。 FIG. 5 shows another embodiment of the invention,
The same parts as in FIG. 2 are given the same numbers. In this embodiment, an intermediate membrane is placed between the first and second immobilized enzyme membranes 11 and 13, and immediately after the sample to be measured is injected, the first immobilized enzyme is used as a catalyst.
The reaction of substrate A to be measured starts, and the measured current value starts to decrease. After the reaction reaches a plateau,
The second substrate to be measured SB diffuses through the intermediate film 13 and reaches the second immobilized enzyme 12, and a reaction of the substrate B using the second immobilized enzyme as a catalyst is started. In this embodiment as well, current changes as shown in FIG. 4 are measured.
このように本発明においては、複数の固定化酵
素と、複数の基質の夫々が、対応した固定化酵素
に到達する時間を互いに相違させるための中間膜
とを設けるようにしたので、単一の酸素電極であ
るにも抱わらず、複数の基質を略同時に測定する
ことができる。尚、本発明は上述した実施例に限
定されることなく幾多の変形が可能である。例え
ば、３種以上の基質を測定するために３種以上の
固定化酵素を設けるようにしても良い。この場
合、夫々の基質の対応した固定化酵素への到達時
間が互いに相違するように、中間膜の材料を選定
する必要がある。又、酸素電極を例に挙げて説明
したが、固定化酵素を触媒とした反応によつて生
成された過酸化水素の濃度を測定するようにした
過酸化水素電極にも本発明を適用することができ
ると共に、酸素系によつてPH電極にも適用するこ
とができる。 In this way, in the present invention, since a plurality of immobilized enzymes and an intermediate membrane are provided to make the times at which each of a plurality of substrates reaches the corresponding immobilized enzymes different from each other, a single Despite being an oxygen electrode, multiple substrates can be measured almost simultaneously. Note that the present invention is not limited to the embodiments described above, and can be modified in many ways. For example, three or more types of immobilized enzymes may be provided in order to measure three or more types of substrates. In this case, it is necessary to select the material of the intermediate film so that the arrival times of each substrate to the corresponding immobilized enzyme are different from each other. Further, although the explanation has been given using an oxygen electrode as an example, the present invention can also be applied to a hydrogen peroxide electrode that measures the concentration of hydrogen peroxide produced by a reaction using an immobilized enzyme as a catalyst. It can also be applied to PH electrodes due to the oxygen system.
第１図は従来の酸素電極を示す図、第２図は本
発明の一実施例を示す図、第３図は酸素電極を用
いた基質測定システムの一例を示す図、第４図は
測定電流値を示す図、第５図は本発明の他の実施
例を示す図である。
１……内管、２……外管、３……カソード、４
……酸素ガス透過性膜、６……アノード、７……
透析膜、１１，１２……固定化酵素膜、１３……
中間膜、２１……酸素電極、２２……水槽、２３
……ビーカ、２４……磁性体、２５……回転磁場
発生装置、２６……Ａ−Ｖ変換器、２７……演算
回路、２８……マイクロシリンジ。
Fig. 1 shows a conventional oxygen electrode, Fig. 2 shows an embodiment of the present invention, Fig. 3 shows an example of a substrate measurement system using an oxygen electrode, and Fig. 4 shows the measurement current. A diagram showing values, FIG. 5 is a diagram showing another embodiment of the present invention. 1... Inner tube, 2... Outer tube, 3... Cathode, 4
...Oxygen gas permeable membrane, 6... Anode, 7...
Dialysis membrane, 11, 12...immobilized enzyme membrane, 13...
Intermediate film, 21... Oxygen electrode, 22... Water tank, 23
... Beaker, 24 ... Magnetic material, 25 ... Rotating magnetic field generator, 26 ... AV converter, 27 ... Arithmetic circuit, 28 ... Microsyringe.
Claims (1)
れた第１の電極と、該内管と外管との間に入れら
れた内部液と、該内部液中に配置された第２の電
極と、該第１電極に接近して配置された第１の被
測定基質に感応性の第１の固定化酵素と、第２の
被測定基質に感応性の第２の固定化酵素と、該第
１と第２の固定化酵素の近傍に配置された部材と
を備え、該部材により、該第１の固定化酵素への
第１の被測定基質の到達時刻と該第２の固定化酵
素への第２の被測定基質の到達時刻とに差が生じ
るように構成されたセンサー電極。 ２ 該第１と第２の基質は、該部材内を拡散して
第１と第２の固定化酵素に到達するように構成さ
れ、該部材内の第１と第２の基質の拡散速度に差
が生じるように、該部材の材質が選択されている
特許請求の範囲第１項記載のセンサー電極。 ３ 該部材は第１と第２の固定化酵素の間に配置
され、該第２の被測定基質は、該部材内を拡散し
て該第２の固定化酵素に到達することによつて、
反応開始時間が第１の被測定基質より遅延させら
れている特許請求の範囲第１項記載のセンサー電
極。[Claims] 1. It has an inner tube and an outer tube, and includes a first electrode placed at the bottom of the inner tube, an internal liquid placed between the inner tube and the outer tube, and a first electrode disposed at the bottom of the inner tube. a second electrode disposed in the internal solution, a first immobilized enzyme sensitive to the first analyte substrate disposed close to the first electrode, and a first immobilized enzyme sensitive to the second analyte substrate; a second immobilized enzyme, and a member disposed near the first and second immobilized enzymes; A sensor electrode configured such that a difference occurs between the time of arrival of the second substrate to be measured and the time of arrival of the second substrate to be measured to the second immobilized enzyme. 2. The first and second substrates are configured to diffuse within the member to reach the first and second immobilized enzymes, and the first and second substrates are configured to diffuse within the member to a rate of diffusion of the first and second substrates within the member. The sensor electrode according to claim 1, wherein the material of the member is selected such that a difference occurs. 3. The member is placed between the first and second immobilized enzymes, and the second substrate to be measured diffuses within the member and reaches the second immobilized enzyme, thereby
The sensor electrode according to claim 1, wherein the reaction start time is delayed compared to the first substance to be measured.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59004305A JPS60147644A (en) | 1984-01-13 | 1984-01-13 | Sensor electrode |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59004305A JPS60147644A (en) | 1984-01-13 | 1984-01-13 | Sensor electrode |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS60147644A JPS60147644A (en) | 1985-08-03 |
| JPH0418621B2 true JPH0418621B2 (en) | 1992-03-27 |
Family
ID=11580786
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59004305A Granted JPS60147644A (en) | 1984-01-13 | 1984-01-13 | Sensor electrode |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS60147644A (en) |
-
1984
- 1984-01-13 JP JP59004305A patent/JPS60147644A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS60147644A (en) | 1985-08-03 |
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