WO1999012020A1 - Cellule de mesure de l'electrochimioluminescence - Google Patents

Cellule de mesure de l'electrochimioluminescence Download PDF

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Publication number
WO1999012020A1
WO1999012020A1 PCT/JP1998/003807 JP9803807W WO9912020A1 WO 1999012020 A1 WO1999012020 A1 WO 1999012020A1 JP 9803807 W JP9803807 W JP 9803807W WO 9912020 A1 WO9912020 A1 WO 9912020A1
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WO
WIPO (PCT)
Prior art keywords
cell
working electrode
counter electrode
magnet
electrode
Prior art date
Application number
PCT/JP1998/003807
Other languages
English (en)
Japanese (ja)
Inventor
Yuzaburo Namba
Michinori Usami
Original Assignee
Eisai Co., Ltd.
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Eisai Co., Ltd. filed Critical Eisai Co., Ltd.
Publication of WO1999012020A1 publication Critical patent/WO1999012020A1/fr

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Classifications

    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/75—Systems in which material is subjected to a chemical reaction, the progress or the result of the reaction being investigated
    • G01N21/76—Chemiluminescence; Bioluminescence

Definitions

  • the present invention relates to a cell for measuring electrochemiluminescence.
  • Electrochemical emission is a phenomenon in which an electroluminescent substance such as a metal chelate and a luminescent auxiliary cause an electrode reaction, and the luminescent substance is excited to emit light.
  • a measuring solution consisting of a reaction product labeled with an electrochemical luminescent substance or an electrolyte containing a luminescent auxiliary substance is introduced into a cell, and an electrode reaction occurs in the cell, and the ion generated by the reaction is removed.
  • a method for detecting light emission from an electrochemiluminescent substance excited by an annihilation reaction is conventionally known.
  • Fig. 1 shows a method for detecting antigen 1 such as a viral antigen, a cancer antigen, or an abnormal metabolite.
  • antigen 1 such as a viral antigen, a cancer antigen, or an abnormal metabolite.
  • magnetic beads 2 binding to an antigen 1 and a labeled antibody 3 are used.
  • the antibody-bound magnetic beads 2 have a configuration in which an antibody 6 made of a monoclonal antibody or the like is immobilized on magnetic beads 5 made of latex or the like containing ferrite.
  • Labeled antibody 3 is provided with a Ru (bpy) 3 electrochemiluminescent substance 7 configuration of the antibodies 8 made of monoclonal antibodies were immobilized on such represented by the following formula (1).
  • the antibody-bound magnetic beads 2 and the labeled antibody 3 are reacted with a sample containing the antigen 1.
  • the antibody-bound magnetic beads 2 and the labeled antibody 3 are conjugated to the antigen 1, and the antigen 1 is brought into a state in which it can be captured and labeled by a magnet (sandwiched state) 9, and detection and quantification are performed.
  • an antigen-binding magnetic bead 11 and a labeled antibody 12 that recognizes antibody 10 are used.
  • the antigen-bound magnetic beads 11 are composed of a solid body of the magnetic beads 13 and the antigens 14.
  • the labeled antibody 12 has a configuration in which an antibody 16 recognizing the antibody 10 is bound to an electrochemiluminescent substance 15. Soshi Then, by reacting the antigen-bound magnetic beads 11 and the labeled antibody 12 with the sample containing the antibody 10 in an antibody reaction, the sample can be captured and labeled by a magnet (sandwich-formed state) 17 by a magnet. Detection and quantification.
  • Figure 3 shows an example of the detection and quantification method, in which an antibody 1 is sandwiched between antibody-bound magnetic beads 2 and a labeled antibody 3 to detect electrochemiluminescence generated by an electrode reaction. Shown in the series. That is, the detection method is
  • the antigen 1 can be collected by a magnet by reacting again with the antigen 1 and the labeled antibody 3 by stirring again, and after the labeled state (sandwiched state) 9 is obtained, the magnet 25 is moved The labeled antigen 1 placed around the container 20 is held in the container 20. Then, by washing in this state, a step of removing the unreacted labeled antibody 3 in the container 20 together with the buffer
  • dihydrogenphosphate force helium ⁇ 2 ⁇ 0 4
  • electrolyte TPA T ripropyl am ine
  • electrochemiluminescent auxiliary substances moistened with comprising measuring liquid, such as such as (electrochemiluminescence (ECL) electrolyte ) 26 is supplied to the container 20 containing the washed (bead)-1 (antibody)-1 (antigen) complex, suspended and sent to the measurement electrode.
  • ECL electrochemical luminescence
  • Ru (bpy) 3 the electrochemiluminescent substance 7 held in 3, is a positive electrode
  • Ru (by) 3 in the ground state again circulates through the reaction shown in Fig. 4, thus producing an electrochemiluminescent material.
  • Ru (bpy) 3, which is 7, is repeatedly excited and emits photons 32 one after another.
  • a photodetector such as a photomultiplier tube
  • the amount of light can be used to detect and quantify the antigen 1 contained in the liquid.
  • the detection method using such electrochemiluminescence not only makes it easier to adjust the measurement solution, but also enables more advanced detection than the measurement method using chemiluminescence (CL). It has high hopes in the field of clinical medicine and other fields as a detection method for spores.
  • the above-described apparatus for detecting by utilizing electrochemiluminescence is provided with a cell through which the measurement solution flows, in which a working electrode and a counter electrode are arranged with a predetermined distance between the surfaces. And are arranged facing each other.
  • a configuration is adopted in which the object to be measured contained in the measurement solution is magnetically attracted to the surface of the working electrode by a magnet.
  • the measurement solution circulated in the cell is the measurement solution prepared in step 7 described above with reference to Fig. 4.
  • antigens sandwiched using antibody-bound magnetic beads and labeled antibodies are contained. Contains.
  • a working electrode, which is a positive electrode, and a counter electrode are provided on the bottom and top surfaces of the cell.
  • a square or rectangular metal plate is used for the working electrode.
  • the counter electrode is composed of a pair of elongated metal plates arranged above the side of the working electrode and a frame-shaped metal plate arranged so as to surround the side of the working electrode above. It is common.
  • Japanese Patent Application Laid-Open No. 7-209189 is known. so is there.
  • the measurement liquid (electrolyte) to which the potential is applied causes ion dissociation at the interface, and the measurement liquid in the cell and the working electrode form an electric double layer, generating a back electromotive voltage determined by the ion species.
  • a potential exceeding the measured voltage is generated between the test solution and the test solution, the current flowing based on the voltage difference causes the actual electrochemical reaction to proceed.
  • An object of the present invention is to provide an electrochemical chemiluminescence measuring cell capable of generating uniform electrochemiluminescence over the entire surface of a working electrode and measuring the generated light with high accuracy. Disclosure of the invention
  • a cell for measuring electrochemiluminescence comprises: a cell through which a measurement solution is flown; and a working electrode, whose surfaces are opposed to each other at a predetermined interval in the cell. And a counter electrode, and a magnet for magnetically adsorbing an object to be measured contained in a measuring solution on the surface of the working electrode, wherein the surface of the working electrode exposed in the cell is exposed.
  • the surface of the counter electrode exposed in the cell has a ring shape that is concentric with the disk shape and has an inner diameter equal to or larger than the diameter of the disk shape.
  • a light transmitting portion is formed at the center.
  • a measurement solution containing an antigen sandwiched by using antibody-bound magnetic beads and a labeled antibody as objects to be measured is passed through the cell.
  • the object to be measured is magnetically attracted to the surface of the working electrode by a magnet.
  • a potential difference is applied between the working electrode and the counter electrode, and an electric current is passed through the measurement solution to cause an electrochemical reaction.
  • uniform electrochemical light emission can be generated over the entire surface of the working electrode.
  • the resulting electrochemiluminescence is formed into a ring shape. The light passes through the center of the formed counter electrode and is detected appropriately.
  • the magnet is formed in a cylindrical shape, and an N pole and an S pole are arranged in a direction of a center axis of the cylindrical body.
  • the counter electrode is formed in a cylindrical shape with a cross section of the ring shape and both ends are open, and the inner surface of the counter electrode is formed in a mirror surface. Then, the oblique light passing through the center of the counter electrode is reflected by the mirror surface, so that it is collected without being diffused, and efficient photometry can be performed.
  • Figure 1 illustrates the basic principle of a method for detecting an antigen using electrochemiluminescence.
  • Figure 2 illustrates the basic principle of the method for detecting antibodies using electrochemiluminescence.
  • Figure 3 is an explanatory view of the process of the detection method using electrochemiluminescence.
  • Figure 4 illustrates the principle of generation of electrochemiluminescence.
  • FIG. 5 is an explanatory diagram of an electrochemiluminescence detection device including a cell according to an embodiment of the present invention.
  • Figure 6 is an exploded view of the main unit.
  • Figure 7 is a cross-sectional view of the bottom surface of the main unit.
  • Figure 8 is a perspective view of the working electrode.
  • Figure 9 is a perspective view of the fixture.
  • Figure 10 is a perspective view of the magnet.
  • Figure 11 is a cross-sectional view of the top surface of the main body.
  • Figure 12 is a perspective view of the counter electrode.
  • Fig. 13 is an explanatory diagram of an embodiment in which a square magnet is placed with magnetic poles parallel to the flow direction of the measurement solution.
  • Fig. 14 is an explanatory diagram of an embodiment in which a square magnet is placed with its magnetic poles perpendicular to the flow direction of the measuring solution.
  • Figure 15 is an explanatory view of an embodiment in which a cylindrical magnet is placed with its magnetic poles perpendicular to the flow direction of the measuring solution.
  • Figure 16 is a graph showing the relationship between flow velocity and ECL emission intensity.
  • a cell 62 is provided inside a main body 61.
  • Fig. 6 shows an exploded view of the main body 61.
  • the main body 61 has a spacer 65 having a space (cell) 62 in the center in the shape of a leaf in a plan view, and a top surface of the cell 62 closely contacting the upper surface of the spacer 65. It has an upper surface 66 for closing and a bottom surface 67 for closely contacting the lower surface of the spacer 65 and closing the lower part of the cell 62.
  • connection ports 69a and 69b for flowing the measurement solution into the cell 62 are formed. Then, the spacer 65, the top surface 66, and the bottom surface 67 are overlapped. This constitutes cell 62.
  • the liquid feed pipe 68 and the drain pipe 70 are connected to the cell 62 through connection ports 67 a and 67 b formed in the bottom face 67, and the pump 71 is connected to the drain pipe 70. Is attached.
  • the pump 71 is composed of, for example, a tube pump. By operating the pump 71, the measurement liquid is introduced into the cell 62 from the liquid supply pipe 68, and the measurement liquid in the cell 62 is drained. Discharged from liquid pipe 70.
  • the measurement solution introduced into the cell 62 is the measurement solution prepared in the step (7) described above with reference to FIG. 3, ie, the antigen formed by sandwiching the antibody-bound magnetic beads 2 and the labeled antibody 3.
  • T is a measuring solution consisting of an electrolyte containing 1 As shown in FIG.
  • a hole 90 is formed in the bottom surface 67 of the cell 62 to insert the working electrode 72 from below. Is formed in a stopper portion 91 for pressing the pressure from above.
  • the working electrode 72 has a disk-shaped flange portion with a larger radius than the upper portion 72a below the upper portion 72a having a disk shape with a radius r. 2b is formed.
  • FIG. 9 shows a fixing device 92 for fixing the working electrode 72 to the bottom surface 67 of the cell 62.
  • the fixing device 92 is a hollow ring having a diameter just fitting into the hole 90. It has a shape. Then, as shown in Fig.
  • a working electrode 72 is inserted into the hole 90 from below, and a fixture 92 is further inserted and pressed under the working electrode 72, so that a disk d of diameter d is placed on the bottom surface 67 of the cell 62.
  • the upper surface of the working electrode 72 having a shape is exposed.
  • the working electrode 72 is made of a metal such as gold, platinum, and nickel, or a conductive material such as carbon.
  • the arm 73 rotates about the axis 76. When the arm 73 is raised, the magnet 75 comes close to the lower surface of the working electrode 72. When the arm 73 is lowered, the magnet 75 is turned to the working electrode 72. It is retracted from the lower recess 72b.
  • FIG. 10 shows a perspective view of the magnet 75.
  • the magnet 75 is formed in a cylindrical shape having a size that fits into a hole 90 formed in the bottom surface 67 of the cell 62.
  • An N-pole and an S-pole are arranged in the direction of the central axis 75 'of the magnet 75 constituting the cylinder.
  • the upper half of the cylinder is the S-pole and the lower half is the N-pole. I have.
  • the S pole of the magnet 75 can be brought closer to the lower surface of the working electrode 72.
  • the upper and lower end face peripheral edges of the magnet 75 having a cylindrical shape are both chamfered, and in the example shown in the figure, the upper and lower end face peripheral edges are all curved surfaces (round surfaces). It is formed in.
  • a counter electrode 77 is provided on the upper surface 66 of the cell 62.
  • the counter electrode 77 has a ring-shaped cross section and a cylindrical shape with both ends open.
  • the inner diameter of the counter electrode 77 is exposed on the bottom 67 of the cell 62. It is the same as or larger than the diameter d of the upper surface of the working electrode 72 having a disc shape.
  • the inner diameter of the counter electrode 77 is larger than the diameter d of the upper surface of the working electrode 72 by about 0.5 mm to 2.0 mm, preferably about 1.0 mm.
  • the width of the cell 62 is preferably larger than the inner diameter of the counter electrode 77 and smaller than the outer diameter. Further, since the inside of the counter electrode 77 is hollow, light can be transmitted.
  • the inner surface of the counter electrode 77 formed in a cylindrical shape is formed on a mirror surface 77a, and light transmitted through the counter electrode 77 is reflected by the mirror surface 77a. It is able to collect light.
  • This counter electrode 77 is also made of a conductive material like the working electrode 72.
  • the counter electrode 77 as described above is fitted and fixed from below into a recess 79 formed on the lower surface of the upper surface 66. Then, as shown in Fig. 5, a voltage is applied between the counter electrode 77 and the working electrode 72 by the power supply device 78, and a current of a predetermined current value flows through the measurement solution in the cell 62. As a result, the electrode reaction takes place. Then, when this electrode reaction is performed, electrochemiluminescence is generated on the surface of the working electrode 72 serving as the positive electrode. In addition, a control signal for controlling the voltage applied to the measurement solution in the cell 62 and the current value of the current flowing in the measurement solution is input to the power supply device 78.
  • the upper surface 66 of the cell 62 is made of a member that transmits light, such as acryl glass, and the electrochemiluminescence generated on the surface of the working electrode 72 is applied to the counter electrode 77 formed in the hollow. Transmitted upward through the interior. Above the upper surface 66, the electrochemiluminescence generated on the surface of the working electrode 72 due to the electrode reaction of the measuring solution is applied to the inside of the counter electrode 77 and the upper surface 66 of the cell 62.
  • a photomultiplier tube (PMT) 80 as a photodetector, which detects and converts it into an electrical signal, is placed in close proximity.
  • the spacers 65 and the bottom surface 67 which are the other members constituting the cell 62, may be made of acrylic or glass like the center of the upper surface 66. Since light transmission is not required for 5 and bottom surface 67, it may be made of a material that is not easily contaminated such as Teflon.
  • the entire body 61 is covered by a shielding means such as a box, and any light other than the light generated by the electrochemiluminescence in the cell 62 enters the photomultiplier tube 80 at all. It is configured so that there is no.
  • a cleaning solution (alkali solution) is introduced into the cell 62 prior to the measurement.
  • the introduction of the cleaning liquid is performed by operating the pump 71 with the tip of the liquid supply pipe 68 being charged into a container (not shown) or the like containing the cleaning liquid.
  • the inner surface of the cell 62 is cleaned, and the surface of the working electrode 72 provided on the bottom surface 67 of the cell 62 and the surface of the counter electrode 77 provided on the upper surface 66 of the cell 62 are removed. Is cleaned, and the subsequent electrode reaction is performed well.
  • the cleaning liquid in the cell 62 is first replaced with the electrolytic solution, the arm 73 is raised, and the magnet 75 is inserted below the working electrode 72. Then, the pump 71 is operated, and a certain amount of the measuring solution is introduced into the cell 62 together with the electrolytic solution.
  • the operation of the pump 7 1 causes the measurement liquid to flow along with the electrolyte from the liquid supply pipe 6 8 to the cell 6 2 and discharged from the drain pipe 70.
  • the measurement solution containing the antigen 1 flows continuously in the cell 62 together with the electrolytic solution
  • the antibody-bound magnetic beads 2 are adsorbed by the magnetic force of the magnet 75, so that the Is collected on the surface of the working electrode 72.
  • the operation of the pump 71 is stopped, and the introduction of the electrolytic solution is terminated.
  • the arm 73 descends, and the magnet 75 retreats from below the working electrode 72.
  • the inside of the cell 62 is filled with the electrolyte which is the measuring solution, and the antigen 1 contained in the predetermined amount of the measuring solution is collected on the surface of the working electrode 72.
  • a voltage is applied between the working electrode 72 and the counter electrode 77 by the power supply device 78, and a current having a predetermined current value based on the control signal flows through the measuring solution in the cell 62.
  • the electrode reaction starts.
  • the control of the voltage applied to the measuring solution in the cell 62 and the current flowing in the measuring solution is performed until the electric double film is formed on the entire surface of the working electrode 72 so that the ion annihilation reaction does not occur.
  • a low potential or low current After the electric double film is formed on the entire surface of the working electrode 72, a high potential or a high current enough to cause a rapid ion annihilation reaction is applied. By changing the potential or the low current in this way, control is performed to perform two-step electrochemiluminescence.
  • a controlled electrode reaction is performed by applying a predetermined potential or current to the measurement solution, and the reaction described above with reference to FIG. Electrochemiluminescence occurs near 72.
  • the light thus generated passes through the inside of the counter electrode 77 attached to the upper surface 66 of the cell 62, is detected by the photomultiplier 80, is converted into an electric signal, and is processed.
  • the inside of the counter electrode 77 is formed on the mirror surface 77a, the light passing through the inside of the counter electrode 77 is reflected and condensed by the mirror surface 77a, and is condensed by the photomultiplier tube 80. Light will enter efficiently.
  • the amount of light generated by electrochemiluminescence depends on the amount of antigen 1 in the test solution.
  • the cleaning liquid (alkaline solution) is introduced into the cell 62 again by the operation of the pump 71, and the cell 62 is cleaned. .
  • the magnet was attached to the electrochemiluminescence detector of Fig. 5 described above under the conditions of Figs. 13 to 15, and the amount of magnetic particles captured as Ru complex-labeled antibody-bound magnetic beads on the surface of the working electrode was measured. It was measured by ECL emission intensity. Then, in order to investigate the ability of magnetic adsorption, the operating amount of the pump was controlled to change the flow rate of the measured solution in the cell, and the relationship between the flow rate and the ECL emission intensity was examined.
  • Fig. 16 As a result, the relationship shown in Fig. 16 was obtained.
  • Fig. 13 when a square magnet is placed with its magnetic pole parallel to the flow direction of the measurement liquid, the flow rate of the measurement liquid is about 2. The maximum emission intensity was observed at 5 cmZsec, and the ECL emission intensity decreased at lower and higher flow rates.
  • Fig. 14 when a square magnet is placed with its magnetic pole perpendicular to the direction of flow of the measurement solution, the peak value of the light emission is obtained when the flow rate of the measurement solution is approximately 2.6 to 3.2 mm / sec. It was recognized that the emission intensity decreased at lower and higher flow rates.
  • Fig. 13 when a square magnet is placed with its magnetic pole parallel to the flow direction of the measurement liquid, the flow rate of the measurement liquid is about 2. The maximum emission intensity was observed at 5 cmZsec, and the ECL emission intensity decreased at lower and higher flow rates.
  • Fig. 14 when a square magnet is placed with its magnetic pole perpendicular to the direction of flow of the measurement solution, the
  • the ECL emission intensity is almost constant over a wide range of the measuring solution flow rate from about 2.2 to 4.2 mm / sec.
  • the emission intensity was measured to be 140 to 120% higher than in the cases of Figs. 13 and 14.
  • the use of a cylindrical magnet with a chamfered end face reduced the deposition of particles at the periphery of the working electrode surface. It was found that by using a columnar magnet chamfered in this way and by setting the magnetic field lines to the vertical direction, the magnetic particles can be accurately captured on the working electrode surface even when the flow rate of the measurement solution fluctuates.
  • a cylindrical magnet can capture magnetic particles more quickly and uniformly than a square magnet, but as long as a square electrode is used as the working electrode, an invalid electrode surface is exposed around the working electrode. It will be. Therefore, in the cell, a disk-shaped working electrode and a ring-shaped counter electrode, which is concentric with the working electrode and whose inner diameter is slightly larger than the working electrode, were arranged. The inner surface of the ring-shaped counter electrode was polished to a mirror surface so that it could reflect light. When an electrochemiluminescence detector configured as described above was created and actually measured, the luminescence was efficiently transmitted to the detector. In addition, when the inner surface of the opposing electrode was painted black to suppress reflection, and when the inner surface of the opposing electrode was polished to improve reflectivity, the detected emission intensity was improved 1.6 times. Industrial applicability
  • the surface of the working electrode exposed in the cell is formed in a disk shape, and the surface of the counter electrode is formed in a predetermined ring shape, whereby uniform electrochemiluminescence can be generated on the entire surface of the working electrode. become able to.
  • the light generated on the working electrode can be efficiently condensed, and highly accurate measurement can be performed.

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  • Physics & Mathematics (AREA)
  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Plasma & Fusion (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Biochemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • General Physics & Mathematics (AREA)
  • Immunology (AREA)
  • Pathology (AREA)
  • Investigating Or Analysing Materials By The Use Of Chemical Reactions (AREA)

Abstract

L'invention concerne une cellule de mesure de l'électrochimioluminescence, qui comporte une cellule permettant l'écoulement d'une solution objective, une électrode de travail et une contre-électrode mutuellement opposées dans la cellule selon un écartement prédéterminé, et un aimant permettant d'amener par attraction magnétique à la surface de l'électrode de travail un objet contenu dans la solution. La surface de l'électrode de travail exposée dans la cellule a la forme d'un disque, tandis que la surface de la contre-électrode exposée dans la cellule se présente comme un anneau concentrique par rapport au disque, et le diamètre intérieur de cet anneau est au moins égal au diamètre du disque. Il y a au centre de l'anneau une partie conçue pour assurer la transmission de la lumière.
PCT/JP1998/003807 1997-08-29 1998-08-27 Cellule de mesure de l'electrochimioluminescence WO1999012020A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP9/249346 1997-08-29
JP24934697A JP3366842B2 (ja) 1997-08-29 1997-08-29 電気化学発光測定用セル

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Publication Number Publication Date
WO1999012020A1 true WO1999012020A1 (fr) 1999-03-11

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102798630A (zh) * 2012-08-16 2012-11-28 中国科学院长春应用化学研究所 一种带有磁富集分离功能的电化学发光电解池
CN113030069A (zh) * 2021-02-01 2021-06-25 苏州易莱生物技术有限公司 用于电化学发光的检测设备的电场发生装置

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2014145619A1 (fr) * 2013-03-15 2014-09-18 Hycor Biomedical, Inc. Dispositif et procédés associés de réalisation de mesures de luminescence et de fluorescence d'un échantillon
CN105891525B (zh) * 2016-07-05 2018-08-21 深圳普门科技有限公司 全自动电化学发光免疫分析仪的检测装置
JP7291422B2 (ja) * 2019-02-27 2023-06-15 国立研究開発法人産業技術総合研究所 微小構造体、その作製方法およびそれを利用した分子検出方法

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JPH04363646A (ja) * 1991-09-10 1992-12-16 Tdk Corp 電気化学発光検出用容器
JPH04369477A (ja) * 1991-06-18 1992-12-22 Olympus Optical Co Ltd 免疫学的試験方法
JPH06509412A (ja) * 1991-02-06 1994-10-20 イゲン，インコーポレーテッド 改良されたルミネセンス検定の方法と装置
JPH07248330A (ja) * 1994-01-24 1995-09-26 Hitachi Ltd 磁性体粒子を利用した免疫分析のための方法及び装置
WO1997010498A1 (fr) * 1995-09-12 1997-03-20 Eisai Co., Ltd. Procede et appareil de detection d'electrochemiluminescence

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH06509412A (ja) * 1991-02-06 1994-10-20 イゲン，インコーポレーテッド 改良されたルミネセンス検定の方法と装置
JPH04369477A (ja) * 1991-06-18 1992-12-22 Olympus Optical Co Ltd 免疫学的試験方法
JPH04363646A (ja) * 1991-09-10 1992-12-16 Tdk Corp 電気化学発光検出用容器
JPH07248330A (ja) * 1994-01-24 1995-09-26 Hitachi Ltd 磁性体粒子を利用した免疫分析のための方法及び装置
WO1997010498A1 (fr) * 1995-09-12 1997-03-20 Eisai Co., Ltd. Procede et appareil de detection d'electrochemiluminescence

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102798630A (zh) * 2012-08-16 2012-11-28 中国科学院长春应用化学研究所 一种带有磁富集分离功能的电化学发光电解池
CN113030069A (zh) * 2021-02-01 2021-06-25 苏州易莱生物技术有限公司 用于电化学发光的检测设备的电场发生装置

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JPH1172437A (ja) 1999-03-16
JP3366842B2 (ja) 2003-01-14

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