An electrochemiluminescence detection device
By combining permanent magnets with magnetic microparticles, the problems of immobilization and dispersion of magnetic microparticles in electrochemiluminescence detection are solved, achieving efficient and stable detection signals and simplified operation, making it suitable for automated and integrated electrochemiluminescence detection devices.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Utility models(China)
- Current Assignee / Owner
- CHONGQING MEDICAL UNIVERSITY
- Filing Date
- 2025-06-05
- Publication Date
- 2026-07-24
AI Technical Summary
Existing electrochemiluminescence detection technologies based on magnetic particles suffer from problems such as magnetic particle immobilization, poor dispersion and stability, complex operation, and are not conducive to device miniaturization and automation.
By combining permanent magnets with magnetic microparticles, the magnetic microparticles are precisely fixed near the working electrode. Combined with a three-electrode electrochemiluminescence design, the operation process is simplified and the signal reproducibility is improved.
It achieves stable in-situ enrichment of magnetic particles, improves detection sensitivity and signal-to-noise ratio, simplifies operation procedures, and is suitable for automated and integrated applications.
Smart Images
Figure CN224553182U_ABST
Abstract
Description
Technical Field
[0001] This utility model relates to the field of electrochemical sensing technology, and in particular to an electrochemiluminescence detection device. Background Technology
[0002] Electrochemiluminescence (ECL) detection technology has become a crucial analytical tool in fields such as biomedical analysis, environmental monitoring, and food safety testing due to its combination of the high controllability of electrochemical excitation and the high sensitivity, wide linear range, and low background noise of chemiluminescence detection. In ECL detection, a three-electrode system (working electrode, reference electrode, and counter electrode) is typically used. Applying a specific potential triggers a chemical reaction on or near the electrode surface, generating excited-state substances. When these substances de-excite and return to their ground state, they release photons, thus achieving highly sensitive detection of the analyte.
[0003] In recent years, magnetic particles (MPs) have been widely used in ECL analytical systems to improve the selectivity and sensitivity of detection. Magnetic particles possess significant advantages such as large specific surface area, ease of surface functionalization (e.g., modification with antibodies, nucleic acid aptamers, and other recognition elements), and the ability to be manipulated by magnetic fields. Through magnetic field manipulation, magnetic particles can efficiently enrich and separate target analytes and carry them to the vicinity of the electrode surface for ECL reactions, greatly enhancing the signal response.
[0004] However, existing ECL detection technologies based on magnetic particles still face some key challenges and limitations in practical applications:
[0005] The problem of magnetic particle immobilization: Stably and uniformly immobilizing functionalized magnetic particles on a specific area of the electrode surface is crucial for obtaining a stable and reliable ECL signal. Traditional methods typically require enriching magnetic particles outside the detection cell (e.g., using a magnetic rack), and then transferring the enriched magnetic particles into the detection cell, or directly adsorbing them using an external magnet within the detection cell. The former is cumbersome and prone to loss or contamination; the latter makes it difficult to precisely control the position and coverage of magnetic particles on the electrode surface, and the placement of the external magnet may also interfere with the electrode system or optical path.
[0006] Dispersion and stability: During the detection process, magnetic particles are prone to sedimentation, aggregation or detachment from the electrode surface under the influence of gravity or solution disturbance, resulting in unstable ECL signals and poor reproducibility.
[0007] Ease of operation and integration: Relying on external magnets for operation is not conducive to the miniaturization, automation and integration of the detection device, and increases the complexity of operation.
[0008] Therefore, there is an urgent need to develop an integrated ECL detection device structure that can achieve in-situ, stable, controllable and efficient fixation of magnetic particles. Utility Model Content
[0009] In view of the shortcomings of the prior art described above, the purpose of this utility model is to provide an electrochemiluminescence detection device that can directly and accurately fix magnetic particles near the key reaction area of the working electrode, ensuring their stability during the detection process, while simplifying the operation process and improving the automation level and reproducibility of the signal.
[0010] The present invention adopts the following technical solution:
[0011] An electrochemiluminescence detection device includes an electrochemiluminescence generating module, a working electrode, a reference electrode, a counter electrode, a permanent magnet, magnetic particles, a transparent container, and a detector. The electrochemiluminescence generating module is connected to the working electrode, reference electrode, and counter electrode via wires. The working electrode, reference electrode, and counter electrode are all fixed to the upper end of the transparent container, with portions of each electrode disposed inside the transparent container. A liquid inlet is provided at the upper end of the transparent container. The permanent magnet is disposed inside the working electrode. The magnetic particles are adsorbed onto the bottom of the counter electrode by the permanent magnet. The detector is disposed on one side of the transparent container.
[0012] Preferably, the above-mentioned electrochemiluminescence detection device further includes a chemiluminescence detection dark box, the transparent container is disposed inside the chemiluminescence detection dark box, the chemiluminescence detection dark box is provided with a wiring hole, the electrochemiluminescence generating module is disposed outside the chemiluminescence detection dark box, and the working electrode, reference electrode and counter electrode are all sealed and connected to the electrochemiluminescence generating module through the wiring hole via a wire.
[0013] Preferably, in the above-mentioned electrochemiluminescence detection device, the lead ends of the working electrode, the reference electrode, and the counter electrode are respectively connected to one end of a wire via an electrode clamp, and the other end of the wire is connected to the electrochemiluminescence generating module.
[0014] Preferably, in the above-mentioned electrochemiluminescence detection device, the working electrode is a glassy carbon electrode.
[0015] Preferably, in the above-mentioned electrochemiluminescence detection device, the reference electrode is an Ag / AgCl electrode.
[0016] Preferably, in the above-mentioned electrochemiluminescence detection device, the working electrode is a magnetic glassy carbon electrode.
[0017] Preferably, in the above-mentioned electrochemiluminescence detection device, the counter electrode is a platinum wire electrode.
[0018] Preferably, in the above-mentioned electrochemiluminescence detection device, the magnetic microparticles include a plurality of magnetic beads, and the surface of each magnetic bead is covered with a sensing coating.
[0019] Preferably, in the above-mentioned electrochemiluminescence detection device, the working electrode includes an electrode body, the electrode body has a cavity inside, the side wall of the cavity has an insulating layer, and the permanent magnet is fixed inside the cavity.
[0020] Compared with the prior art, the beneficial effects of this utility model are as follows:
[0021] This invention achieves magnetic positioning through the combination of permanent magnets and magnetic microparticles, and, in conjunction with the three-electrode electrochemiluminescence design, realizes efficient enrichment, in-situ reaction, and high signal-to-noise ratio detection of target substances. Attached Figure Description
[0022] To more clearly illustrate the technical solutions in the embodiments of this utility model or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of this utility model. For those skilled in the art, other drawings can be obtained based on the structures shown in these drawings without creative effort.
[0023] Figure 1 This is a schematic diagram of an electrochemiluminescence detection device according to an embodiment of the present invention;
[0024] Figure 2 This is a structural diagram of an electrochemiluminescence detection device according to an embodiment of the present invention, when a chemiluminescence detection dark box is provided;
[0025] Figure 3 This is a schematic diagram of the structure of a support component in an electrochemiluminescence detection device according to an embodiment of the present invention;
[0026] Figure 4 This is a schematic diagram showing the connection between the electrochemiluminescence-electrophoresis analysis module and each electrode in an electrochemiluminescence detection device according to an embodiment of the present invention.
[0027] Figure label:
[0028] 1. Electrochemiluminescence generation module; 2. Working electrode; 201. Electrode body; 202. Chamber; 203. Insulating layer; 3. Reference electrode; 4. Counter electrode; 5. Permanent magnet; 6. Magnetic microparticles; 601. Magnetic bead; 602. Sensing coating; 7. Transparent container; 8. Liquid inlet; 9. Chemiluminescence detection dark box; 10. Wiring hole; 11. Wire; 12. Detector. Detailed Implementation
[0029] The following specific examples illustrate the implementation of this utility model. Those skilled in the art can easily understand other advantages and effects of this utility model from the content disclosed in this specification. This utility model can also be implemented or applied through other different specific embodiments, and various details in this specification can also be modified or changed based on different viewpoints and applications without departing from the spirit of this utility model. It should be noted that, unless otherwise specified, the following embodiments and features described therein can be combined with each other.
[0030] In the description of this utility model, unless otherwise stated, "a plurality of" means two or more; the terms "upper," "lower," "left," "right," "inner," "outer," "front end," "rear end," "head," "tail," etc., indicate the orientation or positional relationship based on the orientation or positional relationship shown in the accompanying drawings, and are only for the convenience of describing this utility model and simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation of this utility model. In addition, the terms "first," "second," "third," etc., are used for descriptive purposes only and should not be construed as indicating or implying relative importance.
[0031] In the description of this utility model, it should be noted that, unless otherwise explicitly specified and limited, the terms "connected" and "linked" should be interpreted broadly. For example, they can refer to a fixed connection, a detachable connection, or an integral connection; they can refer to a mechanical connection or an electrical connection; they can refer to a direct connection or an indirect connection through an intermediate medium. Those skilled in the art can understand the specific meaning of the above terms in this utility model according to the specific circumstances.
[0032] The present invention will now be further described with reference to the accompanying drawings.
[0033] This utility model provides an electrochemiluminescence detection device, such as... Figure 1 and Figure 2As shown, the electrochemiluminescence detection device includes an electrochemiluminescence generating module 1, a working electrode 2, a reference electrode 3, a counter electrode 4, a permanent magnet 5, magnetic particles 6, a transparent container 7, and a detector 12. The electrochemiluminescence generating module 1 is connected to the working electrode 2, the reference electrode 3, and the counter electrode 4 via wires. The working electrode 2, the reference electrode 3, and the counter electrode 4 are all fixed to the upper end of the transparent container 7, with portions of the working electrode 2, the reference electrode 3, and the counter electrode 4 disposed inside the transparent container 7. A liquid inlet 8 is provided at the upper end of the transparent container 7. The permanent magnet 5 is disposed inside the working electrode 2. The magnetic particles 6 are adsorbed onto the bottom of the counter electrode 4 by the permanent magnet 5. The detector 12 is disposed on one side of the transparent container 7.
[0034] A permanent magnet 5 is embedded inside the working electrode 2, generating a directional magnetic field. Magnetic microparticles 6 (typically modified with molecularly imprinted polymers or biological probes) are adsorbed and fixed to the bottom of the counter electrode 4 via the permanent magnet 5, achieving specific capture of the target analyte. In practice, the sample solution is injected into the transparent container 7 through the inlet 8, and the target analyte is enriched by the magnetic microparticles 6. The electrochemiluminescence generation module 1 applies a specific voltage to the working electrode 2, the reference electrode 3, and the counter electrode 4, forming a three-electrode system. A redox reaction occurs on the surface of the working electrode 2, generating an active intermediate. The active intermediate generated by the electrode reaction reacts with the co-reactants on the surface of the working electrode 2 to undergo a chemiluminescence reaction, releasing a light signal. The light signal can be captured by an external detector 12 (such as a photomultiplier tube) and converted into an electrical signal, the intensity of which is proportional to the concentration of the target analyte.
[0035] In this embodiment, the permanent magnet 5 is directly integrated into the working electrode 2, ensuring that the magnetic particles 6 are accurately adsorbed onto the bottom of the counter electrode 4, avoiding uneven dispersion. This simplifies the operation process, omits centrifugation / filtration steps, and improves enrichment efficiency. The magnetic particles 6 (such as MMIPs) selectively enrich the target analyte, significantly reducing matrix interference; the electrochemiluminescence signal is generated in situ with low background noise and a detection limit down to the atmolar level, thus achieving high-sensitivity detection. The working electrode 2, reference electrode 3, and counter electrode 4 are fixed to the upper end of the transparent container 7, forming a closed detection environment to avoid contamination; the liquid inlet 8 supports continuous sample injection or batch detection, adapting to automated analysis. The magnetic particles 6 are fixed by the permanent magnet 5, allowing for flexibility. While compatible with classic ECL systems (such as luminol / H2O2, ruthenium terpyridine / TPrA), they can be adapted to different recognition elements, enabling their application in pathogen / toxin / marker detection.
[0036] In some embodiments, such as Figure 2As shown, the electrochemiluminescence detection device also includes a chemiluminescence detection dark box 9, the transparent container 7 is disposed inside the chemiluminescence detection dark box 9, the chemiluminescence detection dark box 9 is provided with a wiring hole 10, the electrochemiluminescence generating module 1 is disposed outside the chemiluminescence detection dark box 9, and the working electrode 2, the reference electrode 3 and the counter electrode 4 are all sealed through the wiring hole 10 by a wire 11 and connected to the electrochemiluminescence generating module 1.
[0037] A transparent container 7 is placed inside the chemiluminescence detection dark chamber 9, forming a fully enclosed, light-proof environment that completely isolates external stray light interference. The chemiluminescence excited on the surface of the working electrode 2 is transmitted losslessly to the detector 12 within the dark chamber 9, ensuring an ultra-high signal-to-noise ratio. The detector 12 is located inside the chemiluminescence detection dark chamber 9, while the electrochemiluminescence generation module 1 is placed outside the dark chamber 9 to prevent its electronic components from generating heat / electromagnetic noise that could interfere with the light signal detection. The wire 11 passes through the sealed wiring hole 10 into the dark chamber 9, ensuring both electrical connection and maintaining the light-tightness of the dark chamber 9.
[0038] In some embodiments, such as Figure 1 As shown, the lead ends of the working electrode 2, the reference electrode 3 and the counter electrode 4 are respectively connected to one end of the wire 10 through the electrode clamp 12, and the other end of the wire 10 is connected to the electrochemiluminescence generating module 1.
[0039] The lead ends (metal conductors) at the top of the working electrode 2, reference electrode 3, and counter electrode 4 are held and fixed by electrode clamps 12; one end of the electrode clamp 12 is connected to the wire 10, and the other end of the wire 10 is connected to the electrochemiluminescence generating module 1, forming a low-impedance current path. The electrode clamp 12 can also be matched with the wiring hole 10 of the chemiluminescence detection dark box 9 to ensure that there is no light leakage when the wire 10 is inserted into the dark box.
[0040] In some embodiments, the working electrode 2 is a glassy carbon electrode or a magnetic glassy carbon electrode. The reference electrode 3 is an Ag / AgCl electrode. The counter electrode 4 is a platinum wire electrode.
[0041] It should be noted that the specific model limitations of the working electrode 2, reference electrode 3 and counter electrode 4 mentioned above are merely exemplary and do not constitute a limitation on this utility model.
[0042] In some embodiments, such as Figure 3 As shown, the magnetic microparticles 6 include a plurality of magnetic beads 601, and the surface of each magnetic bead 601 is covered with a sensing coating 602.
[0043] In this embodiment, the diameter of the magnetic bead 601 can be set to 50-500 nm, and it is attracted to the bottom of the counter electrode 4 in response to the magnetic field of the permanent magnet 5. The sensing coating 602 is a functional layer that uniformly coats the magnetic bead 601, and its thickness can be 10-100 nm. It contains specific recognition elements, such as molecularly imprinted polymers / antibodies / aptamers.
[0044] The sample is injected into the transparent container 7 through the inlet 8. The target molecule is captured by the recognition site of the sensing coating 602 (e.g., antigen-antibody binding / template molecule-imprinted hole matching). The permanent magnet 5 fixes the magnetic particles 6 to the bottom of the counter electrode 4 to prevent the target analyte from being lost due to the scouring of the mobile phase. The electrochemiluminescence generation module 1 applies a voltage to the working electrode 2, generating an active intermediate (e.g., Ru(bpy)33+) on the electrode surface. The active intermediate diffuses to the surface of the magnetic particles 6 and reacts with the target analyte-labeled signal molecules (e.g., enzyme catalytic product H2O2) captured on the sensing coating 602 to produce a luminescence reaction.
[0045] In some embodiments, such as Figure 4 As shown, the working electrode 2 includes an electrode body 201, a chamber 202 is provided inside the electrode body 201, an insulating layer 203 is provided on the side wall of the chamber 202, and the permanent magnet 5 is fixed inside the chamber 202.
[0046] The permanent magnet 5 is embedded in the chamber 202 of the electrode body 201, so that the source of the magnetic field coincides with the electrochemical reaction interface of the working electrode 2. An exemplary arrangement of the permanent magnet 5 is that its N-S pole axis is perpendicular to the electrode surface, forming a high-intensity gradient magnetic field (>0.3T) at the bottom of the electrode, precisely adsorbing the magnetic particles 6 to the active region of the electrode. The insulating layer 203 can be a polytetrafluoroethylene / alumina coating, covering the entire inner wall of the chamber 202 to achieve electrical, chemical, and thermal isolation. Electrical isolation blocks the current path between the permanent magnet 5 and the electrode body 201, preventing short circuits. Chemical isolation prevents electrolyte from seeping into the chamber 202, avoiding oxidation and dissolution of the permanent magnet 5 and contamination of the reaction system. Thermal isolation reduces the impact of heat generated by the electrochemical reaction on the magnetism of the permanent magnet 5. The permanent magnet 5 can be fixed to the center of the chamber 202 by epoxy resin potting, making it resistant to solution flow impacts and ensuring installation stability.
[0047] The above embodiments are only used to illustrate the technical solutions of this utility model, and are not intended to limit it. Although the utility model has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some or all of the technical features. Such modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of this utility model, and they should all be covered within the scope of the claims and specification of this utility model.
Claims
1. An electrochemiluminescence detection device, characterized in that, The device includes an electrochemiluminescence generating module, a working electrode, a reference electrode, a counter electrode, a permanent magnet, magnetic microparticles, a transparent container, and a detector. The electrochemiluminescence generating module is connected to the working electrode, reference electrode, and counter electrode via wires. The working electrode, reference electrode, and counter electrode are all fixed to the upper end of the transparent container, with portions of these electrodes disposed inside the transparent container. A liquid inlet is located at the upper end of the transparent container. The permanent magnet is disposed inside the working electrode. The magnetic microparticles are adsorbed onto the bottom of the counter electrode by the permanent magnet. The detector is disposed on one side of the transparent container.
2. The electrochemiluminescence detection device according to claim 1, characterized in that, It also includes a chemiluminescence detection dark box, the transparent container is disposed inside the chemiluminescence detection dark box, the chemiluminescence detection dark box is provided with a wiring hole, the electrochemiluminescence generating module is disposed outside the chemiluminescence detection dark box, and the working electrode, reference electrode and counter electrode are all sealed and connected to the electrochemiluminescence generating module through the wiring hole via a wire.
3. The electrochemiluminescence detection device according to claim 1, characterized in that, The leads of the working electrode, reference electrode, and counter electrode are each connected to one end of a wire via an electrode clamp, and the other end of the wire is connected to the electrochemiluminescence generation module.
4. The electrochemiluminescence detection device according to claim 1, characterized in that, The working electrode is a glassy carbon electrode.
5. The electrochemiluminescence detection device according to claim 1, characterized in that, The reference electrode is an Ag / AgCl electrode.
6. The electrochemiluminescence detection device according to claim 1, characterized in that, The working electrode is a magnetic glassy carbon electrode.
7. The electrochemiluminescence detection device according to claim 1, characterized in that, The counter electrode is a platinum wire electrode.
8. The electrochemiluminescence detection device according to claim 1, characterized in that, The magnetic microparticles include several magnetic beads, each of which has a sensing coating on its surface.
9. The electrochemiluminescence detection device according to claim 1, characterized in that, The working electrode includes an electrode body, an internal cavity is provided inside the electrode body, an insulating layer is provided on the side wall of the cavity, and the permanent magnet is fixed inside the cavity.