CN216926677U - Electrochemical multi-electrode coplanar array microelectrode with micro electrolytic cell - Google Patents
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Abstract
The utility model provides an electrochemical multi-electrode coplanar array microelectrode with a miniature electrolytic cell, which comprises a plurality of coplanar miniature electrodes, a reference electrode and an auxiliary electrode, wherein the working electrode, the reference electrode and the auxiliary electrode are arranged on the coplanar miniature electrodes; the array microelectrode comprises a plurality of detection passages and can simultaneously detect different substances. The array microelectrode surface is provided with a miniature electrolytic cell, specifically, the dam-enclosing type miniature electrolytic cell is constructed on the microelectrode surface by adopting PCB (printed Circuit Board) ink and can be composed of one or more layers of ink, and the multiple layers of ink can be multiple layers of electrolytic cells with the same diameter or multiple layers of concentric circular electrolytic cells with gradually enlarged diameters from bottom to top.
Description
Technical Field
The utility model belongs to the field of electrochemical detection, and particularly relates to an electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell.
Background
The electrochemical sensor has attracted wide attention because of high detection speed and accurate numerical value, and can be used for on-site emergency detection, and the electrochemical sensor has been developed from pursuit of high sensitivity to highly integrated portable detection so far, but the existing electrochemical sensor still has the defects of difficult preparation, difficult application, poor stability and repeatability and the like. Meanwhile, the electrochemical sensor cannot be integrated into an integrated sensor of a microchip due to a complex preparation process, and thus cannot be applied to wider fields and scenes. Based on the above factors, the development of a micro-integrated electrochemical sensor has a necessary significance.
The electrochemical sensor for immediate detection has the characteristics of rapidness, convenience, cost saving and the like, is particularly characterized by instantly obtaining a detection result, reducing the cost of single detection, meeting the requirement of obtaining an accurate detection result in the shortest time and being gradually widely applied to the fields of biological medical treatment, environmental monitoring and the like.
The core detection element matched with the current instant detection electrochemical sensor mostly adopts a detection card and a detection strip as consumables, and based on the technical requirements of multi-parameter electrochemical detection, the processing technology of the detection element is complex and tedious, the cost is high, the batch production is not facilitated, the technology difficulty is high, and the application range is limited.
In order to solve the problems, the patent provides an electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell, which simplifies the processing technology, reduces the production cost, is beneficial to the batch production of similar products and is applied to the detection of micro liquid molecules such as blood, urine and the like.
SUMMERY OF THE UTILITY MODEL
In view of the above, the present invention provides an electrochemical multi-electrode coplanar array type micro-electrode having a micro-electrolytic cell.
The utility model aims to provide an electrochemical multi-electrode coplanar array microelectrode with a miniature electrolytic cell, wherein the array microelectrode comprises a plurality of coplanar miniature electrodes, and the miniature electrodes specifically comprise a working electrode, a reference electrode and an auxiliary electrode; the array microelectrode comprises a plurality of detection passages, and can simultaneously detect different substances.
Furthermore, in the array microelectrode, the distance between the working electrode and the auxiliary electrode is 0.1-1.5 mm; the distance between the reference electrode and the auxiliary electrode is 0.1-1.5 mm.
Furthermore, the working electrode, the auxiliary electrode and the reference electrode in the array microelectrode are respectively in regular patterns with consistent shapes, including square, round and oval.
The micro electrolytic cell is arranged in the array microelectrode area, a dam is constructed by specifically adopting PCB (printed Circuit Board) ink, a multi-layer structure can be constructed by coating multiple layers of ink, and the dam of the micro electrolytic cell is higher than an electrode plane, so that the surfaces of a working electrode, a reference electrode and an auxiliary electrode are protected from being scratched by external force. The micro electrolytic cell with the size gradually enlarged from bottom to top on the surface of the electrode is beneficial to quantitatively adding modification solution of the working electrode, including enzyme, solid electrolyte, gel electrolyte and the like.
The micro electrolytic cell structure can form a vortex structure on a micro area, is favorable for effective 'enrichment' of detected molecules in liquid, has a fixed area, and is favorable for quantitative analysis of trace liquid molecules.
Furthermore, a micro electrolytic cell is arranged on the surface of the array microelectrode, and particularly, a dam-shaped micro electrolytic cell is constructed on the surface of the microelectrode by adopting PCB (printed circuit board) ink.
Furthermore, the micro electrolytic cell is composed of one or more layers of printing ink, and the multiple layers of printing ink can be multiple layers of electrolytic cells with the same diameter or multiple layers of concentric circular electrolytic cells with gradually enlarged diameters from bottom to top.
Furthermore, the total thickness of the ink dam of the micro electrolytic cell is 10-1500 mu m.
Furthermore, the area of the micro electrolytic cell constructed on the surface of the same kind of electrode is fixed and is slightly higher than the electrode plane.
The electrochemical multi-electrode coplanar array microelectrode with the micro electrolytic cell further comprises an electrode substrate, a micro-fluidic cell and electrode pins, wherein the array microelectrode, the micro-fluidic cell and the electrode pins are arranged on the front surface of the electrode substrate, the array microelectrode is arranged in the micro-fluidic cell, the array microelectrode and the electrode pins are respectively connected through metal circuits on the surface of the electrode substrate in a conducting manner, and the number of the electrode pins is the same as that of the array microelectrode.
Further, the electrode pins are uniformly arranged at equal intervals, and the shapes of the electrode pins comprise a rectangle and a circle.
The array microelectrode and the electrode pins are arranged on the same plane, and the circuit for connecting and conducting the microelectrode and the electrode pins can be a metal circuit on the surface of the electrode substrate without adopting a wire embedding conduction mode in the substrate, so that the selection range of the electrode substrate material is expanded, and the processing cost and the process difficulty are greatly reduced.
Further, the electrode substrate can be ceramic, high polymer material and silicon substrate.
As shown in the attached figure 1, is a schematic diagram of an electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell. As shown in the figure, array microelectrodes and electrode pins are arranged on the front surface of the electrode substrate in a coplanar manner. The array microelectrode comprises a working electrode, an auxiliary electrode and a reference electrode, and specifically comprises seven working electrodes, one auxiliary electrode and seven reference electrodes, wherein the working electrode and the reference electrode are respectively arranged on two sides of the auxiliary electrode. Fifteen microelectrodes and electrode pins are respectively connected through metal circuits on the surface of the electrode substrate to form seven detection paths, and seven specific different substances can be detected in a targeted manner.
FIG. 2 is a schematic view of a microfluidic cell of an electrochemical multi-electrode coplanar array type microelectrode with a micro electrolytic cell. As shown in the figure, a microfluidic system is provided in the area of the microfluidic cell indicated by a dotted frame so that the liquid to be measured passes through all the microelectrodes in sequence.
FIG. 3 is a schematic front view of an electrochemical multi-electrode coplanar array type micro-electrode with a micro-electrolytic cell in example 2. As can be seen from the figure, the upper side of the front surface of the electrode substrate is provided with a circular micro-fluidic cell, and array micro-electrodes are distributed in the micro-fluidic cell and comprise four working electrodes, an auxiliary electrode and a reference electrode, and the working electrodes, the auxiliary electrode and the reference electrode are taken as an array unit. Specifically, a reference electrode with a rectangular unfilled corner is taken as a center, working electrodes are symmetrically distributed at four corners, and a circular auxiliary electrode is arranged on the outer side of the reference electrode. Four working electrodes in the array microelectrode share the auxiliary electrode and the reference electrode to respectively form four detection paths, and four specific different substances can be detected in a targeted manner.
FIG. 4 is a schematic back view of an electrochemical multi-electrode coplanar array type microelectrode with a micro electrolytic cell in example 2. As can be seen from the figure, the lower side of the back of the electrode substrate is provided with six strip-shaped rectangular electrode pins, the number of the pins is the same as that of the microelectrode on the front, and the array-type microelectrodes and the electrode pins are connected and conducted one by one through the metal circuit on the back of the electrode substrate.
FIG. 5 is a schematic cross-sectional view of a micro-electrolytic cell with array microelectrode surfaces. FIG. 5A is a single-layer micro electrolytic cell formed by modifying a single-layer humorous dam on the surface of an array microelectrode, FIG. 5B is a multi-layer micro electrolytic cell with a uniform diameter modified on the surface of the array microelectrode, and FIG. 5C is a concentric circular micro electrolytic cell with a plurality of layers with gradually enlarged diameters from bottom to top modified on the surface of the array microelectrode.
The utility model can arrange a micro-fluidic system in the micro-fluidic cell area, so that the liquid to be detected flows through all the microelectrodes through the sample inlet in sequence and is discharged through the sample outlet, thereby forming the sensing chip which has high multi-electrode integration and can simultaneously detect indexes of various substances.
The multiple electrodes integrated on the surface of the electrode substrate are integrated in an array mode, so that the micro-fluidic route and the detection circuit can be planned, the electrode distance can be reduced and fixed, and the detection result is more accurate and stable.
The utility model has the beneficial effects that:
(1) the array microelectrode and the electrode pins which are connected with the array microelectrode in a conducting way are arranged on the surface of the same electrode substrate in a coplanar way, so that the wire embedding processing in the electrode substrate is avoided, only a metal circuit needs to be processed on the surface of the substrate, the processing cost and the process difficulty are greatly reduced, the selection range of the electrode substrate is expanded, and the array microelectrode is suitable for special environments such as high temperature, high pressure and the like.
(2) The array microelectrode surface uses the ink to construct a multi-level micro electrolytic cell, and the ink dam which is slightly higher than the working electrode plane of the electrolytic cell is beneficial to forming a vortex structure on a micro area on the electrode surface when detecting the liquid to be detected, so that the molecules of the liquid to be detected are effectively enriched, the detection electric signal is enhanced, the detection sensitivity and accuracy are increased, the array microelectrode is convenient to protect, and the array microelectrode is prevented from being scratched by external force pollution; the area of the micro electrolytic cell is fixed, so that quantitative analysis of trace liquid molecule detection is facilitated; the multilayer micro electrolytic cell structure with gradually enlarged size from bottom to top is convenient for quantitatively adding modification solution of the working electrode, including enzyme, solid electrolyte, gel electrolyte and the like.
(3) The array microelectrode integrates the array microelectrode of the three-electrode system in the same area of the electrode substrate, fixes and shortens the distance of the three-electrode system, is favorable for stable signal transmission and improves the sensitivity and the stability of the microelectrode, and meanwhile, the array microelectrode is also convenient to process in design, is favorable for design and planning of a microfluidic system and regulates and controls the flow rate of sample injection liquid.
Drawings
The utility model is further described with the aid of the accompanying drawings, in which, however, the embodiments do not constitute any limitation to the utility model, and, to a person skilled in the art, other drawings can be derived from the following figures without inventive effort.
FIG. 1 is a schematic view of an electrochemical multi-electrode coplanar array type microelectrode having a micro electrolytic cell;
FIG. 2 is a schematic view of a micro fluidic cell having an electrochemical multi-electrode coplanar array type micro electrode of a micro electrolytic cell;
FIG. 3 is a schematic front view of an electrochemical multi-electrode coplanar array type micro-electrode having a micro-electrolytic cell in example 2;
FIG. 4 is a schematic back view of an electrochemical multi-electrode coplanar array type microelectrode having a micro electrolytic cell in example 2;
FIG. 5 is a schematic cross-sectional view of an array-type microelectrode surface micro-electrolytic cell.
Illustration of the drawings:
in fig. 1, a working electrode 1; B. a working electrode 2; C. a working electrode 3; D. a working electrode 4; E. a working electrode 5; F. a working electrode 6; G. a working electrode 7; H. a reference electrode 1; I. a reference electrode 2; J. a reference electrode 3; K. a reference electrode 4; l, reference electrode 5; m, a reference electrode 6; n, reference electrode 7; o, an auxiliary electrode.
In fig. 2, 1, electrode pin 1; 2. an electrode pin 2; 3. an electrode pin 3; 4. an electrode pin 4; 5. an electrode pin 5; 6. an electrode pin 6; 7. an electrode pin 7; 8. an electrode pin 8; 9. an electrode pin 9; 10. an electrode pin 10; 11. an electrode pin 11; 12. an electrode pin 12; 13. an electrode pin 13; 14. electrode pins 14; 15. and an electrode pin 15.
In fig. 3, a, the working electrode 1; B. a working electrode 2; C. a working electrode 3; D. a working electrode 4; E. a reference electrode; F. and an auxiliary electrode.
In fig. 4, 1, electrode pin 1; 2. an electrode pin 2; 3. an electrode pin 3; 4. an electrode pin 4; 5. an electrode pin 5; 6. and an electrode pin 6.
Detailed Description
In order that the objects, aspects and advantages of the present invention will become more apparent, the present invention will be further described in detail with reference to the following detailed description and the accompanying drawings.
The specific embodiment of the utility model comprises the following steps:
example 1
An electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell is disclosed, as shown in figure 1, an array microelectrode and an electrode pin are arranged on the front surface of an electrode substrate in a coplanar manner. The array microelectrode comprises working electrodes, auxiliary electrodes and reference electrodes, and specifically comprises seven working electrodes, one auxiliary electrode and seven reference electrodes, wherein the working electrodes and the reference electrodes are respectively arranged on two sides of the auxiliary electrodes, the auxiliary electrodes are single strip rectangular electrodes, the seven working electrodes are rectangular electrodes with the same shape and specification and are distributed on the upper sides of the auxiliary electrodes, and the seven reference electrodes are rectangular electrodes with the same shape and specification and are distributed on the lower sides of the auxiliary electrodes.
As shown in fig. 2, a microfluidic system is provided in the microfluidic area indicated by a dotted frame so that the liquid to be measured passes through all the microelectrodes in sequence.
The array microelectrode surface is constructed by PCB ink to form a dam, and the area of the micro electrolytic cell is fixed and slightly higher than the electrode plane, as shown in figure 5.
Fifteen microelectrodes and electrode pins are respectively connected through metal circuits on the surface of the electrode substrate to form seven detection paths, and seven specific different substances can be detected in a targeted manner.
In the embodiment, a ceramic substrate is selected as an electrode substrate, in the array microelectrode, a working electrode, a reference electrode and an auxiliary electrode are respectively and correspondingly conducted and connected with strip-shaped rectangular electrode pins on the same plane, seven working electrodes are rectangular microelectrodes with consistent shapes and areas, seven reference electrodes are rectangular microelectrodes with consistent shapes and areas, the auxiliary electrode is a strip-shaped microelectrode, fifteen microelectrodes are connected with the strip-shaped electrode pins uniformly distributed below the substrate through metal circuits processed on the surface of the ceramic substrate, fifteen circuits are not in staggered contact with each other, and the specific conditions are as follows:
TABLE 1 statistical table of array microelectrode and electrode pin conduction
| Serial number | Microelectrode | Electrode contact | Kind of electrode |
| 1 | |
15 | |
| 2 | |
14 | |
| 3 | |
13 | |
| 4 | |
12 | |
| 5 | |
11 | |
| 6 | |
10 | |
| 7 | |
9 | |
| 8 | |
1 | |
| 9 | I | 2 | |
| 10 | |
3 | |
| 11 | |
4 | |
| 12 | |
5 | |
| 13 | |
6 | |
| 14 | |
7 | |
| 15 | |
8 | Auxiliary electrode |
A micro electrolytic cell is arranged in an array microelectrode area on the front surface of an electrode substrate by using PCB (printed circuit board) ink, so that a solution to be detected flows through the surface of the array microelectrode in sequence, and the change of three-electrode electric signals is read by electrode pins, thereby realizing the detection of a specific target substance. A group of three electrodes can form a detection channel, and the specific conditions are as follows:
TABLE 2 statistical table of microelectrode integrated sensor chip detection path
Example 2
An electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell is disclosed, as shown in figure 3, a circular micro-fluidic cell is arranged on the upper side of the front face of an electrode substrate, and array microelectrodes are distributed in the micro-fluidic cell and comprise four working electrodes, an auxiliary electrode and a reference electrode, and the array microelectrodes are taken as an array unit. Specifically, a reference electrode with a rectangular unfilled corner is taken as a center, working electrodes are symmetrically distributed at four corners, and a circular auxiliary electrode (a black circular electrode in the attached figure 3) is arranged at the outer side of the reference electrode.
And a microfluidic system is arranged in the microfluidic area with a circular periphery, so that the liquid to be detected flows through all the microelectrodes in sequence.
As shown in fig. 4, the lower side of the back of the electrode substrate is provided with six long-strip rectangular electrode pins, the number of the pins is the same as that of the microelectrode on the front, and the array microelectrodes and the electrode pins are connected and conducted one by one through the metal circuit on the back of the electrode substrate.
The array microelectrode surface is constructed by PCB ink to form a dam, and the area of the micro electrolytic cell is fixed and slightly higher than the electrode plane, as shown in figure 5.
Four working electrodes in the array microelectrode share the auxiliary electrode and the reference electrode to respectively form four detection paths, and four specific different substances can be detected in a targeted manner.
In the array microelectrode, a working electrode A, B, C, D is respectively connected with electrode pins 1, 6, 2 and 5 in a conducting manner, a reference electrode E is connected with an electrode pin 3 in a conducting manner, an auxiliary electrode F is connected with an electrode pin 4 in a conducting manner, and internal circuits of an electrode substrate are not contacted with each other, and the specific conditions are as follows:
TABLE 3 statistical table of array microelectrode and electrode pin conduction
And arranging a micro-fluidic system in the micro-fluidic pool area on the front surface of the sensing chip, enabling the solution to be detected to flow through the surfaces of the array micro-electrodes in sequence, and reading the change of the three-electrode electric signals through electrode pins on the back surface of the sensing chip to realize the detection of the specific target substance. A group of three electrodes can form a detection channel, and the specific conditions are as follows:
TABLE 4 statistical table of microelectrode integrated sensor chip detection paths
| Detection path | Working electrode | Reference electrode | Auxiliary electrode |
| 1 | A | E | F |
| 2 | B | E | F |
| 3 | C | E | F |
| 4 | D | E | F |
It will be evident to those skilled in the art that the utility model is not limited to the details of the foregoing illustrative embodiments, and that the present invention may be embodied in other specific forms without departing from the spirit or essential attributes thereof. The present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the utility model being indicated by the appended claims rather than by the foregoing description, and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein.
Furthermore, it should be understood that although the present description refers to embodiments, not every embodiment may contain only a single technical solution, and such description is for clarity only, and those skilled in the art should take the description as a whole, and the technical solutions in the embodiments may be combined appropriately to form other embodiments that those skilled in the art can understand. The technical details not described in detail in the present invention can be implemented by any of the prior arts in the field. In particular, all technical features of the utility model which are not described in detail can be achieved by any prior art.
Claims (10)
1. An electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell, wherein the array microelectrode comprises a plurality of coplanar microelectrode, and the microelectrode specifically comprises a working electrode, a reference electrode and an auxiliary electrode; the array microelectrode comprises a plurality of detection paths, and can detect different substances simultaneously.
2. The electrochemical multi-electrode coplanar array microelectrode with a micro-electrolytic cell according to claim 1, wherein the distance between the working electrode and the auxiliary electrode in the array microelectrode is 0.1 to 1.5 mm; the distance between the reference electrode and the auxiliary electrode is 0.1-1.5 mm.
3. The electrochemical multi-electrode coplanar array microelectrode with a micro-electrolytic cell according to claim 1 or 2, wherein the working electrode, the auxiliary electrode and the reference electrode in the array microelectrode are respectively in regular patterns with consistent shapes, including square, round and oval.
4. An electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell according to any of the claims 1 to 3, characterized in that the array microelectrode is provided with a micro electrolytic cell on the surface, in particular a dam type micro electrolytic cell is constructed on the microelectrode surface by using PCB ink.
5. The electrochemical multi-electrode coplanar array microelectrode with the micro electrolytic cell of claim 4, wherein the micro electrolytic cell is composed of one or more layers of ink, the multiple layers of ink can be multiple layers of electrolytic cells with the same diameter, or multiple layers of concentric circular electrolytic cells with gradually enlarged diameters from bottom to top.
6. The electrochemical multi-electrode coplanar array microelectrode with the micro-electrolytic cell of claim 4, wherein the total thickness of the dam of the micro-electrolytic cell is 10 to 1500 μm.
7. The electrochemical multi-electrode coplanar array microelectrode with micro-electrolytic cell of claim 4, wherein the micro-electrolytic cell constructed on the surface of the same kind of electrode has a fixed area slightly higher than the electrode plane.
8. An electrochemical multi-electrode coplanar array microelectrode with a micro electrolytic cell as claimed in any of claims 1 to 7, wherein the array microelectrode further comprises an electrode substrate, a micro fluidic cell and electrode pins, the array microelectrode, the micro fluidic cell and the electrode pins are all arranged on the front surface of the electrode substrate, the array microelectrode is arranged in the micro fluidic cell, the array microelectrode and the electrode pins are respectively connected through metal lines on the surface of the electrode substrate, and the number of the electrode pins is the same as that of the array microelectrode.
9. The electrochemical multi-electrode coplanar array microelectrode with micro-electrolytic cell of claim 8, wherein the electrode pins are uniformly arranged at equal intervals and the shape comprises rectangle and circle.
10. The electrochemical multi-electrode coplanar array microelectrode with the micro-electrolytic cell as claimed in claim 8, wherein the electrode substrate is selected from the group consisting of ceramic, polymer, silicon.
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