CN114384129A - Multi-channel electrochemical detection electrode and sensor - Google Patents
Multi-channel electrochemical detection electrode and sensor Download PDFInfo
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- CN114384129A CN114384129A CN202111653796.7A CN202111653796A CN114384129A CN 114384129 A CN114384129 A CN 114384129A CN 202111653796 A CN202111653796 A CN 202111653796A CN 114384129 A CN114384129 A CN 114384129A
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- G—PHYSICS
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- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/28—Electrolytic cell components
- G01N27/30—Electrodes, e.g. test electrodes; Half-cells
Abstract
The invention provides a multi-channel electrochemical detection electrode and a sensor, wherein the electrode comprises: a sensor substrate, and a working electrode, an auxiliary electrode, and a reference electrode disposed on the sensor substrate; the working electrodes are multiple, and each working electrode is used for collecting different physiological or biochemical signals and simultaneously outputting the collected signals or switching and selectively outputting the collected signals through a multi-channel switch; and each working electrode after switching selection and the reference electrode form a detection voltage loop, and the auxiliary electrode form a detection current loop. The electrode is designed by a multi-channel electrode, and a counter electrode and a reference electrode are multiplexed, so that the electrode has the advantages of simultaneous detection of multiple signals, electrode material saving and compact structure; after the device is combined with an external acquisition circuit, different working electrodes can be sequentially gated for detection, different electrochemical detection modes can be combined, the detection frequency and time can be set as required, and multi-index detection is realized.
Description
Technical Field
The invention relates to the field of sensors, in particular to a multi-channel electrochemical detection electrode and a sensor.
Background
The human health information includes physiological and biochemical information. Such information generally refers to signals detected from the body surface or body interior of a human to assist in clinical diagnosis of the human. The common physiological information comprises body temperature, blood pressure, myoelectric signals, electroencephalogram signals and electrocardiosignals, the biochemical information comprises blood sugar, blood fat, uric acid, lactic acid and the like, and the acquisition of the signals has important significance for monitoring the health condition of a human body. At present, the detection of physiological and biochemical signals of human bodies mostly depends on various sensors, and the core of the sensors lies in the design and modification of detection electrodes of the sensors. Physiological information and biochemical information are converted into electric signals, and then the electric signals are acquired by the acquisition circuit module and finally converted into values of corresponding signals, such as a temperature sensor, an electrocardio sensor, a blood glucose sensor, a lactic acid sensor and the like.
The sensors for collecting the human health information mainly have the following problems: at present, the sensors can only detect single signals, for example, blood sugar sensors and lactic acid sensors can only be singly applied to the detection of blood sugar and lactic acid, and when the sensors are required to detect various signals of a human body, the sensors can only be simply combined, so that the sensors have various devices, large occupied space and complex acquisition circuits. When there is a greater need to detect body signals, such as monitoring of intensive care unit patients, it is more inconvenient.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a multi-channel electrochemical detection electrode and a sensor.
The invention provides a multi-channel electrochemical detection electrode, which comprises: a sensor substrate, and a working electrode, an auxiliary electrode, and a reference electrode disposed on the sensor substrate; the working electrodes share the same pair of reference electrode and auxiliary electrode, and each working electrode is used for collecting different physiological or biochemical signals and simultaneously outputting the collected signals or switching and selectively outputting the collected signals through a multi-channel switch; and simultaneously outputting each working electrode of the acquired signal, or switching each selected working electrode to form a detection voltage loop together with the same reference electrode and form a detection current loop together with the same auxiliary electrode.
According to the multi-channel electrochemical detection electrode provided by one embodiment of the invention, the working electrodes respectively modify biological materials participating in different bioelectrochemical reactions so as to collect corresponding physiological or biochemical signals.
According to the multi-channel electrochemical detection electrode provided by one embodiment of the invention, the biological material comprises a biological active substance capable of catalyzing biochemical reaction or a material with biological recognition function, the biological active substance comprises an enzyme, and the material with biological recognition function comprises an antibody, an antibacterial peptide, an aptamer, an ion selective membrane, a molecular imprinting membrane or a high polymer membrane.
According to the multi-channel electrochemical detection electrode disclosed by the embodiment of the invention, the material structure of each electrode comprises a platinum electrode, a gold electrode or a carbon-based electrode.
According to the multi-channel electrochemical detection electrode provided by one embodiment of the invention, the sensor substrate material comprises silicon wafers, silica gel, glass, polydimethylsiloxane or polyethylene terephthalate.
The invention also provides a multi-channel electrochemical detection sensor, which comprises any one of the multi-channel electrochemical detection electrode and a program-controlled switch; and the working electrode is switched and selected through the program control switch.
A multi-channel electrochemical detection sensor according to one embodiment of the present invention, the sensor further comprising an operational amplifier module; each working electrode is connected to the operational amplifier module through different channels of the program-controlled switch respectively, and the different channels are switched through a switching element of the program-controlled switch; the auxiliary electrode and the reference electrode are both connected to the operational amplifier module; each working electrode and the detection current loop formed by the auxiliary electrode output the amplified detection signal through the operational amplifier module.
According to one embodiment of the invention, the multi-channel electrochemical detection sensor further comprises a filtering module for filtering the detection current signal.
According to one embodiment of the invention, the multi-channel electrochemical detection sensor further comprises a rectification module for rectifying the filtered detection current signal.
According to the multi-channel electrochemical detection sensor provided by the embodiment of the invention, the detection current signal of each working electrode shares the filtering module and the rectifying module.
The multi-channel electrochemical detection electrode and the sensor provided by the invention have the advantages that the multi-channel electrode is designed, the counter electrode and the reference electrode are multiplexed, and the multi-channel electrochemical detection electrode and the sensor have the advantages of simultaneous detection of multiple signals, electrode material saving and compact structure; after the device is combined with an external acquisition circuit, different working electrodes can be sequentially gated for detection, different electrochemical detection modes can be combined, the detection frequency and time can be set as required, and multi-index detection is realized.
Drawings
In order to more clearly illustrate the technical solutions of the present invention or the prior art, the drawings needed for the description of the embodiments or the prior art will be briefly described below, and it is obvious that the drawings in the following description are some embodiments of the present invention, and those skilled in the art can also obtain other drawings according to the drawings without creative efforts.
FIG. 1 is a schematic structural diagram of a multi-channel electrochemical detection electrode provided by the present invention;
FIG. 2 is a second schematic structural diagram of a multi-channel electrochemical detection electrode provided by the present invention;
FIG. 3 is a schematic diagram of a multi-channel electrochemical detection sensor according to the present invention;
FIG. 4 is a second schematic diagram of the multi-channel electrochemical detection sensor according to the present invention;
FIG. 5 is a schematic diagram of the results of glucose assays provided by the present invention;
FIG. 6 is a schematic diagram of the results of the lactic acid assay provided herein;
in the figure: 1. a sensor substrate; 2. a working electrode; 3. an auxiliary electrode; 4. a reference electrode.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention clearer, the technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings, and it is obvious that the described embodiments are some, but not all embodiments of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The invention provides a multi-channel electrochemical detection electrode and a sensor based on electrode multiplexing, which can be used for simultaneously detecting multiple indexes of a patient. The invention realizes the simultaneous detection of various information of human body by designing the multi-channel electrode, structurally multiplexing the counter electrode and the reference electrode and adopting a time-sharing acquisition mode in circuit acquisition. The multi-channel sensor is more compact, saves electrodes, and can make the human health signal detection device more miniaturized and convenient by matching with a multi-channel acquisition and processing circuit, thereby meeting the requirement of multi-channel detection on health indexes of wearers.
The multi-channel electrochemical detection sensor and apparatus of the present invention are described below with reference to fig. 1-6. Fig. 1 is a schematic structural diagram of a multi-channel electrochemical detection electrode provided by the present invention, and as shown in fig. 1, the present invention provides a multi-channel electrochemical detection electrode, including: a sensor substrate 1, and a working electrode 2, an auxiliary electrode 3 and a reference electrode 4 disposed on the sensor substrate 1; the number of the working electrodes 2 is multiple, each working electrode 2 is used for collecting different physiological or biochemical signals, and a pair of reference electrodes and auxiliary electrodes are shared, and the collected signals are output simultaneously or switched and selectively output through a multi-channel switch; each working electrode which simultaneously outputs the collected signal or each working electrode 2 after switching selection forms a detection voltage loop together with the same reference electrode 4 and forms a detection current loop together with the same auxiliary electrode 3.
The situation of two working electrodes is shown in figure 1, the invention designs the multi-channel electrode, structurally multiplexes the counter electrode and the reference electrode through a plurality of working electrodes, adopts a time-sharing acquisition mode in circuit acquisition, can switch and select different working electrodes through a multi-channel switch to realize the simultaneous detection of various information of a human body, and can also output multi-channel acquisition signals simultaneously.
When it is used for biochemical information collection, the arrangement of the multiple electrodes can also be an auxiliary electrode and multiple reference electrodes and multiple working electrodes. When multi-class biochemical information is collected, the functions and detection objects of all the working electrodes are different, and the function of each working electrode depends on chemical modification of the working electrode. According to different chemical modifications, the detection of various physiological or biochemical indexes such as metabolites, proteins, nucleic acids, hormones, exosomes and viruses can be completed.
The detection electrode processing method can be a micro-processing technology, a screen printing technology or a 3D printing technology.
The number of the working electrodes may be two or more according to the detection requirement. Each working electrode detects different physiological signals, biochemical signals and physiological and biochemical signals simultaneously according to the detection requirement. Namely, the number of working electrodes is increased according to detection index data, and the detection of multiple paths of human body signals is realized.
And the auxiliary electrode and the working electrode form a current measuring loop. The auxiliary electrode is an electrode which has low resistance and is not easy to polarize.
And a reference electrode as a reference for measuring the relative potential of its working electrode.
The electrochemical signals can be collected by selecting a proper mode according to different physiological or biochemical signals collected by the working electrode, such as Cyclic Voltammetry (CV), Differential Pulse Voltammetry (DPV), wave voltammetry (SWV), chronoamperometry (I-t), and the like.
When the multi-channel electrochemical detection electrode is used, different sample collection modes and sample introduction modes can be adopted according to in-vitro detection or in-vivo detection. The acquisition circuit can amplify the acquisition module of the working electrode as required, sequentially measure the signal of each channel working electrode during detection, and flexibly set the detection frequency and duration as required. Fig. 2 is a second schematic structural diagram of the multi-channel electrochemical detection electrode provided by the present invention, and as shown in fig. 2, the electrode is similar to fig. 1, except for the position of the reference electrode design.
The multi-channel electrochemical detection electrode provided by the invention has the advantages that the multi-channel electrode is designed, the counter electrode and the reference electrode are multiplexed, and the multi-channel electrochemical detection electrode can be used for simultaneously detecting multi-channel signals, saving electrode materials and having a compact structure; after the device is combined with an external acquisition circuit, different working electrodes can be gated in sequence for detection, various different electrochemical detection modes (such as CV, DPV, SWV, I-t and the like) can be realized, and the detection frequency and time length can be set as required, so that multi-index detection is realized.
In one embodiment, the working electrodes respectively modify biological materials participating in different bioelectrochemical reactions to collect corresponding physiological or biochemical signals.
For example, the number of the working electrodes is two, one working electrode is modified with a biomaterial for detecting glucose, and the other working electrode is modified with a biomaterial for detecting lactate. And then, according to the requirements of glucose and lactic acid detection in different periods, switching through a multi-channel switch to select the corresponding working electrode and output the corresponding biochemical signal.
According to the multi-channel electrochemical detection electrode, each working electrode is respectively modified with biological materials participating in different bioelectrochemical reactions so as to collect corresponding physiological or biochemical signals, the simultaneous detection of multiple information of a human body can be realized by adopting a time-sharing method in signal collection, and the problems of multiple sensor devices and large occupied space during detection of multiple signals can be solved when multiple signals of the human body are detected.
In one embodiment, the biomaterial comprises a bioactive substance capable of catalyzing a biochemical reaction or a material having a biological recognition function, the bioactive substance comprises an enzyme, and the material having a biological recognition function comprises an antibody, an antimicrobial peptide, an aptamer, an ion selective membrane, a molecularly imprinted membrane, or a high polymer membrane.
The sensing function of different targets is realized by modifying different materials on the surface of each working electrode, such as modifying different enzymes, modifying antibodies or aptamers (such as nucleic acid aptamers) aiming at different targets, or modifying different high molecular materials and the like. And during specific detection, switching is carried out according to the multi-way switch, and the selected working electrode is switched to output a corresponding signal.
In one embodiment, the material of each electrode may be a platinum, gold, or carbon-based electrode. Specifically, the working electrode, the reference electrode and the auxiliary electrode of the multi-channel electrode designed by the invention can be made of conductive materials such as platinum, gold or carbon-based electrodes.
In one embodiment, the sensor substrate material includes silicon wafer, glass, silica gel, Polydimethylsiloxane (PDMS), or polyethylene terephthalate (PET), i.e., the material used for the sensor substrate has various choices, determined according to specific requirements.
The invention also provides a multi-channel electrochemical detection sensor, which comprises a program-controlled switch and the multi-channel electrochemical detection electrode of any one of the embodiments; and the working electrode is switched and selected through the program control switch.
Specifically, the working electrodes are gated through the multi-path program control switches respectively, so that signals can be detected in sequence for the working electrodes of all channels of the sensor during signal acquisition, and the program control switches are automatically switched, so that synchronous detection of various kinds of information of a human body can be realized.
In one embodiment, the sensor further comprises an operational amplifier module; each working electrode is connected to the operational amplifier module through different channels of the program-controlled switch respectively, and the different channels are switched through a switching element of the program-controlled switch; the auxiliary electrode and the reference electrode are both connected to the operational amplifier module; each working electrode and the detection current loop formed by the auxiliary electrode output the amplified detection current signal through the operational amplifier module.
Fig. 3 is a schematic structural diagram of the multi-channel electrochemical detection sensor provided by the present invention, and as shown in fig. 3, a working electrode 1(WE1) and a working electrode 2(WE2) are switched by a programmable switch, and one working electrode is gated at each time and then connected to an operational amplifier module. An auxiliary electrode (CE) and a Reference Electrode (RE) are also connected to the operational amplifier module. And the detection current signal between the auxiliary electrode and the working electrode 1 or the working electrode 2 is output through the operational amplifier module. The operational amplifier module provides voltage through a signal source. The operational amplifier module can be formed by combining a plurality of devices such as resistors and the like through one or more operational amplifiers according to specific requirements.
According to the multi-channel electrochemical detection sensor, the operational amplifier module can amplify output detection signals to facilitate detection, the operational amplifier module can be shared, and the electrochemical detection sensor is compact in structure on the whole.
In one embodiment, the sensor further comprises a filtering module for filtering the sensed current signal. For the output signal of the operational amplifier module, a filtering module can be arranged for filtering, so that noise interference is eliminated, and the accuracy of the detection signal is improved.
In one embodiment, the sensor further comprises a rectification module for rectifying the filtered sensed current signal. Correspondingly, the embodiment of the invention rectifies the filtered detection signal through the rectifying module, and the output signal which tends to be direct current is favorable for the measurement of an instrument.
In one embodiment, the detected current signal of each working electrode shares the filtering module and the rectifying module.
Fig. 4 is a second schematic structural diagram of the multi-channel electrochemical detection sensor provided by the present invention, and as shown in fig. 4, the embodiment of the present invention shares the filtering module and the rectifying module, so that output signals of a plurality of working electrodes can be prevented from occupying a plurality of filtering modules and rectifying modules, and the structure of the multi-channel electrochemical detection sensor is more compact.
The multi-channel electrochemical sensor has a compact integral structure, is easy to integrate and package, can be integrated in wearable equipment, implantable equipment and bedside diagnostic equipment, is convenient for home detection of a user, and can be used for chronic disease management and health monitoring.
Fig. 5 is a schematic diagram of a glucose detection result provided by the present invention, fig. 6 is a schematic diagram of a lactic acid detection result provided by the present invention, and as shown in fig. 5 and fig. 6, a fitting curve in the diagrams is obtained by fitting the measured magnitude of the current signal and the concentration of the corresponding analyte in advance. In the detection process, the corresponding glucose concentration can be detected through the current signal 1 output by the working electrode 1, when the lactic acid concentration needs to be detected, the switch is used for switching, and the corresponding lactic acid concentration can be detected through the current signal 2 output by the working electrode 2.
The above-described embodiments are merely illustrative, and the units described as separate parts may or may not be physically separate, and the parts described as units may or may not be physical units, may be located in one place, or may be distributed on a plurality of units. Some or all of the modules may be selected according to actual needs to achieve the purpose of the solution of the present embodiment. One of ordinary skill in the art can understand and implement it without inventive effort.
Finally, it should be noted that: the above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention.
Claims (10)
1. A multi-channel electrochemical detection electrode, comprising:
a sensor substrate, and a working electrode, an auxiliary electrode, and a reference electrode disposed on the sensor substrate;
the working electrodes are multiple, and each working electrode is used for collecting different physiological or biochemical signals and simultaneously outputting the collected signals or switching and selectively outputting the collected signals through a multi-channel switch;
a plurality of working electrodes sharing a pair of auxiliary electrodes and reference electrodes;
and simultaneously outputting each working electrode of the acquired signal, or switching each selected working electrode to form a detection voltage loop together with the same reference electrode and form a detection current loop together with the same auxiliary electrode.
2. The multi-channel electrochemical detection electrode of claim 1, wherein the working electrodes respectively modify biological materials participating in different bioelectrochemical reactions to collect corresponding physiological or biochemical signals.
3. The multi-channel electrochemical detection electrode according to claim 2, wherein the biological material comprises a bioactive substance capable of catalyzing biochemical reactions or a material having a biological recognition function, the bioactive substance comprises an enzyme, and the material having a biological recognition function comprises an antibody, an antimicrobial peptide, an aptamer, an ion selective membrane, a molecular imprinting membrane or a high polymer membrane.
4. The multi-channel electrochemical detection electrode of claim 1, wherein the material structure of each electrode comprises a platinum electrode, a gold electrode, or a carbon-based electrode.
5. The multi-channel electrochemical detection electrode of claim 1, wherein the sensor substrate material comprises silicon wafer, glass, silica gel, polydimethylsiloxane, or polyethylene terephthalate.
6. A multi-channel electrochemical detection sensor comprising a programmable switch and a multi-channel electrochemical detection electrode according to any one of claims 1-5;
and the working electrode is switched and selected through the program control switch.
7. The multi-channel electrochemical detection sensor of claim 6, wherein the sensor further comprises an operational amplifier module;
each working electrode is connected to the operational amplifier module through different channels of the program-controlled switch respectively, and the different channels are switched through a switching element of the program-controlled switch;
the auxiliary electrode and the reference electrode are both connected to the operational amplifier module;
each working electrode and the detection current loop formed by the auxiliary electrode output the amplified detection current signal through the operational amplifier module.
8. The multi-channel electrochemical test sensor of claim 7, further comprising a filtering module for filtering the test current signal.
9. The multi-channel electrochemical test sensor of claim 8, further comprising a rectification module for rectifying the filtered test current signal.
10. The multi-channel electrochemical detection sensor of claim 9, wherein the filtering module and the rectifying module are shared by the detection current signal of each working electrode.
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