CN115479982A - Multi-channel chemical impedance sensor and manufacturing and using methods thereof - Google Patents
Multi-channel chemical impedance sensor and manufacturing and using methods thereof Download PDFInfo
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Abstract
The invention relates to a multi-channel chemical impedance sensor and a manufacturing and using method thereof, and the multi-channel chemical impedance sensor specifically comprises an upper sealing layer front side, a filtering interface layer front side, an electrode layer back side, a lead layer front side and a lower sealing layer which are superposed from top to bottom; the upper sealing layer is an antifouling layer on the surface of the sample introduction channel, the filtering interface layer adopts cellulose filter paper as a substrate, hydrophobic ink is used as a surface layer of the front surface and the back surface, the sample introduction port on one side adopts a wedge-shaped structure and is communicated with the circular sample cell through a corresponding hydrophilic drainage pipeline, and the electrode leads which are arranged in parallel are arranged on the other side and are respectively connected to the corresponding electrode leads on the back surface through holes; the front surface of the electrode layer comprises a plurality of channel working electrodes and a pair of reference and counter electrodes, the working electrodes are distributed around the sample cell at intervals, and lead-out end lines of conductive ink are adopted and connected to the sample cell area through corresponding drainage channels; and the reference electrode and the counter electrode are silk-screened in the sample cell area, and the reference electrode lead and the counter electrode lead are connected to the reverse side lead through corresponding through holes.
Description
Technical Field
The invention relates to the technical field of electrochemical biosensors, in particular to a multi-channel chemical impedance sensor and a manufacturing and using method thereof.
Background
Environmental pollution brings huge risks to food safety, and environmental hormone residue detection has great significance for guaranteeing environmental safety. The traditional method for detecting the environmental hormones comprises a gas chromatography, a high performance liquid chromatography, a liquid chromatography-mass spectrometry combined method and the like, and the detection methods are complex in sample pretreatment procedure, complex in detection steps, large, heavy and expensive detection equipment is required, and the requirement for quickly detecting the environmental hormones is difficult to meet.
The electrochemical analysis method has the advantages of high detection speed, high detection sensitivity and the like, and is widely applied to the aspect of rapid detection of environmental hormones. The electrochemical impedance detection method is characterized in that an electrochemical workstation is utilized to apply sine-changed disturbance potential signals to the electrode ends of the electrochemical impedance sensorE And then measuring the current responsei And (4) changing. The small-sized integrated electrochemical sensor constructed by combining the screen printing technology and the electrochemical analysis method becomes a research hotspot.
Disclosure of Invention
Based on the technical problems mentioned in the background art, the invention provides a multi-channel electrochemical impedance sensor, which comprises an upper sealing layer front surface, a filtering interface layer front surface, an electrode layer back surface, a lead layer front surface and a lower sealing layer which are stacked in sequence; the upper sealing layer is an antifouling layer on the surface of the sample feeding channel, and the front surface of the upper sealing layer is a plastic sealing layer made of polyethylene glycol terephthalate material; the filter interface layer adopts cellulose filter paper as a substrate, hydrophobic ink as front and back surface layers, a sample inlet on one side adopts a wedge-shaped structure, the filter interface layer is communicated with the circular sample cell through corresponding hydrophilic drainage pipelines, electrode leads arranged in parallel are arranged on the other side of the filter interface layer, and the filter interface layer is respectively connected with the corresponding electrode leads on the back side through corresponding through holes; the electrode layer adopts cellulose filter paper as a substrate, the front side of the electrode layer comprises a multi-channel working electrode, a pair of reference electrodes and a counter electrode, the working electrodes are distributed around the sample cell at intervals, and lead-out end lines of conductive ink are adopted and connected to the sample cell area through corresponding drainage channels; the reference electrode and the counter electrode are printed in the sample cell area in a silk screen mode, and the reference electrode lead and the counter electrode lead are connected to the reverse side lead through corresponding through holes; the lead layer is made of PET (polyethylene terephthalate), the PET is used for connecting the multi-channel working electrode of the electrode layer to the multi-channel rotary switch through a conductive ink contact lead by leading out, and the multi-channel working electrode is connected with the working electrode lead of the filtering interface layer; the lower sealing layer is made of PET materials, and the multi-path rotary switch penetrates through the corresponding through hole in the lower sealing layer.
The method for manufacturing the multi-channel electrochemical impedance sensor comprises the steps of designing five structural layers of the multi-channel electrochemical impedance sensor in the claim 1, and respectively printing conductive ink and hydrophobic ink on cellulose filter paper and a PET (polyethylene terephthalate) substrate by utilizing a screen printing technology to form a filtering interface layer, an electrode layer and a lead layer; synthesizing a carbon-based nano composite material by the carbon-based nano material and the nano metal material; modifying the carbon-based nano composite material to the working surface of the electrochemical impedance sensor, and electropolymerizing the electroactive substance to the surface of the carbon-based nano composite material; then fixing the antibody on the surface of the electrochemical impedance sensor, and dropwise adding bovine serum albumin to seal the non-detection active site; finally, the whole surface of the working electrode is sealed integrally by using the film forming effect of chitosan; the five-layer structure is stacked in sequence, and the five-layer structure is pressed together by a hot melting method to form the complete electrochemical impedance sensor.
The electrochemical impedance sensor has the advantages that the electrochemical impedance sensor is simple in structure, high in detection sensitivity, low in price and capable of being manufactured in batches through the five-layer structural design, rapid and high-sensitivity detection of different types of environmental hormones can be achieved, the speed is improved, and the cost is saved.
Drawings
FIG. 1 is a schematic diagram of the overall structure of a multi-channel electrochemical impedance sensor;
FIG. 2 is a schematic diagram of a front side layered structure of a multi-channel electrochemical impedance sensor;
FIG. 3 is a schematic diagram of a reverse layered structure of a multi-channel electrochemical impedance sensor;
FIG. 4 is a schematic diagram of a carbon-based nanocomposite synthesis process;
1: sealing the layer; 2: a filter interface layer; 3: an electrode layer; 4: a wiring layer; 5: a lower sealing layer;
19-1: a reference electrode conductive ink lead on the front side of the filtering interface layer;
20-1: a reference electrode conductive ink lead on the reverse side of the filtering interface layer;
19-2: a working electrode conductive ink lead on the front surface of the filtering interface layer;
20-2: a working electrode conductive ink lead on the back side of the filtering interface layer;
19-3: the front surface of the filtering interface layer is opposite to the electrode conductive ink lead;
20-3: the reverse side of the filtering interface layer is opposite to the electrode conductive ink lead;
19-4: a reference electrode metal lead on the front side of the electrode layer;
20-4: a reference electrode conductive ink lead on the back of the electrode layer;
21: a hollowed-out area;
19-5: the front surface of the electrode layer is opposite to the electrode metal lead;
20-5: the reverse side of the electrode layer is opposite to the electrode conductive ink lead;
7: a lead layer working electrode conductive ink lead;
8: a multi-way rotary switch;
18-1: a reference electrode lead through hole of the filtering and interface layer;
18-2: a working electrode lead through hole of the filtering and interface layer;
18-3: the filtering and interface layer is opposite to the electrode lead through hole;
18-4: an electrode layer reference electrode lead through hole;
18-5: an electrode layer to electrode lead through hole;
18-6: a lower seal layer through hole;
6: a plastic packaging layer; 9: a wedge-shaped sample inlet; 10: a sample drainage conduit; 11: a sample cell; 12: hydrophobic ink; 13: a working electrode; 14: reference and counter electrodes; 15: a conductive ink lead; 16: an electrode layer drainage channel; 17: an electrode layer sample cell region;
1-1: the front surface of the upper sealing layer; 1-2: the back side of the upper sealing layer; 2-1: the front surface of the filtering interface layer; 2-2: filtering the reverse side of the interface layer; 3-1: the front surface of the electrode layer; 3-2: the back surface of the electrode layer; 4-1: the front surface of the lead layer; 4-2: the back surface of the lead layer; 5-1: the front surface of the lower sealing layer; 5-2: the back surface of the lower sealing layer.
Detailed Description
In order to explain the invention in more detail, the invention is further explained with reference to the attached drawings and embodiments, which do not limit the scope of the invention.
In order to realize rapid high-sensitivity detection of environmental hormones, the first object of the invention is to provide a multi-channel electrochemical impedance sensor, which is composed of five layers: an upper sealing layer 1 (half layer), a filtering interface layer 2, an electrode layer 3, a lead layer 4 and a lower sealing layer 5.
The upper sealing layer 1 (half layer) uses PET material as the hydrophobic plastic sealing layer 6 to construct the antifouling layer on the surface of the sensor sample injection channel.
The filtering interface layer 2 is mainly used as a sample introduction filtering layer and an electrode interface layer. A sample is sucked from a wedge-shaped sample inlet 9 on the left side and is connected with a circular sample cell 11 through a drainage pipeline 10 with hydrophilicity, and the filtering interface layer 2 adopts cellulose filter paper as a substrate and can filter the sample to be detected by utilizing the characteristics of the material of the filtering interface layer; the right black parallel finger plugs represent part of the electrode interface leads, the remainder being the hydrophobic ink region 12.
The electrode layer 3 adopts cellulose filter paper as a substrate, and is made into a working electrode, a reference electrode and a counter electrode by utilizing screen printing conductive ink, and comprises a multi-channel working electrode 13 and a pair of reference and counter electrodes 14. The multi-channel working electrode 13 is connected with the middle sample pool 11 through a drainage channel 16 in a circular structure and distributed at intervals of 45 degrees, each channel is led out by conductive ink, and the reference electrode and the counter electrode port are led out by a conductive metal layer.
The lead layer 4 is made of PET materials as a substrate, rectangular contact points are made of conductive ink and are assembled with the electrode layer in a relatively overlapped mode, the multi-channel working electrodes 13 of the electrode layer are led out, channels of the working electrodes are switched through the multi-channel rotary switch 8, and the multi-channel working electrodes are connected with the filtering interface layer 2 through the hollow areas 21 of the electrode layer.
The lower sealing layer 5 uses a PET material as a support substrate of the sensor.
The five-layer structure is bonded together to form a complete electrochemical impedance sensor structure.
In order to realize rapid and high-sensitivity detection of environmental hormones, the second purpose of the invention is to provide a method for detecting different environmental hormones by using a multi-channel electrochemical impedance sensor. Specifically, a carbon-based nano composite material and an environmental hormone antibody to be detected are fixed on the surface of a multi-channel working electrode 13, an electrochemical workstation or a portable electrochemical impedance detector is used for detecting environmental hormones with different concentrations, an impedance electric signal of an electrochemical impedance sensor changes correspondingly along with the concentration, and the rapid detection of the environmental hormones is realized by utilizing the corresponding relation between the impedance electric signal and the concentration.
Fig. 1, fig. 2 and fig. 3 are respectively a schematic diagram of the overall structure, a schematic diagram of the front-side layered structure and a schematic diagram of the back-side layered structure of the multi-channel electrochemical impedance sensor. The multi-channel electrochemical impedance sensor shown in the figure is composed of five layers: the filter comprises an upper sealing layer 1, a filter interface layer 2, an electrode layer 3, a lead layer 4 and a lower sealing layer 5.
A first layer: and the upper sealing layer 1 is formed by constructing an antifouling layer on the surface of the sensor sample injection channel by using a PET material as a plastic sealing layer 6, and comprises a front surface 1-1 and a back surface 1-2.
A second layer: the filtering interface layer 2 comprises a front surface 2-1 and a back surface 2-2, a left sample inlet 9 is of a wedge-shaped structure, the sample inlet is large in area and easy to guide, a sample can be sucked into the sample inlet 9 in a sufficient amount, and a hydrophilic drainage pipeline 10 and a circular sample cell 11 are arranged in the middle area. The filtering interface layer 2 adopts cellulose filter paper as a substrate, and can filter a sample to be detected by utilizing the characteristics of the material of the filtering interface layer; the black parallel insertion part on the right side is an electrode interface lead 19-1, a lead 19-2 and a lead 19-3 which are respectively connected to a reverse lead 20-1, a lead 20-2 and a lead 20-3 through holes 18-1, 18-2 and 18-3; the grey part of the surface layer is the hydrophobic ink area 12.
And a third layer: and an electrode layer 3 comprising a front side 3-1 and a back side 3-2, the layer comprising a multi-channel working electrode 13 and a pair of reference and counter electrodes 14. Cellulose filter paper is used as a substrate, the multi-channel working electrodes are distributed around the sample pool at intervals of 45 degrees, and the end lines 15 are led out by utilizing conductive ink and are connected to a middle sample pool area 17 through a drainage channel 16; the reference and counter electrodes 14 are silk-screened in the sample cell region 17 to serve as a common reference electrode and a common counter electrode of the multi-channel working electrode, and a reference electrode lead 19-4 and a counter electrode lead 19-5 are connected to a reverse lead 20-4 and a lead 20-5 through holes 18-4 and 18-5.
A fourth layer: the lead layer 4 comprises a front surface 4-1 and a back surface 4-2 and is made of PET materials, a conductive ink contact lead 7 is used for leading out a multi-channel working electrode 13 of a third layer, and each working electrode channel is switched through a multi-channel rotary switch 8 and is connected with a lead 20-2 of the second layer 2-2 through a hollow area 21 on the right side of the third layer.
Fifth layer (5): the lower sealing layer comprises a front surface 5-1 and a back surface 5-2, is made of PET materials and is used as a supporting substrate of the sensor. The multi-way rotary switch 8 of the fourth layer penetrates through the fifth layer, passes through the through hole 18-6 and is connected to the through hole 18-6 on the reverse side (5-2) of the fifth layer, so that the switching of each working electrode channel 13 can be carried out from the lower sealing layer.
The stacking sequence of the five-layer structure is as follows: the front surface 1-1 of the upper sealing layer 1 upwards serves as the topmost layer, the front surface 2-1 of the filtering interface layer 2 upwards serves as the second layer, the back surface 2-2 of the filtering interface layer 2 is oppositely stacked with the back surface 3-2 of the electrode layer, the front surface 3-1 of the electrode layer 3 is oppositely assembled with the front surface 4-1 of the lead layer 4, and the back surface 4-2 of the lead layer 4 and the front surface of the lower sealing layer 5 are oppositely assembled
5-1, and laminating the layers by using a thermoplastic method to form a complete electrochemical impedance sensor structure.
The number of channels of the working electrode 13 of the sensor can be expanded into 7-12 channels according to requirements, and the corresponding drainage channel 16 is correspondingly expanded, so that the requirement of simultaneously detecting objects to be detected with different concentrations can be met.
The preparation process of the multi-channel electrochemical impedance sensor comprises the following steps:
(1) Five structural layers of the multichannel electrochemical impedance sensor are designed by using Adobe Illustrator or Auto CAD software, and conductive ink and hydrophobic ink are respectively printed on cellulose filter paper and a PET substrate by using a screen printing technology to form a filter interface layer 2, an electrode layer 3 and a lead layer 4.
(2) The carbon-based nano composite material is synthesized by the carbon-based nano material such as graphene, multi-walled carbon nano tubes and the like and the nano metal material by a solution blending method or an in-situ polymerization method.
(3) Modifying the carbon-based nano composite material to the working surface of the electrochemical impedance sensor by utilizing methods such as electropolymerization or drop coating, and electropolymerizing the electroactive substance to the surface of the carbon-based nano composite material by utilizing a cyclic voltammetry method; then fixing the antibody on the surface of the electrochemical impedance sensor by using a physical or chemical method, and dropwise adding Bovine Serum Albumin (BSA) to seal a non-detection active site; finally, the whole surface of the working electrode is sealed by using the film forming effect of chitosan.
(4) The five-layer structure is stacked in sequence, and the five-layer structure is pressed together by a hot melting method to form the complete electrochemical impedance sensor.
The invention provides a method for detecting different environmental hormones by using a multi-channel electrochemical impedance sensor. In particular to a carbon-based nano composite material and an environmental hormone antibody to be detected which are fixed on the surface of a multi-channel working electrode. The electrochemical impedance sensor is modified by preparing carbon-based nano composite materials from carbon-based nano materials such as graphene and carbon nano tubes and nano metals (nano gold, nano silver, platinum black, nano palladium, nano copper and nano iron) by a solution blending method or an in-situ polymerization method. And detecting the objects to be detected with different concentrations by combining an electrochemical workstation or a portable electrochemical impedance detector.
As shown in fig. 3, the synthesis steps (manufacturing method) of the carbon-based nanocomposite material are as follows:
s1, adding 1mg of graphene and 1mg of multi-walled carbon nanotubes in equal amount into ultrapure water, performing ultrasonic treatment for 1 hour to respectively prepare a graphene dispersion liquid and a multi-walled carbon nanotube dispersion liquid, mixing 1mL of the graphene dispersion liquid and 1mL of the multi-walled carbon nanotube dispersion liquid according to a 1:1 ratio, and stirring at room temperature for 6 hours to obtain a graphene/multi-walled carbon nanotube dispersion liquid;
s2, centrifuging the graphene/multi-walled carbon nanotube dispersion liquid at a high speed for 20 minutes at 8000rpm to remove redundant multi-walled carbon nanotubes, washing with water for multiple times, and drying to obtain a graphene/multi-walled carbon nanotube composite;
s3, re-dispersing the graphene/multi-walled carbon nanotube composite into 2 mL ultrapure water, and carrying out ultrasonic treatment at room temperature for 1 hour to obtain a graphene/multi-walled carbon nanotube dispersion liquid;
and S4, adding the graphene/multi-walled carbon nanotube composite into the 10 mL nano metal particle solution, and stirring at room temperature for 4 hours to obtain the graphene/multi-walled carbon nanotube/nano metal particle carbon-based nano composite material solution.
The invention also discloses a method for modifying the multichannel electrochemical impedance sensor by using the carbon-based nano composite material, which comprises the following steps:
SS1, dropwise adding 15 mu L of graphene/multiwalled carbon nanotube/nano metal particle carbon-based nano composite solution to the surface of the multichannel working electrode, and placing the multichannel working electrode in an electric oven at 50 ℃ for 30 minutes;
SS2, placing the multichannel working electrode modified with the graphene/multiwall carbon nanotube/nano metal particle carbon-based nano composite in a methylene blue solution, and scanning for 50 times by using a cyclic voltammetry, wherein the scanning voltage range is-0.8-1.2V, the scanning speed is 0.1V/s, and the scanning step pitch is 0.001V to obtain the multichannel working electrode modified with the graphene/multiwall carbon nanotube/nano metal particle/polymethylene blue, wherein the electroactive material methylene blue can be replaced by prussian blue, thionine, potassium ferricyanide, malachite green and the like;
SS3, repeatedly washing the prepared multi-channel working electrode by using ultrapure water, removing redundant methylene blue, and airing at room temperature;
SS4, adding 15 mg of BSA powder into 1mL of PBS solution to obtain 10 mg/mL of BSA solution, respectively dropwise coating 10 mu of LBSA solution on the surface of the multichannel working electrode, standing at room temperature for 1 hour, and flushing redundant BSA solution by using ultrapure water;
SS5, successively taking 15 mu L of 250 mu g/mL environmental hormone antibody solution, dripping the solution on the surface of the multi-channel working electrode, and placing the multi-channel working electrode in a refrigerator at 4 ℃ for 12 hours;
and SS6, washing the redundant environmental hormone antibody on the surface of the working electrode by using ultrapure water, soaking the working electrode in the chitosan solution for 1 hour, repeatedly washing by using the ultrapure water, and putting the washed working electrode into a refrigerator at 4 ℃ for later use.
Measuring environmental hormone by adopting the sensor, specifically, dripping 60 mu L of the environmental hormone into a sample inlet of a second filtering interface layer 2, conveying an environmental hormone solution to a sample pool area 17 through the siphoning effect of a drainage channel, filtering by a middle sample pool, flowing into the surface of a multi-channel working electrode of a third electrode layer 3, and incubating for 45 minutes at room temperature; applying an electrochemical impedance detection signal by using an electrochemical workstation or a portable electrochemical impedance detector to detect environmental hormones with different concentrations to obtain a series of impedance spectrum signals, and performing linear fitting on the different concentrations and corresponding equivalent impedances to obtain a working fitting curve; and then, carrying out impedance detection by using an electrochemical workstation or a portable electrochemical impedance detector, and substituting an impedance signal into the fitting curve to calculate the concentration of the environmental hormone.
The invention discloses a multi-channel electrochemical impedance sensor for environmental hormone analysis. The electrochemical impedance sensor is characterized in that an electrode structure is prepared on a PET substrate and a cellulose filter paper substrate by utilizing a screen printing technology, a carbon-based nano composite material (graphene and multi-wall carbon nano tubes), nano metal particles (nano gold, nano silver, platinum black, nano palladium, nano copper, nano iron and the like) and electroactive substances (methylene blue, prussian blue, thionine, potassium ferricyanide, malachite green and the like) are prepared into the nano composite material modified electrochemical impedance sensor by a solution blending method or an in-situ polymerization method, and then different environmental hormone antibodies are assembled on the surface of an electrode to form the multi-channel electrochemical impedance sensor. The invention combines the carbon-based nano composite material, the electroactive substance and the multi-channel electrochemical impedance sensor to realize the simultaneous quantitative analysis of different types of environmental hormones (estradiol, estrone and estriol). The invention has the advantages of low manufacturing cost, good repeatability, high sensitivity, batch measurement and wide application prospect in the field of environmental hormone pollution detection.
The invention combines an electrochemical impedance detection method, modifies an electrochemical impedance sensor by utilizing a carbon-based nano composite material for enhancing a detection signal, and establishes a multi-channel electrochemical impedance sensor for detecting environmental hormones. Compared with the existing method for detecting the environmental hormone, the method has the following advantages:
1. the multi-channel electrochemical workstation or the portable electrochemical impedance detector is used for detection, and the detection equipment is low in price and small in size.
2. The PET material and the cellulose filter paper are used as the substrate material of the electrochemical impedance sensor, so that the electrochemical impedance sensor is low in price and can be repeatedly used.
3. The multi-channel electrochemical impedance sensor can realize the detection of various environmental hormones, the detection method is simple, and the sensor can be produced in batches.
4. Carbon-based nano materials, different electroactive substances and nano metal materials are synthesized into different types of nano composite materials by a solution blending method or an in-situ polymerization method to be used for fixing different environmental hormone antibodies, the nano metal can be used for amplifying detection signals, and the different electroactive substances can be used for simultaneously analyzing different types of environmental hormones.
Claims (7)
1. A multi-channel chemical impedance sensor is characterized by comprising an upper sealing layer front surface, a filtering interface layer front surface, an electrode layer back surface, a lead layer front surface and a lower sealing layer which are superposed from top to bottom;
the upper sealing layer is an antifouling layer on the surface of the sample feeding channel and is a plastic sealing layer made of PET material;
the filter interface layer adopts cellulose filter paper as a substrate, hydrophobic ink as front and back surface layers, a sample inlet on one side adopts a wedge-shaped structure, the filter interface layer is communicated with the circular sample cell through corresponding hydrophilic drainage pipelines, and the other side is provided with inserted electrode leads which are arranged in parallel and are respectively connected to corresponding leads on the back side through holes;
the electrode layer adopts cellulose filter paper as a substrate, the front side of the electrode layer comprises a multi-channel working electrode and a pair of reference and counter electrodes, the multi-channel working electrode is made of screen printing conductive ink, the working electrodes are distributed around the sample pool at intervals and connected to the sample pool area through corresponding drainage channels, and each channel adopts a conductive ink leading-out end line; the reference electrode and the counter electrode are printed in the sample cell area in a silk-screen mode, and the reference electrode lead and the counter electrode lead are connected to the reverse side lead through corresponding through holes;
the lead layer is made of PET (polyethylene terephthalate) material and is provided with rectangular contact points made of conductive ink materials corresponding to the multi-channel working electrodes of the electrode layer on the front side, and the multi-channel working electrodes of the electrode layer are led out and connected to the multi-path rotary switch through conductive ink contact leads and are connected with working electrode leads on the back side of the filtering interface layer;
the lower sealing layer is made of PET materials and serves as a substrate of the sensor, and the multi-path rotary switch penetrates through a through hole in the multi-path rotary switch.
2. The multi-channel chemical impedance sensor as claimed in claim 1, wherein the number of channels of the working electrode can be expanded to 7-12 channels according to requirements, and the corresponding drainage channels are correspondingly expanded, so as to meet the requirement of simultaneous detection of objects to be detected with different concentrations.
3. The multi-channel chemical impedance sensor as claimed in claim 1, wherein the carbon-based nanocomposite material and the environmental hormone antibody to be detected are fixed on the surface of the multi-channel working electrode.
4. A manufacturing method of a multi-channel chemical impedance sensor is characterized by comprising the following steps:
4-1: the multichannel chemical impedance sensor comprises an upper sealing layer front surface, a filtering interface layer front surface, an electrode layer back surface, a lead layer front surface and a lower sealing layer which are superposed from top to bottom; designing five structural layers of the multi-channel electrochemical impedance sensor, and respectively printing conductive ink and hydrophobic ink on cellulose filter paper and a PET (polyethylene terephthalate) substrate by utilizing a screen printing technology to form a filter interface layer, an electrode layer and a lead layer;
4-2: synthesizing a carbon-based nano composite material by using a carbon-based nano material and a nano metal material;
4-3: modifying the carbon-based nano composite material to the working surface of the electrochemical impedance sensor, and electropolymerizing the electroactive substance to the surface of the carbon-based nano composite material; then fixing the antibody on the surface of the electrochemical impedance sensor, and dropwise adding bovine serum albumin to seal non-detection active sites; finally, the whole surface of the working electrode is sealed integrally by utilizing the film forming effect of chitosan;
4-4: the five-layer structure is stacked in sequence, and the five-layer structure is pressed together by a hot melting method to form the complete electrochemical impedance sensor.
5. The method of claim 4, wherein the carbon-based nanocomposite material of step 4-2 is prepared by:
s1, adding 1mg of graphene and 1mg of multi-walled carbon nanotubes in equal amount into ultrapure water, performing ultrasonic treatment for 1 hour to respectively prepare a graphene dispersion liquid and a multi-walled carbon nanotube dispersion liquid, mixing 1mL of the graphene dispersion liquid and 1mL of the multi-walled carbon nanotube dispersion liquid according to a 1:1 ratio, and stirring at room temperature for 6 hours to obtain a graphene/multi-walled carbon nanotube dispersion liquid;
s2, centrifuging the graphene/multi-walled carbon nanotube dispersion liquid at a high speed for 20 minutes at 8000rpm to remove redundant multi-walled carbon nanotubes, washing with water for multiple times, and drying to obtain a graphene/multi-walled carbon nanotube composite;
s3, re-dispersing the graphene/multi-walled carbon nanotube composite into 2 mL ultrapure water, and performing ultrasonic treatment at room temperature for 1 hour to obtain a graphene/multi-walled carbon nanotube dispersion liquid;
and S4, adding the graphene/multi-walled carbon nanotube composite into the 10 mL nano metal particle solution, and stirring at room temperature for 4 hours to obtain the graphene/multi-walled carbon nanotube/nano metal particle carbon-based nano composite material solution.
6. The method for manufacturing a multichannel chemical impedance sensor according to claim 4, wherein the carbon-based nanocomposite material in the step 4-3 is used for modifying the multichannel electrochemical impedance sensor as follows:
SS1, dropwise adding 15 mu L of graphene/multi-walled carbon nanotube/nano metal particle carbon-based nano composite solution onto the surface of a multichannel working electrode, and placing in an electric oven at 50 ℃ for 30 minutes;
SS2, placing the multichannel working electrode for modifying the graphene/multi-walled carbon nanotube/nano metal particle carbon-based nano composite in a methylene blue solution, and scanning for 50 times by using a cyclic voltammetry method, wherein the scanning voltage range is-0.8 to 1.2V, the scanning speed is 0.1V/s, and the scanning step distance is 0.001V to obtain the multichannel working electrode modified by the graphene/multi-walled carbon nanotube/nano metal particle/polymethylene blue;
SS3, repeatedly washing the prepared multi-channel working electrode by using ultrapure water, removing redundant methylene blue, and airing at room temperature;
and SS4, adding 15 mg of BSA powder into 1mL of PBS solution to obtain 10 mg/mL of BSA solution, respectively dropwise coating 10 mu of LBSA solution on the surface of the multichannel working electrode, standing at room temperature for 1 hour, and flushing redundant BSA solution by using ultrapure water.
7. Use of a multi-channel electrochemical impedance sensor according to any of claims 1 to 3 for the detection of different concentrations of environmental hormones, wherein:
7-1: dropwise adding 60 muL of environmental hormone to a sample inlet of the filtering interface layer, conveying the environmental hormone solution to a sample pool area through the siphoning effect of a drainage channel, filtering the environmental hormone solution by the middle sample pool, flowing into the surface of a multi-channel working electrode of the third electrode layer, and incubating for 45 minutes at room temperature;
7-2: detecting environmental hormones with different concentrations to obtain a series of impedance spectrum signals, and performing linear fitting on the different concentrations and corresponding equivalent impedances to obtain a working fitting curve;
7-3: and (5) carrying out impedance detection, and substituting the impedance signal into the fitting curve to calculate the concentration of the environmental hormone.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2023174438A3 (en) * | 2023-04-14 | 2024-02-01 | 杭州柔谷科技有限公司 | Reproductive hormone test system, and flexible sensing electrode and preparation method therefor |
| CN118330010A (en) * | 2024-06-17 | 2024-07-12 | 成都艾立本科技有限公司 | Mass spectrometry method of multi-path liquid phase sampling and multi-path liquid phase sampling system and application |
Citations (16)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| AT229934B (en) * | 1960-07-25 | 1963-10-25 | Licentia Gmbh | Multi-step rotary switch with one or more switch levels in a printed circuit |
| EP0030176A1 (en) * | 1979-11-16 | 1981-06-10 | Crouzet | Switching device for the programmer of a washing machine |
| US20030046811A1 (en) * | 2001-09-10 | 2003-03-13 | Eumed Biotechnology Co., Ltd. | New spacer forming method used for a biosensor |
| US20050183953A1 (en) * | 2004-02-23 | 2005-08-25 | General Life Biotechnolgoy Co., Ltd. | Electrochemical biosensor by screen printing and method of fabricating same |
| CN102914648A (en) * | 2012-10-09 | 2013-02-06 | 重庆医科大学 | Electrochemical immunosensor for detecting toxoplasma gondii IgM antibody and preparation method thereof |
| CN103196984A (en) * | 2013-03-13 | 2013-07-10 | 济南大学 | Preparation method and application of sensor for simultaneous detection of multiple aflatoxins |
| CN103196973A (en) * | 2013-03-13 | 2013-07-10 | 济南大学 | Method for preparing seven-channel aflatoxin immunosensor and application |
| CN103454426A (en) * | 2013-09-10 | 2013-12-18 | 山东理工大学 | Preparation method of nanogold/chitosan-graphene-methylene blue modified immunosensor |
| CN103592437A (en) * | 2013-11-11 | 2014-02-19 | 山东理工大学 | Immunosensor based on modification of graphene-multiwalled carbon-nanogold size-chitosan |
| CN103760209A (en) * | 2014-01-27 | 2014-04-30 | 中国科学院电子学研究所 | Multi-parameter paper-chip electrochemical immunosensor and method for detecting lung cancer markers |
| CN204855530U (en) * | 2015-06-28 | 2015-12-09 | 济南大学 | Detect photoelectricity immunosensor of two kinds of lung cancer marks simultaneously based on quantum dot |
| CN204989190U (en) * | 2015-06-30 | 2016-01-20 | 济南大学 | Detect aflatoxin B1 and B2's electric chemical immunity sensor simultaneously |
| CN109061190A (en) * | 2018-08-22 | 2018-12-21 | 江苏集萃微纳自动化系统与装备技术研究所有限公司 | The preparation of multichannel biosensor array and immune detection application based on paper chip |
| CN112763562A (en) * | 2021-01-28 | 2021-05-07 | 河南工业大学 | Preparation method of branch-shaped walking machine aptamer electrochemical sensor for adenosine triphosphate detection |
| US20210396703A1 (en) * | 2020-06-17 | 2021-12-23 | Northeastern University | Rapid Electrochemical Point-of-Care COVID-19 Detection in Human Saliva |
| CN114705736A (en) * | 2022-03-21 | 2022-07-05 | 山东大学 | Portable multi-channel detection electrochemical sensing system and application thereof |
-
2022
- 2022-11-04 CN CN202211375451.4A patent/CN115479982A/en active Pending
Patent Citations (16)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| AT229934B (en) * | 1960-07-25 | 1963-10-25 | Licentia Gmbh | Multi-step rotary switch with one or more switch levels in a printed circuit |
| EP0030176A1 (en) * | 1979-11-16 | 1981-06-10 | Crouzet | Switching device for the programmer of a washing machine |
| US20030046811A1 (en) * | 2001-09-10 | 2003-03-13 | Eumed Biotechnology Co., Ltd. | New spacer forming method used for a biosensor |
| US20050183953A1 (en) * | 2004-02-23 | 2005-08-25 | General Life Biotechnolgoy Co., Ltd. | Electrochemical biosensor by screen printing and method of fabricating same |
| CN102914648A (en) * | 2012-10-09 | 2013-02-06 | 重庆医科大学 | Electrochemical immunosensor for detecting toxoplasma gondii IgM antibody and preparation method thereof |
| CN103196984A (en) * | 2013-03-13 | 2013-07-10 | 济南大学 | Preparation method and application of sensor for simultaneous detection of multiple aflatoxins |
| CN103196973A (en) * | 2013-03-13 | 2013-07-10 | 济南大学 | Method for preparing seven-channel aflatoxin immunosensor and application |
| CN103454426A (en) * | 2013-09-10 | 2013-12-18 | 山东理工大学 | Preparation method of nanogold/chitosan-graphene-methylene blue modified immunosensor |
| CN103592437A (en) * | 2013-11-11 | 2014-02-19 | 山东理工大学 | Immunosensor based on modification of graphene-multiwalled carbon-nanogold size-chitosan |
| CN103760209A (en) * | 2014-01-27 | 2014-04-30 | 中国科学院电子学研究所 | Multi-parameter paper-chip electrochemical immunosensor and method for detecting lung cancer markers |
| CN204855530U (en) * | 2015-06-28 | 2015-12-09 | 济南大学 | Detect photoelectricity immunosensor of two kinds of lung cancer marks simultaneously based on quantum dot |
| CN204989190U (en) * | 2015-06-30 | 2016-01-20 | 济南大学 | Detect aflatoxin B1 and B2's electric chemical immunity sensor simultaneously |
| CN109061190A (en) * | 2018-08-22 | 2018-12-21 | 江苏集萃微纳自动化系统与装备技术研究所有限公司 | The preparation of multichannel biosensor array and immune detection application based on paper chip |
| US20210396703A1 (en) * | 2020-06-17 | 2021-12-23 | Northeastern University | Rapid Electrochemical Point-of-Care COVID-19 Detection in Human Saliva |
| CN112763562A (en) * | 2021-01-28 | 2021-05-07 | 河南工业大学 | Preparation method of branch-shaped walking machine aptamer electrochemical sensor for adenosine triphosphate detection |
| CN114705736A (en) * | 2022-03-21 | 2022-07-05 | 山东大学 | Portable multi-channel detection electrochemical sensing system and application thereof |
Non-Patent Citations (3)
| Title |
|---|
| DEXIANG FENG ET AL.: "Label-free electrochemical immunosensor for the carcinoembryonic antigen using a glassy carbon electrode modified with electrodeposited Prussian Blue, a graphene and carbon nanotube assembly and an antibody immobilized on gold nanoparticles", 《MICROCHIMICA ACTA》 * |
| YAN FAN ET AL.: "An electrochemical immunosensor based on reduced graphene oxide/multiwalled carbon nanotubes/thionine/gold nanoparticle nanocomposites for the sensitive testing of follicle-stimulating hormone", 《ANALYTICAL METHODS》 * |
| 罗启枚等: "一种基于纳米金/石墨烯/普鲁士蓝(PB)修饰玻碳电极非标记免疫传感器", 《化学传感器》 * |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2023174438A3 (en) * | 2023-04-14 | 2024-02-01 | 杭州柔谷科技有限公司 | Reproductive hormone test system, and flexible sensing electrode and preparation method therefor |
| CN118330010A (en) * | 2024-06-17 | 2024-07-12 | 成都艾立本科技有限公司 | Mass spectrometry method of multi-path liquid phase sampling and multi-path liquid phase sampling system and application |
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