CN114441611B - Wide dynamic measurement range glucose sensor based on organic field effect transistor - Google Patents
Wide dynamic measurement range glucose sensor based on organic field effect transistor Download PDFInfo
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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
- G01N27/327—Biochemical electrodes, e.g. electrical or mechanical details for in vitro measurements
- G01N27/3271—Amperometric enzyme electrodes for analytes in body fluids, e.g. glucose in blood
- G01N27/3272—Test elements therefor, i.e. disposable laminated substrates with electrodes, reagent and channels
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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
- G01N27/327—Biochemical electrodes, e.g. electrical or mechanical details for in vitro measurements
- G01N27/3271—Amperometric enzyme electrodes for analytes in body fluids, e.g. glucose in blood
- G01N27/3273—Devices therefor, e.g. test element readers, circuitry
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
- H10K10/40—Organic transistors
- H10K10/46—Field-effect transistors, e.g. organic thin-film transistors [OTFT]
- H10K10/462—Insulated gate field-effect transistors [IGFETs]
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
- H10K71/13—Deposition of organic active material using liquid deposition, e.g. spin coating using printing techniques, e.g. ink-jet printing or screen printing
- H10K71/135—Deposition of organic active material using liquid deposition, e.g. spin coating using printing techniques, e.g. ink-jet printing or screen printing using ink-jet printing
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
- H10K71/15—Deposition of organic active material using liquid deposition, e.g. spin coating characterised by the solvent used
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Abstract
The invention provides a glucose sensor with a wide dynamic measurement range based on an organic field effect transistor, which consists of a substrate, two P+N organic field effect transistors and glucose oxidase immobilized by hydrogel, wherein the two P+N organic field effect transistors work cooperatively, so that the detection of the wide dynamic measurement range can be realized; by immobilizing the modified glucose oxidase on the channel between the source electrode and the drain electrode by using hydrogel, the detection of low-concentration and relatively high-concentration glucose solution can be realized, and the problem of the linear range of the conventional OFET sensor is effectively solved.
Description
Technical Field
The invention relates to the technical field of sensors, in particular to a glucose sensor with a wide dynamic measurement range based on an organic field effect transistor.
Background
Diabetes is a syndrome caused by inheritance, environmental and other factors acting on the body. Long-term hyperglycemia can cause chronic damage to various tissues and organs of the human body, especially the eyes, kidneys, heart, blood vessels and nerves, and gradually cause dysfunction, thereby severely threatening the health of humans. Diabetes is predicted by the World Health Organization (WHO) to be the seventh leading cause of death in the world by 2030. It is one of the most common diagnostic diseases, with many patients affected each year, and it is expected that 2045 years will reach 7.84 billion. At present, no medicine and method for thoroughly curing diabetes exist. Only blood glucose concentration can be controlled by injecting insulin or oral hypoglycemic drugs. The world health organization suggests that diabetics conduct self-blood glucose tests while regulating insulin based on blood glucose levels in the body. Blood glucose monitoring is therefore of great importance for the diagnosis and treatment of diabetes.
Organic Field Effect Transistors (OFETs) have wide application prospects in organic displays, smart cards, large-scale integrated circuits, sensors and memory devices. OFET sensors are likely to be applied to glucose monitoring due to their attractive properties of ease of use, flexibility and low cost manufacturing processes. However, glucose sensors based on OFET have the disadvantage of narrow measurement range, which makes it difficult to meet the requirements of clinical applications.
Disclosure of Invention
The invention aims to provide a glucose sensor with a wide dynamic measurement range based on an organic field effect transistor, which has a wide dynamic detection range.
In order to solve the technical problems, the technical scheme of the invention is as follows:
a glucose sensor with a wide dynamic measurement range based on organic field effect transistors comprises a substrate, two P+N organic field effect transistors and glucose oxidase immobilized on hydrogel, wherein the two P+N organic field effect transistors are respectively a parallel P+N transistor and a serial P+N transistor; the P+N organic field effect transistor is loaded on a substrate through an evaporation method, screen printing or ink-jet printing technology, 20% glucose oxidase aqueous solution is dripped on a channel between a source electrode and a drain electrode of the P-type transistor/N-type transistor, and the P-type transistor/N-type transistor is stood and dried; the modified glucose oxidase is immobilized on the channel between the source and drain of the p+n organic field effect transistor with a hydrogel.
Preferably, the substrate is a PDMS/PI substrate of the glucose sensor with wide dynamic measurement range based on organic field effect transistors.
Preferably, in the wide dynamic measurement range glucose sensor based on organic field effect transistors, the p+n transistors are connected in series, and the source of the P-type transistor is connected with the gate of the N-type transistor, and the gate of the P-type transistor is connected with the drain of the N-type transistor; the parallel P+N transistor is formed by connecting the source electrode of the P-type transistor with the drain electrode of the N-type transistor and connecting the grid electrodes of the P-type transistor and the N-type transistor.
Preferably, the wide dynamic measurement range glucose sensor based on the organic field effect transistor is characterized in that the P-type transistor is composed of a gate electrode, a source electrode, a drain electrode, an insulator layer and a semiconductor layer (P-type semiconductor); the N-type transistor is an N-type organic field effect transistor and is composed of a grid electrode, a source electrode, a drain electrode, an insulator layer and a semiconductor layer (N-type semiconductor).
Preferably, the wide dynamic measurement range glucose sensor based on the organic field effect transistor is prepared by the following inkjet printing technology: the method comprises the steps of ink-jet printing Jin Moshui (purchased from UTdot) on a substrate and sintering by heating to form a grid electrode, then ink-jet printing silica gel ink (purchased from UTdot) and sintering by heating to form an insulating layer, then ink-jet printing a semiconductor layer and sintering by heating, wherein a P-type semiconductor adopts poly 3-hexylthiophene (P3 HT) solution, an N-type semiconductor adopts P (ND I2 OD-T2) solution (P (NDI 2 OD-T2) is poly (2, 7-bis (2-octyldodecyl) benzo [ LMN ] [3,8] phenanthroline-1, 3,6,8 (2H, 7H) -tetraon-4, 9-diyl) ([ 2,2'] dithiophene-5, 5' -diyl)), and finally ink-jet printing Jin Moshui to form a source electrode and a drain electrode, and sintering by heating.
Preferably, the wide dynamic measurement range glucose sensor based on the organic field effect transistor, wherein the hydrogel is a hydrogel mixture, and the components are as follows: 3w/w% chitosan, 2w/w% acetic acid, 10w/w% glycerol, the balance being water.
The wide dynamic measurement range glucose sensor based on the organic field effect transistor realizes the specific detection of glucose by the change of the mobility of a semiconductor in the organic field effect transistor caused by the adsorption and dissociation between glucose and glucose oxidase GOx.
The wide dynamic measurement range glucose sensor based on the organic field effect transistor changes the transfer characteristic curve of the device by measuring the transfer characteristic curve of the device.
According to the glucose sensor with the wide dynamic measurement range based on the organic field effect transistor, the hydrogel is used for packaging the sensor and fixing glucose oxidase, so that the anti-interference capability of the sensor is improved, the service life of the sensor is prolonged, and the glucose sensor is constructed.
The beneficial effects are that:
the glucose sensor with wide dynamic measurement range based on the organic field effect transistors is characterized in that the two P+N organic field effect transistors work cooperatively, so that the detection with wide dynamic measurement range can be realized; by immobilizing the modified glucose oxidase on the channel between the source electrode and the drain electrode by using hydrogel, the detection of low-concentration and relatively high-concentration glucose solution can be realized, and the problem of the linear range of the conventional OFET sensor is effectively solved.
Drawings
FIG. 1 is a schematic diagram of the overall structure of a wide dynamic measurement range glucose sensor based on organic field effect transistors in accordance with the present invention;
FIG. 2 is a schematic diagram of the connection of two P+N organic field effect transistors of an organic field effect transistor based wide dynamic range glucose sensor of the present invention, wherein the upper diagram is a series P+N transistor and the lower diagram is a parallel P+N transistor;
fig. 3 is a schematic diagram (side view) of the structure of a single organic field effect transistor of the wide dynamic measurement range glucose sensor based on organic field effect transistors of the present invention.
In the figure: a P+N organic field effect transistor B glucose C substrate
D, glucose oxidase aqueous solution E: hydrogel 1: gate 2: source electrode
3: drain electrode 4: insulator layer 5: p-type semiconductor layer 6: n-type semiconductor layer
7: hydrogel immobilized modified glucose oxidase
Detailed Description
A wide dynamic measurement range glucose sensor based on organic field effect transistors and a method for implementing the same according to the present invention will be described in detail with reference to the accompanying examples and drawings.
Example 1
As shown in fig. 1-3, the wide dynamic measurement range glucose sensor based on organic field effect transistors adopts an inkjet printing technology to prepare two p+n organic field effect transistors a on a substrate C, including a series p+n Organic Field Effect Transistor (OFET) and a parallel p+n OFET; the P-type transistor is composed of a grid electrode 1, an insulator layer 4, a P-type semiconductor layer 5, and a source electrode 2 and a drain electrode 3 at the uppermost layer from bottom to top; the N-type transistor is composed of a grid electrode 1, an insulator layer 4, an N-type semiconductor layer 6, and a source electrode 2 and a drain electrode 3 at the uppermost layer from bottom to top.
The series p+n OFET is constructed by connecting the gate 1 of the P-type transistor and the source 2 of the N-type transistor. The parallel p+n OFET is constructed by connecting the gates 1 of the P-type and N-type transistors and connecting the source 2 of the P-type transistor and the drain 3 of the N-type transistor.
Dripping 20% glucose oxidase aqueous solution D on a channel between a source electrode 2 and a drain electrode 3 of the P-type transistor/N-type transistor, standing and airing, dripping hydrogel E on the channel, standing and airing, fixing modified glucose oxidase 7 on the channel between the source electrode 2 and the drain electrode 3 of the P+N organic field effect transistor by using hydrogel, wherein the adopted hydrogel is a hydrogel mixture, and the components are as follows: 3w/w% chitosan, 2w/w% acetic acid, 10w/w% glycerol, the balance being water. The prepared glucose sensor works on the principle that the detection of transistor response changes caused by the adsorption and desorption of glucose oxidase D and glucose B is realized.
The ink-jet printing mode is as follows: the substrate was ink-jet printed Jin Moshui (from UTdot) and heat sintered to form the gate electrode, then ink-jet printed silica gel ink (from UTdot) and heat sintered to form the insulating layer, then ink-jet printed the semiconductor layer and heat sintered, wherein the P-type semiconductor layer 5 was poly 3-hexylthiophene (P3 HT) solution, the N-type semiconductor layer 6 was P (NDI 2 OD-T2) solution, finally ink-jet printed Jin Moshui to form the source and drain electrodes, and heat sintered.
As shown in fig. 2, the two p+n organic field effect transistors consist of a series p+n OFET and a parallel p+n OFET. The series p+n OFET is constructed by connecting the gate 1 of the P-type OFET and the source 2 of the N-type OFET. This connection allows for a cascaded two-stage amplification of the weak detection signal to expand the measurable range. However, the series p+n OFET is unstable, and the N OFET is vulnerable to high input current amplified, and thus it is difficult to detect glucose at high concentration. Therefore, it is proposed to connect the gates 1 of the P-type OFET and the N-type OFET in parallel with p+n OFET and connect the source 2 of the P-type OFET and the drain 3 of the N-type OFET, and compress the unmeasurable high concentration signal in proportion to a measurable range by the parallel suppression effect without amplifying the superposition, thereby enabling the device to operate at high input currents. Parallel p+n OFETs cannot distinguish low input currents due to the parallel inhibition effect and therefore it is difficult to detect low glucose concentrations.
Finally, the series P+N OFET was used to measure 1. Mu. Mol/L to 1mmol/L glucose solution, and the parallel P+NOFET was used to measure 1mmol/L to 1mol/L glucose solution. The cooperation of the two p+n organic field effect transistors allows the biosensor to have a wider dynamic range of glucose measurement.
The specific manufacturing method of the glucose sensor with the wide dynamic detection range is as follows:
1. the substrate was prepared by first fabricating a PDMS/PI substrate, spin-coating Polydimethylsiloxane (PDMS) on a glass sheet at 500rpm with a spin coater, then heating PDMS on a heating plate at 95℃for 60min, treating the PDMS substrate with a 100W oxygen plasma for 30s, and then spin-coating Polyimide (PI) on the PDMS substrate at 2000rpm for 45s with a spin coater.
2. Two p+n organic field effect transistors were prepared, the gate electrode (Jin Moshui), the insulating layer (silica gel ink), the P-type semiconductor layer [1w/w% O-xylene solution of P3HT ], the N-type semiconductor layer [1w/w% P (NDI 2O-T2) in toluene solution ], the source (Jin Moshui) and drain (Jin Moshui) were then heated at 250 ℃ for 2 hours.
3. Modified glucose oxidase, 20w/w% GOx was added drop wise to the transistor sensor.
4. A hydrogel mixture of 3w/w% chitosan, 2w/w% acetic acid, 10w/w% glycerol was applied drop wise to the sensor, encapsulated with hydrogel.
5. The preparation of the sensor was completed after standing overnight.
In measurement, for a low concentration glucose solution (1. Mu. Mol/L-1 mmol/L), measurement was performed using a P+N OFET glucose sensor in series by applying a voltage V between the drain of a P-type OFET transistor and the source of an N-type OFET transistor in series with P+N OFET glucose DS And measuring the current at two ends to obtain a transfer characteristic curve of the glucose sensor. For higher concentration glucose solutions (1 mmol/L-1 mol/L), by applying a gate voltage (3.0V) to the gate of the parallel P+N sensor, a voltage V is applied between the drain of the P-type OFET transistor and the source of the N-type OFET of the parallel P+N OFET sensor DS The OFET glucose sensor is realized to measure.
The foregoing is merely a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, it is possible to make several modifications and adaptations of the structure of the present invention without departing from the principle of the present invention, and those modifications and adaptations of the structure based on the method of the present invention are intended to be within the scope of the present invention.
Claims (5)
1. A wide dynamic measurement range glucose sensor based on organic field effect transistors, characterized by: the preparation method comprises a substrate, two P+N organic field effect transistors and glucose oxidase immobilized by hydrogel, wherein the two P+N organic field effect transistors are respectively a parallel P+N transistor and a serial P+N transistor, wherein the parallel P+N transistor is formed by connecting a source electrode of a P-type transistor and a drain electrode of an N-type transistor and connecting a grid electrode of the P-type transistor and a grid electrode of the N-type transistor; the series P+N transistor is formed by connecting a source electrode of a P-type transistor with a grid electrode of an N-type transistor and connecting the grid electrode of the P-type transistor with a drain electrode of the N-type transistor; the P+N organic field effect transistor is loaded on a substrate through an evaporation method, screen printing or ink-jet printing technology, a 20% glucose oxidase aqueous solution is dripped on a channel between the source electrode and the drain electrode of the P-type transistor and the source electrode and the drain electrode of the N-type transistor, and after standing and airing, the modified glucose oxidase is fixed on the channel between the source electrode and the drain electrode of the P+N organic field effect transistor through hydrogel.
2. The wide dynamic measurement range organic field effect transistor based glucose sensor of claim 1, wherein: the substrate is a PDMS/PI substrate.
3. The wide dynamic measurement range organic field effect transistor based glucose sensor of claim 1, wherein: the P-type transistor is composed of a grid electrode, a source electrode, a drain electrode, an insulator layer and a P-type semiconductor layer; the N-type transistor is an N-type organic field effect transistor and comprises a grid electrode, a source electrode, a drain electrode, an insulator layer and an N-type semiconductor layer.
4. The wide dynamic measurement range organic field effect transistor based glucose sensor of claim 1 or 2, wherein: the P-type transistor and the N-type transistor are prepared by the following inkjet printing technology: and (3) carrying out ink-jet printing of gold ink on the substrate and heating and sintering to form a grid electrode, then carrying out ink-jet printing of silica gel ink and heating and sintering to form an insulating layer, then carrying out ink-jet printing of a semiconductor layer and heating and sintering, wherein a P-type semiconductor adopts a poly 3-hexylthiophene solution, an N-type semiconductor adopts a P (NDI 2 OD-T2) solution, and finally carrying out ink-jet printing of Jin Moshui to form a source electrode and a drain electrode, and heating and sintering.
5. The wide dynamic measurement range organic field effect transistor based glucose sensor of claim 1, wherein: the hydrogel is a hydrogel mixture, and comprises the following components: 3w/w% chitosan, 2w/w% acetic acid, 10w/w% glycerol, the balance being water.
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Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2000187018A (en) * | 1998-12-22 | 2000-07-04 | Matsushita Electric Works Ltd | Semiconductor ion sensor |
CN109256465A (en) * | 2012-03-06 | 2019-01-22 | 生命科学生物传感器诊断私人有限公司 | Organic Thin Film Transistors and its purposes in Application in Sensing |
CN111839532A (en) * | 2020-07-14 | 2020-10-30 | 天津大学 | Flexible epidermis electrochemistry biosensor based on conductive hydrogel |
CN112394100A (en) * | 2020-11-03 | 2021-02-23 | 湖北大学 | Flexible electrochemical transistor sensor based on glycerol gel electrolyte, preparation method of flexible electrochemical transistor sensor and method for detecting glucose |
CN113826205A (en) * | 2017-07-14 | 2021-12-21 | 剑桥企业有限公司 | Power semiconductor device with auxiliary gate structure |
Family Cites Families (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US7794584B2 (en) * | 2005-10-12 | 2010-09-14 | The Research Foundation Of State University Of New York | pH-change sensor and method |
-
2021
- 2021-12-22 CN CN202111579962.3A patent/CN114441611B/en active Active
Patent Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2000187018A (en) * | 1998-12-22 | 2000-07-04 | Matsushita Electric Works Ltd | Semiconductor ion sensor |
CN109256465A (en) * | 2012-03-06 | 2019-01-22 | 生命科学生物传感器诊断私人有限公司 | Organic Thin Film Transistors and its purposes in Application in Sensing |
CN113826205A (en) * | 2017-07-14 | 2021-12-21 | 剑桥企业有限公司 | Power semiconductor device with auxiliary gate structure |
CN111839532A (en) * | 2020-07-14 | 2020-10-30 | 天津大学 | Flexible epidermis electrochemistry biosensor based on conductive hydrogel |
CN112394100A (en) * | 2020-11-03 | 2021-02-23 | 湖北大学 | Flexible electrochemical transistor sensor based on glycerol gel electrolyte, preparation method of flexible electrochemical transistor sensor and method for detecting glucose |
Non-Patent Citations (2)
Title |
---|
Coupling p+n Field-Effect Transistor Circuits for Low Concentration Methane Gas Detection;Ning Han;sensors;第18卷(第3期);正文第2页第3段至第6页第3段 * |
Improving the signal resolution of semiconductor gas sensors to high-concentration gases;Ning Han;Solid State Electronics;第162卷;正文第2页左栏第1段至第5页右栏第4段 * |
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