CN109490392B - Field effect transistor biosensor and preparation method thereof - Google Patents
Field effect transistor biosensor and preparation method thereof Download PDFInfo
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Abstract
The invention relates to the technical field of biosensors, in particular to a field effect transistor biosensor and a preparation method thereof. The field effect transistor biosensor provided by the invention comprises a source electrode in a needle shape, a first insulating layer arranged on the surface of the source electrode, a drain electrode arranged on the surface of the first insulating layer and a second insulating layer arranged on the surface of the drain electrode; wherein a tip portion of the field effect transistor biosensor is divided into a section including a source electrode, a first insulating layer, a drain electrode, and a second insulating layer, and the source electrode and the drain electrode of the tip portion are conducted through a channel connection layer. The field effect transistor biosensor provided by the invention is needle-shaped, and can be directly inserted into a living body to carry out real-time monitoring on biological signal molecules. The invention provides a preparation method of the field effect transistor biosensor, which is simple to operate and can be prepared in batches.
Description
Technical Field
The invention relates to the technical field of biosensors, in particular to a field effect transistor biosensor and a preparation method thereof.
Background
A Field Effect Transistor (FET) biosensor is one of the most potential biosensors in recent years, and has the characteristics of high sensitivity, high analysis speed, less reagent consumption, simple operation, no labeling and the like, and particularly, the great miniaturization and integration thereof have attracted extensive attention in the Field of life science. Most of the current FET biosensors are prepared by standard semiconductor lithography technology, so that the biosensors are basically in the form of a flat silicon-based array electrode. Such a flat-plate type FET biosensor can be used only for in vitro detection of a liquid sample or detection of a cell level, and is difficult to be used for biological detection of a living body.
Currently, real-time living body monitoring is a research hotspot and difficulty in the international advanced science field, the Oilonglan group issues take the lead in developing living body research in China, and a new principle, a new method and a new technology of living body analytical chemistry are established and developed, and a series of important research results are obtained. They mainly concentrate on the research of the brain substance, develop the microdialysis technology for the real-time monitoring of on-line extraction of the brain substance, and also develop the carbon fiber electrodes with different functions for the real-time tracking of the living signal molecules, and these researches lay a good foundation for the development of the domestic living real-time research. However, carbon fiber electrodes belong to electrochemical sensors, are based on electrochemical methods for detecting electroactive substances, and lack specificity. So at present, live real-time research still has some difficulties and challenges.
Disclosure of Invention
The invention aims to provide a field effect transistor biosensor and a preparation method thereof.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides a field effect transistor biosensor, which comprises a source electrode in a needle shape, a first insulating layer arranged on the surface of the source electrode, a drain electrode arranged on the surface of the first insulating layer and a second insulating layer arranged on the surface of the drain electrode, wherein the source electrode is arranged on the surface of the first insulating layer; wherein a tip portion of the field effect transistor biosensor is divided into a section including a source electrode, a first insulating layer, a drain electrode, and a second insulating layer, and the source electrode and the drain electrode of the tip portion are conducted through a channel connection layer.
Preferably, the material of the source electrode comprises stainless steel, gold, platinum or copper.
Preferably, the diameter of the source electrode is 0.15-0.5 mm.
Preferably, the material of the drain electrode comprises gold, platinum or copper.
Preferably, the thickness of the drain electrode is 3-5 μm.
Preferably, the insulating materials forming the first and second insulating layers independently comprise parylene, an electrophoretic paint, or an epoxy resin.
Preferably, the first and second insulating layers have thicknesses of 4 to 10 μm independently.
Preferably, the channel connection material forming the channel connection layer comprises a semiconductor material.
Preferably, the semiconductor material comprises carbon nanotubes, graphene, molybdenum disulfide or silicon nanowires.
The invention provides a preparation method of the field effect transistor biosensor, which comprises the following steps:
sequentially depositing a first insulating layer, a drain electrode and a second insulating layer on the surface of the needle-shaped source electrode to obtain a needle-shaped device;
polishing a tip portion of the needle-type device to obtain a cross section including a source electrode, a first insulating layer, a drain electrode and a second insulating layer;
and arranging a channel connecting layer between the source electrode and the drain electrode of the section to obtain the field effect transistor biosensor.
The invention provides a field effect transistor biosensor, which comprises a source electrode in a needle shape, a first insulating layer arranged on the surface of the source electrode, a drain electrode arranged on the surface of the first insulating layer and a second insulating layer arranged on the surface of the drain electrode, wherein the source electrode is arranged on the surface of the first insulating layer; wherein a tip portion of the field effect transistor biosensor is divided into a section including a source electrode, a first insulating layer, a drain electrode, and a second insulating layer, and the source electrode and the drain electrode of the tip portion are conducted through a channel connection layer. The field effect transistor biosensor provided by the invention is needle-shaped, and can be directly inserted into a living body to carry out real-time monitoring on biological signal molecules.
The invention provides a preparation method of the field effect transistor biosensor, which is simple to operate and can be prepared in batches.
Drawings
FIG. 1 is a schematic structural diagram of a field effect transistor biosensor provided in the present invention, in which 1 is a drain, 2 is an insulating layer, 2-1 is a first insulating layer, 2-2 is a second insulating layer, 3 is a source, and 4 is a channel connecting layer;
FIG. 2 is a graph showing transfer characteristics of the carbon nanotube field effect transistor biosensor prepared in example 1;
FIG. 3 is a graph showing an output characteristic of the biosensor of the carbon nanotube field effect transistor prepared in example 1;
fig. 4 is a graph showing transfer characteristics of the graphene field effect transistor biosensor prepared in example 2;
fig. 5 is a graph showing an output characteristic of the graphene field effect transistor biosensor prepared in example 2.
Detailed Description
The invention provides a field effect transistor biosensor, which comprises a source electrode in a needle shape, a first insulating layer arranged on the surface of the source electrode, a drain electrode arranged on the surface of the first insulating layer and a second insulating layer arranged on the surface of the drain electrode, wherein the source electrode is arranged on the surface of the first insulating layer; wherein a tip portion of the field effect transistor biosensor is divided into a section including a source electrode, a first insulating layer, a drain electrode, and a second insulating layer, and the source electrode and the drain electrode of the tip portion are conducted through a channel connection layer.
In the present invention, the material of the source electrode preferably includes stainless steel, gold, platinum, or copper, and more preferably stainless steel. The specific type of the stainless steel is not specially limited, and the requirement of actual safe use can be met. In the invention, the diameter of the source electrode is preferably 0.15-0.5 mm, and more preferably 0.2-0.4 mm. In the embodiment of the invention, a stainless steel acupuncture needle is used as a source electrode; the invention adopts the stainless steel acupuncture needle as the source electrode, has good rigidity and proper size, has small injury when being inserted into a living body, is convenient to purchase, has low price and is suitable for large-scale production.
In the present invention, the material of the drain is not particularly limited, and may be a material known to those skilled in the art, and in the present invention, the material of the drain preferably includes gold, platinum or copper, and more preferably gold. In the invention, the thickness of the drain electrode is preferably 3-5 μm, and more preferably 3-4 μm.
The insulating material for forming the first insulating layer and the second insulating layer is not particularly limited in the present invention, and any insulating material known to those skilled in the art may be used. In the present invention, the insulating material forming the first and second insulating layers preferably independently comprises parylene, an electrophoretic paint, or an epoxy resin, more preferably parylene. In the present invention, the thicknesses of the first insulating layer and the second insulating layer are independently preferably 4 to 10 μm, and more preferably 6 to 8 μm.
The invention has no special limitation on the thickness and the size of the channel connecting layer and the channel connecting material for forming the channel connecting layer, and can realize the conduction of the source electrode and the drain electrode. In the present invention, the channel connection material preferably includes a semiconductor material, and more preferably includes a carbon nanotube, graphene, molybdenum disulfide, or a silicon nanowire. The present invention is not particularly limited to the specific kind of semiconductor material, and commercially available products known to those skilled in the art may be used.
FIG. 1 is a schematic structural diagram of a field effect transistor biosensor provided in the present invention, in which 1 is a drain, 2 is an insulating layer, 2-1 is a first insulating layer, 2-2 is a second insulating layer, 3 is a source, and 4 is a channel connecting layer; the tip part of the field effect transistor biosensor is drawn out by a dotted line, and is an enlarged tip view, namely the structural schematic diagram of the cross section of the field effect transistor biosensor comprises a source electrode, a first insulating layer, a drain electrode, a second insulating layer and a channel connecting layer, the drain electrode, the first insulating layer, the source electrode and the second insulating layer are arranged from inside to outside in sequence, and the source electrode and the drain electrode are conducted through the channel connecting layer. In fig. 1, in order to more clearly show the positional relationship of the layers, the lengths of the drain electrode, the first insulating layer, the second insulating layer, and the source electrode are set to be stepped.
The invention provides a preparation method of the field effect transistor biosensor, which comprises the following steps:
sequentially depositing a first insulating layer, a drain electrode and a second insulating layer on the surface of the needle-shaped source electrode to obtain a needle-shaped device;
polishing a tip portion of the needle-type device to obtain a cross section including a source electrode, a first insulating layer, a drain electrode and a second insulating layer;
and arranging a channel connecting layer between the source electrode and the drain electrode of the section to obtain the field effect transistor biosensor.
According to the invention, the first insulating layer, the drain electrode and the second insulating layer are sequentially deposited on the surface of the needle-shaped source electrode to obtain the needle-shaped device. The invention has no special limitation on the specific method and operation parameters for depositing the first insulating layer, the drain electrode and the second insulating layer, and the first insulating layer, the drain electrode and the second insulating layer with required thicknesses can be obtained by adopting a deposition method well known by the technical personnel in the field; the invention preferably adopts a chemical vapor deposition method to deposit the first insulating layer and the second insulating layer, and adopts an electroplating method to deposit the drain electrode.
After the pin type device is obtained, the present invention polishes a tip portion of the pin type device to obtain a cross section including a source electrode, a first insulating layer, a drain electrode, and a second insulating layer. The invention has no special limitation on the polishing, and can ensure that a flat section is obtained. The size of the cross section is not particularly limited, and the source electrode and the drain electrode can be exposed, namely the cross section is ensured to comprise the source electrode, the first insulating layer, the drain electrode and the second insulating layer.
After the section comprising the source electrode, the first insulating layer, the drain electrode and the second insulating layer is obtained, the channel connecting layer is arranged between the source electrode and the drain electrode of the section, and the field effect transistor biosensor is obtained. The method for arranging the channel connecting layer is not particularly limited, and the conduction of the source electrode and the drain electrode can be realized. In the present invention, the method for disposing a channel connection layer preferably includes the steps of: dispersing the channel connecting material in dimethyl sulfoxide to obtain channel connecting material dispersion liquid with the concentration of 0.5-2 mg/mL; and coating the channel connecting material dispersion liquid between the source electrode and the drain electrode, and curing for 0.5-2 h at the temperature of 75-85 ℃. The coating amount of the channel connecting material dispersion liquid is not specially limited, and the source electrode and the drain electrode can be conducted by a channel connecting layer formed after curing.
The field effect transistor biosensor provided by the invention is in a needle shape, can be directly inserted into a living body to carry out real-time monitoring on biological signal molecules, and particularly, after the field effect transistor biosensor is prepared according to the scheme, corresponding antigen or antibody can be modified on a channel connecting material, and then the modified field effect transistor biosensor is directly inserted into the living body to carry out real-time monitoring on target molecules. The insertion mode or position of the modified field effect transistor biosensor is not specially limited, and the insertion mode or position can be selected according to actual needs; specifically, if the target molecules of the brain are detected, the brain stereotaxic apparatus is needed to be used for positioning, and the modified field effect transistor biosensor is inserted after the hole is drilled by the electric drill; if the target molecules in the muscle tissue are detected, the modified field effect transistor biosensor is directly inserted into the muscle tissue. In the embodiment of the invention, after the field effect transistor biosensor is prepared according to the scheme, a glutamic acid receptor can be modified on a channel connecting material, then the channel connecting material is positioned by using a brain stereotaxic apparatus, the modified field effect transistor biosensor is inserted after drilling by an electric drill, and release of a glutamate neurotransmitter in hippocampal tissues of the brain is monitored in real time.
The technical solution of the present invention will be clearly and completely described below with reference to the embodiments of the present invention. It is to be understood that the described embodiments are merely exemplary of the invention, and not restrictive of the full scope of the 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.
Example 1
Taking a stainless steel acupuncture needle (with the diameter of 0.2mm) as a source electrode, and depositing parylene as a first insulating layer on the surface of the source electrode by adopting a chemical vapor deposition method, wherein the thickness of the first insulating layer is 8 microns; plating gold on the surface of the first insulating layer by adopting an electroplating method to be used as a drain electrode, wherein the thickness of the gold is 5 mu m; depositing parylene on the surface of the drain electrode by adopting a chemical vapor deposition method to be used as a second insulating layer, wherein the thickness of the parylene is 8 mu m, and obtaining a needle-shaped device;
polishing a tip portion of the needle-type device to obtain a cross section including a source electrode, a first insulating layer, a drain electrode and a second insulating layer;
dispersing carbon nanotubes serving as a channel connecting material in dimethyl sulfoxide to obtain a carbon nanotube dispersion liquid with the concentration of 1 mg/mL;
and coating the carbon nano tube dispersion liquid between a source electrode and a drain electrode on the section, and then curing for 30min at the temperature of 80 ℃ to obtain the carbon nano tube field effect transistor biosensor.
Example 2
Taking a stainless steel acupuncture needle (with the diameter of 0.4mm) as a source electrode, and depositing parylene as a first insulating layer on the surface of the source electrode by adopting a chemical vapor deposition method, wherein the thickness of the first insulating layer is 6 microns; plating gold on the surface of the first insulating layer by adopting an electroplating method to be used as a drain electrode, wherein the thickness of the gold is 3 mu m; depositing parylene on the surface of the drain electrode by adopting a chemical vapor deposition method to be used as a second insulating layer, wherein the thickness of the parylene is 6 microns, and obtaining a needle-shaped device;
polishing a tip portion of the needle-type device to obtain a cross section including a source electrode, a first insulating layer, a drain electrode and a second insulating layer;
dispersing graphene serving as a channel connecting material in dimethyl sulfoxide to obtain graphene dispersion liquid with the concentration of 1 mg/mL;
and coating the graphene dispersion liquid between a source electrode and a drain electrode on the section, and curing for 2 hours at 80 ℃ to obtain the graphene field effect transistor biosensor.
The electrical properties of the carbon nanotube field effect transistor biosensor and the graphene field effect transistor biosensor prepared in examples 1 and 2 were measured as follows:
fig. 2 is a graph showing a transfer characteristic of the carbon nanotube field effect transistor biosensor prepared in example 1, and fig. 3 is a graph showing an output characteristic of the carbon nanotube field effect transistor biosensor prepared in example 1. As can be seen from fig. 2, the carbon nanotube field effect transistor biosensor has typical p-type doping characteristics, which proves its potential to be used as a sensor; as can be seen from FIG. 3, as the gate voltage increases from-0.6V to 0.2V, the leakage current decreases, indicating that the CNT FET biosensor has n-type doping characteristics and is very sensitive to the variation of the gate voltage control current. Therefore, the carbon nano tube field effect transistor biosensor provided by the invention has good electrical properties, and lays a foundation for the subsequent application in real-time monitoring of living bodies.
Fig. 4 is a graph showing a transfer characteristic of the graphene field effect transistor biosensor prepared in example 2, and fig. 5 is a graph showing an output characteristic of the graphene field effect transistor biosensor prepared in example 2. As can be seen from FIG. 4, the graphene field effect transistor biosensor has a significant bipolar characteristic in a small range of gate voltage (-0.4V to 0.8V); as can be seen from FIG. 5, as the gate voltage decreases from 0.3V to-0.1V, the leakage current also decreases, which indicates that the graphene field effect transistor biosensor has p-type doping characteristics and is very sensitive to the change of the gate voltage regulation current. Therefore, the graphene field effect transistor biosensor provided by the invention has good electrical properties, and lays a foundation for the subsequent application in real-time monitoring of living bodies.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Claims (8)
1. A field effect transistor biosensor is characterized by comprising a source electrode in a needle shape, a first insulating layer arranged on the surface of the source electrode, a drain electrode arranged on the surface of the first insulating layer and a second insulating layer arranged on the surface of the drain electrode; the field effect transistor biosensor comprises a field effect transistor biosensor, a first insulating layer, a drain electrode and a second insulating layer, wherein the tip part of the field effect transistor biosensor is divided into a section comprising the source electrode, the first insulating layer, the drain electrode and the second insulating layer, and the source electrode and the drain electrode of the tip part are conducted through a channel connecting layer; the source electrode is made of stainless steel, and the diameter of the source electrode is 0.15-0.5 mm.
2. The FET biosensor of claim 1, wherein the drain electrode comprises gold, platinum, or copper.
3. The field effect transistor biosensor according to claim 1 or 2, wherein the thickness of the drain electrode is 3 to 5 μm.
4. The field effect transistor biosensor of claim 1, wherein the insulating materials forming the first and second insulating layers independently comprise parylene, an electrophoretic paint, or an epoxy.
5. The field effect transistor biosensor according to claim 1 or 4, wherein the first and second insulating layers independently have a thickness of 4 to 10 μm.
6. The field effect transistor biosensor as in claim 1, wherein the channel connection material forming the channel connection layer comprises a semiconductor material.
7. The field effect transistor biosensor in accordance with claim 6, wherein the semiconductor material comprises carbon nanotubes, graphene, molybdenum disulfide, or silicon nanowires.
8. A method for producing the field effect transistor biosensor as claimed in any one of claims 1 to 7, comprising the steps of:
sequentially depositing a first insulating layer, a drain electrode and a second insulating layer on the surface of the needle-shaped source electrode to obtain a needle-shaped device;
polishing a tip portion of the needle-type device to obtain a cross section including a source electrode, a first insulating layer, a drain electrode and a second insulating layer;
and arranging a channel connecting layer between the source electrode and the drain electrode of the section to obtain the field effect transistor biosensor.
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| CN112697843B (en) * | 2020-12-08 | 2023-10-03 | 湘潭大学 | Carbon-based field effect transistor sensor based on negative capacitance effect |
| CN114674897B (en) * | 2022-03-28 | 2023-06-06 | 深圳大学 | Probe-type organic electrochemical transistor sensor for detecting single-cell extracellular pH value, preparation method thereof and detection method thereof |
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| CN101975807A (en) * | 2010-09-09 | 2011-02-16 | 天津大学 | Three-dimensional Pt-Pb nano floricome type enzyme-free glucose sensor electrode as well as preparation and application thereof |
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| CN101975807A (en) * | 2010-09-09 | 2011-02-16 | 天津大学 | Three-dimensional Pt-Pb nano floricome type enzyme-free glucose sensor electrode as well as preparation and application thereof |
| CN108680635A (en) * | 2018-05-22 | 2018-10-19 | 中国科学院烟台海岸带研究所 | One kind can be used for Cu2+Functionalized modification acupuncture pin electrode of detection and preparation method thereof |
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