CN114384140A - Biosensor of graphene/tungsten telluride heterostructure and preparation method and application thereof - Google Patents
Biosensor of graphene/tungsten telluride heterostructure and preparation method and application thereof Download PDFInfo
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- G01N27/414—Ion-sensitive or chemical field-effect transistors, i.e. ISFETS or CHEMFETS
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Abstract
The invention belongs to the technical field of electronic core technology and biomedical engineering, relates to sensor manufacturing and molecular biological information detection, and particularly relates to a biosensor of a graphene/tungsten telluride heterostructure, a preparation method and application. The preparation method comprises the following steps: preparing a single-layer single-crystal graphene material on the surface of a metal foil, etching and removing the metal foil to obtain a single-layer single-crystal graphene film, transferring the single-layer single-crystal graphene film to the surface of conductive glass, etching a graphene channel on the single-layer single-crystal graphene film, and transferring the tungsten telluride film to enable the tungsten telluride film to be lapped on the graphene channel. The invention can realize the detection of DNA biomolecules.
Description
Technical Field
The invention belongs to the technical field of electronic core technology and biomedical engineering, relates to sensor manufacturing and molecular biological information detection, and particularly relates to a biosensor of a graphene/tungsten telluride heterostructure, and a preparation method and application thereof.
Background
The information in this background section is only for enhancement of understanding of the general background of the invention and is not necessarily to be construed as an admission or any form of suggestion that this information forms the prior art that is already known to a person of ordinary skill in the art.
According to the research of the inventor, the field effect biosensor based on graphene can be used for detecting biomolecules such as nucleic acid, protein, glucose and bacteria, and few reports are available about detecting DNA molecules. The research of the inventor finds that the graphene channel field effect transistor cannot distinguish whether a sample to be detected contains DNA molecules, so that the field effect biosensor based on graphene is difficult to detect the DNA molecules.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide a biosensor of a graphene/tungsten telluride heterostructure, a preparation method and application thereof2In combination, the sensitivity and stability of the field effect tube as a biosensor can be increased, thereby realizing the detection of DNA biomolecules.
In order to achieve the purpose, the technical scheme of the invention is as follows:
on the one hand, the biosensor of the graphene/tungsten telluride heterostructure comprises conductive glass, wherein a single-layer single-crystal graphene film is arranged on the surface of the conductive glass, a graphene channel is formed in the single-layer single-crystal graphene film, a tungsten telluride film is arranged on the graphene channel to form a top gate, and the graphene and the tungsten telluride form the graphene/tungsten telluride heterostructure.
On the other hand, the preparation method of the biosensor with the graphene/tungsten telluride heterostructure comprises the steps of preparing a single-layer single-crystal graphene material on the surface of a metal foil, etching and removing the metal foil to obtain a single-layer single-crystal graphene film, transferring the single-layer single-crystal graphene film to the surface of conductive glass, etching a graphene channel on the single-layer single-crystal graphene film, and transferring the tungsten telluride film to enable the tungsten telluride film to be lapped on the graphene channel.
In a third aspect, the application of the biosensor with the graphene/tungsten telluride heterostructure in detecting DNA molecules is provided.
The invention has the beneficial effects that:
1. the graphene/WTE in the biosensor with the graphene/tungsten telluride heterostructure provided by the invention2The heterojunction structure can enable the formed field effect transistor to have extremely high physical adsorption capacity and sensitivityThe detection capability of electrical signals, thereby being capable of realizing high-sensitivity detection of biomolecules such as DNA and the like.
2. The single-layer single-crystal graphene material prepared by the method has the advantages of uniform thickness and extremely high crystallization quality, so that the performance of the formed biosensor based on the field effect transistor can be ensured.
3. According to the invention, the channel is directly scribed on the single-layer single-crystal graphene film, so that new impurities are prevented from being introduced to the surface of the graphene, and the original performance of the graphene is ensured.
4. The preparation method is simple and controllable, and has low cost and high application value.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, are included to provide a further understanding of the invention, and are incorporated in and constitute a part of this specification, illustrate exemplary embodiments of the invention and together with the description serve to explain the invention and not to limit the invention.
FIG. 1 is an EDS diagram of a thin layer of tungsten telluride prepared in example 1 of the present invention;
FIG. 2 is a flow chart of a process for preparing a graphene/tungsten telluride heterostructure biosensor prepared in example 1 of the present invention;
FIG. 3 is a Scanning Electron Microscope (SEM) image of a graphene/tungsten telluride heterostructure in a graphene/tungsten telluride heterostructure biosensor prepared in example 1 of the present invention;
FIG. 4 is a representation diagram of DNA biomolecules detected by the graphene/tungsten telluride heterostructure biosensor prepared in example 1 of the present invention;
FIG. 5 is a characterization diagram of DNA biomolecules detected by the graphene channel field effect transistor prepared in comparative example 1 of the present invention.
Detailed Description
It is to be understood that the following detailed description is exemplary and is intended to provide further explanation of the invention as claimed. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of exemplary embodiments according to the invention. As used herein, the singular forms "a", "an" and "the" are intended to include the plural forms as well, and it should be understood that when the terms "comprises" and/or "comprising" are used in this specification, they specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof, unless the context clearly indicates otherwise.
The invention provides a biosensor with a graphene/tungsten telluride heterostructure, and a preparation method and application thereof, in view of the fact that a graphene channel field effect transistor cannot distinguish whether a sample to be detected contains DNA molecules.
The invention provides a biosensor with a graphene/tungsten telluride heterostructure, which comprises conductive glass, wherein a single-layer single-crystal graphene film is arranged on the surface of the conductive glass, a graphene channel is formed in the single-layer single-crystal graphene film, a tungsten telluride film is arranged on the graphene channel to form a top gate, and the graphene and the tungsten telluride form the graphene/tungsten telluride heterostructure.
In another embodiment of the invention, a method for preparing a biosensor with a graphene/tungsten telluride heterostructure is provided, which includes preparing a single-layer single-crystal graphene material on a surface of a metal foil, etching the metal foil to remove the metal foil to obtain a single-layer single-crystal graphene film, transferring the single-layer single-crystal graphene film to a surface of conductive glass, etching a graphene channel on the single-layer single-crystal graphene film, and transferring the tungsten telluride film to enable the tungsten telluride film to be lapped on the graphene channel.
In some examples of this embodiment, a single layer of single crystal graphene material is prepared on the surface of a metal foil using Chemical Vapor Deposition (CVD). The single-layer single-crystal graphene material is generally prepared from methane.
In one or more embodiments, the process for preparing the single-layer single-crystal graphene material by using the chemical vapor deposition method comprises the following steps: heating the metal foil under the vacuum condition, introducing hydrogen into the metal foil, raising the temperature for annealing, introducing methane for chemical vapor deposition, stopping introducing the methane, cooling, and finally stopping introducing the hydrogen and stopping heating.
The chemical vapor deposition method for growing the single-layer single-crystal graphene requires controlling the time for introducing methane and the annealing time of the copper foil. If the annealing time is too short, the oxide on the surface of the copper foil can not be removed cleanly, and the production quality of the graphene is further influenced. Thus, in one or more embodiments, the time for the annealing treatment is not less than 1 hour. However, if the annealing time is too long, the copper foil is sublimated too much, which results in excessive waste. Therefore, the time of the annealing treatment is preferably 1 to 1.5 hours. The flow rate of hydrogen gas is 45-55 sccm. Can ensure that the growth of the single-layer single crystal graphene is good.
In one or more embodiments, the temperature before the hydrogen gas is introduced into the metal foil is 190-210 ℃.
In one or more embodiments, the annealing treatment is performed at a temperature of 950 to 1050 ℃.
If the time for introducing methane is too short, graphene cannot form a film, and if the time is too long, double-layer graphene or even multi-layer graphene can grow. Thus, in one or more embodiments, the time for introducing the methane is 25-35 min. The flow rate of the methane is 45-55 sccm. Can ensure that the growth of the single-layer single crystal graphene is good. Particularly, when the flow rate ratio of hydrogen to methane is 1: 0.9-1.1, the growth of the single-layer single-crystal graphene can be better ensured.
And the temperature reduction process of stopping introducing the methane is a process of reducing the heating temperature, and when the introduction of the hydrogen is stopped, the heating is stopped, and natural cooling is carried out.
In some examples of this embodiment, the solution in which the metal foil is etched is a ferric chloride solution.
In some examples of this embodiment, a tungsten steel needle is used to scribe a channel in the middle of the single-layer single-crystal graphene thin film as a graphene channel. The channel in the middle of the graphene is realized by means of the tungsten steel needle, and the position, the direction and the force for fixing the action of the tungsten steel needle are all important. In one or more embodiments, the tungsten steel needle and the surface of the single-layer single-crystal graphene film form an included angle of 45 +/-0.5 degrees, and the same force is used and the straight line is kept.
In some examples of this embodiment, the process of transferring the tungsten telluride film to overlap the graphene channel is: and transferring the tungsten telluride film to a thermal release adhesive tape, dropping the thermal release adhesive tape on the graphene channel in an overlapping manner, heating to release the tungsten telluride film on the thermal release adhesive tape, and removing the thermal release adhesive tape to enable the tungsten telluride film to be overlapped on the graphene channel.
The metal foil of the present invention is preferably a copper foil.
In a third embodiment of the invention, the application of the biosensor with the graphene/tungsten telluride heterostructure in the detection of DNA molecules is provided.
In order to make the technical solutions of the present invention more clearly understood by those skilled in the art, the technical solutions of the present invention will be described in detail below with reference to specific embodiments.
Example 1
Two-dimensional graphene/WTE2The preparation method of the heterostructure biosensor, as shown in fig. 2, comprises the following steps:
growing a single-layer single-crystal graphene material on a copper foil by a Chemical Vapor Deposition (CVD) method.
1.1, washing the copper foil three times by using acetone and dilute hydrochloric acid, and then thoroughly washing the copper foil three times by using deionized water, thereby removing organic matters and an oxidation layer on the surface of the copper foil.
1.2 the cleaned copper foil is placed in the middle temperature uniform area of the quartz tube, the vacuum tube furnace is closed, and the air tightness is checked.
1.3 evacuation of the tube to 5X 10 by means of a molecular pump-3Torr。
1.4 the temperature was raised to 200 ℃ and then hydrogen gas was introduced at a flow rate of 50sccm and the gas pressure was changed to 3X 10-1Torr。
After the temperature of 1.5 is raised to 1000 ℃, the temperature is maintained for 1h for annealing treatment of the copper foil.
1.6 after completion of the annealing, methane gas was introduced at a flow rate of 50sccm and the gas pressure was changed to 5X 10-1The temperature and flow rate were maintained at Torr for 30min, after which the methane gas was turned off.
And 1.7, closing the hydrogen and the heater when the temperature is reduced to 100 ℃, taking out the copper foil on which the single-crystal single-layer graphene film grows after natural cooling to room temperature, and storing the material under a vacuum condition.
And secondly, scribing a graphene channel.
2.1 the copper foil with the single-layer single-crystal graphene film is placed in a molten iron chloride solution with the mass fraction of 21% for etching.
2.2 after etching for 40 minutes, the copper is completely corroded, and the transparent graphene film floats on the solution.
2.3 transferring the single-layer single-crystal graphene film into deionized water for cleaning, cleaning once every 10min, cleaning three times in total, and cleaning FeCl on the graphene3And (4) remaining.
2.4, transferring the graphene to a glass substrate with an Indium Tin Oxide (ITO) electrode, after the graphene is naturally dried, scribing a small-size (15 mu m) channel in the middle of the graphene by using a tungsten steel needle under a microscope, wherein in the scribing process, the tungsten steel needle and the surface of the graphene form an included angle of 45 degrees, and the same force is used and a straight line is kept.
(III) transfer WTE2And realizing heterojunction.
3.1 use blue film tape from WTE2Obtaining a thin layer WTE on the crystal2As shown in fig. 1.
3.2 select thin and uniform WTE2Transfer to PDMS thermal release tape.
3.3 utilize high accuracy two-dimensional transfer system to build heterojunction: corresponding WTE2And after the position of the trench, dropping the heat release tape on the graphene, heating to 85 ℃, and lifting the heat release tape, WTE2Remaining on the graphene to form graphene/WTE2Heterojunction, as shown in FIG. 3, to obtain two-dimensional graphene/WTE2A heterostructure biosensor.
Comparative example 1
The preparation process of the graphene channel field effect transistor is as follows:
(A) placing the copper foil with the single-layer single-crystal graphene film on 21 mass percent of ferric chloride (FeCl)3) Etching in aqueous solution.
(B) After 40 minutes, the copper substrate was completely corroded, and the transparent graphene film floated on the solution.
(C) Cleaning FeCl on graphene by using deionized water3And (4) remaining.
(D) And transferring the graphene to a glass substrate with an Indium Tin Oxide (ITO) electrode, waiting for natural drying, and obtaining a channel with the size of 15um in the middle of the graphene by using a tungsten steel needle under an optical microscope.
(E) Using blue film tape from WTE2Obtaining a thin layer WTE on the crystal2。
(F) Selecting thin and uniform WTE2Transfer to PDMS thermal release tape.
(G) And (3) building a heterojunction by using a high-precision two-dimensional transfer system: after the position of the WTE2 and the channel is corresponded, the heat release adhesive tape is dropped on the graphene, the graphene is heated to 85 ℃, the heat release adhesive tape is lifted, the WTE2 is left on the graphene, and graphene/WTE is formed2A heterojunction.
(H) Adhering the transparent groove to the graphene/WTE by using purple light adhesive2And one side of the heterojunction is used as a liquid top gate.
Performing DNA detection on the biosensor prepared in example 1 and the graphene channel field effect transistor prepared in comparative example 1, wherein the detection process comprises the following steps:
the voltage-current across the device in different environments was measured using a gishili 4200-SCS semiconductor characterization system.
(A) Measurements were performed directly in the initial environment (PBS solution) to give a set of voltage-current.
(B) Adding 10nM PBASE solution to react with graphene for six hours, removing redundant PBASE by DMF, and measuring to obtain a group of voltage-electricity.
(C) Adding 1nM DNA to react with PBASE for sixteen hours, removing excess DNA with phosphate, deactivating the excess PBASE reaction group with 100nM ethanolamine, and measuring to obtain a set of voltage-current.
The detection results are shown in FIGS. 4-5, and in FIG. 4, it can be seen that graphene/WTE is shown2The slope of the voltage-current curve of the heterojunction field effect transistor in different environments has obvious change, namely the change can be clearly observed after the DNA molecules are added, and the existence of the DNA molecules can be detected. FIG. 5 shows that the voltage-current of the graphene channel FET in different environments has no obvious change, i.e., whether the graphene channel FET is in a state of being unable to distinguishContains a DNA molecule. Therefore, the biosensor with the graphene/tungsten telluride heterostructure prepared by the method can solve the problem that a graphene channel field effect transistor cannot distinguish DNA molecules.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. The biosensor of the graphene/tungsten telluride heterostructure is characterized by comprising conductive glass, wherein a single-layer single-crystal graphene film is arranged on the surface of the conductive glass, a graphene channel is formed in the single-layer single-crystal graphene film, a tungsten telluride film is arranged on the graphene channel to form a top gate, and the graphene and the tungsten telluride form the graphene/tungsten telluride heterostructure.
2. A preparation method of a biosensor with a graphene/tungsten telluride heterostructure is characterized by preparing a single-layer single-crystal graphene material on the surface of a metal foil, etching and removing the metal foil to obtain a single-layer single-crystal graphene film, transferring the single-layer single-crystal graphene film to the surface of conductive glass, etching a graphene channel on the single-layer single-crystal graphene film, and transferring the tungsten telluride film to enable the tungsten telluride film to be lapped on the graphene channel.
3. The method of claim 2, wherein the single-layer single-crystal graphene material is prepared on the surface of the metal foil by chemical vapor deposition.
4. The method of claim 3, wherein the chemical vapor deposition process for preparing the single-layer single-crystal graphene material comprises: heating the metal foil under the vacuum condition, introducing hydrogen into the metal foil, raising the temperature for annealing, introducing methane for chemical vapor deposition, stopping introducing the methane, cooling, and finally stopping introducing the hydrogen and stopping heating.
5. The method of claim 4, wherein the annealing time is not less than 1 hour; the time of the annealing treatment is preferably 1-1.5 h; preferably, the flow rate of the introduced hydrogen is 45-55 sccm;
or the temperature is 190-210 ℃ before the hydrogen is introduced into the metal foil;
or the annealing temperature is 950-1050 ℃.
6. The method for preparing a graphene/tungsten telluride heterostructure biosensor as claimed in claim 4, wherein the time for introducing methane is 25-35 min; preferably, the flow rate of the introduced methane is 45-55 sccm; preferably, the flow rate ratio of hydrogen to methane is 1: 0.9-1.1.
7. The method of claim 2, wherein the solution for etching the metal foil is ferric chloride solution.
8. The method of claim 2, wherein a tungsten steel needle is used to scribe a channel in the middle of the single-layer single-crystal graphene thin film as a graphene channel; preferably, the tungsten steel needle and the surface of the single-layer single-crystal graphene film form an included angle of 45 +/-0.5 degrees, and the tungsten steel needle and the surface of the single-layer single-crystal graphene film are kept in a straight line with the same force.
9. The method of claim 2, wherein the step of transferring the tungsten telluride film to the graphene channel by overlapping the tungsten telluride film thereon comprises: and transferring the tungsten telluride film to a thermal release adhesive tape, dropping the thermal release adhesive tape on the graphene channel in an overlapping manner, heating to release the tungsten telluride film on the thermal release adhesive tape, and removing the thermal release adhesive tape to enable the tungsten telluride film to be overlapped on the graphene channel.
10. Use of the biosensor of graphene/tungsten telluride heterostructure according to claim 1 or obtained by the preparation method according to any one of claims 2 to 9 in detecting DNA molecules.
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