CN114113244A - Biochemical sensor for double-channel detection - Google Patents
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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
- G01N27/02—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance
- G01N27/22—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance by investigating capacitance
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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
- G01N27/02—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance
- G01N27/22—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating impedance by investigating capacitance
- G01N27/226—Construction of measuring vessels; Electrodes therefor
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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
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- G—PHYSICS
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- G01N27/30—Electrodes, e.g. test electrodes; Half-cells
- G01N27/327—Biochemical electrodes, e.g. electrical or mechanical details for in vitro measurements
- G01N27/3275—Sensing specific biomolecules, e.g. nucleic acid strands, based on an electrode surface reaction
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- G01N27/403—Cells and electrode assemblies
- G01N27/414—Ion-sensitive or chemical field-effect transistors, i.e. ISFETS or CHEMFETS
- G01N27/4145—Ion-sensitive or chemical field-effect transistors, i.e. ISFETS or CHEMFETS specially adapted for biomolecules, e.g. gate electrode with immobilised receptors
Abstract
The invention relates to an analytical biochemical sensor based on two-dimensional material quantum capacitance-conductance dual-channel detection, which comprises the following components: comprises a substrate and a solution; a two-dimensional material layer is arranged on the substrate; the two ends of the two-dimensional material layer are provided with a source electrode and a drain electrode to form a two-dimensional material in-plane conductance detection sensing channel; the solution is provided with a liquid gate electrode, and the liquid gate electrode and the two-dimensional material layer form an out-of-plane quantum capacitance detection sensing channel. The sensor couples the excellent conductivity of the two-dimensional material with the quantum capacitance characteristic of the two-dimensional material, constructs a biochemical detection device which can decouple the conductivity of the two-dimensional material and analyze the change of the carrier concentration and the mobility of the two-dimensional material, does not need to carry a permanent magnet necessary for Hall analysis, can be compatible with a semiconductor process and portable field detection requirements, and provides feasibility for the application of the sensor in portable ion detection and the like.
Description
Technical Field
The invention relates to the technical field of biochemical detection, and particularly provides an analytical two-dimensional material biochemical sensor based on quantum capacitance-conductance dual-channel detection and application thereof in ion detection.
Background
Large scale application of mobile communication and miniature electronic equipment, and phaseThe increasing popularity of interconnect technology in industry and everyday life puts new demands on the development of compact sensor devices for use in various environments. And new nano materials are receiving more and more attention as the basis for developing the core functional components of the next generation of sensors. By accurately regulating and controlling the physical and chemical properties of the nano-materials, ultra-sensitive detection can be realized aiming at a specific sensing target. By graphene and MoS2And the like are an important class of these novel materials. Since the graphene was prepared for the first time in 2004, due to the excellent electrical characteristics and good biocompatibility, stability and the like of the graphene two-dimensional material, the Gr-FET has unique advantages in IVD medical detection and detection applications of environmental target molecules: i) all atoms of the two-dimensional material are positioned on the surface, so that the two-dimensional material is extremely sensitive to environmental changes and has high detection sensitivity; ii) its sensing principle is based on the detection of the charge of the target biochemical molecule by field effect. The adsorption of biochemical molecules on the surface of the two-dimensional material is fast, and meanwhile, the electric signal detection has real-time performance, so that the detection time is short, and the on-line fast detection can be realized. Meanwhile, in recent years, the high-quality and large-area preparation technology of graphene has been greatly improved, and the industry has realized the controllable preparation of wafer-level graphene chips, so that the scenes of graphene applied to various biochemical sensors no longer only stay in a laboratory. For example, Nanosens, USA, incorporated Gr-FET and CRISPR-Cas9 gene editing technology [ nat. Bio. Eng., https:// doiDOI:. org/10.1038/s 41551-019-0371-x-]Without any pre-amplification treatment, the detection limit of the specific gene mutation of the muscular dystrophy genome in a short time can be compared with or even superior to that of technologies such as PCR fluorescence and the like. Recently, an article for rapid (1 minute) clinical detection of SARS-CoV-2 virus using graphene transistors was published in the well-known journal ACS Nano. The detection sensitivity of the kit to clinical samples reaches 243copies/mL, and a direct basis is provided for realizing a compact and rapid diagnosis system based on a two-dimensional material [ ACS Nano, DOI: 10.1021/acsnano.0c02823]。
The existing two-dimensional material field effect biochemical sensor mainly detects the (de) adsorption and (de) combination process of biomarkers on the surface of a two-dimensional material by means of the change of a two-dimensional material conductance (or resistance) signal. However, in such a complex surface interaction process, the charged biomarker can not only affect the carrier concentration of the two-dimensional material through the field effect, but at the same time, it may act as a scattering center to change the carrier mobility of the two-dimensional material. Thus, classical conductance (or resistance) tests cannot distinguish between changes in carrier concentration and mobility of two-dimensional materials, and cannot ascertain the charge or scattering mechanisms of biosensing. I.e. a critical sensing process of analyzing the interaction between the biomolecules and the surface of the two-dimensional material, represents a great limitation. The carrier concentration and the mobility of the two-dimensional material can be respectively obtained by utilizing a semiconductor Hall effect, so that the biochemical sensing mechanism of the material is distinguished [ adv.Funct.Mater.2013,23,2301 ]. However, hall tests generally need to carry heavy permanent magnets [ adv, funct, mater, 2013,23,2301], which makes it difficult to meet the requirements of portable measurement on safety.
Disclosure of Invention
To solve the above problems, the applicant provides:
in one aspect, the application provides an analytical two-dimensional material biochemical sensor based on quantum capacitance-conductance dual-channel detection, which is characterized in that the analytical two-dimensional material biochemical sensor comprises two sensing channels of two-dimensional material quantum capacitance detection and conductance detection.
Further, the analytical two-dimensional material biochemical sensor includes a substrate and a solution; a two-dimensional material layer is arranged on the substrate; the two ends of the two-dimensional material layer are provided with a source electrode and a drain electrode to form a two-dimensional material in-plane conductance detection sensing channel; the solution is provided with a liquid gate electrode, and the liquid gate electrode and the two-dimensional material layer form an out-of-plane quantum capacitance detection sensing channel.
Further, the solution is dropped on or placed in the substrate provided with the two-dimensional material layer.
Further, the source and drain electrode material is selected from gold, platinum, silver, copper or aluminum.
Further, the liquid gate electrode is selected from Ag/AgCl, Hg/Hg2SO4Reversible hydrogen electrode
Further, the two-dimensional material is selected from; graphene, reduced graphene oxide, molybdenum disulfide, or boron nitride; the two-dimensional material is transferred to the substrate by a wet method or a dry method; or directly growing on insulating sapphire or covered with insulating SiO by CVD method2A layer of silicon wafer substrate.
Further, the substrate is selected from silicon, cellulose acetate or polyethylene terephthalate.
Further, the substrate is a silicon substrate; growing a single-layer graphene thin layer by using a CVD (chemical vapor deposition) method by using a metal foil as a substrate, and transferring the graphene thin layer to the silicon substrate by using a PMMA (polymethyl methacrylate) method; the liquid gate electrode is an Ag/AgCl pseudo-reference electrode; the solution is phosphate buffer solution with the pH value of 6.5-7.5; the substrate provided with the two-dimensional material layer is placed in the solution.
Or, the substrate is a PET substrate; transferring the molybdenum disulfide thin layer to a substrate; the liquid gate electrode is Hg/Hg2SO4An electrode; the solution is phosphate buffer solution with the pH value of 6.5-7.5; and dripping the solution on a substrate provided with a two-dimensional material layer.
Alternatively, the substrate is a cellulose acetate substrate; transferring the boron nitride thin layer onto a substrate; the liquid gate electrode is a reversible hydrogen electrode; the solution is phosphate buffer solution with the pH value of 6.5-7.5; and dripping the solution on a substrate provided with a two-dimensional material layer.
In another aspect, the present application provides an ion detection or analysis method using the above analysis type two-dimensional material biochemical sensor, characterized in that the method comprises: scanning different grid voltages to obtain quantum capacitance and conductance characteristic curves of the device; the concentration of ions to be measured is changed to obtain a quantum capacitance and conductance characteristic curve after concentration change, and a concentration-dependent two-dimensional material conductance, carrier concentration and mobility characteristic curve is obtained after decoupling.
Further, the ion may be selected from hydrogen ion, ammonium ion, lithium ion, potassium ion, sodium ion, calcium ion, magnesium ion, aluminum ion, manganese ion, zinc ion, chromium ion, iron ion, ferrous ion, arsenic ion, lead ion, copper ion, cuprous ion, mercury ion, silver ion, hydroxide ion, nitrate ion, chloride ion, sulfate ion, sulfite ion, sulfide ion, carbonate ion, silicate ion, and phosphate ion.
The field effect transistor device of the present application employs a conventional classical top-gate bottom-contact structure device, including a gate, a source, and a drain.
Besides the above materials, the liquid gate electrode may be made of a known material such as platinum wire, gold wire, or graphite electrode, as required.
In addition to the above materials, the two-dimensional material may be selected from known usable materials such as silylene, germanene, phospholene, borolene, stannylene, boron nitride, tungsten disulfide, rhenium diselenide, molybdenum carbide, ditungsten carbide, tungsten carbide, tantalum carbide, a compound having a metal-organic skeleton, a compound having a covalent-organic skeleton, a layered double hydroxide, and an oxide, as needed.
Besides the materials, the substrate can be made of plastics, glass, sapphire, silicon chips plated with silicon dioxide, polyethylene, polypropylene, polybutylene, polystyrene, polyvinyl chloride, polyisobutylene, polyacrylonitrile, polyurethane, polymethyl methacrylate, polymethyl acrylate, polyvinyl acetate, polybutylene terephthalate, polycarbonate and urea resin according to the needs, melamine-formaldehyde resin, melamine urea-formaldehyde resin, phenol resin, epoxy resin, polyoxymethylene, polyethylene oxide, polyhexamethylene adipamide, polycaprolactam, polyimide, polydimethylsiloxane, acrylonitrile-styrene-butadiene copolymer, styrene-butadiene-styrene block copolymer, butyl rubber, butadiene isoprene copolymer, cotton fiber, hemp fiber, wood fiber, grass fiber, and the like are known as usable materials.
Advantageous effects
The invention provides a quantum capacitance-conductance two-channel analysis type two-dimensional material biosensor, which is used for simultaneously testing two-dimensional material quantum capacitance and conductance sensing channels, so that the change of carrier concentration and mobility of the biosensor is distinguished, and the charge or scattering mechanism of the biosensor is proved. The analytical two-dimensional material biosensor based on the quantum capacitance-conductance dual-channel detection, which is constructed by the invention, is compatible with the semiconductor process and portable field detection requirements (without carrying a permanent magnet required by the traditional semiconductor Hall detection). In addition, the portable analysis type two-dimensional material biochip constructed based on the precise electrical detection technology has strong cost competitiveness, has a simple operation flow, avoids complex steps such as fluorescence labeling and amplification, does not need expensive optical instruments, saves the cost of time, manpower and material resources and the like, and provides new research ideas and technical guidance for ion detection and screening of various biomarkers (the detection limit can reach or is superior to the fM magnitude).
Drawings
FIG. 1 is a schematic diagram of the structure and electrical connections of an analytical biochemical sensor based on a two-dimensional material according to the present invention;
fig. 2A, B is a transfer characteristic curve and a capacitance curve before and after hydrogen ion detection on the surface of the two-dimensional graphene-based analytical biochemical sensor according to the present invention;
FIG. 3 is a time-dependent field effect characteristic diagram of an analytic biochemical sensor surface of two-dimensional graphene material according to the present invention for detecting hydrogen ions of different concentrations;
FIG. 4A, B shows the surface detection K of the analytical biochemical sensor based on two-dimensional material molybdenum disulfide according to the present invention+A transfer characteristic curve and a capacitance curve before and after the ion;
FIG. 5 is an analytical biochemical sensor surface of the two-dimensional material molybdenum disulfide of the present invention for detecting different concentrations of K+Time-dependent field effect profile of the ions;
FIG. 6A, B shows the detection of Mg on the surface of an analytical biochemical sensor based on two-dimensional material tungsten disulfide according to the invention2+A transfer characteristic curve and a capacitance curve before and after the ion;
FIG. 7 is an analytical biochemical sensor surface of the two-dimensional material tungsten disulfide of the present invention for detecting Mg at different concentrations2+Time-dependent field effect profile of ions。
Detailed Description
In order that the objects, features and advantages of the invention will become more apparent, the following detailed description of the embodiments of the invention, taken in conjunction with the accompanying drawings, set forth in detail below in order that the invention may be fully understood, but the invention may be practiced in many ways other than as described below. Accordingly, the invention is not limited by the specific implementations disclosed below.
Example 1. detection of hydrogen ions by a graphene field effect transistor based biochemical sensor.
Firstly, preparing a graphene field effect transistor
(1) Growing a single-layer graphene thin layer by using a CVD method by using a metal foil as a base, and transferring the graphene thin layer to a silicon substrate by using a traditional PMMA method.
(2) Patterning graphene by adopting a micro-nano processing technology, preparing source and gold leakage electrodes at two ends of a graphene layer, and then packaging a region outside a graphene thin layer;
(3) and (3) placing the graphene field effect transistor in a buffer solution (such as phosphate buffer solution) environment with the pH value of 6.5-7.5, and inserting an Ag/AgCl (pseudo) reference electrode to form a grid electrode.
Experiment process of applying quantum capacitance-conductance dual-channel analysis type graphene field effect transistor to hydrogen ion detection
(1) The source, drain and gate of the prepared graphene field effect transistor are connected to a lock-in amplifier capable of simultaneously carrying out dual-channel detection according to the phase shown in figure 1. One of the channels detects a current or voltage between a source and a drain of graphene, and the other channel detects an interface current or voltage between graphene and a gate solution.
(2) Changing the gate voltage V of grapheneref(e.g., scan range of-0.5V-0.3V) recording a channel under constant current source (e.g., I)ds-1 μ A) voltage V in the devicedsThe conductance (G, fig. 2 left) of the device is obtained through conversion by formula 1, that is, the transfer characteristic curve of the graphene device; record simultaneously anotherOne channel at constant voltage, e.g. VacCurrent and phase difference psi at-7.07 mV, converted by equation 2 to obtain the interface capacitance (C)inter) Curve with gate voltage (right in fig. 2). Through the transmission characteristic curve G (V)ref) Charge neutral points (CNPs, also called Dirac points) of graphene devices can be obtained, where V isDirac＝-90mV。
According to the transconductance g between the graphene source and the graphene drainmAnd the value of the interface capacitance (which can be taken here to be 2. mu.F/cm) away from the Dirac point2) The initial field effect carrier mobility and carrier density can be derived as:
μ＝gm/Cinter (3)
and
n＝G/eμ (4)
the hole of the graphene before ion detection is 1000cm through calculation2V.s, electron 1200cm2/V·s。
(4) Grid voltage, i.e. V, near the inflection point of the transfer characteristicrefAnd (3) testing the performance of detecting the hydrogen ion concentration of the material (50 mV), namely replacing the solution to be detected with different hydrogen ion concentrations to carry out real-time sensing test, and simultaneously monitoring and obtaining the conductance change and the interface capacitance change of the two-dimensional material to obtain a time-dependent field effect and a characteristic curve of the interface capacitance. Specifically, the grid electrode is inserted into a buffer solution (e.g., phosphate buffer solution) having a pH value of 3.5 to 7.5, and the pH value is electrically measured in real time from high to low in sequence. For example, 0.05mL of a buffer solution having a pH of 7.5 was added dropwise, and the voltage and current of the two channels in the device were recorded to obtain a time-dependent field effect and interface capacitance curve. Then, according to equations 3 and 4, the variation curves of the carrier mobility and the carrier concentration with the detection are obtained, as shown in fig. 3.
As can be seen from the data analysis, the adsorption of ions leads to: i) suppression of carrier mobility; ii) VrefIncrease in electron density when the voltage is 0V. This can be attributed to the displacement Δ V of the Dirac pointDirac-30 mV: when positively charged hydrogen ions are bound to the graphene surface, they move 30mV in the negative direction. The change in conductance due to carrier mobility and carrier density may be in the same direction or opposite. It is clear that conductance-based measurements alone do not describe a comprehensive picture of the biosensing response. That is, conventional conductance measurements by themselves cannot account for the complex changes in graphene conductance Δ G caused by carrier mobility or carrier density. And through the capacitance-conductance dual-channel analysis type graphene field effect transistor, the initial field effect carrier mobility and the carrier density can be deduced, and the complex change of the graphene conductance delta G caused by the carrier mobility or the carrier density is solved, so that more information is obtained. From the obvious peak appearing in fig. 3 when the solution with the pH to be measured is dropped, it can be seen that the immunosensor shows higher sensitivity in detecting different hydrogen ion concentrations compared with the conventional conductance signal.
Example 2. detection of potassium ions by a biochemical sensor based on a molybdenum disulfide field effect transistor.
Firstly, preparing a molybdenum disulfide field effect transistor
And transferring the molybdenum disulfide thin layer onto a polymer (such as a PET) substrate, and respectively welding a source electrode and a drain electrode at two ends of the molybdenum disulfide thin layer to encapsulate the region outside the molybdenum disulfide thin layer. Dropping buffer solution (such as phosphate buffer solution) with pH value of 6.5-7.5 onto the surface of molybdenum disulfide to obtain Hg/Hg2SO4And inserted into the droplets to form the gate.
Experiment process of applying capacitance-conductance double-channel analysis type molybdenum disulfide field effect transistor to potassium ion detection
(1) The source, drain and gate of the prepared molybdenum disulfide field effect transistor are connected to a phase-locked amplifier which can simultaneously carry out double-channel detection according to the phase shown in figure 1. One of the channels detects current or voltage between the source and drain electrodes through the molybdenum disulfide, and the other channel detects interface current or voltage between the molybdenum disulfide and the gate solution.
(2) Changing the gate voltage of molybdenum disulfide (such as scanning range of-0.3V-0.4V), recording the change curve of conductance to obtain the transmission characteristic curve G (V)ref) And neutral point, here VCNP60 mV. While the change in capacitance is recorded in the other channel, as shown on the left of fig. 4. (3) Calculating the initial carrier mobility and carrier density of the molybdenum disulfide before detection, wherein the hole is 40cm before ion detection2V.s, electron 36cm2/V·s。
(4) Grid voltage, i.e. V, near the inflection point of the transfer characteristicrefAnd (3) testing the performance of detecting the hydrogen ion concentration of the material (50 mV), namely performing real-time sensing test on the solution to be detected by replacing different potassium ion concentrations, and monitoring to obtain the conductance change of the two-dimensional material. Then, the performance of detecting the potassium ion concentration is tested, namely a time-dependent field effect characteristic curve is tested. The grid is inserted into a buffer (e.g., phosphate buffer) having a pH of 3.5-7.5, and the pH is sequentially measured electrically from high to low in real time. For example, 0.05mL of a buffer solution with pH 7.5 was added dropwise, the voltage in the device was recorded, and the data was normalized to obtain a time-dependent field effect characteristic curve, as shown in FIG. 5.
As can be seen from the data analysis, the adsorption of ions leads to: i) suppression of carrier mobility; ii) VrefIncrease in electron density when the voltage is 0V. This can be attributed to the displacement Δ V of the Dirac pointDirac-10 mV: when positively charged potassium ions are bound to the molybdenum disulphide surface, they move 50mV in the negative direction. The change in conductance due to carrier mobility and carrier density may be in the same direction or opposite. It is clear that conductance-based measurements alone do not describe a comprehensive picture of the biosensing response. That is, conventional conductivity measurements by themselves cannot account for the complex changes in molybdenum disulfide conductance Δ G caused by carrier mobility or carrier density. The capacitance-conductance dual-channel analysis type molybdenum disulfide field effect transistor can deduce the initial field effect carrier mobility and the carrier density, and the initial field effect carrier mobility or the carrier density is solvedResulting in a complex change in the conductance deltag of the molybdenum disulphide, thus obtaining more information. From the apparent peak in fig. 5, which appears when the solution with the pH to be measured is added dropwise, it can be seen that the immunosensor shows higher sensitivity in detecting different concentrations of potassium ions, compared to the conventional conductance signal.
Example 3. detection of magnesium ions by a biochemical sensor based on boron nitride field effect transistors.
Firstly, preparing a tungsten disulfide field effect transistor
And transferring the boron nitride thin layer onto a cellulose (such as cellulose acetate) substrate, and respectively welding a source electrode and a drain electrode at two ends of tungsten disulfide to encapsulate the area outside the boron nitride thin layer. And (3) dropwise adding a buffer solution (such as a phosphate buffer solution) with the pH value of 6.5-7.5 onto the surface of the boron nitride, and selecting a reversible hydrogen electrode as a reference electrode to be used as a grid electrode of the device.
Experimental process for applying capacitance-conductance dual-channel analysis type boron nitride field effect transistor to magnesium ion detection
(1) The source, drain and gate of the prepared tungsten disulfide field effect transistor are connected to a phase-locked amplifier which can simultaneously carry out double-channel detection according to the phase-locked amplifier shown in figure 1. One of the channels detects a current or voltage between the source and drain through which tungsten disulfide passes, and the other channel detects an interface current or voltage between tungsten disulfide and the gate solution.
(2) Changing the gate voltage of tungsten disulfide (such as scanning range of-0.5V-0.3V), recording the change curve of conductance to obtain the transmission characteristic curve G (V)ref) And neutral point, here VCNP-30 mV. While the change in capacitance is recorded in the other channel, as shown on the left of fig. 6.
(3) Calculating the initial carrier mobility and carrier density of tungsten disulfide before detection, wherein the hole is 30cm before ion detection2V.s, electron of 24cm2/V·s。
(4) Grid voltage, i.e. V, near the inflection point of the transfer characteristicrefTesting the performance of detecting the hydrogen ion concentration of the magnesium ion solution at 50mV, namely replacing the solution to be detected with different magnesium ion concentrations to carry out real-time sensing test, and simultaneously monitoring to obtain two-dimensionalThe conductance of the material changes. Then, the performance of detecting the concentration of the magnesium ions is tested, namely a time-dependent field effect characteristic curve is tested. And inserting the grid into a buffer solution (such as a phosphate buffer solution) with the pH value of 3.5-7.5, and sequentially carrying out real-time electrical measurement from high to low in the pH value. For example, 0.05mL of a buffer solution with pH 7.5 was added dropwise, the voltage in the device was recorded, and the data was normalized to obtain a time-dependent field effect characteristic curve, as shown in FIG. 7.
As can be seen from the data analysis, the adsorption of ions leads to: i) suppression of carrier mobility; ii) VrefIncrease in electron density when the voltage is 0V. This can be attributed to the displacement Δ V of the Dirac pointDirac-170 mV: when positively charged magnesium ions are bound to the tungsten disulfide surface, they move 170mV in the negative direction. The change in conductance due to carrier mobility and carrier density may be in the same direction or opposite. It is clear that conductance-based measurements alone do not describe a comprehensive picture of the biosensing response. That is, conventional conductance measurements by themselves cannot account for the complex changes in tungsten disulfide conductance Δ G caused by carrier mobility or carrier density. And through the capacitance-conductance dual-channel analysis type tungsten disulfide field effect transistor, the initial field effect carrier mobility and the carrier density can be deduced, and the complex change of tungsten disulfide conductance delta G caused by the carrier mobility or the carrier density is solved, so that more information is obtained. From the obvious peak in fig. 7, which appears when the solution with the pH to be measured is dropped, it can be seen that the immunosensor shows higher sensitivity in detecting different magnesium ion concentrations compared to the conventional conductance signal.
Claims (10)
1. An analytical two-dimensional material biochemical sensor based on quantum capacitance-conductance dual-channel detection is characterized by comprising two sensing channels of two-dimensional material quantum capacitance detection and conductance detection.
2. The analytical two-dimensional material biochemical sensor according to claim 1, comprising a substrate and a solution; a two-dimensional material layer is arranged on the substrate; the two ends of the two-dimensional material layer are provided with a source electrode and a drain electrode to form a two-dimensional material in-plane conductance detection sensing channel; the solution is provided with a liquid gate electrode, and the liquid gate electrode and the two-dimensional material layer form an out-of-plane quantum capacitance detection sensing channel.
3. The analytical two-dimensional material biochemical sensor according to claim 2, wherein the solution is dropped on or in the substrate provided with the two-dimensional material layer.
4. The analytical two-dimensional material biochemical sensor according to claim 2 or 3, wherein the source-drain electrode material is selected from gold, platinum, silver, copper, or aluminum.
5. The analytical two-dimensional material biochemical sensor according to any one of claims 2 to 4, wherein the liquid gate electrode is selected from the group consisting of Ag/AgCl, Hg/Hg2SO4And a reversible hydrogen electrode.
6. The analytical two-dimensional material biochemical sensor according to any one of claims 2 to 5, the two-dimensional material being selected from; graphene, reduced graphene oxide, molybdenum disulfide, or boron nitride; the two-dimensional material is transferred to the substrate by a wet method or a dry method; or directly growing on insulating sapphire or covered with insulating SiO by CVD method2A layer of silicon wafer substrate.
7. The analytical two-dimensional material biochemical sensor according to any one of claims 2 to 6, wherein the substrate is selected from silicon, cellulose acetate, or polyethylene terephthalate.
8. The analytical two-dimensional material biochemical sensor according to any one of claims 2 to 7, wherein the substrate is a silicon substrate; growing a single-layer graphene thin layer by using a CVD (chemical vapor deposition) method by using a metal foil as a substrate, and transferring the graphene thin layer to the silicon substrate by using a PMMA (polymethyl methacrylate) method; the liquid gate electrode is an Ag/AgCl pseudo-reference electrode; the solution is phosphate buffer solution with the pH value of 6.5-7.5; the substrate provided with the two-dimensional material layer is placed in the solution.
Or, the substrate is a PET substrate; transferring the molybdenum disulfide thin layer to a substrate; the liquid gate electrode is Hg/Hg2SO4An electrode; the solution is phosphate buffer solution with the pH value of 6.5-7.5; and dripping the solution on a substrate provided with a two-dimensional material layer.
Alternatively, the substrate is a cellulose acetate substrate; transferring the boron nitride thin layer onto a substrate; the liquid gate electrode is a reversible hydrogen electrode; the solution is phosphate buffer solution with the pH value of 6.5-7.5; and dripping the solution on a substrate provided with a two-dimensional material layer.
9. An ion detection or analysis method using the analysis type two-dimensional material biochemical sensor according to any one of claims 1 to 7, characterized in that the method comprises: scanning different grid voltages to obtain quantum capacitance and conductance characteristic curves of the device; the concentration of ions to be measured is changed to obtain a quantum capacitance and conductance characteristic curve after concentration change, and a concentration-dependent two-dimensional material conductance, carrier concentration and mobility characteristic curve is obtained after decoupling.
10. The method of claim 9, wherein the ion is selected from the group consisting of hydrogen ion, ammonium ion, lithium ion, potassium ion, sodium ion, calcium ion, magnesium ion, aluminum ion, manganese ion, zinc ion, chromium ion, iron ion, ferrous ion, arsenic ion, lead ion, copper ion, cuprous ion, mercury ion, silver ion, hydroxide ion, nitrate ion, chloride ion, sulfate ion, sulfite ion, sulfide ion, carbonate ion, silicate ion, and phosphate ion.
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