CN102313765A - Biosensor base on zinc oxide and high electron mobility transistor and its preparation method - Google Patents
Biosensor base on zinc oxide and high electron mobility transistor and its preparation method Download PDFInfo
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Abstract
The invention provides a biosensor base on zinc oxide and high electron mobility transistor and its preparation method, which belongs to the nano-material application field. The invention is characterized by using a molecular beam epitaxy (MBE) system to prepare an AlGaAs/GaAsHEMT layered structure. A method of heat vapor plating is used to prepare a nickel/gold-germanium /nickel/gold alloy electrode, a silica insulating layer is deposited on the surface of the device to obtain the AlGaAs/GaAsHEMT. A gas-solid method is used for preparing T-ZnO. T-ZnO is modified on a grid electrode of HEMT and a bio-enzyme solution and a Nafion solution are added add drop by drop on a T-ZnO layer. The prepared device is placed at the low temperature for a period of time and then can detect the concentration of the solution to the corresponding biological solution. The invention has the advantage that the prepared device is capable of modifying different biological enzyme through the grid electrode to detect the concentration of the solution to the corresponding biological solution, and has the merits of high sensitivity, low detection limitation, wide detection scope, fast response speed, simple structure and stable performance, so that the biosensor provides the possibility to an practical application.
Description
Technical field
The invention belongs to fields of nano material application, semiconductor devices is combined with bio-measurement, both given full play to the summary responses of semiconductor devices, realized trace measurement again biomolecule.
Background technology
Along with the continuous development of nanometer science and technology, increasing achievement in research is applied to the bio-medical field.Realize trace measurement for biomolecule, can let us grasp and control the health condition of human body better.As the uric acid molecule is carried out trace measurement, we can prevent and treat suffering from gout person in advance, and its gouty probability is reduced greatly.And for example, can to potential diabetes a prevention in advance be arranged by let us, reduce the incidence probability of diabetes greatly the trace measurement of glucose molecule.Biology sensor has caused many biomaterial researchers' attention as the main matter carrier of detectable biomolecule microscopic concentration.Researchers have attempted diverse ways in order to obtain the detection limit of lower biomolecule.
In clinical, the measurement of these biomolecule used more at present the method for optical measurement.Measuring period is long, and complicated operation and detection limit are low to be the shortcoming of this method.Therefore researchers with energy dropped into seek more reliable, the method that measuring limit is lower.The method of measuring biomolecule is mainly through measuring the hydrogen peroxide that (1) reaction generates, the content of (2) dissolved oxygen, and the absorption spectrum of (3) product.Then be that the hydrogen peroxide that the main measuring quantitative response generates is measured biomolecule concentration by the three-electrode system of broad research at present.Though the biology sensor that three-electrode system constitutes is by big quantity research, the method that adopts semiconductor devices to combine with functional material is then seldom appeared in the newspapers.
HEMT (HEMT) is extensively applied to various noise amplifiers, frequency amplifier and microwave integrated circuit because it has high speed, high frequency and low noise performance characteristics.Its unique two-dimensional electron gas effect makes it that advantage incomparable with other semiconductor devices arranged on microscopic measurement.When the grid of HEMT because when adding biological solution and its two-dimensional electron gas passage is exerted an influence.Thereby make the drain current of HEMT change, change the concentration of coming detection of biological solution through measuring this.And having higher equipotential, the zinc paste (ZnO) that good electron transports performance and bio-compatible performance then becomes the biomaterial of function admirable.Wherein four-needle-like zinc oxide (T-ZnO) is considered to be used for fixing the ideal material of biomolecule because of its unique appearance structure has high specific surface area.
About utilization HEMT or T-ZnO seldom at the report of biomolecule field of measurement.(B. S. Kang, H. T. Wang, F. Ren et al. Appl. Phys. Lett 91. 2007,252103) such as the Kang of Univ Florida USA comes detecting glucose concentration with the HEMT that gallium nitride makes up with the method that the ZnO array combines.The Lei of University of Science & Technology, Beijing etc. (Y. Lei, X. Q. Yan, N. Luo et al. Colloids and Surfaces A, 2010, the working electrode of 361:169-173) modifying in traditional three-electrode system with T-ZnO is measured concentration of glucose.
Up to the present, HEMT applies to biological detection and also just combines its preparation technology's more complicated with the ZnO nano-array.And that T-ZnO is used for the research of biological detection is also just at the early-stage.The detection limit of the three-electrode system of modifying with T-ZnO is generally a microampere rank.
Summary of the invention
The present invention seeks in order to simplify HEMT grid modification process; Increase the influence of grid simultaneously to the two-dimensional electron gas passage; And the detection limit that further reduces biological solution is to receiving the peace rank, and the method that the HEMT that provides a kind of device to be made up by gallium arsenide (GaAs) combines with T-ZnO prepares bio-sensing.
A kind of based on zinc paste and HEMT biology sensor; Be characterised in that with AlGaAs/GaAs HEMT (HEMT) be substrate; And use micron order four-needle-like zinc oxide (T-ZnO), glucolase or uricase and Nafion to carry out grid successively and modify; The biosensor structure that is constituted is simple, stable performance, and response is sensitive.
Aforesaid preparation method realizes through following three steps:
1. through using EPI GEN-II type molecular beam epitaxy (MBE) system to prepare the layer structure of AlGaAs/GaAs HEMT.Wherein each layer structure is respectively: GaAs layer 1 μ m, AlGaAs layer 3 nm mix AlGaAs layer 22 nm of Si, mix GaAs cap layer 5 nm of Si.Use the method for hot vapor deposition to prepare the thick electrode (wherein the thickness of nickel/germanium gold/nickel/gold is respectively 500/2040/100/500 Ethylmercurichlorendimide) of nickel gold germanium nickel gold 100 nm then, the last thick silicon dioxide insulating layer of deposition 200 nm on electrode again.Can obtain AlGaAs/GaAs HEMT.
2. through using the gas-solid method to prepare four-needle-like zinc oxide (T-ZnO).Zinc powder and acetic acid zinc powder mixed at 10: 1 being placed in 660 ℃ of tubular furnace reaction 15 minutes with mol ratio, the flow velocity of Oxygen Flow and argon gas stream is respectively 300 sccm (standard cubic centimeter per minute) and 15 sccm.Can obtain the T-ZnO of average-size about 5 μ m at last.
3. T-ZnO is dissolved in ethanolic solution, evenly is coated on the grid of HEMT, at room temperature dry naturally, form the thick T-ZnO layer of 5 μ m.On the T-ZnO layer, drip glucolase or uricase then, and drip Nafion (U.S. ALDRICH company provides) solution immediately.Again the device for preparing is placed shading place 15 minutes, take out then and place 4 ℃ of refrigerators to preserve 24 hours, promptly can obtain glucose/uric acid biology sensor.
The HEMT that why selects GaAs to make up is because GaAs is small gap material (1.4 eV); When the electronics at gate surface place changes; Cap layer GaAs material can inspire electronics more easily and enter into the two-dimensional electron gas passage; Thereby the variation of gate surface is passed to the two-dimensional electron gas passage, finally causes the variation of grid current, realize detection biomolecule solution.
T-ZnO is easier to adsorb the biology enzyme molecule.When the biology enzyme molecule on being adsorbed on T-ZnO reacted with the biomolecule of being surveyed, the electron transfer that is produced made the equipotential of T-ZnO descend, thereby the surface of grid is changed, and finally makes drain current change.For the further electronic transport effect of performance T-ZnO in biology sensor, can use nanoscale T-ZnO to make up biology sensor.
In addition, owing to can use different biology enzyme molecules to come the grid of modified biological sensor, therefore can make up the biology sensor of surveying different biological solution concentration.For example, except can making up glucose/uric acid biology sensor, also can on the grid of biology sensor, modify lactalase and make up lactic biological sensor.
Come the method for the corresponding biological solution of modified biological sensor grid structure detection similar with other biology enzyme molecule with the method that makes up glucose/Uricase biosensor.Only need select for use specific biology enzyme molecule to modify with this step of biology enzyme molecular modification grid, constructed biology sensor promptly can be measured corresponding biological solution.
The invention has the advantages that:
1. sensor preparation technology is simple and easy, HEMT and T-ZnO is successfully combined to be used for biological solution survey.
2. biological solution detecting concentration detection limit drops to the nanomole level, and the response time of device is lower than 1 second.
3. sensor is easy to carry, and is easy to use.
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Description of drawings
Fig. 1 is with the prepared T-ZnO ESEM shape appearance figure of size about 5 μ m that comes out of gas-solid method.
Fig. 2 is by T-ZnO and the constructed biosensor structure synoptic diagram of HEMT.
Fig. 3 biosensor surface ESEM shape appearance figure; Illustration is represented biology enzyme and T-ZnO absorption shape appearance figure.
It is to be that the uric acid solution of 0.2 nM, 2 nM, 20 nM, 200 nM, 2 μ M, 20 μ M and 200 μ M is surveyed resulting current time graph of a relation to concentration respectively under 0.5 V at bias voltage that Fig. 4 uses constructed Uricase biosensor.
It is to be that the glucose solution of 0.3 nM, 3 nM, 30 nM, 300 nM, 3 μ M, 30 μ M and 300 μ M is surveyed resultant current time graph of a relation to concentration respectively under 0.5 V at bias voltage that Fig. 5 uses constructed glucolase biology sensor.
Embodiment:
Below in conjunction with object lesson technical scheme of the present invention is described:
Embodiment 1:
1. adopt the MBE technology to prepare the AlGaAs/GaAs HEMT, its specification is: the GaAs layer is that 1 μ m is thick, and the AlGaAs layer is that 3 nm are thick, and the AlGaAs layer of mixing Si is that 22 nm are thick, and the cap layer GaAs that mixes Si is that 5 nm are thick.Use the method for hot vapor deposition to prepare the thick electrode of nickel gold germanium nickel gold 100 nm then, the last thick silicon dioxide insulating layer of deposition 200 nm on electrode again, 0.5 * 5 mm is respectively reserved in both sides
2Do not cover the electrode of insulation course.
2. modify AlGaAs/GaAs HEMT gate surface with the four-needle-like zinc oxide of CVD method preparation size about 5 μ m then.The method of modifying is that the four-needle-like zinc oxide for preparing is evenly dispersed in the gate surface of HEMT through ethanol, and the zinc oxide film of formation is about 5 μ m.
3. the glucolase molecule that on zinc oxide film, drips activity and be 109 U/mg is modified, and drips Nafion and make its film forming fix these four-needle-like zinc oxides.Place refrigerator to preserve 24 hours the biology sensor of having modified biology enzyme, just can measure glucose solution.
4. carrying out need biology sensor being incubated 15 minutes in 37 ℃ of isoperibols before the glucose solution measurement.The method that adopts two electrodes of two probes and glucose biological sensors of electrochemical workstation (SI 1287) to constitute the measurement loop during measurement is measured, and the bias voltage of measurement is 0.5 V.Concentration is the grid that 7.4 glucose solution drops to the biology sensor modified successively from 0.3 nM to 0.3 mM pH, obtains the response signal of various concentration from electrochemical workstation.
Embodiment 2:
1. the first step is said among structure AlGaAs/GaAs HEMT institute's method of application such as the embodiment 1.
2. preparation four-needle-like zinc oxide, and it is said to modify among HEMT grid methods such as the embodiment 1 for second step with these zinc paste.
3. the uricase molecule that on zinc oxide film, drips activity and be 4.43 U/mg is modified, and drips Nafion and make its film forming fix these four-needle-like zinc oxides.Place refrigerator to preserve 24 hours the biology sensor of having modified biology enzyme, just can measure uric acid solution.
4. carrying out need biology sensor being incubated 15 minutes in 37 ℃ of isoperibols before the measurement of uric acid solution.The method that adopts two electrodes of two probes and uric acid biology sensors of electrochemical workstation (SI 1287) to constitute the measurement loop during measurement is measured, and the bias voltage of measurement is 0.5 V.Concentration is the grid that 7.02 uric acid solution drops to the biology sensor modified successively from 0.2 nM to 0.2 mM pH, obtains the response signal of various concentration from electrochemical workstation.
Claims (4)
1. one kind based on zinc paste and HEMT biology sensor; It is characterized in that being called for short HEMT with the AlGaAs/GaAs HEMT is substrate, and to use the micron order four-needle-like zinc oxide successively be that T-ZnO, glucolase or uricase and Nafion carry out grid and modify.
2. one kind prepares the said method based on zinc paste and HEMT biology sensor of claim 1, it is characterized in that:
Through using EPI GEN-II type MBE system to prepare the layer structure of AlGaAs/GaAs HEMT; Wherein each layer structure is respectively: GaAs layer 1 μ m, and AlGaAs layer 3 nm mix AlGaAs layer 22 nm of Si, mix GaAs cap layer 5 nm of Si; Use the method for hot vapor deposition to prepare the thick electrode of nickel gold germanium nickel gold 100 nm then, wherein the thickness of nickel/germanium gold/nickel/gold is respectively 500/2040/100/500 Ethylmercurichlorendimide, the last thick silicon dioxide insulating layer of deposition 200 nm on electrode again; Can obtain AlGaAs/GaAs HEMT;
Through using the gas-solid method to prepare four-needle-like zinc oxide; Zinc powder and acetic acid zinc powder mixed at 10: 1 being placed in 660 ℃ of tubular furnace reaction 15 minutes with mol ratio, the flow velocity of Oxygen Flow and argon gas stream is respectively 300 sccm (standard cubic centimeter per minute) and 15 sccm; Can obtain the T-ZnO of average-size about 5 μ m at last;
T-ZnO is dissolved in ethanolic solution, evenly is coated on the grid of HEMT, at room temperature dry naturally, form the thick T-ZnO layer of 5 μ m; On the T-ZnO layer, drip glucolase or uricase then, and drip the Nafion solution that U.S. ALDRICH company provides immediately; Again the device for preparing is placed shading place 15 minutes, take out then and place 4 ℃ of refrigerators to preserve 24 hours, promptly can obtain glucose/uric acid biology sensor.
3. as claimed in claim 1 based on zinc paste and HEMT biology sensor, it is characterized in that: with AlGaAs/GaAs HEMT is substrate, and uses microscale/nanoscale T-ZnO, biology enzyme molecule and Nafion to carry out grid successively and modify.
4. like the method for the said preparation of claim 2 based on zinc paste and HEMT biology sensor; It is characterized in that: prepare AlGaAs/GaAs HEMT with EPI GEN-II type MBE system and hot evaporation coating method; The T-ZnO that is equipped with microscale/nanoscale then with the gas-solid legal system; And prepared T-ZnO is scattered in gate surface with ethanol forms the T-ZnO thin layer; Use biology enzyme molecule and Nafion to modify grid more successively, wherein the way of contact of biology enzyme molecule and T-ZnO is electrostatic adsorption, and Nafion is used for fixing T-ZnO.
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| CN103760206A (en) * | 2014-01-14 | 2014-04-30 | 江苏新广联科技股份有限公司 | Blood glucose test chip based on gallium nitride material |
| CN104101626A (en) * | 2013-04-02 | 2014-10-15 | 北京科技大学 | Method for measurement of DNA hybridization by graphene modified high electron mobility transistor |
| CN104880493A (en) * | 2014-02-28 | 2015-09-02 | 中国科学院半导体研究所 | GaAs-based PHEMT biosensor and making method thereof |
| CN104880558A (en) * | 2014-02-28 | 2015-09-02 | 中国科学院半导体研究所 | InP-based HEMT tumor marker sensor and manufacturing method thereof |
| CN108982600A (en) * | 2018-05-30 | 2018-12-11 | 杨丽娜 | Based on gallium oxide/gallic acid zinc hetero-junctions nano-array flexible gas sensor and preparation method thereof |
| CN109270148A (en) * | 2018-10-17 | 2019-01-25 | 湖北大学 | The electrochemical transistor sensor and its anti-interference method of interference free performance, application |
| CN110470713A (en) * | 2019-07-03 | 2019-11-19 | 大连理工大学 | A kind of glucose sensor of GaN base transistor with high electronic transfer rate |
| US10724981B2 (en) | 2017-10-13 | 2020-07-28 | National Taiwan University | Microfluidic chip and manufacturing method thereof and integrated microfluidic chip system |
| CN112432985A (en) * | 2019-08-26 | 2021-03-02 | 北京中医药大学 | Application of AlGaAs/GaAs HEMT biosensor in identification of MIF (micro-interference-rejection factor) potential inhibitor |
| CN113009127A (en) * | 2019-12-19 | 2021-06-22 | 北京中医药大学 | Application of biosensor and protein combined immunoreaction in detection of deoxyschizandrin signal channel for treating oligospermia |
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| CN104101626A (en) * | 2013-04-02 | 2014-10-15 | 北京科技大学 | Method for measurement of DNA hybridization by graphene modified high electron mobility transistor |
| CN104101626B (en) * | 2013-04-02 | 2016-08-03 | 北京科技大学 | Graphene modified HEMT is utilized to measure DNA hydridization method |
| CN103760206B (en) * | 2014-01-14 | 2016-07-06 | 江苏新广联科技股份有限公司 | Blood glucose test chip based on gallium nitride material |
| CN103760206A (en) * | 2014-01-14 | 2014-04-30 | 江苏新广联科技股份有限公司 | Blood glucose test chip based on gallium nitride material |
| CN104880493A (en) * | 2014-02-28 | 2015-09-02 | 中国科学院半导体研究所 | GaAs-based PHEMT biosensor and making method thereof |
| CN104880558A (en) * | 2014-02-28 | 2015-09-02 | 中国科学院半导体研究所 | InP-based HEMT tumor marker sensor and manufacturing method thereof |
| CN104880493B (en) * | 2014-02-28 | 2017-11-24 | 中国科学院半导体研究所 | GaAs base PHEMT biology sensors and preparation method thereof |
| US10724981B2 (en) | 2017-10-13 | 2020-07-28 | National Taiwan University | Microfluidic chip and manufacturing method thereof and integrated microfluidic chip system |
| CN108982600A (en) * | 2018-05-30 | 2018-12-11 | 杨丽娜 | Based on gallium oxide/gallic acid zinc hetero-junctions nano-array flexible gas sensor and preparation method thereof |
| CN109270148A (en) * | 2018-10-17 | 2019-01-25 | 湖北大学 | The electrochemical transistor sensor and its anti-interference method of interference free performance, application |
| CN110470713A (en) * | 2019-07-03 | 2019-11-19 | 大连理工大学 | A kind of glucose sensor of GaN base transistor with high electronic transfer rate |
| CN110470713B (en) * | 2019-07-03 | 2024-05-07 | 大连理工大学 | Glucose sensor of gallium nitride-based high electron mobility transistor |
| CN112432985A (en) * | 2019-08-26 | 2021-03-02 | 北京中医药大学 | Application of AlGaAs/GaAs HEMT biosensor in identification of MIF (micro-interference-rejection factor) potential inhibitor |
| CN112432985B (en) * | 2019-08-26 | 2022-07-19 | 北京中医药大学 | Application of AlGaAs/GaAs HEMT biosensor in identification of MIF potential inhibitor |
| CN113009127A (en) * | 2019-12-19 | 2021-06-22 | 北京中医药大学 | Application of biosensor and protein combined immunoreaction in detection of deoxyschizandrin signal channel for treating oligospermia |
| CN113009127B (en) * | 2019-12-19 | 2023-07-07 | 北京中医药大学 | Application of biosensor combined protein immune response method in detecting schizandrin A treating oligospermia signal path |
| CN113130656A (en) * | 2021-04-12 | 2021-07-16 | 中国科学院宁波材料技术与工程研究所 | Field effect transistor biosensor and preparation method and application thereof |
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