CN109946349A - Organic field effect tube and preparation method thereof and biogenic amine gas sensor - Google Patents
Organic field effect tube and preparation method thereof and biogenic amine gas sensor Download PDFInfo
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- CN109946349A CN109946349A CN201910260445.6A CN201910260445A CN109946349A CN 109946349 A CN109946349 A CN 109946349A CN 201910260445 A CN201910260445 A CN 201910260445A CN 109946349 A CN109946349 A CN 109946349A
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Abstract
The present invention discloses a kind of organic field effect tube and preparation method thereof and biogenic amine gas sensor, organic field effect tube includes the substrate being cascading from bottom to top, organic semiconductor layer, biogenic amine sensitive layer, insulating layer and grid, drain electrode and source electrode, the region that organic semiconductor layer is covered in source electrode and drain electrode and is not covered by source electrode and drain electrode on substrate are additionally provided on substrate；Biogenic amine sensitive layer is set to larger than organic semiconductor layer to the susceptibility of biogenic amine to the susceptibility of biogenic amine.In the present invention, organic field effect tube under energized state can form conducting channel in biogenic amine sensitive layer and organic semiconductor layer, when there are biogenic amines, biogenic amine and biogenic amine sensitive layer, organic semiconductor layer generate the resistance for chemically reacting and changing conducting channel, variation by perceiving resistance can sense biogenic amine, the susceptibility of detection is effectively improved, the purpose realized optimizing detection effect, improve detection efficiency.
Description
Technical field
The present invention relates to the technical fields of gas detection, in particular to carry out gas detection using organic semiconducting materials
Technical field, and in particular to a kind of organic field effect tube and preparation method thereof and biogenic amine gas sensor.
Background technique
Biogenic amine is a kind of nitrogenous low molecule organic base, is mainly acted on and being formed by amino acid decarboxylase, is widely present in richness
Containing in amino acid, the meat products of protein, aquatic products and fermented product.Biogenic amine can be divided into three classes according to its structure: aliphatic,
Including putrescine, cadaverine, spermine, spermidine etc.；Aromatic series, including tyrasamine, phenyl ethylamine etc.；Heterocyclic amine, including histamine, tryptamines etc..
Suitable biogenic amine be maintain human normal physiological function necessary to, if but human body biogenic amine excess intake can be drawn
Allergic reaction is played, it may threat to life when serious.In addition, biogenic amine often generates in food decay or fermentation process, eat
The breaking-out of product poisoning and certain toxicological profiles and histamine and tyrasamine have substantial connection, and biogenic amine in food content can be used as food
The important indicator of quality.Therefore, effective, the quick detection of biogenic amine in food has important meaning to food quality and safety
Justice.
Due to lacking chromophoric group in biological amine molecule, itself makes not only without UV absorption but also unstressed configuration and electro-chemical activity
Separation and the measurement for obtaining different kind organism amine are extremely difficult.Tradition measurement biogenic amine relies primarily on biochemical class method, such as enzyme biology
Sensor method, thin-layered chromatography, gas chromatography, the chromatography of ions, capillary electrophoresis and high performance liquid chromatography etc.,
In, high performance liquid chromatography is because have column effect is high, separative efficiency is high, analysis speed is fast, high sensitivity, quantitative analysis are accurate etc.
Advantage, most of scholar is using it as the main method of analysis biogenic amine in food, but the method detection limit is small, is once only capable of examining
A sample is surveyed, at high cost, overall efficiency is low.To solve the above-mentioned problems, propose that one kind passes through inorganic, metal oxide at present
Semiconductor gas sensor is come the method that measures biogenic amine, but this method has operating temperature high, needs heater；To majority
Organic gas detection sensitivity is low；The drawbacks such as detection range is narrow.
Summary of the invention
The main object of the present invention is to propose a kind of organic field effect tube, preparation method and biogenic amine gas sensing
Device, it is intended to solve the problems, such as that detection sensitivity is low existing for traditional detection method, detection efficiency is low.
To achieve the above object, a kind of organic field effect tube proposed by the present invention, for sensing the biology in food
Amine, the organic field effect tube include substrate, organic semiconductor layer, the biogenic amine sensitivity being cascading from bottom to top
Layer, insulating layer and grid, the upper end of the substrate are additionally provided with source electrode and drain electrode, and the organic semiconductor layer is covered on the leakage
The region not covered by the drain electrode and the source electrode on pole and the source electrode and on the substrate；
Wherein, the biogenic amine sensitive layer is set to larger than the organic semiconductor layer to life to the susceptibility of biogenic amine
The susceptibility of object amine.
Optionally, the material of the organic semiconductor layer is to have the following structure formula (I), (II), (III), (IV) shown knot
Any one in the compound of structure:
Optionally, the material of the biogenic amine sensitive layer is the chemical combination for having the following structure structure shown in formula (V), (VI)
Any one in object:
Wherein, in structural formula (V): M=Au or M=Co.
Optionally, the material of the insulating layer is water or phosphate buffered saline solution.
Optionally, the material of the substrate is glass, silicon wafer or ceramics；Alternatively,
The material of the source electrode, the drain electrode and the grid is aluminium or gold.
Optionally, the organic semiconductor layer with a thickness of 60nm~70nm；Alternatively,
The biogenic amine sensitive layer with a thickness of 8nm~12nm；Alternatively,
The substrate with a thickness of 45nm~55nm.
In addition, the present invention also proposes a kind of method for preparing organic field effect tube as described above, including following step
It is rapid:
One substrate is provided；
Setting drain electrode and source electrode over the substrate；
The region not covered by the drain electrode and the source electrode on the source electrode and the drain electrode and on the substrate
On, organic semiconductor layer is set；
Biogenic amine sensitive layer is set on the organic semiconductor layer；
Insulating layer is set on the biogenic amine sensitive layer；
Grid is set on the insulating layer, to obtain the organic field effect tube.
Optionally, the setting method of the grid, the source electrode and the drain electrode be vacuum thermal evaporation, magnetron sputtering or
The chemical vapor deposition of person's plasma enhancing.
Optionally, described includes: sensitive in the biogenic amine the step of insulating layer is arranged on the biogenic amine sensitive layer
The water or phosphate buffered saline solution of 1~3 μ L are added dropwise on layer, constitutes the insulating layer.
In addition, the present invention also proposes a kind of biogenic amine gas sensor, including organic field effect tube as described above.
In technical solution provided by the invention, the organic field effect tube under energized state can be in the biology
Amine sensitive layer and the organic semiconductor layer form conducting channel, when in environment there are when biogenic amine, biogenic amine and the biology
Amine sensitive layer, the organic semiconductor layer generate chemical reaction, will change the resistance of the conducting channel, therefore, pass through perception
The purpose of biogenic amine in sensing environment can be realized in the variation of the resistance；In addition, in the top of the drain electrode and the source electrode
The organic semiconductor layer is set, adds the biogenic amine more sensitive to biogenic amine above the organic semiconductor layer
Sensitive layer not only contributes to the contact area for increasing the organic field effect tube and biogenic amine, moreover it is possible to effectively improve detection
Susceptibility, realize optimizing detection effect, improve detection efficiency purpose.
Detailed description of the invention
In order to more clearly explain the embodiment of the invention or the technical proposal in the existing technology, to embodiment or will show below
There is attached drawing needed in technical description to be briefly described, it should be apparent that, the accompanying drawings in the following description is only this
Some embodiments of invention for those of ordinary skill in the art without creative efforts, can be with
The structure shown according to these attached drawings obtains other attached drawings.
Fig. 1 is the structural schematic diagram of an embodiment of organic field effect tube provided by the invention.
Drawing reference numeral explanation:
| Label | Title | Label | Title |
| 100 | Organic field effect tube | 3 | Organic semiconductor layer |
| 1 | Substrate | 4 | Biogenic amine sensitive layer |
| 21 | Drain electrode | 5 | Insulating layer |
| 22 | Source electrode | 6 | Grid |
The embodiments will be further described with reference to the accompanying drawings for the realization, the function and the advantages of the object of the present invention.
Specific embodiment
Following will be combined with the drawings in the embodiments of the present invention, and technical solution in the embodiment of the present invention carries out clear, complete
Site preparation description, it is clear that described embodiment is only a part of the embodiments of the present invention, instead of all the embodiments.Base
Embodiment in the present invention, it is obtained by those of ordinary skill in the art without making creative efforts it is all its
His embodiment, shall fall within the protection scope of the present invention.
It is to be appreciated that if relating to directionality instruction (such as up, down, left, right, before and after ...) in the embodiment of the present invention,
Then directionality instruction be only used for explain under a certain particular pose (as shown in the picture) between each component relative positional relationship,
Motion conditions etc., if the particular pose changes, directionality instruction is also correspondingly changed correspondingly.
In addition, being somebody's turn to do " first ", " second " etc. if relating to the description of " first ", " second " etc. in the embodiment of the present invention
Description be used for description purposes only, be not understood to indicate or imply its relative importance or implicitly indicate indicated skill
The quantity of art feature." first " is defined as a result, the feature of " second " can explicitly or implicitly include at least one spy
Sign.In addition, the meaning of the "and/or" occurred in full text, including three schemes arranged side by side, by taking " A and/or B " as an example, including the side A
The scheme that case or B scheme or A and B meet simultaneously.In addition, the technical solution between each embodiment can be combined with each other, but
To be based on can be realized by those of ordinary skill in the art, when the combination of technical solution occur it is conflicting or can not
Will be understood that the combination of this technical solution is not present when realization, also not the present invention claims protection scope within.
Due to lacking chromophoric group in biological amine molecule, itself makes not only without UV absorption but also unstressed configuration and electro-chemical activity
Separation and the measurement for obtaining different kind organism amine are extremely difficult.Tradition measurement biogenic amine relies primarily on biochemical class method, such as enzyme biology
Sensor method, thin-layered chromatography, gas chromatography, the chromatography of ions, capillary electrophoresis and high performance liquid chromatography etc.,
In, high performance liquid chromatography is because have column effect is high, separative efficiency is high, analysis speed is fast, high sensitivity, quantitative analysis are accurate etc.
Advantage, most of scholar is using it as the main method of analysis biogenic amine in food, but the method detection limit is small, is once only capable of examining
A sample is surveyed, at high cost, overall efficiency is low.To solve the above-mentioned problems, propose that one kind passes through inorganic, metal oxide at present
Semiconductor gas sensor is come the method that measures biogenic amine, but this method has operating temperature high, needs heater；To majority
Organic gas detection sensitivity is low；The drawbacks such as detection range is narrow.
In consideration of it, the present invention provides a kind of biogenic amine gas sensor, the biogenic amine gas sensor includes organic field
Effect transistor and other components, Fig. 1 is an embodiment of organic field effect tube provided by the invention, due to of the invention
Primary object is the improvement to organic field effect tube, below in conjunction with specific attached drawing mainly to organic effect crystal
Pipe is illustrated.
Referring to Fig. 1, in the present embodiment, the organic field effect tube 100 is used to sense the biogenic amine in environment
And its content, the biogenic amine being particularly suitable in sensing food, the organic field effect tube 100 include from bottom to top successively
Substrate 1, organic semiconductor layer 3, biogenic amine sensitive layer 4, insulating layer 5 and the grid 6 being stacked, in addition, the substrate 1
Upper end is additionally provided with drain electrode 21 and source electrode 22, the organic semiconductor layer 3 be covered on the drain electrode 21 and the source electrode 22 and
The region not covered by the drain electrode 21 and the source electrode 22 on the substrate 1.In addition, 4 pairs of biologies of the biogenic amine sensitive layer
The susceptibility of amine is set to larger than the organic semiconductor layer 3 to the susceptibility of biogenic amine, can specifically be embodied in: the life
The material of object amine sensitive layer 4 is quick greater than the material of the organic semiconductor layer 3 or the biogenic amine to the susceptibility of biogenic amine
The contact area of sense layer 4 and biogenic amine is greater than the contact area of the organic semiconductor layer 3 and biogenic amine.At work, to institute
It states grid 6 and the drain electrode 21 applies positive voltages, negative voltage or ground connection applied to the source electrode 22, it is the source electrode 22, described
Drain electrode 21 and the grid 6 that is, capacitor two pole plates, the organic semiconductor layer 3, the biogenic amine sensitive layer 4
The successively contact conducting between the insulating layer 5, so that the organic field effect tube 100 is generally in energized state, structure
At capacitor.
In technical solution provided by the invention, the organic field effect tube 100 under energized state can be in the life
Object amine sensitive layer 4 and the organic semiconductor layer 3 form conducting channel, when in environment there are when biogenic amine, biogenic amine and described
Biogenic amine sensitive layer 4, the organic semiconductor layer 3 generate chemical reaction, will change the resistance of the conducting channel, therefore, lead to
Cross perceive the resistance variation can be realized sensing environment in biogenic amine purpose；In addition, in the drain electrode 21 and the source
The organic semiconductor layer 3 is arranged in the top of pole 22, it is more sensitive to biogenic amine to add in the top of the organic semiconductor layer 3
The biogenic amine sensitive layer 4, not only contribute to increase the contact area of the organic field effect tube 100 and biogenic amine,
The susceptibility of detection can also be effectively improved, the purpose realized optimizing detection effect, improve detection efficiency.
Further, in the present embodiment, the material of the organic semiconductor layer 3 be have the following structure formula (I),
(II), (III), structure shown in (IV) compound in any one:
Wherein, the compound in structural formula (I) is PDI8-CN2 material, the compound in structural formula (II) is P3HT material
Material, the compound in structural formula (III) they are Pentacene material, the compound in structural formula (IV) is PEDOT:PSS material, on
State compound at normal temperature can with biogenic amine generate it is sensitive react, specifically, biological amine gas can be fast by grain boundary
Speed passes through the organic semiconductor layer 3 into electric charge accumulating layer, then generates trap in grain boundary to reduce electric charge carrier
Mobility, thus quickly change conducting channel resistance, realize Sensitive Detection biogenic amine purpose；Above compound is existing
There is product, can be compatible with the substrate 1, it is adapted to low temperature process and mass production.
In addition, in the present embodiment, the material of the biogenic amine sensitive layer 4 is has the following structure formula (V), (VI) institute
Show any one in the compound of structure:
Wherein, in structural formula (V): M=Au or M=Co.Compound in structural formula (V) be Au-EHO material,
Compound in structural formula (VI) is Co-EHO material, and the biogenic amine sensitive layer 4 is covered on the upper of the organic semiconductor layer 3
Side, the biogenic amine in direct contact environment, since the Au-EHO material and the Co-EHO material are compared to the PDI8-
CN2 material, the P3HT material, the Pentacene material and the PEDOT:PSS material have biogenic amine higher quick
Sensitivity, specifically, biogenic amine gas molecule can enter the hole of the biogenic amine sensitive layer 4, then sensitive with the biogenic amine
The molecule of layer 4 carries out bonding and generates electric dipole, the conductive characteristic of the organic semiconductor layer 3 is further influenced, so that described
100 pairs of organic field effect tube biological amine gas are more sensitive, then facilitate to widen the organic field effect tube 100
Detection range, and be conducive to accelerate detection speed, to improve detection efficiency.
Then, in the present embodiment, the material of the insulating layer 5 is water or phosphate buffered saline solution, compared to tradition
Inorganic insulating material, the dielectric constant with higher of insulating layer 5 that water or phosphate buffered saline solution are formed can effectively improve
The capacitor of the organic field effect tube 100 drops to improve the conducting electric current in the organic field effect tube 100
Operating voltage needed for the low organic field effect tube 100.In use, the grid 6 is inserted directly into water or phosphoric acid is slow
It rushes in salting liquid.
Further, in the present embodiment, the material of the substrate 1 is glass, silicon wafer or ceramics, is had good exhausted
Edge and material price is cheap is conducive to mitigate economic cost burden；Alternatively, the drain electrode 21, the source electrode 22 and the grid
The material of pole 6 is that aluminium or gold facilitate while not increasing the volume and quality of the organic field effect tube 100
Expand capacitance.
Further, in the present embodiment, the organic semiconductor layer 3 with a thickness of 60nm~70nm or the life
Object amine sensitive layer 4 with a thickness of 8nm~12nm or the substrate 1 with a thickness of 45nm~55nm, and preferably 50nm.Institute
State source electrode 22 described in the thickness effect of organic semiconductor layer 3, the biogenic amine sensitive layer 4 and the insulating layer 5, the drain electrode 21
With the capacitive sensing between the grid 6, if the thickness is larger, capacitor that the organic field effect tube 100 senses
Change smaller or even good capacitive sensing can not be formed, influences to the instantaneously sense of biogenic amine；Conversely, if the thickness is smaller,
The operating voltage then needed is larger, is unfavorable for the use of user, it is preferred that the organic semiconductor layer 3 with a thickness of
65nm, the biogenic amine sensitive layer 4 with a thickness of 10nm.
In addition, the present invention also proposes a kind of method for preparing the organic field effect tube 100, following step is specifically included
It is rapid:
Step S10: a substrate 1 is provided；
Step S20: setting drain electrode 21 and source electrode 22 on the substrate 1；
Step S30: not by 21 and of the drain electrode in the drain electrode 21 and the source electrode 22 and on the substrate 1
On the region that the source electrode 22 covers, organic semiconductor layer 3 is set；
Step S40: biogenic amine sensitive layer 4 is set on the organic semiconductor layer 3；
Step S50: insulating layer 5 is set on the biogenic amine sensitive layer 4；
Step S60: grid 6 is set on the insulating layer 5, to obtain the organic field effect tube 100.
In the present embodiment, according to practical application, the material and thickness of the suitable substrate 1 are chosen, using silicon wafer as
For the substrate 1, successively it is cleaned by ultrasonic the silicon wafer using acetone, isopropyl acetone etc., is then rinsed with ethyl alcohol and deionized water
The silicon wafer, finally with being dried with nitrogen silicon chip surface；Then, the drain electrode 21 and the source electrode 22 are deposited on the substrate 1,
Then on the drain electrode 21, the source electrode 22 and the substrate 1 continue that the organic semiconductor layer 3 and the life is successively deposited
Object amine sensitive layer 4；The insulating layer 5 is prepared on the biogenic amine sensitive layer 4, finally on the insulating layer 5 described in setting
Grid 6, such as the insulating layer 5 is inserted into at least lower end of the grid 6, obtain the organic field effect tube 100.
Further, in the present embodiment, the setting method of the grid 6, the source electrode 22 and the drain electrode 21 is
The chemical vapor deposition of vacuum thermal evaporation, magnetron sputtering or plasma enhancing.For example, the substrate 1 is placed in Vacuum Deposition
It is 6.5 × 10 in vacuum degree in film machine-4Gold is deposited under conditions of Pa on the substrate 1 with the speed of 1A/s, obtains the leakage
Pole 21 and the source electrode 22.The specific preparation method of the grid 6 is similar to the above, does not repeat, in addition, magnetron sputtering or
The specific steps and related request of the chemical vapor deposition of plasma enhancing can refer to the prior art, not be described further herein.
Further, in the present embodiment, the step S50 includes: 1~3 μ L of dropwise addition on the biogenic amine sensitive layer 4
Water or phosphate buffered saline solution, constitute the insulating layer 5.For example, drop can be used needing to detect in the environment of biogenic amine
It manages toward the water or phosphate buffered saline solution that about 2 μ L are added dropwise on the biogenic amine sensitive layer 4, is then again inserted into the grid 6
In water or phosphate buffered saline solution, to constitute the complete organic field effect tube 100.The tool of the insulating layer 5
Scale of construction value, constituent etc. can be adaptively adjusted according to practical application, pointedly to detect under varying environment not
Same biogenic amine more fast and effeciently obtains more accurate result.
Be illustrated by taking a specific embodiment of the organic field effect tube 100 as an example, can at room temperature,
Using the glass of 50nm thickness as substrate 1, drain electrode 21 and the source electrode 22 of gold system are set by way of magnetron sputtering on substrate；So
It is not covered afterwards by the drain electrode 21 and the source electrode 22 in the drain electrode 21 and the source electrode 22 and on the substrate 1
On region, the organic semiconductor layer 3 of 65nm thickness is set by way of vapor deposition, and the material of the organic semiconductor layer 3 is
P3HT；On the organic semiconductor layer 3, the biogenic amine sensitive layer 4 of 10nm thickness, and the biology are set by way of vapor deposition
The material of amine sensitive layer 4 is Co-EHO；The phosphate buffered saline solution of 2 μ L is drawn simultaneously with suction pipe on the biogenic amine sensitive layer 4
It is added dropwise on the biogenic amine sensitive layer 4, constitutes insulating layer 5；Finally on the insulating layer 5 by way of vacuum thermal evaporation
The grid 6 of gold system is set, to obtain the organic field effect tube 100.Using the measuring technique of existing measuring device,
It can effectively detect in Vg=0.6V, this corresponding saturation current of organic field effect tube 100 is 0.9 μ A, and carrier moves
Shifting rate is 2.3x10-3cm2/ Vs, threshold voltage 0.03V, response speed 0.2s illustrate the organic field prepared by the present invention
Effect transistor 100 is good to the response results of biogenic amine at room temperature, fast response time, high sensitivity.
The above description is only a preferred embodiment of the present invention, is not intended to limit the scope of the invention, all at this
Under the inventive concept of invention, using equivalent structure transformation made by description of the invention and accompanying drawing content, or directly/use indirectly
It is included in other related technical areas in scope of patent protection of the invention.
Claims (10)
1. a kind of organic field effect tube, for sensing the biogenic amine in food, which is characterized in that the organic effect is brilliant
Body pipe includes the substrate being cascading from bottom to top, organic semiconductor layer, biogenic amine sensitive layer, insulating layer and grid,
The upper end of the substrate is additionally provided with drain electrode and source electrode, the organic semiconductor layer is covered on the drain electrode and the source electrode, with
And the region not covered by the drain electrode and the source electrode on the substrate；
Wherein, the biogenic amine sensitive layer is set to larger than the organic semiconductor layer to biogenic amine to the susceptibility of biogenic amine
Susceptibility.
2. organic field effect tube as described in claim 1, which is characterized in that the material of the organic semiconductor layer is tool
Just like any one in the compound of structure shown in flowering structure formula (I), (II), (III), (IV):
。
3. organic field effect tube as described in claim 1, which is characterized in that the material of the biogenic amine sensitive layer is tool
Just like any one in the compound of structure shown in flowering structure formula (V), (VI):
Wherein, in structural formula (V): M=Au or M=Co.
4. organic field effect tube as described in claim 1, which is characterized in that the material of the insulating layer is water or phosphorus
Acid buffering salting liquid.
5. organic field effect tube as described in claim 1, which is characterized in that the material of the substrate is glass, silicon wafer
Or ceramics；Alternatively,
The material of the source electrode, the drain electrode and the grid is aluminium or gold.
6. organic field effect tube as described in claim 1, which is characterized in that the organic semiconductor layer with a thickness of
60nm~70nm；Alternatively,
The biogenic amine sensitive layer with a thickness of 8nm~12nm；Alternatively,
The substrate with a thickness of 45nm~55nm.
7. a kind of preparation method of the organic field effect tube as described in claim 1 to 6 any one, which is characterized in that
The following steps are included:
One substrate is provided；
Setting drain electrode and source electrode over the substrate；
On the region not covered by the drain electrode and the source electrode in the drain electrode and the source electrode and on the substrate,
Organic semiconductor layer is set；
Biogenic amine sensitive layer is set on the organic semiconductor layer；
Insulating layer is set on the biogenic amine sensitive layer；
Grid is set on the insulating layer, to obtain the organic field effect tube.
8. the preparation method of organic field effect tube as claimed in claim 7, which is characterized in that the grid, the source
The setting method of pole and the drain electrode is the chemical vapor deposition of vacuum thermal evaporation, magnetron sputtering or plasma enhancing.
9. the preparation method of organic field effect tube as claimed in claim 7, which is characterized in that described in the biogenic amine
The step of insulating layer is arranged on sensitive layer includes: the water or phosphate-buffered salt that 1~3 μ L is added dropwise on the biogenic amine sensitive layer
Solution constitutes the insulating layer.
10. a kind of biogenic amine gas sensor, which is characterized in that including the organic field as described in claim 1 to 6 any one
Effect transistor.
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| CN111211222A (en) * | 2020-02-19 | 2020-05-29 | 国家纳米科学中心 | Application of organic thin film transistor and Young modulus value evaluation method of organic thin film based on organic thin film transistor |
| CN112304929A (en) * | 2019-07-24 | 2021-02-02 | 高雄大学 | Method and device for detecting biogenic amine in food materials |
| CN112432977A (en) * | 2020-11-18 | 2021-03-02 | 中国科学院上海微***与信息技术研究所 | Organic field effect transistor gas sensor and preparation method thereof |
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