CN105301055B - A kind of organic field-effect tube nitrogen dioxide sensor - Google Patents
A kind of organic field-effect tube nitrogen dioxide sensor Download PDFInfo
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- CN105301055B CN105301055B CN201510830580.1A CN201510830580A CN105301055B CN 105301055 B CN105301055 B CN 105301055B CN 201510830580 A CN201510830580 A CN 201510830580A CN 105301055 B CN105301055 B CN 105301055B
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- organic semiconductor
- nitrogen dioxide
- effect tube
- zinc oxide
- oxide nanoparticle
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Abstract
The invention discloses a kind of organic field-effect tube nitrogen dioxide sensors, are followed successively by substrate, gate electrode, insulating layer from top to bottom, and the surface of insulating layer is dispersed with Zinc oxide nanoparticle layer；The organic semiconductor layer of promising discontinuous film is set on Zinc oxide nanoparticle layer, precipitation has the impurity molecule organic semiconductor contacted with Zinc oxide nanoparticle on organic semiconductor layer and in gap, and source electrode and drain electrode is provided on impurity molecule organic semiconductor.The present invention reduces organic field-effect tube device performance by the way that impurity molecule organic semiconductor is introduced discrete organic semiconductor layer, and then raising is to the responsiveness of nitrogen dioxide, Zinc oxide nanoparticle can improve the selectivity to nitrogen dioxide, and highly sensitive high echo probe is realized to nitrogen dioxide so as to fulfill the device；The field-effect tube nitrogen dioxide sensor is prepared simply, and operating voltage is low, replaces substrate and the characteristics such as flexible, transparent can be realized.
Description
Technical field
The invention belongs to sensor preparing technical field, more particularly to a kind of organic field-effect tube nitrogen dioxide sensor.
Background technology
In the daily production and living of the mankind, direct or indirect releases many pernicious gases into air, as ammonia,
Nitrogen dioxide, sulfur dioxide, formaldehyde, hydrogen sulfide etc..These pernicious gases drastically influence the health of the mankind, high concentration
Also entail dangers to life security.
In the past more than ten years, researcher have developed largely based on metal-oxide film, optical fiber and
The gas sensor of biomaterial.From the gas sensor of operation principle, currently on the market mainstream, mostly resistance-type senses
Device is reacted in film surface by gas molecule and causes the variation of conductivity, macroscopically passes through the variation of detection resistance value
To realize the detection to gas concentration.And non-resistor is mainly realized pair by using some physical effects and device property
The detection of gas, such as capacitance（C-V）Change, the C-V characteristic of Schottky diode and metal-oxide-semiconductcor field effect
Ying Guan（MOSFET）The characteristics such as threshold voltage variation.In the sensor based on transistor, grid voltage is due to measured matter
Influence can generate slight variation, due to the amplification of transistor in itself, will obtain the apparent channel current of variation, pass through
The detection to test substance can be realized in detection channel current, and the resistance compared to more difficult monitoring is easier to detect.
With the rapid development of organic electronics and its application in sensor field, with organic field-effect tube (organic
Thin-film transistor, OTFT) based on the chemical sensor that forms become a research heat of sensor field
Point is applied to inorganic and volatile organic compounds detections and has wide coverage.Compared with traditional gas sensor, base
In OTFT structures gas sensor other than there is high sensitivity, can use at normal temperatures, also with it is several significantly
Advantage：
1) will be difficult to the high resistance change transitions detected using transistor fundamental characteristics is the curent change that easily detects；
2) sensitivity of sensor can be adjusted by proper choice of the gate operational voltages of device；
3) multiparameter model more has the identification and analysis using gas；
4) electrical property of sensor can be conveniently adjusted by the chemical modification to organic molecule, improves sensitivity；
5) organic matter flexibility is good, can be bent, and can be easily made variously-shaped；
6) it is easily integrated, large area sensor array can be prepared, convenient for developing to integrated, micromation direction.
Invention content
Present invention aims to overcome that the shortcomings that traditional gas sensor, it is simple to provide a kind of preparation process, is produced into
This is cheap, detects and be capable of a kind of organic field-effect tube gas based on mix insulation layer of multi-parameter response available for gas
Sensor and preparation method thereof.
The technical scheme is that：
A kind of organic field-effect tube nitrogen dioxide sensor, from top to bottom as substrate, gate electrode, insulating layer, oxidation
Zinc nanoparticles, organic semiconductor layer, impurity molecule organic semiconductor, source electrode and drain electrode, which is characterized in that described organic
Semiconductor layer is discontinuous film；The surface of insulating layer is dispersed with Zinc oxide nanoparticle；The impurity organic semiconductor point
Son is deposited in organic semiconductor lamellar spacing and is contacted with Zinc oxide nanoparticle.
Further, the organic semiconductor layer is made of p-type small molecule organic semiconductor material, including aphthacene, simultaneously
Pentaphene, 6, one kind in 13-two three isopropyl ester silicon substrate acetylene pentacenes, rubrene or six thiophene, the organic semiconductor thickness
It spends for 20 nm-, 30 nm.
Further, the impurity molecule organic semiconductor is the p-type small molecule of N-shaped small molecule or high electron density,
The N-shaped small molecule includes, C60, N, N '-diamyl -3,4,9,10- dicarboximides, N, N '-diphenyl -3,4, and 9,10-
Dicarboximide, N, N '-dioctyl -3,4,9,10- dicarboximides, N, N'- bis- (2,5- di-tert-butyl-phenyls) -3,4,
9,10- dicarboximides, perfluor CuPc, Isosorbide-5-Nitrae, 5,8- naphthalenetetracarbacidic acidic acid anhydrides, the p-type small molecule include CuPc, phthalocyanine
Zinc, Cobalt Phthalocyanine；
Further, the thickness of insulating layer be 500 nm -2000 nm, the Zinc oxide nanoparticle a diameter of 5
nm – 10 nm。
Further, the material of the polymer insulation layer is polystyrene, poly- а-methyl styrene, polymethylacrylic acid
Methyl esters, makrolon, dimethyl silicone polymer, polyvinyl alcohol, polyvinylpyrrolidone or pla-pcl and they between
One kind in copolymer.
Further, gate electrode, source electrode and drain electrode are made of one kind in gold, silver or copper and its alloy material, source
The thickness of electrode and drain electrode is 50 ~ 100 nm.
Further, the substrate for silicon chip, glass, thin polymer film, metal foil, plant fiber, fibrin gel,
It is one or more in gelatin, polylactic acid, viral fiber element, polylactic acid-co-glycolic acid.
The invention also discloses a kind of preparation methods of organic field-effect tube nitrogen dioxide sensor, include the following steps：
1. first substrate is thoroughly cleaned, it is dry after cleaning；
2. prepare gate electrode in substrate surface；
3. there is the insulating layer of Zinc oxide nanoparticle in gate electrode Dispersion on surface prepared above；
4. discontinuous organic semiconductor layer is prepared on the insulating layer；
5. prepare source electrode and drain electrode on the organic semiconductor layer.
Further, step 3. in, insulating layer pass through spin coating, roller coating, drop film, coining, printing or spraying in a kind of side
Prepared by method, Zinc oxide nanoparticle is prepared using a kind of method in quick spin coating, printing or spraying.
Further, step 2. 5. in, gate electrode, source electrode, drain electrode be by vacuum thermal evaporation, magnetron sputtering, etc.
It is prepared by a kind of method in the chemical vapor deposition of gas ions enhancing, silk-screen printing, printing or spin coating, the step 4. in, institute
It is by the chemical vapor deposition of plasma enhancing, thermal oxide, spin coating, vacuum evaporation, roller coating, drop to state organic semiconductor layer
It is prepared by a kind of method in film, coining, printing or spraying.
Compared with prior art, the advantage of the invention is that：
First, by the way that Zinc oxide nanoparticle is introduced surface of insulating layer, change the wellability of surface of insulating layer, after making
The organic semiconductor layer of continuous growth forms discontinuous film；
2nd, impurity molecule organic semiconductor is deposited in the gap of discontinuous organic semiconductor layer, due to itself characteristic
Play the role of hole trap, reduce the initial performance of device, when device is exposed in nitrogen dioxide gas, impurity has
The trap effect of machine semiconductor molecule, which can greatly weaken, even to disappear, so that device performance is substantially improved, and then obtains
Higher response；
3rd, the Zinc oxide nanoparticle in surface of insulating layer, can be to device threshold after nitrogen dioxide gas is adsorbed
Voltage produces bigger effect, so that device threshold voltage is linear with nitrogen dioxide gas concentration, and then realizes whole
The multi-parameter detection of a device；
4th, the present invention can work at room temperature, without heating source, reduce device cost and energy consumption, zinc oxide nano
Rice grain and required insulating materials derive from a wealth of sources, and have realized industrialized production, and the advantage is for the sensor that largely uses
It is particularly important.
Description of the drawings
Fig. 1 is the structure diagram of the present invention；
In figure：1-1 source electrodes, 1-2 drain electrodes, 2- impurity molecule organic semiconductors, 3- organic semiconductor layers, 4- zinc oxide
Nano particle 5- insulating layers, 6- gate electrodes, 7- substrates.
Fig. 2 is the principle of the present invention schematic diagram；
Fig. 3 is embodiment 1, for the response curve of the nitrogen dioxide of various concentration.
Specific embodiment
The invention will be further described below in conjunction with the accompanying drawings.
With reference to Fig. 1, a kind of organic field-effect tube gas sensor based on mix insulation layer of the invention, including substrate 7,
Gate electrode 6, insulating layer 5, Zinc oxide nanoparticle 4, organic semiconductor layer 3, impurity molecule organic semiconductor 2, source electrode and leakage
Electrode 1, the gate electrode setting and substrate, insulating layer are set on gate electrode, and source electrode and drain electrode is set respectively
On organic semiconductor layer；The organic semiconductor layer is discontinuous film；The surface of insulating layer is dispersed with zinc oxide nano
Rice grain；The impurity molecule organic semiconductor is deposited in organic semiconductor lamellar spacing and is contacted with Zinc oxide nanoparticle.
The following is specific embodiments of the present invention：
Embodiment 1：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 50 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 500 nm, and a diameter of 5 nm of zinc-oxide nano, organic semiconductor layer material is simultaneously five
Benzene, thickness are 20 nm, and impurity molecule organic semiconductor is CuPc, and source electrode drain electrode is Au, and thickness is 50 nm.
Preparation method is as follows：
1. thoroughly being cleaned to the glass substrate 7 for having sputtered gate electrode ITO, dried up after cleaning with drying nitrogen；
2. mix insulation layer 5 is prepared on ITO using spin-coating method；
3. Zinc oxide nanoparticle is prepared in surface of insulating layer using spin-coating method；
4. pentacene organic semiconductor layer and CuPc impurity molecule organic semiconductor are prepared using vacuum vapour deposition；
4. source electrode drain electrode is prepared using vacuum vapour deposition.
Embodiment 2：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 100 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 2000 nm, and a diameter of 10 nm of zinc-oxide nano, organic semiconductor layer material is simultaneously
Pentaphene, thickness are 30 nm, and impurity molecule organic semiconductor is CuPc, and source electrode drain electrode is Au, and thickness is 100 nm.
Preparation method is such as embodiment 1.
Embodiment 3：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 80 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 1000 nm, and a diameter of 8 nm of zinc-oxide nano, organic semiconductor layer material is simultaneously
Pentaphene, thickness be 25 nm, impurity molecule organic semiconductor be N, N '-diamyl -3,4,9,10- dicarboximides, source electrode
Drain electrode is Au, and thickness is 80 nm.
Preparation method is such as embodiment 1.
Embodiment 4：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 80 nm, and mix insulation layer 5 is by polyphenyl second
Alkene mixes, thickness be 2000 nm, a diameter of 8 nm of zinc-oxide nano, organic semiconductor layer material be pentacene, thickness
For 25 nm, impurity molecule organic semiconductor is N, N '-diamyl -3,4,9,10- dicarboximides, and source electrode drain electrode is equal
For Au, thickness is 80 nm.
Preparation method is such as embodiment 1.
Embodiment 5：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 80 nm, and mix insulation layer 5 is by polyphenyl second
Alkene mixes, thickness be 2000 nm, a diameter of 8 nm of zinc-oxide nano, organic semiconductor layer material be six thiophene, thickness
For 25 nm, impurity molecule organic semiconductor is N, N '-diamyl -3,4,9,10- dicarboximides, and source electrode drain electrode is equal
For Au, thickness is 80 nm.
Preparation method is such as embodiment 1.
Embodiment 6：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 50 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 500 nm, and a diameter of 5 nm of zinc-oxide nano, organic semiconductor layer material is six thiophenes
Fen, thickness are 20 nm, and impurity molecule organic semiconductor is CuPc, and source electrode drain electrode is Au, and thickness is 50 nm.
Preparation method is such as embodiment 1.
Embodiment 7：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 50 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 500 nm, and a diameter of 5 nm of zinc-oxide nano, organic semiconductor layer material is six thiophenes
Fen, thickness are 20 nm, and impurity molecule organic semiconductor is perfluor CuPc, and source electrode drain electrode is Au, and thickness is 50 nm.
Preparation method is such as embodiment 1.
Embodiment 8：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 50 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 500 nm, and a diameter of 5 nm of zinc-oxide nano, organic semiconductor layer material is red glimmering
Alkene, thickness are 20 nm, and impurity molecule organic semiconductor is perfluor CuPc, and source electrode drain electrode is Au, and thickness is 50 nm.
Preparation method is such as embodiment 1.
Embodiment 9：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 50 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 500 nm, and a diameter of 5 nm of zinc-oxide nano, organic semiconductor layer material is 6,
13-two three isopropyl ester silicon substrate acetylene pentacenes, thickness are 20 nm, and impurity molecule organic semiconductor is CuPc, and source electrode is leaked electricity
Pole is Au, and thickness is 50 nm.
Preparation method is as follows：
1. thoroughly being cleaned to the glass substrate 7 for having sputtered gate electrode ITO, dried up after cleaning with drying nitrogen；
2. mix insulation layer 5 is prepared on ITO using spin-coating method；
3. Zinc oxide nanoparticle is prepared in surface of insulating layer using spin-coating method；
4. 6,13-two three isopropyl ester silicon substrate acetylene pentacene organic semiconductor layers are prepared using spray coating method；
5. impurity molecule organic semiconductor CuPc is prepared using vacuum vapour deposition；
4. source electrode and drain electrode is prepared using vacuum vapour deposition.
Embodiment 10：
As shown in Figure 1：Substrate 7 is glass, and gate electrode 6 is ITO, and thickness is 100 nm, and mix insulation layer 5 is by poly- methyl
Methyl acrylate mixes, and thickness is 200 nm, and a diameter of 5 nm of zinc-oxide nano, organic semiconductor layer material is 6,
13-two three isopropyl ester silicon substrate acetylene pentacenes, thickness be 30 nm, impurity molecule organic semiconductor be N, N '-diamyl-3,4,
9,10- dicarboximides, source electrode drain electrode are Au, and thickness is 50 nm..
Preparation method is as follows：
1. the glass substrate 7 for having sputtered gate electrode ITO is thoroughly cleaned, dried up after cleaning with drying nitrogen；
2. mix insulation layer 5 is prepared on ITO using spin-coating method；
3. Zinc oxide nanoparticle is prepared in surface of insulating layer using spin-coating method；
4. 6,13-two three isopropyl ester silicon substrate acetylene pentacene organic semiconductor layers are prepared using spray coating method；
5. it is sub- to prepare impurity molecule organic semiconductor N, N '-two formyls of diamyl -3,4,9,10- using spray coating method method
Amine；
5. source electrode and drain electrode is prepared using vacuum vapour deposition.
The embodiment of the present invention is better embodiment, but its specific implementation is not limited to this, the ordinary skill people of this field
Member easily according to above-described embodiment, understands the spirit of the present invention, and makes different amplification and variation, without departing from this hair
It is bright, all belong within protection scope of the present invention.
Claims (10)
1. a kind of organic field-effect tube nitrogen dioxide sensor, is followed successively by substrate from top to bottom（7）, gate electrode（6）, insulating layer
（5）, which is characterized in that the insulating layer（5）Dispersion on surface has Zinc oxide nanoparticle (4)；Zinc oxide nanoparticle（4）On
The organic semiconductor layer of promising discontinuous film is set（3）, organic semiconductor layer（3）It sinks in the upper and gap of organic semiconductor layer
Shallow lake has and Zinc oxide nanoparticle（4）The impurity molecule organic semiconductor of contact（2）, impurity molecule organic semiconductor（2）On set
It is equipped with source electrode（1-1）And drain electrode（1-2）.
2. a kind of organic field-effect tube nitrogen dioxide sensor according to claim 1, which is characterized in that described organic half
Conductor layer（3）It is made of p-type small molecule organic semiconductor material, including aphthacene, pentacene, 6,13-two three isopropyl ester silicon substrates
One kind in acetylene pentacene, rubrene or six thiophene, the organic semiconductor layer thickness are 20 nm-, 30 nm.
3. a kind of organic field-effect tube nitrogen dioxide sensor according to claim 1, which is characterized in that the impurity has
Machine semiconductor molecule（2）For N-shaped small molecule or the p-type small molecule of high electron density, the N-shaped small molecule includes C60, N,
N '-diamyl -3,4,9,10- dicarboximides, N, N '-diphenyl -3,4,9,10- dicarboximides, N, N '-two are pungent
Bis- (2,5- the di-tert-butyl-phenyls) -3,4,9,10- dicarboximides of base -3,4,9,10- dicarboximides, N, N'-, perfluor
CuPc, Isosorbide-5-Nitrae, 5,8- naphthalenetetracarbacidic acidic acid anhydrides, the p-type small molecule include CuPc, Phthalocyanine Zinc, Cobalt Phthalocyanine.
A kind of 4. organic field-effect tube nitrogen dioxide sensor according to claim 1, which is characterized in that the insulating layer
（5）Thickness be 500 nm -2000 nm, the Zinc oxide nanoparticle（4）Particle diameter be 5 nm -10 nm.
A kind of 5. organic field-effect tube nitrogen dioxide sensor according to claim 1, which is characterized in that the insulating layer
For polystyrene, poly- а-methyl styrene, polymethyl methacrylate, makrolon, dimethyl silicone polymer, polyvinyl alcohol,
One kind in polyvinylpyrrolidone or pla-pcl and copolymer between them.
A kind of 6. organic field-effect tube nitrogen dioxide sensor according to claim 1, which is characterized in that gate electrode（6）、
Source electrode（1-1）And drain electrode（1-2）It is made of one kind in gold, silver or copper and its alloy material, source electrode（1-1）And electric leakage
Pole（1-2）Thickness be 50 ~ 100 nm.
A kind of 7. organic field-effect tube nitrogen dioxide sensor according to claim 1, which is characterized in that the substrate
（7）For silicon chip, glass, thin polymer film, metal foil, plant fiber, fibrin gel, gelatin, polylactic acid, viral fiber
It is one or more in element, polylactic acid-co-glycolic acid.
8. according to a kind of preparation method of organic field-effect tube nitrogen dioxide sensor of claim 1-7 any one of them,
It is characterized in that, includes the following steps：
1. first substrate is thoroughly cleaned, it is dry after cleaning；
2. prepare gate electrode in substrate surface；
3. there is the insulating layer of Zinc oxide nanoparticle in gate electrode Dispersion on surface prepared above；
4. discontinuous organic semiconductor layer is prepared on the insulating layer；
5. preparing impurity molecule organic semiconductor on the organic semiconductor layer, source electricity is prepared on impurity molecule organic semiconductor
Pole and drain electrode.
9. preparation method according to claim 8, which is characterized in that step 3. in, insulating layer passes through spin coating, roller coating, drop
Prepared by a kind of method in film, coining, printing or spraying, Zinc oxide nanoparticle is using in quick spin coating, printing or spraying
It is prepared by a kind of method.
10. preparation method according to claim 8, which is characterized in that step 2. 5. in, gate electrode, source electrode, drain electrode
It is by vacuum thermal evaporation, magnetron sputtering, the chemical vapor deposition of plasma enhancing, silk-screen printing, printing or spin coating
It is prepared by a kind of method, the step 4. in, the organic semiconductor layer is chemical vapor deposition, the heat by plasma enhancing
It is prepared by a kind of method in oxidation, spin coating, vacuum evaporation, roller coating, drop film, coining, printing or spraying.
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| CN106596653A (en) * | 2016-12-09 | 2017-04-26 | 长春工业大学 | Method for preparing three-dimensional efficient organic thin-film sensor device |
| CN110261461B (en) * | 2019-07-08 | 2021-06-01 | 长春工业大学 | Preparation method of ultrathin heterojunction composite film gas sensor based on OFETs |
| CN110501385A (en) * | 2019-08-29 | 2019-11-26 | 电子科技大学 | A kind of Organic Thin Film Transistors nitrogen dioxide sensor and preparation method thereof based on air dielectric layer |
| CN112649472A (en) * | 2021-01-09 | 2021-04-13 | 长春工业大学 | NO based on electrostatic spraying polymer insulation layer2Preparation method of gas sensor |
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