CN109946349B - Organic field effect transistor, preparation method thereof and biogenic amine gas-sensitive sensor - Google Patents
Organic field effect transistor, preparation method thereof and biogenic amine gas-sensitive sensor Download PDFInfo
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Abstract
The invention discloses an organic field effect transistor, a preparation method thereof and a biogenic amine gas sensor, wherein the organic field effect transistor comprises a substrate, an organic semiconductor layer, a biogenic amine sensitive layer, an insulating layer and a grid which are sequentially stacked from bottom to top, wherein the substrate is also provided with a drain electrode and a source electrode, the organic semiconductor layer covers the source electrode and the drain electrode and the area which is not covered by the source electrode and the drain electrode on the substrate; the sensitivity of the biogenic amine sensitive layer to biogenic amine is set to be greater than the sensitivity of the organic semiconductor layer to biogenic amine. In the invention, the organic field effect transistor in a power-on state can form a conductive channel on the biogenic amine sensitive layer and the organic semiconductor layer, when biogenic amine exists, the biogenic amine sensitive layer and the organic semiconductor layer generate chemical reaction to change the resistance of the conductive channel, and the biogenic amine can be sensed by sensing the change of the resistance, so that the detection sensitivity is effectively improved, and the purposes of optimizing the detection effect and improving the detection efficiency are realized.
Description
Technical Field
The invention relates to the technical field of gas detection, in particular to the technical field of gas detection by using an organic semiconductor material, and specifically relates to an organic field effect transistor, a preparation method thereof and a biological amine gas-sensitive sensor.
Background
Biogenic amine is nitrogen-containing low-molecular organic alkali, is mainly formed by decarboxylation of amino acid, and is widely applied to meat products, aquatic products and fermented products rich in amino acid and protein. Biogenic amines can be classified into three groups according to their structure: aliphatic, including putrescine, cadaverine, spermine, spermidine, and the like; aromatic, including tyramine, phenethylamine, and the like; heterocyclic amines including histamine, tryptamine, and the like. Proper amounts of biogenic amines are necessary to maintain normal physiological functions of the human body, but if the biogenic amines are ingested into the human body in excess, allergic reactions are caused, and in severe cases, the life can be threatened. In addition, biogenic amines are often produced during the decay or fermentation of food, the onset of food poisoning and certain toxicological properties are closely related to histamine and tyramine, and the biogenic amine content in food can be used as an important index of food quality. Therefore, the effective and rapid detection of biogenic amine in food has important significance on food quality and safety.
Due to the lack of chromophoric groups in biogenic amine molecules, the biogenic amine has no ultraviolet absorption, fluorescence and electrochemical activity, so that the separation and the determination of various biogenic amines are very difficult. The traditional method for measuring biogenic amine mainly depends on biochemical methods, such as an enzyme biosensor method, a thin-layer chromatography method, a gas chromatography method, an ion chromatography method, a capillary electrophoresis method, a high performance liquid chromatography method and the like, wherein the high performance liquid chromatography method has the advantages of high column efficiency, high separation efficiency, high analysis speed, high sensitivity, accurate quantitative analysis and the like, and most students take the biogenic amine as a main method for analyzing biogenic amine in food, but the method has small detection amount, can detect only one sample at a time, and has high cost and low overall efficiency. In order to solve the above problems, a method for measuring biogenic amines by an inorganic metal oxide semiconductor gas sensor has been proposed, but the method has a high operating temperature and requires a heater; the sensitivity of detecting most organic gases is low; narrow detection range and the like.
Disclosure of Invention
The invention mainly aims to provide an organic field effect transistor, a preparation method and a biogenic amine gas sensor, and aims to solve the problems of low detection sensitivity and low detection efficiency of the traditional detection method.
In order to achieve the above object, the present invention provides an organic field effect transistor for sensing biogenic amine in food, the organic field effect transistor includes a substrate, an organic semiconductor layer, a biogenic amine sensitive layer, an insulating layer and a gate electrode, which are sequentially stacked from bottom to top, wherein the upper end of the substrate is further provided with a source electrode and a drain electrode, the organic semiconductor layer covers the drain electrode and the source electrode, and the substrate is covered by the drain electrode and the source electrode;
wherein the sensitivity of the biogenic amine sensitive layer to biogenic amine is set to be greater than the sensitivity of the organic semiconductor layer to biogenic amine.
Optionally, the material of the organic semiconductor layer is any one of compounds having structures shown in the following structural formulas (I), (II), (III) and (IV):
optionally, the material of the biogenic amine sensitive layer is any one of compounds having the structures shown in the following structural formulas (V) and (VI):
wherein, in structural formula (v): and M ═ Au or M ═ Co.
Optionally, the material of the insulating layer is water or phosphate buffered saline.
Optionally, the substrate is made of glass, silicon wafer or ceramic; alternatively, the first and second electrodes may be,
the source electrode, the drain electrode and the grid electrode are made of aluminum or gold.
Optionally, the thickness of the organic semiconductor layer is 60nm to 70 nm; alternatively, the first and second electrodes may be,
the thickness of the biogenic amine sensitive layer is 8 nm-12 nm; alternatively, the first and second electrodes may be,
the thickness of the substrate is 45 nm-55 nm.
In addition, the present invention also provides a method for preparing the organic field effect transistor as described above, comprising the steps of:
providing a substrate;
arranging a drain electrode and a source electrode on the substrate;
providing an organic semiconductor layer on the source electrode and the drain electrode and on a region of the substrate not covered by the drain electrode and the source electrode;
disposing a biogenic amine sensitive layer on the organic semiconductor layer;
arranging an insulating layer on the biogenic amine sensitive layer;
and arranging a grid electrode on the insulating layer to obtain the organic field effect transistor.
Optionally, the gate, the source, and the drain are all disposed by vacuum thermal evaporation, magnetron sputtering, or plasma-enhanced chemical vapor deposition.
Optionally, the step of disposing an insulating layer on the biogenic amine sensitive layer comprises: and dripping 1-3 mu L of water or phosphate buffer solution on the biogenic amine sensitive layer to form the insulating layer.
In addition, the invention also provides a biological amine gas-sensitive sensor which comprises the organic field effect transistor.
In the technical scheme provided by the invention, the organic field effect transistor in a power-on state can form a conducting channel on the biogenic amine sensitive layer and the organic semiconductor layer, when biogenic amine exists in the environment, the biogenic amine sensitive layer and the organic semiconductor layer generate chemical reaction, and the resistance of the conducting channel is changed, so that the aim of sensing the biogenic amine in the environment can be realized by sensing the change of the resistance; in addition, the organic semiconductor layer is arranged above the drain electrode and the source electrode, and the biogenic amine sensitive layer which is more sensitive to biogenic amine is additionally arranged above the organic semiconductor layer, so that the contact area of the organic field effect transistor and the biogenic amine is increased, the detection sensitivity can be effectively improved, and the purposes of optimizing the detection effect and improving the detection efficiency are achieved.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, it is obvious that the drawings in the following description are only some embodiments of the present invention, and for those skilled in the art, other drawings can be obtained according to the structures shown in the drawings without creative efforts.
Fig. 1 is a schematic structural diagram of an organic field effect transistor according to an embodiment of the present invention.
The reference numbers illustrate:
| reference numerals | Name (R) | Reference numerals | Name (R) |
| 100 | Organic |
3 | |
| 1 | Substrate | 4 | Biogenic amine |
| 21 | |
5 | |
| 22 | |
6 | Grid electrode |
The implementation, functional features and advantages of the objects of the present invention will be further explained with reference to the accompanying drawings.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
It should be noted that, if directional indications (such as up, down, left, right, front, and back … …) are involved in the embodiment of the present invention, the directional indications are only used to explain the relative positional relationship between the components, the movement situation, and the like in a specific posture (as shown in the drawing), and if the specific posture is changed, the directional indications are changed accordingly.
In addition, if there is a description of "first", "second", etc. in an embodiment of the present invention, the description of "first", "second", etc. is for descriptive purposes only and is not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include at least one such feature. In addition, the meaning of "and/or" appearing throughout includes three juxtapositions, exemplified by "A and/or B" including either A or B or both A and B. In addition, technical solutions between various embodiments may be combined with each other, but must be realized by a person skilled in the art, and when the technical solutions are contradictory or cannot be realized, such a combination should not be considered to exist, and is not within the protection scope of the present invention.
Due to the lack of chromophoric groups in biogenic amine molecules, the biogenic amine has no ultraviolet absorption, fluorescence and electrochemical activity, so that the separation and the determination of various biogenic amines are very difficult. The traditional method for measuring biogenic amine mainly depends on biochemical methods, such as an enzyme biosensor method, a thin-layer chromatography method, a gas chromatography method, an ion chromatography method, a capillary electrophoresis method, a high performance liquid chromatography method and the like, wherein the high performance liquid chromatography method has the advantages of high column efficiency, high separation efficiency, high analysis speed, high sensitivity, accurate quantitative analysis and the like, and most students take the biogenic amine as a main method for analyzing biogenic amine in food, but the method has small detection amount, can detect only one sample at a time, and has high cost and low overall efficiency. In order to solve the above problems, a method for measuring biogenic amines by an inorganic metal oxide semiconductor gas sensor has been proposed, but the method has a high operating temperature and requires a heater; the sensitivity of detecting most organic gases is low; narrow detection range and the like.
In view of the above, the present invention provides a biological amine gas sensor, which includes an organic field effect transistor and other components, fig. 1 is an embodiment of the organic field effect transistor provided in the present invention, and since the main inventive point of the present invention lies in the improvement of the organic field effect transistor, the following description mainly refers to the organic field effect transistor with reference to the specific drawings.
Referring to fig. 1, in the present embodiment, the organic field effect transistor 100 is used for sensing biogenic amine in an environment and a content thereof, and is particularly suitable for sensing biogenic amine in food, the organic field effect transistor 100 includes a substrate 1, an organic semiconductor layer 3, a biogenic amine sensitive layer 4, an insulating layer 5, and a gate electrode 6, which are sequentially stacked from bottom to top, in addition, a drain electrode 21 and a source electrode 22 are further disposed at an upper end of the substrate 1, and the organic semiconductor layer 3 covers the drain electrode 21 and the source electrode 22, and a region of the substrate 1 not covered by the drain electrode 21 and the source electrode 22. In addition, the sensitivity of the biogenic amine sensitive layer 4 to biogenic amine is set to be greater than the sensitivity of the organic semiconductor layer 3 to biogenic amine, which can be embodied in particular by: the material of the biological amine sensitive layer 4 has higher sensitivity to biological amine than the material of the organic semiconductor layer 3, or the contact area of the biological amine sensitive layer 4 and the biological amine is larger than the contact area of the organic semiconductor layer 3 and the biological amine. In operation, a positive voltage is applied to the gate electrode 6 and the drain electrode 21, a negative voltage is applied to the source electrode 22, or the source electrode 22, the drain electrode 21 and the gate electrode 6 are equivalent to two electrode plates of a capacitor, and the organic semiconductor layer 3, the biogenic amine sensitive layer 4 and the insulating layer 5 are in contact conduction layer by layer, so that the organic field effect transistor 100 is in an electrified state as a whole to form the capacitor.
In the technical scheme provided by the invention, the organic field effect transistor 100 in a power-on state can form a conductive channel between the biogenic amine sensitive layer 4 and the organic semiconductor layer 3, when biogenic amine exists in the environment, the biogenic amine sensitive layer 4 and the organic semiconductor layer 3 generate chemical reaction, and the resistance of the conductive channel is changed, so that the aim of sensing the biogenic amine in the environment can be achieved by sensing the change of the resistance; in addition, the organic semiconductor layer 3 is arranged above the drain electrode 21 and the source electrode 22, and the biogenic amine sensitive layer 4 which is more sensitive to biogenic amine is additionally arranged above the organic semiconductor layer 3, so that the contact area between the organic field effect transistor 100 and the biogenic amine is increased, the detection sensitivity can be effectively improved, and the purposes of optimizing the detection effect and improving the detection efficiency are achieved.
Further, in the present embodiment, the material of the organic semiconductor layer 3 is any one of compounds having structures represented by the following structural formulae (i), (ii), (iii), and (iv):
wherein, the compound in the structural formula (I) is PDI8-CN2 material, the compound in the structural formula (II) is P3HT material, the compound in the structural formula (III) is Pentacene material, and the compound in the structural formula (IV) is PEDOT: the PSS material can react with biogenic amine sensitively at normal temperature, specifically biogenic amine gas can rapidly penetrate through the organic semiconductor layer 3 through a grain boundary to enter a charge accumulation layer, and then a trap is generated at the grain boundary to reduce the mobility of a charge carrier, so that the resistance of a conductive channel is rapidly changed, and the aim of sensitively detecting biogenic amine is fulfilled; the above compounds are all existing products, are compatible with the substrate 1, and are suitable for low-temperature processing and mass production.
In addition, in this embodiment, the material of the biogenic amine sensitive layer 4 is any one of compounds having structures represented by the following structural formulas (v) and (vi):
wherein, in structural formula (v): and M ═ Au or M ═ Co. The compound in the structural formula (V) is Au-EHO material, the compound in the structural formula (VI) is Co-EHO material, the biological amine sensitive layer 4 covers the organic semiconductor layer 3 and is directly contacted with biological amine in the environment, and the organic semiconductor layer is characterized in that the Au-EHO material and the Co-EHO material are compared with the PDI8-CN2 material, the P3HT material, the Pentacene material and the PEDOT: the PSS material has higher sensitivity to biogenic amine, specifically, biogenic amine gas molecules enter a cavity of the biogenic amine sensitive layer 4 and then are bonded with molecules of the biogenic amine sensitive layer 4 to generate an electric dipole, so that the conductive characteristic of the organic semiconductor layer 3 is further influenced, the organic field effect transistor 100 is more sensitive to biogenic amine gas, the detection range of the organic field effect transistor 100 is widened, the detection speed is accelerated, and the detection efficiency is improved.
Next, in this embodiment, the insulating layer 5 is made of water or phosphate buffered saline, and compared with a conventional inorganic insulating material, the insulating layer 5 formed by water or phosphate buffered saline has a higher dielectric constant, which can effectively improve the capacitance of the organic field effect transistor 100, thereby improving the on-state current in the organic field effect transistor 100 and reducing the operating voltage required by the organic field effect transistor 100. When in use, the grid electrode 6 is directly inserted into water or phosphate buffer saline solution.
Further, in this embodiment, the substrate 1 is made of glass, silicon wafer or ceramic, and has good insulation property and low material price, which is beneficial to reducing the burden of economic cost; alternatively, the material of the drain electrode 21, the source electrode 22, and the gate electrode 6 is aluminum or gold, which helps to expand the capacitance without increasing the volume and mass of the organic field effect transistor 100.
Further, in the present embodiment, the thickness of the organic semiconductor layer 3 is 60nm to 70nm, or the thickness of the biogenic amine sensitive layer 4 is 8nm to 12nm, or the thickness of the substrate 1 is 45nm to 55nm, and preferably 50 nm. The thicknesses of the organic semiconductor layer 3, the biogenic amine sensitive layer 4 and the insulating layer 5 affect capacitance induction among the source electrode 22, the drain electrode 21 and the gate electrode 6, if the thicknesses are larger, capacitance change sensed by the organic field effect transistor 100 is smaller, even good capacitance induction cannot be formed, and instant sensing of biogenic amine is affected; on the contrary, if the thickness is small, the required working voltage is large, which is not favorable for the user, therefore, it is preferable that the thickness of the organic semiconductor layer 3 is 65nm and the thickness of the biogenic amine sensitive layer 4 is 10 nm.
In addition, the present invention also provides a method for preparing the organic field effect transistor 100, which specifically comprises the following steps:
step S10: providing a substrate 1;
step S20: providing a drain electrode 21 and a source electrode 22 on the substrate 1;
step S30: providing an organic semiconductor layer 3 on the drain electrode 21 and the source electrode 22 and on a region of the substrate 1 not covered by the drain electrode 21 and the source electrode 22;
step S40: a biogenic amine sensitive layer 4 is arranged on the organic semiconductor layer 3;
step S50: an insulating layer 5 is arranged on the biological amine sensitive layer 4;
step S60: a gate electrode 6 is provided on the insulating layer 5 to obtain the organic field effect transistor 100.
In this embodiment, according to practical application, a suitable material and thickness of the substrate 1 are selected, a silicon wafer is taken as the substrate 1 as an example, the silicon wafer is sequentially ultrasonically cleaned by acetone, isopropyl alcohol and the like, then the silicon wafer is rinsed by ethanol and deionized water, and finally the surface of the silicon wafer is dried by nitrogen; then, evaporating the drain electrode 21 and the source electrode 22 on the substrate 1, and then continuing to evaporate the organic semiconductor layer 3 and the biogenic amine sensitive layer 4 on the drain electrode 21, the source electrode 22 and the substrate 1 in sequence; the insulating layer 5 is prepared on the biogenic amine sensitive layer 4, and finally the gate electrode 6 is disposed on the insulating layer 5, for example, at least the lower end of the gate electrode 6 is inserted into the insulating layer 5, so as to obtain the organic field effect transistor 100.
Further, in this embodiment, the gate electrode 6, the source electrode 22 and the drain electrode 21 are disposed by vacuum thermal evaporation, magnetron sputtering or plasma enhanced chemical vapor deposition. For example, the substrate 1 is placed in a vacuum coater in a degree of vacuum of 6.5X 10-4And evaporating gold on the substrate 1 at the speed of 1A/s under the condition of Pa to obtain the drain electrode 21 and the source electrode 22. The specific preparation method of the gate 6 is similar to that described above and is not described in detail, and in addition, the specific steps and related requirements of magnetron sputtering or plasma enhanced chemical vapor deposition can refer to the prior art and are not described in detail herein.
Further, in this embodiment, the step S50 includes: and dripping 1-3 mu L of water or phosphate buffer solution on the biogenic amine sensitive layer 4 to form the insulating layer 5. For example, in an environment where biogenic amine needs to be detected, about 2 μ L of water or phosphate buffered saline solution may be dropped on the biogenic amine sensitive layer 4 by using a dropper, and then the gate electrode 6 is inserted into the water or phosphate buffered saline solution, thereby forming the complete organic field effect transistor 100. The specific quantity, composition and the like of the insulating layer 5 can be adaptively adjusted according to practical application, so that different biogenic amines under different environments can be detected in a targeted manner, and more accurate results can be obtained more quickly and effectively.
Taking a specific embodiment of the organic field effect transistor 100 as an example, a 50nm thick glass substrate 1 may be provided with a gold drain electrode 21 and a gold source electrode 22 by magnetron sputtering on the substrate at room temperature; then, an organic semiconductor layer 3 with a thickness of 65nm is arranged on the drain electrode 21 and the source electrode 22 and on the substrate 1 in the area not covered by the drain electrode 21 and the source electrode 22 by means of vapor deposition, and the material of the organic semiconductor layer 3 is P3 HT; arranging a biogenic amine sensitive layer 4 with the thickness of 10nm on the organic semiconductor layer 3 in an evaporation mode, wherein the material of the biogenic amine sensitive layer 4 is Co-EHO; sucking 2 mu L of phosphate buffer salt solution on the biogenic amine sensitive layer 4 by using a suction pipe and dripping the phosphate buffer salt solution on the biogenic amine sensitive layer 4 to form an insulating layer 5; finally, a gold gate electrode 6 is provided on the insulating layer 5 by vacuum thermal evaporation to obtain the organic field effect transistor 100. By using the measurement technology of the existing measurement equipment, it can be effectively detected that when Vg is equal to 0.6V, the saturation current corresponding to the organic field effect transistor 100 is 0.9 μ a, and the carrier mobility is 2.3 × 10-3cm2The threshold voltage is 0.03V, the response speed is 0.2s, and the organic field effect transistor 100 prepared by the method has good response result to biogenic amine at room temperature, high response speed and high sensitivity.
The above description is only a preferred embodiment of the present invention, and is not intended to limit the scope of the present invention, and all modifications and equivalents of the present invention, which are made by the contents of the present specification and the accompanying drawings, or directly/indirectly applied to other related technical fields, are included in the scope of the present invention.
Claims (9)
1. An organic field effect transistor is used for sensing biogenic amine in food and is characterized by comprising a substrate, an organic semiconductor layer, a biogenic amine sensitive layer, an insulating layer and a grid which are sequentially stacked from bottom to top, wherein the upper end of the substrate is also provided with a drain electrode and a source electrode, the organic semiconductor layer covers the drain electrode and the source electrode and the substrate is not covered by the drain electrode and the source electrode;
wherein the sensitivity of the biogenic amine sensitive layer to biogenic amines is set to be greater than the sensitivity of the organic semiconductor layer to biogenic amines;
the material of the organic semiconductor layer is any one of compounds with structures shown in the following structural formulas (I), (II), (III) and (IV):
2. the organic field-effect transistor according to claim 1, wherein a material of the biogenic amine sensitive layer is a compound having a structure represented by the following structural formula (v):
wherein, in structural formula (v): and M ═ Au or M ═ Co.
3. The organic field-effect transistor according to claim 1, wherein a material of the insulating layer is water or phosphate buffered saline.
4. The organic field-effect transistor according to claim 1, wherein a material of the substrate is glass, a silicon wafer, or ceramic; alternatively, the first and second electrodes may be,
the source electrode, the drain electrode and the grid electrode are made of aluminum or gold.
5. The organic field-effect transistor according to claim 1, wherein the thickness of the organic semiconductor layer is 60nm to 70 nm; alternatively, the first and second electrodes may be,
the thickness of the biogenic amine sensitive layer is 8 nm-12 nm; alternatively, the first and second electrodes may be,
the thickness of the substrate is 45 nm-55 nm.
6. A method of manufacturing an organic field effect transistor according to any of claims 1 to 5, comprising the steps of:
providing a substrate;
arranging a drain electrode and a source electrode on the substrate;
providing an organic semiconductor layer on the drain electrode and the source electrode and on a region of the substrate not covered by the drain electrode and the source electrode;
disposing a biogenic amine sensitive layer on the organic semiconductor layer;
arranging an insulating layer on the biogenic amine sensitive layer;
and arranging a grid electrode on the insulating layer to obtain the organic field effect transistor.
7. The method of claim 6, wherein the gate electrode, the source electrode and the drain electrode are disposed by vacuum thermal evaporation, magnetron sputtering or plasma enhanced chemical vapor deposition.
8. The method of manufacturing an organic field effect transistor according to claim 6, wherein the step of providing an insulating layer on the biogenic amine sensitive layer comprises: and dripping 1-3 mu L of water or phosphate buffer solution on the biogenic amine sensitive layer to form the insulating layer.
9. A biogenic amine gas sensor, comprising an organic field effect transistor according to any one of claims 1 to 5.
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