CN110657898A - Temperature sensor based on double-layer graphene and preparation method - Google Patents
Temperature sensor based on double-layer graphene and preparation method Download PDFInfo
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- CN110657898A CN110657898A CN201910957146.8A CN201910957146A CN110657898A CN 110657898 A CN110657898 A CN 110657898A CN 201910957146 A CN201910957146 A CN 201910957146A CN 110657898 A CN110657898 A CN 110657898A
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- G01K7/00—Measuring temperature based on the use of electric or magnetic elements directly sensitive to heat ; Power supply therefor, e.g. using thermoelectric elements
- G01K7/16—Measuring temperature based on the use of electric or magnetic elements directly sensitive to heat ; Power supply therefor, e.g. using thermoelectric elements using resistive elements
- G01K7/18—Measuring temperature based on the use of electric or magnetic elements directly sensitive to heat ; Power supply therefor, e.g. using thermoelectric elements using resistive elements the element being a linear resistance, e.g. platinum resistance thermometer
- G01K7/183—Measuring temperature based on the use of electric or magnetic elements directly sensitive to heat ; Power supply therefor, e.g. using thermoelectric elements using resistive elements the element being a linear resistance, e.g. platinum resistance thermometer characterised by the use of the resistive element
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Abstract
A novel temperature sensor based on double-layer graphene comprises at least double-layer graphene, a pair of metal electrodes and a substrate; double-layer graphene grows or is arranged on the substrate, the double-layer graphene has an overlapping area, namely a stacking area, and the double-layer graphene is respectively connected with a pair of electrodes. Each layer of graphene is connected with a metal electrode, and the electrode material is selected from various metal materials with good conductivity such as titanium, gold, chromium, silver or copper; temperature sensors suitable for different purposes are developed through the spacing between graphene layers, the rotation angle or the overlapping contact area, or changing the materials of electrodes, leads and substrates. The graphene can be from graphene prepared by a chemical vapor deposition method, graphene prepared by a silicon carbide epitaxial method and exfoliated graphene. And manufacturing an electrode at one end of each of the two layers of graphene by using an electron beam lithography technology or a lithography technology, and performing electron beam evaporation or thermal evaporation on the metal electrode. The sensor effectively improves the heat conduction performance and the sensitivity of the sensor.
Description
Technical Field
The invention belongs to the field of temperature sensors, and particularly relates to a novel flexible temperature sensor based on double-layer or few-layer graphene, which is expected to be applied to the fields of aerospace, intelligent weapons, intelligent buildings, health monitoring and the like.
Background
In the current technical development, the temperature sensor has wide application value in various fields such as production, life and the like. Common sensors can be classified into contact type and non-contact type according to different measurement modes. The sensitivity of the conventional contact temperature sensor needs to be improved, and the application range is narrow. The non-contact temperature sensor has high intrinsic noise and is greatly influenced by the outside.
Graphene is a two-dimensional star material, and has received great attention due to its excellent electrical, thermal and mechanical properties. The coupling effect between the electrons and the phonons of the graphene is weak, so that the temperature sensor based on the graphene as a sensitive element is expected to realize temperature detection with high detection speed and high sensitivity in a high-temperature interval, and is expected to be applied in the field of aerospace. As an electronic skin for the development trend of the electronic industry, monitoring of body temperature is a key health parameter. However, it remains challenging to make a real-time, biocompatible, lightweight, easy to operate, and highly accurate flexible temperature sensor.
In the prior art of manufacturing a temperature sensor by using a carbon material, carbon black, graphene oxide and a three-dimensional graphene material are used as common sensitive element materials, so that the transparency is difficult to realize, and the performance stability of the temperature sensor in different batches is poor. In the invention, the intrinsic graphene is utilized, so that the stability and the sensitivity of the temperature sensor can be greatly improved.
Disclosure of Invention
The invention aims to provide a novel temperature sensor based on double-layer or few-layer graphene and a preparation method thereof, and the novel temperature sensor is expected to be applied to the fields of aerospace, intelligent weapons, intelligent buildings, health monitoring and the like by adjusting the inter-graphene coupling atomic layer spacing, contact corners, contact areas and the like.
The technical scheme of the invention is as follows: a temperature sensor based on double-layer graphene comprises at least double-layer graphene 1, a pair of electrodes 2 and a substrate 4; double-layer graphene is grown or placed on the substrate 4, the double-layer graphene has a stacking area, the double-layer graphene is respectively connected with one of the pair of electrodes 2, and temperature sensors suitable for different fields are developed through the distance between the graphene layers, the rotation angle or the stacking contact area, or the material of the electrode, the lead and the substrate is changed.
The graphene with at least two layers or more layers is used as a sensitive element. The thickness of graphene ranges from two layers to multiple layers, with the size (certain dimension) of the area-superposed region being on the order of nanometers to centimeters. The bi-layer or multi-layer graphene can be stacked to form various structures through various rotation angles of the two-layer graphene.
The graphene material of the temperature sensitive element comprises three to five layers of graphene and the like. Each layer of graphene is connected with a metal electrode, and the electrode material can be selected from various metal materials with good conductivity, such as titanium, gold, chromium, silver or copper. Two layers of graphene with overlapped areas are selected to be connected with the electrodes.
The electrode used in the present invention is formed by electron beam lithography or photolithography on one end of each of two graphene layers, and a desired metal electrode is formed by electron beam evaporation or thermal evaporation. The electrode material can be selected from various metal materials with good electric conductivity, such as titanium, gold, chromium and the like.
According to the preparation method, the graphene is used as a raw material, and the preparation method is suitable for growing graphene materials obtained by various ways such as graphene prepared by a chemical vapor deposition method, graphene prepared by a silicon carbide epitaxial method, stripped graphene and the like on the surface of a substrate.
The substrate used may comprise SiO with different thickness2Si substrate of the layer, polymer materials, including flexible polymer materials such as polyimide, PET, PI, and the like.
The temperature sensor based on the double-layer graphene can adjust the distance, the rotation angle, the contact area and the like between graphene layers when the double-layer graphene is manufactured. The interlayer spacing of the graphene can be controlled by the annealing temperature, and the higher the annealing temperature is, the smaller the interlayer spacing is. The annealing temperature is 100-800 ℃, in particular to annealing under high vacuum.
Parameters such as the interlayer spacing, the rotation angle and the contact area directly influence the resistance of the graphene. The sensitive element material graphene is not limited to a double layer, and can be expanded to a few layers of graphene. The size of the graphene can be regulated, so that the temperature sensor is arbitrary in shape and size.
Has the advantages that:
1) according to the invention, the interlayer coupling effect of the overlapping region of the double-layer or multi-layer graphene is utilized to realize temperature sensing, and the adjustment and control of the interlayer spacing can be realized by adjusting the annealing condition of the stacked graphene, so that the sensitivity and the use temperature range of the graphene sensor are adjusted.
2) According to the invention, temperature sensing is realized through the interlayer coupling effect of graphene, the sensitivity and stability of the sensor are effectively improved, and the sensor is very favorable for being applied to the fields of aerospace, intelligent weapons, intelligent buildings, health monitoring and the like.
3) The preparation method is a universal method and is suitable for graphene prepared by a chemical vapor deposition method and graphene prepared by a silicon carbide epitaxial method or stripped graphene; the invention also includes bi-layer and few-layer graphene, and the like.
4) The whole process related by the invention is very simple and convenient, is suitable for graphene samples with any size and shape, and is beneficial to future large-scale application. The temperature application range can reach below 600 ℃.
In summary, the present invention utilizes the coupling effect between graphene layers to realize the temperature sensing function. Compared with the traditional method using graphene oxide, carbon black and the like as sensitive elements, the stability and the sensitivity of the temperature sensor are greatly improved by utilizing the interlayer coupling effect. The whole process is simple and convenient to operate, and is expected to be applied to the fields of aerospace, intelligent weapons, intelligent buildings, electronic skin health monitoring and the like.
Graphene is not limited to only bi-layers, but can be extended to a few layers of graphene as a sensitive element. The sensor is effective in improving the thermal conductivity and sensitivity of the sensor.
Description of the drawings:
fig. 1 is a schematic top view of a graphene temperature sensor. Reference numerals: the sensor comprises a sensitive element graphene 1, an electrode 2, a lead 3, a substrate 4 and a lead through hole 5.
FIG. 2 is a side view of a bi-layer graphene stack. The interlayer coupling effect and the interlayer spacing d can be regulated and controlled by the annealing condition of the graphene sensitive element.
FIG. 3 is a top view of a three-layer graphene stack. Different interlayer coupling distances are realized by adjusting and controlling the three layers through adjusting annealing conditions. Reference numerals: A. b and C represent three layers of graphene on the substrate.
The specific implementation mode is as follows:
as shown in the figure: the invention provides a novel temperature sensor based on double-layer or few-layer graphene. The graphene is taken as a sensitive element, and the structure of the graphene comprises graphene 1, an electrode 2, a lead 3, a substrate 4 and a lead through hole 5. The lead connecting electrode penetrates through the lead through hole 5 to be externally connected, and the graphene can be graphene prepared by a chemical vapor deposition method, graphene prepared by a silicon carbide epitaxial method and stripped graphene.
The method comprises the following specific steps: the double-layer graphene is placed on a substrate, an electrode two-needle method or a four-needle method is manufactured at one end of each of the double-layer graphene by using an electron beam lithography technology or a lithography technology, and a desired metal electrode is subjected to electron beam evaporation or thermal evaporation.
According to the invention, graphene is adopted as a raw material, and the quality and size of the graphene can be effectively regulated and controlled by changing a graphene preparation method, the graphene prepared by a chemical vapor deposition method, the graphene prepared by a silicon carbide epitaxial method or the stripped graphene.
The substrate used in the present invention includes SiO with different thickness2The Si substrate of the layer, a polymer material, the polymer material mainly comprising a flexible polymer material, including polyimide, PET, PU, PI, and the like. Or may be a non-flexible polymeric material.
When double-layer or few-layer graphene is manufactured, the coupling effect atomic layer spacing between graphene layers can be regulated and controlled by regulating annealing conditions, and the stacking rotation angle, the contact area and the like can be regulated and controlled. Wherein the annealing condition of the graphene is as follows: the annealing temperature is 100-800 ℃, the pressure is 1E-5 Pa-1E-1 Pa, and the treatment time is 1-60 minutes. The thickness of the graphene can range from two to more layers, and the area of the overlapping can range from nanometer to centimeter.
Example 1
Graphene prepared by using a chemical vapor deposition method is used as a sensitive element of a temperature sensor, the rotation angle of two stacked layers of graphene is 90 degrees, the two stacked layers of graphene are annealed at 600 ℃ under high vacuum, and the temperature sensor is manufactured according to the structure shown in the attached figure 1. When external temperature acts on the double-layer graphene, the interlayer spacing of the double-layer graphene is changed, so that the conductivity and resistivity between the graphene layers are changed, and the change of the sensed environmental temperature is reflected by detecting the magnitude of current flowing between two electrodes of the graphene. The obtained temperature sensor has extremely high electric signal response stability at the temperature of 600 ℃ in the temperature test, and can be used for the temperature test at the test temperature of less than 600 ℃. Wherein the relationship between the relative resistance and the temperature is linear in the range of-273 deg.C to 600 deg.C (0K to 873K), i.e., Δ R ═ a.T + b, where R is the resistance, a, b are constants, and T is the temperature (in K).
Example 2
The difference from the embodiment 1 is that: graphene prepared by using a chemical vapor deposition method is used as a sensitive element of a temperature sensor, three layers of stacked graphene are shown in figure 3, the three layers of stacked graphene are annealed at 600 ℃ under high vacuum, and the temperature sensor is manufactured according to the structure shown in figure 1. When external temperature acts on three layers of graphene, the interlayer spacing of the graphene is changed, so that the conductivity and resistivity between the graphene layers are changed, and the change of the sensed environmental temperature is reflected by detecting the magnitude of current flowing between two electrodes of the graphene. The obtained temperature sensor has extremely high electric signal response stability at the temperature of 600 ℃ in the temperature test, and can be used for the temperature test at the test temperature of less than 600 ℃.
Example 3
The difference from the embodiment 1 is that: graphene prepared by a silicon carbide epitaxial method is used as a sensitive element of a temperature sensor, the rotation angle of two stacked graphene layers is 90 degrees, the two stacked graphene layers are annealed at 600 ℃ under high vacuum, and the temperature sensor is manufactured according to the structure shown in the attached figure 1. When external temperature acts on the double-layer graphene, the interlayer spacing of the double-layer graphene is changed, so that the conductivity and resistivity between the graphene layers are changed, and the change of the sensed environmental temperature is reflected by detecting the magnitude of current flowing between two electrodes of the graphene. The obtained temperature sensor has extremely high electric signal response stability at the temperature of 600 ℃ in the temperature test, and can be used for the temperature test at the test temperature of less than 600 ℃.
Example 4
The difference from the embodiment 1 is that:
graphene prepared by mechanical stripping is used as a sensitive element of a temperature sensor, the rotation angle of two stacked layers of graphene is 90 degrees, the two stacked layers of graphene are annealed at 600 ℃ under high vacuum, and the temperature sensor is manufactured according to the structure shown in the attached figure 1. When external temperature acts on the double-layer graphene, the interlayer spacing of the double-layer graphene is changed, so that the conductivity and resistivity between the graphene layers are changed, and the change of the sensed environmental temperature is reflected by detecting the magnitude of current flowing between two electrodes of the graphene. The obtained temperature sensor has extremely high electric signal response stability at the temperature of 600 ℃ in the temperature test, and can be used for the temperature test at the test temperature of less than 600 ℃.
Example 5
The difference from the embodiment 1 is that: graphene prepared by using a chemical vapor deposition method is used as a sensitive element of a temperature sensor, the rotation angle of the stacked two-layer graphene is 10 degrees, the stacked two-layer graphene is annealed at 600 ℃ under high vacuum, and the temperature sensor is manufactured according to the structure shown in the attached figure 1. When external temperature acts on the double-layer graphene, the interlayer spacing of the double-layer graphene is changed, so that the conductivity and resistivity between the graphene layers are changed, and the change of the sensed environmental temperature is reflected by detecting the magnitude of current flowing between two electrodes of the graphene. The obtained temperature sensor has extremely high electric signal response stability at the temperature of 600 ℃, so that the temperature sensor can be used for testing the temperature of which the testing temperature is lower than 600 ℃, and has anti-interference capability of different degrees.
Example 6
The difference from the embodiment 1 is that: graphene prepared by using a chemical vapor deposition method is used as a sensitive element of a temperature sensor, the rotation angle of two stacked layers of graphene is 90 degrees, the two stacked layers of graphene are annealed at 400 ℃ under high vacuum, and the temperature sensor is manufactured according to the structure shown in the attached figure 1. When external temperature acts on the double-layer graphene, the interlayer spacing of the double-layer graphene is changed, so that the conductivity and resistivity between the graphene layers are changed, and the change of the sensed environmental temperature is reflected by detecting the magnitude of current flowing between two electrodes of the graphene. The obtained temperature sensor has extremely high electric signal response stability at 400 ℃ in temperature test, so that the temperature sensor can be used for temperature test at the test temperature of lower than 400 ℃ and has higher detection sensitivity.
Example 7
The difference from the embodiment 2 is that: graphene prepared by a chemical vapor deposition method is used as a sensitive element of a temperature sensor, and two layers of graphene stacked together and close to a substrate are annealed at 800 ℃ under high vacuum. And then, stacking a third layer of graphene on the substrate, annealing the obtained three layers of graphene at 200 ℃ under high vacuum as shown in the attached figure 3, and regulating and controlling the coupling effect among the three layers to realize different interlayer distances.
While the invention has been described with reference to the preferred embodiments, it is not intended to be limited thereto. Those skilled in the art to which the invention pertains will appreciate that various changes, substitutions and alterations can be made herein without departing from the spirit and scope of the invention. Therefore, the protection scope of the present invention should be determined by the appended claims.
Claims (9)
1. A temperature sensor based on double-layer graphene is characterized by comprising at least double-layer graphene, a pair of metal electrodes and a substrate; double-layer graphene grows or is arranged on the substrate, the double-layer graphene has an overlapping area, namely a stacking area, and the double-layer graphene is respectively connected with a pair of electrodes.
2. The dual-layer graphene-based temperature sensor of claim 1, wherein the temperature sensitive element graphene material comprises three to five layers of graphene.
3. The double-layer graphene-based temperature sensor according to claim 1 or 2, wherein each layer of graphene is connected with a metal electrode; temperature sensors suitable for different purposes are developed through the spacing between graphene layers, the rotation angle or the overlapping contact area, or changing the materials of electrodes, leads and substrates.
4. The double-layer graphene-based temperature sensor according to claim 1 or 2, wherein the substrate used comprises SiO with different thicknesses2A Si substrate of a layer, a polymer material including polyimide, PET and PI.
5. A method for preparing the temperature sensor based on the double-layer graphene according to any one of claims 1 to 4, wherein an electrode is used, an electrode is manufactured at one end of each of the two layers of graphene by using an electron beam lithography technique or a photolithography technique, and a desired metal electrode is evaporated by using an electron beam or heat; the method is suitable for growing or placing graphene materials obtained by various ways of preparing graphene by a chemical vapor deposition method, preparing graphene by a silicon carbide epitaxial method and stripping the graphene on the surface of a substrate.
6. The method for preparing the temperature sensor based on the double-layer graphene according to claim 5, wherein when the temperature sensor based on the double-layer graphene is used for preparing the double-layer graphene, the spacing, the rotation angle, the contact area and the like between graphene layers are adjusted; the interlayer spacing of the graphene is controlled by annealing temperature, and the higher the annealing temperature is, the smaller the interlayer spacing is; the annealing temperature is 100-800 ℃.
7. The method of claim 6, wherein annealing is performed under high vacuum.
8. The method of claim 5 or 6, wherein the parameters of the interlayer distance, the rotation angle and the contact area directly influence the resistance of the graphene.
9. The method of claim 5 or 6, wherein the thickness of the graphene ranges from two to more layers, and the size of the overlapped area ranges from nanometer to centimeter.
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| US8198976B2 (en) * | 2006-08-18 | 2012-06-12 | The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration | Flexible thin metal film thermal sensing system |
| CN103630254A (en) * | 2013-11-18 | 2014-03-12 | 西安电子科技大学 | Graphene temperature sensor and preparing process thereof |
| CN105222920A (en) * | 2015-10-08 | 2016-01-06 | 中国电子科技集团公司第五十五研究所 | CVD graphene temperature sensor, sensor-based system and temperature sensor preparation method |
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Application publication date: 20200107 |