CN111624240B - Sensing/transduction coupling self-driven gas sensor and preparation method thereof - Google Patents
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Abstract
The invention relates to a sensing/transduction coupling self-driven gas sensor and a preparation method thereof. The invention integrates the gas sensitive material and the piezoelectric transduction material together, fully integrates the characteristics of room temperature gas detection, flexibility and piezoelectric ceramic high-voltage electricity response of the dielectric gas sensitive polymer, utilizes external force excitation to promote gas sensitivity and transduction cross coupling and 'passive' conversion into detection electric signals, realizes gas sensitivity/transduction coupling self-driven gas detection, and solves the problem that the 'gas sensitivity' and 'transduction' processes of most of the current gas sensors are independent and split. The invention provides the gas-sensitive and energy-converting simultaneous same-ground cross coupling, realizes the synergy, has the characteristics of zero power consumption, high sensitivity, flexibility, convenience for integration and the like, can be used for self-driven environment monitoring and human body physiological monitoring, and does not need to be provided with a power supply.
Description
Technical Field
The invention relates to the technical field of energy collection, micro-electro-mechanical systems (MEMS) and electronic polymer sensitive materials, in particular to a sensing/transduction coupling self-driven gas sensor and a preparation method thereof.
Background
With the development of modern industry, people enjoy more and more convenience and suffer more and more serious environmental pollution hazards. According to the release of World Health Organization (WHO) surveys, nearly ten million people die each year due to environmental pollution or premature death. The source of harmful gas in the air is wide, and the harmful gas is generated in the combustion of coal, petroleum, natural gas and the like, industrial production processes, tail gas discharged by vehicles in transportation processes, underground mining and tunneling construction processes and the like. Volatile organic pollutant gases (formaldehyde, benzene and benzene compounds, methanol, acetone and the like) can be encountered everywhere in life, and are harmful to human health all the time, and once diseases are caused, the situation that the pollutants cannot be reversed and cannot be recovered is achieved.
Secondly, along with the rapid development of world economy, the demand of human society for energy supply is getting larger and larger, and the nonrenewable traditional energy supply modes such as coal, petroleum, natural gas, nuclear energy and the like cannot meet the development demand of the times due to the serious pollution to the environment, so that the research of clean and renewable new energy is a problem which needs to be solved urgently at present. New energy resources, such as mechanical energy, heat energy, solar energy and the like, which are recycled and regenerated are gradually recognized, developed and utilized by people in the past decades, and the new energy technology is utilized to provide effective measures for environmental management and ecological protection, so that the new energy resource technology is an important solution for overcoming global energy shortage and meeting sustainable development of human society.
The mechanical energy in the environment is one of the most ideal alternative energy sources due to the advantages of wide distribution, various expression forms, easy conversion and the like. If the mechanical energy in the environment can be collected and stored by using an effective means and converted into electric energy, the electric energy can be used for supplying power and continuing the journey for the operation of microelectronic devices such as implantable medical equipment, a sensing system, a wearable electronic device, portable equipment and the like, so that the limitation of the problems of large size, short service life, poor safety and the like caused by the conventional battery power supply is broken through.
Disclosure of Invention
The invention aims to: the device embeds piezoelectric transduction materials into polymer gas-sensitive materials, excites cross coupling of gas sensitivity and transduction through external force and converts the cross coupling into detection electric signals passively so as to realize real-time spontaneous active detection on gas types and concentrations.
The technical scheme adopted by the invention is as follows:
a perception/transduction coupling self-driven gas sensor structurally comprises a flexible substrate, flexible interdigital electrodes and a piezoelectric ceramic-gas-sensitive polymer composite film, wherein the flexible interdigital electrodes are arranged on the flexible substrate, piezoelectric ceramic particles are compounded with a dielectric polymer gas-sensitive material and are deposited on the flexible interdigital electrodes; a gas sensitive interface is arranged above the composite film, and a transduction interface is arranged below the composite film and the interface of the flexible interdigital electrode; the flexible interdigital electrode is led out through a lead for detecting an electric signal output by the sensor. The gas sensitive material and the piezoelectric transduction material are integrated together, and external force excitation is utilized to promote gas sensitivity and transduction cross coupling and passive conversion into detection electric signals, so that gas sensitivity/transduction coupling self-driven gas detection is realized.
The working principle of the device is that the gas reaction is utilized to change the dielectric constant of the gas-sensitive polymer, so that the electric field intensity distributed by two phases of the composite material is changed, the electric field intensity distributed on the piezoelectric ceramic is changed, and the external specific gas reaction is modulated to a piezoelectric output signal, so that the concentration of the external atmosphere can be reversely deduced through the size of the piezoelectric output, and the self-powered gas detection is realized.
Further, the stress applied on the composite film is extrusion, stretching or bending.
Furthermore, the volume fraction of the doping amount of the piezoelectric ceramic particles and the piezoelectric ceramic in the dielectric polymer gas-sensitive material composite material is 10-60%, and the thickness of the composite material film is 10-500 nm.
Further, the dielectric polymer gas-sensitive material is a composite film composed of any one or more of polyaniline, polyethylene oxide, polyethylene imine, sodium polystyrene sulfonate, polyaniline, polyimide, chitosan and graphene oxide.
Further, the piezoelectric ceramic particles are made of any one of barium titanate piezoelectric ceramics, lead zirconate titanate piezoelectric ceramics, niobate piezoelectric ceramics, potassium sodium niobate, and lead magnesium niobate piezoelectric ceramics.
Further, the flexible substrate includes polyimide, polytetrafluoroethylene, polyvinyl fluoride, and the like.
Further, depositing the interdigital electrode on the flexible substrate by adopting an evaporation or sputtering method, wherein the thickness of the interdigital electrode is about 10-50 μm; the gas-sensitive material is deposited on the interdigital electrode by adopting any one of electrostatic spinning, tape casting, spin coating, spraying, drop coating, sol-gel, self-assembly and chemical vapor deposition and combining a stripping process to form a gas-sensitive structure.
In order to achieve the above object, the present invention further provides a method for manufacturing a sensing/transduction coupling self-driven gas sensor, which specifically comprises the following steps:
(1) cleaning and drying the flexible substrate by using a chemical reagent;
(2) depositing an interdigital electrode on a flexible substrate by adopting a sputtering or evaporation process;
(3) mixing a piezoceramic material and a gas-sensitive material for standby;
(4) depositing the piezoelectric ceramic-gas-sensitive mixed material on the interdigital electrodes by adopting any one of electrostatic spinning, tape casting, spin coating, spraying, drop coating, sol-gel, self-assembly and chemical vapor deposition and combining a stripping process to form a gas-sensitive structure;
(5) and (5) polarizing the gas-sensitive composite material.
Furthermore, the polarization process acts on the interdigital electrode, and the polarization process parameters of the gas-sensitive composite material are that the field intensity of a polarization electric field is 0.1 kv/mm-100 kv/mm, the polarization temperature is 20 ℃ -200 ℃, and the polarization time is 60 min-600 min.
In summary, compared with the prior art, the invention has the following beneficial effects:
the traditional gas sensor is independent and split in gas sensitivity and energy conversion, so that the integration is inconvenient and the power consumption is reduced; the invention provides a perception/transduction coupling self-driven gas sensor and a preparation method thereof, the device embeds piezoelectric transduction material into polymer gas sensitive material, and excites the cross coupling of gas sensitivity and transduction through external force and converts the cross coupling into detection electric signal passively so as to realize the real-time spontaneous active detection of gas type and concentration; the invention provides a self-powered gas sensor sensitivity mechanism and a self-powered gas sensor sensitivity model based on a piezoelectric ceramic-dielectric gas-sensitive polymer, and provides a sensing/transduction coupling self-driven gas-sensitive structure which can independently work without external power supply; the advantages of piezoelectric ceramic high-voltage output response and room-temperature gas detection and flexibility of the gas-sensitive polymer material are fully combined, and flexible self-driven environmental atmosphere/human body exhaled gas monitoring can be realized.
Drawings
FIG. 1 is a schematic diagram of a self-driven gas sensor with sensing/transducing coupling according to the present invention;
fig. 2 is a diagram of a power generation mechanism of a sensing/transducing coupling self-driven gas sensor according to the present invention.
The reference signs are: 1-flexible substrate, 2-flexible interdigital electrode, 3-dielectric polymer gas sensitive material and 4-piezoelectric ceramic particles.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the detailed description and specific examples, while indicating the preferred embodiment of the invention, are intended for purposes of illustration only and are not intended to limit the scope of the invention.
Thus, the following detailed description of the embodiments of the present invention, presented in the figures, is not intended to limit the scope of the invention, as claimed, but is merely representative of selected embodiments of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments of the present invention without making any creative effort, shall fall within the protection scope of the present invention.
The invention will be further described with reference to the accompanying figures 1-2 and examples.
Example (b):
as shown in fig. 1, a self-powered gas sensor with sensing/transduction coupling structurally comprises a flexible substrate, flexible interdigital electrodes and a piezoelectric ceramic-gas-sensitive polymer composite film, wherein the flexible interdigital electrodes are arranged on the flexible substrate, and piezoelectric ceramic particles are compounded with a dielectric polymer gas-sensitive material and deposited on the flexible interdigital electrodes; a gas sensitive interface is arranged above the composite film, and a transduction interface is arranged below the composite film and the interface of the flexible interdigital electrode; the flexible interdigital electrode is led out through a lead for detecting an electric signal output by the sensor. The gas-sensitive material and the piezoelectric transduction material are integrated together, and external force is utilized to excite the gas-sensitive material and the transduction material to be cross-coupled and passively converted into detection electric signals, so that the gas-sensitive/transduction coupling self-driven gas detection is realized.
The power generation mechanism of the gas sensor is shown in fig. 2. The electric domains are randomly distributed within the ceramic prior to poling and tend to align in the direction of the applied electric field when subjected to a strong electric field, in which case the device does not output an electrical signal due to internal electrical balance if no external force is applied to the sensor. When the device is stretched, the distance between the two interdigitated electrodes changes and the total polarization of the composite material between the two electrodes will change accordingly, resulting in a voltage potential between the two electrodes. The free charge will then flow through an external circuit, moving and accumulating at the electrode surface to keep the potential balanced. Thus, an electrical signal is generated due to the movement of electrons in the external circuit. When the external force is released, the distance between the interdigital electrodes returns to the initial state, and thus the piezoelectric potential disappears. In this case, the accumulated charges flow back in the opposite direction, thereby generating an opposite electric signal. Thus, a periodic alternating electrical signal is obtained during the continuous application and release of external forces on the device.
The gas-sensitive mechanism of the gas sensor is as follows: for the oxidizing gas, along with the increase of the gas concentration, the hole concentration in the gas-sensitive composite material is increased, and the dielectric constant of the P-type polymer is increased, so that an electric field can be more distributed on the piezoelectric ceramic, the piezoelectric coefficient of the composite film is correspondingly increased, and the output signal is further increased; for reducing gas, along with the increase of the gas concentration, the hole concentration in the gas-sensitive composite material is reduced, so that an electric field is less distributed on the piezoelectric ceramic, the piezoelectric coefficient of the composite film is correspondingly reduced, the output signal is further reduced, and the self-driven detection of the type and the concentration of the gas to be detected is realized.
When the device structure is in dry air, oxygen molecules adsorb and abstract free electrons in the sensitive film to form oxygen ions (formula 1):
O2+2e-→2O-(1)
when an oxidizing gas is introduced, with NO2For example. NO2The free electrons (formula 2) of the sensitive film are captured, the hole concentration of the gas sensitive film is increased, the dielectric constant of the P-type polymer is increased, the piezoelectric coefficient of the composite film is increased, and therefore the output current is increased. With introduction of NO2The concentration is increased, the hole concentration of the gas-sensitive film is further increased, so that the dielectric constant of the polymer and the piezoelectric coefficient of the composite film are further increased, and the output current is further increased:
NO2+e-＝NO2 -(2)
while introducing reducing gas, with NH3For example. NH (NH)3The hole concentration of the gas-sensitive film is reduced (formula 3), so that the dielectric constant of the polymer is reduced, the piezoelectric coefficient of the composite film is reduced, and the output current is reduced. With the introduction of NH3The concentration is increased, and the hole concentration of the gas-sensitive film is further reduced, so that the dielectric constant of the polymer and the composite film are causedFurther reducing the output current:
2NH3+5O-→2NO+3H2O+5e-(3)
therefore, the real-time self-powered detection of the type and the concentration of the gas to be detected can be realized by detecting the output signal.
The above-mentioned embodiments only express the specific embodiments of the present application, and the description thereof is more specific and detailed, but not construed as limiting the scope of the present application. It should be noted that, for those skilled in the art, without departing from the technical idea of the present application, several changes and modifications can be made, which are all within the protection scope of the present application.
Claims (10)
1. A perception/transduction coupling self-driven gas sensor is characterized in that the self-driven gas sensor structurally comprises a flexible substrate, flexible interdigital electrodes and a piezoelectric ceramic-gas-sensitive polymer composite film, wherein the flexible interdigital electrodes are arranged on the flexible substrate, and piezoelectric ceramic particles are compounded with a dielectric polymer gas-sensitive material and deposited on the flexible interdigital electrodes; a gas sensitive interface is arranged above the composite film, and a transduction interface is arranged below the composite film and the interface of the flexible interdigital electrode; the flexible interdigital electrode is led out through a lead for detecting an electric signal output by the sensor.
2. The sensor of claim 1, wherein the gas sensitive material and the piezoelectric transducer material are integrated, and external force is used to excite the cross coupling between gas sensing and transducer and transform the cross coupling into detection electrical signal, so as to realize gas sensing/transducer coupling self-driven gas detection.
3. The sensor of claim 2, wherein the stress applied to the composite membrane is compressive, tensile or bending.
4. The sensor/transducer coupled self-driven gas sensor as claimed in claim 1, wherein the volume fraction of the doping amount of the piezoelectric ceramic particles and the piezoelectric ceramic in the dielectric polymer gas-sensitive material composite material is 10-60%, and the thickness of the composite material film is 10-500 nm.
5. The sensor/transducer coupled self-driven gas sensor as claimed in claim 1, wherein the dielectric polymer gas-sensitive material is composed of one or more of polyaniline, polyethylene oxide, polyethylene imine, sodium polystyrene sulfonate, polyimide, chitosan and graphene oxide.
6. The sensor/transducer coupled self-driven gas sensor according to claim 1, wherein the piezoelectric ceramic particles are made of any one of barium titanate piezoelectric ceramic, lead zirconate titanate piezoelectric ceramic, niobate piezoelectric ceramic, potassium sodium niobate, and lead magnesium niobate piezoelectric ceramic.
7. The sensor-transducer coupled self-driven gas sensor of claim 1, wherein the flexible substrate is made of a material comprising any one or more of polyimide, polytetrafluoroethylene, polyvinyl fluoride, polyethylene terephthalate, polyethylene, polypropylene, polystyrene, and polyethylene naphthalate.
8. The sensor/transduction coupling self-driven gas sensor according to claim 1, wherein the interdigital electrodes are deposited on the flexible substrate by evaporation or sputtering, and the thickness of the interdigital electrodes is about 10-50 μm; the gas-sensitive material is deposited on the interdigital electrode by adopting any one of electrostatic spinning, tape casting, spin coating, spraying, drop coating, sol-gel, self-assembly and chemical vapor deposition and combining a stripping process to form a gas-sensitive structure.
9. The method for preparing the sensing/transducing coupling self-driven gas sensor according to any one of claims 1 to 8, comprising the following steps:
(1) cleaning and drying the flexible substrate by using a chemical reagent;
(2) depositing an interdigital electrode on a flexible substrate by adopting a sputtering or evaporation process;
(3) mixing a piezoceramic material and a gas-sensitive material for standby;
(4) depositing the piezoelectric ceramic-gas-sensitive mixed material on the interdigital electrodes by adopting any one of electrostatic spinning, tape casting, spin coating, spraying, drop coating, sol-gel, self-assembly and chemical vapor deposition and combining a stripping process to form a gas-sensitive structure;
(5) and (5) polarizing the gas-sensitive composite material.
10. The method for preparing a sensor/transducer coupled self-driven gas sensor according to claim 9, wherein a polarization process is performed on the interdigital electrode, and the parameters of the polarization process of the gas-sensitive composite material are that the field strength of a polarization electric field is 0.1 kV/mm-100 kV/mm, the polarization temperature is 20 ℃ to 200 ℃, and the polarization time is 60min to 600 min.
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| CN113008124B (en) * | 2021-02-20 | 2023-10-17 | 宁波诺丁汉新材料研究院有限公司 | Multimode sensor and preparation method thereof |
| CN113834862B (en) * | 2021-09-17 | 2023-05-30 | 电子科技大学 | Method for regulating/enhancing sensitivity of self-driven flexible gas sensor by interface stress |
| CN114034744B (en) * | 2021-11-05 | 2023-03-17 | 电子科技大学 | High-performance self-driven humidity sensor and preparation method thereof |
| CN114235950A (en) * | 2021-11-19 | 2022-03-25 | 华南理工大学 | Method for reducing working temperature of semiconductor sensitive film in surface acoustic wave gas sensor |
| CN114323407B (en) * | 2021-12-28 | 2022-09-09 | 电子科技大学 | Flexible film type self-driven multifunctional sensor and preparation method thereof |
| CN114858316B (en) * | 2022-04-27 | 2023-09-01 | 电子科技大学 | Dynamic and static whole-course sensitive human-computer interface sensor and preparation method thereof |
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