CN111682796B - Flexible piezoelectric energy collector based on negative poisson ratio macroscopic graphene film - Google Patents
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- H—ELECTRICITY
- H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
- H02N—ELECTRIC MACHINES NOT OTHERWISE PROVIDED FOR
- H02N2/00—Electric machines in general using piezoelectric effect, electrostriction or magnetostriction
- H02N2/18—Electric machines in general using piezoelectric effect, electrostriction or magnetostriction producing electrical output from mechanical input, e.g. generators
- H02N2/186—Vibration harvesters
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/184—Preparation
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/198—Graphene oxide
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- H—ELECTRICITY
- H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
- H02N—ELECTRIC MACHINES NOT OTHERWISE PROVIDED FOR
- H02N2/00—Electric machines in general using piezoelectric effect, electrostriction or magnetostriction
- H02N2/22—Methods relating to manufacturing, e.g. assembling, calibration
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2204/00—Structure or properties of graphene
- C01B2204/20—Graphene characterized by its properties
- C01B2204/22—Electronic properties
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2204/00—Structure or properties of graphene
- C01B2204/20—Graphene characterized by its properties
- C01B2204/26—Mechanical properties
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2204/00—Structure or properties of graphene
- C01B2204/20—Graphene characterized by its properties
- C01B2204/32—Size or surface area
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- Nanotechnology (AREA)
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Abstract
The invention relates to a flexible piezoelectric energy collector based on a macroscopic graphene film with negative poisson ratio, which comprises a flexible substrate and a laminated structure piezoelectric power generation unit fixed on the surface of the flexible substrate, wherein a wire is arranged on the surface of the laminated structure piezoelectric power generation unit and used for leading out charges/voltages generated after the flexible piezoelectric energy collector is subjected to tensile deformation, and the laminated structure piezoelectric power generation unit comprises the macroscopic graphene film with negative poisson ratio and the flexible piezoelectric film. According to the invention, the flexible and high-conductivity macroscopic graphene film with the negative poisson ratio effect is utilized, the negative poisson ratio effect is introduced into the flexible piezoelectric energy collector, and the tensile deformation of the piezoelectric film is changed from original unidirectional stretching to stretching in two vertical directions in the plane when the device works by means of strain coupling between the piezoelectric film in the piezoelectric power generation unit with the negative poisson ratio macroscopic graphene film, so that the electric output performance of the device is improved.
Description
Technical Field
The invention relates to the technical field of environmental energy collection, in particular to a flexible piezoelectric energy collector based on a negative poisson ratio macroscopic graphene film.
Background
In recent years, with the development of electronic information technology and the progress of human society, wearable electronics have exhibited a wide market prospect. At the same time, the energy crisis and environmental pollution problems caused by the transitional consumption of fossil fuels have prompted the search for new renewable energy sources to power these electronics. In the wearable device, mechanical energy related to human body movement, such as bending of joints of fingers, elbows and the like, stepping of feet during walking, beating of hearts or pulses, expansion of chest during breathing and the like, are collected and utilized, so that the wearable intelligent electronic device can be conveniently powered. The piezoelectric energy collector can realize conversion from mechanical energy to electric energy based on the piezoelectric effect principle of materials. Compared with other forms of environmental mechanical energy collection technologies, such as electrostatic, electromagnetic induction, triboelectric and the like, the piezoelectric energy collection device has the advantages of simple and compact structure, high energy conversion efficiency, good electric energy output stability, easiness in flexibility, easiness in integration with electronic devices and the like, and has good development and application potential.
In order to meet the requirements of flexible piezoelectric energy harvesting applications, piezoelectric materials should not only have excellent piezoelectric properties, but must also be flexible. For this reason, various flexible piezoelectric materials have been developed successively, and there are mainly piezoelectric nanomaterials, inorganic piezoelectric thin films, piezoelectric polymers, piezoelectric composite materials, and the like. In fact, development of various flexible piezoelectric materials and performance optimization thereof are always important in development of flexible piezoelectric energy collectors. Nevertheless, the electrical output performance of most flexible piezoelectric energy harvesting devices is still low at present, and the energy consumption requirements of most electronic devices cannot be met. One of the reasons for this is that the mechanical structure of the device is not yet optimal and the performance of the piezoelectric material is not fully utilized. Besides the optimization of the performance of the piezoelectric material, the optimization of the mechanical structure of the device is also an effective way for improving the electrical output performance of the flexible piezoelectric energy collection device. Therefore, to develop high performance piezoelectric energy harvesting devices, optimization of piezoelectric material performance should be combined with optimization of device mechanics.
Poisson's ratio is a fundamental mechanical property parameter of a material. Materials with negative poisson's ratio exhibit an "auxetic effect", i.e. the material expands laterally when uniaxially stretched. The performance of the piezoelectric device can be improved by reasonably utilizing the negative poisson's ratio effect of the material. Li et al [ AIP adv.,2017, 015104] and Ferguson et al [ Sens. Materialers A,2018,282,90-96] are based on finite element calculations and experiments, respectively, which prove that the adoption of a stainless steel substrate with a negative Poisson ratio structure can significantly improve the electric output power of a rigid vibration dynamic energy collecting device. However, such rigid vibrating piezoelectric energy collectors have insufficient flexibility and are difficult to apply in wearable devices; the negative poisson's ratio effect is introduced by the structural design of the stainless steel substrate, again limiting the flexibility of the device. Therefore, finding an effective way to introduce the negative poisson's ratio effect into a flexible piezoelectric energy collector would be of great significance in the development of high performance flexible piezoelectric energy collectors, as well as in facilitating their use in wearable electronics.
Disclosure of Invention
The invention aims to overcome the defects of the prior art, and aims to provide a flexible piezoelectric energy collector based on a macroscopic graphene film with negative poisson ratio.
The technical scheme for solving the technical problems is as follows:
the flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film comprises a flexible substrate and a laminated structure piezoelectric power generation unit fixed on the surface of the flexible substrate, wherein a wire is arranged on the surface of the laminated structure piezoelectric power generation unit and used for leading out charges/voltages generated after the flexible piezoelectric energy collector is subjected to tensile deformation, and the laminated structure piezoelectric power generation unit comprises the negative poisson ratio macroscopic graphene film and the flexible piezoelectric film.
Further, in the piezoelectric power generation unit with the laminated structure, the negative poisson ratio macroscopic graphene film is fixed on the upper side and the lower side of the flexible piezoelectric film.
Further, the preparation method of the negative poisson ratio macroscopic graphene film comprises the following steps:
Step 1, preparing graphene oxide by adopting an improved oxidation method or an electrochemical stripping method;
Step 2, dispersing graphene oxide with ultrapure water to form graphene oxide dispersion liquid with the solid content of 2-4%, and preparing the graphene oxide dispersion liquid into a graphene oxide film by adopting a tape casting method;
And step 3, placing the graphene oxide film obtained in the step2 in a high-temperature graphitization furnace, and performing high-temperature treatment at 2000-3000 ℃ under the protection of inert atmosphere to obtain the negative poisson ratio macroscopic graphene film.
Further, the film thickness of the negative poisson ratio macroscopic graphene is 5-200 mu m, the poisson ratio is-0.5-0, the Young modulus is 0.01-20GPa, and the conductivity is not lower than 10 4 S/m.
Further, the piezoelectric film is made of at least one of PVDF and copolymers thereof or piezoelectric composite materials, and has a thickness of 10-100 μm.
Further, the flexible substrate is made of at least one of PET, polyimide, epoxy, aluminum, copper and stainless steel, and has a thickness of 50-500 μm.
Further, the number of the laminated piezoelectric power generation units is one or more, the laminated piezoelectric power generation units are arranged on the substrate in a transverse, longitudinal or array mode, and the electric connection mode among the laminated piezoelectric power generation units is serial or parallel.
Further, when the flexible piezoelectric energy collector works, strain coupling exists between the piezoelectric film and the negative poisson ratio macroscopic graphene film in the piezoelectric power generation unit with the laminated structure, so that the piezoelectric film is stretched in two perpendicular directions in the plane of the piezoelectric film.
The beneficial effects of the invention are as follows: according to the invention, the flexible and high-conductivity macroscopic graphene film with the negative poisson ratio effect is utilized, the negative poisson ratio effect is introduced into the flexible piezoelectric energy collector, and the tensile deformation of the piezoelectric film is changed from original unidirectional stretching to stretching in two vertical directions in the plane when the device works by means of strain coupling between the piezoelectric film in the piezoelectric power generation unit with the negative poisson ratio macroscopic graphene film, so that the electric output performance of the device is improved.
Drawings
FIG. 1 is a schematic diagram of the structure of the piezoelectric power generating unit of the present invention before and after deformation when a single laminated structure is adopted;
FIG. 2 is a photograph of a piezoelectric power generating unit of a laminated structure according to the present invention;
FIG. 3 is a photograph of a flexible piezoelectric energy harvester of the present invention;
FIG. 4 is a typical waveform of the output open circuit voltage during repeated bending of the present invention;
FIG. 5 is a typical waveform of the output short circuit current during repeated bending of the present invention;
FIG. 6 is a graph of the open circuit voltage versus short circuit current peak to peak for a flexible piezoelectric energy harvester according to the present invention and based on metallic silver;
FIG. 7 is a measurement of Poisson's ratio for a negative Poisson's ratio macroscopic graphene film in the present invention;
FIG. 8 is a cross-sectional micro-morphology of a negative poisson's ratio macroscopic graphene film according to the present invention;
FIG. 9 is a photograph of a negative Poisson's ratio macroscopic graphene film in accordance with the present invention;
Fig. 10 is a schematic diagram showing the structure of the piezoelectric power generating unit before and after the deformation of the present invention when two stacked structures are used.
The list of components represented by the various numbers in the drawings is as follows:
1. a flexible substrate; 2. a piezoelectric film; 3. negative poisson ratio macroscopic graphene film; 4. and (5) conducting wires.
Detailed Description
The principles and features of the present invention are described below with examples given for the purpose of illustration only and are not intended to limit the scope of the invention.
In the description of this patent, the terms "intermediate," "upper," "lower," "transverse," "longitudinal," and the like are merely used for convenience in describing the patent and to simplify the description, and are not to be construed as limiting the patent.
In the description of this patent, it is to be noted that the terms "bonded," "connected," "coated," "laminated," "affixed," and the like are to be construed broadly as meaning interrelated terms, unless otherwise specifically defined and limited. The specific meaning of the terms in this patent will be understood by those of ordinary skill in the art as the case may be.
As shown in fig. 1, the flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film provided by the invention comprises a flexible substrate and a piezoelectric power generation unit with a laminated structure fixed on the flexible substrate, wherein the piezoelectric power generation unit with the laminated structure is a sandwich structure formed by bonding the negative poisson ratio macroscopic graphene film on the upper side and the lower side of the flexible piezoelectric film.
The working mode of the flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film is that the flexible substrate is bent to drive the piezoelectric power generation unit with the laminated structure fixed on the flexible substrate to generate tensile deformation, and the generated voltage/current is led out from the surface of the graphene through a lead.
The flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film can be manufactured according to the following steps:
step 1, selecting a PVDF piezoelectric film 2 with the thickness of 50 mu m, wherein the PVDF piezoelectric film 2 is fully pre-polarized in advance, the piezoelectric strain constant |d 33 |=21pC/N, and electrodes used for removing polarization are cut to 3.5X1.2 cm 2;
Step 2, selecting a macroscopic graphene film 3 with a negative poisson ratio and a thickness of 200 mu m, and cutting the macroscopic graphene film to 3.0x1.0cm 2;
step 3, uniformly coating a thin layer of conductive silver adhesive on the surface to be pasted of the negative poisson ratio macroscopic graphene film 3 obtained by cutting in the step 2, respectively bonding two pieces of negative poisson ratio macroscopic graphene film 3 on two sides of the PVDF piezoelectric film 2 obtained by cutting in the step 2, and standing at room temperature to solidify the conductive silver adhesive to obtain the piezoelectric power generation unit with the laminated structure shown in the figure 2;
step 4, sticking conductive copper foil adhesive tapes on the surfaces of the upper layer and the lower layer of the negative poisson ratio macroscopic graphene film 3 of the piezoelectric power generation unit with the laminated structure obtained in the step3 to serve as leads for outputting electric signals;
Step 5, selecting a PET thin plate with the thickness of 260 mu m, cutting the PET thin plate to 10.0 multiplied by 2.0cm 2, and taking the PET thin plate as the flexible substrate 1 of the piezoelectric energy collector;
And 6, fixing the laminated structure piezoelectric power generation unit adhered with the conductive copper foil wire 4 obtained in the step 4 to the middle position of the PET flexible substrate in the step 5 in a manner of respectively fixing two ends of the laminated structure piezoelectric power generation unit to the PET flexible substrate by using epoxy resin glue to obtain the flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film shown in the figure 3.
The flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film, which is obtained according to the steps, has good flexibility and can be easily bent.
By repeatedly bending the substrate to drive the piezoelectric generating unit with the laminated structure fixed on the substrate to stretch and deform so as to generate voltage/current signal output, an electrometer is adopted to detect the voltage/current signal output generated by the device in the repeated bending process, fig. 4 is a typical open-circuit voltage signal waveform, fig. 5 is a typical short-circuit current signal waveform, and it can be seen that the electrical output of the device is continuous and stable.
The same structural design is adopted, but negative poisson ratio macroscopic graphene is replaced by metallic silver, a flexible piezoelectric energy collector based on a metal electrode is obtained as a control group, the open circuit voltage and the short circuit current of the two piezoelectric energy collectors under the same working condition are compared, statistical results of 4 samples of each group are given in fig. 6, and it can be seen that the flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film has an open circuit voltage increased by about 65% and a short circuit current increased by about 64% compared with the piezoelectric energy collector based on the metal electrode.
The negative poisson ratio macroscopic graphene film can be manufactured by the following steps:
step 1: dispersing graphene oxide with ultrapure water by taking the graphene oxide as a raw material, and magnetically stirring for 4 hours at 400rpm to form a dispersion liquid with the concentration of 3%;
step 2: introducing graphene oxide into a glass die, enabling the graphene oxide to self-level, standing at room temperature, drying and forming a film;
Step 3: and (3) placing the graphene oxide film obtained in the step (2) in a high-temperature graphitization furnace, performing high-temperature treatment under the protection of Ar atmosphere, wherein the heating rate is 10 ℃/min, the heat preservation temperature and time are 1300 ℃ for 2h, then 3000 ℃ for 1h, and cooling to room temperature to obtain the negative poisson ratio macroscopic graphene film.
The macroscopic graphene film obtained according to the above steps has a poisson ratio of a negative value, and as shown in fig. 7, the relation between longitudinal strain and transverse strain under uniaxial stretching conditions is shown, and the poisson ratio of the macroscopic graphene film obtained is about-0.39.
According to the negative poisson ratio macroscopic graphene film obtained by the steps, the thickness is about 200 mu m, and as shown in a cross section microscopic morphology diagram of the film in FIG. 8, the negative poisson ratio macroscopic graphene film is formed by stacking sheets and has a loose porous structure.
The negative poisson ratio macroscopic graphene film obtained according to the above steps has good flexibility, and the macroscopic graphene film can be easily bent as shown in fig. 9.
The negative poisson ratio macroscopic graphene film obtained according to the steps has good conductivity, and the four-probe conductivity test shows that the conductivity is about 10 5 S/m.
The negative poisson ratio macroscopic graphene film obtained according to the steps can be used for assembling the flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film.
In the invention, the number of the piezoelectric power generation units with the laminated structure is one or more, the piezoelectric power generation units with the laminated structure are arranged on the substrate in a transverse, longitudinal or array mode, and the electrical connection modes among the piezoelectric power generation units with the laminated structure are in series or parallel connection, as shown in fig. 1, the piezoelectric power generation units with the laminated structure are a flexible piezoelectric energy collector structure schematic diagram arranged on the substrate; as shown in fig. 10, a schematic structural view of a flexible piezoelectric energy collector in which two piezoelectric power generating units of laminated structure are juxtaposed in a lateral fashion over a substrate is shown.
Fig. 10 shows a flexible piezoelectric energy collector of negative poisson's ratio macroscopic graphene, wherein two piezoelectric power generating units with laminated structure are transversely arranged on a substrate and electrically connected in series.
The flexible piezoelectric energy collector of negative poisson's ratio macroscopic graphene with two stacked piezoelectric power generating units in fig. 10 can give a higher open circuit voltage, which is about 2 times the open circuit voltage of the piezoelectric energy collector with one stacked piezoelectric power generating unit.
The foregoing description of the preferred embodiments of the invention is not intended to limit the invention to the precise form disclosed, and any such modifications, equivalents, and alternatives falling within the spirit and scope of the invention are intended to be included within the scope of the invention.
Claims (6)
1. The flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film is characterized by comprising a flexible substrate (1) and a laminated structure piezoelectric power generation unit fixed on the surface of the flexible substrate (1), wherein a wire (4) is arranged on the surface of the laminated structure piezoelectric power generation unit, the wire (4) is used for leading out charges/voltages generated after the flexible piezoelectric energy collector is subjected to tensile deformation, and the laminated structure piezoelectric power generation unit comprises a negative poisson ratio macroscopic graphene film (3) and a flexible piezoelectric film (2);
The preparation method of the negative poisson ratio macroscopic graphene film (3) comprises the following steps:
Step 1, preparing graphene oxide by adopting an improved oxidation method or an electrochemical stripping method;
Step 2, dispersing graphene oxide with ultrapure water to form graphene oxide dispersion liquid with the solid content of 2-4%, and preparing the graphene oxide dispersion liquid into a graphene oxide film by adopting a tape casting method;
Step 3, placing the graphene oxide film obtained in the step 2 into a high-temperature graphitization furnace, and performing high-temperature treatment at 2000-3000 ℃ under the protection of inert atmosphere to obtain a negative poisson ratio macroscopic graphene film (3); the thickness of the negative poisson ratio macroscopic graphene film (3) is 5-200 mu m, the poisson ratio is-0.5-0, the Young modulus is 0.01-20GPa, and the conductivity is not lower than 10 4 S/m.
2. The flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film according to claim 1 is characterized in that in the laminated structure piezoelectric power generation unit, the negative poisson ratio macroscopic graphene film (3) is fixed on the upper side and the lower side of the flexible piezoelectric film (2).
3. The flexible piezoelectric energy collector based on negative poisson's ratio macroscopic graphene film according to claim 2, characterized in that the piezoelectric film (2) is made of PVDF and at least one of its copolymers or piezoelectric composite material, with a thickness of 10-100 μm.
4. The negative poisson ratio macroscopic graphene film based flexible piezoelectric energy collector according to claim 1, wherein the flexible substrate (1) is made of at least one of PET, polyimide, epoxy, aluminum, copper and stainless steel, and has a thickness of 50-500 μιη.
5. The flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film according to claim 1, wherein the number of the piezoelectric generating units with the laminated structure is one or more, the piezoelectric generating units with the laminated structure are arranged on the substrate in a transverse, longitudinal or array mode, and the electrical connection mode among the piezoelectric generating units with the laminated structure is serial or parallel.
6. The flexible piezoelectric energy collector based on the negative poisson ratio macroscopic graphene film according to claim 1, wherein when the flexible piezoelectric energy collector works, strain coupling exists between the piezoelectric film (2) and the negative poisson ratio macroscopic graphene film (3) in the piezoelectric power generation unit with the laminated structure, so that the piezoelectric film (2) is stretched in two perpendicular directions in the plane of the piezoelectric film.
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| US11905651B2 (en) * | 2020-06-18 | 2024-02-20 | Swift Textile Metalizing LLC | Auxetic fabric reinforced elastomers |
| CN112532106A (en) * | 2020-10-30 | 2021-03-19 | 武汉汉烯科技有限公司 | Flexible piezoelectric energy collector based on macroscopic graphene film negative Poisson ratio structure |
| CN112600461B (en) * | 2020-12-04 | 2023-08-11 | 安徽融兆智能有限公司 | Piezoelectric energy collector |
| CN113630040A (en) * | 2021-08-11 | 2021-11-09 | 武汉理工大学 | Flexible piezoelectric energy collection system based on graphene assembly film |
| CN113904589B (en) * | 2021-09-13 | 2022-09-02 | 广东墨睿科技有限公司 | Preparation method of piezoelectric film substrate-enhanced graphene power generation device |
| CN114221577B (en) * | 2021-12-14 | 2023-02-28 | 哈尔滨工业大学 | Nonlinear piezoelectric energy collector based on elastic cable and negative Poisson's ratio structure |
| CN115259145A (en) * | 2022-07-29 | 2022-11-01 | 武汉汉烯科技有限公司 | Preparation method of high-conductivity macroscopic graphene assembly film close to lower limit of Poisson ratio |
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