KR20170062641A - Structure and manufacturing method of organic-inorganic hybrid piezoelectric nano-generator - Google Patents

Structure and manufacturing method of organic-inorganic hybrid piezoelectric nano-generator Download PDF

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KR20170062641A
KR20170062641A KR1020150167801A KR20150167801A KR20170062641A KR 20170062641 A KR20170062641 A KR 20170062641A KR 1020150167801 A KR1020150167801 A KR 1020150167801A KR 20150167801 A KR20150167801 A KR 20150167801A KR 20170062641 A KR20170062641 A KR 20170062641A
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piezoelectric
semiconductor layer
polymer
nano
electrode
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KR101768911B1 (en
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문두경
이의진
유준영
한용운
고의진
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건국대학교 산학협력단
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    • H01L41/047—
    • H01L41/083—
    • H01L41/187—
    • H01L41/193—
    • H01L41/27—
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02N—ELECTRIC MACHINES NOT OTHERWISE PROVIDED FOR
    • H02N11/00—Generators or motors not provided for elsewhere; Alleged perpetua mobilia obtained by electric or magnetic means
    • H02N11/002—Generators

Abstract

The present invention relates to a nano-power generator and a method of manufacturing the same. More particularly, the present invention relates to a nano-power generator and a method of manufacturing the same. More particularly, the present invention relates to a nano- And a manufacturing method thereof.
A piezoelectric nano-power plant according to the present invention uses a polyvinylidene fluoride (PVDF) as a piezoelectric polymer material and a substrate material to produce a piezoelectric / electrostrictive hybrid piezoelectric / electro-nanoelectric power plant And 72% and 60%, respectively, compared with the conventional PVDF based piezoelectric nano-power generation device.
In addition, according to the method for manufacturing a piezoelectric nano-power plant according to the present invention, it is possible to manufacture mechanically and chemically stable and flexible piezoelectric nano-power generation devices. In addition, since the device can be manufactured by a roll-to-roll process using a flexible substrate and a solution process, a large-area piezoelectric nano-power plant can be produced at an economical production cost.
The fabricated oil-and-inorganic hybrid piezoelectric nano-power plant can be applied as a power source for wearable electronic equipment and portable power supply equipment due to characteristics such as high power output characteristics and flexibility.

Description

TECHNICAL FIELD [0001] The present invention relates to a piezoelectric / electrostrictive device, and more particularly, to a piezoelectric / electrostrictive hybrid piezoelectric /

The present invention relates to a nano-power generator and a method of manufacturing the same. More particularly, the present invention relates to a nano-power generator and a method of manufacturing the same. More particularly, the present invention relates to a nano- And a manufacturing method thereof.

Piezoelectric nano-power plant is a device that converts abandoned mechanical energy into electric energy, which is often found in the vicinity, and is attracting attention as a device that can meet the increasing electric power demand due to the development and diffusion of electronic devices. Piezoelectric nanowire power plants consist of piezoelectric materials and electrodes that convert mechanical energy into electrical energy. Typical examples of piezoelectric materials include polymer piezoelectric materials, piezoelectric composites, and inorganic nanostructures. Among them, the polymer piezoelectric material has excellent thermal and chemical stability, and it is possible to manufacture an economical and flexible device because of low unit price and flexibility of the material.

Polyvinylidene fluoride (PVDF) is a typical polymer piezoelectric material that generates electricity when bent or pulled. PVDF is the material with the highest dielectric constant among polymer materials.

Non-Patent Document 1 discloses a method of forming a PVDF nanofiber using a PVDF solution and manufacturing and evaluating a nanodevice. Non-Patent Document 2 discloses a piezoelectric nanofiber using P (VDF-TrFE) polymer and graphene, Power generation devices. In both cases, the polymer substrate has a separate device structure, and there is a limit to the problem of low output in the unit device.

Accordingly, the present inventors have completed a piezoelectric nanowire power plant in which an inorganic semiconductor layer and a polymer semiconductor layer are further added in addition to a conventional PVDF substrate, and the maximum voltage and current of the piezoelectric nanowire power generator The inventors have confirmed that the present invention is significantly improved compared to the power generation device, and completed the invention.

(Non-Patent Document 0001) Direct-Write Piezoelectric Polymeric Nanogenerator with High Energy Conversion Efficiency, Chieh Chang, Van H. Tran, Junbo Wang, Yiin-Kuen Fuh, Liwei Lin, Nano Lett. 10 Issue 2, pp. 726-731.

(Non-Patent Document 0002) Highly Stretchable Piezoelectric-Pyroelectric Hybrid Nanogenerator, Ju-Hyuck Lee, Keun Young Lee, Manoj Kumar Gupta, Tae Yun Kim, Dae-Yeong Lee, Junho Oh, Changkook Ryu, Won Jong Yoo, Chong-Yun Kang Seok-Jin Yoon, Ji-Beom Yoo, Sang-Woo Kim, Adv. Mater. 2014, Vol. 26, pp. 765-769

SUMMARY OF THE INVENTION An object of the present invention is to solve the conventional problems as described above and to provide a piezoelectric / . In order to achieve the above object, the present invention provides a piezoelectric nano-power plant improved in problems by applying an inorganic semiconductor or a polymer semiconductor material.

Another object of the present invention is to provide a fabrication method of an organic / inorganic hybrid piezoelectric nanowire power plant by applying an inorganic semiconductor or a polymer semiconductor material to PVDF.

According to an aspect of the present invention, there is provided a semiconductor device comprising a piezoelectric polymer substrate, a first electrode including an electrode disposed under the piezoelectric polymer substrate, an inorganic semiconductor layer disposed on the piezoelectric polymer substrate, A charge transport layer disposed on the polymer semiconductor layer; And a second electrode disposed on the charge transport layer. The present invention also provides an organic-inorganic hybrid piezoelectric nano-electric power plant including the first electrode and the second electrode.

The piezoelectric polymer substrate may be formed of at least one selected from the group consisting of polyvinylidene fluoride (PVDF), poly (vinylidene fluoride trifluoroethylene), poly (VDF-TrFE), polydimethylsiloxane (PDMS), and a PDMS-piezoelectric semiconductor composite film.

The inorganic semiconductor layer is characterized by comprising at least one material selected from the group consisting of zinc oxide (ZnO), titanium oxide (TiOx), barium titanium oxide (BaTiO 3).

The polymer semiconductor layer is made of a conjugated polymer and has a thickness of 50 to 200 nm.

Wherein the conjugated polymer is selected from the group consisting of poly [(4,8-di- (2-ethylhexyloxy) benzo [1,2 -bis: 4,5-bis] dithiophene-2,6-diyl (Poly [(4,8-di- (2-ethylhexyloxy) -2,2'-bithiophene] ) benzo [1,2- b: 4,5-b '] dithiophene-2,6-diyl) -tallow- (5,5'-yl) -4,4'-bis (2-ethylhexyl) '-Bithiophene)], PBDTBiTh (2EH)].

[Chemical Formula 1]

Figure pat00001

In Formula 1, n is an integer of 1 to 100,000.

Wherein the charge transport layer is formed of a metal oxide semiconductor material or a conductive polymer material.

Wherein the first electrode and the second electrode are made of at least one metal selected from the group consisting of aluminum (Al), gold (Au), and silver (Ag).

Wherein the first electrode and the second electrode are made of one or more transparent conductive metal oxides selected from the group consisting of indium tin oxide (ITO), indium zinc tin oxide (IZTO), and aluminum doped zinc oxide (AZO) .

(1) preparing a piezoelectric polymer substrate; (2) forming an inorganic semiconductor layer on the piezoelectric polymer substrate; (3) forming a polymer semiconductor layer on the inorganic semiconductor layer; And (4) forming a charge transport layer on the polymer semiconductor layer. The present invention also provides a method of manufacturing an organic-inorganic hybrid piezoelectric nano-electric power plant.

The preparation of the piezoelectric polymer substrate is characterized by modifying the surface of the piezoelectric polymer substrate with ozone generated by ultraviolet rays or oxygen radicals generated by plasma.

A piezoelectric nano-power plant according to the present invention uses a polyvinylidene fluoride (PVDF) as a piezoelectric polymer material and a substrate material to produce a piezoelectric / electrostrictive hybrid piezoelectric / electro-nanoelectric power plant And 72% and 60%, respectively, compared with the conventional PVDF based piezoelectric nano-power generation device.

In addition, according to the method for manufacturing a piezoelectric nano-power plant according to the present invention, it is possible to manufacture mechanically and chemically stable and flexible piezoelectric nano-power generation devices. In addition, since the device can be manufactured by a roll-to-roll process using a flexible substrate and a solution process, a large-area piezoelectric nano-power plant can be produced at an economical production cost.

The fabricated oil-and-inorganic hybrid piezoelectric nano-power plant can be applied as a power source for wearable electronic equipment and portable power supply equipment due to characteristics such as high power output characteristics and flexibility.

1 is a cross-sectional view of an oil-and-inorganic hybrid piezoelectric nano-power plant according to the present invention.
2 is a perspective view for explaining a driving mode according to the physical force of the oil-and-inorganic hybrid piezoelectric nano-power plant.
FIG. 3 is a graph showing voltage and current output characteristics of a piezoelectric / electrostrictive hybrid piezoelectric nanowire generator according to the present invention.
4 is a graph showing voltage and current output characteristics of a PVDF single-layer nano-power plant.

Hereinafter, the present invention will be described in detail.

The present invention relates to a piezoelectric polymer substrate, a first electrode including an electrode disposed under the piezoelectric polymer substrate, an inorganic semiconductor layer disposed on the piezoelectric polymer substrate, and a polymer semiconductor layer disposed on the inorganic semiconductor layer. A charge transport layer disposed on the polymer semiconductor layer; And a second electrode disposed on the charge transport layer. The present invention also provides an organic-inorganic hybrid piezoelectric nano-electric power plant including the first electrode and the second electrode.

In addition, the present invention provides a method of fabricating a U-inorganic hybrid piezoelectric nano-electric power generation device. The specific process of the oil-inorganic hybrid piezoelectric nano power plant is as follows: (1) preparing a piezoelectric polymer substrate; (2) forming an inorganic semiconductor layer on the piezoelectric polymer substrate; (3) forming a polymer semiconductor layer on the inorganic semiconductor layer; And (4) forming a charge transport layer on the polymer semiconductor layer.

The preparation of the piezoelectric polymer substrate may be performed by modifying the surface of the piezoelectric polymer substrate with ozone generated by ultraviolet rays or oxygen radicals generated by plasma.

As shown in FIG. 1, the first electrode 110, the piezoelectric polymer substrate 120, the inorganic polymer electrolyte membrane 120, the inorganic polymer electrolyte membrane 120, The semiconductor layer 130, the polymer semiconductor layer 140, the charge transport layer 150, and the second electrode 160 are stacked.

In the present invention, the piezoelectric polymer substrate 120 used in manufacturing the organic-inorganic hybrid piezoelectric power generation device is formed of a material selected from the group consisting of polyvinylidene fluoride (PVDF), poly (vinylidene fluoride-trifluoroethylene) such as a piezoelectric polymer and a composite material including a polymer electrolyte membrane, a polymer electrolyte membrane, a polymer electrolyte membrane, a polymer electrolyte membrane, a polymer electrolyte membrane, a polymer electrolyte membrane, a polymer electrolyte membrane, a polymer electrolyte membrane, and a polymer electrolyte membrane. A PVDF piezoelectric polymer substrate was used as the substrate.

On the other hand, if the surface of the piezoelectric polymer substrate 120 is hydrophilically modified and pretreated, the formation of the inorganic semiconductor layer 130 is facilitated and the quality of the thin film can be improved. Techniques for this include (i) a method of modifying the surface through ozone generated by using ultraviolet rays in a vacuum state, (ii) a method of modifying the surface by using oxygen radicals generated by plasma, and One of the above methods may be selected and applied. In the present invention, a method of modifying the surface through ozone generated by using ultraviolet rays is used. In the present invention, the method of modifying the surface of the piezoelectric polymer substrate 120 is not particularly limited, Is also irrelevant.

The inorganic semiconductor layer 130 is formed by applying an inorganic semiconductor material to one side of the substrate or coating the inorganic semiconductor material in a film form using sputtering, E-Beam, spin coating, screen printing, inkjet printing, doctor blade or gravure printing . The inorganic semiconductor layer 130 is mainly an n-type material and includes ZnO, TiOx, and BaTiO 3 that can form a pn junction with the polymer semiconductor layer 140. In the present invention, ZnO nanoparticles through a solution process are applied to the inorganic semiconductor layer 130.

When the inorganic semiconductor layer 130 is formed, the ZnO nanoparticle solution is preferably spin-coated and then heated at a temperature ranging from room temperature to 80 ° C, more preferably 80 ° C. Meanwhile, the spin coating and the heat treatment are preferably carried out in an atmospheric condition or a nitrogen atmosphere, more preferably in an atmospheric condition.

As the polymer semiconductor layer 140 material of the present invention, a conjugated polymer such as poly [(4,8-di- (2-ethylhexyloxy) benzo [1,2 -bis: 4,5-bis'] dithiophen- 2,6-diyl) -ald- (5,5'-yl-4,4'-bis (2-ethylhexyl) -2,2'-bithiophen)] ([Poly [ - (2-ethylhexyloxy) benzo [1,2-b: 4,5-b '] dithiophene-2,6-diyl) -tallow- (5,5'-yl-4,4'-bis (2- ) -2,2'-bithiophene] and PBDTBiTh (2EH) (represented by the following Chemical Formula 1 and synthesized by the present inventor) were used. The polymer semiconductor layer 140 was prepared by dissolving conjugated high molecular materials in an organic solvent The polymer semiconductor layer 140 is introduced into the solution dissolved in an organic solvent to a thickness of 50 to 200 nm, preferably 80 to 150 nm, by spin coating or the like. At this time, in order to form the polymer semiconductor layer 140, , Screen printing, spray coating, doctor blade, brush painting, etc. can be applied.

[Chemical Formula 1]

Figure pat00002

In the general formula (1), n is an integer of 1 to 100,000.

The charge transport layer 150 is introduced to smooth the movement of charge from the polymer semiconductor layer to the second electrode. As the charge transport layer 150, a metal oxide semiconductor material such as MoO 3 or WoO 3 and a conductive polymer such as poly (3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT: PSS) may be applied.

The first electrode 110 and the second electrode 160 transfer electric energy, current, and voltage generated when a physical force is applied to the piezoelectric polymer substrate. The first electrode 110 and the second electrode 160 may be formed of a metal material such as Al, Au, or Ag or indium tin oxide (ITO), indium zinc tin oxide (IZTO), aluminum doped zinc oxide Of a transparent conductive metal oxide.

The oil-and-inorganic hybrid piezoelectric nano-power plant manufactured as described above has a cross-sectional structure as shown in FIG. 1, and when subjected to external physical force or pressure, deformation occurs in the same manner as in FIG. 2, As this deformation progresses, it is driven and power is generated.

Hereinafter, the present invention will be described in more detail with reference to Examples. It is to be understood by those skilled in the art that these embodiments are for illustrating the present invention only and that the scope of the present invention is not construed as being limited by these embodiments.

Example 1. Fabrication of a U-Inorganic Hybrid Piezoelectric Nano-Power Generator

The polymeric semiconductor layer 140, the charge transport layer 150, the first electrode 110, and the first electrode 110 are formed in order to fabricate the organic / inorganic hybrid piezoelectric nanoelectric power plant using the PVDF piezoelectric polymer substrate 120. [ The thickness of the two electrodes 160 and the manufacturing process were optimized.

We fabricated the piezoelectric / electrostrictive hybrid piezoelectric / electrostrictive nano-power plant with a structure of Al (100 nm) / PVDF / ZnO (100 nm) / PBDTBiTh (2EH) (80 nm) / MoO 3 (10 nm) / Ag (100 nm).

Specifically, the surface of the PVDF substrate 120 is modified through ozone generated using ultraviolet rays, and a ZnO nanoparticle solution prepared from zinc nitrate hexahydrate, sodium hydroxide, ammonia, ultrapure water or the like is spin-coated thereon, And the ZnO inorganic semiconductor layer 130 was formed by heat treatment.

A PBDTBiTh (2EH) conjugated polymer solution dissolved in chlorobenzene at a concentration of 10 mg / ml was spin-coated on the inorganic semiconductor layer 130 and then heat-treated at 80 ° C. The polymer semiconductor layer (140) was formed to a thickness of 80 nm.

The charge transport layer 150, the first electrode 110 and the second electrode 160 are transferred to a high vacuum chamber (not more than 10 -6 torr) of a thermal evaporator to form a charge transport layer MoO 3 (0.3 Å / s, 10 Nm), a first electrode (5 Å / s, 100 nm), and a second electrode (Ag (2 Å / s, 100 nm)).

Such a manufacturing method is a method capable of producing a device by a roll-to-roll process using a flexible substrate and a solution process, so that a large-area piezoelectric nano-power plant can be produced at an economical production cost.

Comparative Example 1. Fabrication of PVDF single material piezoelectric nano-electric power generation device

A piezoelectric nanotube power plant formed of only the charge transport layer 150, the first electrode 110 and the second electrode 160 on the PVDF piezoelectric polymer substrate 120 was manufactured as a comparative example. The charge transport layer, 1 < / RTI > and 2 < nd > electrodes.

Experimental Example 1. Characterization of a U-Inorganic Hybrid Piezoelectric Nanowire Power Plant

In order to measure the electrical characteristics of the piezoelectric nano-power plant manufactured in Example 1 and Comparative Example 1, each characteristic was evaluated using a Keithley DMM7510 (Keithley DMM7510, Keithley, USA) and a banding tester (Science Town, Korea) Respectively.

Figure pat00003

The comparison between Example 1 and Comparative Example 1 is made by comparing the characteristics of the ZnO Inorganic Semiconductor Layer and the PBDTBiTh (2EH) polymer semiconductor layer introduced (FIG. 3) and (FIG. 4) Respectively. (FIG. 3) is a time-voltage, time-current graph of Example 1, and FIG. 4 is a time-voltage, time-current graph of Comparative Example 1. FIG. The maximum voltage and the maximum current of Example 1 and Comparative Example 1 were determined from Table 1 (FIG. 3) and FIG. 4 (Table 1). (Comparative Example 1) in which the maximum voltage and current of the organic-inorganic hybrid piezoelectric nano-electric power generation device (Example 1) used by introducing ZnO and PBDTBiTh (2EH) were not introduced Respectively, by 72% and 60%, respectively. This is because the pn junction of the ZnO inorganic semiconductor and the PBDTBiTh (2EH) polymer semiconductor improves the collection and migration of the charge generated on the PVDF substrate, and demonstrates the superiority of the first embodiment of the piezoelectric nano-power plant.

Having described specific portions of the present invention in detail, those skilled in the art will appreciate that these specific embodiments are merely preferred embodiments and that the scope of the present invention is not limited thereby. something to do. Accordingly, the actual scope of the present invention will be defined by the appended claims and their equivalents.

110: first electrode
120: Piezoelectric polymer substrate
130: Inorganic semiconductor layer
140: Polymer semiconductor layer
150: charge transport layer
160: Second electrode

Claims (10)

Piezoelectric polymer substrate;
A first electrode including an electrode disposed under the piezoelectric polymer substrate;
An inorganic semiconductor layer disposed on the piezoelectric polymer substrate;
A polymer semiconductor layer disposed on the inorganic semiconductor layer;
A charge transport layer disposed on the polymer semiconductor layer; And
And a second electrode disposed above the charge transport layer.
The method according to claim 1,
The piezoelectric polymer substrate may be formed of a material selected from the group consisting of polyvinylidene fluoride (PVDF), poly (vinylidene fluoride trifluoroethylene) copolymer (P) (VDF-TrFE), polydimethylsiloxane Inorganic hybrid piezoelectric nano-electric power generation device, wherein the piezoelectric / electrostrictive device comprises at least one material selected from the group consisting of polydimethylsiloxane (PDMS) and a PDMS-piezoelectric semiconductor composite film.
The method according to claim 1,
The inorganic semiconductor layer is zinc oxide (ZnO), titanium oxide (TiOx), barium titanium oxide (BaTiO 3), characterized in that oil of one or more material selected from the group consisting of - inorganic hybrid nano piezoelectric power generating device.
The method according to claim 1,
Wherein the polymer semiconductor layer is made of a conjugated polymer and has a thickness of 50 to 200 nm.
5. The method of claim 4,
Wherein the conjugated polymer is selected from the group consisting of poly [(4,8-di- (2-ethylhexyloxy) benzo [1,2 -bis: 4,5-bis] dithiophene-2,6-diyl (Poly [(4,8-di- (2-ethylhexyloxy) -2,2'-bithiophene] ) benzo [1,2- b: 4,5-b '] dithiophene-2,6-diyl) -tallow- (5,5'-yl) -4,4'-bis (2-ethylhexyl) '-Bithiophene)], PBDTBiTh (2EH)].
[Chemical Formula 1]
Figure pat00004

In Formula 1, n is an integer of 1 to 100,000.
The method according to claim 1,
Wherein the charge transport layer is made of a metal oxide semiconductor material or a conductive high molecular material.
The method according to claim 1,
Wherein the first electrode and the second electrode are made of at least one metal selected from the group consisting of aluminum (Al), gold (Au), and silver (Ag).
The method according to claim 1,
Wherein the first electrode and the second electrode are made of one or more transparent conductive metal oxides selected from the group consisting of indium tin oxide (ITO), indium zinc tin oxide (IZTO), and aluminum doped zinc oxide (AZO) Wherein the piezoelectric nanowire power generation device is a piezoelectric / electrostrictive hybrid piezoelectric / electrostrictive device.
(1) preparing a piezoelectric polymer substrate;
(2) forming an inorganic semiconductor layer on the piezoelectric polymer substrate;
(3) forming a polymer semiconductor layer on the inorganic semiconductor layer; And
(4) forming a charge transport layer on the polymer semiconductor layer; and (4) forming a charge transport layer on the polymer semiconductor layer.
10. The method of claim 9,
Wherein the preparation of the piezoelectric polymer substrate comprises modifying the surface of the piezoelectric polymer substrate with ozone generated by ultraviolet rays or oxygen radicals generated by plasma.
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Cited By (3)

* Cited by examiner, † Cited by third party
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CN113652034A (en) * 2021-07-15 2021-11-16 哈尔滨理工大学 GNP/PS-BT/PVDF selective composite film and preparation method thereof
CN117042582A (en) * 2023-10-08 2023-11-10 之江实验室 Self-supporting stretchable piezoelectric film, ultrasonic sensor and preparation method of ultrasonic sensor
US11932558B1 (en) * 2020-03-02 2024-03-19 University Of Rhode Island Board Of Trustees Piezocatalysis using piezoelectric polymers

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KR101213190B1 (en) * 2011-07-19 2012-12-18 서울대학교산학협력단 Fabricating method of piezoelectric nanogenerator

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11932558B1 (en) * 2020-03-02 2024-03-19 University Of Rhode Island Board Of Trustees Piezocatalysis using piezoelectric polymers
CN113652034A (en) * 2021-07-15 2021-11-16 哈尔滨理工大学 GNP/PS-BT/PVDF selective composite film and preparation method thereof
CN117042582A (en) * 2023-10-08 2023-11-10 之江实验室 Self-supporting stretchable piezoelectric film, ultrasonic sensor and preparation method of ultrasonic sensor
CN117042582B (en) * 2023-10-08 2024-02-09 之江实验室 Self-supporting stretchable piezoelectric film, ultrasonic sensor and preparation method of ultrasonic sensor

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