KR20160069346A - Inorganic actin-myosin coupling for stretchable electronics and energy storage - Google Patents
Inorganic actin-myosin coupling for stretchable electronics and energy storage Download PDFInfo
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- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
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Abstract
Description
The present invention relates to a stretchable electronic device and an inorganic actin-myosin linkage for energy storage, and more particularly to an actin-myosin linkage mechanism of muscle fibers in an organism by graphene-carbon nanotubes The present invention relates to a technique for developing a new elastic electronic device that can be energy-saved and converted and applied to an electronic device (graphene-CNT) and has elasticity like muscle fibers of an organism.
Recently, the rapid development of electronic information devices is promoting the spread of portable information communication devices and smart devices. Future electronic systems in the next stage can be attached to human body or developed into a form that can be inserted inside human body, And it is expected to develop into a device capable of detecting a medical bio-signal. Therefore, there is a growing interest in the development of artificial electronic skin capable of being attached to human skin, body, or curved part while bending or stretching recently. In particular, research on the development of elastic electrodes has been actively carried out as a key material technology for implementing artificial electronic skin that can bend or stretch. Stretchable electronic devices act as connection, actuation, and physical support between active devices while minimizing stress generated when bending or stretching the device, and maintain a constant electrical conductivity against mechanical deformation to minimize degradation of the final flexible electronic device performance .
Korean Patent Laid-Open Publication No. 2014-0121325 discloses a stretchable electronic circuit and a method of manufacturing the same, wherein a stretchable substrate having a first flat surface and a first corrugated surface outside the first flat surface is formed on a mold substrate A method of manufacturing an elastic electronic circuit using a corrugated surface is used.
US Patent Publication No. 2012-0177934 discloses a method of manufacturing a flexible electrode in which carbon nanotubes are introduced into a coating containing an elastomer.
U.S. Patent Publication No. 2012-0258311 discloses a method of manufacturing a transparent electrode comprising a conductive film as a conductive film which can be used for a flexible silicon thin film semiconductor device.
However, there is no known any flexible electronic device imitating the actin-lysine interaction of an organism anywhere above.
The present invention is directed to a novel flexible electronic device that mimics the actin-myosin interaction of an organism.
In living organisms, various types of intracellular / extracellular motions are made by the interaction of actin-myosin. The basic mechanism of this actin-myosin bond is similar to the concept of stretchable electronic devices as well as movement of organisms.
In inorganic systems that mimic actin-myosin bonds, graphene acts as a floating track as the function of actin filaments in the muscle fibers of an organism, while carbon nanotubes (CNTs: Carbon NanoTube) To the expansion and contraction movement of the motor. Such a system not only imitates the basic mechanism of human motion but also implements performance that was not possible with conventional electronics.
Based on this, the present invention proposes an inorganic system mimicking an actin-myosin bond using a low-dimensional carbon isotope and applies it to various electronic devices.
The present invention relates to a novel stretchable electronic device capable of maintaining mechanical and electrical stability against deformation such as stretching, twisting and the like by applying the interaction mechanism of actin-myosin bond, which is an organic muscle system, to graphene-carbon nanotube bond The purpose is to provide.
The present invention relates to an elastic body made of a material which can be stretched; A carbon nanotube layer formed on an upper surface of the elastic body; And a graphene layer formed on an upper surface of the carbon nanotube layer, wherein the graphene layer and the carbon nanotube layer perform an operation of forming or releasing cross bridges by van der Waals force Thereby providing a stretchable electric device using a graphene-carbon nanotube bond.
In one embodiment of the present invention, the carbon nanotube layer is a layer in which carbon nanotubes are continuously connected to each other when the elastic body is not drawn, and the graphene layer is formed of a discontinuous flake flake).
In one embodiment of the present invention, the carbon nanotube layer is hydrophilized and dispersed.
In one embodiment of the present invention, the carbon nanotube layer is formed to a thickness of 100 nm or more, and the graphene layer is formed to a thickness of 1 nm to 1 μm.
A method of manufacturing a flexible electrical device using a graphene-carbon nanotube bond according to an embodiment of the present invention includes: expanding and fixing an elastic substrate in a two-dimensional form to fabricate an inorganic actin-myosin structure; Forming a carbon nanotube layer using a solution in which carbon nanotubes are dispersed on a substrate made of the elastic material; Forming a graphene layer using a solution in which graphene is dispersed on the carbon nanotube layer; And loosening the elastic substrate.
The step of forming the carbon nanotube layer and the step of forming the graphene layer on the carbon nanotube layer may further include drying the dispersion medium by drying the carbon nanotube layer and the graphene layer.
According to another embodiment of the present invention, there is provided a method of manufacturing a flexible electrical device using a graphene-carbon nanotube bond, wherein the step of forming the carbon nanotube layer comprises the steps of: providing a carbon nanotube (Iljin Nanotech) L is formed on the substrate made of the two-dimensional elastic body to a thickness of 100 nm or more.
Also, in the method of manufacturing a flexible electrical device using a graphene-carbon nanotube bond according to an embodiment of the present invention, the step of forming the graphene layer may include a step of dispersing graphene in a solvent at a concentration of 0.5 g / L A solution is formed on the carbon nanotube layer to a thickness of 1 nm to 1 占 퐉.
Also, in the method for manufacturing a flexible electrical device using a graphene-carbon nanotube bond according to an embodiment of the present invention, the carbon nanotube may be formed by using an acid solution at 80 to 120 ° C for 3 hours or more to make the surface hydrophilic Thereby performing pre-processing.
Also, in the method of manufacturing a flexible electrical device using a graphene-carbon nanotube bond according to an embodiment of the present invention, the graphene may be manufactured by chemical vapor deposition or graphene oxide reduction. Methods for producing graphene from graphene oxide include a chemical reduction method using a reducing agent, a thermal reduction method using a microwave, and a reduction method using a solvent thermal synthesis method.
In addition, in the method of manufacturing a flexible electrical device using a graphene-carbon nanotube bond according to an embodiment of the present invention, the elastic material can be used without limitation as long as it is used as a substrate of a flexible electronic device. , Rubber, latex or PVA, silk, plastic or the like can be used.
In addition, in the method of manufacturing an elastic energy storage device using a graphene-carbon nanotube bond according to an embodiment of the present invention, the elastic substrate mainly uses a polymer material having elasticity, for example, polyvinyl alcohol, Poly ethylene oxide, polyacrylonitrile, poly methyl methacrylate, poly vinyl chloride, polyvinyl chloride / polymethyl methacrylate copolymer (polyvinyl chloride / polymethyl methacrylate copolymer) vinyl chloride / poly methyl methacrylate blend, polyvinylidene fluoride, polyvinylidene fluoride-hexafluoro propylene, and the like. .
In addition, an elastic energy storage device using a graphene-carbon nanotube bond according to an embodiment of the present invention includes an electrolyte gel prepared by mixing a material that can be used as an electrolyte with the polymer material, dissolving the gel, Can be prepared through a manufacturing step.
The present invention relates to a stretchable electronic device and an inorganic actin-myosin bond for energy storage, wherein graphene acts as an actin in implementing an inorganic actin-myosine bond, and the carbon nanotube plays a role of myosin Carbon nanotube-bonded structure capable of storing and converting energy through a dielectric double layer of graphene, so as to have a mechanically stable stretchability even when physical energy is externally applied, There is an effect that can be provided.
FIG. 1 is a view for explaining atomic scale interaction of actin-myosin and graphene-carbon nanotube, respectively, according to an embodiment of the present invention.
2 is a view for explaining a micro-sized structure of an inorganic actin-myosin (graphene-carbon nanotube) according to an embodiment of the present invention.
FIG. 3 is a view for explaining an inorganic actin-myosin (graphene-carbon nanotube) on various substrates according to an embodiment of the present invention.
4 is a view for explaining a characteristic of dielectric energy storage of an inorganic actin-myosin (graphene-carbon nanotube) on various substrates according to an embodiment of the present invention.
5 is a schematic view of a graphene piece on a carbon nanotube cluster according to an embodiment of the present invention.
6 is a view for explaining a method of manufacturing a graphene-carbon nanotube inorganic muscle having a crumpled structure according to an embodiment of the present invention.
BEST MODE FOR CARRYING OUT THE INVENTION Hereinafter, one embodiment of a flexible electrode according to the present invention and inorganic actin-myosin binding for energy storage will be described with reference to the accompanying drawings.
The inorganic electronic device basically does not have ductility and stretchability of an organism. Until now, the elasticity strategy of inorganic electronic devices was based on a stretchable wave structure or stretchable material, and the inspiration of the elasticity strategy was obtained only from the phenomenological characteristics of biological action, I did.
Thus, the present invention seeks to propose a graphene-carbon nanotube weapon system inspired by the actin-myosin power stroke mechanism of muscle motions to realize biomimetic stretchable electronic devices and energy storage. Such a muscle-imitating system allows randomly floating plates to store and transform energy through the formation of electrical double layers with a wide surface, making them stretchable in all directions in tension, shear and mixed modes.
A typical cell involved in the movement of higher animals is the sarcomere of muscle tissue. The extermination includes actin filaments having functions such as a myosin molecule having the same function as a molecular motor and a track for controlling the movement of the motor assembly.
The present invention utilizes a thin and wrinkled graphene-carbon nanotube layer capable of withstanding all-round tautness and relaxation, as shown in FIG. 1A to mimic the molecular motor and track.
FIG. 1B shows the stroke operation similarity of the graphene-carbon nanotube bonding system and the actin-myosin bonding system of the present invention. Both of these systems operate in a low affinity and high affinity affinity cycling state between the motor (myosin) and the track (actin).
During biological muscle movement, muscles contract through the action of forming or releasing chemical bonds (cross bridges) with the thin actin filament molecules at the head of myosin. More specifically, the biological muscle movement uses chemical energy. When ATP (adenosine triphosphate) binds to myosin hair, binding of myosin hair and actin filament is released. ATP, which is bound to myosin hair, Phosphate) and Pi (inorganic phosphoric acid), and the myosin hair is again bound to the actin filament using the energy released in this process. The hydrolyzed ADP and Pi are separated from the myosin head, and the myosin head leans and the muscle contraction movement is performed while pushing the actin filament bonded to the myosin head in the direction in which the myosin head is inclined.
On the other hand, in the inorganic system of the present invention, cross bridges are formed by Van der Walls interaction between nanocarbon tube filaments and graphene sheets. That is, the nanocarbon tube has elasticity through the action of forming or releasing a graphene sheet and cross bridges, which actin actin like myosin. As described above, the cross bridges of graphene sheets and carbon nanotubes are formed in a so-called AB laminated structure (bonded to a closed chain structure of six carbons), and the state in which the carbon nanotubes are separated from the graphene sheet is called a so- Structure.
Whether cross-bridges between carbon nanotubes and graphenes are formed or released is based on physical energy. That is, the chemical energy obtained from the hydrolysis of ATP in the organism is replaced by external physical energy such as pulling or biting in the inorganic system. The AB stacking binding energy of the graphene and carbon nanotubes is 0.49 eV UC -1 per unit cell. In addition, the energy when the carbon atom is pushed is 0.08 eV UC -1 , which is six times lower than the binding energy, in order to change the graphene and carbon nanotubes from the AB lamination bond to the AA laminate state. Since the AB layer is the most stable structure in the graphene-carbon nanotube bond structure, the surface atoms of the carbon nanotubes naturally migrate to the carbon atom holes of graphene. As a result, the edges of the carbon nanotube are continuously moved forward while performing docking / undocking with the graphene plate. This phenomenon causes dissociation of the inorganic bonds between the carbon nanotubes and the graphene, and the carbon nanotubes move along the surface of the graphene plate.
As described above, in the organic muscle system, after the ADP is separated from the myosin head, the myosin head is separated from the actin filament while being recombined with ATP, and the actin filament and the cross bridge are again formed At this time, the myosin head moves 11 nm from the previous cross bridge point and combines with the actin filament. Similarly, in a graphene-carbon nanotube bond, it shifts 2.46 Å, which is equal to the distance from a hole made up of six carbon atoms of adjacent graphene.
FIG. 2 shows an optical / scanning electron microscope (SEM) image and a three-dimensional finite element modeling (3D-FEM) of the mechanics of the graphene-carbon nanotube muscle on an elastic substrate.
An arbitrary myosin movement is caused by contraction and relaxation of the human muscle. Likewise, the carbon nanotube movement on the graphene track is represented by the stretching and releasing of inorganic muscles inspired by actin-myosin bonds.
FIG. 2B shows an optical image and 3D-FEM of a graphene-nano carbon tube layer twisted and twisted into one axis and two axes. As shown, the inorganic design of the present invention (graphene-carbon nanotube bond) can withstand large scale or complex deformation such as muscle bending.
Modifications of graphene-carbon nanotube connections include the following steps.
1) The graphene-carbon nanotubes contain many non-coplanar corrugations such as wrinkled paper, which are physically expanded by external forces (see FIG. 2C and FIG. 6).
2) After further expansion of the structure (after expansion), a further twisted carbon nanotube cluster at the micrometer level is pulled and graphene bound to the carbon nanotube cluster by van der Waals force (See D in Fig. 2).
Microscopically, each cross bridge between the graphene and carbon nanotube layers is randomly subdivided into a stretch of the carbon nanotube network. The serpentine carbon nanotube network has non-directional and non-coplanarity. Since the graphene pieces repeatedly provide 2D tracks, the cross bridges are constantly rebuilt while the carbon nanotubes are moving regardless of the direction.
From a broad point of view, the graphene piece which can not be deformed during the rebuilding of the cross bridge is pulled by the stretching of the carbon nanotube filament. This is similar to the movement of the tectonic plates of continental drift (see Figures 2D and 5).
The activation energy for the graphene sheet is 0.08 eV UC - 1 , which is much smaller than the strain energy of the graphene sheet. In the SEM image shown in FIG. 2C, each solid graphene area is indicated as a bright area. The size of the graphene piece when stretching and releasing is 100 μm 2 . Graphene sheets have many advantages due to their electrical, mechanical and thermal properties, but they are not stretchable and the advantages are irreversibly reduced when the graphene sheet is deformed. However, in the inorganic muscle system of the present invention, graphene can be stretched to a high level while maintaining its inherent advantages.
According to the percolation theory, percolation islands cause a decrease in the conductivity index, but in the case of carbon nanotube stretch motors connected to graphene pieces, the unique characteristics of the graphene surface are maintained even at high strain rates Reference).
This has not previously been feasible in a stretch system, and it is also possible to stably store a large amount of energy in a dielectric double layer.
Stretchable energy storage is one of the most complex systems among various electronic devices because the movement of ions must be considered. Moreover, in next generation technologies such as integrating electronic devices into surgical gloves or hemispherical substrates as described above, energy storage conversion systems are limiting factors for achieving full power independence and flexibility.
Graphene slices have a large dielectric bilayer that is energy-induced due to extremely high surface area, as well as providing a fluid, unmodifiable micro-area for the activated device on the deformed carbon nanotube stretch circuit.
In a dielectric bilayer mechanism, the specific surface area of a material is directly proportional to the energy storage conversion performance, and graphene is currently considered the best candidate for use in an energy storage conversion system.
In order to manufacture an inorganic muscle for energy storage, the present invention uses a stretchable polymer material as a disk for graphene-carbon nanotube inorganic muscle, for example, polyvinyl alcohol, poly ethylene oxide ), Polyacrylonitrile, poly methyl methacrylate, poly vinyl chloride, poly vinyl chloride / poly methyl methacrylate blend (polyvinyl chloride / poly methyl methacrylate blend) Polyvinylidene fluoride, polyvinylidene fluoride-hexafluoro propylene, and the like can be used. The elastic polymer material may include an electrolyte. As the electrolyte, a plurality of salts including Li, such as H 3 PO 4 , H 2 SO 4 , KOH, NaOH, KCl, NaCl, and LiCl may be used.
The elasticity of the energy storage system comes not only from elastic carbon nanotube clusters but also from substrates made of elastic polymeric materials. Elastic polymer materials and carbon nanotube clusters constitute a network chain that meanders at atomic and microscale levels, which maintains the structure of the electrodes and contributes to reversibility of deformation.
Hereinafter, the present invention will be described in more detail with reference to examples.
[Example]
1. Graphene-Carbon Nanotube Inorganic Muscle Manufacturing Method
6 is a view for explaining a process of manufacturing a graphene-carbon nanotube inorganic muscle having a crumpled structure according to an embodiment of the present invention.
As shown in Fig. 6, various elastomers (rubber, latex, PVA, etc.) are stretched and fixed two-dimensionally in order to produce the inorganic actin-myosin structure first.
To 200 μl ethanol was added 70% HNO 3 at 110 ° C for 8 hours to make the surface hydrophilic The solution prepared by dispersing the carbon nanotubes (ILJIN Nanotech.) Pretreated in the solution at a concentration of 0.5 g / L is applied in 10 layers on the substrate made of the two-dimensional elastic body. After the carbon nanotubes were applied, they were dried through natural drying at room temperature and then used.
Following this procedure, a solution in which graphene ink is dispersed at a concentration of 0.5 g / L in ethanol (200 μl) is applied in triplicate to the carbon nanotube layer.
The graphene was prepared from graphene oxide in a microwave oven for 2 minutes.
Thereafter, when the elastic substrate is loosened, the corrugated graphene-carbon nanotube layer is formed.
2. Manufacture of electrosurgical gloves and contact lenses
To demonstrate the formation of electrical circuitry on surgical gloves and contact lenses, stretching was performed after bonding LED cells (HSMC-C150 (3.2 mm x 1.6 mm) onto a silver paste using conventional brazing methods, During the stretching, the LED worked perfectly.
3. Manufacture of inorganic muscle which stores energy
PVA powder, 5 g of H 3 PO 4 4g And 40 ml of water were mixed to prepare an electrolyte gel PVA / H 3 PO 4 .
The PVA / H 3 PO 4 prepared above is vigorously stirred while heating at 385 K until it becomes clear.
Thereafter, PVA / H 3 PO 4 To prepare the film the PVA / H 3 PO 4 The gel is poured into a Petri dish, dried and fixed in two dimensions.
The PVA / H 3 PO 4 A 10-fold solution of carbon nanotubes (ILJIN Nanotech.) Dispersed in 200 μl of ethanol on a film at a concentration of 0.5 g / L, and a solution in which graphene ink was dispersed at a concentration of 0.5 g / L in ethanol (200 μl) Is applied on the carbon nanotube layer in three layers.
Subsequently, the carbon nanotubes and the graphene ink were dispersed in PVA / H 3 PO 4 It is also applied to the opposite side of the film.
Relaxing the stretched film completes the corrugated energy storage system.
In the present invention, a field emission scanning microscope (AURIGA, Carl Zeiss) was used as an SEM image used to measure the shape and electrical characteristics of the inorganic muscle (graphene-carbon nanotube muscle).
In addition, C / Ds and CVs were performed in the range of 0 ~ 0.8V using a computer controlled constant current device (ZIVE SP2, ZtVE, LAB). All C / D and CV curves are based on 10 analytical data.
In order to examine the characteristics of the graphene-carbon nanotube inorganic muscle according to the above embodiment, the following analysis was performed.
FIG. 3 is a view for explaining an inorganic actin-myosin (graphene-carbon nanotube) on various substrates according to the above embodiment, wherein a change in conductivity in various deformation states is monitored to obtain a stable connection between pieces of graphene Respectively.
As shown in Fig. 3A, in the case of uniaxial deformation, the resistance of the inorganic muscle structure hardly changes under a tensile strain of 80%. In this case, the strain of 80% refers to a state in which the length is increased to 180% at a certain axis when the electrode is not stretched at 100%.
As shown by the percolation threshold value in Figure 3B, the limiting strain of the structure is 75%. In this case, the critical strain means a percolation thresh-hold in a state where the electrical performance begins to deteriorate. Despite this limit strain value, the electrical activity of the inorganic muscle structure of the present invention showed a reversible reversibility during 100 cycles of stretching-releasing over 150% strain. Therefore, even if the structure is deformed beyond the critical strain, it is stable without affecting its electrical activity characteristics.
In FIG. 3C, in order to examine the system error under extreme mixed strain conditions, an inorganic muscle layer was placed on a rubber balloon and conductivity was measured during repeated shrinkage and expansion. It induces biaxial deformation and shear deformation of the inorganic muscle layer installed in the rubber balloon by air injection.
FIG. 3D shows an inorganic muscle layer in a contracted and expanded state during conducting conductivity measurements. As shown, the rubber balloon was expanded to 140%, and as a result, the inorganic muscle was found to have an excellent electrical conductivity over 100 cycles up to 80% deformation. Referring to FIG. 3E, the 3D-FEM simulation results show that the expansion of the graphene-carbon nanotube on the rubber balloon is 136% (the radius of the balloon is 2 cm).
Further, the present invention demonstrated inorganic muscles such as electric circuits in an electrosurgical glove and a hemispherical contact lens, as shown in F and G of Fig. Light-emitting diodes (LEDs) in flexible circuits have been incorporated into graphene chips through traditional soldering methods. The LEDs work well in an elongated and curved environment, which is believed to be due to the fact that the unstrained regions supporting the LEDs may flow freely along the stretched carbon nanotubes.
The above results show that the inorganic muscle of the present invention does not necessarily have to be designed according to the installation environment due to the actual biomimetic structure, and can be attached to the curved surface.
For example, as shown in G of FIG. 3, it can be attached to the curved portion of the contact lens, and maintains the ability of correcting the visual acuity after the actual electronic circuit is inserted. As a result, the inorganic muscle system of the present invention can be used for the fusion of a hemispherical photodetector with an electronic device which is not possible in the prior art.
On the other hand, elastic energy storage is one of the most complex systems among various electronic devices because the movement of ions must be considered. Moreover, in next generation technologies such as integrating electronic devices into surgical gloves or hemispherical substrates as described above, energy storage conversion systems are limiting factors for achieving full power independence and flexibility.
FIG. 4 shows the dielectric energy storage characteristics of the graphene-carbon nanotube inorganic muscle of the present invention.
4 (a) is a graph showing the charging / discharging curve (C / Ds) of the inorganic muscle during stretching. Based on the mass of the active element in the graphene layer, the non - conducting capacity is 329 F g - 1 . This is higher than the performance of the non-stretchable dielectric electrode materials reported so far. In addition, the capacitance based on the total mass, including passive components, is 58.4 F g - 1 , which is much more efficient than in the case of conventional stretch systems. The inorganic muscle has a stable charge / discharge performance for 3.3 hours during deformation and can be stretched to a strain of 80% without degradation.
Figures 4B and 4C show representative C / Ds and cyclic voltammetric curves (CVs) of the inorganic muscle measured at various currents and scan speeds when no strain, 80% increase, and 360 degrees twist, respectively Graph. The CVs show that the system has a rectangular shape within the selected potential range, even under highly deformed conditions and high scan rates, and has excellent capacitance even at high strain rates. This result is consistent with C / Ds.
Optical image and 3D FEM simulation when 360 degrees twisted indicate that the system has mechanical stability (FIG. 2B).
The results of FIGS. 4B and C (C / D and CV) show that the inventive inorganic muscle system has a stable and high energy storage characteristic even at 360 ° twisted state (349 F g -1 ). The curves in FIGS. 4 (B) and 4 (C) show little change compared to the original relaxed state, rather a little higher performance, and the mechanical and electrical durability of the overall system is high.
Therefore, the inorganic muscle of the graphene-carbon nanotube according to the present invention can maintain its chemical and electrical properties even when it is stretched, so that it is suitable for use as a stretchable electronic device and has a high energy storage characteristic, It is used for renewable energy platforms such as solar energy, wind power, and tidal power generation through smart grid, energy storage devices of wearable devices such as mobile phones, curved TVs, energy storage devices for flexible devices, smart watches and wearable electronic devices .
While the present invention has been particularly shown and described with reference to exemplary embodiments thereof, it is clearly understood that the same is by way of illustration and example only and is not to be taken by way of limitation, I will understand. Accordingly, the technical scope of the present invention should be defined by the following claims.
Claims (7)
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KR101908604B1 (en) * | 2018-02-08 | 2018-10-16 | 주식회사 케이비엘러먼트 | Manufacturing method for transparent electrode panel using composite solution of CNT and graphene, and transparent electrode panel prepared by the same |
KR102198396B1 (en) * | 2019-07-24 | 2021-01-05 | 고려대학교 세종산학협력단 | Stretchable display and manufacturing method thereof |
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KR101908604B1 (en) * | 2018-02-08 | 2018-10-16 | 주식회사 케이비엘러먼트 | Manufacturing method for transparent electrode panel using composite solution of CNT and graphene, and transparent electrode panel prepared by the same |
KR102198396B1 (en) * | 2019-07-24 | 2021-01-05 | 고려대학교 세종산학협력단 | Stretchable display and manufacturing method thereof |
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