KR20170015742A - Method of manufacturing non-oxidized graphene using shear flow exfoliation and electrochemical pretreatment and apparatus for manufacturing the same - Google Patents
Method of manufacturing non-oxidized graphene using shear flow exfoliation and electrochemical pretreatment and apparatus for manufacturing the same Download PDFInfo
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- KR20170015742A KR20170015742A KR1020150108551A KR20150108551A KR20170015742A KR 20170015742 A KR20170015742 A KR 20170015742A KR 1020150108551 A KR1020150108551 A KR 1020150108551A KR 20150108551 A KR20150108551 A KR 20150108551A KR 20170015742 A KR20170015742 A KR 20170015742A
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Abstract
Description
The present invention relates to a graphene manufacturing method, and more particularly, to a non-oxidized graphene manufacturing method using electrochemical pretreatment and shear flow separation.
The present invention also relates to a manufacturing apparatus suitable for achieving the graphene manufacturing method.
Graphene is generally defined as a carbon monolayer of a hexagonal crystal structure with a two-dimensional planar structure.
Graphene is a carbon material expected to be applied to various fields such as semiconductors and displays because it has advantages of showing excellent electric conductivity, thermal conductivity and mechanical strength compared to conventional carbon materials.
Such graphene is manufactured in various ways.
1 schematically shows a method for producing graphene using an oxidation / reduction method.
Referring to FIG. 1, a method of manufacturing graphene using an oxidation / reduction method includes the steps of forming graphite oxide by oxidizing graphite, peeling the graphene oxide to obtain graphene oxide, To produce graphene.
In the case of the graphene production method using the oxidation / reduction method, it is possible to produce graphene in a large quantity using low-cost graphite as a raw material, and it has an advantage that a solution process using a graphene dispersion can be performed. However, in this method, since carbon crystals are destroyed during the oxidation of graphite, there are many chemical and structural defects in the graphene produced, resulting in poor graphene performance.
Fig. 2 schematically shows a method for producing graphene by directly peeling graphite using ultrasonic waves.
Referring to FIG. 2, in the method of manufacturing graphene using ultrasound, graphene is directly stripped in a solvent to which ultrasonic waves are applied to produce graphene. This method does not involve an oxidation / reduction step, so that graphene having few defects can be produced, and excellent electrical characteristics can be secured. However, in this method, there is a disadvantage in that the production rate of graphene is low due to the limitation of the peeling efficiency of the graphite. In addition, there are limitations in this method because it is difficult to continuously mass-produce graphene due to the technical limitations of ultrasonic equipment.
As another method of producing graphene, there is a method of synthesizing graphene at a high temperature by using chemical vapor deposition (CVD) or the like. This method has an advantage that graphene can be directly formed on a substrate, but there is a disadvantage that it is expensive to manufacture graphene according to a high temperature process.
As a background art related to the present invention, Korean Patent Laid-Open Publication No. 10-2011-0077606 (published on Jul. 07, 2011) discloses that graphene is prepared by adding graphite to 1-propanol followed by ultrasonic degradation Method is disclosed.
It is an object of the present invention to provide a method of producing non-oxidized graphene using electrochemical pretreatment and shear flow separation.
Another object of the present invention is to provide a graphene manufacturing apparatus that can be applied to the graphene manufacturing method.
According to another aspect of the present invention, there is provided a method of manufacturing a graphene, comprising: electrochemically pretreating a graphite material to lower an interlayer coupling force; Injecting an electrochemically pretreated graphite material into the reaction space of a shear flow reactor in which a solvent is stored in a reaction space; And rotating the fluid into which the graphite-based material is injected to produce graphene by peeling the graphite-based material with a shear force generated by the rotational flow of the fluid.
In this case, the electrochemical pretreatment step may include: a pre-treatment reactor including a working electrode including a graphite-based material, a conductive counter electrode, and an electrolyte in which the working electrode and the counter electrode are immersed, And applying a voltage to the gate electrode.
In addition, the electrolyte may include at least one of an aqueous electrolyte, an organic solvent-based electrolyte, and an ionic liquid electrolyte.
In addition, the working electrode may include a graphite rod, a graphite plate, or a three-dimensional sponge type CVD graphite.
The shear flow reactor may include an inner body extending in a horizontal direction and a cylindrical outer body surrounding the inner body in a state spaced apart from the inner body and forming a reaction space in the inner body.
Further, the rotation speed of the inner body can be adjusted to 100 rpm or more.
In addition, the solvent may include at least one of N-methyl-2-pyrrolidinone (NMP) and N, N-dimethylformamide (DMF).
The fluid may include one or more of NaC (sodium cholate) poly vinyl alcohol (PVA), poly vinyl pyrrolidone (PVP), polystyrenesulfonate (PSS), dodecylbenzene sulfonic acid (DBSA) And may further include a dispersant.
According to an aspect of the present invention, there is provided a graphene manufacturing apparatus including: a pretreatment reactor for electrochemically pretreating a graphite material to lower interlayer coupling force; And a shear flow reactor for separating the electrochemically pretreated graphite-based material from the pre-treatment reactor by a shear force generated by rotational flow of the fluid to produce graphene, A body portion including a cylindrical outer body surrounding the inner body and spaced apart from the inner body to form a reaction space therein; and an electrochemical pretreatment unit disposed on one side of the cylindrical outer body, A discharge port formed at the other side of the cylindrical outer body for discharging graphene obtained by separating graphite by a shear force generated by rotational flow of a fluid stored in the reaction space, And a driving unit for rotating the inner body.
At this time, the pretreatment reactor may include a working electrode including a graphite-based material, a conductive counter electrode, and an electrolyte in which the working counter electrode and the conductive counter electrode are immersed.
According to the method for producing graphene according to the present invention, the graphite can be effectively stripped by using the shear flow of the fluid, and the graphene can be continuously and mass-produced.
In addition, in the case of the graphene production method according to the present invention, high-quality non-oxidized graphene can be produced without oxidation / reduction.
1 schematically shows a method for producing graphene using an oxidation / reduction method.
2 schematically shows a method of manufacturing graphene using ultrasonic waves.
FIG. 3 schematically shows a method of manufacturing graphene using electrochemical pretreatment and shear flow separation according to the present invention.
4 is a perspective view schematically showing an example of a shear flow reactor applicable to the graphene manufacturing method according to the present invention.
5 is a cross-sectional view schematically showing an example of a shear flow reactor applicable to the graphene manufacturing method according to the present invention.
6 is a schematic view of a graphene manufacturing apparatus according to an embodiment of the present invention.
Figure 7 schematically shows an example of an electrochemical pretreatment reactor.
Figure 8 schematically illustrates the process by which graphene is produced from a graphite-based material when applying the method according to the present invention.
BRIEF DESCRIPTION OF THE DRAWINGS The advantages and features of the present invention, and how to accomplish them, will become apparent with reference to the embodiments and drawings described in detail below. However, it is to be understood that the present invention is not limited to the disclosed embodiments, but may be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. It is intended that the disclosure of the present invention be limited only by the terms of the appended claims.
Hereinafter, a method and apparatus for producing non-oxidized graphene using electrochemical pretreatment and shear flow separation according to the present invention will be described in detail with reference to the accompanying drawings.
FIG. 3 schematically shows a method of manufacturing graphene using electrochemical pretreatment and shear flow separation according to the present invention.
Referring to FIG. 3, the method for producing graphene according to the present invention uses electrochemical pretreatment and shear flow. More specifically, in the present invention, the interlayer coupling force of the graphite material is lowered through electrochemical pretreatment, and then the graphite material is peeled off through shear flow separation to produce graphene.
In the step of using the electrochemical pretreatment of the present invention, by applying a voltage difference between the working electrode and the conductive counter electrode in the electrochemical pretreatment reactor, the ionic substance contained in the electrolyte is permeated into the working electrode, that is, between each graphene layer of the graphite material do. Referring to FIG. 8, when an ionic material penetrates between each graphene layer of the graphite material as shown in FIG. 8 (a), the ionic material contributes to lowering the interlayer coupling force between the graphene layers, (b), the interlayer bonding force between the graphene layers is lowered, and at the same time, the graphite pieces are separated from the matrix. Thereafter, the separated graphite pieces are put into a shear flow reactor, and the graphene completely peeled as shown in Fig. 8 (c) is produced in the shear flow reactor.
The pretreatment reactor includes a working electrode including a graphite-based material, a conductive counter electrode, and an electrolyte in which the working electrode and the conductive counter electrode are immersed, examples of which are shown in Fig.
The working
The
The electrolyte may include at least one of an aqueous electrolyte, an organic solvent-based electrolyte, and an ionic liquid electrolyte. Aqueous electrolyte is sulfuric acid (H 2 SO 4), phosphoric acid (H 3 PO4), polystyrene sulfonic acid (poly (styrenesulfonate); PSS) an acid (acid), such that acid aqueous solution dissolved in water electrolyte, ammonium sulfate ((NH 4 ) 2 SO 4), sodium sulfate (Na 2 SO 4), potassium sulphate (K 2 SO 4) as and the like, an inorganic salt such that the aqueous solution electrolyte dissolved in water, an organic solvent-based electrolyte is a tetraethylammonium tetrafluoroborate There is an organic solvent electrolyte in which a salt of tetraethylammonium tetrafluoroborate (TEABF4) is dissolved in a solvent of acetonitrile or propylene carbonate. As the ionic liquid electrolyte, an alkylimidazolium ionic liquid, an alkylpyrrolidinium There is an ionic liquid.
In the step of applying the shear flow of the present invention, the fluid is rotated to form a Taylor fluid flow, and the graphite material is peeled off by a shear force generated by the rotational flow of the fluid to produce graphene . At this time, the shear force applied to the graphite-based material should be sufficient to overcome the strong Van der Waals attractive force between each graphene layer of the graphite. This is because the rotational speed of the reactor, , Increase of fluid temperature, and addition of additives (dispersant, etc.).
In order to produce graphene using shear flow, a shear flow reactor as in the example shown in Figs. 4 and 5 is used in the present invention.
Referring to FIGS. 4 and 5, the reactor using the Taylor fluid includes an
The length of the shear flow reactor can be from about 10 cm to 1 m, and the volume of the reaction space can be from about 10 mL to about 10L. However, the length of the shear flow reactor and the volume of the reaction space are not necessarily limited thereto.
The Taylor fluid flow of the present invention means that the outer cylinder is fixed and when the inner cylinder rotates, the fluid flows in the direction of rotation of the inner cylinder, and a force flows in the direction of the outer cylinder from the inner cylinder side by centrifugal force. This is the vortex of a high-pitched array that rotates in opposite directions regularly along the axial direction as the fluid becomes unstable as the rotational speed of the inner cylinder increases. The Taylor fluid flow can be formed according to the rotational speed of the fluid, the radius and the distance of the inner body and the outer body, the viscosity of the fluid, and the shear flow force is greatly increased as the Taylor fluid is formed.
That is, the present invention is characterized in that a graphite material electrochemically pretreated is injected into a fluid containing a solvent, which is stored in a
6, the graphite-based material may be injected from one side of the cylindrical
The solvent contained in the fluid may include at least one of NMP (N-methyl-2-pyrrolidinone) and DMF (N, N-dimethylformamide). In the case of these NMP and DMF, there is a characteristic of having surface energy similar to graphene.
Further, the fluid may further include a dispersant to improve the peeling efficiency of the graphite-based material. The dispersing agent may include at least one of NaC (sodium cholate) poly vinyl alcohol (PVA), polyvinyl pyrrolidone (PVP), polystyrenesulfonate (PSS), dodecylbenzene sulfonic acid (DBSA) and ionic liquid.
On the other hand, as a method of further improving the fluidity of the fluid, there is a method of controlling the rotation speed of the
6 is a schematic view of a graphene manufacturing apparatus according to an embodiment of the present invention.
Referring to FIG. 6, the apparatus for producing graphene according to the present invention includes an
For the continuous process, the
In addition, when a plurality of electrochemical pretreatment reactors are arranged, the productivity can be further improved. The discharge ports of the electrochemical pretreatment reactor may be connected to one inlet of the shear flow reactor, and the inlet ports of the shear flow reactor may be separately disposed at the discharge ports of the electrochemical pretreatment reactor. The electrochemical pretreatment reaction can be carried out simultaneously in all the reactors. If necessary, the reaction proceeds in some pre-treatment reactors and may be in a standstill state in other pre-treatment reactors, and the working electrode of the pre- If the material is exhausted, the pretreatment reaction may proceed in other pretreatment reactors.
The reactor includes a horizontally extending
The
The
The discharged product can be separated by centrifugation or the like into graphene and other graphite materials, solvents or the like having a layer number of less than about 10 layers, that is, 1 to 9 layers. When 10 layers are to be determined as graphene, 10 or more layers of graphite-based materials, solvents and the like can be introduced into the reactor through the
The driving
In addition, a
The
The
As described above, according to the method of manufacturing graphene according to the present invention, graphite can be effectively stripped by electrochemical pretreatment and shear flow separation, and graphene can be continuously and mass-produced.
Further, in the case of the graphene production method according to the present invention, it is possible to produce non-oxidized graphene by direct peeling of graphite without accompanying oxidation / reduction, And is an environmentally friendly way.
The produced graphene can be utilized in various fields such as electrode materials for energy storage devices such as conductive graphene ink and supercapacitor for manufacturing printed electronic devices, and heat dissipation and composite materials.
While the present invention has been described in connection with what is presently considered to be practical exemplary embodiments, it is to be understood that the invention is not limited to the disclosed embodiments, but, on the contrary, It is to be understood that the invention may be embodied in other specific forms without departing from the spirit or essential characteristics thereof. It is therefore to be understood that the above-described embodiments are illustrative in all aspects and not restrictive.
405: rotating shaft 410: inner body
420: Cylindrical outer body 430: Reaction space
601: Inlet port 602: Outlet port
605: Electrochemical Pretreatment Reactor
620: heater 630: support
710: working electrode (graphite material)
720: counter electrode 730: electrolyte
Claims (10)
Injecting an electrochemically pretreated graphite material into the reaction space of a shear flow reactor in which a solvent is stored in a reaction space; And
And rotating the fluid into which the graphite-based material is injected to produce graphene by peeling the graphite-based material with a shear force generated by rotational flow of the fluid.
Wherein the electrochemical pretreatment step comprises the steps of: applying a voltage difference between the working electrode and the conductive counter electrode in a pretreatment reactor including a working electrode containing a graphite-based material, a conductive counter electrode, and an electrolyte in which the working electrode and the counter electrode are immersed Wherein the graphening step is carried out by applying a graphene to the graphene.
Wherein the electrolyte comprises at least one of an aqueous electrolyte, an organic solvent-based electrolyte, and an ionic liquid electrolyte.
Wherein the working electrode comprises a graphite rod, a graphite plate, or a three-dimensional sponge-like CVD graphite.
The shear flow reactor
An inner body extending in a horizontal direction,
And a cylindrical outer body surrounding the inner body and spaced apart from the inner body to form a reaction space therein.
Wherein the rotational speed of the inner body is adjusted to 100 rpm or more.
Wherein the solvent comprises at least one of NMP (N-methyl-2-pyrrolidinone) and DMF (N, N-dimethylformamide).
The fluid may be a dispersant comprising at least one of NaC (sodium cholate) poly vinyl alcohol (PVA), poly vinyl pyrrolidone (PVP), polystyrenesulfonate (PSS), dodecylbenzene sulfonic acid (DBSA) ≪ / RTI >
And a shear flow reactor for producing graphene by stripping the electrochemically pretreated graphite material in the pre-treatment reactor with a shear force generated by the rotational flow of the fluid,
Wherein the shear flow reactor comprises:
A body portion including an inner body extending in a horizontal direction and a cylindrical outer body surrounding the inner body and forming a reaction space inside the inner body while being spaced apart from the inner body;
An input port formed on one side of the cylindrical outer body for inputting electrochemically pretreated graphite material,
A discharge port formed on the other side of the cylindrical outer body for discharging graphene obtained by separating graphite by a shear force generated by rotational flow of a fluid stored in the reaction space;
And a driving unit for rotating the inner body.
The pre-
A working electrode including a graphite-based material,
A conductive counter electrode,
And an electrolyte in which the working electrode and the conductive counter electrode are immersed.
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CN107601479A (en) * | 2017-10-16 | 2018-01-19 | 合肥工业大学 | Graphene prepared by the preparation method and this method of a kind of graphene |
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CN107601479A (en) * | 2017-10-16 | 2018-01-19 | 合肥工业大学 | Graphene prepared by the preparation method and this method of a kind of graphene |
WO2021096094A1 (en) * | 2019-11-15 | 2021-05-20 | 주식회사 엘지에너지솔루션 | Method for producing graphene nanosheets |
KR102221095B1 (en) * | 2020-01-22 | 2021-02-26 | 주식회사 케이비엘러먼트 | Manufacturing method of graphene-filler composite thermally conductive material and graphene-filler composite thermally conductive material manu factured by the same |
KR20210112144A (en) | 2020-03-04 | 2021-09-14 | (주)투디엠 | Apparatus for exfoliation of 2-dimensional material |
KR102361553B1 (en) * | 2020-11-18 | 2022-02-14 | 주식회사 케이비엘러먼트 | Manufacturing method of graphene coated inorganic particle and graphene coated inorganic manufactured by the same |
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