KR20200106374A - Carbon-containing materials obtained from spent coffee ground, method for manufacturing the same and use of the same - Google Patents

Abstract

The present invention relates to a carbon-containing material obtained from spent coffee grounds, a method for preparing the same and a use thereof. The present invention provides a carbon-containing material obtained from spent coffee grounds, in which the carbon-containing material is selected from high-purity graphene, carbon nanotube and respective derivatives thereof. In addition, the present invention provides a method for preparing a carbon-containing material, comprising: a first process for preparing spent coffee grounds; a second process for generating a carbon body from the spent coffee grounds prepared in the first process; and a third process for reacting the carbon body generated from the second process with a decomposing agent. The decomposing agent exhibits selective decomposition reactivity depending on the type of the carbon body, and includes at least one selected from an enzyme and a microorganism. According to the present invention, an industrially useful component is separated from spent coffee grounds and synthesized, and thus the recyclability of spent coffee grounds is increased, and the spent coffee grounds are transformed into a high value-added material, thereby enabling the generation of new profits. Further, spent coffee grounds may be widely recycled into a useful resource for various purposes and fields.

Description

Carbon-containing material obtained from coffee grounds, its manufacturing method and uses {CARBON-CONTAINING MATERIALS OBTAINED FROM SPENT COFFEE GROUND, METHOD FOR MANUFACTURING THE SAME AND USE OF THE SAME}

The present invention relates to a carbon-containing material obtained from coffee grounds (Spent Coffee Ground), a manufacturing method and use thereof, and in more detail, graphene or carbon nanoparticles obtained by separating/synthesizing coffee grounds through a specific treatment. Carbon-containing material such as a tube (carbon nanotube) and its use, a method for producing a carbon-containing material capable of producing the carbon-containing material with high yield and high purity, and a composite containing the carbon-containing material and its use Etc.

Coffee grounds (Spent Coffee Ground) is a solid residue generated in the coffee industry, which is mainly generated from coffee beans in the manufacturing process of espresso or water-soluble coffee. As coffee consumption increases, coffee grounds are also generated. According to the International Coffee Organization (ICO), about 550 to 670 kg of coffee grounds are generated from one ton of coffee beans, and more than 5.8 million tons of coffee grounds are reported every year.

Coffee grounds have been disposed of by landfill or incineration like general industrial waste, but recently, as interest in coffee grounds increases, recyclability as an industrial resource has been proposed. Recycling of coffee grounds has technical significance in terms of environmental, industrial and economical aspects in that it reduces waste emission and utilizes it as a useful resource, and such coffee grounds recycling technology has been proposed in patent literature or papers.

For example, Korean Patent Publication No. 10-1247146 and Korean Patent Publication No. 10-2013-0019820 disclose a deodorant using coffee grounds, and Korean Patent Publication No. 10-1621268 and Korean Registered Patent In Publication No. 10-1876555, etc., solid fuel using coffee grounds is proposed. In addition, Korean Patent Laid-Open Publication No. 10-2017-0094591 and the like have proposed a mushroom cultivation system using coffee grounds, and Korean Patent Publication No. 10-1257214 and the like disclose functional pulp using coffee grounds.

However, the recycling of coffee grounds according to the prior art as described above is, in most cases, recycling as a bulking agent. Recycling as a bulking agent is limited in the use of coffee grounds. Specifically, in the conventional recycling of coffee grounds, the collected coffee grounds are simply dried and pulverized and used without performing separate chemical treatment or extraction and separation. Accordingly, recycling of coffee grounds according to the prior art is a deodorant or solid fuel, and its application is limited to some products, and most of the coffee grounds are being disposed of.

Coffee grounds contain industrially useful ingredients, but contain harmful ingredients such as soil and livestock. Therefore, in recycling coffee grounds, there is a need for a method that first examines/analyzes components of coffee grounds, separates and synthesizes industrially useful components, and can be effectively used for various purposes.

Meanwhile, carbon bodies such as graphene and carbon nanotubes (CNT) are used in various industrial fields. Graphene has a plate-shaped two-dimensional structure in which carbon atoms are connected in a hexagonal shape, and carbon nanotubes (CNTs) have a tube-shaped carbon connection structure. These carbon bodies have electrical, thermal, and optical properties, and the application range thereof is wide. For example, graphene is attracting attention as a semiconductor material that can replace silicon in the future because it is structurally and chemically stable and has higher carrier mobility than silicon. In addition, graphene is excellent in transparency and conductivity, so it is very useful as an electric device such as an electrode for a display device or an electrode for a solar cell.

Conventionally, in manufacturing carbon bodies such as graphene as described above, in most cases, a hydrocarbon-based gas such as acetylene (C ₂ H ₂ ) or ethylene (C ₂ H ₄ ) is used as a raw material for chemical vapor deposition (CVD; Chemical Vapor). It is manufactured by growing it through deposition). For example, Japanese Laid-Open Patent No. JP2017-095327 and Japanese Laid-Open Patent No. JP2017-171570 disclose technologies related to the above. However, such a conventional manufacturing method has a high cost of raw materials such as acetylene (C ₂ H ₂ ) or ethylene (C ₂ H ₄ ), and requires expensive deposition equipment, at least in economical efficiency.

Korean Patent Publication No. 10-1247146 Korean Patent Application Publication No. 10-2013-0019820 Korean Patent Publication No. 10-1621268 Korean Patent Publication No. 10-1876555 Korean Patent Application Publication No. 10-2017-0094591 Korean Patent Publication No. 10-1257214 Japanese Patent Application Publication No. JP2017-095327 Japanese Patent Application Publication No. JP2017-171570

Accordingly, the present invention is to improve the recyclability of coffee grounds by separating and synthesizing industrially useful components from coffee grounds through a specific treatment, and converting it into a high value-added material to solve the environmental problems caused by the disposal of coffee grounds. There is a purpose.

Specifically, the present invention provides a carbon-containing material obtained by separating and synthesizing it from coffee grounds, and its industrial use, a manufacturing method capable of preparing the carbon-containing material by separating the carbon-containing material from coffee grounds in high yield and high purity, and the carbon-containing material It is an object to provide a composite comprising a and a use thereof.

In order to achieve the above object, the present invention provides a carbon-containing material obtained from coffee grounds. The carbon-containing material includes at least one selected from graphene, graphene allotropes, graphene derivatives, carbon nanotubes, carbon nanotube derivatives, and aromatic hydrocarbons.

In addition, the present invention,

A first step of preparing coffee grounds;

A second step of generating a carbon body from the coffee grounds prepared in the first step; And

It provides a method for producing a carbon-containing material from coffee grounds, including a third step of reacting the carbon body produced in the second step with a decomposing agent.

According to one embodiment, the second process,

A first step of mixing the coffee grounds with silicon dioxide (SiO ₂ ) and then heat-treating in an inert atmosphere; And

And washing the coffee grounds heat treated in the first step with hydrofluoric acid (HF) and then performing heat treatment in an inert atmosphere.

In addition, the decomposing agent in the third step has a selective decomposition reactivity according to the type of carbon body, and it may include at least one selected from enzymes and microorganisms.

Additionally, the present invention provides a composite comprising the carbon-containing material and plastic. In addition, the present invention provides the use of the carbon-containing material and composite.

According to the present invention, industrially useful components are separated and synthesized from coffee grounds through a specific treatment, so that the recyclability of coffee grounds is improved and it is converted into a high value-added material, thereby generating new profits.

In addition, according to the present invention, coffee grounds are not limited to use, and can be widely recycled as a useful resource for various uses and fields.

1 is a photograph of a synthesized carbon body according to an embodiment of the present invention.
2 is an SEM and TEM image of a carbon body synthesized according to an embodiment of the present invention.
3 is a photograph showing a state in which graphene oxide is decomposed by myeloperoxidase (MPO) according to an embodiment of the present invention.
4 is a SEM image showing a state in which graphene oxide is decomposed over time by myeloperoxidase (MPO) according to an embodiment of the present invention.

The term "and/or" used in the present invention is used to mean including at least one or more of the elements listed before and after. The term "one or more" used in the present invention means one or two or more pluralities.

According to a first aspect, the present invention provides a carbon-containing material obtained from Spent Coffee Ground. According to a second aspect, the present invention provides a method for producing a carbon-containing material capable of producing the carbon-containing material from coffee grounds with high purity and/or high yield. The present invention, according to a third aspect, provides a separation method capable of separating industrially useful components from coffee grounds with high purity and/or high yield. According to a fourth aspect, the present invention provides a composite comprising the carbon-containing material. According to a fifth aspect, the present invention provides a method for producing the composite. The present invention provides, according to a sixth aspect, the use of the carbon-containing material. Further, according to the seventh aspect, the present invention provides the use of the composite.

[1] substances containing carbon

The carbon-containing material according to the present invention is derived from coffee grounds (Spent Coffee Ground), which is not particularly limited as long as it contains at least a carbon (C) atom. The carbon-containing substance includes, for example, a carbon body and/or a hydrocarbon compound.

In the present invention, the "carbon body" has a crystal structure of a carbon (C) atom, which is, for example, graphene, carbon nanotubes (CNTs), carbon nanofibers (CNF; carbon nanofibers), allotropes thereof, and derivatives thereof. Specifically, the carbon body obtained from coffee grounds according to the present invention is graphene, graphene allotropes, graphene derivatives, carbon nanotubes (CNT), carbon nanotubes (CNT) derivatives, carbon nanofibers (CNF) and carbon nanofibers. It may be a composite containing one or two or more selected from (CNF) derivatives and the like. In addition, the carbon body has a size (thickness) of a nanometer, and includes a carbon nanosheet of the above carbon material and a porous mass of the carbon nanosheet.

The carbon body is as well known. For example, the graphene has a plate-shaped two-dimensional structure in which carbon atoms are connected in a hexagonal shape, which may include a single layer or 10 or less layers of graphene.

Examples of the graphene allotrope include graphene, graphite, and fullerene. In this case, the graphite is a structure in which graphene having a two-dimensional structure is stacked, and this may include 10 or more layers of graphene. The fullerene includes carbon rings in which carbon atoms are arranged and connected in a pentagonal or hexagonal shape, and these carbon rings are combined to have a hollow hollow shape (eg, a soccer ball shape). The graphene derivatives include oxidized graphene, reduced graphene, graphene nanoribbons, fluorographene, porous graphene, and graphdiyne. ) And the like.

In addition, the carbon nanotube (CNT) includes a single-walled carbon nanotube (SWCNT; Single-Walled carbon nanotube) and/or a multi-walled carbon nanotube (MWCNT; Multi-Walled carbon nanotube). The carbon nanotube (CNT) derivative is a carbon nanotube (CNT) to which an organic substance is bonded or functionalized with an organic substance, which is, for example, a carbon nanotube functionalized with polyethylene glycol (PEG) (SWCNT-PEG). ; SWCNT functionalized with PEG), carbon nanotubes functionalized with aminoanthracene (SWCNT functionalized with aminoanthracene), carbon nanotubes functionalized with polyethylene glycol (PEG) and aminoanthracene (SWCNT functionalized with PEG and aminoanthracene), Carbon nanotubes functionalized with aminofluorene (SWCNT functionalized with aminofluorene), and/or carbon nanotubes functionalized with polyethylene glycol (PEG) and aminofluorene (SWCNT functionalized with PEG and aminofluorene), etc. I can.

In the present invention, the "hydrocarbon compound" contains an aromatic and/or aliphatic hydrocarbon. The hydrocarbon compound includes an aromatic hydrocarbon produced by decomposition of the carbon body according to one embodiment. The aromatic hydrocarbon is not particularly limited as long as it has at least one benzene ring in the molecule, and specific examples thereof are 2-methoxy naphthalene, 2-naphthol, and cinnamic aldehyde. And one or more selected from isophthalic acid.

The carbon-containing material according to the present invention is included here if it is obtained from coffee grounds. Specifically, the carbon-containing material uses coffee grounds as a raw material, but is obtained through processes such as extraction and separation of coffee grounds, chemical treatment, heat treatment, enzyme decomposition and/or microbial decomposition according to the present invention. It is selected from carbon bodies (graphene, etc.) and hydrocarbon compounds (aromatics, etc.) depending on progress and/or process conditions. Hereinafter, specific embodiments of the carbon-containing material will be described while explaining the manufacturing method according to the present invention.

[2] preparation of carbon-containing substances

The method for producing a carbon-containing material according to the present invention uses coffee grounds as a raw material, and includes a synthesis process of generating a carbon body from the coffee grounds. The carbon body produced through this synthesis process is as described above as graphene, carbon nanotubes (CNT) and/or derivatives thereof. In addition, the method for producing a carbon-containing material according to the present invention is performed before or after the synthesis process is performed, and drying, grinding, washing, extraction, chemical treatment, heat treatment, enzyme It may further include one or more selected from processes such as decomposition, microbial decomposition, separation and purification.

According to one embodiment, a method for producing a carbon-containing material according to the present invention comprises: a first step of preparing coffee grounds; A second step of synthesizing a carbon body from the coffee grounds prepared in the first step; And a third step of reacting the carbon body obtained in the second step with a decomposing agent. In addition, the method for producing a carbon-containing material according to the present invention may further include a fourth process of separating and purifying a target product (carbon-containing material) in addition to the above processes. Each process is described as follows.

(1) Preparation of coffee grounds (the first step)

Coffee grounds can be used by collecting solid residues generated in the coffee industry, for example, after extracting soluble solids from coffee beans through water, hot water and/or steam. In addition, the collected coffee grounds can be used after drying or grinding to an appropriate size.

According to one embodiment, the first step may include a step of washing the collected coffee grounds using an acid solution or an alkali solution. Impurities or ash components contained in coffee grounds can be removed by this cleaning process. And after washing, it can be used after drying and/or grinding.

(2) Synthesis of carbon body (second step)

Carbon bodies are produced from the prepared coffee grounds. This second process for this is a first step of mixing the coffee grounds with silicon dioxide (SiO ₂ ) and then heat-treating in an inert atmosphere according to one embodiment, and the coffee grounds heat treated in the first step with hydrofluoric acid ( HF) and then heat treatment in an inert atmosphere. Through this second process, a carbon precursor contained in coffee grounds is synthesized into a carbon body such as graphene. In addition, the carbon body synthesized through the second process may have porosity in some cases.

In the first step, for example, after obtaining a SiO ₂ dispersion in which silicon dioxide (SiO ₂ ) is dispersed in a solvent, coffee grounds powder is added and mixed in the SiO ₂ dispersion, and then heat treated at a temperature of 800° C. or higher in an inert atmosphere. It can be done in a way. In this case, the inert atmosphere may be, for example, a gas atmosphere such as argon (Ar) and/or nitrogen (N ₂ ). The heat treatment may be performed for 1 hour to 5 hours at a temperature of 800 to 1,200°C, for example.

In the second step, for example, after washing by impregnating in a hydrofluoric acid (HF) solution, in an inert atmosphere such as argon (Ar) and/or nitrogen (N ₂ ) gas, at a temperature of 800 to 1,200°C for 1 hour It can be carried out by a method of heat treatment for 5 hours. SiO ₂ and ash components are removed by the hydrofluoric acid (HF) cleaning and heat treatment in the second step, so that a high-purity carbon body may be produced.

Attached Figure 1 is a photograph of each specimen according to an exemplary embodiment of the present invention, showing a photograph of heat treatment by putting coffee grounds in a SiO ₂ dispersion, and a photograph after performing hydrofluoric acid (HF) cleaning and heat treatment. And the accompanying Figure 2 shows the SEM and TEM images of the carbon body synthesized according to an exemplary embodiment of the present invention.

According to another embodiment of the present invention, the second process comprises the steps of: (a) obtaining an extract obtained by solvent-extracting the coffee grounds; (b) heat-treating the extract obtained in step (a); (c) mixing the extract heat-treated in step (b) with silicon dioxide (SiO ₂ ) and then heat-treating in an inert atmosphere; And (d) washing the extract heat-treated in step (c) with hydrofluoric acid (HF) and then performing heat treatment in an inert atmosphere.

The step (a) may be performed using water, an organic solvent, and/or a mixture thereof as an extraction solvent. This solvent extraction may be performed at room temperature or warm conditions. In the step (b), the extract may be separated and recovered through filtration after solvent extraction, and the recovered extract may be heat-treated at, for example, 80° C. or higher.

Steps (c) and (d) are the same as the first and second steps described above. Specifically, in step (c), the extract after step (b) is added to the SiO ₂ dispersion and mixed, and then in an inert atmosphere (Ar, N _2, etc.) at a temperature of 800 to 1,200° C. for 1 hour to 5 hours. During the heat treatment process, the step (d) is washed by impregnating the extract subjected to step (c) in a hydrofluoric acid (HF) solution, and then 800 to 1,200 in an inert atmosphere (Ar, N _2, etc.). It can be carried out by a method of heat treatment for 1 hour to 5 hours at a temperature of ℃. When performing steps (a) to (b) as described above, a high-purity carbon body can be produced in a high yield.

In addition, in the second step, as a component contained in the coffee grounds, it is preferable to synthesize one or more carbon precursors selected from compounds represented by the following formulas A and B as a carbon body. That is, the carbon-containing material according to the present invention may be obtained by synthesizing one or more carbon precursors selected from compounds represented by the following formulas A and B among components contained in coffee grounds. In the present invention, "synthesis" means that a component (carbon precursor) contained in coffee grounds is formed into carbon bodies such as graphene and carbon nanotubes (CNT) by the second process.

[Formula A]

[Formula B]

In Formula A, Ra and Rb are the same as or different from each other, and Ra and Rb are each H, OH, an aliphatic hydrocarbon, an aromatic hydrocarbon or OCOR ¹ (where R ¹ is an aliphatic hydrocarbon or an aromatic hydrocarbon). In addition, R ₁ , R ₂ and R ₃ in Formula B are the same as or different from each other, and R ₁ , R ₂ and R ₃ are each H, OH, aliphatic hydrocarbon, aromatic hydrocarbon, CHO or COOH. According to the present invention, the compounds of Formulas A and B act as carbon precursors useful in the synthesis of carbon bodies. Such a carbon precursor may include one or more selected from compounds represented by the following Chemical Formulas 1 to 5, for example.

[Formula 1]

[Formula 2]

[Formula 3]

[Formula 4]

[Formula 5]

The compounds (carbon precursors) represented by Chemical Formulas 1 to 5 may be synthesized as high-quality carbon bodies. Specifically, the compounds (carbon precursors) represented by Chemical Formulas 1 to 5 are advantageous in the production of graphene and carbon nanotubes (CNTs) having excellent electrical, thermal and optical properties, etc., which are also highly pure and high-yield carbon Sieve can be created.

(3) Decomposition reaction (third step)

Next, the carbon body produced in the second step is reacted with a decomposition agent. The carbon body generated through the second process may include a plurality of carbon bodies of two or more different types. Specifically, the carbon bodies obtained in the second step are two or more selected from graphene, graphene allotropes, graphene derivatives, carbon nanotubes (CNT) and carbon nanotubes (CNT) derivatives, and different carbon bodies are used. It can be included in plural.

In the third step, a decomposition agent is added and mixed with the above-described carbon bodies to react. At this time, in the third step, the plurality of carbon bodies are reacted so that at least one carbon body is selectively decomposed. To this end, the decomposing agent is used that has a selective decomposition reactivity according to the type of carbon body, and specifically, one or more selected from enzymes and microorganisms may be used.

In the present invention, "selective decomposition reactivity" is one that has a selective decomposition reactivity for a specific carbon body, for example, among carbon bodies, carbon nanotubes (CNT) are not decomposed, but graphene can be decomposed. it means. As a desired product (carbon-containing material) through such a selective decomposition reaction, for example, graphene, carbon nanotubes (CNT), or decomposition products thereof can be obtained. To this end, an enzyme and/or a microorganism is used as the decomposing agent, but the type of enzyme and/or microorganism may be differently used depending on the desired product (carbon-containing material).

As the enzyme, according to one embodiment, an enzyme having a selective decomposition reactivity in the presence of hydrogen peroxide (H ₂ O ₂ ) may be used. Such enzymes are, for example, myeloperoxidase (MPO), manganese peroxidase (MnP; manganese peroxidase), horseradish peroxidase (HRP) and/or lactoperoxidase. It may be selected from peroxidase enzymes such as LPO; lactoperoxidase. These peroxidase enzymes have a selective decomposition reactivity for specific carbon bodies depending on their type.

According to a specific embodiment, the third process may include a step of reacting in the presence of hydrogen peroxide (H ₂ O ₂ ) and a reaction catalyst using the above peroxidase enzyme as a decomposing agent. In this case, the reaction catalyst may be selected from a compound having at least one selected from a halogen group (X = -Cl, -Br, etc.), a cyanide group (-CN) and a thiocyanide group (-SCN). Such a reaction catalyst is selected from, for example, sodium chloride (NaCl), potassium bromide (KBr), potassium cyanide (KCN), potassium ferrocyanide (K ₄ Fe (CN) ₆ ) and/or potassium thiocyanide (KSCN). Can be.

In one example, myeloperoxidase (MPO) is used as the decomposing agent and reacted with hydrogen peroxide (H ₂ O ₂ ) in the presence of a reaction catalyst, but a halogen compound (X = Cl) is used as the reaction catalyst. When reacted, a halogen compound (X = Cl) and hydrogen peroxide (H ₂ O ₂ ) react with the myeloperoxidase (MPO) to generate HOCl, and the HOCl is a graphene oxide as a graphene derivative. Effectively decompose

3 is a photo (left) of dispersing graphene oxide obtained according to an exemplary embodiment of the present invention in a solvent, and a photo after reaction by adding myeloperoxidase (MPO) thereto (right). to be. And, the attached Figure 4 is a SEM image showing the decomposition result according to the time course (A: initial, B: 15 hours, C: 24 hours after) after the addition of myeloperoxidase (MPO). First, as shown in FIG. 3, it was found that the solution became clear by the addition of myeloperoxidase (MPO), and as shown in FIG. 4, it gradually decomposed as time passed, and after 24 hours It could be seen that the graphene oxide completely disappeared.

In addition, the microorganisms include bacteria and/or fungi, which are, for example, Pseudomonas sp . ), the genus Vibrio sp . ), Mycobacterium sp . , Marinobacter sp . , and Sphingomonas sp . ) And the like, selected from Naphthalene-degrading bacteria. These naphthalene-degrading bacteria have selective decomposition reactivity to graphene and derivatives thereof.

The microorganisms are for example Burkholderia curryensis ( Burkholderia kururiensis), Delph Tia foot lance ash (Delftia acidovorans), Pomona to Stephen's notes malto pilriah (Stenotrophomonas maltophilia ), Trabusiella guamensis guamensis ), Sparassis Latifolia latifolia ) and Trametes versicola ( Trametes versicolor ) and the like, and for another example, white-rot fungi such as Phanerochaete chrysosporium may be used. These microorganisms have selective decomposition reactivity to single-walled carbon nanotubes (SWCNT), multi-walled carbon nanotubes (MWCNT), graphene derivatives, and the like according to each type.

[Table 1] below shows the species of microorganisms having selective decomposition reactivity according to the type of carbon body.

<Microorganisms with selective decomposition reaction according to the type of carbon body> Carbon body Microbes Taxonomy Species of microorganism GRA and its derivatives (GO, graphite, RGO, etc.) Group 1
(Bacteria) Naphthalene-degrading bacteria: Pseudomonas , Vibrio , Mycobacterium , Marinobacter, Sphingomonas, etc. MWCNT Group 2
(Bacteria) Burkholderia kururiensis, Delftia acidovorans, Stenotrophomonas maltophilia , Trabusiella guamensis, etc. SWCNT Group 3
(Fungi) Sparassis latifolia, Trametes versicolor, etc. SWCNT, graphene derivatives (GRA nanoribbon, etc.) Group 4
(Fungi) White-rot fungi: Phanerochaete chrysosporium, etc.
* GRA: Graphene
* GO: Graphene oxide
* RGO: Reduced graphene
* SWCNT: Single-walled carbon nanotube
* MWCNT: Multi-walled carbon nanotube

As illustrated in [Table 1], the microorganism has a selective decomposition reactivity with respect to a specific carbon body according to its type. Accordingly, in the third step, the type of microorganism is changed according to the desired carbon body to undergo decomposition reaction.

Referring to [Table 1], for example, in the case of using a multi-walled carbon nanotube (MWCNT) as a target carbon body, the carbon body obtained in the second step is reacted with a microorganism, but the microorganism is a naphthalene of the first group. -React by selecting and using Naphthalene-degrading bacteria and the fourth group of white-rot fungi. At this time, graphene, single-walled carbon nanotubes (SWCNTs) and derivatives thereof are decomposed by the selective decomposition reactivity of the first group and the fourth group microorganisms. That is, graphene and its derivatives are decomposed by microorganisms of the first group, and single-walled carbon nanotubes (SWCNTs) and graphene derivatives are decomposed by microorganisms of the fourth group. Accordingly, most of the carbon bodies remaining after the reaction are multi-walled carbon nanotubes (MWCNTs), and high purity and high yield multi-walled carbon nanotubes (MWCNTs) can be obtained through the selective decomposition reactivity of microorganisms.

In addition, for another example, when graphene is used as a target carbon body, the carbon body obtained in the second step is reacted with a decomposing agent, but the decomposing agent may be a microorganism and an enzyme. Specifically, first, the microorganisms of the second group and the fourth group in [Table 1] are used as microorganisms to react. And the myeloperoxidase (MPO) is used as an enzyme, but reacted in the presence of hydrogen peroxide (H ₂ O ₂ ). At this time, multi-walled carbon nanotubes (MWCNT) are decomposed by microorganisms of the second group, and single-walled carbon nanotubes (SWCNTs) and graphene derivatives are decomposed by microorganisms of the fourth group. In addition, graphene oxide is decomposed by the myeloperoxidase (MPO). Accordingly, most of the carbon bodies remaining after the reaction are graphene, and graphene of high purity and high yield can be obtained through the selective decomposition reactivity of microorganisms and enzymes.

As described above, the carbon body obtained through the third process is obtained through the selective decomposition reactivity of microorganisms and/or enzymes, which is high-purity graphene, carbon nanotubes (CNT), or derivatives thereof. The carbon body obtained through the third process is graphene or carbon nanotubes (CNT) in one example.

Further, in the third step, a hydrocarbon compound is produced by the decomposition reaction. At this time, most of the hydrocarbon compounds include aromatic hydrocarbons produced by decomposition of the carbon body. Specifically, in the third process, graphene, carbon nanotubes (CNTs) and derivatives thereof are decomposed by the decomposing agent (microorganisms and/or enzymes) to produce, for example, 2-methoxy naphthalene (2 Decomposition products such as -methoxy naphthalene), 2-naphthol, cinnamaldehyde and/or isophthalic acid are produced. Additionally, the decomposition products may include CO ₂ and the like.

(4) Separation (4th step)

This fourth step is an optional step, and through the fourth step, the desired final product (carbon-containing material) can be separated and recovered with high purity. This fourth process (separation process) may be performed after the second process is performed, or after the third process is performed. For example, after the second step is performed, the carbon body may be recovered through the fourth step. In addition, after the third step is performed, a specific carbon body (graphene or CNT) and aromatic hydrocarbon having high purity may be recovered through the fourth step.

The fourth process can be carried out in various ways depending on the final product (carbon-containing material). This fourth step is not particularly limited as long as it can be recovered by separating and purifying carbon bodies (graphene, etc.) and/or hydrocarbon compounds (aromatic hydrocarbons, etc.) as the desired final product in high purity. This fourth process is a physical and/or chemical method, and may include, for example, a membrane separation method, an adsorption method, an absorption method, a separation method using a difference in boiling point, a cooling separation method, and/or a separation method through acid or alkali treatment. Is not limited by.

[3] complex

The composite according to the present invention comprises at least the above carbon-containing material. The composite according to the present invention specifically includes a first material and a second material, wherein the first material is obtained from coffee grounds according to the present invention, and the carbon body (graphene and CNT, etc.) and/or a hydrocarbon compound It includes a carbon-containing material selected from (aromatic hydrocarbons, etc.). The second material is not particularly limited, but it may be selected from plastic and/or ceramic. According to one embodiment, the composite according to the invention is a mixture comprising a carbon-containing material (first material) and a plastic (second material), which may be liquid or solid. In this case, the solid may be a powder type, a granular type and/or a pellet type.

The plastic is a material that can be heated and/or pressurized, and includes a resin. The resin includes natural resins and synthetic resins. The plastic may be selected according to the purpose and use of the composite, and may be selected from, for example, bioplastic and/or engineering plastic. The bioplastic is biodegradable and may be selected from polylactic acid (PLA) and/or polycaprolactone (PCL), for example.

[4] Use

The carbon-containing material and composite according to the present invention can be used in various industrial fields and uses, and their application fields and uses are not particularly limited. The carbon-containing material and composite according to the present invention can be widely used in the energy field, the electronic field, the precision machine field, the high temperature machine field, the medicine field, the food field, the cosmetics field, and the wastewater treatment field.

The carbon body (graphene, CNT, etc.) and the composite containing the same, for example, electrode material for energy storage device, 3D printer material, electronic device material, semiconductor material, sensor material, filter material, surgical medical tool material and It can be used as a container material for food storage. In addition, the hydrocarbon compound (aromatic hydrocarbon, etc.) and a composite containing the same may be used as, for example, pharmaceuticals, pharmaceuticals, cosmetics, elastic materials, shielding materials, antibacterial materials and sensor materials.

Claims (16)

A first step of preparing coffee grounds;
A second step of generating a carbon body from the coffee grounds prepared in the first step; And
And a third step of reacting the carbon body produced in the second step with a decomposing agent.
The method of claim 1,
The second step,
A first step of mixing the coffee grounds with silicon dioxide (SiO ₂ ) and then heat-treating in an inert atmosphere; And
And cleaning the coffee grounds heat treated in the first step with hydrofluoric acid (HF) and then performing heat treatment in an inert atmosphere.
The method of claim 1,
The second step,
(a) obtaining an extract obtained by solvent-extracting the coffee grounds;
(b) heat-treating the extract obtained in step (a);
(c) mixing the extract heat treated in step (b) with silicon dioxide (SiO ₂ ) and then heat-treating in an inert atmosphere; And
(d) washing the extract heat treated in step (c) with hydrofluoric acid (HF) and then heat-treating in an inert atmosphere. A method for producing a carbon-containing material from coffee grounds.
The method of claim 1,
The carbon body obtained in the second process includes a plurality of carbon bodies selected from graphene, graphene allotrope, graphene derivative, carbon nanotube and carbon nanotube derivative,
The third step is a method of producing a carbon-containing material from coffee grounds, characterized in that the reaction is performed so that at least one carbon body is selectively decomposed from among the plurality of carbon bodies.
The method of claim 1,
The method of producing a carbon-containing material from coffee grounds, characterized in that the decomposition agent has a selective decomposition reactivity according to the type of carbon body.
The method of claim 1,
The method of producing a carbon-containing material from coffee grounds, characterized in that the decomposition agent is at least one selected from enzymes and microorganisms.
The method of claim 1,
The method for producing a carbon-containing material from coffee grounds, characterized in that the disintegrant includes a peroxidase enzyme.
The method of claim 7,
The third step is a method for producing a carbon-containing material, characterized in that it comprises the step of reacting a carbon body with a peroxidase enzyme, and reacting with hydrogen peroxide (H ₂ O ₂ ) in the presence of a reaction catalyst.
The method of claim 8,
The reaction catalyst is a method for producing a carbon-containing material, characterized in that it comprises a compound having at least one selected from a halogen group, a cyanide group and a thiocyanide group.
The method of claim 1,
In the second step, as a component contained in the coffee grounds, at least one carbon precursor selected from the compounds represented by the following formulas A and B is synthesized as a carbon body, a method for producing a carbon-containing material from coffee grounds.
[Formula A]

[Formula B]

(In Formula A, Ra and Rb are the same as or different from each other, and Ra and Rb are each H, OH, aliphatic hydrocarbon, aromatic hydrocarbon, or OCOR ¹ (where R ¹ is an aliphatic hydrocarbon or aromatic hydrocarbon); in Formula B R ₁ , R ₂ and R ₃ are the same as or different from each other, and R ₁ , R ₂ and R ₃ are each H, OH, aliphatic hydrocarbon, aromatic hydrocarbon, CHO or COOH.)
It is a carbon-containing material produced by the method according to claim 1,
The carbon-containing material is a carbon-containing material obtained from coffee grounds, characterized in that it contains at least one selected from graphene, graphene allotropes, graphene derivatives, carbon nanotubes, carbon nanotube derivatives, and aromatic hydrocarbons.
The method of claim 11,
The aromatic hydrocarbon is a carbon-containing material obtained from coffee grounds, characterized in that one or more selected from graphene, graphene allotropes, graphene derivatives, carbon nanotubes and carbon nanotube derivatives are decomposed.
The method of claim 11,
The aromatic hydrocarbon is coffee grounds, characterized in that it contains at least one selected from 2-methoxy naphthalene, 2-naphthol, cinnamaldehyde, and isophthalic acid Carbon-containing material obtained from.
A carbon-containing material, characterized in that obtained by synthesizing at least one carbon precursor selected from compounds represented by the following formulas A and B among the components contained in the coffee grounds.
[Formula A]

[Formula B]

(In Formula A, Ra and Rb are the same as or different from each other, and Ra and Rb are each H, OH, aliphatic hydrocarbon, aromatic hydrocarbon, or OCOR ¹ (where R ¹ is an aliphatic hydrocarbon or aromatic hydrocarbon); in Formula B R ₁ , R ₂ and R ₃ are the same as or different from each other, and R ₁ , R ₂ and R ₃ are each H, OH, aliphatic hydrocarbon, aromatic hydrocarbon, CHO or COOH.)
The method of claim 13,
The carbon-containing material is a carbon-containing material obtained from coffee grounds, characterized in that it comprises at least one selected from graphene, graphene allotropes, graphene derivatives, carbon nanotubes and carbon nanotube derivatives.
A composite comprising the carbon-containing material according to any one of claims 11 to 15.

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