KR20200095606A - Method for preparing carbon-carbon nitride complex and carbon-carbon nitride complex prepared thereby - Google Patents

Abstract

The present invention provides a method for preparing a carbon-carbon nitride complex, comprising the steps of: preparing a mixed solution by mixing glucose, melamine, cyanuric acid, and a solvent; recovering a complex precursor from the mixed solution; and firing the complex precursor. The present invention can control a shape, size, and composition of the precursor and the carbon-carbon nitride complex.

Description

Method for preparing carbon-carbon nitride complex and carbon-carbon nitride complex prepared thereby

The present invention relates to a method for producing a carbon-carbon nitride composite containing meso pores. More specifically, the present invention provides a method for producing a carbon-carbon nitride composite capable of controlling the structure of a carbon-carbon nitride composite.

Nanoporous materials are materials having a certain porous structure, and are usually composed of ordered or disordered pore structures having a size of 0.4 nm to 100 nm. According to the definition of the International Federation of Pure and Applied Chemistry (IUPAC), it can be classified into micro pores with a diameter of 2 nm or less, meso pores of 2 nm to 50 nm, and macro pores of 50 nm or more by pore size.

Nanoporous materials exhibit various properties such as molecular sieve, shape selectivity, adsorption, stability and durability due to their high specific surface area per volume, high porosity, fluid permeability, regularity and uniform pore structure. The application range of separation and sensor is very wide.

Depending on the type of nanoporous material, the size of pores, porosity, pore distribution, composition, and surface characteristics are different, so an appropriate material can be selected according to the application field. Nanoporous materials are in the spotlight as core technologies for the development of various separators, energy saving/storage/change materials, chemical/electrical active materials, and materials for information/electronics, and are recognized as important technologies of high added value.

The lithium-sulfur secondary battery is the most anticipated secondary battery as the next-generation battery of the lithium ion battery that is currently most widely used. A secondary battery largely composed of a positive electrode, a negative electrode, a separator, and an electrolyte has a positive electrode and a negative electrode positioned with a separator interposed between the electrode to prevent electrical short-circuit and physical contact. As a condition that the secondary battery must have, first, the insertion and desorption of ions in the electrode must be easy, and the structure of the electrode must be stably maintained during the charging/discharging process.

The lithium-sulfur secondary battery has a high theoretical capacity of 1672mAh/g and an energy density of 2600Wh/kg, can be easily obtained in the vicinity due to its abundant reserves, and is in the spotlight as a commercial research material because it is an eco-friendly material. However, despite numerous studies being conducted, the electrical conductivity of sulfur contained in the positive electrode active material is not good, and the lithium-sulfur secondary battery still needs improvement of cycle characteristics, such as the elution of lithium polysulfide generated after the reaction at the positive electrode. .

In particular, the lithium polysulfide intermediate generated during charging and discharging is dissolved in the organic electrolyte and eluted, or the insoluble final product (Li ₂ S) is deposited inside and on the positive electrode pores, resulting in reduction of positive electrode active material and capacity reduction. As a method to do so, it is common to use a mesoporous carbon material that has conductivity and can support expanded sulfur through a reduction reaction as a support for sulfur.

However, in order to support a large amount of sulfur, it must have a high pore volume, and for this purpose, the pore diameter of carbon must be increased to several tens of nanometers, and the pore diameter must be made small so that the polysulfide can be positioned close to the surface of the carbon support. do. The conventional method for synthesizing a carbon support having mesopores having a diameter of 2 nm to 50 nm and having a high pore volume is complicated in the synthesis process and uses harmful toxic substances for synthesis, so it is not easy for mass production.

One object of the present invention is to provide a method for producing a carbon-carbon nitride composite.

Another object of the present invention is to provide a carbon-carbon nitride composite prepared by the above manufacturing method.

One aspect of the present invention comprises the steps of preparing a mixed solution by mixing glucose, melamine, cyanuric acid and a solvent; Recovering the composite precursor from the mixed solution; It provides a method for producing a carbon-carbon nitride composite comprising; and firing the composite precursor.

In one embodiment of the present invention, the glucose may be 0.1 to 100 times the total weight of the melamine and cyanuric acid.

In one embodiment of the present invention, the solvent may include any one selected from the group consisting of THF, acetonitrile, DMSO, DMF, HMPA, and combinations thereof.

In one embodiment of the present invention, the step of preparing the mixed solution may be performed at 50°C to 150°C.

In one embodiment of the present invention, the step of recovering the complex precursor may be performed by any one method selected from the group consisting of centrifugation, filtration, evaporation, recrystallization, precipitation, and combinations thereof.

In one embodiment of the present invention, the step of recovering the composite precursor may further include washing and/or drying.

In an embodiment of the present invention, the firing of the composite precursor may be performed at 400°C to 800°C.

In one embodiment of the present invention, the firing of the composite precursor may be performed for 1 to 20 hours.

One aspect of the present invention provides a carbon-carbon nitride composite prepared by the above manufacturing method.

In one embodiment of the present invention, the carbon-carbon nitride composite may include 20% to 50% by weight of carbon based on the total weight of the carbon-carbon nitride composite.

In one embodiment of the present invention, the carbon-carbon nitride composite may include pores having a diagonal length of 2 nm to 50 nm.

In one embodiment of the present invention, the carbon-carbon nitride composite may include pores having a total volume of 0.1cm ³ /g to 3.0cm ³ /g.

In one embodiment of the present invention, the carbon-carbon nitride composite may have a spherical shape.

In the method of manufacturing a carbon-carbon nitride composite according to an embodiment of the present invention, a precursor can be easily mass-synthesized in a solution using inexpensive molecular materials. In addition, the carbon-carbon nitride complex according to an embodiment of the present invention has the advantage that the shape, size, and composition of the precursor and the carbon-carbon nitride complex can be adjusted by controlling the mass ratio of the molecular substance in the solution. .

It should be understood that the effects of the present invention are not limited to the above-described effects, and include all effects that can be deduced from the configuration of the invention described in the detailed description or claims of the present invention.

1 is a TEM (FIG. 1a)) and SEM (FIG. 1b) and c)) image showing the surface of a carbon-carbon nitride composite manufactured according to an embodiment of the present invention.
2 is a SEM image of a carbon-carbon nitride composite prepared according to an embodiment of the present invention and before and after a firing process of a comparative example.
3 is a graph showing the results of Fourier transform infrared spectroscopy (FIG. 3a) and nuclear magnetic resonance (FIG. 3b)) of a carbon-carbon nitride composite prepared according to an embodiment of the present invention.
4 is a graph showing a mass ratio according to a firing temperature of a composite precursor prepared according to an embodiment of the present invention.

Hereinafter, the present invention will be described with reference to the accompanying drawings. However, the present invention may be implemented in a number of different forms, and therefore is not limited to the embodiments described herein. In addition, parts not related to the description are omitted in the drawings to clearly describe the present invention.

Throughout the specification, when a part is said to be "connected (connected, contacted, coupled)" to another part, it is not only "directly connected", but also "indirectly connected" with another member in between. "It includes the case where it is. In addition, when a part "includes" a certain component, it means that other components may be further provided, not excluding other components unless otherwise specified.

The terms used in the present specification are only used to describe specific embodiments, and are not intended to limit the present invention.

One aspect of the present invention comprises the steps of preparing a mixed solution by mixing glucose, melamine, cyanuric acid and a solvent; Recovering the composite precursor from the mixed solution; It provides a method for producing a carbon-carbon nitride composite comprising; and firing the composite precursor.

First, the method for preparing a carbon-carbon nitride composite according to the present invention includes preparing a mixed solution by mixing glucose, melamine, cyanuric acid, and a solvent.

The step of preparing the mixed solution may be performed at 50°C to 150°C, for example 80°C to 100°C, for example 90°C. To this end, the step of preparing the mixed solution may further include heating.

If the heating step is lower than 50° C., it may not be possible to prepare a complex precursor of a desired shape, and the glucose, melamine, cyanuric acid, and solvent may not be properly mixed. Conversely, if the heating step is higher than 150° C., the reaction may be affected by exceeding the boiling point of the solvent, and a side reaction may proceed, making it impossible to obtain a desired reactant.

There is no problem before and after the addition of glucose, melamine and cyanuric acid in the step of preparing the mixed solution. Preparation of the mixed solution may include, for example, (i) heating a solution in which glucose, melamine, and a solvent are mixed, and a solution in which cyanuric acid and a solvent are mixed, respectively, followed by mixing; (ii) a method of heating a solution in which glucose, cyanuric acid and a solvent are mixed, and a solvent in which melamine and a solvent are mixed, respectively, followed by heating; Or (iii) a solution of a mixture of glucose and a solvent, a solution of a mixture of melamine and a solvent, and a solution of a mixture of cyanuric acid and a solvent, respectively, and then simultaneously mixing the three solutions.

The glucose is initially provided together with melamine and/or cyanuric acid in the step of preparing the mixed solution. Melamine and cyanuric acid form melamine cyanurate through hydrogen bonding in the mixed solution preparation step, and glucose plays a role of interfering with the hydrogen bonding of melamine cyanurate. Therefore, it is preferable that glucose is added before the hydrogen bonding between melamine and cyanuric acid begins.

In the present specification, "melamine cyanurate" refers to a product obtained by hydrogen bonding and reacting with melamine and cyanuric acid in a ratio of 1:1.

The melamine and cyanuric acid may be provided in a molar ratio of 1:2 to 2:1, for example, 1:1 based on the weight of each.

In the step of preparing the mixed solution, the glucose may be 0.1 to 100 times, for example, 1 to 50 times, for example, 10 to 20 times, based on the total weight of melamine and cyanuric acid.

The content of glucose may be a modulator capable of controlling any one selected from the group consisting of microstructure, composition, pore structure, density, and combinations thereof.

As the amount of glucose increases, the composite precursor forms microfibers having a certain size and shape, and forms and precipitates the composite precursor into spherical particles having a uniform and high density in shape and size. When the precipitated composite precursor is fired at high temperature, it is possible to induce medium-sized mesopores to withstand the volume expansion of a large amount of discharge products while the carbon nitride, which has excellent adhesion properties to carbon and sulfur, is uniformly distributed in the structure. have.

In one embodiment of the present invention, the solvent is not limited as long as it is an organic solvent that dissolves without reacting with the glucose, melamine and cyanuric acid, for example, THF, acetonitrile, DMSO, DMF, HMPA, and combinations thereof. Any one selected from the group consisting of, for example, may be DMSO.

The solvent may be included in an amount of 1 to 2 times, for example, 1.2 to 1.8 times, for example, 1.5 times, based on the weight of the glucose, melamine and cyanuric acid.

If the solvent is contained in an amount of less than 1 times the weight of glucose, melamine and cyanuric acid, solutes may be precipitated, and if it is contained more than 2 times, the amount of dissolved solutes increases, resulting in the size and shape of the complex precursor. can be changed.

In the step of preparing the mixed solution, melamine and cyanuric acid may form melamine cyanurate, which is a spherical crystal aggregate, in an organic solvent. After forming a two-dimensional network of hexagonal patterns through hydrogen bonding, the plates of these two-dimensional hexagonal patterns can become spherical particles reaching several microns through stacking and aggregation.

This directional growth can be controlled by modifying the intermolecular interactions. For example, DMSO at about 90° C. may be a hydrogen bond receptor for melamine, and may interfere with hydrogen bonding between melamine and cyanuric acid. At this time, the Van der Waals interaction between the two-dimensional networks is maintained as it is and z-axis growth occurs, which forms hexagonal microfibers.

The glucose can be introduced into a complex precursor by competitively interfering with hydrogen bonding between melamine and cyanuric acid or acting as a structural derivative by a hydrogen bonding functional group in a trans configuration outside the two-dimensional plane.

At this time, the content of glucose may be a factor capable of controlling any one selected from the group consisting of the microstructure, composition, pore structure, density, and combinations thereof of the complex precursor.

Next, the method for producing a carbon-carbon nitride composite according to the present invention includes the step of recovering the composite precursor from the mixed solution.

The step of recovering the composite precursor refers to a process of removing only the mixture by removing the solvent that has not reacted with the mixture. The step of recovering the precursor means, for example, any one process selected from the group consisting of centrifugation, filtration, evaporation, recrystallization, precipitation, and combinations thereof, and may be, for example, a filtration process, For example, it may be a vacuum filtration process.

The reduced pressure filtration process is a method of separating solids and liquids that are not mixed with each other, and is a method of reducing the pressure inside the flask and filtering by using the suction force for the filtrate generated at this time. For example, by separating the solvent from the mixed solution using vacuum filtration, the resulting solid complex precursor may be obtained.

The step of recovering the composite precursor may further include washing and/or drying. Through the washing and drying process, the yield can be increased by additionally removing the solvent remaining in the composite precursor.

Next, the method for producing a carbon-carbon nitride composite according to the present invention includes the step of firing the composite precursor.

In the present invention, "calcination" refers to carbonization by heating the composite precursor to a high temperature.

The temperature of the firing step may be 400°C to 800°C, for example 450°C to 750°C, for example 600°C. If the temperature of the firing step is less than 400°C, the material may have a molecular shape similar to that of the composite precursor, and if it exceeds 800°C, all organic substances may be decomposed into gas.

The firing step may be performed for 1 hour to 20 hours, for example 9 hours to 10 hours.

The firing may be performed under an inert gas condition, for example, nitrogen and/or argon gas conditions.

One aspect of the present invention provides a carbon-carbon nitride composite prepared by the above manufacturing method.

In the present specification, “carbon-carbon nitride complex” refers to a composite of a carbon-based material formed by carbonization of carbon nitride and glucose produced through high-temperature condensation polymerization of melamine and cyanuric acid at high temperature.

The carbon nitride contains a large amount of nitrogen atoms having an unshared electron pair, which is advantageous for adsorption of lithium polysulfide, and thus may play a role of suppressing the elution of lithium polysulfide, which is a problem in a lithium-sulfur secondary battery. . However, due to the low conductivity of 10 ^-11 S/m, carbon nitride is limited in its use as an electrode material of a battery, so it must be mixed with a conductive material to increase conductivity. For example, since glucose having the molecular formula C ₆ H ₁₂ O ₆ is carbonized to generate a carbon-based conductive material, it may be combined with the carbon nitride to supplement the electron transport ability of the carbon nitride. .

In the present specification, “polysulfide” refers to “polysulfide ion (Sx ^2-, x is 8, 6, 4 or 2)” and “lithium polysulfide (Li ₂ S _x or LiS _x ^- , x is 8, 6, 4). Or 2)”.

The carbon-carbon nitride composite may include 20% to 50% by weight, for example, 25% to 45% by weight of carbon based on the total weight.

If the contained carbon is less than 20% by weight, the sulfur utilization ability may be lowered due to low conductivity, and if it is more than 50% by weight, the adsorption capacity of lithium polysulfide may be lowered due to a low nitrogen content.

The carbon-carbon nitride composite may include pores.

The pores may carry sulfur in a lithium-sulfur secondary battery, or may serve to promote an oxidation-reduction reaction of sulfur.

Most of the lithium-sulfur secondary battery research conducted so far uses a low sulfur content (≤2mg/cm ² ), so even assuming 100% efficiency, the area capacity is about 3.35mAh/cm ² Is lower than the maximum area capacity of (about 4mAh/cm ² ).

Therefore, in order to develop a lithium-sulfur secondary battery having a high energy density, the sulfur content should be 6 mg/cm ² or more, and the mass ratio and sulfur utilization rate of the sulfur active material in the positive electrode should be maximized, and the mass of the electrolyte in the battery should be minimized. do.

In the lithium-sulfur secondary battery, cyclic S ₈ is converted into linear lithium polysulfide (Li ₂ S _x , x is 1 to 8) at the time of discharge, and at this time, it exhibits stepwise reduction behavior at a specific voltage. Therefore, when an intermediate of lithium polysulfide is formed during charging and discharging, and the intermediate is dissolved in an organic electrolyte and eluted, or when an insoluble final product (Li ₂ S) is deposited on the inside and surface of the cathode pores, the cathode active material decreases and capacity decreases. There are subsequent problems.

To solve this problem, it is a common method to use a mesoporous carbon material that has conductivity and can support expanded sulfur through a reduction reaction as a support for sulfur.

The carbon-carbon nitride composite may include pores having a diagonal length of 2 nm to 50 nm.

If the pore size is less than 2 nm, pore clogging may occur in the process of impregnating sulfur, the positive active material of lithium-sulfur secondary batteries, so that sulfur may not be uniformly supported in each pore, and the amount of sulfur supported in the pores decreases due to the limitation of pore volume Can be. In addition, if the pore size exceeds 50 nm, polysulfide, an intermediate product of the positive electrode, may be eluted during charging and discharging of the lithium-sulfur secondary battery.

The carbon-carbon nitride composite may include pores having a total volume of 0.1cm ³ /g to 3.0cm ³ /g. If the volume of the pores is less than 0.1cm ³ /g, pore clogging may occur in the process of impregnating sulfur, which is the positive electrode active material of lithium-sulfur secondary batteries, so that sulfur may not be uniformly contained in each pore. Due to this, the amount of sulfur supported in the pores may decrease. In addition, if the volume of the pores exceeds 3.0cm ³ /g, polysulfide, an intermediate product of the positive electrode, can be easily eluted during charging and discharging of the lithium-sulfur secondary battery.

In one embodiment of the present invention, the carbon-carbon nitride composite may have a shape including any one selected from the group consisting of spherical, tubular, linear, planar, and combinations thereof, for example, spherical. For example, when the carbon-carbon nitride composite has a spherical shape, it may secure a relatively high surface area compared to a tubular, linear, or planar shape, and further include the pores.

The carbon-carbon nitride composite of the present invention includes mesopores, and thus molecular sieve, shape selectivity, adsorption, stability and durability due to its high specific surface area, high porosity, fluid permeability, regularity and uniform pore structure. Has a variety of characteristics. For this reason, it can be applied to catalysts, electrical electronics, separation, sensors, and the like.

In addition, the carbon-carbon nitride composite of the present invention is capable of controlling the structure, depending on the size of pores, porosity, pore distribution, composition, and surface characteristics, various separators, energy saving/storage/change materials, chemical/electrical active materials. , It can be applied to the development of materials for information/electronics.

An aspect of the present invention provides a positive electrode active material including the carbon-carbon nitride composite and sulfur.

In the present specification, the "positive electrode active material" refers to a material forming a positive electrode of a lithium-sulfur secondary battery, and means supporting sulfur in the pores of the carbon-carbon nitride composite according to an embodiment of the present invention.

In an embodiment of the present invention, the carbon-carbon nitride composite may be included in an amount of 25% to 95% by weight, for example, 25% to 35% by weight in the positive active material.

When the carbon-carbon nitride composite is contained in an amount of less than 25% by weight, sufficient sulfur may not be supported, and volume expansion and low electrical conductivity of sulfur may be problematic during the charging and discharging process of the lithium-sulfur secondary battery. Conversely, when it is contained in an amount of more than 95% by weight, it may not function as an active material. However, it should be noted that the energy density of the lithium-sulfur secondary battery may decrease if it is contained in an amount exceeding 35% by weight.

In an embodiment of the present invention, the sulfur may be elemental sulfur (S ₈ ) or a sulfur compound having an SS bond. For _{example, Li 2 S n (n≥1)} , dissolved in the cache solrayiteu _{(catholyte) Li 2 S n (} n≥1), the organic sulfur compound (organosulfur compound) and a carbon-sulfur polymer ((C ₂ S _x ) _n , x may be any one selected from the group consisting of 2.5 to 50, n≥2), and combinations thereof, for example, sublimed sulfur.

During the reduction reaction of the lithium-sulfur secondary battery (when discharging), the oxidation number of S decreases as the SS bond is disconnected, and the oxidation number of S increases during the oxidation reaction (when charging), and an oxidation-reduction reaction in which the SS bond is formed again. To store and generate electrical energy.

In an embodiment of the present invention, the sulfur is 60% by weight based on the total weight of the positive electrode active material. It may be included in to 70% by weight.

When sulfur is contained in an amount of less than 60% by weight, the energy density of the lithium-sulfur secondary battery may decrease. Conversely, when it is contained in an amount of more than 70% by weight, the volume of sulfur expands and decreases during the charging and discharging process Electrical conductivity and the like can be a problem.

Example

Example 1. Preparation of carbon-carbon nitride composite

In one container, 0.5 g of melamine, 20.2 g of glucose, and 20 mL of a DMSO solvent were added, and 0.51 g of cyanuric acid and 10 mL of a DMSO solvent were added to another container. Each of the containers was heated in an oven at 90° C. for 24 hours, mixed, and heated in an oven at 90° C. for an additional 24 hours.

In order to remove DMSO, which is the solvent of the mixture, the mixture was filtered under reduced pressure using a vacuum pump and a cellulose filter paper (pore size: 11 μm), and the material was recovered and washed several times with ethanol to remove residual DMSO. The obtained powder was dried once more in an oven at 90° C. to obtain a carbon-carbon nitride composite precursor in powder form.

The precursor was maintained in a nitrogen atmosphere at a temperature of 30° C. for 1 hour, heated to 600° C. at 2.3° C./min, and fired for 4 hours to obtain a carbon-carbon nitride composite.

Example 2. Preparation of carbon-carbon nitride composite

In Example 1, a carbon-carbon nitride complex was obtained in the same manner as in Example 1, except that 10.1 g of glucose was added instead of 20.2 g of glucose.

Comparative Example 1. Preparation of carbon nitride

In Example 1, carbon nitride was obtained in the same manner as in Example 1, except that glucose was not added instead of adding 20.2 g of glucose.

Experimental Example 1. Observation of the surface of the carbon-carbon nitride composite

In order to observe the surface of the carbon-carbon nitride composite, the carbon-carbon nitride composite prepared in Example 1 was observed with a scanning electron microscope (SEM) and a transmission electron microscope (TEM) (FIG. 1). The carbon-carbon nitride complex precursors prepared in Example 1, Example 2, and Comparative Example 1, and the carbon-carbon nitride complex/carbon nitride were observed with a scanning electron microscope (SEM) (FIG. 2).

As a result of observation, the carbon-carbon nitride composite precursor and the carbon-carbon nitride composite have a shape close to a spherical shape, and the carbon-carbon nitride composite prepared according to Example 1 is carbon prepared according to Example 2. It was found that the carbon nitride composite was more spherical than the carbon nitride of Comparative Example 1, and thus, as the amount of glucose initially added increased, it was found to have a shape close to the spherical shape. In addition, it was confirmed that the composite had large mesopores of about 40 nm and a pore volume of 1.96 cm ³ /g.

Experimental Example 2. Elemental analysis of carbon-carbon nitride complex

In order to determine the constituent elements of the carbon-carbon nitride composite, the carbon-carbon nitride composites prepared in Examples 1, 2 and Comparative Example 1 were subjected to mass spectrometry, and the carbon prepared in Example 1- The carbon nitride complex was analyzed by Fourier transform infrared spectroscopy (FT-IR) and nuclear magnetic resonance (NMR).

As a result of the experiment, it was confirmed that the carbon nitride of Comparative Example 1 had about 29% by weight of carbon, whereas the carbon-carbon nitride composite of Example 1 had about 41% by weight of carbon, and the initial addition It was confirmed that the carbon content of the resulting carbon-carbon nitride complex increased as the glucose content increased.

Table 1 below shows the results of mass spectrometry.

In addition, according to Fourier transform infrared spectroscopy and nuclear magnetic resonance analysis, it was confirmed that glucose and melamine cyanurate proceeded independently. It was found that glucose forms amorphous carbon through polyaromatic condensation, and melamine cyanurate forms carbon nitrides having tri-s-triazine as a basic structure, respectively (FIG. 3):

Example Carbon (C) content (% by weight) Nitrogen (N) content (% by weight) Example 1 41.81 42.50 Example 2 33.96 51.91 Comparative Example 1 29.40 50.27

Experimental Example 3. BET specific surface area analysis of carbon-carbon nitride composite

In order to analyze the specific surface area of the carbon-carbon nitride composite, the volume of the monomolecular layer when nitrogen gas is physically adsorbed on the surface of the carbon-carbon nitride composites prepared according to Examples 1, 2, and Comparative Example 1. The surface area was calculated using Equation 1 below:

[Equation 1]

A=V _m (N _a )(A _m )/V ₀

(In the above formula, A is the surface area of the adsorbent, V _m is the gas volume required for adsorption of the monolayer, V ₀ is the molar volume of the adsorption gas, N _a is the number of Avogadro, and A _m is the cross-sectional area of the gas molecule.)

The experimental results are shown in Table 2 below.

As a result of the experiment, it was found that the surface area and pore volume of the resulting carbon-carbon nitride complex increased as the initially added glucose content increased:

Example 1 Example 2 Comparative Example 1 Surface area (m ² /g) 316 303 126 Pore volume (cm ³ /g) 2.0 0.7 0.2

Experimental Example 4. Thermal mass spectrometry of carbon-carbon nitride composite

Thermal mass spectrometry was performed using a Thermogravimetric Analysis (TGA) analyzer to determine an appropriate temperature for firing the precursor of the carbon-carbon nitride composite: N ₂ condition, 10° C./min.

As a result of the experiment, it was confirmed that the precursor of the carbon-carbon nitride complex was converted into the carbon-carbon nitride complex at about 400°C (FIG. 4).

The above description of the present invention is for illustration only, and those skilled in the art to which the present invention pertains can understand that the present invention can be easily modified into other specific forms without changing the technical spirit or essential features of the present invention. will be. Therefore, it should be understood that the embodiments described above are illustrative and non-limiting in all respects.

The scope of the present invention is indicated by the following claims, and all modifications or variations derived from the meaning and scope of the claims and their equivalent concepts should be interpreted to be included in the scope of the present invention.

Claims (13)

Preparing a mixed solution by mixing glucose, melamine, cyanuric acid, and a solvent;
Recovering the composite precursor from the mixed solution; And
Firing the composite precursor;
A method for producing a carbon-carbon nitride composite comprising a. The method of claim 1,
The method for producing a carbon-carbon nitride composite, characterized in that the glucose is provided in an amount of 0.1 to 100 times based on the total weight of the melamine and cyanuric acid. The method of claim 1,
The solvent is THF, acetonitrile, DMSO, DMF, HMPA, and a method for producing a carbon-carbon nitride composite comprising any one selected from the group consisting of a combination thereof. The method of claim 1,
The manufacturing method of the carbon-carbon nitride composite, characterized in that the step of preparing the mixed solution is carried out at 50 ℃ to 150 ℃. The method of claim 1,
The step of recovering the composite precursor is performed by any one method selected from the group consisting of centrifugation, filtration, evaporation, recrystallization, precipitation, and combinations thereof. The method of claim 1,
The step of recovering the composite precursor further comprises washing and/or drying a process for producing a carbon-carbon nitride composite. The method of claim 1,
The step of firing the composite precursor is a method of producing a carbon-carbon nitride composite, characterized in that carried out at 400 ℃ to 800 ℃. The method of claim 1,
The step of firing the composite precursor is a method of producing a carbon-carbon nitride composite, characterized in that performed for 1 to 20 hours. A carbon-carbon nitride composite prepared by the manufacturing method according to any one of claims 1 to 8. The method of claim 9,
The carbon-carbon nitride composite is a carbon-carbon nitride composite, characterized in that it contains 20% to 50% by weight of carbon based on the total weight of the carbon-carbon nitride composite. The method of claim 9,
The carbon-carbon nitride composite is a carbon-carbon nitride composite, characterized in that it comprises pores having a diagonal length of 2 nm to 50 nm. The method of claim 9,
The carbon-carbon nitride composite is a carbon-carbon nitride composite, characterized in that it comprises pores having a total volume of 0.1cm ³ /g to 3.0cm ³ /g. The method of claim 9,
The carbon-carbon nitride composite, characterized in that the spherical carbon-carbon nitride composite.

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