KR101636195B1 - Method of fabricating composite comprising copper oxide and magnesium oxide - Google Patents

Abstract

Provided is a preparation method of a composite comprising copper oxide and magnesium oxide. The preparation method may comprise the following steps of: preparing copper oxide by mixing and refluxing a solution containing copper and a basic solution; preparing magnesium oxide by mixing and refluxing a solution containing magnesium and a base solution; and preparing complex of the copper oxide and the magnesium oxide by providing an acidic solvent to the copper oxide and the magnesium oxide.

Description

BACKGROUND OF THE INVENTION 1. Field of the Invention [0001] The present invention relates to a method for producing a composite of copper oxide and magnesium oxide,

The present invention relates to a method for producing a composite of copper oxide and magnesium oxide, and more particularly to a method for producing a composite of copper oxide and magnesium oxide by mixing and refluxing copper oxide and magnesium oxide.

The photocatalyst means a catalyst that acts to decompose pollutants around the center by receiving a light energy and causing a redox reaction. In other words, the photocatalyst means a substance that promotes a chemical reaction by using incident light.

In general, metal oxides are widely used as photocatalysts. Typically, for example, there is titanium dioxide (TiO ₂ ). The photocatalytic effect of titanium dioxide is superior to other photocatalysts, it is relatively inexpensive, has excellent durability, and is highly toxic and highly toxic. Therefore, it does not cause pollution even after disposal. Is also widely used.

In order to improve the photocatalytic effect of titanium dioxide, for example, Korean Patent Laid-Open Publication No. 10-2013-0070327 (Application No. 10-2011-0137590, applicant: Seoul National University Industry & University Collaboration Team) A titanium dioxide precursor, titanium chloride, is added to the graphene solution to prepare a grafted oxide sheet in which titanium dioxide is bonded in the form of a nanorod, and the grafted sheet is dried and then heat-treated to prepare a graft sheet bonded with the titanium dioxide nanorod Lt; / RTI >

In order for titanium dioxide to exhibit the photocatalytic effect, UV light should be irradiated for a relatively long time. In order to solve such problems, it is necessary to research and develop a method for producing a composite having excellent photocatalytic effect by using various metal oxides.

Korean Patent Publication No. 10-2013-0070327

SUMMARY OF THE INVENTION It is an object of the present invention to provide a process for producing a composite of copper oxide and magnesium oxide, which is excellent in photocatalytic effect.

Another technical problem to be solved by the present invention is to provide a method for manufacturing a composite of copper oxide and magnesium oxide with a simplified manufacturing process.

Another technical problem to be solved by the present invention is to provide a method for manufacturing a composite of copper oxide and magnesium oxide with reduced manufacturing costs.

The problems to be solved by the present invention are not limited to those described above.

In order to solve the above technical problems, the present invention provides a method for producing a composite of copper oxide and magnesium oxide.

According to one embodiment, the method of producing the composite comprises mixing and refluxing a solution containing copper and a basic solution to produce copper oxide, mixing and mixing the magnesium-containing solution and the basic solution, Reflux to produce a magnesium oxide, and providing an acidic solvent to the copper oxide and the magnesium oxide to produce a composite of the copper oxide and the magnesium oxide.

According to one embodiment, the copper oxide and the magnesium oxide may comprise a flower shape.

According to one embodiment, the basic solution may include at least one of an ammonia aqueous solution (NH ₄ OH), an aqueous sodium hydroxide solution (NaOH), or an aqueous potassium hydroxide solution (KOH).

According to one embodiment, the method of manufacturing the composite may further include sintering the composite.

According to one embodiment, the step of preparing the composite of copper oxide and magnesium oxide comprises the steps of: preparing the mixed solution by providing the acidic solvent to the copper oxide and the magnesium oxide; diluting and stirring the mixed solution; , And drying the mixed solution.

According to one embodiment, the weight ratio of the magnesium oxide to the weight of the copper oxide may be greater than 2 in the mixed solution.

According to one embodiment, the mixed solution may include diluted with deionized water.

According to one embodiment, the acidic solvent may comprise a HNO ₃ solution.

According to an embodiment of the present invention, the basic aqueous solution includes an aqueous ammonia solution, and the step of preparing the copper oxide comprises reacting copper ions contained in the solution containing copper with ammonia contained in the aqueous ammonia solution, Ammonia composite is prepared and the copper-ammonia composite is reacted with a hydroxyl group contained in the aqueous ammonia solution to produce the copper oxide, wherein the copper oxide is self-organized in the form of a flower .

According to one embodiment, the step of preparing the copper-ammonia composite is performed at room temperature, and the step of preparing the copper oxide is performed at a reflux temperature of the solution containing the copper and the aqueous ammonia solution .

According to one embodiment, the composite may comprise a flower shape.

In order to solve the above technical problem, the present invention provides a photocatalyst.

According to one embodiment, the photocatalyst may comprise a composite prepared according to the above described embodiments.

According to an embodiment of the present invention, a copper oxide and a magnesium oxide are produced by a reflux process using a basic solution, and the copper oxide and the magnesium oxide are provided with an acidic solvent so that a composite of the copper oxide and the magnesium oxide is produced . This can provide a method for producing a composite of copper oxide and magnesium oxide, which has excellent photocatalytic effect, simplifies the manufacturing process, and has a reduced manufacturing cost.

1 is a flowchart illustrating a method of manufacturing a composite of copper oxide and magnesium oxide according to an embodiment of the present invention.
2 is a flowchart illustrating a method of manufacturing copper oxide used in a method of manufacturing a composite according to an embodiment of the present invention.
3 is a SEM photograph illustrating a flower shape of copper oxide produced using NH ₄ OH according to an embodiment of the present invention.
4 is a SEM photograph illustrating a flower shape of copper oxide produced using KOH and NaOH according to an embodiment of the present invention.
5 is a SEM photograph illustrating a flower shape of magnesium oxide according to an embodiment of the present invention.
FIG. 6 is a SEM photograph illustrating a flower shape of a composite of copper oxide and magnesium oxide according to an embodiment of the present invention.
7 is a graph of XRD results of a composite of copper oxide and magnesium oxide according to an embodiment of the present invention.
8 is a graph showing methyl orange decomposition results of a composite of copper oxide and magnesium oxide according to an embodiment of the present invention.
9 is a graph showing methylene blue decomposition results of a composite of copper oxide and magnesium oxide according to an embodiment of the present invention.

Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the accompanying drawings. However, the technical spirit of the present invention is not limited to the embodiments described herein but may be embodied in other forms. Rather, the embodiments disclosed herein are provided so that the disclosure can be thorough and complete, and will fully convey the scope of the invention to those skilled in the art.

Further, in the drawings, the thicknesses of the films and regions are exaggerated for an effective explanation of the technical content. Also, while the terms first, second, third, etc. in the various embodiments of the present disclosure are used to describe various components, these components should not be limited by these terms. These terms have only been used to distinguish one component from another. Thus, what is referred to as a first component in any one embodiment may be referred to as a second component in another embodiment. Each embodiment described and exemplified herein also includes its complementary embodiment. Also, in this specification, 'and / or' are used to include at least one of the front and rear components.

The singular forms "a", "an", and "the" include plural referents unless the context clearly dictates otherwise. It is also to be understood that the terms such as " comprises "or" having "are intended to specify the presence of stated features, integers, Should not be understood to exclude the presence or addition of one or more other elements, elements, or combinations thereof.

In the following description of the present invention, a detailed description of known functions and configurations incorporated herein will be omitted when it may make the subject matter of the present invention rather unclear.

Also, in this specification, a flower shape refers to a shape in which a plurality of flat or curved films are randomly or regularly aggregated to form a flower-like shape . The components described herein having a flower shape include the meaning that they have a nano or micro sized flower shape.

FIG. 1 is a flow chart for explaining a method of manufacturing a composite of copper oxide and magnesium oxide according to an embodiment of the present invention, and FIG. 2 is a view illustrating a method of manufacturing copper oxide used in a method of manufacturing a composite according to an embodiment of the present invention. Fig.

Referring to FIG. 1, a copper oxide may be prepared by mixing and refluxing a solution containing copper and a basic solution (S110). The copper oxide may be in a flower shape. A method of producing the copper oxide will be described in detail with reference to FIG.

Referring to FIG. 2, a solution containing the copper is prepared (S210). According to one embodiment, the solution containing copper may be an aqueous solution of copper nitrate (Cu (NO) _{3 3} H ₂ O). The solution containing copper is dissolved in deionized water and stirred until homogeneous blue light appears.

According to one embodiment, the basic solution may be an ammonia aqueous solution (NH ₄ OH), an aqueous sodium hydroxide solution (NaOH), or an aqueous potassium hydroxide solution (KOH And the like. The solution containing copper and the basic solution can be sufficiently stirred at room temperature.

The copper oxide may be prepared by refluxing the copper-containing solution and the basic solution (S230). For example, the copper-containing solution and the basic solution can be refluxed at 100 ° C for 12 hours. The copper contained in the solution containing copper may react with the basic solution and self-organize in a flower form.

Specifically, for example, when the basic solution is an aqueous ammonia solution, at a normal temperature, copper ions contained in the solution containing copper react with ammonia contained in the aqueous ammonia solution as shown in the following formula (1) , A copper-ammonia composite and water can be prepared.

≪ Formula 1 >

Cu ²⁺ + 4NH ₃ H ₂ O -> [Cu (NH ₃ ) ₄ ] ²⁺ + 4H ₂ O

The copper-ammonia composite reacts with the hydroxyl group contained in the aqueous ammonia solution at the reaction temperature condition in which the reflux is carried out to produce the copper oxide with high reactivity and surface energy Thus, the copper oxide can be self-organizing in the form of a flower.

(2)

[Cu (NH ₃ ) ₄ ] ²⁺ + OH ^- -> CuO + 4NH ₄ OH

According to this embodiment of the present invention, as described above, the solution containing copper and the basic solution are sufficiently stirred at room temperature to perform the reflux after the copper-ammonia composite is prepared. Thus, from the copper-ammonia composite, the copper oxide in flower form can be easily produced by the reflux process.

The copper oxide may be recovered and cleaned (S240). According to one embodiment, the copper oxide may be precipitated and then recovered using a centrifuge. Thereafter, the copper oxide may be washed with a cleaning solution (e.g., methanol). After the copper oxide is recovered and washed, it can be dried.

1, a method of manufacturing a composite of copper oxide and magnesium oxide according to an embodiment of the present invention will be described.

Referring to FIG. 1, magnesium oxide may be prepared by mixing and refluxing a solution containing magnesium and the basic solution (S120). The magnesium oxide may be a flower shape. The magnesium oxide may be prepared using the basic solution used for the production of the copper oxide. In other words, the basic solution may include at least one of an ammonia aqueous solution (NH ₄ OH), an aqueous sodium hydroxide solution (NaOH), or an aqueous potassium hydroxide solution (KOH).

The step of preparing the magnesium oxide may be substantially the same as the step of producing the copper oxide, except that the solution containing the magnesium is used instead of using the solution containing the copper. Thus, the manufacturing apparatus and the source solutions used for the production of the copper oxide can be used as they are, so that the manufacturing process can be simplified and the manufacturing cost can be reduced.

Specifically, the step of preparing the magnesium oxide may include preparing a solution containing magnesium, mixing the basic solution with the magnesium-containing solution, mixing the magnesium-containing solution and the basic solution with a ripple The magnesium oxide may be prepared by a process comprising the steps of: preparing a magnesium oxide; According to one embodiment, the solution containing magnesium may be an aqueous magnesium sulfate solution (MgSO ₄ 7H ₂ O).

In the embodiment of the present invention described above, it is described that the magnesium oxide is manufactured after the copper oxide is manufactured. However, the manufacturing step of the copper oxide and the magnesium oxide manufacturing step are not limited in order. In other words, after the magnesium oxide is produced, the copper oxide may be prepared, or the magnesium oxide and the copper oxide may be simultaneously produced.

After the copper oxide and the magnesium oxide are prepared, a composite of the copper oxide and the magnesium oxide may be prepared (S130) by providing an acidic solvent to the copper oxide and the magnesium oxide. According to one embodiment, the acidic solvent may be nitric acid (HNO ₃ ). The composite of the copper oxide and the magnesium oxide may be in the form of a flower.

Wherein the step of preparing the composite of copper oxide and magnesium oxide comprises the steps of: preparing the mixed solution by providing the acidic solvent to the copper oxide and the magnesium oxide; diluting and stirring the mixed solution; And drying the solution.

According to an embodiment of the present invention, after the copper oxide and the magnesium oxide are produced, the composite may be produced. Accordingly, the ratio of the copper oxide and the magnesium oxide in the composite can be adjusted. Therefore, the ratio of the copper oxide and the magnesium oxide can be adjusted according to the use of the composite, so that the characteristics of the composite can be adaptively adjusted.

According to one embodiment, the weight ratio of the magnesium oxide to the weight of the copper oxide may be greater than 2 in the mixed solution. As a result, the photocatalytic properties of the mixture can be improved.

According to one embodiment, the mixed solution may be diluted with deionized water, then stirred, and dried. After the mixed solution is dried and the composite recovered, the composite can be sintered.

Hereinafter, the evaluation results of properties of the composite of copper oxide and magnesium oxide produced according to the above-described method of producing the composite of the present invention will be described.

Manufacture of Copper Oxide

3 is a SEM photograph illustrating a flower shape of copper oxide produced using NH ₄ OH according to an embodiment of the present invention.

Referring to FIG. 3, 0.1 M of Cu (NO) _{3 3} H ₂ O was prepared as a solution containing copper. Cu (NO) _{3 3} H ₂ O was dissolved in 100 ml of deionized water and stirred until homogeneous blue light was observed. Then, NH ₄ OH of 5M was prepared as a basic solution, NH ₄ OH was added, and reflux was performed at 100 ° C for 12 hours to prepare copper oxide.

After completion of the reaction, the reaction mixture was spontaneously warmed to room temperature, and the copper oxide was recovered using a centrifugal separator. The recovered copper oxide was washed with methanol and dried at 100 DEG C for 2 hours.

As shown in FIG. 3, it can be confirmed that the copper oxide having a flower shape was produced using NH ₄ OH and Cu (NO) _{3 3} H ₂ O.

4 is a SEM photograph illustrating a flower shape of copper oxide produced using KOH and NaOH according to an embodiment of the present invention.

Referring to FIG. 4, copper oxide was prepared using KOH and NaOH in addition to NH ₄ OH under the same conditions as described above, and then SEM photographs of copper oxide were taken. 4 (a) is a SEM image of copper oxide prepared using a KOH solution, and (b) of FIG. 4 is a SEM image of copper oxide prepared using NaOH. As can be seen from FIG. 4, it can be confirmed that a flower-like copper oxide can be easily produced using a basic solution.

Manufacture of Magnesium Oxide

5 is a SEM photograph illustrating a flower shape of magnesium oxide according to an embodiment of the present invention.

Referring to FIG. 5, 0.1 M MgSO ₄ 7H ₂ O was prepared as a solution containing magnesium. MgSO ₄ 7H ₂ O was dissolved in 100 ml of deionized water. Thereafter, as a basic solution, 0.5 M NH ₄ OH was prepared, NH ₄ OH was added, and refluxed at 100 ° C for 12 hours to prepare magnesium oxide.

After the reaction was completed, the magnesium oxide was washed with deionized water and dried at 120 DEG C for 1 hour. Thereafter, the magnesium oxide was calcined at 400 ° C for 2 hours.

As can be seen from FIG. 5, it was confirmed that the magnesium oxide having a flower shape was produced using MgSO ₄ 7H ₂ O and NH ₄ OH.

Preparation of a composite of copper oxide and magnesium oxide

FIG. 6 is a SEM photograph illustrating a flower shape of a composite of copper oxide and magnesium oxide according to an embodiment of the present invention.

Referring to FIG. 6, a composite of copper oxide and magnesium oxide was prepared using the copper oxide and the magnesium oxide prepared by the above-described method.

Specifically, according to the first to fourth embodiments of the present invention, 0.125 g, 0.25 g, 0.5 g, and 0.75 g of magnesium oxide were mixed in 5 ml of deionized water, respectively, with 0.25 g of copper oxide, .

Thereafter, 0.1 ml of HNO3 was added to the mixed solutions, and the mixture was diluted with 45 ml of deionized water, stirred for 12 hours and dried to obtain a mixture according to the first to fourth embodiments in which the proportions of copper oxide and magnesium oxide were different As shown in Table 1 below.

division Amount of magnesium oxide First Embodiment 0.125 g Second Embodiment 0.25 g Third Embodiment 0.5 g Fourth Embodiment 0.75 g

6 (a) to 6 (d) are SEM photographs of complexes of copper oxide and magnesium oxide prepared according to the first to fourth embodiments, respectively. As can be seen from FIG. 6, it can be confirmed that the composite of copper oxide and magnesium oxide produced according to the embodiment of the present invention has a flower shape.

7 is a graph of XRD results of a composite of copper oxide and magnesium oxide according to an embodiment of the present invention.

Referring to FIG. 7, XRD data of the composites according to the first to fourth embodiments described with reference to FIG. 6 were measured. As can be seen from Fig. 7, it is confirmed that the composites according to the first to fourth embodiments have a copper oxide peak and a magnesium oxide peak.

FIG. 8 is a graph showing a result of methyl orange decomposition of a composite of copper oxide and magnesium oxide according to an embodiment of the present invention, and FIG. 9 is a graph showing the results of methylene blue decomposition of a composite of copper oxide and magnesium oxide methylene blue) decomposition.

Referring to Figs. 8 and 9, in accordance with an embodiment of the present invention, a combination of the methyl orange dye and the methylene blue dye according to the first to fourth embodiments described above was provided to evaluate photocatalytic properties. As a comparative example to the examples of the present invention, copper oxide and magnesium oxide were provided to the methyl orange dye and the methylene blue dye, and the photocatalytic properties were evaluated.

As can be seen from Figs. 8 and 9, when using the composites according to the first to fourth embodiments, it can be confirmed that the dyes are decomposed at a remarkably high speed as compared with the case of using the copper oxide. Also, the composite according to the fourth embodiment wherein the weight ratio of magnesium oxide to copper oxide is greater than 2, decomposes the dyes at a faster rate than the composites according to the first to third embodiments, copper oxide, and magnesium oxide .

While the present invention has been particularly shown and described with reference to exemplary embodiments thereof, it is to be understood that the scope of the present invention is not limited to the disclosed exemplary embodiments. It will also be appreciated that many modifications and variations will be apparent to those skilled in the art without departing from the scope of the invention.

Claims (12)

Mixing and refluxing a solution containing copper and a basic solution to produce copper oxide;
Mixing and refluxing a solution containing magnesium and the basic solution to produce magnesium oxide; And
And providing an acidic solvent to the copper oxide and the magnesium oxide to produce a composite of the copper oxide and the magnesium oxide.
The method according to claim 1,
Wherein the copper oxide and the magnesium oxide are in a flower shape.
The method according to claim 1,
The basic solution is an aqueous ammonia solution (NH ₄ OH), method of producing a complex containing at least one of a sodium hydroxide solution (NaOH), or an aqueous solution of potassium hydroxide (KOH) hydroxide.
The method according to claim 1,
And sintering the composite. ≪ Desc / Clms Page number 19 >
The method according to claim 1,
Wherein the step of preparing the composite of copper oxide and magnesium oxide comprises:
Providing the acidic solvent to the copper oxide and the magnesium oxide to prepare a mixed solution;
Diluting and stirring the mixed solution; And
And drying the mixed solution.
6. The method of claim 5,
Wherein the weight ratio of the magnesium oxide to the weight of the copper oxide is greater than 2 in the mixed solution.
6. The method of claim 5,
Wherein the mixed solution is diluted with deionized water.
The method according to claim 1,
Method of producing a composite in which the acidic solvent comprises HNO ₃ solution.
The method according to claim 1,
Wherein the basic aqueous solution comprises an aqueous ammonia solution,
The step of producing the copper oxide comprises:
Reacting copper ions contained in the solution containing copper with ammonia contained in the aqueous ammonia solution to produce a copper-ammonia composite; And
Wherein the copper-ammonia composite is reacted with hydroxyl groups contained in the aqueous ammonia solution to produce the copper oxide, wherein the copper oxide is self-organized in the form of a flower.
10. The method of claim 9,
The step of preparing the copper-ammonia composite is carried out at room temperature,
Wherein the step of preparing the copper oxide comprises performing the solution containing the copper and the aqueous ammonia solution at a reflux temperature.
The method according to claim 1,
Wherein the composite comprises a flower shape.
A photocatalyst comprising a composite prepared according to any one of claims 1 to 11.

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