Method of mechanochemically converting carbon dioxide

Abstract

The present invention provides a method of mechanochemically converting carbon dioxide, the method comprising the steps of: preparing a rotatable reaction container including a plurality of iron balls (S100); introducing a reaction catalyst including a metal oxide into the reaction container (S200); introducing carbon dioxide and hydrogen into the reaction container (S300); and rotating the reaction container to convert carbon dioxide and hydrogen into methane (S400).

Description

Mechanochemical carbon dioxide conversion method

[0001] The present invention relates to carbon capture, utilization, and storage (CCUS) technology.

[0002] Since the Paris Climate Agreement officially came into effect in November 2016, interest in "carbon neutrality" has rapidly increased. To date, more than 120 countries and regions have pledged to significantly reduce emissions and have set clear timelines for achieving carbon neutrality. Developed countries, led by the European Union, have announced a timeline of 71 years to achieve carbon neutrality, the United States 43 years (withdrawing in 2020 and returning in 2021), Japan 37 years, China 30 years, and South Korea has declared its goal of achieving carbon neutrality by 2050.

[0003] To achieve the "carbon neutrality" goal by the set deadline, relevant national and regional organizations are actively pursuing various support policies to promote the development of low-carbon technologies. In particular, they are continuously introducing various policies to encourage the development of carbon capture, utilization, and storage (CCUS) technology and industry. They are also establishing a systematic system for the theory, core technologies, and related strategies of CO2 capture, transportation, utilization, and storage, thereby accelerating technological innovation.

[0004] Currently, the global CCUS market is still in the industrial demonstration phase, with relatively small project scales and high costs. However, various policies encouraging technological development are expected to attract diverse capital, including energy sector investment institutions and individual investors, to the CCUS industry. This will accelerate the research and development of core technologies and revitalize the industry as a whole.

[0005] Conventionally, industrialized CCUS is mainly based on thermochemical reactions, but this has the problem that the reaction proceeds at high temperatures (300-600°C) due to the stable C=O double bond of carbon dioxide, resulting in high energy consumption and production costs.

[0006] One object of the present invention is to provide a mechanochemical carbon dioxide conversion method that can be performed at a lower temperature than existing high-temperature thermochemical catalyst technologies.

[0007] Another object of the present invention is to provide a carbon dioxide conversion method that can use commonly used mechano-chemical equipment.

[0008] According to one aspect of the present invention, a mechanochemical carbon dioxide conversion method is provided, comprising the steps of: preparing a rotatable reaction vessel containing a plurality of iron balls (S100); introducing a reaction catalyst composed of a metal oxide into the reaction vessel (S200); introducing carbon dioxide and hydrogen into the reaction vessel (S300); and rotating the reaction vessel so that the carbon dioxide and hydrogen are converted into methane (S400).

[0009] According to another aspect of the present invention, a mechanochemical carbon dioxide conversion device is provided, comprising: a rotatable reaction vessel containing a plurality of iron balls, carbon dioxide, and hydrogen; and a reaction catalyst composed of a metal oxide introduced into the reaction vessel; wherein when the reaction vessel rotates, carbon dioxide and hydrogen are converted into methane.

[0010] The mechanochemical CO2 reduction technology proposed in the present invention can be performed at a lower temperature (below 80°C) than the existing high-temperature thermochemical catalyst technology, resulting in lower energy consumption and the potential to further expand the CCUS market.

[0011] Furthermore, the present invention yields a high-purity methane product, which is considered a promising method for storing renewable energy and boasts the highest energy density of 55.5 GJ / ton among carbon products. Methane, a major component of natural gas, can be directly transported and utilized as a fuel in industrial infrastructure. For these reasons, the present invention holds enormous production value.

[0012] At the same time, the mechano-chemical equipment used in the present invention is a common and popular industrial equipment, which can provide an infrastructure for the industrialization of mechanochemical carbon dioxide reduction technology.

[0013] FIG. 1 is a drawing showing a mechanochemical carbon dioxide conversion device according to one embodiment of the present invention.

[0014] FIG. 2 is a drawing illustrating a mechanochemical carbon dioxide conversion method according to another aspect of the present invention.

[0015] Figure 3 shows the conversion rate of carbon dioxide as a result of an experiment on a carbon dioxide conversion method according to one embodiment of the present invention.

[0016] Figure 4 shows the concentration of methane as a result of an experiment on a carbon dioxide conversion method according to one embodiment of the present invention.

[0017] The above objectives, other objectives, features, and advantages will be readily understood through the following preferred embodiments, illustrated in the accompanying drawings. However, the embodiments described herein are not limited to the embodiments described herein and may be embodied in other forms. Rather, the embodiments introduced herein are provided to ensure that the disclosed content is thorough and complete, and to sufficiently convey the technical concepts to those skilled in the art.

[0018] In describing each drawing, similar reference numerals are used to designate similar components. In the attached drawings, the dimensions of structures are shown exaggerated for clarity of the present invention. Terms such as first, second, etc. may be used to describe various components, but the components should not be limited by the terms. The terms are used only to distinguish one component from another. For example, a first component may be referred to as a second component, and similarly, a second component may also be referred to as a first component, without departing from the scope of the present invention. The singular expression includes the plural expression unless the context clearly indicates otherwise.

[0019] In this specification, it should be understood that terms such as "include" or "have" are intended to specify the presence of a feature, number, step, operation, component, part or combination thereof described in the specification, but do not preclude the possibility of the presence or addition of one or more other features, numbers, steps, operations, components, parts or combinations thereof. In addition, when it is said that a part such as a layer, film, region or plate is "on" another part, this includes not only the case where it is "directly above" the other part, but also the case where there is another part in between. Conversely, when it is said that a part such as a layer, film, region or plate is "under" another part, this includes not only the case where it is "directly below" the other part, but also the case where there is another part in between.

[0020] Unless otherwise specified, all numbers, values, and / or expressions expressing quantities of ingredients, reaction conditions, polymer compositions, and blends used herein are approximations that inherently reflect, among other things, the various uncertainties of measurement that arise in obtaining such values, and therefore should be understood as being modified in all instances by the term "about." Furthermore, whenever a numerical range is disclosed herein, such range is continuous and includes every value from the minimum value to the maximum value inclusive, unless otherwise indicated. Furthermore, whenever such a range refers to an integer, every integer from the minimum value to the maximum value inclusive, unless otherwise indicated, is included.

[0021] In this specification, when a range is described for a variable, the variable will be understood to include all values ​​within the described range including the described endpoints of the range. For example, the range "5 to 10" will be understood to include the values ​​5, 6, 7, 8, 9, and 10, as well as any subranges such as 6 to 10, 7 to 10, 6 to 9, 7 to 9, etc., and any value between integers that fall within the described range, such as 5.5, 6.5, 7.5, 5.5 to 8.5, and 6.5 to 9. Also, for example, a range of "10% to 30%" would be understood to include all integers up to and including 30%, as well as any subranges such as 10% to 15%, 12% to 18%, 20% to 30%, etc., and any value between reasonable integers within the stated range, such as 10.5%, 15.5%, 25.5%, etc.

[0022]

[0023] The carbon dioxide conversion device of the present invention can be used in the carbon dioxide methanation reaction, one of the chemical conversion methods of carbon dioxide. The carbon dioxide methanation reaction converts carbon dioxide into methanogens, as shown in Chemical Formula 1 below, and the methane obtained thereby is used directly as an energy source or for the synthesis of liquid hydrocarbons.

[0024]

[0025] Chemical Formula 1

[0026] CO2+ 4H2-> CH4+ 2H2O

[0027]

[0028] The mechano-chemical equipment used for the mechanochemical carbon dioxide conversion according to the present invention basically includes a stationary outer container (B), a rotatable inner container (A), a scraper (C) and an armor (D) installed stationary within the inner container, and when the parent particles and child particles introduced into the inner container (A) pass through the armor (D), they are mechanically and chemically complexed, which is called a dry particle coating process or a mechano-chemical process.

[0029]

[0030] The above mechanochemical equipment may utilize the Mechanofusion System AMS of HOSOKAWA MICRON CORPORATION, which is commercially available, and the scope of the present invention is not limited thereto.

[0031]

[0032] FIG. 1 is a drawing showing a mechanochemical carbon dioxide conversion device according to one embodiment of the present invention.

[0033]

[0034] Referring to FIG. 1, a carbon dioxide conversion device according to one embodiment of the present invention may include a rotatable reaction vessel that accommodates a plurality of iron balls, carbon dioxide, and hydrogen; and a reaction catalyst composed of a metal oxide that is introduced into the reaction vessel.

[0035] In one embodiment, the plurality of iron balls may be 900 iron balls, and each iron ball may have a weight of 0.5 g.

[0036] In one embodiment, the metal oxide constituting the reaction catalyst may be a mixture of two or more metal oxides.

[0037] In one embodiment, the pressure of carbon dioxide contained within the reaction vessel may be 1 to 3 bar. By controlling the pressure of carbon dioxide, the concentration of carbon dioxide adsorbed on the catalyst surface can be controlled, thereby changing characteristics such as reaction rate, selectivity, and conversion rate.

[0038] In one embodiment, the pressure of hydrogen contained within the reaction vessel may be 7 to 10 bar. By controlling the pressure of hydrogen and using high-pressure hydrogen, the hydrogenation process of carbon dioxide can be accelerated.

[0039] In one embodiment, the rotation speed of the reaction vessel may be 500 to 600 rpm to convert carbon dioxide and hydrogen into methane. By utilizing a high rotation speed of the reaction vessel, defects can be generated on the catalyst surface, thereby enhancing the adsorption of carbon dioxide and hydrogen, and supplying the energy required for the reaction.

[0040]

[0041] FIG. 2 is a drawing illustrating a mechanochemical carbon dioxide conversion method according to another aspect of the present invention.

[0042] Referring to FIG. 2, a method for converting carbon dioxide according to one embodiment of the present invention may include a step (S100) of preparing a rotatable reaction vessel containing a plurality of iron balls; a step (S200) of introducing a reaction catalyst composed of a metal oxide into the reaction vessel; a step (S300) of introducing carbon dioxide and hydrogen into the reaction vessel; and a step (S400) of rotating the reaction vessel so that the carbon dioxide and hydrogen are converted into methane.

[0043] In one embodiment, the plurality of iron balls may be 900 iron balls, and each iron ball may have a weight of 0.5 g.

[0044] In one embodiment, the metal oxide constituting the reaction catalyst may be a mixture of two or more metal oxides.

[0045] In one embodiment, in the step (S300) of introducing carbon dioxide and hydrogen into the reaction vessel, the pressure of carbon dioxide within the reaction vessel may be 1 to 3 bar. By controlling the pressure of carbon dioxide, the concentration of carbon dioxide adsorbed on the catalyst surface can be controlled, thereby changing characteristics such as reaction rate, selectivity, and conversion rate.

[0046] In one embodiment, in the step (S300) of introducing carbon dioxide and hydrogen into the reaction vessel, the pressure of the hydrogen may be 7 to 10 bar. By controlling the pressure of the hydrogen and using high-pressure hydrogen, the hydrogenation process of carbon dioxide can be accelerated.

[0047] In one embodiment, in the step of rotating the reaction vessel (S400), the rotation speed of the reaction vessel may be 500 to 600 rpm. By utilizing a high rotation speed of the reaction vessel, defects can be generated on the catalyst surface, thereby enhancing the adsorption of carbon dioxide and hydrogen, and supplying the energy required for the reaction.

[0048]

[0049] Hereinafter, the present invention will be described in more detail with reference to examples. The following examples are merely illustrative examples to aid understanding of the present invention and are not intended to limit the scope of the present invention.

[0050]

[0051] Example: Mechanochemical carbon dioxide conversion

[0052] Ni / ZrO2 was added as a reaction catalyst into the reaction vessel, and 500 g of iron balls were prepared and placed in the reaction vessel.

[0053] In one embodiment, the pressure of hydrogen in the reaction vessel was set to 7.5 bar and the pressure of CO2 was set to 2 bar.

[0054] The reaction vessel was rotated at a speed of 550 rpm to react carbon dioxide and hydrogen to convert them into methane.

[0055]

[0056] Next, the reaction results are shown in Figures 2 and 3.

[0057]

[0058] FIG. 3 and FIG. 4 are results of an experiment on a carbon dioxide conversion method according to one embodiment of the present invention, where FIG. 3 shows the conversion rate of carbon dioxide and FIG. 4 shows the concentration of methane.

[0059]

[0060] Referring to FIGS. 3 and 4, using the carbon dioxide conversion method according to one embodiment of the present invention, a carbon dioxide conversion rate of up to 99.5% can be obtained, and a methane concentration of up to 99.1% can be obtained.

Claims

1. A step of preparing a rotatable reaction vessel containing a plurality of iron balls (S100); Step (S200) of introducing a reaction catalyst composed of a metal oxide into a reaction vessel; Step (S300) of introducing carbon dioxide and hydrogen into a reaction vessel; and A step (S400) of rotating the reaction vessel to convert carbon dioxide and hydrogen into methane; Mechanochemical carbon dioxide conversion method.

2. In paragraph 1, In the step (S300) of introducing carbon dioxide and hydrogen into the reaction vessel, The pressure of carbon dioxide inside the reaction vessel is 1 to 3 bar. Mechanochemical carbon dioxide conversion method.

3. In paragraph 1, In the step (S300) of introducing carbon dioxide and hydrogen into the reaction vessel, The pressure of hydrogen is 7 to 10 bar, Mechanochemical carbon dioxide conversion method.

4. In paragraph 1, In the step of rotating the reaction vessel (S400), The rotation speed of the reaction vessel is 500 to 600 rmp, Mechanochemical carbon dioxide conversion method.

5. A rotatable reaction vessel containing a plurality of iron balls, carbon dioxide, and hydrogen; and A reaction catalyst comprising a metal oxide which is introduced into a reaction vessel; As the reactor rotates, carbon dioxide and hydrogen are converted into methane. Mechanical and chemical carbon dioxide conversion device.

6. In paragraph 5, The pressure of carbon dioxide contained within the reaction vessel is 1 to 3 bar. Mechanical and chemical carbon dioxide conversion device.

7. In paragraph 5, The pressure of hydrogen contained in the reaction vessel is 7 to 10 bar. Mechanical and chemical carbon dioxide conversion device.

8. In paragraph 5, In the step of rotating the reaction vessel, The rotation speed of the reaction vessel is 500 to 600 rmp to convert carbon dioxide and hydrogen into methane. Mechanical and chemical carbon dioxide conversion device.

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