Cryogenic distillation apparatus, with excellent heat insulation and heat shielding effects, for separating and purifying deuterium, and deuterium separation method using same

Abstract

The present invention relates to: a cryogenic distillation apparatus for separating and purifying deuterium, the cryogenic distillation apparatus having excellent heat insulation and heat shielding effects; and a deuterium separation method using same. The present invention provides a cryogenic distillation apparatus for separating and purifying deuterium, the cryogenic distillation apparatus having excellent heat insulation and heat shielding effects, and comprising: a main body (10); a main heat exchanger (130) which separates deuterium (D2) and hydrogen deuteride (HD) through cryogenic distillation inside the main body (10); and a main refrigerator (140) which cools the main heat exchanger (130) to a predetermined target temperature, wherein a heating film and a demister filter are provided inside the main heat exchanger (130).

Description

Cryogenic distillation apparatus for deuterium separation and purification with excellent thermal insulation and heat shielding effects and a method for separating deuterium using the same

[0001] The present invention relates to a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, and a method for separating deuterium using the same. More specifically, due to the excellent thermal insulation and heat shielding effects inside the apparatus, rapid temperature changes caused by the outside can be prevented, thereby effectively removing deuteride hydrogen, which is an impurity, from a mixed gas of deuterium and deuteride hydrogen. This improves the purity and recovery rate of high-purity deuterium and enhances the economic efficiency of the process and the quality of the product. The invention relates to a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, and a method for separating deuterium using the same.

[0002] Various utility gases are used in the manufacturing process of semiconductor and LCD devices. Semiconductor devices are manufactured by repeatedly performing a series of processes, including film deposition, photolithography, etching, impurity implantation, and metallization.

[0003] Various types of gases are used in the execution of the above series of processes for manufacturing such semiconductor devices. Among them, deuterium (D2) is known to be used in high-pressure annealing equipment to prevent leakage current caused by tunneling phenomena occurring in processes of 28 nm or less.

[0004] Meanwhile, deuterium (D) is an isotope of hydrogen (H, light hydrogen) in which there is one additional neutron in the nucleus of ordinary hydrogen. The molecular form of deuterium is D2, and the atomic weight of deuterium is approximately twice that of a hydrogen atom (1.007947 u) (2.014102 u).

[0005] Unlike other isotopes, deuterium is chemically stable and does not undergo nuclear fission. Therefore, its stability can be enhanced compared to ordinary hydrogen based on changes in reactivity caused by mass variations. For this reason, there has recently been a trend to prefer deuterium in the electronics and semiconductor industries, and active research is currently underway.

[0006] Generally, deuterium (D₂) is produced by electrolyzing heavy water (D₂O), but in this process, its isotope, hydrogen deuteride (HD), is present in trace amounts as an impurity within the deuterium produced.

[0007] To eliminate this, distillation can be used to separate specific components by utilizing the difference in boiling points of each component in a mixture. In particular, when separating a mixture of gases containing deuterium and hydrogen deuteride, which have low boiling points, cryogenic distillation, which involves distilling at very low temperatures, can be utilized to effectively separate the two substances. However, the aforementioned cryogenic distillation method has the disadvantage of consuming a large amount of energy to maintain the cryogenic temperature, and there is a problem with the difficulty of controlling the temperature according to minute differences in boiling points in a low-temperature environment.

[0008] Another method for purifying impurities from mixed gases involves using a porous adsorbent with excellent selective adsorption capacity for only one component of the mixed gas. However, this method has a limitation in that it is very difficult to control the selectivity for the adsorbate when the physical and chemical properties of the mixed gases are similar.

[0009] Due to the above, further research and development is required for deuterium separation and purification technology that maximizes the removal of hydrogen deutride, an impurity, and improves purity and recovery rates.

[0010] The present invention was devised to solve the problems of the prior art described above, and aims to provide technical details regarding a cryogenic distillation apparatus for deuterium separation and purification with excellent thermal insulation and heat shielding effects, and a method for separating deuterium using the same, which prevents rapid temperature changes caused by the outside due to the excellent thermal insulation and heat shielding effects inside the apparatus, thereby effectively removing deuterium impurities from a mixed gas of deuterium and deuteriumized hydrogen, improving the purity and recovery rate of high-purity deuterium, and enhancing the economic efficiency of the process and product quality.

[0011] The present invention relates to a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, and a method for separating deuterium using the same.

[0012] To achieve the technical objectives described above, the present invention provides a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, comprising: a main body (10); a main heat exchanger (130) for separating deuterium (D2) and hydrogen dehydrogenated (HD) through cryogenic distillation inside the main body (10); and a main refrigerator (140) for cooling the main heat exchanger (130) to a predetermined target temperature, wherein the main heat exchanger (130) is characterized by having a heating film and a demister filter inside.

[0013] According to a preferred embodiment of the present invention, the system may further include an auxiliary heat exchanger (150) into which deuterium hydrogen gas separated from the main heat exchanger (130) is injected, and may be characterized by having an activated carbon filter (151) inside the auxiliary heat exchanger (150) that selectively adsorbs only the deuterium hydrogen.

[0014] In addition, according to a preferred embodiment of the present invention, the invention may further include a preheat exchanger (100) formed inside the main body (10), an auxiliary chiller (110) for preheating the preheat exchanger (100), and a cooling pipe (120) installed spirally along the outside of the preheat exchanger (100), having an inlet formed at one end through which a mixed gas containing deuterium (D2) and hydrogen dehydrogenated (HD) is injected.

[0015] In addition, according to a preferred embodiment of the present invention, the device may further include a protective case (11) formed inside the main body (10), and the device may be characterized in that the preheat exchanger (100), main heat exchanger (130), and auxiliary heat exchanger (150) are installed inside the protective case (11).

[0016] In addition, according to a preferred embodiment of the present invention, the target temperature may be characterized by separation taking place at a temperature of 20 to 25 K.

[0017] In addition, according to a preferred embodiment of the present invention, a method for separating deuterium using a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects may include: (a) introducing the deuterium-deuteriumized hydrogen mixed gas into a main heat exchanger (130) equipped with a heating film and a demister filter inside and cooling it to a temperature of 20 to 25 K to separate and remove the deuteriumized hydrogen, which is an impurity; and (b) raising the temperature of the high-purity liquid deuterium from which the deuteriumized hydrogen has been removed to a temperature of 25 to 100 K to obtain high-purity gaseous deuterium.

[0018] The cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects according to the present invention and the deuterium separation method using the same can prevent rapid temperature changes caused by the outside due to the excellent thermal insulation and heat shielding effects inside the apparatus, thereby effectively removing deuterium, which is an impurity, from a mixed gas of deuterium and deuteriumized hydrogen, and can improve the purity and recovery rate of high-purity deuterium, as well as the economic efficiency of the process and the quality of the product.

[0019] FIG. 1 is a drawing illustrating a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects according to an embodiment of the present invention, and a method for separating deuterium using the same.

[0020] FIG. 2 is a flowchart illustrating a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects according to an embodiment of the present invention, and a method for separating deuterium using the same.

[0021] FIG. 3 is a diagram showing the gas chromatography (GC) results after deuterium separation and purification according to an embodiment of the present invention.

[0022] Hereinafter, a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects according to the present invention and a method for separating deuterium using the same will be described in more detail with reference to specific examples. However, the embodiments introduced below are provided as examples to ensure that the concept of the present invention is sufficiently conveyed to those skilled in the art.

[0023] Accordingly, the present invention is not limited to the embodiments presented below and may be embodied in other forms, and the embodiments presented below are described merely to clarify the concept of the present invention and are not limited thereto.

[0024] Unless otherwise defined, technical and scientific terms used herein have the meanings commonly understood by those skilled in the art to which this invention pertains, and are defined in consideration of their functions in the present invention; such definitions may vary depending on the intent or convention of the user or operator. Therefore, the definitions of these terms should be based on the content throughout this specification, and descriptions of known functions and configurations that could unnecessarily obscure the essence of the present invention are omitted in the following description.

[0025] Additionally, the singular form used in the specification and attached claims may be intended to include the plural form unless specifically indicated otherwise in the context.

[0026] In addition, the thickness of lines or the size of components shown in the drawings may be exaggerated for clarity and convenience of explanation.

[0027] In addition, in the present invention, heavy water (D2O) refers to two deuterium atoms (D) with a mass number of 2 combined with one oxygen atom (O), and deuterium hydrogen (HD) refers to one deuterium atom (D) with a mass number of 2 combined with one light hydrogen atom (H) with a mass number of 1.

[0028] The present invention will be described in detail below.

[0029] In the cryogenic distillation apparatus for separating and purifying deuterium having excellent thermal insulation and heat shielding effects according to the present invention, the apparatus comprises a main body (10), a main heat exchanger (130) for separating deuterium (D2) and deuteriumized hydrogen (HD) through cryogenic distillation inside the main body (10), and a main refrigerator (140) for cooling the main heat exchanger (130) to a predetermined target temperature, wherein the main heat exchanger (130) is characterized by having a heating film and a demister filter inside.

[0030] In the present invention, the main body (10) may refer to the entire cryogenic distillation tower for deuterium separation and purification equipped with a pre-cooling system. Additionally, the main body (10) may further include a protective case (11) formed inside, and the pre-heat exchanger (100), main heat exchanger (130), and auxiliary heat exchanger (150) may be installed inside the protective case (11).

[0031] The initial vacuum inside the protective case (11) can be maintained at 0 to 1 Pa. When the vacuum pressure inside the protective case (11) is within the above range, there is no convection because the gas flow is in the free molecular motion region, and the gas phase thermal conductivity is reduced, thereby eliminating the amount of heat transfer by the gas.

[0032] In addition, in the present invention, the protective case (11) is a vacuum insulation cooling box and can maintain a vacuum and insulation state through multilayer insulation (MLI), and the multilayer insulation may be composed of a sandwich structure in which a low-conductivity material called a spacer is inserted between several layers of radiation-reflecting metal films called a shield.

[0033] The above shield may be made of a gold or aluminum-based material with high reflectivity, and the above spacer may be made of low-conductivity glass fiber, silk, or nylon, but is not limited thereto.

[0034] By using a vacuum insulation cooling box as the above protective case (11), it is possible to have excellent thermal insulation properties that prevent cold air leakage to the outside while having an excellent heat shielding effect against heat entering from the outside. In addition, energy efficiency can be increased, and the ability to finely control the temperature of the condenser can be improved, thereby increasing the yield of high-purity deuterium and improving the economic efficiency of the process.

[0035] In addition, the protective case (11) can be cooled to a temperature of 10 to 20K. This allows heat entering from the outside to be effectively blocked, while also improving the temperature control capability of the preheat exchanger (100), thereby improving the process efficiency of the cryogenic distillation apparatus for deuterium separation and purification according to the present invention, and increasing the recovery rate and purity of high-purity deuterium and improving the quality of the product.

[0036] In addition, in the present invention, the main heat exchanger (130) is a location in which one side is connected to the cooling pipe (120) to receive the pre-cooled mixed gas of deuterium and deuterated hydrogen, and to separate and purify the deuterium and deuterated hydrogen by cryogenic distillation.

[0037] In addition, the interior of the main heat exchanger (130) may be equipped with a heating film and a demister filter.

[0038] The heating film described above may have a heat-blocking function that blocks heat entering from the outside and a thermal insulation function that reflects heat from the inside to prevent cold air from leaking out. By including the heating film to increase energy efficiency, the economic feasibility of the process may be enhanced, and the ability to finely control the temperature of the condenser may be improved, which can increase the purity of the product and consequently lead to an improvement in quality.

[0039] The above demister filter can remove impurities, such as dust and foreign substances, contained in the injected mixed gas. The above demister filter is a dust collection filter with high corrosion resistance, and is generally a filter that separates and removes impurities contained in a fluid. The above demister filter is not restricted by thickness, has a large porosity, and has excellent dust collection capabilities because its entire surface area is exposed to the air, resulting in a large contact effect with the fluid. In addition, it can capture up to 80% of dust particles of 10 to 30 µm based on the gravimetric method, and it is suitable for locations with high dust generation because it has good air permeability, low air resistance, and is easy to store and clean.

[0040] Specifically, the main heat exchanger (130) may include four to five stages of demister filters to effectively remove impurities, such as dust and foreign substances, contained in the deuterium-deuteriumized hydrogen mixed gas flowing into the main heat exchanger (130). In addition, this may have the effect of improving product quality and stably obtaining high-purity deuterium.

[0041] Additionally, a main refrigerator (140) may be attached to one side of the main heat exchanger (130) so that the main heat exchanger (130) can be cooled to a predetermined target temperature. The target temperature may be a temperature at which hydrogen deuterated, an impurity, is removed in a gaseous state through cryogenic distillation. Specifically, the target temperature may be characterized by separation occurring at a temperature of 20 to 25 K. When the target temperature falls within the above range, hydrogen deuterated can be effectively separated to improve the recovery rate of high-purity deuterium. If the target temperature is less than 20 K, the vaporization of hydrogen deuterated does not occur, so the effect of improving the purity of high-purity deuterium may be insufficient, and if it exceeds 25 K, the vaporization of hydrogen deuterated and deuterium occurs simultaneously, which may lower the recovery rate of high-purity deuterium.

[0042] In the present invention, the main refrigerator (140) may be characterized by having an upper portion installed outside the main body (10) and a lower portion installed inside the main body (10). Additionally, the main heat exchanger may be characterized by being installed below the main refrigerator (140).

[0043] Additionally, the main refrigerator (140) can cool the main heat exchanger (130) to a predetermined target temperature, and the target temperature may be 20 to 25K.

[0044] In addition, a method for separating deuterium using a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects may include: (a) a step of introducing the deuterium-deuteriumized hydrogen mixed gas into a main heat exchanger (130) equipped with a heating film and a demister filter inside and cooling it to a temperature of 20 to 25 K to separate and remove the deuteriumized hydrogen, which is an impurity; and (b) a step of raising the temperature of the high-purity liquid deuterium from which the deuteriumized hydrogen has been removed to a temperature of 25 to 100 K to obtain high-purity gaseous deuterium.

[0045] (a) Step of introducing the deuterium-deuterium hydrogen mixed gas into a main heat exchanger (130) equipped with a heating film and a demister filter inside, and raising the temperature to 20 to 25 K to separate and remove the deuterium hydrogen, which is an impurity; may be characterized by including a process of cooling the mixed gas to a temperature of 20 to 25 K to vaporize and separate and remove only the deuterium hydrogen, which is an impurity. Preferably, the mixed gas may be cooled to a temperature of 22 K. By cooling the mixed gas to 22 K, the selectivity of vaporizing the deuterium hydrogen, which is an impurity, can be improved, and the yield of high-purity deuterium can be increased.

[0046] Additionally, the above step (a) may be characterized by being performed inside the main heat exchanger (130). At this time, a heating film and a demister filter may be provided inside the main heat exchanger (130). By providing this, not only is fine temperature control possible, but the removal effect of impurity particles is excellent, so the selective vaporization of the deuteriumized hydrogen can be performed more effectively, and the purity improvement effect of the deuterium can be excellent.

[0047] In addition, in step (a) above, phase separation may occur due to the difference in boiling points of the deuterium-deuterium hydrogen mixed gas. More specifically, the deuterium exists in a liquid state and the deuterium hydrogen exists in a gaseous state, so that impurities can be effectively separated and removed by selectively exhausting the deuterium hydrogen.

[0048] (b) Step of obtaining high-purity gaseous deuterium by raising the temperature of the high-purity liquid deuterium from which the deuterium hydrogen has been removed to a temperature of 25 to 100 K; may include a process of obtaining deuterium with improved purity by vaporizing it from the main heat exchanger (130) in which the deuterium hydrogen has been removed.

[0049] Including the above steps, it is possible to effectively remove deuteride hydrogen, which is an impurity, from the deuterium and deuteride hydrogen mixed gas and obtain high-purity deuterium, while simultaneously improving the purity and recovery rate of deuterium to be economically advantageous.

[0050] In addition, in a method for separating deuterium using a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, the method may further include a step (c) of pre-cooling a deuterium-deuterided hydrogen mixed gas injected through an inlet at one end of a cooling pipe (120) provided in the cryogenic distillation apparatus for separating and purifying deuterium to a temperature of 70 to 80 K before step (a). The step (c) may take place in the cooling pipe (120), and the deuterium-deuterided hydrogen mixed gas at 70 to 80 K that has undergone pre-cooling may exist in a gaseous state.

[0051] By further including the above step (c), the removal effect of deuteride hydrogen, which is an impurity, from the deuterium-deuteride hydrogen mixed gas may be enhanced, and the purity and recovery rate of deuterium may be improved.

[0052] In the present invention, the auxiliary heat exchanger (150) may be a location where deuterium hydrogen gas separated from the main heat exchanger (130) is introduced. Additionally, an activated carbon filter (151) that adsorbs the deuterium hydrogen may be provided inside the auxiliary heat exchanger (150), thereby having the effect of adsorbing and removing the deuterium hydrogen introduced from the main heat exchanger (130).

[0053] The above activated carbon filter (151) can adsorb the deuterium hydrogen. Specifically, the above activated carbon filter (151) may include surface-modified activated carbon. The surface-modified activated carbon has functional groups introduced to its surface and increased porosity, thereby exhibiting excellent adsorption capacity for deuterium hydrogen.

[0054] In the surface modification step of the surface-modified activated carbon described above, carbon surface treatment methods such as acid treatment, ozone treatment, and plasma treatment may be utilized, and preferably, an ozone treatment method may be utilized. Through the ozone treatment method, the carbon surface is oxidized, increasing surface roughness and surface oxygen content, which can improve the adsorption capacity for hydrogen deuteride.

[0055] In addition, the remaining deuterium hydrogen after adsorption can be discharged through a connected pipe.

[0056] The auxiliary heat exchanger (150) is installed at the bottom of the auxiliary refrigerator (110) and can be cooled to a temperature of 10 to 20 K by the auxiliary refrigerator (110). Through this, the deuterated hydrogen gas introduced into the auxiliary heat exchanger (150) can be liquefied.

[0057] In the present invention, the preheat exchanger (100) is formed inside the main body (10) and may be installed in the middle section of the auxiliary refrigerator (110). Accordingly, the preheat exchanger (100) may be preheated by the auxiliary refrigerator (110). The preheating may be characterized by a temperature of 70 to 80K.

[0058] In addition, the above preheat exchanger (100) has the cooling pipe (120) installed on its exterior to preheat the deuterium-deuterium hydrogen mixed gas flowing in through the cooling pipe (120).

[0059] Additionally, the above-mentioned preheat exchanger (100) may be characterized by having grooves at regular intervals along its exterior, and the above-mentioned cooling pipe (120) may be installed spirally along the grooves. Through the above-mentioned structural features, the contact area between the preheat exchanger (100) and the cooling pipe (120) may be increased. Furthermore, the above-mentioned preheat exchanger (100) and the cooling pipe (120) may be characterized by having excellent heat exchange efficiency.

[0060] In the present invention, the auxiliary refrigerator (110) may be a device that cools by exchanging heat. A refrigerant may flow inside the auxiliary refrigerator (110) to promote heat convection and perform a cooling function, and the refrigerant may be a cryogenic refrigerant and may be supplied into the auxiliary refrigerator and discharged from the auxiliary refrigerator through a cryogenic refrigerant circulation system. The type of refrigerant may be nitrogen or helium, but is not limited thereto.

[0061] The above auxiliary chiller (110) may have its upper portion installed outside the main body (10), and its middle and lower portions installed inside the main body (10). Additionally, a preheat exchanger (100) may be installed in the middle portion of the auxiliary chiller, and an auxiliary heat exchanger (150) may be installed in the lower portion.

[0062] In this regard, the auxiliary chiller (110) may have the function of pre-cooling the pre-heat exchanger (100) installed in the middle section.

[0063] When pre-cooling the above pre-heat exchanger (100), the temperature may be characterized as being 70 to 80K.

[0064] Additionally, the auxiliary chiller (110) can cool the auxiliary heat exchanger (150) installed at the bottom. The cooling may be characterized by a temperature of 10 to 20K. Preferably, the cooling may be characterized by a temperature of 15K.

[0065] In the present invention, the cooling pipe (120) is installed spirally along the outside of the preheat exchanger (100), and one end forms an inlet, through which a mixed gas containing deuterium and hydrogen deuterated is injected and flows along the pipe, and heat is transferred to the preheat exchanger (100) to be preheated.

[0066] In addition, the structural feature of the cooling tube (120) may be that it is wound spirally along a groove provided on the outside of the heat exchanger, and due to the structural feature, the contact area between the cooling tube (120) and the preheater (100) is increased, so that the heat exchange efficiency and cooling efficiency may be excellent.

[0067] And, in the cooling pipe (120), pre-cooling of the deuterium-deuterium hydrogen mixture gas may occur.

[0068] The above pre-cooling may be characterized by a process in which the deuterium-deuterium hydrogen mixed gas injected through the inlet of one end of the cooling pipe (120) is pre-cooled before being introduced into the main heat exchanger (130).

[0069] In addition, the above pre-cooling may be characterized by a temperature of 70 to 80K. When the cooling temperature falls within the above range, the thermal efficiency and thermal stability of cryogenic distillation may be increased, and fine temperature control during the heating process of cryogenic distillation may be facilitated, thereby improving the selectivity for removing hydrogen deuteride, which is an impurity. If the cooling temperature is less than 10K, efficiency may decrease in terms of energy, and if it exceeds 20K, the effect of improving thermal efficiency and thermal stability through pre-cooling may be insufficient.

[0070] In the present invention, the pump (160) may be a vacuum pump that reduces internal pressure by being coupled to an inlet formed at one end of a cooling pipe (120), an auxiliary heat exchanger (150), and a part of a main heat exchanger (130).

[0071] The present invention will be explained in more detail below with reference to examples and comparative examples.

[0072] However, the following examples and comparative examples are merely illustrative of the invention for further detailed explanation, and the invention is not limited to the following examples and comparative examples.

[0073] Experimental Method

[0074] For a deuterium-hydrogen deuteride mixed gas at a temperature of 300K and a hydrogen deuteride concentration of 1666 ppm,

[0075] (a) The above deuterium-deuterium hydrogen mixture gas is introduced into a main heat exchanger (130) equipped with a heating film and a demister filter, and cooled to a temperature of 22K to separate and remove the deuterium hydrogen, which is an impurity. Then, (b) the high-purity liquid deuterium from which the deuterium hydrogen has been removed is heated to a temperature of 100K to obtain high-purity gaseous deuterium.

[0076] <Example 1>

[0077] According to the above experimental method, deuterium-deuterium-hydrogen mixture gas was removed and deuterium was obtained.

[0078] <Example 2>

[0079] (a) Before step, (c) pre-cooling the deuterium-deuterium mixed gas injected through the inlet of one end of the cooling tube (120) provided in the cryogenic distillation apparatus for deuterium separation and purification to a temperature of 70 to 80 K; except for further including the step of removing deuterium from the mixed gas and obtaining deuterium in the same manner as in Example 1.

[0080] <Comparative Example 1>

[0081] (a) In step, the main heat exchanger (130) removes hydrogen deuterated from the mixed gas and obtains deuterium in the same manner as in Example 1, except that it is not equipped with a heating film and a demister filter inside.

[0082] <Experimental Example 1> - Evaluation of Enhanced Effect of Deuterium Hydrogen Removal through Deuterium Separation and Purification

[0083] To evaluate the effect of removing hydrogen deuterated and improving purity through the separation and purification of deuterium performed by each example and comparative example, the concentration of hydrogen deuterated (HD) was measured using a high-precision mass spectrometer (Gas / MS, Finnigan MAT271) and is shown in below.

[0084] Classification Purification Pre-Example 1 Example 2 Comparative Example 1 HD Concentration (ppm) 16669057601492

[0085] As a result of evaluating the improved effect of removing deuterated hydrogen through deuterated separation and purification performed in each example and comparative example through , Examples 1 and 2, which are equipped with a heating film and a demister filter inside the main heat exchanger (130), showed a relatively lower concentration of deuterated hydrogen, an impurity, compared to Comparative Example 1, which is not equipped with a heating film and a demister filter. Through this, it was confirmed that the effect of removing deuterated hydrogen is excellent when a heating film and a demister filter are equipped inside the main heat exchanger (130).

[0086] In addition, in the case of Example 2, which further includes the step of pre-cooling the deuterium-deuteriumized hydrogen mixed gas injected through the inlet of one end of the cooling pipe (120) provided in the cryogenic distillation device for deuterium separation and purification to a temperature of 77K before step (a), the concentration of deuteriumized hydrogen was measured to be lower compared to Example 1, which does not include step (c), so it was confirmed that the deuteriumized hydrogen removal effect is superior when step (c) is further included.

[0087] And Figure 3 shows the gas chromatography (GC) results after deuterium separation and purification, and by referring to Figure 3, it can be confirmed that deuterium separation and purification is clearly achieved.

[0088] <Experimental Example 2> - Evaluation of the Effect of Improving Deuterium Purity and Recovery Rate through Deuterium Separation and Purification

[0089] To evaluate the effect of improving the recovery concentration and recovery rate of deuterium through the separation and purification of deuterium performed by each example and comparative example, the concentration of deuterium was measured using a low-vacuum gas injection quadrupole mass spectrometer (QMS), and the purity and recovery rate of deuterium obtained by each example and comparative example are shown in .

[0090] Classification Example 1 Example 2 Comparative Example 1 D2 Recovery Concentration (ppm) 48 10 9 49 72 44 27 18 D2 Recovery Rate (%) 97.05 98.8 08 1.95

[0091] Based on the evaluation of the improvement in purity and recovery rate of deuterium during the separation and purification process of deuterium using , it was confirmed that Examples 1 and 2, which are equipped with a heating film and a demister filter inside the main heat exchanger (130), have higher deuterium purity and recovery rate compared to Comparative Example 1, which is not equipped with a heating film and a demister filter. In addition, in the case of Example 2, which further includes the step of pre-cooling the deuterium-deuterided hydrogen mixed gas injected through the inlet of one end of the cooling pipe (120) equipped in the cryogenic distillation apparatus for deuterium separation and purification (step (c)) to a temperature of 77K, it was confirmed that the purity and recovery rate of deuterium are further improved compared to Example 1, which is not equipped with step (c). As a result of the comprehensive evaluation, it was confirmed that Example 2 exhibited the lowest HD concentration, the highest D2 purity, and the highest recovery rate, indicating the most superior deuterium separation and purification effect.

[0092] Although preferred embodiments of the present invention have been described above, those skilled in the art will understand that various modifications and changes can be made to the present invention without departing from the technical spirit of the invention as described in the following claims.

Claims

1. In a cryogenic distillation apparatus for separating and purifying deuterium, Main body (10); A main heat exchanger (130) that separates deuterium (D2) and hydrogen deuterated (HD) through cryogenic distillation inside the main body (10); and It includes a main refrigerator (140) that cools the main heat exchanger (130) to a predetermined target temperature, and A cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, comprising the above main heat exchanger (130) which is characterized by having a heating film and a demister filter inside.

2. In Paragraph 1, It further includes an auxiliary heat exchanger (150) into which hydrogen gas separated from the main heat exchanger (130) is injected, and A cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, characterized by having an activated carbon filter (151) that selectively adsorbs only the deuterium hydrogen inside the auxiliary heat exchanger (150).

3. In Paragraph 1, A preheat exchanger (100) formed inside the main body (10); An auxiliary chiller (110) for pre-cooling the above pre-heat exchanger (100); and A cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, further comprising: a cooling pipe (120) installed spirally along the outside of the above-mentioned preheat exchanger (100), having an inlet formed at one end, through which a mixed gas containing deuterium (D2) and deuterated hydrogen (HD) is injected.

4. In Paragraph 1, It further includes a protective case (11) formed inside the main body (10), and A cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, characterized in that the above-mentioned preheat exchanger (100), main heat exchanger (130), and auxiliary heat exchanger (150) are installed inside the above-mentioned protective case (11).

5. In Paragraph 1, The above target temperature is, A cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, characterized by separation taking place at a temperature of 20 to 25K.

6. A method for separating deuterium using a cryogenic distillation apparatus for separating and purifying deuterium with excellent thermal insulation and heat shielding effects, (a) a step of introducing the above deuterium-deuterium hydrogen mixed gas into a main heat exchanger (130) equipped with a heating film and a demister filter inside, and cooling it to a temperature of 20 to 25K to separate and remove the deuterium hydrogen, which is an impurity; and (b) a step of heating the high-purity liquid deuterium from which the deuterated hydrogen has been removed to a temperature of 25 to 100 K to obtain high-purity gaseous deuterium; a deuterium separation method comprising.

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