JP2014055094A - Ammonia purification apparatus, and regeneration method thereof - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide an ammonia purification apparatus that requires only a short time for regeneration of itself after removing impurities in crude ammonia by bringing the crude ammonia into contact with a catalyst having nickel as an active ingredient and synthetic zeolite, and to provide a regeneration method thereof.SOLUTION: An ammonia purification apparatus includes an introduction line of a regeneration gas, an exhaust line of a regeneration gas, and a pressure regulator installed on the exhaust line of a regeneration gas located downstream of a synthetic zeolite bed. A process for regenerating the ammonia regeneration apparatus includes a step for letting an inert gas or a gas mixture of the inert gas and ammonia pass through the synthetic zeolite under heating to remove impurities from the synthetic zeolite, a step for letting the inert gas pass through the synthetic zeolite to cool the synthetic zeolite, an a step for letting the pressurized gas mixture of the inert gas and ammonia pass through the synthetic zeolite for the synthetic zeolite to adsorb the ammonia.

Description

  The present invention relates to an apparatus for purifying crude ammonia containing impurities such as oxygen, carbon dioxide and water, and a method for regenerating the ammonia purification apparatus after purifying ammonia.

  Gallium nitride compound semiconductors are widely used as elements such as light emitting diodes and laser diodes. This gallium nitride compound semiconductor manufacturing process (gallium nitride compound semiconductor process) is usually performed by vapor-phase growth of a gallium nitride compound on a substrate such as sapphire by MOCVD, and a raw material used for this As the gas, for example, Group III trimethylgallium, trimethylindium, trimethylaluminum, and Group V ammonia are used. In the gallium nitride compound semiconductor process, high-purity ammonia is required.

  Generally, crude ammonia (industrial crude ammonia) commercially available for industrial use contains hydrogen, nitrogen, oxygen, carbon dioxide, water and the like. As high-purity ammonia, industrial crude ammonia is further obtained by removing impurities by distillation, rectification, or liquefaction, or diluted with high-purity inert gas. Commercially available in form. However, the high-purity ammonia is very expensive as compared with industrial crude ammonia, and the gallium nitride compound semiconductor process has a disadvantage that the running cost becomes extremely expensive. Moreover, most of them are not used in semiconductor processes and are discarded in large quantities without being reacted. For this reason, a method for purifying ammonia has been developed that can supply industrial crude ammonia continuously to the semiconductor process to produce a semiconductor at low cost.

For example, a method of removing impurities by bringing crude ammonia into contact with a catalyst containing nickel as a main component (Japanese Patent Laid-Open Nos. 5-124813 and 6-107412), industrial crude ammonia, and a catalyst containing nickel as an active ingredient There is a method (JP-A-2002-37624) for removing impurities contained in crude ammonia by contacting with synthetic zeolite having a pore diameter of 4 to 10 liters after contacting with.
Japanese Patent Laid-Open No. 5-124813 Japanese Patent Laid-Open No. 6-107412 JP 2002-37624 A

  However, when industrial crude ammonia is refined with a nickel catalyst and synthetic zeolite and purified ammonia is continuously supplied to the gallium nitride compound semiconductor process, even if there are two purification lines, the industrial concentration is high. When a large amount of crude ammonia for purification is purified, it takes longer to regenerate the other ammonia purification device than the time available for purification by the other ammonia purification device, and the purified ammonia is continuously removed from the gallium nitride compound. There is a possibility that it cannot be supplied to the semiconductor process.

  Regarding the regeneration of the ammonia purifier, the nickel catalyst after use is usually completed by heating the hydrogen-containing gas through the catalyst cylinder while heating and removing oxygen and the like captured during the purification of ammonia. In addition, the synthetic zeolite after use is usually (1) after passing an inert gas (or a mixed gas of inert gas and ammonia) through an adsorption cylinder while heating to remove water adsorbed during the purification of ammonia. (2) An inert gas is circulated and cooled. (3) Ammonia (or a mixed gas of inert gas and ammonia) is gradually circulated to adsorb ammonia to complete the process.

  The reason for adsorbing ammonia on the synthetic zeolite in advance before resuming the purification of ammonia is that, unless such preparation is made, a large amount of heat of adsorption is generated at the start of ammonia purification, and impurities contained in the ammonia are adsorbed by the synthetic zeolite. This is because there is a possibility that it cannot be removed. The above-mentioned “problem that it takes longer to regenerate the purification device than the time during which the purification treatment can be performed” is controlled by reducing the flow rate so that the synthetic zeolite does not rise to a temperature at which ammonia cannot be adsorbed in the step (3). As a result, ammonia (or a mixed gas of inert gas and ammonia) must be circulated, so that the effect of increasing the processing time is great.

  In order to solve this problem, the method of simply increasing the amount of synthetic zeolite charged in the step (3) increases the purification time of ammonia, but the ammonia is adsorbed to the synthetic zeolite even during regeneration of the ammonia purification device. Since a large amount of heat of adsorption is generated during the process, it takes time. In particular, when the diameter of the adsorption cylinder is increased, there is a problem that the regeneration time is significantly increased. Further, in the process of (3), the method of circulating a mixed gas having a low ammonia content suppresses the temperature increase of the synthetic zeolite (the circulation of the inert gas exhibits a cooling effect), Adsorption of ammonia takes time and the problem is not solved. Therefore, the problem to be solved by the present invention is to provide an ammonia purification apparatus and a regeneration method thereof that do not take time for regeneration.

  As a result of intensive studies to solve the above-mentioned problems, the inventors of the present invention, in the regeneration of the ammonia purification apparatus as described above, when adsorbing ammonia to the synthetic zeolite, a gas having a relatively low content of ammonia was used. If it is circulated under pressure, the partial pressure of ammonia is high even if its content is low. Therefore, ammonia can be adsorbed to the synthetic zeolite in a short time without a sudden rise in temperature, and the regeneration gas discharged after the synthetic zeolite is distributed. It is found that if a pressure regulator is provided in the line, the regenerated gas (mixed gas of inert gas and ammonia) can be easily circulated to the ammonia refining device, and the ammonia refining device of the present invention and the regenerating method thereof are reached. did.

  That is, the first invention of the present application is an ammonia purifying apparatus comprising a catalyst cylinder having a catalyst filling portion containing nickel as an active ingredient, an adsorption cylinder having a synthetic zeolite filling portion, and a crude ammonia introduction line. A refining gas introduction line, a regeneration gas discharge line, and a regeneration gas discharge line after circulating the synthetic zeolite are equipped with a pressure regulator, and the ammonia purifying apparatus is characterized in that:

  Further, the second invention of the present application is an ammonia purifying apparatus comprising a refining cylinder having a catalyst filling portion containing nickel as an active component and a filling portion of synthetic zeolite, and a crude ammonia introduction line, wherein regenerative gas introduction A purification apparatus for ammonia, comprising a line, a regeneration gas discharge line, and a regeneration gas discharge line after circulation of synthetic zeolite, and a pressure regulator.

  The third invention of the present application is a method of regenerating the ammonia purification device after purifying the ammonia with the ammonia purification device of the first invention, wherein an inert gas or inert gas is added to the adsorption cylinder under heating. A process of removing impurities from the synthetic zeolite by circulating a mixed gas of active gas and ammonia, a process of circulating an inert gas through the adsorption cylinder and cooling the synthetic zeolite, and a mixture of inert gas and ammonia pressurized to the adsorption cylinder A method for regenerating an ammonia refining apparatus, comprising a step of circulating gas and adsorbing ammonia to a synthetic zeolite.

  The fourth invention of the present application is a method of regenerating the ammonia purification apparatus after purifying the ammonia with the ammonia purification apparatus of the second invention, wherein the purification cylinder is heated with an inert gas or an inert gas. A process of removing impurities from the synthetic zeolite by circulating a mixed gas of active gas and ammonia, a process of circulating an inert gas through the purification cylinder and cooling the synthetic zeolite, and a mixture of inert gas and ammonia pressurized in the purification cylinder A method for regenerating an ammonia refining apparatus, comprising a step of circulating gas and adsorbing ammonia to a synthetic zeolite.

  According to the ammonia purifying apparatus and the regeneration method of the present invention, ammonia can be adsorbed on the synthetic zeolite, which is the main cause of long time in the regeneration of the ammonia purifying apparatus, in a shorter time than the conventional method. It is possible to shorten the regeneration time of the purification apparatus. As a result, it takes longer to regenerate the other ammonia purification device than the time that can be purified by one ammonia purification device, eliminating the problem that purified ammonia cannot be continuously supplied to the gallium nitride compound semiconductor process. Can do.

The present invention relates to an ammonia purification device for removing impurities contained in crude ammonia by contacting the crude ammonia with a catalyst containing nickel as an active ingredient and synthetic zeolite, and a method for regenerating the ammonia purification device. Applies to
Hereinafter, the ammonia purifying apparatus and the regeneration method of the present invention will be described in detail with reference to FIGS. 1 to 3, but the present invention is not limited thereto. These drawings are configuration diagrams showing an example of the ammonia purifying apparatus of the present invention. (FIGS. 1 and 2 correspond to the invention of claim 1 and FIG. 3 corresponds to the invention of claim 2).

  As shown in FIG. 1 and FIG. 2, the purification apparatus of the first invention of the present application includes a catalyst cylinder 3 having a catalyst filling portion 1 containing nickel as an active component, an adsorption cylinder 4 having a synthetic zeolite filling portion 2, And a refining gas introduction line 7, a regeneration gas discharge line 8, and a pressure regulator 9 (for example, an opening / closing function) in the regeneration gas discharge line after circulating the synthetic zeolite. A pressure regulating valve equipped with an ammonia refining device.

  Further, as shown in FIG. 3, the refining apparatus of the second invention of the present application is a purifying cylinder 5 having a catalyst filling portion 1 and a synthetic zeolite filling portion 2 containing nickel as an active ingredient, and a crude ammonia introduction line. 6, a pressure regulator 9 (for example, a pressure regulating valve having an opening / closing function) in the regeneration gas introduction line 7, the regeneration gas discharge line 8, and the regeneration gas discharge line after circulating the synthetic zeolite. An ammonia purification apparatus comprising:

  In the present invention, the installation location of the pressure regulator 9 is not particularly limited as long as it is on the gas discharge port of the adsorption cylinder 4 or the purification cylinder 5 or the regeneration gas discharge line 8 on the downstream side of the gas discharge port. However, it is preferably provided on the regeneration gas discharge line 8 within 100 cm, more preferably within 50 cm from the gas discharge port. The regeneration gas introduction line 7 is connected to the inert gas introduction line 11, the hydrogen introduction line 12, the ammonia introduction line 13, etc. in the purifiers of the first and second inventions, and these gases or A mixed gas can be supplied to each cylinder as a regeneration gas. As ammonia which is one of the regeneration gases, purified ammonia obtained by the present invention can be used. The regenerative gas is discharged to the outside via the regenerative gas discharge line 8 after flowing through each cylinder. In each figure, the installation positions of the regeneration gas introduction line 7 and the regeneration gas discharge line 8 are not fixed, and for example, these installation positions can be exchanged.

  The catalyst containing nickel as an active ingredient used in the present invention is mainly composed of a nickel compound which is easily reduced, such as metallic nickel or nickel oxide. Further, a metal component other than nickel may contain a small amount of metal such as chromium, iron, cobalt, or copper. These nickels may be used alone or in a form supported on a catalyst carrier, but are usually supported on a catalyst carrier for the purpose of increasing the contact efficiency between the nickel surface and gas. It is preferable to use it in the form.

As a method for supporting nickel on a carrier, for example, carrier powders such as diatomaceous earth, alumina, silica alumina, aluminosilicate, and calcium silicate are dispersed in an aqueous solution of nickel salt, and an alkali is further added to add nickel on the carrier powder. The cake obtained by precipitating the components and then filtering and washing with water as necessary is dried at 120 to 150 ° C. and then baked at 300 ° C. or higher, and the baked product is pulverized, or NiCO ₃ , Ni (OH) ₂ Inorganic salts such as Ni (NO ₃ ) ₂ and organic salts such as NiC ₂ O ₄ and Ni (CH ₃ COO) ₂ are fired and pulverized, and then heat-resistant cement is mixed and fired. .

  These are usually formed into a molded body by extrusion molding, tableting molding or the like, and are used as they are or after being crushed to an appropriate size as required. As a molding method, a dry method or a wet method can be used, and a small amount of water, a lubricant, or the like may be used. Moreover, since there exists what is marketed as a nickel-type catalyst, you may use what was selected from them. The point is that reduced nickel, nickel oxide or the like is finely dispersed and has a large surface area and high contact efficiency with the gas.

The BET specific surface area of the catalyst containing nickel as an active ingredient is usually 10 to 300 m ² / g, preferably 30 to 250 m ² / g. Moreover, the content rate of nickel with respect to the whole catalyst is 5 to 95 wt% normally, Preferably it is 20 to 95 wt%. If the nickel content is less than 5 wt%, the ability to remove oxygen will be low, and if it is higher than 95 wt%, sintering may occur during hydrogen reduction and the activity may be reduced. Catalysts containing nickel as an active ingredient are usually subjected to hydrogen reduction in order to activate them before use. The hydrogen reduction can be performed, for example, by passing a mixed gas of hydrogen and nitrogen at about 350 ° C. or less at an empty cylinder linear velocity (LV) of about 5 cm / sec.

  The synthetic zeolite used in the present invention is a synthetic zeolite obtained by chemically substituting a part of sodium of a synthetic crystalline aluminosilicate hydrous sodium salt with potassium. This synthetic zeolite crystal has a large number of pores inside and is characterized by substantially uniform pore diameters. These synthetic zeolites are usually used after being molded into a spherical product having a diameter of 4 to 20 mesh, a columnar product having a diameter of 1.5 to 4 mm, and a height of 5 to 20 mm so that it can be used efficiently. In the present invention, preferably, synthetic zeolite having a pore diameter corresponding to 4 to 10 mm is used. Synthetic zeolite is usually activated while aerated with an inert gas at a temperature of about 200 to 350 ° C. before use.

  The regeneration method of the ammonia purification apparatus of the third invention of the present application is a method of regenerating the ammonia purification apparatus after purifying ammonia with the ammonia purification apparatus as shown in FIGS. In this step, an inert gas or a mixed gas of inert gas and ammonia is circulated through the adsorption cylinder to remove impurities from the synthetic zeolite, an inert gas is circulated through the adsorption cylinder and the synthetic zeolite is cooled, and the adsorption cylinder is pressurized. The regeneration method includes a step of passing the mixed gas of inert gas and ammonia and adsorbing ammonia to the synthetic zeolite.

  Further, in the regeneration method of the ammonia purifying apparatus according to the fourth invention of the present application, after purifying ammonia with an ammonia purifying apparatus as shown in FIG. 3, an inert gas or an inert gas and ammonia are put into a purifying cylinder under heating. A process of removing impurities from the synthetic zeolite by circulating a mixed gas, a process of circulating an inert gas through the purification cylinder and cooling the synthetic zeolite, and a mixture of inert gas and ammonia pressurized to the purification cylinder This is a regeneration method including a step of adsorbing ammonia on synthetic zeolite.

  In the present invention, during the purification of ammonia, mainly oxygen and carbon dioxide are removed from the crude ammonia by contact with a catalyst containing nickel as an active ingredient, and mainly from the crude ammonia by the contact with synthetic zeolite. Carbon and water are removed. Therefore, before regeneration of the ammonia purifier, oxygen and carbon dioxide are mainly captured by the catalyst containing nickel as active components, and carbon dioxide and water are mainly adsorbed by the synthetic zeolite. These impurities are efficiently removed by the regeneration method of the ammonia purifying apparatus of the present invention, and ammonia can be purified again.

  In the present invention, regeneration of a catalyst containing nickel as an active ingredient is performed by passing a hydrogen-containing gas from a regeneration gas introduction line to a catalyst containing nickel as an active ingredient under heating (150 to 350 ° C.), and using nickel as an active ingredient. This is done by removing impurities from the catalyst. In addition, regeneration of synthetic zeolite (1) circulates an inert gas or a mixed gas of inert gas and ammonia from the regeneration gas introduction line to the synthetic zeolite under heating (200 to 350 ° C.) to remove impurities from the synthetic zeolite. (2) Pass the inert gas from the regeneration gas introduction line to the synthetic zeolite and cool the synthetic zeolite. (3) Inert gas and ammonia pressurized from the regeneration gas introduction line to the synthetic zeolite The mixed gas is circulated, finally 100% ammonia is circulated, and the synthetic zeolite is adsorbed with ammonia.

  Regeneration of the ammonia purifier usually takes longer to regenerate the synthetic zeolite than to regenerate the catalyst containing nickel as an active ingredient. Further, the process (3) takes a long time even during regeneration of the synthetic zeolite. However, the present invention can greatly shorten the step (3). This is because, in the step (3), a large amount of heat of adsorption is generated when ammonia is adsorbed on the synthetic zeolite, but if the mixed gas of inert gas and ammonia is circulated in a pressurized state, it is inactive. This is because the circulation of the gas exhibits the effect of cooling, and ammonia has a high partial pressure even if the content is low, so that ammonia can be adsorbed on the synthetic zeolite in a short time.

  The introduction of the pressurized gas in the step (3) of the present invention can be carried out by a pressure regulator installed in the regeneration gas discharge line after the synthetic zeolite is distributed. The absolute pressure of the mixed gas when adsorbing ammonia on the synthetic zeolite is usually adjusted by a pressure regulator so as to be 120 to 500 kPa, preferably 150 to 400 kPa. Moreover, the content rate of ammonia contained in mixed gas is 5-50 vol% normally, Preferably it is 6-30 vol%. When the ammonia content is less than 5 vol%, it takes time to adsorb ammonia to the synthetic zeolite, and when the ammonia content exceeds 50 vol%, it is difficult to obtain a cooling effect due to the circulation of the inert gas. Further, the cylinder linear velocity (LV) of the mixed gas varies depending on the condition of the mixed gas to be introduced, the filling state of the synthetic zeolite, the operating conditions such as pressure, etc., and cannot be specified unconditionally, but is usually 100 cm / sec or less, preferably Is 30 cm / sec or less.

  EXAMPLES Next, although an Example demonstrates this invention concretely, this invention is not limited by these.

[Example 1]
(Production of ammonia purification equipment)
Ammonia purification having a structure as shown in FIG. 1 provided with two series of purification lines comprising a stainless steel catalyst cylinder (inner diameter 108.3 mm, length 1000 mm) and a stainless steel adsorption cylinder (inner diameter 108.3 mm, length 1000 mm). A device was made. Each catalyst cylinder is filled with a commercially available nickel catalyst so that the filling length is 400 mm, and each adsorption cylinder is filled with commercially available synthetic zeolite equivalent to 4 kg (Molecular Sieves 4A, manufactured by Union Carbide) with a filling length of 600 mm. It filled so that it might become. In addition, five thermocouples for temperature measurement were installed in the filled portion of the synthetic zeolite so as to be equidistant from the upstream side toward the downstream side.

  Next, for one of the purification lines, the nickel catalyst was heated to 250 ° C., and the nickel catalyst was reduced by flowing a mixed gas of hydrogen and nitrogen at normal pressure through the catalyst cylinder. In addition, the synthetic zeolite is heated to 300 ° C., and nitrogen is passed through the adsorption cylinder at normal pressure to activate the synthetic zeolite. After the heating is stopped and nitrogen is flown and cooled, A mixed gas of ammonia was flowed, and then 100% ammonia was flowed to adsorb ammonia on the synthetic zeolite. Furthermore, the same treatment was performed on the nickel catalyst and synthetic zeolite in the other purification line.

(Ammonia purification)
The industrial crude ammonia containing oxygen, carbon dioxide, and water as impurities was circulated through one of the purification lines at normal temperature, normal pressure, and a flow rate of 200 L / min to purify ammonia. After starting the purification process, the purified ammonia is sampled from the purified ammonia outlet at a predetermined time, and oxygen, carbon dioxide, and water in the gas are sampled using GC-TCD, GC-FID, and FT-IR. The concentration of was measured. As a result, a small amount of water was first detected (the adsorption cylinder was broken), so the purification line was switched to the other purification line.

(Regeneration of ammonia purification equipment)
The valves were switched so that the regeneration gas (hydrogen, nitrogen, ammonia) could be introduced from the regeneration gas introduction line to the ammonia-purified line, and the regeneration gas could be discharged from the ammonia-purified line to the regeneration gas discharge line. Next, the nickel catalyst is heated to 250 ° C., and a mixed gas of hydrogen and nitrogen (hydrogen 5 vol%, nitrogen 95 vol%) is flowed at a flow rate of 20 L / min at normal pressure for 8 hours from the regeneration gas introduction line. Reduction treatment was performed.

  Subsequently, the synthetic zeolite was heated to 300 ° C., and nitrogen was allowed to flow through the adsorption cylinder at a flow rate of 20 L / min at normal pressure for 12 hours to remove impurities from the synthetic zeolite. While adjusting the pressure regulating valve, a mixed gas of nitrogen and ammonia pressurized to the synthetic zeolite (absolute pressure 450 kPa, ammonia 20 vol%) was flowed to adsorb the ammonia to the synthetic zeolite. During this time, a large amount of mixed gas is allowed to flow under the condition that the temperature of the thermocouple installation position of the adsorption cylinder is 200 ° C. or less. Finally, 100% ammonia is allowed to flow, and ammonia is adsorbed onto the synthetic zeolite. Processing completed. As a result, it was found that the ammonia adsorption treatment on the synthetic zeolite took 11.2 hours.

[Example 2]
Using the same ammonia purifier as in Example 1, ammonia was purified in the same manner as in Example 1, and then the ammonia purifier was regenerated. The regeneration of the ammonia purifier was carried out in the same manner as in Example 1 except that the absolute pressure of the mixed gas of nitrogen and ammonia was lowered to 300 kPa by adjusting the pressure regulating valve in the adsorption process of ammonia on the synthetic zeolite. The device was regenerated. As a result, it took 11.8 hours for the ammonia adsorption treatment on the synthetic zeolite.

[Example 3]
Using the same ammonia purifier as in Example 1, ammonia was purified in the same manner as in Example 1, and then the ammonia purifier was regenerated. The regeneration of the ammonia purifier was carried out in the same manner as in Example 1 except that the ammonia concentration in the mixed gas of nitrogen and ammonia was increased to 30 vol% in the ammonia adsorption treatment on the synthetic zeolite. As a result, it took 12.3 hours for the adsorption of ammonia to the synthetic zeolite.

[Example 4]
Using the same ammonia purifier as in Example 1, ammonia was purified in the same manner as in Example 1, and then the ammonia purifier was regenerated. The regeneration of the ammonia purifier was performed in the same manner as in Example 1 except that the ammonia concentration in the mixed gas of nitrogen and ammonia was lowered to 10 vol% in the ammonia adsorption treatment on the synthetic zeolite. As a result, it took 11.5 hours for the adsorption treatment of ammonia on the synthetic zeolite.

[Comparative Example 1]
Using the same ammonia purifier as in Example 1, ammonia was purified in the same manner as in Example 1, and then the ammonia purifier was regenerated. The regeneration of the ammonia purifier was carried out in the same manner as in Example 1 except that, in the ammonia adsorption treatment on the synthetic zeolite, the pressure regulating valve was adjusted and the mixed gas of nitrogen and ammonia was lowered to normal pressure. As a result, it took 12.7 hours to adsorb ammonia onto the synthetic zeolite.

  As described above, the embodiment of the present invention can greatly reduce the adsorption time of ammonia to the synthetic zeolite in the regeneration of the ammonia purification apparatus, compared with the comparative example, so that the regeneration time of the ammonia purification apparatus can be shortened. is there.

Configuration diagram showing an example of an ammonia purification apparatus of the present invention The block diagram which shows an example of the refiner | purifier of ammonia other than FIG. 1 of this invention The block diagram which shows an example of the refiner | purifier of ammonia other than FIG. 1, FIG. 2 of this invention

DESCRIPTION OF SYMBOLS 1 Packing part of catalyst which uses nickel as an active ingredient 2 Packing part of synthetic zeolite 3 Catalyst cylinder 4 Adsorption cylinder 5 Purification cylinder 6 Introduction line of crude ammonia 7 Regeneration gas introduction line 8 Regeneration gas discharge line 9 Pressure regulator 10 Extraction port 11 Inert gas introduction line 12 Hydrogen introduction line 13 Ammonia introduction line

Claims (8)

  A purification apparatus for ammonia, comprising a catalyst cylinder having a catalyst filling portion containing nickel as an active ingredient, an adsorption cylinder having a filling portion of synthetic zeolite, and a crude ammonia introduction line, comprising a regeneration gas introduction line and regeneration gas discharge A purification apparatus for ammonia, comprising a pressure regulator in the regeneration gas discharge line after circulation of the line and the synthetic zeolite.   A refining cylinder having a catalyst-filling portion containing nickel as an active ingredient and a filling portion of synthetic zeolite, and an ammonia purifying apparatus comprising a crude ammonia introduction line, a regeneration gas introduction line, a regeneration gas discharge line, and a synthetic zeolite A device for purifying ammonia, comprising a pressure regulator in the regeneration gas discharge line after distribution.   A method for regenerating an ammonia purifying apparatus after purifying ammonia with the ammonia purifying apparatus according to claim 1, wherein an inert gas or a mixed gas of inert gas and ammonia is circulated through an adsorption cylinder under heating. Removing the impurities from the synthetic zeolite, circulating the inert gas through the adsorption cylinder and cooling the synthetic zeolite, and circulating a mixed gas of inert gas and ammonia pressurized in the adsorption cylinder A method for regenerating an ammonia purification device, comprising a step of adsorbing.   A method for regenerating an ammonia purifying apparatus after purifying ammonia by the ammonia purifying apparatus according to claim 2, wherein the inert gas or a mixed gas of the inert gas and ammonia is circulated through the purifying cylinder under heating. The process of removing impurities from the synthetic zeolite, the process of circulating an inert gas in the purification cylinder and cooling the synthetic zeolite, and the circulation of a mixed gas of inert gas and ammonia pressurized in the purification cylinder and passing ammonia into the synthetic zeolite A method for regenerating an ammonia purification device, comprising a step of adsorbing.   The absolute pressure of the pressurized inert gas and mixed gas of ammonia is adjusted with a pressure regulator so that it may become 120-500 kPa at the time of a contact with a synthetic zeolite. Method for regenerating ammonia purification equipment.   The regeneration method for an ammonia purifier according to claim 3 or 4, wherein the content of ammonia contained in the pressurized inert gas and ammonia mixed gas is 5 to 50 vol%.   The method for regenerating an ammonia purifier according to claim 3, further comprising a step of removing impurities from the catalyst containing nickel as an active component by flowing a hydrogen-containing gas through the catalyst cylinder under heating.   Furthermore, the regeneration method of the ammonia purification apparatus of Claim 4 including the process of distribute | circulating a hydrogen containing gas to a refinement | purification cylinder under a heating, and removing an impurity from the catalyst which uses nickel as an active ingredient.

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