CN114160121A - Multi-dimensional particle denitration catalyst and production method thereof - Google Patents
Multi-dimensional particle denitration catalyst and production method thereof Download PDFInfo
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- CN114160121A CN114160121A CN202111610381.1A CN202111610381A CN114160121A CN 114160121 A CN114160121 A CN 114160121A CN 202111610381 A CN202111610381 A CN 202111610381A CN 114160121 A CN114160121 A CN 114160121A
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- 239000003054 catalyst Substances 0.000 title claims abstract description 73
- 239000002245 particle Substances 0.000 title claims abstract description 70
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 40
- 239000000843 powder Substances 0.000 claims abstract description 58
- 238000001035 drying Methods 0.000 claims abstract description 54
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 52
- 239000012798 spherical particle Substances 0.000 claims abstract description 47
- MAKDTFFYCIMFQP-UHFFFAOYSA-N titanium tungsten Chemical compound [Ti].[W] MAKDTFFYCIMFQP-UHFFFAOYSA-N 0.000 claims abstract description 29
- 239000011230 binding agent Substances 0.000 claims abstract description 23
- 229910052751 metal Inorganic materials 0.000 claims abstract description 23
- 239000002184 metal Substances 0.000 claims abstract description 23
- 239000002994 raw material Substances 0.000 claims abstract description 23
- 229910052720 vanadium Inorganic materials 0.000 claims abstract description 23
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims abstract description 23
- 239000008367 deionised water Substances 0.000 claims abstract description 17
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 17
- 239000002270 dispersing agent Substances 0.000 claims abstract description 17
- 150000003839 salts Chemical class 0.000 claims abstract description 17
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 17
- 238000005096 rolling process Methods 0.000 claims abstract description 15
- 238000005303 weighing Methods 0.000 claims abstract description 15
- 238000007598 dipping method Methods 0.000 claims abstract description 9
- 238000003892 spreading Methods 0.000 claims description 12
- 230000007480 spreading Effects 0.000 claims description 12
- 238000000034 method Methods 0.000 claims description 10
- 230000008569 process Effects 0.000 claims description 7
- 239000012266 salt solution Substances 0.000 claims description 6
- 238000002791 soaking Methods 0.000 claims description 6
- 230000003197 catalytic effect Effects 0.000 abstract description 10
- 238000010248 power generation Methods 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000003546 flue gas Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 239000011149 active material Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/24—Chromium, molybdenum or tungsten
- B01J23/30—Tungsten
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Catalysts (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
Abstract
The embodiment of the invention provides a multi-dimensional particle denitration catalyst and a production method thereof, belonging to the technical field of catalysts. The multi-dimensional particle denitration catalyst comprises the following raw materials in parts by weight: 30-40% of light alumina seeds, 20-40% of alumina powder, 10-20% of titanium tungsten powder, 1-3% of vanadium metal salt, 1-4% of binder, 2-3% of synergist, 1-5% of dispersant and 5-15% of deionized water. The production method comprises the steps of quantitative weighing, rolling of spherical particles, drying and roasting, dipping, secondary drying and roasting and the like. The invention can effectively simplify the production process, reduce the production cost of the multi-dimensional particle denitration catalyst and improve the catalytic efficiency of the multi-dimensional particle denitration catalyst.
Description
Technical Field
The invention relates to the technical field of catalysts, and particularly relates to a multi-dimensional particle denitration catalyst and a production method thereof.
Background
The SCR catalyst in China is mainly applied to two fields of thermal power plants and automobile exhaust treatment at present. In the field of thermal power plants, although hydropower and nuclear power development technologies are gradually mature, new low-pollution or even pollution-free power generation is actively built in China, for China with large power consumption, thermal power generation still accounts for a large proportion, and a multi-dimensional particle denitration catalyst is required to be used in the thermal power generation process. Therefore, the amount of the multi-dimensional particle denitration catalyst is still large.
The SCR method is considered as the most effective flue gas denitration method among various flue gas denitration techniques. The selection of the catalyst is the focus of the SCR technology, and the catalytic efficiency varies with the reaction temperature required for different catalysts. Low temperature, high efficiency SCR catalysts have been the focus of research. The active materials of the SCR catalysts which are widely used at present include two main types of noble metals and metal oxides, and the materials used as the carriers of the SCR catalysts generally adopt materials with larger specific surface areas, such as activated carbon, metal oxides and molecular sieves. However, the denitration catalyst in the prior art has the defects of complex production process, low catalytic efficiency, higher purchase cost of production equipment, longer production period and the like.
Disclosure of Invention
The embodiment of the invention aims to provide a multi-dimensional particle denitration catalyst and a production method thereof, and aims to effectively simplify the production process, reduce the production cost of the multi-dimensional particle denitration catalyst and improve the catalytic efficiency of the multi-dimensional particle denitration catalyst.
In a first aspect, the multi-dimensional particle denitration catalyst provided by the embodiment of the invention comprises the following raw materials in parts by weight: 30-40% of light alumina seeds, 20-40% of alumina powder, 10-20% of titanium tungsten powder, 1-3% of vanadium metal salt, 1-4% of binder, 2-3% of synergist, 1-5% of dispersant and 5-15% of deionized water.
Preferably, the multi-dimensional particle denitration catalyst comprises the following raw materials in parts by weight: 40% of light alumina seeds, 30% of alumina powder, 10% of titanium tungsten powder, 1% of vanadium metal salt, 1.5% of binder, 2% of synergist, 2% of dispersant and 12% of deionized water.
Preferably, the multi-dimensional particle denitration catalyst comprises the following raw materials in parts by weight: 30% of light alumina seeds, 30% of alumina powder, 25% of titanium tungsten powder, 3% of vanadium metal salt, 2% of binder, 3% of synergist, 3% of dispersant and 7% of deionized water.
Preferably, the multi-dimensional particle denitration catalyst comprises the following raw materials in parts by weight: 35% of light alumina seeds, 35% of alumina powder, 12% of titanium tungsten powder, 2% of vanadium metal salt, 1% of binder, 2% of synergist, 2% of dispersant and 12% of deionized water.
Preferably, the multi-dimensional particle denitration catalyst comprises the following raw materials in parts by weight: 25% of light alumina seeds, 40% of alumina powder, 15% of titanium tungsten powder, 3% of vanadium metal salt, 2% of binder, 3% of synergist, 3% of dispersant and 9% of deionized water.
In a second aspect, the embodiment of the present invention provides a production method of a multi-dimensional granular denitration catalyst, which is used for preparing the multi-dimensional granular denitration catalyst, and the production method includes the following steps:
quantitative weighing: weighing all the raw materials according to a pre-designed proportion;
rolling the spherical particles: adding the light alumina seeds into a ball rolling machine, adding the alumina powder firstly, then adding the titanium tungsten powder, and continuously adding the binder and the synergist in the process of adding the alumina powder and the titanium tungsten powder to obtain ball particles;
drying and roasting: uniformly spreading rolled spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying the spherical particles, then roasting the spherical particles in a furnace for 6-10 hours, and controlling the temperature at 550 ℃;
dipping: soaking the baked and cooled spherical particles in a vanadium metal salt solution for 2 hours;
secondary drying and roasting: uniformly spreading the soaked spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying, then roasting in a furnace for 6-10 hours, and controlling the temperature at 500 ℃ to obtain the multi-dimensional particle denitration catalyst.
The invention has the beneficial effects that: the embodiment of the invention provides a multi-dimensional particle denitration catalyst and a production method thereof, wherein the multi-dimensional particle denitration catalyst comprises the following raw materials in parts by weight: 30% -40% of light alumina seeds, 20% -40% of alumina powder, 10% -20% of titanium tungsten powder, 1% -3% of vanadium metal salt, 1% -4% of binder, 2% -3% of synergist, 1% -5% of dispersing agent and 5% -15% of deionized water, so that the catalytic efficiency of the multi-dimensional particle denitration catalyst can be effectively improved. In addition, the production method comprises the steps of quantitative weighing, rolling of spherical particles, drying roasting, dipping, secondary drying roasting and the like, so that the production process can be effectively simplified, and the production cost of the multi-dimensional particle denitration catalyst is reduced.
In order to make the aforementioned and other objects, features and advantages of the invention more comprehensible, preferred embodiments accompanied with figures are described in detail below.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention more apparent, the technical solutions of the embodiments of the present invention will be clearly and completely described below, and it is apparent that the described embodiments are some embodiments of the present invention, but not all embodiments. All other embodiments, which can be obtained by a person skilled in the art without any inventive step based on the embodiments of the present invention, are within the scope of the present invention. Thus, the detailed description of the embodiments of the present invention provided below is not intended to limit the scope of the invention as claimed, but is merely representative of selected embodiments of the invention.
Example 1
The production method of the multi-dimensional particle denitration catalyst provided by the embodiment of the invention can comprise the following steps:
quantitative weighing: weighing all the raw materials according to a pre-designed proportion.
Rolling the spherical particles: and adding the light alumina seeds into a ball rolling machine, adding the alumina powder firstly, then adding the titanium tungsten powder, and continuously adding the binder and the synergist in the process of adding the alumina powder and the titanium tungsten powder to obtain the ball particles.
Drying and roasting: uniformly spreading rolled spherical particles, putting the spherical particles into a drying room to accelerate drying for 2-3 days, completely drying the spherical particles, then roasting the spherical particles in a furnace for 6-10 hours, and controlling the temperature at 550 ℃.
Dipping: and soaking the baked and cooled ball particles in a vanadium metal salt solution for 2 hours.
Secondary drying and roasting: uniformly spreading the soaked spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying, then roasting in a furnace for 6-10 hours, and controlling the temperature at 500 ℃ to obtain the multi-dimensional particle denitration catalyst.
The production method of the multi-dimensional particle denitration catalyst can effectively simplify the production process and reduce the production cost of the multi-dimensional particle denitration catalyst.
In the embodiment of the invention, the multi-dimensional particle denitration catalyst can comprise the following raw materials in parts by weight: 40% of light alumina seeds, 30% of alumina powder, 10% of titanium tungsten powder, 1% of vanadium metal salt, 1.5% of binder, 2% of synergist, 2% of dispersant and 12% of deionized water. The multi-dimensional particle denitration catalyst can improve the catalytic efficiency of the multi-dimensional particle denitration catalyst.
Example 2
The production method of the multi-dimensional particle denitration catalyst provided by the embodiment of the invention can comprise the following steps:
quantitative weighing: weighing all the raw materials according to a pre-designed proportion.
Rolling the spherical particles: and adding the light alumina seeds into a ball rolling machine, adding the alumina powder firstly, then adding the titanium tungsten powder, and continuously adding the binder and the synergist in the process of adding the alumina powder and the titanium tungsten powder to obtain the ball particles.
Drying and roasting: uniformly spreading rolled spherical particles, putting the spherical particles into a drying room to accelerate drying for 2-3 days, completely drying the spherical particles, then roasting the spherical particles in a furnace for 6-10 hours, and controlling the temperature at 550 ℃.
Dipping: and soaking the baked and cooled ball particles in a vanadium metal salt solution for 2 hours.
Secondary drying and roasting: uniformly spreading the soaked spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying, then roasting in a furnace for 6-10 hours, and controlling the temperature at 500 ℃ to obtain the multi-dimensional particle denitration catalyst.
The production method of the multi-dimensional particle denitration catalyst can effectively simplify the production process and reduce the production cost of the multi-dimensional particle denitration catalyst.
In the embodiment of the invention, the multi-dimensional particle denitration catalyst can comprise the following raw materials in parts by weight: 30% of light alumina seeds, 30% of alumina powder, 25% of titanium tungsten powder, 3% of vanadium metal salt, 2% of binder, 3% of synergist, 3% of dispersant and 7% of deionized water. The multi-dimensional particle denitration catalyst can improve the catalytic efficiency of the multi-dimensional particle denitration catalyst.
Example 3
The production method of the multi-dimensional particle denitration catalyst provided by the embodiment of the invention can comprise the following steps:
quantitative weighing: weighing all the raw materials according to a pre-designed proportion.
Rolling the spherical particles: and adding the light alumina seeds into a ball rolling machine, adding the alumina powder firstly, then adding the titanium tungsten powder, and continuously adding the binder and the synergist in the process of adding the alumina powder and the titanium tungsten powder to obtain the ball particles.
Drying and roasting: uniformly spreading rolled spherical particles, putting the spherical particles into a drying room to accelerate drying for 2-3 days, completely drying the spherical particles, then roasting the spherical particles in a furnace for 6-10 hours, and controlling the temperature at 550 ℃.
Dipping: and soaking the baked and cooled ball particles in a vanadium metal salt solution for 2 hours.
Secondary drying and roasting: uniformly spreading the soaked spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying, then roasting in a furnace for 6-10 hours, and controlling the temperature at 500 ℃ to obtain the multi-dimensional particle denitration catalyst.
The production method of the multi-dimensional particle denitration catalyst can effectively simplify the production process and reduce the production cost of the multi-dimensional particle denitration catalyst.
In the embodiment of the invention, the multi-dimensional particle denitration catalyst can comprise the following raw materials in parts by weight: 35% of light alumina seeds, 35% of alumina powder, 12% of titanium tungsten powder, 2% of vanadium metal salt, 1% of binder, 2% of synergist, 2% of dispersant and 12% of deionized water. The multi-dimensional particle denitration catalyst can improve the catalytic efficiency of the multi-dimensional particle denitration catalyst.
Example 4
The production method of the multi-dimensional particle denitration catalyst provided by the embodiment of the invention can comprise the following steps:
quantitative weighing: weighing all the raw materials according to a pre-designed proportion.
Rolling the spherical particles: and adding the light alumina seeds into a ball rolling machine, adding the alumina powder firstly, then adding the titanium tungsten powder, and continuously adding the binder and the synergist in the process of adding the alumina powder and the titanium tungsten powder to obtain the ball particles.
Drying and roasting: uniformly spreading rolled spherical particles, putting the spherical particles into a drying room to accelerate drying for 2-3 days, completely drying the spherical particles, then roasting the spherical particles in a furnace for 6-10 hours, and controlling the temperature at 550 ℃.
Dipping: and soaking the baked and cooled ball particles in a vanadium metal salt solution for 2 hours.
Secondary drying and roasting: uniformly spreading the soaked spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying, then roasting in a furnace for 6-10 hours, and controlling the temperature at 500 ℃ to obtain the multi-dimensional particle denitration catalyst.
The production method of the multi-dimensional particle denitration catalyst can effectively simplify the production process and reduce the production cost of the multi-dimensional particle denitration catalyst.
In the embodiment of the invention, the multi-dimensional particle denitration catalyst can comprise the following raw materials in parts by weight: 25% of light alumina seeds, 40% of alumina powder, 15% of titanium tungsten powder, 3% of vanadium metal salt, 2% of binder, 3% of synergist, 3% of dispersant and 9% of deionized water. The multi-dimensional particle denitration catalyst can improve the catalytic efficiency of the multi-dimensional particle denitration catalyst.
In summary, the embodiment of the present invention provides a multi-dimensional particle denitration catalyst and a production method thereof, wherein the multi-dimensional particle denitration catalyst comprises the following raw materials in parts by weight: 30% -40% of light alumina seeds, 20% -40% of alumina powder, 10% -20% of titanium tungsten powder, 1% -3% of vanadium metal salt, 1% -4% of binder, 2% -3% of synergist, 1% -5% of dispersing agent and 5% -15% of deionized water, so that the catalytic efficiency of the multi-dimensional particle denitration catalyst can be effectively improved. In addition, the production method comprises the steps of quantitative weighing, rolling of spherical particles, drying roasting, dipping, secondary drying roasting and the like, so that the production process can be effectively simplified, and the production cost of the multi-dimensional particle denitration catalyst is reduced.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (6)
1. The multi-dimensional particle denitration catalyst is characterized by comprising the following raw materials in parts by weight: 30-40% of light alumina seeds, 20-40% of alumina powder, 10-20% of titanium tungsten powder, 1-3% of vanadium metal salt, 1-4% of binder, 2-3% of synergist, 1-5% of dispersant and 5-15% of deionized water.
2. The multi-dimensional particle denitration catalyst according to claim 1, comprising the following raw materials in parts by weight: 40% of light alumina seeds, 30% of alumina powder, 10% of titanium tungsten powder, 1% of vanadium metal salt, 1.5% of binder, 2% of synergist, 2% of dispersant and 12% of deionized water.
3. The multi-dimensional particle denitration catalyst according to claim 1, comprising the following raw materials in parts by weight: 30% of light alumina seeds, 30% of alumina powder, 25% of titanium tungsten powder, 3% of vanadium metal salt, 2% of binder, 3% of synergist, 3% of dispersant and 7% of deionized water.
4. The multi-dimensional particle denitration catalyst according to claim 1, comprising the following raw materials in parts by weight: 35% of light alumina seeds, 35% of alumina powder, 12% of titanium tungsten powder, 2% of vanadium metal salt, 1% of binder, 2% of synergist, 2% of dispersant and 12% of deionized water.
5. The multi-dimensional particle denitration catalyst according to claim 1, comprising the following raw materials in parts by weight: 25% of light alumina seeds, 40% of alumina powder, 15% of titanium tungsten powder, 3% of vanadium metal salt, 2% of binder, 3% of synergist, 3% of dispersant and 9% of deionized water.
6. A production method of a multi-dimensional particulate denitration catalyst for preparing the multi-dimensional particulate denitration catalyst according to any one of claims 1 to 5, comprising the steps of:
quantitative weighing: weighing all the raw materials according to a pre-designed proportion;
rolling the spherical particles: adding the light alumina seeds into a ball rolling machine, adding the alumina powder firstly, then adding the titanium tungsten powder, and continuously adding the binder and the synergist in the process of adding the alumina powder and the titanium tungsten powder to obtain ball particles;
drying and roasting: uniformly spreading rolled spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying the spherical particles, then roasting the spherical particles in a furnace for 6-10 hours, and controlling the temperature at 550 ℃;
dipping: soaking the baked and cooled spherical particles in a vanadium metal salt solution for 2 hours;
secondary drying and roasting: uniformly spreading the soaked spherical particles, putting the spherical particles into a drying room for accelerated drying for 2-3 days, completely drying, then roasting in a furnace for 6-10 hours, and controlling the temperature at 500 ℃ to obtain the multi-dimensional particle denitration catalyst.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114602455A (en) * | 2022-03-27 | 2022-06-10 | 山东亮剑环保新材料有限公司 | Foaming honeycomb denitration catalyst and production method thereof |
| CN114602459A (en) * | 2022-03-27 | 2022-06-10 | 山东亮剑环保新材料有限公司 | Composite denitration catalyst and production method thereof |
| CN114931943A (en) * | 2022-05-18 | 2022-08-23 | 山东亮剑环保新材料有限公司 | SCR denitration catalyst and production method thereof |
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