CN114907186A - Method for directly preparing methanol from carbon dioxide and hydrogen - Google Patents
Method for directly preparing methanol from carbon dioxide and hydrogen Download PDFInfo
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- CN114907186A CN114907186A CN202210433699.5A CN202210433699A CN114907186A CN 114907186 A CN114907186 A CN 114907186A CN 202210433699 A CN202210433699 A CN 202210433699A CN 114907186 A CN114907186 A CN 114907186A
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
- C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
- C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
- C07C29/152—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases characterised by the reactor used
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
- C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
- C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
- C07C29/1516—Multisteps
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
Abstract
The invention discloses a method for directly preparing methanol from carbon dioxide and hydrogen, belonging to the technical field of chemical industry. The method of the invention comprises the following steps: mixing the hydrogen/carbon dioxide feed gas with the compressed recycle gas to obtain a raw material mixed gas, and preheating the raw material mixed gas to be divided into a first tower inlet gas and a second tower inlet gas; preheating first tower gas entering the tower after passing through a shell side annular gap of the synthesis tower, and reacting the first tower gas entering the tower, and preheating second tower gas entering the tower and reacting the second tower gas entering the first reaction bed; the first bed outlet gas is preheated and enters the second reaction bed layer for reaction; the outlet gas of the second bed enters a third reaction bed layer for reaction after being preheated by the second tower inlet gas; and (3) preheating the raw material mixed gas by the outlet gas of the three beds, then carrying out gas-liquid separation, introducing the separated liquid into a next methanol flash evaporation process, mixing the separated gas serving as compressed circulating gas with the pressurized hydrogen/carbon dioxide raw material gas to obtain a raw material mixed gas, and reacting again. The invention has the advantages of low investment and high single-pass conversion rate of carbon dioxide.
Description
Technical Field
The invention belongs to the technical field of chemical industry, and particularly relates to a method for directly preparing methanol from carbon dioxide and hydrogen.
Background
Carbon dioxide is a cheap, easily-obtained and environment-friendly renewable carbon resource, and methanol is a basic organic chemical raw material and plays a very important role in industrial production. Methanol can be directly used as an excellent fuel, and can also be used for chemical products such as synthetic fibers, formaldehyde, plastics, medicines, pesticides, dyes, synthetic proteins and the like. The carbon dioxide is used as raw material, and the CO is produced by hydrogenation to produce methanol 2 One of the important ways of scientific resource utilization and greenhouse gas emission reduction has great significance on green and sustainable development and is highly fit with the double-carbon target of carbon peak reaching and carbon neutralization in China. In the prior art, the technology for preparing methanol by carbon dioxide hydrogenation mainly comprises the traditional direct hydrogenation method, the traditional photocatalytic reduction method, the traditional electro-catalytic reduction method and the traditional biological catalytic reduction method. The method capable of realizing industrial production is mainly based on a direct hydrogenation method. A typical production process for preparing methanol by directly hydrogenating carbon dioxide has the defects of high investment, low carbon dioxide conversion rate and high power consumption, a methanol synthesis tower serving as a core device is usually a shell-and-tube reactor, a catalyst is filled in the tube layer, and water vapor flows away from the shell side. Therefore, it is an urgent problem to be solved by those skilled in the art to provide a method for preparing methanol by direct hydrogenation of carbon dioxide with low investment and high carbon dioxide conversion rate.
Disclosure of Invention
The present invention aims to provide a method for directly preparing methanol from carbon dioxide and hydrogen, so as to solve at least part of the problems.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
the invention provides a method for directly preparing methanol from carbon dioxide and hydrogen, which is carried out by adopting a carbon dioxide hydrogenation synthesis tower, wherein three reaction bed layers and two shell-and-tube heat exchangers are arranged in the carbon dioxide hydrogenation synthesis tower, and the method comprises the following steps:
step 1, mixing the pressurized hydrogen/carbon dioxide raw material gas with the pressurized compressed recycle gas to obtain a raw material mixed gas, and dividing the raw material mixed gas into two parts, namely a first tower inlet gas and a second tower inlet gas after preheating;
and 5, preheating the raw material mixed gas by using the outlet gas of the three beds as a heat source, cooling the outlet gas of the three beds after heat exchange, carrying out gas-liquid separation, introducing the separated liquid into a next methanol flash evaporation process, compressing the separated gas, mixing the compressed gas serving as a compressed circulating gas with the pressurized hydrogen/carbon dioxide raw material gas to obtain the raw material mixed gas, and reacting again.
The invention divides the raw material gas mixture into one strand of annular space which enters the synthesis tower to protect the synthesis tower. The outlet gas of each bed layer which is not completely reacted is used as the inlet gas of a lower bed layer for continuous reaction, and the gas which is not completely reacted and goes out of the tower is used as the circulating gas for reaction again after gas-liquid separation, so that the raw material resources are effectively utilized; the production cost is reduced.
The invention adopts the outlet gas of the bed layer to preheat the inlet gas, effectively utilizes the heat energy and saves the energy.
In some embodiments of the invention, the pressurized hydrogen/carbon dioxide feed gas has a molar ratio of hydrogen (pure) to carbon dioxide (pure) of 3: 1.
In some embodiments of the invention, the pressure of the pressurized hydrogen/carbon dioxide feed gas is 5.0-10.0 MPa; the pressure of the compressed circulating gas after pressurization is 5.0-10.0 MPa.
In some embodiments of the invention, the volume ratio of the pressurized compressed recycle gas to the pressurized hydrogen/carbon dioxide feed gas is 3-5: 1.
In some embodiments of the present invention, in step 1, one of the raw material mixed gases is separated as a cold shock gas, and directly enters the first reaction bed from the top of the synthesis tower, so as to adjust the inlet temperature of the first bed.
In some embodiments of the invention, the operating pressure in the carbon dioxide hydrogenation synthesis tower is 5.0-10.0 MPa, and the operating temperature is 210-290 ℃.
In some embodiments of the invention, the inlet gas of each bed is preheated to 210-250 ℃ and then enters each bed for reaction.
In some embodiments of the present invention, in step 5, a part of the separated gas is extracted to form purge gas for export, and the rest gas is compressed and used as compressed recycle gas.
In some embodiments of the invention, the separated liquid enters a methanol flash drum, and after flash evaporation, crude methanol and flash vapor are obtained.
Compared with the prior art, the invention has the following beneficial effects:
the invention has scientific design and ingenious conception, and the raw material mixed gas is divided into a strand of cold shock gas, and the rest of mixed gas is divided into a first tower gas and a second tower gas after being preheated, wherein the first tower gas enters the annular space of the carbon dioxide hydrogenation synthesis tower to protect the synthesis tower. The catalyst filling amount of the synthesis tower is large, and the resistance is reduced. The synthesis tower outlet gas is cooled by the inlet and outlet heat exchangers, and then enters a cooling separator integrating cooling and separation into a whole to obtain circulating gas and purge gas, and the liquid is subjected to flash evaporation to obtain crude methanol.
The invention arranges a plurality of reaction beds and heat exchangers in the carbon dioxide hydrogenation synthesis tower, thereby effectively utilizing heat. The outlet gas of each bed layer which is not completely reacted is used as the inlet gas of a lower bed layer for continuous reaction, and the tower gas which is not completely reacted is used as the circulating gas for reaction again after gas-liquid separation, so that the raw material resources are effectively utilized; the production cost is reduced.
The invention arranges a plurality of reaction bed layer heat exchangers in one synthesis tower, thus reducing the occupied area and the equipment investment.
The method for preparing the methanol from the carbon dioxide and the hydrogen has the advantages of high one-way conversion rate, reduced operation resistance, small circulation amount and low power consumption of the circulator, and is particularly suitable for preparing the methanol from the carbon dioxide and the hydrogen.
Drawings
FIG. 1 is a schematic structural diagram of an apparatus for directly preparing methanol from carbon dioxide and hydrogen in example 1 of the present invention.
FIG. 2 is a schematic structural diagram of an apparatus for directly preparing methanol from carbon dioxide and hydrogen in example 2 of the present invention.
FIG. 3 is a schematic structural diagram of a reaction bed and a heat exchanger in a carbon dioxide hydrogenation synthesis tower according to example 1 of the present invention.
FIG. 4 is a schematic structural diagram of the reaction bed and the heat exchanger inside the carbon dioxide hydrogenation synthesis tower of example 2 of the present invention.
Wherein, the names corresponding to the reference numbers are:
the system comprises a 1-carbon dioxide hydrogenation synthesis tower, a 2-inlet-outlet heat exchanger, a 3-cooling separator, a 4-recycle gas compressor, a 5-methanol flash tank, a 6-first reaction bed, a 7-second reaction bed, an 8-third reaction bed, a 9-upper heat exchanger, a 10-lower heat exchanger, a 101-raw gas conveying pipe, a 102-cold shock gas conveying pipe, a 103-first inlet main pipe, a 104-second inlet main pipe, a 105-outlet main pipe, a 106-compression recycle gas conveying pipe, a 107-recycle gas conveying pipe, a 108-purge gas external conveying pipe, a 109-flash gas external conveying pipe and a 110-crude methanol external conveying pipe.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail below with reference to the accompanying drawings. It is to be understood that the described embodiments are merely exemplary of the invention, and not restrictive of the full scope of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
A method for directly preparing methanol from carbon dioxide and hydrogen is carried out by adopting a carbon dioxide hydrogenation synthesis tower, wherein three reaction beds and two shell-and-tube heat exchangers are arranged in the carbon dioxide hydrogenation synthesis tower, and the method comprises the following steps:
step 1, mixing the pressurized hydrogen/carbon dioxide raw material gas with the pressurized compressed recycle gas to obtain a raw material mixed gas, and dividing the raw material mixed gas into two parts, namely a first tower inlet gas and a second tower inlet gas after preheating;
and 5, taking the outlet gas of the three beds as a heat source raw material mixed gas, cooling the outlet gas of the three beds after heat exchange, carrying out gas-liquid separation, enabling the separated liquid to enter a next methanol flash evaporation process, compressing the separated gas, mixing the compressed gas serving as a compressed circulating gas with the pressurized hydrogen/carbon dioxide raw material gas to obtain a raw material mixed gas, and participating in the reaction again.
The molar ratio of hydrogen to carbon dioxide in the pressurized hydrogen/carbon dioxide feed gas was 3: 1.
The pressure of the pressurized hydrogen/carbon dioxide raw material gas is 5.0-10.0 MPa; the pressure of the compressed circulating gas after pressurization is 5.0-10.0 MPa.
The volume ratio of the compressed recycle gas after pressurization to the hydrogen/carbon dioxide raw material gas after pressurization is 3-5: 1.
The operating pressure in the carbon dioxide hydrogenation synthesis tower is 5.0-10.0 MPa, and the operating temperature is 210-290 ℃.
And preheating inlet gas of each bed layer to 210-250 ℃, and then entering each bed layer for reaction.
In the step 5, a part of the separated gas is extracted to form purge gas for output, and the rest gas is compressed and then used as compressed circulating gas.
And the separated liquid enters a methanol flash evaporation tank, and crude methanol and flash evaporation gas are obtained after flash evaporation.
Example 1
As shown in fig. 1 and 3, this embodiment discloses an apparatus for directly preparing methanol from carbon dioxide and hydrogen, which includes an inlet/outlet heat exchanger 2, a cooling separator 3, a recycle gas compressor 4, a methanol flash tank 5, and a carbon dioxide hydrogenation synthesis tower 1 with an annular space.
The shell pass inlet of the inlet-outlet heat exchanger 2 is connected with a raw material gas conveying pipe 101, and the shell pass outlet of the inlet-outlet heat exchanger 2 is connected with the bottom annular gap inlet and the top gas inlet of the carbon dioxide hydrogenation synthesis tower 1 through a first tower inlet main line pipe 103 and a second tower inlet main line pipe 104 respectively.
The carbon dioxide hydrogenation synthesis tower 1 is internally provided with three reaction beds and two shell-and-tube heat exchangers, and the three reaction beds are arranged in a radial direction. The shell side inlet of an upper heat exchanger 9 positioned at the upper part of the carbon dioxide hydrogenation synthetic tower 1 is connected with the outlet of the annular gas, the shell side outlet of the upper heat exchanger 9 is connected with the gas inlet of the first reaction bed layer 6, the tube side inlet of the upper heat exchanger 9 is connected with the gas outlet of the first reaction bed layer 6, and the tube side outlet of the upper heat exchanger 9 is connected with the gas inlet of the second reaction bed layer 7;
a shell pass inlet of a lower heat exchanger 10 positioned at the lower part of the carbon dioxide hydrogenation synthetic tower 1 is connected with a gas inlet pipeline of the carbon dioxide hydrogenation synthetic tower 1, and a shell pass outlet of the shell pass inlet is connected with a gas inlet of the first reaction bed layer 6;
the gas outlet of the second reaction bed layer 7 is connected with the tube side inlet of the lower heat exchanger 10, the tube side outlet of the lower heat exchanger 10 is connected with the gas inlet of the third reaction bed layer 8, and the gas outlet of the third reaction bed layer 8 is connected with the tube side inlet of the inlet-outlet heat exchanger 2 through a tower outlet main line pipe 105.
The tube side outlet of the inlet-outlet heat exchanger 2 is connected with the cooling separator 3 for gas-liquid separation of the reaction gas.
The outlet of the cooling separator 3 is connected to the inlet of the recycle gas compressor 4 via a recycle gas duct 107, and a purge gas outflow pipe 108 is connected to the recycle gas duct 107.
The compressed gas outlet of the recycle gas compressor 4 is connected with the raw material gas conveying pipeline 101 through a compressed recycle gas conveying pipe 106.
The liquid outlet of the cooling separator 3 is connected with a methanol flash tank 5. The methanol flash tank 5 is connected to a flash gas outward transfer pipe 109 and a crude methanol outward transfer pipe 110.
Example 2
As shown in fig. 2 and 4, this embodiment discloses a device for directly preparing methanol from carbon dioxide and hydrogen, and compared with the device of embodiment 1, this embodiment further includes a quench gas delivery pipe 102, one end of the quench gas delivery pipe 102 is connected to the raw material gas delivery pipe 101, and the other end is connected to the inlet of the first reaction bed layer through the top inlet of the carbon dioxide hydrogenation synthesis tower 1, so as to input part of the raw material gas mixture as quench gas into the first reaction bed layer and adjust the temperature of the inlet gas of the first reaction bed layer.
Example 3
This example discloses a method for preparing methanol using the apparatus of example 2, specifically:
step 1. pressurized Hydrogen/carbon dioxide feed gas S1 (about 4 ten thousand Nm) 3 H) and pressurized compressed recycle gas S6 (about 15 ten thousand Nm) 3 H) mixing, separating out a small stream of cold shock gas S1B, directly feeding into the first reaction bed layer of the carbon dioxide hydrogenation synthetic tower 1, and using forRegulating the temperature of the inlet gas of the first bed layer of the synthesis tower, heating the rest mixed raw material gas S1A to about 210 ℃ through the inlet-outlet heat exchanger 2, and then dividing the gas into first tower inlet gas S2A and second tower inlet gas S2B. In the pressurized hydrogen/carbon dioxide raw material gas, the molar ratio of hydrogen (pure) to carbon dioxide (pure) is 3:1, the pressure of the pressurized hydrogen/carbon dioxide raw material gas is 9.1 MPa; the pressure of the compressed recycle gas after pressurization was 9.1 MPa.
And 2, after passing through an annular space on the shell side of the carbon dioxide hydrogenation synthesis tower 1, the first tower gas S2A enters an upper heat exchanger 9 in the carbon dioxide hydrogenation synthesis tower 1 for preheating, and then enters a first bed layer 6 together with a second tower gas S2B preheated by a lower heat exchanger 10 in the carbon dioxide hydrogenation synthesis tower 1 for methanol synthesis reaction.
And 4, the outlet gas of the second bed enters a lower heat exchanger 10, after the second tower inlet gas S2B is preheated, the outlet gas of the second bed is used as inlet gas of a third bed to enter a third bed 8 of the carbon dioxide hydrogenation synthetic tower 1, the outlet gas of the third bed, namely synthetic tower outlet gas S3, the pressure is 8.8MP (G), the temperature is about 250 ℃, and the methanol content is about 6% (v).
And 5, the outlet gas S3 of the synthesis tower enters an inlet-outlet heat exchanger 2, the mixed gas S1A at the inlet of the carbon dioxide hydrogenation synthesis tower 1 is preheated, the cooled gas S4 enters a cooling separator 3 for cooling and separating methanol, and the outlet gas S5 of the cooling separator and the outlet liquid L1 of the cooling separator are obtained.
To prevent inert gas buildup, a vent partial purge gas S5A (about 1500 Nm) is bled from the cold separator outlet column gas S5 (about 1500 Nm) 3 H), the purge gas can be further recycled hydrogen to make up for fresh gas or used for other purposes, and the rest is used as recycle gas S5B.
The recycle gas S5B is pressurized by a recycle gas compressor 4 (the shaft power of the recycle compressor is about 350KW) to obtain pressurized compressed recycle gas S6, S6 and pressurized hydrogen/carbon dioxide feed gas S1 which are used as reaction gases.
The cooled separator outlet liquid L1 was fed to methanol flash drum 5 to obtain crude methanol L3 (about 20t/h), flash gas S7 (about 360 Nm/h) 3 And/h) comprehensive utilization after further treatment.
Finally, it should be noted that: the above embodiments are merely preferred embodiments of the present invention to illustrate the technical solutions of the present invention, and not to limit the technical solutions, and certainly not to limit the patent scope of the present invention. However, all the insubstantial changes or modifications made without departing from the spirit and spirit of the invention are intended to be included within the scope of the invention; in addition, the technical scheme of the invention is directly or indirectly applied to other related technical fields, and the technical scheme is included in the patent protection scope of the invention.
Claims (9)
1. A method for directly preparing methanol from carbon dioxide and hydrogen is characterized by being carried out by adopting a carbon dioxide hydrogenation synthesis tower, wherein three reaction beds and two shell-and-tube heat exchangers are arranged in the carbon dioxide hydrogenation synthesis tower, and the method comprises the following steps:
step 1, mixing the pressurized hydrogen/carbon dioxide raw material gas with the pressurized compressed recycle gas to obtain a raw material mixed gas, and dividing the raw material mixed gas into two parts, namely a first tower inlet gas and a second tower inlet gas after preheating;
step 2, preheating the first tower gas in the tower after passing through a shell side annular space of the carbon dioxide hydrogenation synthesis tower, and then reacting in a first reaction bed layer, and preheating the second tower gas in the tower, and then reacting in the first reaction bed layer;
step 3, preheating first tower inlet gas by using first bed outlet gas as a heat source, and allowing the first bed outlet gas subjected to heat exchange to enter a second reaction bed layer for reaction as second bed inlet gas;
step 4, preheating second tower inlet gas by using second bed outlet gas as a heat source, and allowing the second bed outlet gas after heat exchange to enter a third reaction bed layer for reaction as third bed inlet gas;
and 5, preheating the raw material mixed gas by using the outlet gas of the three beds as a heat source, cooling the outlet gas of the three beds after heat exchange, carrying out gas-liquid separation, introducing the separated liquid into a next methanol flash evaporation process, compressing the separated gas, mixing the compressed gas serving as a compressed circulating gas with the pressurized hydrogen/carbon dioxide raw material gas to obtain the raw material mixed gas, and reacting again.
2. The method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein the molar ratio of hydrogen to carbon dioxide in the pressurized hydrogen/carbon dioxide feed gas is 3: 1.
3. the method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein the pressure of the pressurized hydrogen/carbon dioxide raw gas is 5.0-10.0 MPa; the pressure of the compressed circulating gas after pressurization is 5.0-10.0 MPa.
4. The method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein the volume ratio of the compressed recycle gas after pressurization to the hydrogen/carbon dioxide raw material gas after pressurization is 3-5: 1.
5. The method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein in the step 1, a strand of the raw material mixed gas is separated as cold shock gas and directly enters the first reaction bed layer from the top of the synthesis tower, and the temperature of the inlet gas of the first reaction bed layer is adjusted.
6. The method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein the operating pressure in the carbon dioxide hydrogenation synthesis tower is 5.0-10.0 MPa, and the operating temperature is 210-290 ℃.
7. The method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein the inlet gas of each bed is preheated to 210-250 ℃ and then enters each bed for reaction.
8. The method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein in step 5, a part of the separated gas is extracted to form purge gas for export, and the rest gas is compressed and used as compressed recycle gas.
9. The method for directly preparing methanol from carbon dioxide and hydrogen according to claim 1, wherein the separated liquid enters a methanol flash tank and is flashed to obtain crude methanol and flash gas.
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| CN202210433699.5A CN114907186A (en) | 2022-04-24 | 2022-04-24 | Method for directly preparing methanol from carbon dioxide and hydrogen |
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| CN202210433699.5A CN114907186A (en) | 2022-04-24 | 2022-04-24 | Method for directly preparing methanol from carbon dioxide and hydrogen |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115259997A (en) * | 2022-08-29 | 2022-11-01 | 上海岚泽能源科技有限公司 | Self-heat-transfer synthesis process for preparing methanol by carbon dioxide hydrogenation |
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| CN115259997A (en) * | 2022-08-29 | 2022-11-01 | 上海岚泽能源科技有限公司 | Self-heat-transfer synthesis process for preparing methanol by carbon dioxide hydrogenation |
| CN115259997B (en) * | 2022-08-29 | 2023-11-14 | 上海岚泽能源科技有限公司 | Self-heat-transfer type synthesis process for preparing methanol by carbon dioxide hydrogenation |
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