CN1676459A - Technique for deep purifying material gas for synthesizing ammonia - Google Patents
Technique for deep purifying material gas for synthesizing ammonia Download PDFInfo
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Abstract
The present invention relates to a deep purification technique of raw material gas for synthesizing ammonia. Said invention adopts 'dimethyl ether-methanation' new process to purifying raw material gas for producing synthetic ammonia so as to can convert the harmful gas CO and CO2 into dimethyl ether, and the CO and Co2 in residual gas can be undergone the process of methanation to reach the standard of refined gas.
Description
The technical field is as follows: the invention belongs to the technical field of nitrogen fertilizer industry, and particularly relates to a deep purification technology for producing synthetic ammonia raw material gas by taking coal, natural gas and heavy oil as raw materials.
Background art: the ammonia synthesis process is the foundation of all the nitrogen fertilizer industries at present and is also used in the high energy consumption industryα -Fe is very sensitive to the toxicity of trace oxygen and oxide, if 20PPm of CO in raw material gas reduces the reaction speed of synthetic ammonia by 15% -20%, corresponding to 4% -6% reduction of yield of medium pressure ammonia, especially 2% -3% of CO is remained after the raw material gas of synthetic ammonia using coal and coke as raw material is transformed, CO is a gas which is neither acidic nor alkaline, the difficulty and cost of complete removal are very large, but for industrial production of synthetic ammonia, it must be removed to PPm (10 PPm)-6) The concentration of the stage, otherwise the ammonia synthesis process will not be able to proceed.
At present, the micro CO and CO are removed domestically2The method mainly comprises a copper washing method, a low-pressure methanation method and methanolation-methanation. The copper washing method comprises dissolving electrolytic copper in cuprammonium acetate solution, which is a complex solution composed of ammonia and acetic acid, and passing through Cu+Absorbing CO with ion under pressure of 12.5MPa and temperature below 10 deg.C, heating to about 80 deg.C with steam for regeneration, cooling with water and freezing method, and recycling. The method is characterized by mature technology and no increase of inert gas methane (CH) in purified gas4) But the method has the defects of low raw material gas purification degree, high operation cost, complex process, highoperation difficulty and the like, and also has the problems of environmental pollution, high equipment investment and the like. The low-pressure methanation method is to add 1 to 3 percent of CO and CO under the pressure of 0.5 to 3MPa2Is converted into methane. The method is characterized by simple process. The disadvantages are as follows: CO + CO in feed gas at low pressure2The content is high. The methanation reaction consumes hydrogen, although the inert gas has little toxicity to the synthetic ammonia catalyst. But due to the discharge of inert gas H2、N2The gas is discharged along with the air, so that the energy consumption is increased, the production capacity is reduced, the potential energy loss is large, and the overall economic benefit is poor; an external heat source is required to maintain the operation temperature in the process, the cold and hot diseases of the process are prominent, and the operation fluctuation is large; the equipment is huge under low pressure, and the catalyst consumption and investment are more; the purification difficulty of sulfide is high under low pressure, and the service life of the catalyst is short. The medium-pressure methanol-methanol combination and medium-pressure methanation process is characterized in that the converted and desulfurized gas contains 3 to 5 percent of CO and CO under the pressure of 12.0 to 13.0MPa2Through a medium pressure methanol system, a portion of the methanol is produced, with 0.5% -2% of the CO + CO remaining2And then medium pressure methanation is carried out under the pressure of 12.0-13.0 MPa. Because of the restriction of chemical equilibrium, the conversion rate of methanol is not very high, and because 0.5 to 0.8 percent of inert gas methane is still generated in the methanation process, the consumption of the raw material gas of synthetic ammonia is also high. The high-pressure methanolizing and methanation process adopts 24.0-31.4MPa high-pressure methanolizingand high-pressure methanation reaction to make the raw material gas after medium-pressure alcohol combination or decarbonized raw material gas after desulfurization undergo the process of seven-stage (six-stage) pressure-raising treatment by means of compressor adopting oil-free lubrication technology to make pressure be equal to that of high-pressure ring for synthesizing ammonia, and requires residual CO + CO2Between 0.5 percent and 2 percent, a hydrolysis fine desulfurization device needs to be heated at normal temperature to ensure that the sulfur content is less than 0.01PPm, and the service life of the methanol catalyst is influenced by overhigh total sulfur. At the same time, the user can select the desired position,under high-pressure operation conditions, the equipment requirement is high, and particularly, the methanol catalyst and the methanation catalyst are difficult to operate and have high catalyst strength.
In medium and small nitrogen fertilizer plants taking coal as a raw material in China, high-temperature conversion carbonization (or decarburization) -copper washing processes are widely adopted for semi-water gas after wet desulphurization, and the processes have abundant production experience. In the technical transformation of nitrogen fertilizer plants, the alcohol is introduced for expanding the product variety to form a high temperature change-carbonization (decarburization) -alcohol-copper washing process, and after alcohol catalysts are developed by research institutes of the southern chemical companies in the seventies, dozens of small and medium nitrogen fertilizer devices are used for co-producing methanol in China. The method is characterized in that: when carbon ammonia or urea is produced, a byproduct methanol in an ammonia plant is produced, and a part of carbon monoxide is consumed in the production of methanol, so that the load of copper washing is reduced; the requirement on the change rate of the carbon monoxide can be slightly relaxed, and the steam for conversion is reduced. The problems with this procedure are: the equipment is huge, and a copper washing bundle purification switch with complex operation is still needed; because of the large operation fluctuation of nitrogen fertilizer plants, the poor stability of the operation of the bi-alcohol and the poor desulfurization effect, the bi-alcohol catalyst is easy to inactivate, and the utilization coefficient of the catalyst is not high.
For the development of "methanolation-methanation" process in foreign countries, methanolation process was proposed by Topusolo corporation in the annual meeting of chemical engineering in the United states of America in 1991, which is described in detail in NITROGEN (1992) NO 197. In order to prevent ammonia synthesis catalyst from poisoning, the synthesis ammonia process needs to remove trace amounts of CO and CO in synthesis gas2Common use of methaneChemical conversion of residual CO, CO2Adding H2Conversion to CH4. Producing a portion of methanol with a residual of 0.5-2% CO + CO by a medium pressure methanol system2And then medium pressure methanation is carried out under the pressure of 12.0-13.0 MPa. Because of the restriction of chemical equilibrium, the conversion rate of methanol is not very high, so that the methanation process still produces more than 0.5 percent of inert gas methane, and the consumption of the raw material gas for synthesizing ammonia is also high.
The invention content is as follows: the invention aims to: provides a deep purification technology for synthesis ammonia raw material gas, which reduces the consumption of synthesis ammonia raw material gas and the consumption of cost per ton of ammonia.
The invention is characterized in that the raw material gas is compressed and then sent to transform, and then is desulfurized, carbonized or decarbonized by wet method, and the decarbonized gas is compressed and then desulfurized by dry method; then the residual amount of carbon monoxide and carbon dioxide in the raw material gas reaches the standard of refined gas through a dimethyl ether-methanation system.
The dimethyl ether-methanation system is under the conditions of reaction pressure of 3.0 MPa-31.4 MPa, reaction temperature of 230-350 ℃ and space velocity of synthetic gas of 500h-1～5000h-1Under the condition, the decarbonized gas is desulfurized and then generates dimethyl ether in a dimethyl ether synthesis tower, thereby removing CO + CO2To ensure that CO + CO is in the outlet gas of the dimethyl ether synthetic tower2The content is less than 0.5 percent; the outlet gas of the dimethyl ether synthesis tower enters a methanation tower after crude ether is separated, the reaction pressure is 3.0MPa to 31.4MPa, the reaction temperature is 300 ℃ to 350 ℃, and the space velocity of the synthesis gas is 5000h-1～15000h-1The methanation reaction is carried out under the condition, CO + CO in the outlet gas of the methanation tower2The content is less than 10 PPm.
The reaction temperature of the dimethyl ether system is preferably as follows: 250-300 ℃; the reaction pressure is preferably: 10.0MPa to 12 MPa;the air speed of the synthetic gas is preferably as follows: 1000h-1～3000h-1。
The composition volume content of the decarbonization gas is as follows: 1% -20% of CO + CO2(ii) a 50 to 85 percent of hydrogen(ii) a 10 to 30% nitrogen; 0.1 to 3 percent of methane, and the total sulfur is less than 0.1 PPm. Preferably, the method comprises the following steps: 2% -10% of CO + CO2(ii) a 70.74 to 75.06 percent of hydrogen; 17.28 to 19.44 percent of nitrogen; 0.66 to 0.93 percent of methane, and the total sulfur is less than 0.1 PPm.
The transformed and desulfurized product contains 2 to 10 percent of CO and CO2The gas passes through a dimethyl ether-methanation system and CO + CO in the outlet gas of a dimethyl ether synthetic tower2The content was<0.5%, followed by demethanization. As the CO conversion rate in the dimethyl ether process is much higher than that in the methanol process, the CO content in the outlet gas of the dimethyl ether reactor is greatly reduced, so that the inert gas methane generated in the methanation process is greatly reduced, and the consumption of the synthesis ammonia raw material gas is also reduced compared with the methanolation-methanation process.
The deep purification technology of the raw material gas for synthesizing ammonia has the advantages that the conversion rate in the dimethyl ether process is high, so that the inert gas methane generated in the methanation process is greatly reduced, the consumption of the raw material gas for synthesizing ammonia is also reduced, the consumption of cost per ton of ammonia is reduced, and the market competitiveness is improved.
Description of the drawings: FIG. 1 is a schematic block diagram of the process of the present invention.
Decarbonized gas subjected to fine desulfurization in attached drawing [ 1]]Passing through an oil separator [ 2]]With methyl ether column outlet gas in heat exchanger I3]After heat exchange, enters a dimethyl ether tower (4)]Synthesis of dimethyl ether from CO + CO2And H2The dimethyl ether is generated by the following steps:
as can be seen from the above reaction, CO + CO2Methanol produced in the reaction formulae (1) and (2) is consumed(ii) a The methanol is consumed as a reactant in the reaction (3) to generate dimethyl ether and water, which is equivalent to the reduction of the concentration of the product in the reaction (1) and the reaction (2), so that the reaction moves to the direction favorable for positive reaction and the reduction of CO + CO2The concentration of (c).
The reacted gas is cooled by decarbonized gas in a heat exchanger I3, then enters a heat exchanger II 5 to exchange cooling with the outlet gas of an ether separator [9], the cooled gas sequentially enters a water cooler [6], an ether separator [7], an ammonia cooler [8], the ether separator [9], the heat exchanger II 5 and a heat exchanger III [10], enters a methanation furnace [11]after heat exchange, the methanation reaction gas sequentially enters a heat exchanger III [10], a water cooler [12], after moisture is separated in a water separator [13], the methanation reaction gas enters a compressor [14]to be compressed and enters a synthetic ammonia system.
The specific implementation mode is as follows: the invention is further illustrated by the following examples.
Example one
The coal is used as raw material to produce semi-water gas. Semi-water gas is compressed, transformed, desulfurized by wet method (ammonia water neutralization method, ammonia water liquid phase catalysis method, ADA method, FD method, baking method, etc.), carbonized or decarbonized (propylene carbonate method, MDEA method, water washing method, etc.), and H is removed2S and CO2. The decarbonized gas is compressed, desulfurized by a dry method (an activated carbon method, an iron oxide method, a normal-temperature zinc oxide method and the like), and then synthesized into the dimethyl ether by a synthesis tower filled with a dimethyl ether catalyst, wherein the synthesis conditions are as follows: the reaction temperature is 259-298 ℃, the reaction pressure is 10.7-11.5 MPa, and the space velocity is 1850-2050 h-1The dimethyl ether catalyst adopts Chinese patents: the catalyst disclosed in publication No. CN13561630, the composition of the dimethyl ether synthesis tower tail gas is as follows: CO + CO2＜0.5％，H271.45％～76.54％，N220.33％～22.87％，DME 1.9％～2.7％，CH40.78％～1.09％。
The dimethyl ether synthesis tower back gas enters a methanation reactor after being cooled and separated from crude ether, and the methanation reaction conditions are as follows: the reaction temperature is 305-355 ℃, the reaction pressure is 10.2-11.1 MPa, and the airspeed is 15000-16500 h-1The methanation catalyst adopts a J105 type methanation catalyst invented by southern research institute, and the gas after the methanation synthesis tower comprises the following components: CO + CO25～7PPm，H2/N2≈3，CH41.29％～1.59％。
Cooling the methanation tower after gas to separate trace moisture, compressing and sending to the synthetic ammonia process. The operational data of each node is shown in table 1.
TABLE 1 semi-water gas-decarbonized gas-dimethyl ether synthesis-methanation process node operation data
| Node point | Temperature of | Pressure of MPa | Airspeed h-1 | Gas composition vol% | Total sulfur PPm | ||||
| CO | CO2 | H2 | N2 | CH4 | |||||
| Semi-water gas | At normal temperature | 0.1 | / | 30～32 | 7～9 | 40～42 | 16～18 | 0.61～0.86 | ～500 |
| Post-tower gas of decarburization tower | At normal temperature | 0.5～1.2 | / | 4～5 | 0.3～0.8 | 70.74～75.06 | 17.28～19.44 | 0.66～0.93 | ～11.7 |
| After-gas of fine desulfurization tower | At normal temperature | 1012 | 500～200 | 4～5 | 0.3～0.8 | 70.74～75.06 | 17.28～19.44 | 0.66～0.93 | ＜0.1 |
| Dimethyl ether column tail gas | 250～300 | 10～12 | 1000～6000 | CO+CO2＜0.5％ | 71.45～76.54 | 20.33～22.87 | 0.78～1.09 | / | |
| Methanation column tail gas | 300～350 | 10～12 | 8000～15000 | CO+CO2＜10PPm | H2/N2≈3 | 1.29～1.59 | / | ||
Example two
The heavy oil as raw material is used to prepare raw material gas for synthesizing ammonia, and features that air is used to replace oxygen and ordinary-pressure intermittent gasification is used in chemical industryThe process flow is as follows. Under the condition of 1250 ℃, the feed gas composition is as follows: methane is less than 1.5 percent, carbon monoxide is 15 to 20 percent, carbon dioxide is 7 to 10 percent, hydrogen is 40 to 48 percent, and nitrogen is 20 to 22 percent. The raw material gas is compressed, transformed, desulfurized by wet method (ammonia water neutralization method, ammonia water liquid phase catalysis method, ADA method, FD method, baking gum method, etc.), carbonized or decarbonized (propylene carbonate method, MDEA method, water washing method, etc.), and H is removed2S and CO2. The decarbonized gas is compressed, desulfurized by a dry method (an activated carbon method, an iron oxide method, a normal-temperature zinc oxide method and the like), and then synthesized into the dimethyl ether by a synthesis tower filled with a dimethyl ether catalyst, wherein the synthesis conditions are as follows: the reaction temperature is 253-292 ℃, the reaction pressure is 10.7-11.5 MPa, and the airspeed is 1450-1550 h-1And the dimethyl ether catalyst adopts Chinese patents: the catalyst disclosed in publication No. CN13561630, the composition of the dimethyl ether synthesis tower tail gas is as follows: CO + CO2＜0.4％，H265.37％～76.94％，N219.28％～24.43％，DME 1.9％～2.7％，CH4＜1.93％。
The dimethyl ether synthesis tower back gas enters a methanation reactor after being cooled and separated from crude ether, and the methanation reaction conditions are as follows: the reaction temperature is 295-345 ℃, the reaction pressure is 10.2-11.1 MPa, and the space velocity is 13500-14800 h-1The methanation catalyst adopts a J105 type methanation catalyst invented by southern research institute, and the gas after the methanation synthesis tower comprises the following components: CO + CO21～3PPm，H2/N2≈3，CH4＜2.43％。
Cooling the methanation tower after gas to separate trace moisture, compressing and sending to the synthetic ammonia process. The operational data of each node is shown in table 2.
Table 2. operation data of each node in heavy oil gas production-decarbonization gas-dimethyl ether synthesis-methanation process
| Node point | Temperature of | Pressure of MPa | Airspeed h-1 | Gas composition vol% | Total sulfur PPm | ||||
| CO | CO2 | H2 | N2 | CH4 | |||||
| Heavy oil gas production | 1250 | 0.1 | / | 20～30 | 7～10 | 40～49 | 15～19 | ＜1.5 | ＜160 |
| Post-gas of decarburization gas tower | At normal temperature | 0.5～1.2 | / | 4～5 | 0.3～0.8 | 65.57～75.40 | 16.39～20.77 | ＜1.64 | ～11.7 |
| After-gas of fine desulfurization tower | At normal temperature | 10～12 | 500～200 | 4～5 | 0.3～0.8 | 65.57～75.40 | 16.39～20.77 | ＜1.64 | ＜0.1 |
| Dimethyl ether column tail gas | 250～300 | 10～12 | 1000～6000 | CO+CO2＜0.5％ | 65.37～76.94 | 19.28～24.43 | ＜1.93 | / | |
| Methanation column tail gas | 300～350 | 10～12 | 8000～15000 | CO+CO2＜10PPm | H2/N2≈3 | ＜2.43 | / | ||
EXAMPLE III
The method comprises the following steps of preparing raw material gas for synthesizing ammonia by taking natural gas as a raw material, wherein the prepared raw material gas comprises the following components at the pressure of 31atm, the first-stage conversion temperature of 800-820 ℃ and the second-stage conversion temperature of about 1000 ℃: 0.3% of methane, 12.8% of carbon monoxide, 7.6% of carbon dioxide, 57% of hydrogen and 22.3% of nitrogen. Compressing and transforming raw material gas, wet desulfurizing (ammonia water neutralization, ammonia water liquid phase catalysis, ADA method, FD method, baking method, etc.), carbonizing or decarbonizing (propylene carbonate method, MDEA method, etc.),Water washing method, etc.), removing H2S and CO2. The decarbonized gas is compressed and then passesDry desulfurization (active carbon method, iron oxide method, normal temperature zinc oxide method, etc.) and then synthesis of dimethyl ether by a synthesis tower filled with dimethyl ether catalyst, wherein the synthesis conditions are as follows: the reaction temperature is 253-292 ℃, the reaction pressure is 10.7-11.5 MPa, and the airspeed is 1450-1550 h-1And the dimethyl ether catalyst adopts Chinese patents: the catalyst disclosed in publication No. CN13561630, the composition of the dimethyl ether synthesis tower tail gas is as follows: CO + CO2＜0.4％，H265.37％～76.94％，N219.28％～24.43％，DME 1.9％～2.7％，CH4＜1.93％。
The dimethyl ether synthesis tower back gas enters a methanation reactor after being cooled and separated from crude ether, and the methanation reaction conditions are as follows: the reaction temperature is 305-359 ℃, the reaction pressure is 10.2-11.1 MPa, and the airspeed is 16000-17800 h-1The methanation catalyst adopts a J105 type methanation catalyst invented by southern research institute, and the gas after the methanation synthesis tower comprises the following components: CO + CO28～10PPm，H2/N2≈3，CH40.9％～1.17％。
Cooling the methanation tower after gas to separate trace moisture, compressing and sending to the synthetic ammonia process. The operational data of each node is shown in table 3.
TABLE 3 operation data of each node of the two-stage reformed gas-decarbonized gas-dimethyl ether synthesis-methanation process
| Node point | Temperature of | Pressure of MPa | Airspeed h-1 | Gas composition vol% | Total sulfur PPm | ||||
| CO | CO2 | H2 | N2 | CH4 | |||||
| Secondary reformed gas | 1000 | 31 | / | 11.8～13.8 | 6.6～8.6 | 55～59 | 15～18.3 | 0.30.5 | ～500 |
| Post-gas of decarburization gas tower | At normal temperature | 31 | / | 5～7 | 0.2～0.8 | 66.8871.21 | 16.23～19.81 | 0.32～0.54 | ～11.7 |
| After-gas of fine desulfurization tower | At normal temperature | 10～12 | 500～200 | 5～7 | 0.2～0.8 | 66.88～71.21 | 16.23～19.81 | 0.32～0.54 | ＜0.1 |
| Dimethyl ether column tail gas | 250～300 | 10～12 | 1000～6000 | CO+CO2＜0.5％ | 66.93～72.31 | 20.16～24.60 | 0.4～0.67 | / | |
| Methanation column tail gas | 300～350 | 10～12 | 8000～15000 | ＜10PPm | H2/N2≈3 | 0.9～1.17 | / | ||
Claims (8)
1. A deep purification technology for raw gas of synthetic ammonia uses coal as raw material to produce semi-water gas, or uses heavy oil as raw material to prepare raw gas of synthetic ammonia, or uses natural gas as raw material to prepare raw gas of synthetic ammonia, and is characterized in that the raw gas is compressed and then sent to transform, and then is desulfurized by wet method, carbonization or decarbonization, and the decarbonization gas is compressed and then desulfurized by dry method; then the residual amount of carbon monoxide and carbon dioxide in the raw material gas reaches the standard of refined gas through a dimethyl ether-methanation system.
2. The deep purification technology for synthesis ammonia raw gas as claimed in claim 1, wherein the dimethyl ether-methanation system is operated at a reaction pressure of 3.0 MPa-31.4 MPa, a reaction temperature of 230-350 ℃, and a synthesis gas space velocity of 500h-1～5000h-1Under the condition, the decarbonized gas is desulfurized and then generates dimethyl ether in a dimethyl ether synthesis tower, thereby removing CO + CO2To ensure that CO + CO is in the outlet gas of the dimethyl ether synthetic tower2The content is less than 0.5 percent.
3. The deep purification technology for synthesis ammonia raw gas as claimed in claim 1, wherein the dimethyl ether synthesis system of dimethyl ether-methanation systemCrude ether is separated from tower outlet gas and then enters a methanation tower, the reaction pressure is 3.0MPa to 31.4MPa, the reaction temperature is 300 ℃ to 350 ℃, and the space velocity of the synthesis gas is 5000h-1～15000h-1The methanation reaction is carried out under the condition, CO + CO in the outlet gas of the methanation tower2The content is less than 10 PPm.
4. The process according to claim 1, wherein the decarbonized gas comprises the following components by volume: 1% -20% of CO + CO2(ii) a 50 to 85 percent of hydrogen; 10 to 30% nitrogen; 0.1 to 3 percent of methane, and the total sulfur is less than 0.1 PPm.
5. The process according to claim 4, wherein the decarbonized gas comprises the following components by volume: 2% -10% of CO + CO2(ii) a 70.74 to 75.06 percent of hydrogen; 17.28 to 19.44 percent of nitrogen; 0.66 to 0.93 percent of methane, and the total sulfur is less than 0.1 PPm.
6. The deep purification technology for synthesis ammonia raw gas as claimed in claim 2, wherein the reaction temperature is as follows: 250-300 ℃.
7. The process of claim 2, wherein the reaction pressure is: 10.0-12 MPa.
8. The process of claim 2, wherein the synthesis gas space velocity is: 1000h-1～3000h-1。
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN100450927C (en) * | 2006-12-11 | 2009-01-14 | 山西丰喜肥业（集团）股份有限公司临猗分公司 | Isopressing conversion decarburization process in ammonia synthesis |
| CN103588222A (en) * | 2013-11-25 | 2014-02-19 | 安徽淮化股份有限公司 | Production technology for low-carbon synthetic ammonia |
| CN106672898A (en) * | 2017-01-17 | 2017-05-17 | 青海盐湖工业股份有限公司 | Method for synthesizing ammonia by taking byproduct tail gas in process of producing acetylene by pyrolyzing natural gas as raw material |
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| CN1019663B (en) * | 1990-09-04 | 1992-12-30 | 湖南省化肥工业公司 | Refining process for synthetic ammonia raw material gas |
| CN1020707C (en) * | 1990-09-29 | 1993-05-19 | 武汉制氨厂 | Copper cleaning technology replaced by deep exchanged match methanization process |
| CN1031871C (en) * | 1994-03-18 | 1996-05-29 | 四川省眉山县氮肥厂 | Process for purifying raw gas of ammonia synthesis |
| CN1043469C (en) * | 1994-03-30 | 1999-05-26 | 湖南安淳节能技术有限公司 | Ammonia-alcohol ratio adjustable technology for refining raw-material gas for synthesis of ammonia |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN100450927C (en) * | 2006-12-11 | 2009-01-14 | 山西丰喜肥业（集团）股份有限公司临猗分公司 | Isopressing conversion decarburization process in ammonia synthesis |
| CN103588222A (en) * | 2013-11-25 | 2014-02-19 | 安徽淮化股份有限公司 | Production technology for low-carbon synthetic ammonia |
| CN106672898A (en) * | 2017-01-17 | 2017-05-17 | 青海盐湖工业股份有限公司 | Method for synthesizing ammonia by taking byproduct tail gas in process of producing acetylene by pyrolyzing natural gas as raw material |
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