CN1428403A - Method for making synthetic gas by using fluidized bed coal and methane rich fuel gas co-gasification - Google Patents
Method for making synthetic gas by using fluidized bed coal and methane rich fuel gas co-gasification Download PDFInfo
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Abstract
The method for preparing synthetic gas by using fluidized bed coal and methane-enriched fuel gas through cogasification includes the following steps: breaking raw material coal and making its grain size be less than 8 mm, making the broken coal pass through drying system, raw coal bin and metering system, and feeding the coal into fluidized bed gasification furnace, making steam and oxygen gas pass through gas distribution plate, ash-removing ring pipe and central jet pipe and come into the gasification furnace, and feeding methane-enriched natural gas, coal layer gas or gas discharged from chemical fertilizer plant into concentratino phase section reaction zone of fluidized bed gasification furnace from its lower or side portion gas inlet pipe to make cogasification with coal at 950-1100 deg.c to prepare synthetic gas.
Description
The technical field is as follows:
the invention belongs to a method for preparing synthesis gas, and particularly relates to a method for preparing synthesis gas by co-gasifying coal in a fluidized bed and methane-rich fuel gas.
Background art:
methane is a main component of natural gas, coal bed gas and exhausted gas of a chemical fertilizer plant, methane-rich fuel gas in China, namely natural gas, coal bed gas, exhausted gas of the chemical fertilizer plant and the like, is rich in reserves, and plays an important role in the development of the energy chemical synthesis industry in the future. Because the methane has stable molecular structure and is difficult to directly convert chemically, the methane is usually first converted into synthesis gas (CO + H)2) Further synthesizing a series of fine chemical products such as ammonia, methanol and the like, fuels and olefins, and the process for preparing the synthesis gas from methane is the basis of the whole natural gas chemical industry.
The main methods for preparing synthesis gas by methane conversion comprise: steam catalytic reforming, Air Partial Oxidation (APO) reforming (including selective oxidative reforming), and CO2-CH4Transformation, and the like.
(1) The methane steam catalytic conversion process is industrialized, and the steam conversion process commonly adopted by modern ammonia plants comprises the following steps:the U.S. Kellogg method, the British ICI method, the Danish Halder Tops phi e method, the French ONIA-GEGA method, the U.S. Chemico method, the Foster-Wheeler method, and the like. However, 1 mole of CH4Formation of 1 mol CO and 3 mol H2H in synthesis gas2The ratio of/CO is up to 3. This ratio is for the synthesis of a series of organic compounds, H2The ratio of/CO is too high, and therefore, the process of two-stage oxygen-enriched partial oxidation and the like is often adopted in the industry to increase the CO content in the synthesis gas. The minimum water-carbon ratio for ensuring no carbon precipitation in the conversion pipe is about 1.0, but is usually 2-3 times larger in actual production. The main problems of this process are therefore: long conversion process flow, large investment, high water-carbon ratio, large energy consumption, easy sintering, low poisoning resistance and the like.
(2) The APO process developed by the U.S. Foster-Hewler energy company has the advantages of no need of primary and secondary converters, low water consumption, greatly reduced reaction temperature (less than 800 ℃) when catalyst is available, and H in the synthesis gas2the/CO ratio is low, the methane conversion per pass is close to 90%, but the service life of the catalyst is not long and the price is high. Without a catalyst, under the condition of 900-1000 ℃,the conversion rate of methane is extremely low, partial oxidation reaction of methane is relatively thorough, the reaction temperature is about 1350 ℃, and the material quality of equipment is improvedHigher requirements are imposed.
(3)CO2The reaction with the synthesis gas prepared by the catalytic conversion of methane is a reversible strong endothermic reaction, has high design requirements on a reactor and large energy consumption, and cannot be widely used so far.
At present, the price of petroleum and natural gas rises, and chemical synthesis plants using natural gas as a raw material face serious problems of cost rise and product lack of competitiveness. The development of synthesis gas production has mainly focused on flexibly regulating H in the synthesis gas according to product requirements2The ratio of/CO, thereby achieving the purposes of reasonably utilizing resources, saving investment, and reducing energy consumption and production cost.
The purpose of the invention is as follows:
the invention aims to provide a method for preparing synthesis gas from natural gas, coal bed gas or exhausted gas of a fertilizer plant, which is rich in methane and fuel gas, with low cost and high efficiency.
Theoretically, the main reactions of coal gasification are:
the combustion reaction provides a large amount of heat to allow the gasification reaction to proceed. After the methane is added, the gasification reaction of the steam, carbon dioxide and carbon and methane can be simultaneously carried out as long as the combustion reaction (carbon and oxygen or methane and oxygen) provides enough heat.
In the process of fluidized bed coal gasification, coal is pyrolyzed and gasified to generate coal semicoke, and the semicoke has porous and high specific surface area (BET is more than 200 m)2Per g) and the semicoke has a plurality of functional groups, mayCan provide conversion active sites for methane conversion, generate intermediate transition substances, and then further convert the intermediate transition substances into CO and H2. In the fluidized bed gasification furnace, the reaction of methane and steam can be carried out at the temperature of 950-1000 ℃, reasonable conversion rate is achieved, and H is prepared by co-gasification of coal and methane2The ratio of the carbon to the oxygen is 1-1.5, so that the structure of the conversion reactor is simplified, and H in the synthesis gas is regulated2Purpose of the/CO ratio.
The invention aims to realize the purpose that raw coal is firstly crushed to be less than 8mm and then enters a fluidized bed gasification furnace through a drying system, a raw coal bin and a coal feeding metering system; steam and oxygen enter the gasification furnace through the gas distribution plate, the ash discharge ring pipe and the central jet pipe, natural gas, coal bed gas or exhausted methane-rich fuel gas of a fertilizer plant enters a dense phase section reaction area of the fluidized bed gasification furnace through a lower part or a side part gas inlet pipe, and the methane-rich fuel gas and coal are co-gasified at the temperature of 950-1100 ℃ to prepare synthesis gas.
The processing method comprises the following steps:
(1) crushing raw coal, sieving, drying coal smaller than 8mm to remove external water, and adding into a coal hopper;
(2) heating to ensure that the bottom temperature of the fluidized bed gasification furnace is 800-950 ℃ and the top temperature is 400-500 ℃;
(3) introducing a certain amount of air and steam through the lower part of the gasification furnace, and adding raw coal with theparticle size of less than 8mm into the gasification furnace, wherein the ratio of the air to the coal is 2.0-3.5 Nm3The ratio of steam to coal is 0.3 to 0.6 kg/kg. After bed layer establishment and system stabilization, oxygen/steam blast is switched to, the ratio of the height of the material static bed layer in the fluidized bed to the diameter of the reactor is 0.5-1.5, and the ratio of oxygen to coal is 0.25-0.5 Nm3Kg, the ratio of steam to coal is 0.5-1.0 kg/kg;
(4) natural gas, coal bed gas or exhausted gas of chemical fertilizer plant, which is rich in methane, is fed into the dense phase reaction zone of fluidized bed gasifier from the lower or lateral gas inlet pipe and is pressurized at 950-1100 deg.C and normal pressure or at 0.3-0.8 Nm/coal ratio3/kg, the ratio of the total oxygen amount to the methane-rich fuel gas is 1.4 to 3Nm3/Nm3Amount of water vaporAnd methane-rich fuel gas) in a ratio of 3 to 5kg/Nm3Under the condition of (1), co-gasification of fluidized bed coal and methane-rich fuel gas is carried out to prepare synthesis gas.
In order to realize the invention, a fluidized bed gasification furnace device and a process flow are adopted, wherein the process flow comprises systems of coal preparation, feeding, gas supply, gasification, dust removal, waste heat recovery and the like.
Compared with the prior art, the invention has the following advantages:
(1) the reaction temperature in the process is moderate (950-1100 ℃), no catalyst is added, the maximum methane conversion rate can reach 90%, the content of methane in the synthesis gas is low, the sum of the contents of other hydrocarbon substances is less than 0.5%, and no substance with more than C6 exists.
(2) H in composition of synthesis gas prepared by co-gasification of coal and methane-rich fuel gas2The ratio of/CO is less than 1.5, usually about 1.3, and completely meets the requirements of various chemical synthesis.
(3) Stable operation, wide operation range, low operation cost and low energy consumption.
(4) The fluidized bed is suitable for various coal types, so that the co-gasification of the coal and the natural gas is not limited by the coal types.
(5) The feeding proportion of the coal and the methane-rich fuel gas can be adjusted in a wider range, so that the process can prepare the synthesis gas by taking the coal as the raw material, and can also add a certain amount of methane-rich fuel gas according to market price and synthesis requirements and add the methane-rich fuel gas into a two-stage catalytic reactor for steam conversion, thereby realizing technical improvement of the prior process.
The present invention will be described in further detail with reference to the accompanying drawings and examples.
FIG. 1 is a flow chart of the present invention.
As shown in the figure, 1 is a gas cylinder, 2 is a gas flowmeter, 3 is a distilled water storage tank, 4 is a water flowmeter, 5 is distilled water, 6 is a steam generating and gas mixer, 7 is raw coal of 0-8 mm, 8 is a coal hopper, 9 is a raw coal feeder, 10 is a fluidized bed gasifier, 11 is a natural gas (or methane) inlet pipe, 12 is an ash discharger at the lower part of the gasifier 10, 13 is an ash hopper at the lower part of the ash discharger 12, 14 is ash, 15 is a cyclone separator connected with the upper part of the gasifier 10, 16 is a fly ash collecting tank connected with the lower part of the cyclone separator 15, 17 is fly ash, 18 is air, 19 is a gas water cooler connected with an upper outlet pipe of the cyclone separator 15, 20 is inlet water, 21 is outlet water, 22 is synthesis gas, 23 is a gas-liquid separator connected with the lower part of the gas water cooler 19, and 24 is cooling water.
The specific implementation mode is as follows:
example 1
Crushing raw coal until the granularity is less than 8mm, drying and then filling the raw coal into a coal hopper 8 for later use. Heating to make the bottom temperature of the fluidized bed gasification furnace reach 900 ℃ and the top temperature reach 400 ℃. Air is introduced from the lower part of the gasification furnace 10, the steam generation and gas mixer 6 is started, and the water flow meter 4 controls the introduction of the water vapor. Raw coal with the particle size of 0-8 mm is added into a gasification furnace 10 from a coal hopper 10 through a raw coal feeder 9, the coal feeding amount is 1.58kg/h, and the air amount is 4.5Nm3The steam amount is 0.8 kg/h. After bed layer is established and system is stabilized, opening O in the gas cylinder 12And N2Gas is measured by a flowmeter 2 and enters the gasification furnace from the bottom of the gasification furnace, and the steam flow is increased, and the oxygen inlet amount is 1.55Nm3H, steam amount 2.4kg/h, nitrogen amount 0.30Nm3H, air is turned off. After stable operation, the natural gas cylinder is opened, the natural gas is metered by the flowmeter 2 and then enters a dense phase section reaction zone of the fluidized bed gasification furnace through the natural gas inlet pipe 11 at the bottom of the gasification furnace, and the natural gas inlet amount is 0.5Nm3And h, the operating temperature of the fluidized bed gasification furnace is 1007 ℃. The ratio of natural gas to coal is 0.316Nm3/kg, total oxygen to natural gas ratio of 3Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 4.8kg/Nm3. The ash in the gasification furnace 10 is periodically discharged into an ash bucket 13 through an ash discharger 12 at the lower part of the gasification furnace, and the ash is discharged from the ash bucket 13. The synthetic gas enters a cyclone separator 15 from the top of the gasification furnace 10 to separate fly ash from gas; the fly ash enters a fly ash collection tank 16, and the fly ash is discharged from the fly ash collection tank 16; the synthesis gas from the cyclone 15 is cooled by a gas cooler 19 and then enters a gas-liquid separator 23 to finally obtain clean synthesis gas. The indices of the synthesis gas produced are shown in table 1.
Example 2:
adjusting the oxygen intake to 1.45Nm3H, natural gas to coal ratio of 0.316Nm3/kg, total oxygen to natural gas ratio of 2.9Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 4.8kg/Nm3. Gasification ofThe furnace temperature was controlled at 1021 ℃ as in example 1.
Example 3:
adjusting the natural gas air inflow to 0.75Nm3H, steam flow 2.3kg/h, oxygen intake 1.55Nm3H, nitrogen amount 0.32Nm3H, natural gas to coal ratio of 0.475Nm3/kg, total oxygen to natural gas ratio of 2.07Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 3.07kg/Nm3. The vaporization temperature was 1017 ℃ as in example 1.
Example 4:
adjusting the natural gas air input to 0.75Nm3H, coal feed 1.58kg/h, oxygen feed 1.75Nm3H, steam amount 2.94kg/h, nitrogen amount 0.31Nm3H, natural gas to coal ratio of 0.475Nm3/kg, total oxygen to natural gas ratio of 2.33Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 3.92kg/Nm3. The vaporization temperature was 1027 ℃ as in example 1.
Example 5:
adjusting the natural gas air input to 0.75Nm3H, coal feed 1.62kg/h, oxygen feed 1.35Nm3H, steam amount 2.4kg/h, nitrogen amount 0.30Nm3H, natural gas to coal ratio of 0.463Nm3/kg, total oxygen to natural gas ratio of 1.8Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 3.2kg/Nm3. The vaporization temperature was 1030 ℃ as in example 1.
Example 6:
adjusting the natural gas air input to 0.75Nm3H, coal feed 1.62kg/h, oxygen feed 1.25Nm3H, steam amount 2.4kg/h, nitrogen amount 0.30Nm3H, natural gas to coal ratio of 0.463Nm3/kg, total oxygen to natural gas ratio of 1.67Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 3.2kg/Nm3. The vaporization temperature was 1032 ℃ as in example 1.
Example 7:
adjusting the natural gas air input to 0.75Nm3H, coal feed 1.21kg/h, oxygen feed 1.25Nm3H, steam amount 2.76kg/h, nitrogen amount 0.27Nm3H, natural gas to coal ratio of 0.620Nm3/kg, total oxygen to natural gas ratio of 1.67Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 3.68kg/Nm3. The gasification temperature was 1037 ℃ as in example 1.
Example 8:
adjusting the natural gas air input to 0.875Nm3H, coal feed 1.21kg/h, oxygen feed 1.25Nm3H, steam amount 2.76kg/h, nitrogen amount 0.30Nm3Per h, natural gas to coal ratio of 0.723Nm3/kg, total oxygen to natural gas ratio of 1.43Nm3/Nm3The ratio of the amount of water vapor to the amount of natural gas is3.15kg/Nm3. The vaporization temperature was 1020 ℃ as in example 1.
Example 9:
into 0.75Nm3Per H simulation of purge gas (60% H) of fertilizer plant2,25%N2,15%CH4) Coal feeding amount of 1.51kg/h and oxygen feeding amount of 1.55Nm3H, steam amount 2.46kg/h, nitrogen amount 0.30Nm3H, purge gas to coal ratio of 0.50Nm3/kg, total oxygen amount to purge gas ratio of 2.07Nm3/Nm3The ratio of the amount of steam to the amount of natural gas was 3.28kg/Nm3. The vaporization temperature was 1025 ℃ as in example 1.
Example 10:
into 0.75Nm3Simulated coal bed gas (85% CH)49% of C2H4, 3% of N2, 3% of CO2), 1.58kg/H of coal feeding amount and 1.68Nm of oxygen feeding amount3H, steam amount 2.9kg/h, nitrogen amount 0.31Nm3H, the ratio of coal bed gas to coal is 0.475Nm3/kg, total oxygen to coal bed gas ratio of 2.24Nm3/Nm3The ratio of the steam amount to the coal bed gas is 3.87kg/Nm3. The gasification temperature is 1015 ℃, the rest is the same asExample 1.
The composition of the synthesis gas produced by co-gasification of coal with natural gas in a fluidized bed as carried out under the conditions of examples 1-10 and the methane conversion are given in table 1. TABLE 1
Note that*: different conditions and different methane conversion rates for H production2The residual methane in the synthesis gas with different CO ratios can be solved by a matched process.
Syngas composition (dry basis Vol%) | Gas heat value Kcal/Nm3 | Methane conversion Percentage ratio%* | |||||
H2 | CO | CH4 | CO2 | N2 | |||
Example 1 | 37.89 | 32.09 | 1.79 | 20.74 | 7.48 | 2298 | 82.5 |
Example 2 | 39.18 | 31.73 | 0.96 | 20.70 | 7.42 | 2248 | 90.3 |
Example 3 | 39.61 | 28.61 | 5.15 | 20.42 | 7.21 | 2565 | 63.0 |
Example 4 | 39.01 | 30.80 | 3.31 | 20.48 | 6.41 | 2438 | 74.1 |
Example 5 | 38.56 | 28.26 | 6.05 | 20.36 | 6.77 | 2608 | 56.5 |
Example 6 | 39.52 | 25.71 | 7.03 | 20.36 | 7.38 | 2654 | 53.7 |
Example 7 | 38.87 | 26.74 | 6.70 | 20.37 | 6.81 | 2735 | 56.8 |
Example 8 | 37.14 | 26.35 | 8.13 | 20.44 | 7.94 | 2705 | 57.3 |
Example 9 | 37.1 | 26.6 | 1.8 | 21.3 | 13.2 | 2123.7 | 65.2 |
Example 10 | 39.18 | 30.18 | 3.76 | 20.56 | 6.32 | 2467 | 70.1 |
Claims (2)
1. A method for preparing synthetic gas by co-gasification of fluidized bed coal and methane-rich fuel gas is characterized in that raw coal is firstly crushed to be less than 8mm and then enters a fluidized bed gasification furnace through a drying system, a raw coal bin and a coal feeding metering system; steam and oxygen enter the gasification furnace through the gas distribution plate, the ash discharge ring pipe and the central jet pipe, natural gas, coal bed gas or exhausted methane-rich fuel gas of a fertilizer plant enters a dense phase section reaction area of the fluidized bed gasification furnace through a lower part or a side part gas inlet pipe, and the methane-rich fuel gas and coal are co-gasified at the temperature of 950-1100 ℃ to prepare synthesis gas.
2. The method of claim 1 for producing syngas by co-gasification of fluidized bed coal and methane-rich fuel gas, comprising the steps of: (1) crushing raw coal, sieving, drying coal smaller than 8mm to remove external water, and adding into a coal hopper;
(2) heating to ensure that the bottom temperature of the fluidized bed gasification furnace is 800-950 ℃ and the top temperature is 400-500 ℃;
(3) introducing a certain amount of air and steam through the lower part of the gasification furnace, and adding raw coal with the particle size of less than 8mm into the gasification furnace, wherein the ratio of the air to the coal is 2.0-3.5 Nm3The ratio of steam to coal is 0.3 to 0.6 kg/kg. After bed layer establishment and system stabilization, oxygen/steam blast is switched to, the ratio of the height of the material static bed layer in the fluidized bed to the diameter of the reactor is 0.5-1.5, and the ratio of oxygen to coal is 0.25-0.5 Nm3Kg, the ratio of steam to coal is 0.5-1.0 kg/kg;
(4) natural gas, coal bed gas or exhausted gas of chemical fertilizer plant, which is rich in methane, is fed into the dense phase reaction zone of fluidized bed gasifier from the lower or lateral gas inlet pipe and is pressurized at 950-1100 deg.C and normal pressure or at 0.3-0.8 Nm/coal ratio3/kg, the ratio of the total oxygen amount to the methane-rich fuel gas is 1.4 to 3Nm3/Nm3The amount of steam and the methane-rich fuel gas) is 3 to 5kg/Nm3Under the condition of (1), co-gasification of fluidized bed coal and methane-rich fuel gas is carried out to prepare synthesis gas.
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Cited By (11)
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CN100404409C (en) * | 2005-01-05 | 2008-07-23 | 山西中天煤化有限公司 | Process for preparing synthetic gas by reforming carbon dioxide-methane |
CN100445352C (en) * | 2006-06-24 | 2008-12-24 | 中国科学院山西煤炭化学研究所 | Method for preparing fuel gas by fluidized bed co-gasification of biomass and coal |
CN101484554A (en) * | 2006-06-01 | 2009-07-15 | 格雷特波因特能源公司 | Catalytic steam gasification process with recovery and recycle of alkali metal compounds |
CN102120936A (en) * | 2010-01-07 | 2011-07-13 | 中国科学院过程工程研究所 | Method and device for jet/preoxidation/pyrolysis/fluidized bed gasification of carbon-containing solid fuel |
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CN104694170A (en) * | 2015-03-25 | 2015-06-10 | 西北化工研究院 | Method for producing synthesis gas with carbon powder and natural gas/methane as raw materials |
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CN100404409C (en) * | 2005-01-05 | 2008-07-23 | 山西中天煤化有限公司 | Process for preparing synthetic gas by reforming carbon dioxide-methane |
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CN100445352C (en) * | 2006-06-24 | 2008-12-24 | 中国科学院山西煤炭化学研究所 | Method for preparing fuel gas by fluidized bed co-gasification of biomass and coal |
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CN102939359B (en) * | 2010-04-13 | 2015-11-25 | 伊内奥斯美国公司 | Carbonaceous material gasification process |
CN102939359A (en) * | 2010-04-13 | 2013-02-20 | 伊内奥斯美国公司 | Methods for gasification of carbonaceous materials |
CN102234545A (en) * | 2010-04-28 | 2011-11-09 | 中国石油化工股份有限公司 | Preparation method of synthesis gas by gasifying carbonaceous materials |
CN102234545B (en) * | 2010-04-28 | 2014-10-01 | 中国石油化工股份有限公司 | Preparation method of synthesis gas by gasifying carbonaceous materials |
CN104694170A (en) * | 2015-03-25 | 2015-06-10 | 西北化工研究院 | Method for producing synthesis gas with carbon powder and natural gas/methane as raw materials |
CN104694170B (en) * | 2015-03-25 | 2017-02-22 | 西北化工研究院 | Method for producing synthesis gas with carbon powder and natural gas/methane as raw materials |
CN105062568A (en) * | 2015-07-21 | 2015-11-18 | 西北化工研究院 | Method for utilizing coal and natural gas jointly to produce synthesis gas |
CN105602625A (en) * | 2016-03-14 | 2016-05-25 | 鲁西化工集团股份有限公司煤化工分公司 | Novel technique for recycling fly ash |
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