CN1156754A - Method for continuously gasifying coal (coke) and purifying synthesized gas - Google Patents
Method for continuously gasifying coal (coke) and purifying synthesized gas Download PDFInfo
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- CN1156754A CN1156754A CN 96117856 CN96117856A CN1156754A CN 1156754 A CN1156754 A CN 1156754A CN 96117856 CN96117856 CN 96117856 CN 96117856 A CN96117856 A CN 96117856A CN 1156754 A CN1156754 A CN 1156754A
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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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E20/00—Combustion technologies with mitigation potential
- Y02E20/16—Combined cycle power plant [CCPP], or combined cycle gas turbine [CCGT]
- Y02E20/18—Integrated gasification combined cycle [IGCC], e.g. combined with carbon capture and storage [CCS]
Abstract
A process features that coal (or coke) as raw material is charged to gasifying furnace from the feeder connected to top of gasifying furnace and having sealing device, and the gasifying agent containing oxygen and steam is charged to gasifying furnace from its bottom. In gasifying furnace, redox reaction takes place to obtain semi-water gas or water gas, which is dusted and then goes into afterheat boiler to generate steam, which along with the steam from jacket boiler of gasifying furnace is over-heat treated and used as gasifying agent. Said semi-water gas or water gas is washed in washing tower and then refined to obtain refined synthetic gas.
Description
The invention relates to a method for continuously gasifying coal (coke) and refining synthesis gas by using coal (anthracite) and coke as raw materials.
In China, nearly thousands of middle and small nitrogen fertilizer plants exist, most of the plants use anthracite or coke as a raw material, and adopt an atmospheric fixed bed intermittent gasification technology, so that the process is backward, the energy consumption is high, the requirement on the granularity of the raw material is high (the coke is 25-75 m/m; the anthracite is 50-100 m/m), the utilization rate of the raw material is low, the product cost is high, the flow is long, the equipment structure is complex, each furnace system is provided with a respective hydraulic valve control system, the centralized control cannot be realized, and the environment is polluted.
The application number 93110917.5 discloses a coal (coke) atmospheric pressure continuous oxygen-enriched air gas-making process technology, which proposes the concept of oxygen-enriched continuous gasification, but it only makes a more precise measurement and calculation on the composition property of the raw coke, the raw utilization rate is still very low (up to 36%), the heat weight recovery rate is low, especially the harmful substances (such as organic sulfur, olefin, etc.) generated in the gasification process are ignored, so that the existing device can not produce qualified ammonia synthesis gas.
In view of the above, the present invention aims to provide a method for continuously gasifying coal (coke) and refining synthesis gas, which has the advantages of high thermal efficiency, energy saving, consumption reduction, high production capacity, easy centralized control, less environmental pollution, and complete purification of harmful substances in synthesis gas, so as to completely refine the coal (coke).
The purpose of the invention is realized by the following steps: the method is that coal (coke) raw material is added into a gasification furnace from a feeder containing a sealing device connected with a gasification furnace top of a slag-containing layer, a gasification combustion zone, a reduction zone, a dry distillation zone and a drying zone, gasification agent containing oxygen gas (oxygen-enriched air) and steam is fed from the gasification furnace bottom, semi-water gas or water gas prepared after oxidation-reduction reaction in the gasification furnace is sent into a waste heat boiler through a steam overheating dust remover to generate steam, the steam is used as the gasification agent after being heated with steam generated by a jacket boiler of the gasification furnace, the semi-water gas or water gas is purified after impurities are removed by a washing tower and then goes to a refining process to obtain refined synthesis gas, and slag is automatically discharged out of the furnace. The oxygen content concentration of the gasifying agent is more than or equal to 93 percent, and the gasifying agent and superheated steam are introduced together from the bottom of the furnace, wherein H2O/O2Approximately equal to 2 molecular ratio, and can generate CO and H rich after oxidation-reduction reaction with coal (coke) in a gasification furnace2Water gas (CO + H)2More than 80 percent), the qualified synthesis gas can be prepared after wet purification of the water gas in the refining process (see figure 1), and the synthesis gas can be used for preparing methanol, ethanol and the like, and other cheap devices can adopt a membrane separation device.
The gasification agent is oxygen-enriched air obtained by mixing oxygen from a pressure swing adsorption device such as a membrane separation device or other cheap oxygen supply devices such as a membrane separation device with air by using steam, and the oxygen-enriched air is subjected to oxidation-reduction reaction with coal (coke) in a gasification furnace to obtain the semi-water gas (see figure 1).
In the refining process, the semi-water gas is subjected to wet purification desulfurization, medium-temperature conversion, low-temperature conversion, deep conversion, carbonization, dry fine desulfurization and methanation to obtain qualified ammonia synthesis gas (see figure 1), which is a process applicable to producing ammonium bicarbonate products in small and medium fertilizer plants.
In the refining process, the semi-water gas is subjected to wet purification, desulfurization, medium-low temperature transformation, deep transformation, solution purification and decarburization, dry desulfurization and methanation to obtain qualified ammonia synthesis gas (see figure 1), so that the method is suitable for the process for producing urea products in medium and small fertilizer plants.
The catalyst used in the low-temperature shift in the refining step is a compound containing cobalt oxide and molybdenum oxide for converting organic sulfur (such as COS) into H2S is convenient to remove in the post process.
The oxygen concentration from the non-cryogenic air separation device is at least 93%, the oxygen content in the prepared oxygen-enriched raw gas is 45-55%, the prepared oxygen-enriched air is sprayed by hot condensate liquid at least 50 ℃ and then is mixed with steam, the gas saturation temperature reaches 85-90 ℃, and then the air is sent into a gasification furnace, so that a heat source is fully utilized.
The coal (coke) can be anthracite or coke (soil coke).
The coal (coke) can be formed coal pressed from anthracite and coke powder.
The granularity range of the coal (coke) raw material is 5-80 mm.
The method of the present invention is that coal (coke) raw material is continuously added from the top of the gasification furnace, oxygen-enriched air is fed from the bottom of the gasification furnace as gasification agent to carry out countercurrent gasification, the entering gasification agent is further uniformly distributed on the ash layer in the gasification furnace to prevent the grate from being affected by high temperature and prolong the service life, the gasification agent is preheated by the heat of the ash, in the gasification combustion zone in the gasification furnace, carbon in the raw material is oxidized by oxygen in the oxidant to generate CO2And CO and release a large amount of heat in the reaction formula
(the above reaction system is based on the oxygen content of oxygen-enriched air being 48%) CO2CO is reduced in the reduction layer of the gasification furnace, water vapor is decomposed into hydrogen, fuel is preheated by hot gas, and the reaction formula is as follows:
H2o (steam), CO2、H2S, organic sulfur, tar, methane, olefins, ammonia, nitrogen, hydrogen, and small amounts of cyanide. The hot gas evaporates the water content of the fuel in the drying zone of the gasifier by means of the heat of the rising gas, and the semi-water gas accumulates in the upper part of the fuel bed of the gasifier, i.e. in the free space.
When the semi-water gas is sent to the refining process for wet purification and desulfurization, alkaline aqueous solution (such as ammonia water, sodium carbonate, etc.) is mainly used, a small amount of active catalyst (such as shellac, ADA, hydroquinone, etc.) is added into the alkaline aqueous solution, and countercurrent absorption is carried out in a desulfurizing tower to remove sulfide (mainly H) contained in the gas2S), the removal efficiency is more than 95%. In the medium-temperature conversion step, CO and water vapor in the semi-water gas are converted into CO2And H2The reaction is carried out on a catalyst bed layer at the temperature of 260-360 ℃, and the reaction formula is as follows:
Because the semi-water gas contains H when being converted2S also contains a small amount of organic sulfur (such as COS, etc.), so the conversion catalyst should contain cobalt oxide and molybdenum oxide compounds to convert organic sulfur into H2S is convenient to be removed in the post process, and the reaction formula is as follows:
CO of the changed semi-water gas2To a relatively high concentration (about 30%), the gas is scrubbed with aqueous ammonia (containing ammonium carbonate) to remove CO during the carbonation stage2At the same time, CO2Reacting with ammonia water to generate ammonium bicarbonate, wherein the reaction formula is as follows:
The gas treated by the above process is substantially H2、N2Gas but contain a very small amount of CO and CO2Needs to be removed in the methanation process, and the principle is that a small amount of CO and CO is removed in the presence of a catalyst2Carrying out H addition2The reaction achieves the purpose of clearing, and the reaction formula is as follows:
The gas after the reaction contains a small amount of inert gas CH4(Ar) is in addition already pure H2、N2And (6) synthesizing gas.
Compared with the prior art, the invention has the following advantages:
1, complete research is carried out on changing the original gasification furnace into continuous gasification, so that the production capacity is greatly improved and can be 2 to 3 times of that of the original furnace; the particle size range of the raw materials can be expanded to 5-80 mm, namely the utilization rate of the raw materials is improved to 70% from the original 30%, and the pressed molded coal of pulverized coal can be used;
2, the raw materials entering the gasification furnace are uniformly distributed, the combustion and gasification reaction are completely carried out, the carrying amount of harmful substances is reduced, the burden of treating the harmful substances in the subsequent process is correspondingly reduced, the outlet temperature of the gasification furnace is 800 ℃ (the outlet temperature of patent application 93110917.5 is 700 ℃), and the heat recovery is increased;
3, the invention provides a method for preparing synthesis gas (CO + H) by using high-concentration oxygen (93 percent)2More than 80 percent) of the total process method opens up a new way for the development of products (preparing hydroxyl and carbonyl compounds) in small nitrogenous fertilizer plants in China.
In conclusion, the method has the advantages of high thermal efficiency, energy conservation, reduction, high production capacity, easy realization of centralized control, less environmental pollution and capability of completely purifying harmful substances in the synthesis gas.
The following detailed description of the embodiments of the present invention is provided in conjunction with the accompanying drawings, but the scope of the present invention is not limited to the following embodiments:
FIG. 1 is a process flow diagram of the present invention.
Example 1:
in order to save investment, the continuous gasification furnace I is realized by improving the original U.G.I intermittent fixed bed gas furnace; the raw material coal (coke) is fed into the furnace through a specially designed feeder which can meet the requirements of continuous gasification and uniform feeding, is closed, wear-resistant and safe, and then sequentially enters a drying layer, a dry distillation layer, a reduction layer and an oxidation layer, and then is automatically and continuously discharged. Oxygen (93% O or more) from Pressure Swing Adsorption (PSA) or other oxygen production plant 32) Preparing air from an air blower 2 in proportion until the concentration of oxygen in the oxygen-enriched air is 45-55%, and spraying hot condensate in a saturator 4 to enable the temperature to reach 50 ℃; then mixing the mixture with steam in a mixer 5 to enable the gas saturation temperature to reach 85-90 ℃, and then sending the mixture into a gasification furnace 1 from bottom to top to be used as a gasification agent. In-furnaceThe semi-water gas which is generated by the high-temperature reaction and is sent out from a gas holder 9 at the outlet of the upper part of the furnace is firstly subjected to wet desulphurization 10 to lead H contained in the gas2Removing more than 95% of S, introducing the gas into a conversion system, reducing CO from 40% to about 5% by medium-temperature conversion 11, controlling the temperature to be about 280 ℃, and generally controlling the steam-gas ratio to be 0.5-0.6; after the medium temperature shift 11, the gas enters the low and deep temperature shift 12 at 175-185 ℃ through internal heat exchange to reduce CO to about 0.5%.
In this case, the shift catalyst is of the cobalt-molybdenum system because of the presence of organic sulfur in the gas. Through the whole transformationThe post gas is sent into carbonization 14; on the one hand, the ammonium bicarbonate product is prepared, and on the other hand, the aim of removing CO2 is also fulfilled. CO after carbonization2Reduced to less than 0.2% of H2S is 0.01g/M3The gas is then subjected to dry desulfurization 15 to remove H2And the S is reduced to be below 0.1PPM, and the methanation 16 is carried out. In order to remove the trace impurities in the gas and remove the gas from the bottom, the temperature reaches 700-800 ℃, most coal dust is removed by a steam overheating dust remover 6, most heat is recovered by a waste heat boiler 7 after the steam is heated, the gas temperature is reduced to 250 ℃, then the gas enters a washing tower 8 to be cooled to below 40 ℃, and then the gas is sent to a semi-water gas cabinet 9. The gasification furnace 1 is provided with an improved jacket boiler and a waste heat boiler 7, and the byproduct of 0.2MPa steam is superheated by a heater 6, decompressed to 0.07MPa and then sent into the furnace together with oxygen-enriched air. Because of some differences between the continuous gasification and the batch gasification, the produced semi-water gas (water gas) contains a small amount of organic sulfur, olefin and other harmful substances for ammonia synthesis, and the harmful substances are required to be removed in the subsequent process. According to the production process route of different products (ammonium bicarbonate and urea) adopted by the current small nitrogen fertilizer plant part in China, the refined gas for preparing ammonia synthesis (including the synthesis gas preparation) has different process flows which are respectively explained as follows:
1) the product is ammonium bicarbonate added with 0-8% (wt) of inorganic compound, and the trace impurities in the methanated gas are reduced to below 10PPM to meet the quality requirement of preparing ammonia synthesis gas.
2) The product is urea
Semi-water coal according to the above processGas is subjected to medium, low and deep temperature conversion 11, 12, and is sent into a solution purification system 17 after internal heat exchange to mainly remove CO2And sulfides (organic sulfur and inorganic sulfur), the gas is subjected to dry desulfurization 13 and then methanation 18 (inorganic compounds are added) to prepare qualified ammonia synthesis gas.
At low and deep temperature change, the catalyst can be added with cobalt oxide and molybdenum oxide compounds.
Example 2:
according to the process flow 1-10 in the attached figure 1, the gasifying agent adopts more than or equal to 93 percent of high-concentration waste oxygen to be mixed with superheated steam according to H2O/O2Continuous gasification with the molecular ratio of about 2 can produce CO + H rich2And (3) performing wet desulphurization on the water gas (10), and then performing wet desulphurization on the water gas to obtain qualified synthetic gas for further processing (such as processing to prepare hydroxyl, carbonyl compounds and the like) after the water gas passes through a Benfield solution (MDEA) in a purification system 19.
If methanol catalyst (Cu, Zn, Al) is added into the synthesis tower 20, the methanol product can be obtained after passing through the rectifying device 21.
If an ethanol catalyst (rhodium catalyst) is added into the synthesis tower 20, an ethanol product (or acetaldehyde product) can be obtained after passing through the rectifying device 21.
Claims (10)
1. A process for continuously gasifying coal (coke) and refining synthetic gas includes such steps as adding coal (coke) to gasifier from the feeder containing sealing unit, feeding gasifying agent containing oxygen and steam from the bottom of gasifier, oxidizing-reducing reaction to obtain semi-water gas or water gas, passing through steam-overheat duster, delivering it to waste heat boiler to generate steam, overheating together with steam generated by jacket boiler of gasifier, removing impurities from semi-water gas or water gas, washing, and refining.
2. The method for continuous coal (coke) gasification and syngas refining as claimed in claim 1, wherein the gasifying agent contains oxygen with concentration>93%, and H is introduced into the gasifying agent from the bottom of the furnace together with superheated steam2O/O2Approximately equal to 2 molecular ratio, and can generate CO and H rich after oxidation-reduction reaction with coal (coke) in a gasification furnace2And performing wet purification, desulfurization and decarburization on the water gas in a refining process to obtain qualified synthesis gas.
3. The method according to claim 1, wherein the gasifying agent is oxygen-enriched air obtained by mixing steam and oxygen from a pressure swing adsorption device, a membrane separation device or other cheap oxygen supply devices with air, and the semi-water gas is obtained by oxidation-reduction reaction with the coal (coke) in the gasifier.
4. The method for continuous coal (coke) gasification and syngas refining as claimed in claim 3, wherein the qualified ammonia syngas is obtained from the semi-water gas in the refining process through wet purification and desulfurization, medium temperature shift, low temperature shift, deep shift, carbonization, dry fine desulfurization and methanation.
5. The method for continuous coal (coke) gasification and syngas refining as claimed in claim 3, wherein the qualified ammonia syngas is obtained after wet purification and desulfurization, medium and low temperatureshift, solution purification and decarburization, desulfurization and methanation of the semi-water gas in the refining process.
6. The method for continuous coal (coke) gasification and syngas refining as claimed in claim 4 or 5, characterized in that the catalyst used in low temperature shift in the refining step is a compound containing cobalt oxide and molybdenum oxide.
7. The method according to claim 3, wherein the oxygen concentration of the membrane separation device or other inexpensive support device of the pressure swing adsorption device is at least 93%, the oxygen content of the oxygen-enriched air is 45-55% (by volume), the oxygen-enriched air is sprayed with hot condensate at least 50 ℃ and then mixed with steam to reach a gas saturation temperature of 85-90 ℃, and then fed into the gasification furnace.
8. The method for continuous coal (coke) gasification and syngas refining according to claim 1, wherein the coal (coke) can be anthracite or coke.
9. The method for continuous coal (coke) gasification and syngas refining according to claim 1, wherein the coal (coke) is briquette formed by pressing anthracite and coke powder.
10. The method for continuous coal (coke) gasification and syngas refining according to claim 1, wherein the particle size of the coal (coke) raw material is in the range of 5-80 mm.
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| CN96117856A CN1057322C (en) | 1996-12-30 | 1996-12-30 | Method for continuously gasifying coal (coke) and purifying synthesized gas |
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| CN96117856A CN1057322C (en) | 1996-12-30 | 1996-12-30 | Method for continuously gasifying coal (coke) and purifying synthesized gas |
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| CN100419049C (en) * | 2006-05-09 | 2008-09-17 | 黑龙江黑化集团有限公司 | Process of producing synthetic gas of carbinol and dimethyl ether by all oxygen gasifying of poor goal |
| CN101659395A (en) * | 2009-05-07 | 2010-03-03 | 湖北双环科技股份有限公司 | Process for preparing feed gas for synthetic ammonia by two-stage furnace coal gasification taking cold-pressed briquette as raw material |
| CN102206512A (en) * | 2011-04-25 | 2011-10-05 | 湖北双环科技股份有限公司 | Method for preparing semiwater gas through oxygen-rich air continuous gasification |
| CN102391892A (en) * | 2011-09-21 | 2012-03-28 | 首钢总公司 | Blast furnace gas enrichment apparatus and method |
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| CN102690686A (en) * | 2012-06-01 | 2012-09-26 | 中国石油和化工勘察设计协会煤化工设计技术中心 | Method for preparing ammonia synthesis gas by pressing and continuously gasifying anthracite by oxygen-enriched air |
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| CN102994151A (en) * | 2012-12-13 | 2013-03-27 | 新疆宜化化工有限公司 | Method for preparing semi-water gas through oxygen-enrichment continuous gasification |
| CN103154210A (en) * | 2010-08-16 | 2013-06-12 | 能源与环境研究中心基金会 | Sandwich gasification process for high-efficiency conversion of carbonaceous fuels to clean syngas with zero residual carbon discharge |
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| CN1092799A (en) * | 1993-03-23 | 1994-09-28 | 四川蜀华化工新技术开发有限公司 | Coal (Jiao) process for atmospheric continuous oxygen-enriched air gasification of coal (coke) |
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- 1996-12-30 CN CN96117856A patent/CN1057322C/en not_active Expired - Fee Related
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| CN107090318A (en) * | 2008-01-07 | 2017-08-25 | 通用电气公司 | Promote the method and apparatus of synthetic natural gas production |
| CN102876386B (en) * | 2009-02-18 | 2014-01-01 | 刘宏建 | Gasification method for preparing gas by using fixed bed gasifier |
| CN102876386A (en) * | 2009-02-18 | 2013-01-16 | 刘宏建 | Gasification method for preparing gas by using fixed bed gasifier |
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| CN102994151A (en) * | 2012-12-13 | 2013-03-27 | 新疆宜化化工有限公司 | Method for preparing semi-water gas through oxygen-enrichment continuous gasification |
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