CN104986732A - Method for preparing synthesis gas through coke oven gas and coal gas - Google Patents
Method for preparing synthesis gas through coke oven gas and coal gas Download PDFInfo
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- CN104986732A CN104986732A CN201510388476.1A CN201510388476A CN104986732A CN 104986732 A CN104986732 A CN 104986732A CN 201510388476 A CN201510388476 A CN 201510388476A CN 104986732 A CN104986732 A CN 104986732A
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Abstract
The invention provides a method for preparing synthesis gas through coke oven gas and coal gas. The coke oven gas and the coal gas are fed to a gas holder to be fully mixed, mixed gas is obtained, methane reforming is conducted on one part of the mixed gas, reformed gas and the other part of mixed gas converge, and are compressed and then purified, H2S, remaining CO2 and other impurities are removed, removed hydrogen sulfide is desulphurized and recovered, removed CO2 is emptied, methane separation is conducted on purified coarse feed gas, liquefied natural gas products or compressed natural gas products are prepared through separated methane gas, and the pure synthesis gas meeting the requirement of the hydrogen-carbon ratio of synthesis downstream products is prepared through gas in which methane is separated. The method has the advantage that the coal gas and the coke oven gas are comprehensively utilized.
Description
Technical field
The invention belongs to a kind of method that will coke-oven gas and gas maked coal utilized to prepare synthetic gas.
Background technology
Synthetic gas is with carbon monoxide and hydrogen for main ingredient, as a kind of unstripped gas of industrial chemicals.Synthetic gas is of many uses, is synthetic ammonia, Sweet natural gas, methyl alcohol, ethylene glycol, low-carbon alkene, the most basic raw material of synthesis wet goods product.The raw material range of synthetic gas is very wide, is produced, also can be produced by the light hydrocarbons such as Sweet natural gas and petroleum naphtha, also can be produced through partial oxidation process by heavy oil by carbon containing mineral matter as the solid fuel gasification such as coal, charcoal.
Synthetic gas composition (volume %) that various method is produced has very big difference: H
2: 32 ~ 67, CO:10 ~ 57, CO
2: 2 ~ 28, CH
4: 0.1 ~ 14, N
2: 0.6 ~ 23.In addition, the H of trace is also had
2the objectionable constituent such as S, COS, HCN.By the synthetic gas obtained by these raw materials, because its H/C mol ratio difference is huge, the needs of sintetics usually directly can not be met, its composition need be adjusted, the main method of adjustment utilizes water-gas reaction (transformationreation), to reduce carbon monoxide, improves the content of hydrogen.
Rich coal resources in China, coal becomes the starting material of many basic chemical industry products, particularly with the low-quality brown coal on the ground such as Inner Mongol, Xinjiang for raw material, through the synthetic gas that vapourizing furnace is obtained, then carrying out the synthesis of downstream Chemicals is that the clean and effective of coal utilizes effective way, but (gas composition volume percent is: CO:45-62%, H to have the feature of " the many hydrogen of carbon is few " by producing synthesis gas from coal
2: 18-29%, CO
2: 8-21%, CH
4: 7-16%, H
2s:0.15-0.65%), carrying out downstream Chemicals synthesis often needs to carry out benefit hydrogen or water-gas shift operating unit, reaches suitable hydrogen-carbon ratio.Meanwhile, China is also first coke production state in the world, produces the coke a large amount of coke-oven gas of by-product simultaneously.The main component of coke-oven gas is the hydrogen of (volume ratio): 48-65%, the methane of 18-30%, the CO+CO of 8-18%
2.In addition, the H of trace is also had
2the objectionable constituent such as S, COS, HCN.These coke-oven gas parts are used for methyl alcohol processed, synthetic ammonia and factory's combustion gas, and remote districts are then emitted in vain.Current coke-oven gas nearly 300 billion cubic meter coke(oven)gas more than needed every year except production synthetic ammonia and methyl alcohol, due to the feature of coke-oven gas composition " the many carbon of hydrogen is few ", cause the capacity usage ratio of coke-oven gas present stage to be about about 55%, cause huge energy dissipation and environmental pollution.
From the feature of coke-oven gas and gas maked coal, synthetic ammonia, Sweet natural gas, methyl alcohol, ethylene glycol is produced separately by coke-oven gas or gas maked coal, low-carbon alkene, synthesis wet goods product, all exist component ratio unbalanced, utilize insufficient problem: the many carbon of coke-oven gas hydrogen is few, separately must occur that a large amount of hydrogen remains for the synthesis of product, or need other supplementary carbon source; And the many hydrogen of gas maked coal carbon is few, is used alone and will there will be a large amount of carbon residue, or need a large amount of supplemental hydrogen source in addition.
In current actual production, the feature few to the many hydrogen of gas maked coal carbon, generally by water-gas shift, obtained rational hydrogen-carbon ratio; Few to the many carbon of coke-oven gas hydrogen, the feature that methane content is high, usually adopts methane carbon dioxide reformation to solve, but no matter is water-gas shift, or methane reforming all exists, and investment is high, power consumption is large, operation runs the problems such as complicated.
If coke-oven gas and synthetic gas are mixed in proportion, can reach and learn from other's strong points to offset one's weaknesses, form the gas composition meeting the different Chemicals of synthesis, realize " it uses gas to the greatest extent " of coke-oven gas and gas maked coal, turn waste into wealth, reduce water-gas shift or methane reforming workshop section, reach that technical process is simple, less investment, operation, overhead charges are low.The method not only produces obvious economic benefit and environmental benefit, also significant to Energy restructuring.
Summary of the invention
The object of this invention is to provide a kind of utilize coke-oven gas and gas maked coal realizing the comprehensive utilization of gas maked coal and coke-oven gas and prepare the method for synthetic gas.
It is few that the present invention can make full use of the many hydrogen of gas maked coal composition carbon, and the feature that the many carbon of coke-oven gas hydrogen is few, both are mixed by a certain percentage, learns from other's strong points to offset one's weaknesses, meet the hydrogen-carbon ratio requirement of synthesis multiple product.Solve simultaneously and adopt separately coke-oven gas production chemical product to need to mend carbon or adopt separately gas maked coal inhibition and generation chemical product to need the shortcoming of mending hydrogen or carrying out water-gas shift, realize the comprehensive utilization of gas maked coal and coke-oven gas.
For achieving the above object, the present invention adopts following scheme:
(1) coke-oven gas and gas maked coal are passed into gas holder and be fully mixed to get gas mixture, a part of gas mixture carries out methane reforming, reformed gas and another part gas mixture is converged and compresses, and forms the coarse raw materials gas meeting chemical industry synthesis hydrogen-carbon ratio and require;
(2) coarse raw materials gas purifies after compression, removes H
2s and remaining CO
2deng impurity, the hydrogen sulfide desulfuration removed reclaims, the CO removed
2gas emptying, coarse raw materials gas after purification carries out methane separation, isolated methane gas obtains LNG product (natural gas liquids) or CNG product (compressed natural gas), and the gas isolating methane obtains the pure synthetic gas meeting synthesis derived product hydrogen-carbon ratio and require.
Synthetic gas as above can be used for producing Sweet natural gas, methyl alcohol, ethylene glycol, dme, low-carbon alkene, synthesis wet goods, but is not limited to listed several prods
The source of coke-oven gas as above can be tamping coke furnace, top dress coke oven, dichotomic type coke oven or twin coke oven.
The source of gas maked coal as above can be crushed coal pressurized-gasification furnace, Lurgi gasifier, ash agglomerating stove, texaco coal-water slurry gasification stove, multi-nozzle coal slurry gasifier or space flight stove etc.
The mol ratio of coke-oven gas as above and gas maked coal is between 0.2-9.0:1.
The percent by volume that the gas mixture carrying out methane reforming as above accounts for total gas mixture is 10-95%.
Methane reforming as above adopts Ni/ γ-Al
2o
3or Ru/ γ-Al
2o
3catalyzer, temperature is 600-750 DEG C, and pressure is 1.0-4.0MPa.
Raw material gas purifying as above can be tannin process, ADA method, thermokalite method, NHD method, low-temperature rectisol method or complex iron etc.
Raw material gas purifying as above preferably adopts low-temperature rectisol, and its service temperature is-35 ~-55 DEG C, and working pressure is 2.0-6.5MPa, H in the coarse raw materials gas after low-temperature rectisol
2s<0.1ppm, CO
2<20ppm.
Due to the coarse raw materials gas complicated component that synthetic gas and coke-oven gas form.Its gaseous fraction comprises CO, H
2, CO
2, CH
4the H of denier
2s, organosulfur, tar, lipid acid, petroleum naphtha etc.Except CO, H in these components
2active principle, all the other all components comprise CO
2all need the detrimental impurity that removes with sulfide, the arduousness of its purification task as seen.Make a general survey of current various gas purifying technique, this person with heavy responsibilities's non-cryogenic methanol wash column can be taken on and do not belong to.This is because only have low-temperature rectisol to purify just all can remove various objectionable constituent neatly, such as CO in same device
2, H
2s, COS, C
4h
4s, HCN, NH
3, H
2o, C
2above hydro carbons (comprising light oil, aromatic hydrocarbon, petroleum naphtha, alkene and colloid etc.) and other carbonyl compound etc., and other any purification process all cannot be accomplished.In addition, low-temp methanol washing process also has following various significant advantage compared with other purification process:
1. receptivity is strong, and solution circulated amount is little
2. methanol solvate is cheap and easy to get, and regeneration energy consumption is low
3. gas purification degree is high
4. solvent thermal stability and chemical stability good, solvent is not degraded, non-foaming, does not corrode equipment
5. first alcohol and water can dissolve each other by arbitrary proportion, utilizes this characteristic can with its dried feed gas
Low-temperature rectisol achieves removing of plurality of impurities in the same apparatus, and for the multiple purification process combination of other purifying methods, operation is relatively single, reasonable, and convenient operation manages.
Methane separation as above can adopt supercritical gas extraction isolation technique or adopt the cold separation technology of the U.S. safe this and the neat company of Bock Lightware, separation temperature is-150 DEG C to-170 DEG C, preferably-155 DEG C to-165 DEG C, separating pressure is 3-8Mpa, preferred 4.0-5.5Mpa.
The present invention compared with prior art, has clear superiority:
1, synthetic gas hydrogen-carbon ratio is controlled, meets multiple product synthesis requirement.The present invention is few according to the many carbon of coke-oven gas hydrogen, and the feature that the many hydrogen of gas maked coal composition carbon is few, both mixed by a certain percentage, learn from other's strong points to offset one's weaknesses, gas mixture is reformed and purifying treatment through portion of methane, then through methane separation, obtained pure synthetic gas.The synthetic gas that the inventive method obtains can meet the hydrogen-carbon ratio requirement of synthesis multiple product, such as produce synthetic ammonia, Sweet natural gas, methyl alcohol, low-carbon alcohol, dme, ethylene glycol, low-carbon alkene, the hydrogen-carbon ratio of synthesis wet goods product requirement from 1.0 to 5.0 not etc., and is difficult to meet hydrogen-carbon ratio requirement by coke-oven gas or gas maked coal separately.Isolate gas product to use as the fuel of more high value simultaneously.
2, the present invention solves simultaneously and adopts separately coke-oven gas production chemical product to need to mend carbon or adopt separately gas maked coal inhibition and generation chemical product to need to mend hydrogen, and makes the technical process of above-mentioned two kinds of gases recycling long, complicated operation, shortcoming costly.The shortcoming of two kinds of gas resources organically combines by the present invention, become the advantage of mutual supplement with each other's advantages, and the different derived product of synthesis can be realized by the ratio of mixture controlling coke-oven gas and gas maked coal to the requirement of hydrogen-carbon ratio, realize turning waste into wealth of gas maked coal and coke-oven gas, comprehensive utilization.
Accompanying drawing explanation
Fig. 1 is process flow sheet of the present invention.
Embodiment
Below in conjunction with specific embodiment, the present invention is described in detail, and these embodiments are only for specifically describing the present invention more in detail, and the scope that should not be construed as the above-mentioned theme of the present invention is only limitted to the restriction of following embodiment.
Embodiment 1
(volume percent consists of H to the coke-oven gas produced by top dress coke oven
2: 54%, CH
4: 25%, CO+CO
2: 15%, N
2: 6%) and volume crushed coal pressure gasifying produce gas maked coal (volume percent consists of CO:52%, H
2: 23%, CO
2: 14%, CH
4: 11%, H
2s:0.25%) send into gas holder by mole throughput ratio 6.0:1 fully to mix, the gas mixture of 40% volume carries out at Ni/ γ-Al
2o
3catalyzer, temperature 610 DEG C, methane reforming is carried out under pressure 1.2MPa condition, the gas mixture of reformed gas and all the other 60% volumes is converged and compresses, form the coarse raw materials gas that H:Cmoleratio is 3.13, coarse raw materials gas enters low-temperature rectisol purification after compression, at pressure 4.5MPa, removes H under temperature-43 DEG C of conditions
2s and CO
2deng impurity, obtain H
2s content is less than 0.1ppm, CO
2content is less than the unstripped gas of 20ppm, the rear H removed
2s desulfuration reclaims, the CO removed
2gas emptying, coarse raw materials gas after purification enters low temperature separation process methane separation, and at pressure 5.5MPa, under temperature-163 DEG C of conditions, separation of methane obtains LNG (natural gas liquids) product, obtaining H:Cmoleratio is 3.13, can meet the pure synthetic gas that synthetic gas preparing natural gas uses.
Embodiment 2
(volume percent consists of H to the coke-oven gas produced by tamping coke furnace
2: 60%, CH
4: 23%, CO+CO
2: 11%, N
2: 6%) and crushed coal pressure gasifying produce gas maked coal (volume percent consists of CO:54%, H
2: 26%, CO
2: 10%, CH
4: 10%, H
2s:0.03%) send into gas holder by mole throughput ratio 2.0:1 fully to mix, the gas mixture of about 25% volume enters methane reforming, at Ru/ γ-Al
2o
3catalyzer, temperature 710 DEG C, reforms under pressure 2.0MPa condition, reformed gas and gas mixture are converged and compress, form the coarse raw materials gas that H:Cmoleratio is 2.08, coarse raw materials gas enters hot alkali purification after compression, at pressure 1.6MPa, under temperature 98 DEG C of conditions, remove H
2s and CO
2deng impurity, obtain H
2s content is less than 0.1ppm, CO
2content is less than the unstripped gas of 20ppm, the rear H removed
2s desulfuration reclaims, the CO removed
2gas emptying, coarse raw materials gas after purification enters supercritical methane and is separated, at pressure 4.5MPa, the supercritical state separation of methane of temperature-77 DEG C obtains CNG (compressed natural gas) product, obtaining H:Cmoleratio after methane separation is 2.08, can meet the pure synthetic gas that synthesising gas systeming carbinol uses.
Embodiment 3
(volume percent consists of H to the coke-oven gas produced by tamping coke furnace
2: 48%, CH
4: 28%, CO+CO
2: 17%, N
2: 7%) and texaco coal-water slurry gasification stove produce gas maked coal (volume percent consists of CO:49%, H
2: 24%, CO
2: 14%, CH
4: 13%, H
2s:0.03%) send into gas holder by mole throughput ratio 6.0:1 fully to mix, the gas mixture of about 80% volume enters methane reforming, at Ru/ γ-Al
2o
3catalyzer, temperature 670 DEG C, reforms under pressure 2.3MPa condition, reformed gas and gas mixture are converged and compress, form the coarse raw materials gas that H:Cmoleratio is 2.27, coarse raw materials gas enters low-temperature rectisol purification after compression, at pressure 5.0MPa, under temperature-49 DEG C of conditions, remove H
2s and CO
2deng impurity, obtain H
2s content is less than 0.1ppm, CO
2content is less than the unstripped gas of 20ppm, the rear H removed
2s desulfuration reclaims, the CO removed
2gas emptying, coarse raw materials gas after purification enters low temperature separation process methane separation, at pressure 5.0MPa, under temperature-167 DEG C of conditions, separation of methane obtains LNG (natural gas liquids) product, obtaining H:Cmoleratio after methane separation is 2.27, can meet the pure synthetic gas that synthetic gas synthetic oil uses.
Embodiment 4
(volume percent consists of H to the coke-oven gas produced by twin coke oven
2: 56%, CH
4: 27%, CO+CO
2: 12%, N
2: 5%) and ash agglomerating stove stove produce gas maked coal (volume percent consists of CO:52%, H
2: 25%, CO
2: 11%, CH
4: 12%, H
2s:0.04%) send into gas holder by mole throughput ratio 1:1 fully to mix, the gas mixture of about 55% volume enters methane reforming, at Ni/ γ-Al
2o
3catalyzer, temperature 650 DEG C, carries out reforming under pressure 2.0MPa condition, reformed gas and gas mixture are converged and compress, form the coarse raw materials gas that H:Cmoleratio is 1.32, coarse raw materials gas enters the purification of NHD method after compression, at pressure 2.5MPa, under temperature 2 DEG C of conditions, remove H
2s and CO
2deng impurity, obtain H
2s content is less than 0.1ppm, CO
2content is less than the unstripped gas of 20ppm, the rear H removed
2s desulfuration reclaims, the CO removed
2gas emptying, coarse raw materials gas after purification enters supercritical methane and is separated, at pressure 4.55MPa, the supercritical state separation of methane of temperature-77.5 DEG C obtains CNG (compressed natural gas) product, obtaining H:Cmoleratio after methane separation is 1.32, can meet the pure synthetic gas that synthetic gas preparing dimethy ether uses.
Claims (11)
1. utilize coke-oven gas and gas maked coal to prepare a method for synthetic gas, it is characterized in that comprising the steps:
(1) coke-oven gas and gas maked coal are passed into gas holder and be fully mixed to get gas mixture, a part of gas mixture carries out methane reforming, reformed gas and another part gas mixture is converged and compresses, and forms the coarse raw materials gas meeting chemical industry synthesis hydrogen-carbon ratio and require;
(2) coarse raw materials gas purifies after compression, removes H
2s and remaining CO
2deng impurity, the hydrogen sulfide desulfuration removed reclaims, the CO removed
2gas emptying, the coarse raw materials gas after purification carries out methane separation, and isolated methane gas obtains liquefied natural gas product or compressed natural gas product, and the gas isolating methane obtains the pure synthetic gas meeting synthesis derived product hydrogen-carbon ratio and require.
2. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, is characterized in that the source of described coke-oven gas is tamping coke furnace, top dress coke oven, dichotomic type coke oven or twin coke oven.
3. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, is characterized in that the source of described gas maked coal is crushed coal pressurized-gasification furnace, Lurgi gasifier, ash agglomerating stove, texaco coal-water slurry gasification stove, multi-nozzle coal slurry gasifier or space flight stove.
4. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, is characterized in that the mol ratio of described coke-oven gas and gas maked coal is between 0.2-9.0:1.
5. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, is characterized in that the percent by volume that the described gas mixture carrying out methane reforming accounts for total gas mixture is 10-95%.
6. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, is characterized in that described methane reforming adopts Ni/ γ-Al
2o
3or Ru/ γ-Al
2o
3catalyzer, temperature is 600-750 DEG C, and pressure is 1.0-4.0MPa.
7. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, is characterized in that described raw material gas purifying is tannin process, ADA method, thermokalite method, NHD method, low-temperature rectisol method or complex iron.
8. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, it is characterized in that described raw material gas purifying adopts low-temperature rectisol, its service temperature is-35 ~-55 DEG C, and working pressure is 2.0-6.5MPa, H in the coarse raw materials gas after low-temperature rectisol
2s<0.1ppm, CO
2<20ppm.
9. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 1, it is characterized in that described methane separation can adopt supercritical gas extraction isolation technique or adopt the cold separation technology of the U.S. safe this and the neat company of Bock Lightware, separation temperature is-150 DEG C to-170 DEG C, and separating pressure is 3-8Mpa.
10. a kind of method utilizing coke-oven gas and gas maked coal to prepare synthetic gas as claimed in claim 9, it is characterized in that described separation temperature is-155 DEG C to-165 DEG C, separating pressure is 4.0-5.5Mpa.
11. a kind of methods utilizing coke-oven gas and gas maked coal to prepare synthetic gas as described in any one of claim 1-10, is characterized in that described synthetic gas is for the production of Sweet natural gas, methyl alcohol, ethylene glycol, dme, low-carbon alkene or synthetic oil.
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| CN110243992A (en) * | 2018-03-09 | 2019-09-17 | 国家能源投资集团有限责任公司 | The preparation method and Catalyst evaluation test system of evaluating catalyst unstripped gas |
| CN110885708A (en) * | 2019-11-21 | 2020-03-17 | 山西焦煤集团有限责任公司 | Coal desulfurization and deliming experimental method utilizing supercritical fluid osmotic dissolution capacity |
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| CN104986732B (en) | 2017-01-04 |
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