CN103804138A - Technology for producing methanol through coke oven gas - Google Patents

Technology for producing methanol through coke oven gas Download PDF

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Publication number
CN103804138A
CN103804138A CN201410086174.4A CN201410086174A CN103804138A CN 103804138 A CN103804138 A CN 103804138A CN 201410086174 A CN201410086174 A CN 201410086174A CN 103804138 A CN103804138 A CN 103804138A
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gas
coke
oven
coke oven
methyl alcohol
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CN103804138B (en
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易群
张继龙
张小超
郑华艳
荆洁颖
李刚
任龙
任晓霞
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Taiyuan University of Technology
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    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
    • C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
    • C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
    • C07C29/1516—Multisteps
    • C07C29/1518—Multisteps one step being the formation of initial mixture of carbon oxides and hydrogen for synthesis
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0211—Processes for making hydrogen or synthesis gas containing a reforming step containing a non-catalytic reforming step
    • C01B2203/0222—Processes for making hydrogen or synthesis gas containing a reforming step containing a non-catalytic reforming step containing a non-catalytic carbon dioxide reforming step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/061—Methanol production

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Industrial Gases (AREA)

Abstract

The invention relates to a technology for producing methanol through coke oven gas, belonging to the technical field of coking and methanol preparation. The technology comprises the steps of purifying crude coke oven gas generated by a coke oven, to obtain clean coke oven gas, mixing the clean coke oven gas with CO2 separated by a separator, and sending in a CO2 coke oven gas reformer; boosting the reformed synthesis gas through a compressor, mixing the boosted reformed synthesis gas with circulating reaction gas to enter a methanol synthesizer for reaction; performing gas-liquid separation to the generated methanol and unreacted gas, outputting crude methanol from the bottom, boosting the unreacted gas from the top through a circulating compressor, sending in a gas buffer tank, wherein a part of gas is sent to an oil separator for circulating use; mixing the other part of gas, as fuel gas, with a part of coke oven gas to enter a coke oven vertical fire channel, performing combustion and heat transfer together with oxygen from an air separator, wherein the generated waste gas is subjected to gas-liquid separation to remove CO2 for circulation use. According to the technology, the gradient utilization of chemical energy can be realized, CO2 can be efficiently recycled, and internal carbon compensation of the technology can be realized, no purge gas and flue gas are generated, zero emission can be realized, and the high-efficiency clean utilization of coking industry resources can be promoted.

Description

A kind of coke-oven gas methanol technics processed
Technical field
The present invention relates to a kind of coke-oven gas methanol technics processed, be specifically related to the synthetic middle unreacting gas of a kind of methyl alcohol and do coke oven combustion gas, the CO in coke oven exhaust gas 2processing method with clean coke-oven gas preparing synthetic gas by reforming methyl alcohol processed.Belong to coking technology and methyl alcohol technical field.
Background technology
Synthesising gas systeming carbinol is the most important Technology of carbon geochemistry.Can be by gasification preparing synthetic gas methyl alcohol processed again, also can be by preparing synthetic gas by natural gas partial oxidation methyl alcohol processed again, also having popular especially at present field is coke-oven gas methyl alcohol processed.The increase of coke output impels the increase of coke-oven gas, 1 ton of coke of every production 400Nm that will have an appointment 3coke-oven gas produce.Within 2012, coke-oven gas output reaches 1,945 hundred million Nm 3, be equivalent to 6.5 West-East National Gas Transmission Project year displacements (analysis and suggestion that coke-oven gas utilizes, Coal Chemical Industry, 2013,3:4-8), can produce approximately 9,000 ten thousand tons of methyl alcohol.But coke-oven gas is because its hydrogen richness surpasses 50%, so hydrogen-carbon ratio is much larger than theoretical synthesizing methanol amount, need to mend carbon and make up technological process, and at present coking industry do not have unnecessary carbon source for, so be generally to increase vapourizing furnace to mend carbon, increase so again the investment of coal chemical enterprise, also increased source of pollution.
In addition, in methyl alcohol is synthetic, synthetic gas per pass conversion is very low, and substantially in 7% left and right, optimum technique is also only more than 20% at present.So a large amount of unreacting gas need to recycle, and has increased energy consumption, and can enrichment CO in recirculation process 2, need speed venting and supplementary virgin gas of regular discharge to carry out keeping system and normally move.And generally direct " point day a lamp " or offer boiler or reformer etc. as fuel of venting of speeding, contaminate environment and consume hydrogen resource.These problems are that methyl alcohol enterprise need solve always.
Summary of the invention
The object of the invention is, for above problem, provides the technique of a kind of coke-oven gas methyl alcohol processed, coke oven produce waste gas by gas-liquid separator by CO 2isolate with purify after clean coke-oven gas make synthetic gas by reformation, then enter methyl alcohol synthesizer by pressurization, unreacting gas circulates by gas-liquid separator separates rear section, remaining is used for heating coke oven as coke oven fuel gas and oxygen combustion, form large coking circulation route, solved that coke-oven gas methyl alcohol processed need to be mended carbon and the problem of the bleed air exhaust of speeding.
The present invention is achieved by the following technical solutions:
A kind of coke-oven gas methanol technics processed, is characterized in that: comprise the following steps:
I, air is sent into air trap, the O of generation 2send in coke oven; Coking coal is sent into coke oven, obtain product coke and thick coke-oven gas;
The thick coke-oven gas that II, coke oven produce obtains clean coke-oven gas through dedusting, denitrogenation, after washing benzene, desulfurizing and purifying operation, sends into gas holder;
The waste gas that III, coke oven combustion produce is through CO 2water separator is isolated CO 2, mix and send into CO with the clean coke-oven gas of part of gas holder output in step II 2coke-oven gas reformer; Another part coke-oven gas of gas holder output turns back to recycle in coke oven;
Synthetic gas after IV, reformation is sent into oil separator after compressor supercharging, enters methyl alcohol synthesizer top after preheater preheating, reacts;
The methanol vapor generating in V, methyl alcohol synthesizer and unreacting gas be from the bottom output of methyl alcohol synthesizer, enters gas-liquid separator separates and go out thick methyl alcohol and export from bottom after preheater heat exchange, heat exchanger heat exchange cooling;
VI, unreacting gas are sent into gas buffer tank from the output of gas-liquid separator top through recycle compressor pressurization;
Part unreacting gas in VII, gas buffer tank enters oil separator, and the synthetic gas after reforming with step III mixes, and then sends into methyl alcohol synthesizer; Another part unreacting gas in gas buffer tank turns back in coke oven as fuel gas utilization.
Further, the coke-oven gas that the unreacting gas that described step VII is returned returns with step III mixes as fuel gas and enters coke oven vertical flame path, and the oxygen coming with air trap burns, for coking provides heat.
Further, in described step III, gas holder is sent to CO 2the clean coke-oven gas ratio of coke-oven gas reformer accounts for the 50%-90% of coke-oven gas total amount.
Further, the described unreacting gas ratio of returning to coke oven combustion heat supply accounts for the 10%-70% of unreacting gas total amount.
CO 2water separator is isolated CO 2amount be exhaust gas volume 21-25%, the 66-76% that isolated water is exhaust gas volume, isolated O 2for the 0-12% of exhaust gas volume.
The advantage of coke-oven gas provided by the invention methanol technics processed is:
1) effectively utilize the carbon, the hydrogen resource that in production process, produce, realized CO 2the recycling of high-efficiency low energy consumption, for internal system, oneself mends carbon, avoids extra increasing to mend the extra investment and the energy expenditure that in carbon process, cause, has simplified production technique, has reduced system investment and production energy consumption, has reduced CO 2discharge;
2) the integrated degree of coupling of process system is high, utilizes low-grade unreacting gas Substitute For Partial higher-grade coke-oven gas combustion heat supplying, reduces combustion processes power loss, has realized the cascade utilization of chemical energy, has improved whole production system energy utilization efficiency;
3) every grade of resource of whole industrial chain of coking all " is eaten dry squeezing only ", and Energy resources trans-utilization degree is high, and element is complementary to be utilized, CO 2near zero release, each production link matching complete, has formed complete environment-protective circulating and has produced chain;
4) compared with the system of mending carbon production technique with tradition, this system has been preserved most of original production equipment and equipment, only, in original technical suitable change of having carried out, still realized the variation of whole system overall efficiency matter and the lifting of benefit, new technology easily realizes industrialization promotion at short notice.
Accompanying drawing explanation
Fig. 1 is the process flow sheet of coke-oven gas of the present invention methyl alcohol processed.
1-coke oven in figure; 2-purification unit; 3-gas holder; 4-CO 2water separator; 5-CO 2coke-oven gas reformer; 6-compressor; 7-oil separator; 8-methyl alcohol synthesizer; 9-gas preheater; 10-heat exchanger; 11-gas-liquid separator; 12-recycle compressor; 13-gas buffer tank; 14-air trap.
Embodiment
Further illustrate the present invention below in conjunction with drawings and Examples, the invention will be further described, understands the claimed technological thought of the present invention so that clearer.But be not limited to following examples.
Embodiment 1: the device of coke-oven gas methyl alcohol processed
Fig. 1 shows the technical process of coke-oven gas methyl alcohol processed.
By reference to the accompanying drawings, technical process of the present invention is:
The thick coke-oven gas that coke oven 1 produces obtains clean coke-oven gas after purifying in unit 2 through dedusting, denitrogenation, washing benzene, desulfurizing and purifying operation, sends into gas holder 3; The waste gas that coke oven 1 burning produces is through CO 2water separator 4 is isolated CO 2the part coke-oven gas of exporting with gas holder 3 mixes sends into CO 2coke-oven gas reformer 5 carries out reforming reaction; Reaction formula is: CO 2+ CH 4=2CO+2H 2.
Be rich in CO+H 2synthetic gas after compressor 6 supercharging 5MPa, send into oil separator 7, mix with the unreacting gas returning, after gas preheater 9 preheatings, enter methyl alcohol synthesizer 8 tops and react.
The methanol vapor that building-up reactions generates and unreacting gas, from the 8 bottom outputs of methyl alcohol synthesizer, enter gas-liquid separator 11 after gas preheater 9, heat exchanger 10 heat exchange coolings, isolate thick methyl alcohol from gas-liquid separator 11 bottom outputs;
Unreacting gas is sent into gas buffer tank 13 from gas-liquid separator 11 tops outputs through recycle compressor 12 pressurizations, and part unreacting gas enters oil separator 7, and to loop methyl alcohol synthetic; The clean coke-oven gas of part that remaining unreacting gas is exported as fuel gas and gas holder 3 is mixed into coke oven 1 flue, burns with the oxygen of air trap 14, and be coking by coke oven heat supply.
Embodiment 2: the technique of coke-oven gas methyl alcohol processed
Specifically comprise the following steps:
(1) air is sent into air trap, the O of generation 2send in coke oven; Coking coal is sent into coke oven, obtain product coke and thick coke-oven gas;
(2) the thick coke-oven gas that coke oven produces obtains clean coke-oven gas through dedusting, denitrogenation, after washing benzene, desulfurizing and purifying operation, sends into gas holder;
(3) waste gas that coke oven combustion produces is through CO 2water separator is isolated 95% CO 2, mix and send into CO with 88% coke-oven gas of gas holder output 2coke-oven gas reformer, carries out reforming reaction (CO 2+ CH 4=2CO+2H 2);
(4) be rich in CO+H 2synthetic gas after compressor supercharging 5MPa, send into oil separator, the unreacting gas returning with circulation mixes and after gas preheater preheating, enters methyl alcohol synthesizer top and react.
(5) methanol vapor generating and unreacting gas are from the output of methyl alcohol synthesizer bottom, after preheater heat exchange, heat exchanger heat exchange cooling, enter gas-liquid separator separates and go out thick methyl alcohol and export from bottom, unreacting gas is sent into gas buffer tank from the output of gas-liquid separator top through recycle compressor pressurization;
(6) unreacting gas in gas buffer tank: wherein 65%(volume ratio) enter oil separator and reform after synthetic gas mix, then enter methyl alcohol synthesizer; Remaining 35% unreacting gas mixes with 12% clean coke-oven gas of gas holder output the flue that enters coke oven as fuel gas, and the oxygen coming with air trap carries out combustion heat supplying.
Take the coking enterprise of 5,000,000 tons of scale coke as example, implement according to above-mentioned operational path, can methanol 78.8 ten thousand tons, methyl alcohol CO per ton 2quantity discharged is 0.3 ton, mends carbon production process reduce discharging 64% CO with respect to gasification gas (water-gas) 2.
Embodiment 3: the technique of coke-oven gas methyl alcohol processed
Specifically comprise the following steps:
(1) air is sent into air trap, the O of generation 2send in coke oven; Coking coal is sent into coke oven, obtain product coke and thick coke-oven gas;
(2) the thick coke-oven gas that coke oven produces obtains clean coke-oven gas through dedusting, denitrogenation, after washing benzene, desulfurizing and purifying operation, sends into gas holder;
(3) waste gas that coke oven combustion produces is through CO 2water separator is isolated 99.5% CO 2, mix and send into CO with 68% coke-oven gas of gas holder output 2coke-oven gas reformer, carries out reforming reaction (CO 2+ CH 4=2CO+2H 2);
(4) be rich in CO+H 2synthetic gas after compressor supercharging 5MPa, send into oil separator, the unreacting gas returning with circulation mixes and after gas preheater preheating, enters methyl alcohol synthesizer top and react.
(5) methanol vapor generating and unreacting gas are from the output of methyl alcohol synthesizer bottom, after preheater heat exchange, heat exchanger heat exchange cooling, enter gas-liquid separator separates and go out thick methyl alcohol and export from bottom, unreacting gas is sent into gas buffer tank from the output of gas-liquid separator top through recycle compressor pressurization;
(6) unreacting gas in gas buffer tank: wherein 80%(volume ratio) enter oil separator and reform after synthetic gas mix, then enter methyl alcohol synthesizer; Remaining 20% unreacting gas mixes with 32% clean coke-oven gas of gas holder output the flue that enters coke oven as fuel gas, and the oxygen coming with air trap carries out combustion heat supplying.
Take the coking enterprise of 5,000,000 tons of scale coke as example, implement according to above-mentioned operational path, can methanol 1,080,000 tons, methyl alcohol CO per ton 2quantity discharged is 0.39 ton, mends carbon production process reduce discharging 56% CO with respect to gasification gas (water-gas) 2.
Embodiment 4: the technique of coke-oven gas methyl alcohol processed
Specifically comprise the following steps:
(1) air is sent into air trap, the O of generation 2send in coke oven; Coking coal is sent into coke oven, obtain product coke and thick coke-oven gas;
(2) the thick coke-oven gas that coke oven produces obtains clean coke-oven gas through dedusting, denitrogenation, after washing benzene, desulfurizing and purifying operation, sends into gas holder;
(3) waste gas that coke oven combustion produces is through CO 2water separator is isolated 99.5% CO 2, mix and send into CO with 59% coke-oven gas of gas holder output 2coke-oven gas reformer, carries out reforming reaction (CO 2+ CH 4=2CO+2H 2);
(4) be rich in CO+H 2synthetic gas after compressor supercharging 5MPa, send into oil separator, the unreacting gas returning with circulation mixes and after gas preheater preheating, enters methyl alcohol synthesizer top and react.
(5) methanol vapor generating and unreacting gas are from the output of methyl alcohol synthesizer bottom, after preheater heat exchange, heat exchanger heat exchange cooling, enter gas-liquid separator separates and go out thick methyl alcohol and export from bottom, unreacting gas is sent into gas buffer tank from the output of gas-liquid separator top through recycle compressor pressurization;
(6) unreacting gas in gas buffer tank: wherein 90%(volume ratio) enter oil separator and reform after synthetic gas mix, then enter methyl alcohol synthesizer; Remaining 10% unreacting gas mixes with 41% clean coke-oven gas of gas holder output the flue that enters coke oven as fuel gas, and the oxygen coming with air trap carries out combustion heat supplying.
Take the coking enterprise of 5,000,000 tons of scale coke as example, implement according to above-mentioned operational path, can methanol 680,000 tons, methyl alcohol CO per ton 2quantity discharged is 0.43 ton, mends carbon production process reduce discharging 52% CO with respect to gasification gas (water-gas) 2.
Above embodiment is only illustrated the specific embodiment of the present invention by reference to the accompanying drawings; concerning being engaged in those skilled in the art; can be according to above description scheme and design; make other various corresponding changes and distortion, and these all changes and distortion all should belong to the protection domain of the claims in the present invention within.

Claims (4)

1. a coke-oven gas methanol technics processed, is characterized in that: comprise the following steps:
I, air is sent into air trap, the O of generation 2send in coke oven; Coking coal is sent into coke oven, obtain product coke and thick coke-oven gas;
The thick coke-oven gas that II, coke oven produce obtains clean coke-oven gas through dedusting, denitrogenation, after washing benzene, desulfurizing and purifying operation, sends into gas holder;
The waste gas that III, coke oven combustion produce is through CO 2water separator is isolated CO 2, mix and send into CO with the clean coke-oven gas of part of gas holder output in step II 2coke-oven gas reformer; Another part coke-oven gas of gas holder output turns back to recycle in coke oven;
Synthetic gas after IV, reformation is sent into oil separator after compressor supercharging, enters methyl alcohol synthesizer top after preheater preheating, reacts;
The methanol vapor generating in V, methyl alcohol synthesizer and unreacting gas be from the bottom output of methyl alcohol synthesizer, enters gas-liquid separator separates and go out thick methyl alcohol and export from bottom after preheater heat exchange, heat exchanger heat exchange cooling;
VI, unreacting gas are sent into gas buffer tank from the output of gas-liquid separator top through recycle compressor pressurization;
Part unreacting gas in VII, gas buffer tank enters oil separator, and the synthetic gas after reforming with step III mixes, and then sends into methyl alcohol synthesizer; Another part unreacting gas in gas buffer tank turns back in coke oven as fuel gas utilization.
2. coke-oven gas according to claim 1 methanol technics processed, it is characterized in that: the coke-oven gas that the unreacting gas that described step VII is returned returns with step III mixes as fuel gas and enters coke oven vertical flame path, the oxygen coming with air trap burns, for coking provides heat.
3. coke-oven gas according to claim 1 and 2 methanol technics processed, is characterized in that: the described unreacting gas ratio of returning to coke oven combustion heat supply accounts for the 10%-70% of unreacting gas total amount.
4. coke-oven gas according to claim 1 methanol technics processed, is characterized in that: in described step III, gas holder is sent to CO 2the clean coke-oven gas ratio of coke-oven gas reformer accounts for the 50%-90% of coke-oven gas total amount.
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Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104341267A (en) * 2014-10-11 2015-02-11 神华集团有限责任公司 Method for preparing methanol from high-sulfur coal
CN105061142A (en) * 2015-07-31 2015-11-18 赛鼎工程有限公司 Technology for synthesizing low carbon alcohol and hydrogen as byproduct from coke oven gas
CN105111045A (en) * 2015-07-31 2015-12-02 赛鼎工程有限公司 Method for synthesizing lower alcohol by coke oven gas and secondarily producing natural gas and liquid ammonia
CN107973270A (en) * 2017-10-12 2018-05-01 东华工程科技股份有限公司 A kind of coke-stove gas mends carbon conversion preparing ethylene glycol synthesis gas process
CN109553508A (en) * 2019-01-17 2019-04-02 河北科技大学 A kind of device and method of the direct steam reformation production methanol of coal oven dithio-gas
CN113292394A (en) * 2021-06-15 2021-08-24 河海大学 Coke oven gas coupling waste incineration power generation system methyl alcohol system
CN113527052A (en) * 2021-06-17 2021-10-22 中石化宁波工程有限公司 Process for preparing methanol from methane

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Cited By (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104341267A (en) * 2014-10-11 2015-02-11 神华集团有限责任公司 Method for preparing methanol from high-sulfur coal
CN105061142A (en) * 2015-07-31 2015-11-18 赛鼎工程有限公司 Technology for synthesizing low carbon alcohol and hydrogen as byproduct from coke oven gas
CN105111045A (en) * 2015-07-31 2015-12-02 赛鼎工程有限公司 Method for synthesizing lower alcohol by coke oven gas and secondarily producing natural gas and liquid ammonia
CN105061142B (en) * 2015-07-31 2018-02-06 赛鼎工程有限公司 A kind of technique by coke-stove gas synthesis of low-carbon alcohol and by-product hydrogen
CN105111045B (en) * 2015-07-31 2018-07-03 赛鼎工程有限公司 By the method for coke-stove gas synthesis of low-carbon alcohol and by-product natural gas and liquefied ammonia
CN107973270A (en) * 2017-10-12 2018-05-01 东华工程科技股份有限公司 A kind of coke-stove gas mends carbon conversion preparing ethylene glycol synthesis gas process
CN109553508A (en) * 2019-01-17 2019-04-02 河北科技大学 A kind of device and method of the direct steam reformation production methanol of coal oven dithio-gas
CN109553508B (en) * 2019-01-17 2024-03-29 河北科技大学 Device and method for producing methanol by directly reforming raw coke oven gas with water vapor
CN113292394A (en) * 2021-06-15 2021-08-24 河海大学 Coke oven gas coupling waste incineration power generation system methyl alcohol system
CN113527052A (en) * 2021-06-17 2021-10-22 中石化宁波工程有限公司 Process for preparing methanol from methane
CN113527052B (en) * 2021-06-17 2024-03-22 中石化宁波工程有限公司 Methane-to-methanol process

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