CN101597527A - A kind of method of utilizing coke(oven)gas to produce synthetic natural gas - Google Patents

A kind of method of utilizing coke(oven)gas to produce synthetic natural gas Download PDF

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CN101597527A
CN101597527A CN 200910074849 CN200910074849A CN101597527A CN 101597527 A CN101597527 A CN 101597527A CN 200910074849 CN200910074849 CN 200910074849 CN 200910074849 A CN200910074849 A CN 200910074849A CN 101597527 A CN101597527 A CN 101597527A
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gas
oven
coke
natural gas
synthetic natural
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CN 200910074849
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CN101597527B (en
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谢克昌
苗茂谦
张文效
乔海星
赵炜
上官炬
王殿忠
白玉祥
张永发
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Shanxi Keling Environment Engineering Design Technology Co., Ltd.
Taiyuan University of Technology
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SHANXI KELING ENVIRONMENT ENGINEERING DESIGN TECHNOLOGY Co Ltd
Taiyuan University of Technology
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Abstract

A kind of method of utilizing coke(oven)gas to produce synthetic natural gas is to mend carbon source in the coke(oven)gas after thick desulfurization, makes coke(oven)gas gas volume per-cent satisfy (H 2-3CO)/CO 2The stoichiometric ratio of ≈ 4, compression boosts to 0.5～5.4MPa, and smart desulfurization enters methanator, carries out methanation reaction under the effect of Ni series catalysts, obtains artificial Sweet natural gas, and then prepares natural gas liquids.The present invention optimizes H in the coke(oven)gas by mend carbon in coke(oven)gas 2, CO, CO 2Stoichiometric ratio, improved the productive rate of synthetic natural gas.The synthetic natural gas technology of producing of the present invention is suitable for making the H in the coke(oven)gas with tens supporting to the coke-oven plant of hundreds of ton 2, CO, CO 2And the CO that replenishes 2Be fully used, have realistic meaning for improving resource utilization and strengthen environmental protection.

Description

A kind of method of utilizing coke(oven)gas to produce synthetic natural gas
Technical field
The present invention relates to a kind of preparation method of synthetic natural gas, be specifically related to a kind of method of utilizing coke(oven)gas to produce synthetic natural gas.
Background technology
China is a coke production big country, and about 300,000,000 tons/year of throughput effluxes about 60,000,000,000 Nm of coke(oven)gas 3/ year.Coke(oven)gas wherein directly enters in the torch greatly and fires except as domestic fuel, generating, the synthesizing methanol, has both wasted resource, has polluted environment again.Components such as the benzene that contains in the coke(oven)gas, naphthalene, tar are partially recycled at the change product, and all the other components are H 254～59%, CH 424～28%, N 23～6%, CO 21.4～2.5%, CO 5～8%, O 20.3～0.7%, also have a spot of impurity sulfide.Its resource characteristic is CH 4Content is about 1/4, H 2Content nearly 60%.
Along with the enforcement of policies such as the domestic strategy of sustainable development and reinforcement environmental protection, domestic demand to Sweet natural gas grows with each passing day, and estimates that the demand of China's natural gas in 2010 will reach 1000～110,000,000,000 m 3, and the output of the same period can only reach 900～95,000,000,000 m 3The demand of the year two thousand twenty China's natural gas will reach 2,000 hundred million m 3, the same period, output can only reach 1400～1,600 hundred million m 3Therefore, in order to solve the problem of China's natural gas disparities between supply and demand, except the domestic existing resource of abundance, also must be by all kinds of means, multimode ground enlarges resource provision, synthetic natural gas is exactly one of effective channel.
Recent years, domestic had many patents to make the method that relevant elaboration: CN1935956A, CN1952082A, CN1952083A, CN1952084A and US4318997 etc. all disclose the artificial Sweet natural gas of usefulness coke(oven)gas multistage catalytic production of methane prepared in reaction about the technology by synthetic artificial Sweet natural gas (SNG) of coke(oven)gas and natural gas liquids (LNG), its significant disadvantage is owing to the carbon source deficiency, the H in the coke(oven)gas 2Be not fully used.
CN101100622A discloses a kind of carbon of mending in coke(oven)gas, utilize the method for reaction of multistage catalytic production of methane and PSA isolation technique production synthetic natural gas.Though this method has made full use of the H in the coke(oven)gas 2Resource, but also exist long flow path, big, the CH of investment 4The shortcoming low with the heat energy recycle rate.
Summary of the invention
The purpose of this invention is to provide a kind of method of utilizing coke(oven)gas to produce synthetic natural gas, this method is optimized H in the coke(oven)gas by mend carbon in coke(oven)gas 2, CO, CO 2Stoichiometric ratio, to improve the productive rate of synthetic natural gas.
The objective of the invention is to be achieved through the following technical solutions:
A kind of method of utilizing coke(oven)gas to produce synthetic natural gas may further comprise the steps:
A). coke(oven)gas is removed most inorganic sulfurs and part organosulfur through thick desulfurization;
B). mend carbon source in the coke(oven)gas after thick desulfurization, make the volume percent of gas in the coke(oven)gas satisfy (H 2-3CO)/CO 2The stoichiometric ratio of ≈ 4 boosts to 0.5～5.4MPa with the gas mixture compression;
C). the smart desulfurization of the gas mixture after the compression makes total sulfur≤0.1ppm wherein;
D). the gas mixture after the purification enters methanator, carries out methanation reaction under the effect of Ni series catalysts, obtains the artificial Sweet natural gas of lighter hydrocarbons content 80～95%;
E). the artificial Sweet natural gas that will make carries out depth decarburization and deep dehydration;
F). the artificial natural gas via low temperature separation process after the removal of impurities, prepare natural gas liquids, its calorific value is about 8500Kcal/Nm 3(35530KJ/Nm 3).
Supplementary carbon source described in the present invention can be CO 2, CO, water-gas or their mixture.These supplementary carbon sources can be supplied with by the decarbonization process waste gas of fertilizer plant or Methanol Plant, also can be supplied with by the desulfurization process waste gas of fertilizer plant or Methanol Plant, can also reclaim from the flue gas that boiler is discharged.
Thick desulfurization among the present invention and smart desulfurizing and purifying technology can be with reference to the methods in the present coke(oven)gas system methanol technics.The wet oxidation process desulfurization is adopted in thick desulfurization, through H in the coke(oven)gas of this operation 2S≤20mg/Nm 3, the organic sulfur removal rate is not less than 50%.Dry desulfurization is adopted in smart desulfurization, makes total sulfur≤0.1ppm wherein, and other impurity satisfy the methanation requirement.
Methanation reaction of the present invention adopts water-cooled tubulation methanator, and water passes through from the tube side of reactor, and the Ni series catalysts is with Al 2O 3Be carrier, be contained in the shell side of reactor that reaction gas passes through from shell side.Reaction pressure 0.5～the 5.4MPa of methanation reaction, 250～400 ℃ of temperature.The reaction heat that reaction is emitted is heated into mesohigh steam with water coolant, can reclaim the power as compressor.
The present invention also is equipped with water pump on the water inlet pipe before water inlet cold type tubulation methanator, can accelerate the velocity of flow of water, and the temperature of reaction of control catalyst bed prevents catalyst overheating.
Depth decarburization of the present invention adopts the MDEA method, and deep dehydration adopts sieve method, impurity CO in the artificial Sweet natural gas after this two step, operation was handled 2≤ 100ppm, H 2O≤0.1ppm, total sulfur≤0.1ppm.Simultaneously, the CO that tells by the depth decarburization operation 2Gas returns as benefit carbon carbon source and recycles, and the regeneration tail gas of deep dehydration operation is provided as fuel gas outward.
The present invention utilizes the method for low temperature separation process with the N in the artificial Sweet natural gas 2Remove, to produce the energy and industrial chemicals---the natural gas liquids of high-quality cleaning, simultaneously, coke-oven gas methanation reaction and low temperature separation process among the present invention are all finished under same pressure rating, the methanation operation is not established circulation loop, once by H in the reactor behind the methanator 2≤ 1%, CO 2≤ 1%, CO can not survey, and can reach technic index.
Coke(oven)gas of the present invention is produced synthetic natural gas technology and is suitable for making the H in the coke(oven)gas with tens supporting to the coke-oven plant of hundreds of ton 2, CO, CO 2And the CO that replenishes 2Be fully used, have realistic meaning for improving resource utilization and strengthen environmental protection.
The synthetic natural gas technology of producing coke(oven)gas of the present invention has effectively utilized the CO that produces Greenhouse effect 2Waste gas makes the H in the coke(oven)gas 2, CO, CO 2Obtain sufficient chemical reaction, methane recovery is bordering on 98%, and the heat energy that reaction produces can be produced the higher-grade steam of 4.0～10.0MPa, as the power of compressor.Therefore, the present invention has objectively reduced CO 2Discharging has rationally utilized resource, is a reduction of discharging, energy-conservation, the energy project of making rational use of resources.
Coke(oven)gas of the present invention is produced synthetic natural gas technology is finished the methanation reaction and the Sweet natural gas of coke(oven)gas under same pressure rating low temperature separation process, circulation loop is not established in methanation, once by making lighter hydrocarbons content behind the methanation reaction greater than 90% artificial Sweet natural gas, the CO that deviates from 2Can recycle, regeneration tail gas can be used as fuel gas, with the PSA separating technology relatively, the CH of low temperature separation process 4Rate of recovery height, the present invention's technical process on the whole is short, reduced investment.
Coke(oven)gas of the present invention is produced synthetic natural gas process using water-cooled tubulation methanator, and is provided with water pump on water inlet pipe, can accelerate the velocity of flow of water, guarantees not overtemperature of beds; Also in technology, be provided with thick desulfurization and smart desulfurization process, guarantee the total sulfur≤0.1ppm of unstripped gas.The use of these two measures can make prolong the work-ing life of catalyzer, methanation conversion yield height, and production cost is low.
Embodiment
Below provide a specific examples that utilizes coke(oven)gas to produce synthetic natural gas, the process gases balance sheet sees Table 1 in this example.
Table 1 coke(oven)gas is produced synthetic natural gas gaseous equilibrium table
Component 1 2 3 4 5 6 7 8 9 10
CO，％ 7.50 7.10 7.10 0 0 0 0 0
H 2，％ 57.50 54.42 5442 1.23 1.23 0 1.93 14.09
CO 2，％ 2.80 100.00 100.00 8.00 8.00 0.20 0 0 0 0
CH 4，％ 24.50 23.19 23.19 83.64 83.81 91.60 0 14.32
O 2，％ 6.50 0.47 0.47 0 0 0 0 0
N 2，％ 4.60 4.35 4.35 9.53 9.55 2.47 96.90 70.65
Ar，％ 0.40 0.38 0.38 083 0.83 0.87 1.17 0.94
C 2H 6，％ 1.87 1.77 1.77 388 3.89 4.29 0 0
C 3H 8，％ 0.22 0.21 0.21 0.46 0.46 0.51 0 0
C 4H 10，％ 0.11 0.11 011 0.23 0.23 0.26 0 0
H 2S 5.6g/Nm 3 20mg/Nm 3 ≤0.1ppm
Organosulfur 6000mg/Nm 3 3000mg/Nm 3
∑，Nm 3/h 23500 1305.33 22.67 24828 24828 1137 11314.33 10189.02 148.73 976.19
P，MPa 5.35 5.10 5.05
T，℃ 40 40 40 40 40 40
Coke-oven plant's product reclaims the coke(oven)gas of sending here, and gas composition sees Table component 1 in 1, after the thick desulfurization of wet oxidation process, with the CO that accounts for coke(oven)gas volume 5.65% 2Gas (comprises the CO that external decarburization waste gas (component 2) and depth decarburization operation produce 2Gas (component 3)) mix, the composition of gas mixture sees Table component 4 in 1, and the stoichiometric ratio of main ingredient satisfies (H 2-3CO)/CO 2=4.14, H 2S is by 5.6g/Nm 3Reduce to 20mg/Nm 3, organosulfur is by 600mg/Nm 3Reduce to 300mg/Nm 3After the compression of the compressed machine of gas mixture, boost to 5.35MPa, adopt dry method to carry out smart desulfurization, obtain the reaction gas of total sulfur≤0.1ppm shown in the component 5 in the table 1, enter in the water-cooled tubulation methanator, under 300～400 ℃ of temperature be carried on Al 2O 3Ni catalyzer contact on the carrier, at this, H 2, CO, CO 2Because methanation reaction is finished in the effect of Ni catalyzer.The reaction heat that produces in the methanation reaction process is taken away by the mobile water coolant, produces mesohigh steam, guarantees not overtemperature of beds, and mesohigh steam returns the power as compressor.The gas composition that goes out the methanation operation sees Table component 6 in 1, and wherein lighter hydrocarbons content 88.21%, H 2Content 1.23%, CO 2Content 0.20%, CO contain measurement and do not go out, and obtain artificial Sweet natural gas.After artificial Sweet natural gas adopts the MDEA method to carry out depth decarburization, by component 7 visible CO 2Contain measurement and do not go out, the CO that deviates from 2Return as mending carbon gas and recycle.Then more artificial Sweet natural gas is carried out deep dehydration by molecular sieve, remove H 2Be sent to ice chest behind the impurity such as O, the outer fuel gas that is provided as of the regeneration tail gas (component 10 in the table 1) that dehydration produces.Feed the artificial Sweet natural gas process low temperature separation process in the ice chest, tell N 2After (component 9 in the table 1) emptying, make natural gas liquids (component 8 in the table 1) as high-quality clean energy or industrial chemicals.
In addition, the artificial Sweet natural gas of the intermediates of present embodiment (component 6) directly can also be made the fine compressed natural gas used as vehicle fuel.

Claims (10)

1, a kind of method of utilizing coke(oven)gas to produce synthetic natural gas may further comprise the steps:
A). coke(oven)gas is removed most inorganic sulfurs and part organosulfur through thick desulfurization;
B). mend carbon source in the coke(oven)gas after thick desulfurization, make the volume percent of gas in the coke(oven)gas satisfy (H 2-3CO)/CO 2The stoichiometric ratio of ≈ 4 boosts to 0.5～5.4MPa with the gas mixture compression;
C). the smart desulfurization of the gas mixture after the compression makes total sulfur≤0.1ppm wherein;
D). the gas mixture after the purification enters methanator, carries out methanation reaction under the effect of Ni series catalysts, obtains the artificial Sweet natural gas of lighter hydrocarbons content 80～95%;
E). the artificial Sweet natural gas that will make carries out depth decarburization and deep dehydration;
F). the artificial natural gas via low temperature separation process after the removal of impurities prepares natural gas liquids.
2, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 1 is characterized in that described additional carbon source is CO 2, CO, water-gas or their mixture.
3, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 1 and 2 is characterized in that described carbon source from fertilizer plant or Methanol Plant decarbonization process waste gas, perhaps from fertilizer plant or Methanol Plant desulfurization process waste gas.
4, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 1 and 2 is characterized in that described carbon source is from the boiler smoke that reclaims.
5, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 1 is characterized in that the desulfurization of described thick desulfurization employing wet oxidation process, and dry desulfurization is adopted in smart desulfurization.
6, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 1, it is characterized in that described methanation reaction carries out in water-cooled tubulation methanator, water passes through from tube side, and catalyzer is contained in the shell side, and reaction gas passes through from shell side.
7,, it is characterized in that the reaction pressure 0.5～5.4MPa of described methanation reaction, 250～400 ℃ of temperature according to claim 1 or the 6 described methods of utilizing coke(oven)gas to produce synthetic natural gas.
8, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 6 is characterized in that being equipped with on the water inlet pipe before water-cooled tubulation methanator the water pump that helps to accelerate water flow velocity.
9, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 1 is characterized in that described depth decarburization adopts the MDEA method, and deep dehydration adopts sieve method.
10, the method for utilizing coke(oven)gas to produce synthetic natural gas according to claim 1 is characterized in that the CO that is told by the depth decarburization operation 2Gas returns as benefit carbon carbon source and recycles.
CN 200910074849 2009-07-07 2009-07-07 Method for making synthetic natural gas by utilizing coke oven gas Expired - Fee Related CN101597527B (en)

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CN101775319A (en) * 2010-02-11 2010-07-14 山西科灵环境工程设计技术有限公司 Method for producing synthetic natural gas SNG from coal and processing installation thereof
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