CN104152201A - Coal syngas circulation gas free methanation technology - Google Patents

Coal syngas circulation gas free methanation technology Download PDF

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CN104152201A
CN104152201A CN201410413845.3A CN201410413845A CN104152201A CN 104152201 A CN104152201 A CN 104152201A CN 201410413845 A CN201410413845 A CN 201410413845A CN 104152201 A CN104152201 A CN 104152201A
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methanator
gas
methanation
divided
spleen
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CN201410413845.3A
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CN104152201B (en
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宋鹏飞
杨宽辉
姚辉超
刘玉成
侯建国
何洋
王秀林
冯雅晨
高振
李敬
穆祥宇
郑珩
张瑜
张新波
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中海石油气电集团有限责任公司
西南化工研究设计院有限公司
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Abstract

The invention belongs to the chemical engineering field, and specifically relates to a coal syngas circulation gas free methanation technology. The technology firstly divides a methanation reactor into two parts, the purified raw material gas is divided into a plurality of gas flows, then the gas flows is introduced into the front methanation reactor, wherein parts of the front methanation reactor are connected through a combination mode of serial connection and parallel connection; the gas in the each level of methanation reactors in the front part goes out from the outlet of the first reactor and the outlet is serially connected to other level methanation reactors, or the gas is divided into a plurality of gas flows and enters other level reactors which are connected through a combination mode of serial connection and parallel connection. The technology adopts water steam as the diluting gas for diluting the raw material gas in a methanation reactor, the water steam is mainly applied to the high temperature methanation reaction technology, the pressure of the by-product namely steam is larger than the methanation reaction pressure, and thus the steam can be directly added into the raw material gas in a methanation reactor. The technology does not need a circulation gas compressor, so the production cost is reduced. Because the methanation reaction is a strong heat dissipation reaction, the added water stream is reduced so as to improve the energy utilization rate.

Description

A kind of producing synthesis gas from coal is without the methanation process of circulation gas
Technical field
The invention belongs to chemical field, relate to the method for the methanation process that is rich in H2, CO and CO2 gas, be specially the methanation process of a kind of producing synthesis gas from coal without circulation gas.
Background technology
China's fossil energy is taking coal as Main Resources, and coal reserves are very abundant, and the explored reserves of possessing are up to more than 1.28 trillion tons at present.Oil, natural gas source are relatively poor, and domestic oil and gas production far can not meet the needs of national economy high speed development, must rely on a large amount of imports to support China's expanding economy.China's imported crude oil rises to 2.5 hundred million tons in 2011 by 0.7 hundred million tons in 2000, petroleum import interdependency is overseas reached to 55.2% in 2012.Within 2009, China's natural gas output is 830 × 10 8nm 3, increased by 7.7% compared with 2008.Apparent consumption amount is 874.5 × 10 8nm 3, increase by 11.5% on a year-on-year basis.Compared with output in domestic, domestic Sweet natural gas insufficiency of supply-demand reaches billion cubic meter more than 40.Within 2010, China's natural gas increases by 12.1% on a year-on-year basis, reaches 944.8 × 10 8nm 3.To exceed 2000 × 10 to the year two thousand twenty natural gas demand 8nm 3left and right, and output only has 1000 × 10 8nm 3, in addition 50% by dependence on import or other substitute energys.The Demand of Oil & Gas of cumulative year after year, will become the bottleneck that restricts China's Economic development.Therefore, make full use of the coal resources advantage of China's abundant, greatly develop Coal Chemical Industry new high-tech industry, produce coal preparing natural gas, for optimizing China's energy structure, ensure Chinese energy safety, ensure the Sustainable development of national economy, extremely urgent, imperative.Can to predict future be domestic or the demand of Sweet natural gas is all existed to very large breach abroad, therefore utilizes coal resources production synthetic natural gas that the Sweet natural gas that is a kind of reality is supplemented to source.
The methanation technology of existing coal to SNG or LNG is controlled temperature with the complex appts of multiple gas circulation machines and heat exchanger conventionally, and the circulation gas of employing, up to 5 times more than, has not only increased facility investment and also increased considerably circulation gas power consumption.Research and development are urgent without circulation gas, the real genus of more energy-conservation, lower-cost technique.
 
Summary of the invention
The object of the invention is to for above technical problem, provide and can greatly shorten heating-up time and recovery time, save a large amount of high pure nitrogens, make reduction process more flexible, it is easier to control, and is conducive to that methanation catalysts at different levels reduction is more balanced, a kind of coal preparing natural gas methanation catalyst two-part hyperthermic reduction thoroughly.
The object of the invention realizes by following technical proposals:
Producing synthesis gas from coal is without a methanation process for circulation gas, and first this technique be divided into two portions by methanator, then the unstripped gas after purifying is divided into some thighs and enters the fore portion methanator connecting with series-multiple connection array mode; First half methanators at different levels inside enters other grade of methanator from the first reactor outlet gas with series system or is divided into some thighs and enters other stage reactor connecting with series-multiple connection array mode; Subsequently working off one's feeling vent one's spleen of half fore portion methanator entered to latter half methanator with series system, or be divided into the some strands of latter half methanators that enter with the connection of series-multiple connection array mode; The unstripped gas water vapour that enters First methanator is diluted; Methanation gas after penultimate methanator is carried out cooling, condensation separation water, then enter last methanator, remaining CO and CO 2react away, then separate or liquefy, obtain SNG or LNG.
The described unstripped gas by after purifying is divided into N thigh, is preferably divided into 2 strands, 3 strands or 4 strands.
Described is divided into two portions by methanator, contains 3 or 4 methanators in first half, and latter half contains 3 or 4 methanators.
The unstripped gas water vapour that enters the first methanator is diluted, and water vapour consumption is to enter 20%~60% of the first methanator unstripped gas molar weight.
In this technique, be 260 DEG C~320 DEG C to entering the gas temperature of First methanator, after last methanator, gas cooling temperature is 40 DEG C~80 DEG C.
A kind of producing synthesis gas from coal is without the methanation process of circulation gas, as preferably, this technique specifically comprises the following steps: first methanator is divided into two portions, be first half and latter half, the methanator of first half is 4, i.e. the first methanator, the second methanator, front three alkylation reactors and tetramethyl alkylation reactors; Latter half comprises 3 methanation reactions, i.e. the 5th methanator, pregnancy alkylation reactors and the 7th methanator.Adopt gasification purified gas as unstripped gas, then unstripped gas is divided into four strands, after the first stock-traders' know-how heating, mix with overheated steam, temperature is 270 DEG C~320 DEG C, pressure is 2.0 MPa~4.0 MPa, then enters in the first methanator, carries out methanation reaction.Entering useless pot through the reacted gas of the first methanator carries out cooling, and byproduct steam, then the first methanator is worked off one's feeling vent one's spleen and is divided into two groups, wherein one group of first methanator worked off one's feeling vent one's spleen and is mixed in the second methanator and carries out methanation reaction with second strand of unstripped gas, and temperature is 260 DEG C~320 DEG C; The gas that goes out the second methanator enter useless pot carry out cooling, and byproduct steam; Another is organized the first methanator and works off one's feeling vent one's spleen and be mixed in front three alkylation reactors and carry out methanation reaction with the 3rd strand of unstripped gas and the second methanator three that works off one's feeling vent one's spleen, and temperature is 260 DEG C~320 DEG C; The gas of front three alkylation reactors enter useless pot carry out cooling, and byproduct steam.Front three alkanisation reactor outlet gas after heat exchange, with from after wherein one mixes of unstripped gas, 260 DEG C~320 DEG C of temperature, enter tetramethyl alkylation reactors, tetramethyl alkylation reactors is worked off one's feeling vent one's spleen after the heat exchange of useless pot through gas-liquid separation, enters the 5th methanator with 260 DEG C~320 DEG C.Now existing 90% above CO+CO 2react away.The 5th methanation is worked off one's feeling vent one's spleen and enter pregnancy alkylation reactors with 260 DEG C~320 DEG C after heat exchange, the gas that goes out pregnancy alkylation reactors carries out being cooled to 40 DEG C~80 DEG C after heat exchange again, in separator after Separation of Water, be heated to 260 DEG C and enter the 7th methanator, further by remaining CO and CO 2react away.
Compared with prior art, beneficial effect of the present invention is:
(1), the present invention adopts water vapour as the carrier gas that enters methanator unstripped gas, and the gas after methanation returns as carrier gas, mainly for high-temperature methanation reaction process, because the pressure of byproduct steam in methanation reaction process is greater than methanation reaction pressure, can directly join in the unstripped gas of methanator.Water vapour as carrier gas advantage is: one, save recycle gas compressor, and save investment, reduce power consumption; Its two, in unstripped gas, contain C 2above hydro carbons, for high-temperature methanation reaction, adds water vapour can suppress coking reaction, has protected catalyzer.
(2), this technique do not need recycle gas compressor, saved production cost.
(3), because methanation reaction is strong exothermal reaction, in order to improve capacity usage ratio, add steam vapour amount to lack as far as possible.The present invention takes a unstripped gas point multiply to enter methanator, only in the unstripped gas that enters the first methanation main reactor, adds water vapour, makes like this steam consumption relatively greatly reduce, and has improved the capacity usage ratio of methanation process.
 
Brief description of the drawings
Fig. 1 is the process flow diagram of embodiment 1 in the present invention.
Fig. 2 is the process flow diagram of embodiment 2 in the present invention.
Fig. 3 is the process flow diagram of embodiment 3 in the present invention.
Embodiment
Disclosed arbitrary feature in this specification sheets (comprising any accessory claim, summary), unless narration especially all can be replaced by other equivalences or the alternative features with similar object.,, unless narration especially, each feature is an example in a series of equivalences or similar characteristics.
Embodiment 1:
This process flow diagram is shown in Fig. 1, as shown in Figure 1, and pressure 3.5MPa, 100000Nm 3in the synthetic gas of/h and synthetic gas, total sulfur is less than 0.1ppm, f=(n h2-n cO2)/(n cO+ n cO2)=3.005, the composition (percent by volume, wet basis) of concrete synthetic gas is: H 2: 64.00, CH 4: 14.30, CO:20.10, CO 2: 0.90, N 2: 0.50, H 2o:0.30.Unstripped gas is divided into four stocks according to 0.22,0.15,0.25,0.38 and does not enter first, second, third, fourth methanator, the first stock-traders' know-how heats afterwards and overheated steam mixing temperature is 300 DEG C, then enter in the first methanator, carry out methanation reaction.Be 630 DEG C of temperature through the reacted gas of the first methanator, then entering useless pot carries out cooling, and byproduct steam, then the first methanator is worked off one's feeling vent one's spleen and is 7:3 according to volume ratio again ratio divides two groups to enter respectively second, third methanator, wherein one group of first methanator enters after working off one's feeling vent one's spleen and mixing with second strand of unstripped gas and in the second methanator, carries out methanation reaction, temperature is 300 DEG C, the temperature of the gas of the second methanator be 630 DEG C enter useless pot carry out cooling, and byproduct steam; Another group is worked off one's feeling vent one's spleen to work off one's feeling vent one's spleen to enter after three mixes with the 3rd strand of unstripped gas and the second methanator from the first methanator and in front three alkylation reactors, is carried out methanation reaction, temperature is 300 DEG C, the temperature of the gas of front three alkylation reactors is 630 DEG C, enter useless pot carry out cooling, and byproduct steam.The 4th strand of unstripped gas and front three alkanisation reactor outlet gas mix, after enter in tetramethyl alkylation reactors and carry out methanation reaction, mixing temperature is 300 DEG C; The temperature that tetramethyl alkylation reactors is worked off one's feeling vent one's spleen is 630 DEG C, and after useless pot and material-heat-exchanging, temperature is 150 DEG C, enters gas-liquid separator, after separation, is 300 DEG C and enters the 5th methanator again through being heated to temperature.Now existing 90% above CO+CO 2react.The 5th methanation temperature of working off one's feeling vent one's spleen is 530 DEG C, after heat exchange, enter pregnancy alkanisation main reactor with 300 DEG C, the gas temperature that goes out pregnancy alkylation reactors is 395 DEG C, carry out being cooled to again 40 DEG C~80 DEG C after heat exchange, in separator after Separation of Water, being heated to 260 DEG C of temperature that enter the 7th methanator is 320 DEG C, further by remaining CO and CO 2react away.
embodiment 2:
The present embodiment carries out according to technical process shown in Fig. 2, pressure 3.5MPa, 100000Nm 3in the synthetic gas of/h and synthetic gas, total sulfur is less than 0.1ppm, f=(n h2-n cO2)/(n cO+ n cO2)=3.005, the composition (volume fraction, wet basis) of concrete synthetic gas is: H 2: 64.00, CH 4: 14.30, CO:20.10, CO 2: 0.90, N 2: 0.50, H 2o:0.30.Unstripped gas is divided into three stocks according to 0.32,0.21,0.47 and does not enter first, second, third methanator, after the first stock-traders' know-how heating, mixes (260 DEG C of temperature) with overheated steam, then enters in the first methanator, carries out methanation reaction.Entering useless pot through the reacted gas of the first methanator (650 DEG C of temperature) carries out cooling, and byproduct steam, then the first methanator is worked off one's feeling vent one's spleen and is divided two stocks not enter second, third methanator according to 0.6,0.4 ratio again, wherein one first methanator enters in the second methanator after working off one's feeling vent one's spleen and mixing (260 DEG C of temperature) with second strand of unstripped gas, carry out methanation reaction, the gas (650 DEG C of temperature) of the second methanator enter useless pot carry out cooling, and byproduct steam; Another strand first methanator is worked off one's feeling vent one's spleen and is mixed with the 3rd strand of unstripped gas and the second methanator three that works off one's feeling vent one's spleen, 260 DEG C of temperature, enter in front three alkylation reactors, carry out methanation reaction, the gas (650 DEG C of temperature) of front three alkylation reactors enter useless pot carry out cooling, and byproduct steam.300 DEG C, front three alkanisation reactor outlet gas after heat exchange is divided into two stocks according to 0.4,0.6 ratio again and does not enter the 4th, the 5th methanator.Tetramethyl alkylation reactors is worked off one's feeling vent one's spleen after (510 DEG C of temperature) mixes from front three alkanisation reactor outlet gas with one after the heat exchange of useless pot and is entered the 5th methanator.Now existing 90% above CO+CO 2react.The 5th methanation work off one's feeling vent one's spleen (465 DEG C of temperature) after heat exchange, enter pregnancy alkanisation main reactor with 300 DEG C, the gas (359 DEG C of temperature) that goes out pregnancy alkanisation main reactor carries out being cooled to 40 DEG C~80 DEG C after heat exchange again, in separator after Separation of Water, be heated to 260 DEG C and enter the 7th methanator (320 DEG C of temperature), further by remaining CO and CO 2react away.
embodiment 3:
The present embodiment is according to technical process shown in Fig. 3, pressure 3.5MPa, 100000Nm 3in the synthetic gas of/h and synthetic gas, total sulfur is less than 0.1ppm, f=(n h2-n cO2)/(n cO+ n cO2)=3.005, the composition (volume fraction, wet basis) of concrete synthetic gas is: H 2: 64.00, CH 4: 14.30, CO:20.10, CO 2: 0.90, N 2: 0.50, H 2o:0.30.Unstripped gas is divided into three stocks according to 0.32,0.21,0.47 and does not enter first, second, third methanator, after the first stock-traders' know-how heating, mixes (260 DEG C of temperature) with overheated steam, then enters in the first methanator, carries out methanation reaction.Entering useless pot through the reacted gas of the first methanator (650 DEG C of temperature) carries out cooling, and byproduct steam, then the first methanator is worked off one's feeling vent one's spleen and is divided two stocks not enter second, third methanator according to 0.6,0.4 ratio again, wherein one first methanator enters in the second methanator after working off one's feeling vent one's spleen and mixing (260 DEG C of temperature) with second strand of unstripped gas, carry out methanation reaction, the gas (650 DEG C of temperature) of the second methanator enter useless pot carry out cooling, and byproduct steam; Another strand first methanator is worked off one's feeling vent one's spleen and is mixed with the 3rd strand of unstripped gas and the second methanator three that works off one's feeling vent one's spleen, 260 DEG C of temperature, enter in front three alkylation reactors, carry out methanation reaction, the gas (650 DEG C of temperature) of front three alkylation reactors enter useless pot carry out cooling, and byproduct steam.300 DEG C, front three alkanisation reactor outlet gas after heat exchange enters tetramethyl alkylation reactors.Tetramethyl alkylation reactors work off one's feeling vent one's spleen (520 DEG C of temperature) after the heat exchange of useless pot, enter the 5th methanator to 300 DEG C.Now existing 90% above CO+CO2 reacts.The 5th methanation work off one's feeling vent one's spleen (470 DEG C of temperature) after heat exchange, enter pregnancy alkanisation main reactor with 300 DEG C, the gas (365 DEG C of temperature) that goes out pregnancy alkanisation main reactor carries out being cooled to 40 DEG C~80 DEG C after heat exchange again, in separator after Separation of Water, be heated to 260 DEG C and enter the 7th methanator (310 DEG C of temperature), further by remaining CO and CO 2react away.

Claims (8)

1. producing synthesis gas from coal, without a methanation process for circulation gas, is characterized in that: first methanator is divided into two portions, then the unstripped gas after purifying is divided into some thighs and enters the fore portion methanator connecting with series-multiple connection array mode; First half methanators at different levels inside enters other grade of methanator from the first reactor outlet gas with series system or is divided into some thighs and enters other stage reactor connecting with series-multiple connection array mode; Subsequently working off one's feeling vent one's spleen of half fore portion methanator entered to latter half methanator with series system, or be divided into the some strands of latter half methanators that enter with the connection of series-multiple connection array mode; The unstripped gas water vapour that enters First methanator is diluted; Methanation gas after penultimate methanator is carried out cooling, condensation separation water, then enter last methanator, remaining CO and CO 2react away, then separate or liquefy, obtain SNG or LNG.
2. producing synthesis gas from coal according to claim 1, without the methanation process of circulation gas, is characterized in that: the described unstripped gas by after purifying is divided into some strands, is divided into 2 strands, 3 strands or 4 strands.
3. producing synthesis gas from coal according to claim 1 is without the methanation process of circulation gas, it is characterized in that: the unstripped gas water vapour that enters the first methanator is diluted, and water vapour consumption is to enter 20%~60% of the first methanator unstripped gas molar weight.
4. producing synthesis gas from coal according to claim 1, without the methanation process of circulation gas, is characterized in that: the gas temperature that enters First methanator is 260 DEG C~320 DEG C, and after last methanator, gas cooling temperature is 40 DEG C~80 DEG C.
5. a producing synthesis gas from coal is without the methanation process of circulation gas, it is characterized in that: this technique specifically comprises the following steps: first methanator is divided into two portions, be first half and latter half, the methanator of first half is 4, i.e. the first methanator, the second methanator, front three alkylation reactors and tetramethyl alkylation reactors; Latter half comprises 3 methanation reactions, i.e. the 5th methanator, pregnancy alkylation reactors and the 7th methanator; Adopt gasification purified gas as unstripped gas, then unstripped gas is divided into four strands, after the first stock-traders' know-how heating, mix with overheated steam, temperature is 270 DEG C~320 DEG C, pressure is 2.0 MPa~4.0 MPa, then enters in the first methanator, carries out methanation reaction; Entering useless pot through the reacted gas of the first methanator carries out cooling, and byproduct steam, then the first methanator is worked off one's feeling vent one's spleen and is divided into two groups, wherein one group of first methanator worked off one's feeling vent one's spleen and is mixed in the second methanator and carries out methanation reaction with second strand of unstripped gas, and temperature is 260 DEG C~320 DEG C; The gas that goes out the second methanator enter useless pot carry out cooling, and byproduct steam; Another is organized the first methanator and works off one's feeling vent one's spleen and be mixed in front three alkylation reactors and carry out methanation reaction with the 3rd strand of unstripped gas and the second methanator three that works off one's feeling vent one's spleen, and temperature is 260 DEG C~320 DEG C; The gas of front three alkylation reactors enter useless pot carry out cooling, and byproduct steam; Front three alkanisation reactor outlet gas after heat exchange, with from after wherein one mixes of unstripped gas, 260 DEG C~320 DEG C of temperature, enter tetramethyl alkylation reactors, tetramethyl alkylation reactors is worked off one's feeling vent one's spleen after the heat exchange of useless pot through gas-liquid separation, enters the 5th methanator with 260 DEG C~320 DEG C; Now existing 90% above CO+CO 2react away; The 5th methanation is worked off one's feeling vent one's spleen and enter pregnancy alkylation reactors with 260 DEG C~320 DEG C after heat exchange, the gas that goes out pregnancy alkylation reactors carries out being cooled to 40 DEG C~80 DEG C after heat exchange again, in separator after Separation of Water, be heated to 260 DEG C and enter the 7th methanator, further by remaining CO and CO 2react away.
6. the methanation process without circulation gas according to claim 1 or producing synthesis gas from coal claimed in claim 5, it is characterized in that: described is divided into two portions by methanator, in first half, contain 3 or 4 methanators, latter half contains 3 or 4 methanators.
According to claim 1 or producing synthesis gas from coal claimed in claim 5 without the methanation process of circulation gas, it is characterized in that: in described first half methanator, working off one's feeling vent one's spleen of last methanator directly enters in the First methanator in latter half methanator.
8. the methanation process without circulation gas according to claim 1 or producing synthesis gas from coal claimed in claim 5, it is characterized in that: in described first half methanator, working off one's feeling vent one's spleen of last methanator is divided into two groups, in the First methanator that first group directly enters in latter half methanator, other one group of gas enters second methanator in latter half methanator after mixing with working off one's feeling vent one's spleen of First methanator in latter half methanator.
CN201410413845.3A 2014-08-21 2014-08-21 Coal syngas circulation gas free methanation technology CN104152201B (en)

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CN105296035A (en) * 2015-11-27 2016-02-03 中国海洋石油总公司 Hydrogen supplying methanation method for preparing synthetic natural gas
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CN106190382A (en) * 2016-07-16 2016-12-07 中国科学院山西煤炭化学研究所 The technique that producing synthesis gas from coal carries out methanation synthesis substitute natural gas
CN106118773B (en) * 2016-07-16 2019-04-02 中国科学院山西煤炭化学研究所 A kind of synthesis gas methanation process that hydrogen converts completely
CN106190382B (en) * 2016-07-16 2019-08-06 中国科学院山西煤炭化学研究所 Producing synthesis gas from coal carries out the technique that methane is combined to substitute natural gas
CN109593580A (en) * 2018-12-21 2019-04-09 惠生工程(中国)有限公司 A kind of semi-coke furnace tail gas fine de-sulfur and adiabatic methanation process
CN109593580B (en) * 2018-12-21 2021-02-05 惠生工程(中国)有限公司 Semi-coke furnace tail gas fine desulfurization and adiabatic methanation process
CN110938481A (en) * 2019-11-26 2020-03-31 浙江天禄环境科技有限公司 LNG preparation process for quality-divided utilization of low-rank coal

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