CN102911756A - Technology for producing methane through low-rank coal - Google Patents
Technology for producing methane through low-rank coal Download PDFInfo
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Abstract
A technology for producing methane through low-rank coal is that the low-rank coal is pyrolyzed so as to obtain pyro-char and pyrolysis gas which contains tar. The pyrolysis gas which contains the tar is cooled and separated so as to obtain the tar, water and the pyrolysis gas; the pyro-char is fed into a methanator, the easily reactive pyro-char is reacted with circulated hydrogen at a high temperature and a high pressure so as to obtain methanation gas, and the difficult reactive pyro-char is fed into a gasification reactor to be reacted with water vapor and oxygen, so that gasification gas is produced. The methanation gas and the gasification gas are used as heat sources to directly supply heat for the pyrolytic reaction of feed coal in a pyrolysis reactor. The pyrolysis gas and the gasification gas are separated or mixed to be converted, decarbonized and separated, so that hydrogen-rich gas is obtained, and the pyrolysis gas and the methanation gas are subjected to heat exchange, purified and separated to obtain the hydrogen-rich gas, so that hydrogen sources are provided for a methanation unit. The substitute natural gas which is produced by the technology has the advantages of high thermal efficiency, low hydrogen consumption, quick methanation reaction speed and the like.
Description
Technical field
The present invention relates to a kind of technique of low order preparing methane from coal, particularly a kind of low-rank coal of utilizing is respectively through the technique of the low order preparing methane from coal of super-dry, pyrolysis, pyrolysis char methanation, the gasification of methanation residue.
Technical background
The Natural Gas Demand of China is the trend that escalates, and the supply breach strengthens day by day.China's natural gas demand average growth rate per annum will reach 15% before estimating the year two thousand thirty, and the China's natural gas demand will reach 4000-5000 hundred million m3 when the time comes, wherein approximately 50% want dependence on import.The natural gas supply deficiency will directly affect China's economic construction and social development.China's low-rank coal resource is relatively abundant, and the coal preparing natural gas is the important channel that coal resources transform, and also is the powerful measure that realizes that Sweet natural gas replenishes.
Existing document CN102344841A discloses a kind of " a kind of method of utilizing coal based synthetic gas to prepare substitute natural gas ", the method existing with coal based synthetic gas by desulfurization, conversion after, carry out the two-stage methanation reaction, hydrogen in the coal based synthetic gas and carbon monoxide, carbon dioxide reaction generate methane, obtain the Sweet natural gas of methane percent by volume more than 94% by condensation separation.Wherein first step methanator gas inlet temperature is 200-350 ℃, reactor pressure is 2-5MPa, methanator gas inlet, second stage temperature is 300-360 ℃, reactor pressure is than the low 0.08-0.18MPa of first step methanator internal pressure, and catalyzer is selected nickel catalyst.The method is indirect methanation process, and need to carry out the two-stage methanation reaction, and technical process is long; The principle of this technique is:
CO+3H
2→CH
4+H
2O （Ⅰ） CO
2+4H
2→CH
4+2H
2O （Ⅱ）
Can be found out by (I): generate the methane of a part, have the hydrogen of a part to be wasted because generate water, can find out the methane that generates a part by (II), bimolecular hydrogen is arranged be wasted because generate water, cause system's hydrogen consumption high; This process heat is not coupled in addition, causes energy dissipation.
Existing document CN102061182A discloses a kind of " method of coal hydrogenation pyrolysis and gasification coupling ", and the technical process of the method is: the feed coal with granularity≤2mm carries out drying and preheating first, dry rear total water≤8%; Preheating temperature is 250-350 ℃, and wherein the feed coal of 60-80% enters the coal hydrogenation pyrolysis stove and carries out hydropyrolysis, and synthesis pressure is 1.0-3.0MPa, and temperature is 550-680 ℃; The pyrolysis gas-phase product enters the purification separation system; Whole semicokes that the coal hydrogenation pyrolysis stove produces are sent into burnt hydrogasification stove and are carried out hydrogasification, and vapor pressure is 1.0-3.0MPa, and temperature is 327-427 ℃, and the gasification gas-phase product enters the separation system purification separation; The feed coal of 20-40% after the dry and preheating with in rich hydrogen generator, carry out gasification reaction from the burnt grain of hydrogasification stove and oxygen and water vapour, reaction pressure is 1.0-3.0MPa, temperature is 900-1500 ℃.The method needs the feed coal after dry and the preheating to be separated complex operation by different usage quantitys; Do not realize the coupling of heat, power loss is large; During the transformation efficiency of semicoke in the burnt hydrogasification stove 〉=70%, semicoke hydrogenation methanation speed is very low, causes whole methanation reaction speed not high.
Summary of the invention
The technical problem to be solved in the present invention is the problem that hydrogen gas consumption is large in the Hydrogenation methane technology, heat utilization rate is lower, and provides a kind of low-rank coal methane technology processed.
It is a kind of technique of low order preparing methane from coal that the present invention addresses the above problem institute's Adopts measure, and its described technique follows these steps to carry out:
(1) 3～10mm low-rank coal is carried out drying under 110～200 ℃, makes its moisture content be down to 5～8%(wt%), after send into pyrolysis reactor, under 300～700 ℃ and condition of normal pressure, carry out pyrolysis, the pyrolysis that obtains pyrolysis char and contain tar generates gas;
Pyrolysis char being sent in the methanator, is 750～930 ℃ in temperature again, and pressure is to react under the 3-5Mpa, the part and vaporized chemical H of easily reacting in the pyrolysis char
2C+2H occurs
2→ CH
4Reaction generates and is rich in CH
4Reaction generate gas, react remaining methanation residue and send into gasifying reactor and carry out pressurized gasification;
(2) the pyrolysis generation gas that contains tar is exported, and through cooling, separation, purification, obtains tar and pyrolysis generation gas, again pyrolysis is generated gas and carry out CO conversion and gas delivery, obtain methane, carbonic acid gas and hydrogen-rich gas, wherein methane is as output of products, and hydrogen-rich gas is as the circulation gas I;
(3) 500 ~ 800 ℃ methanation of methanator output generates gas, sends into pyrolysis reactor and coal charge and carries out indirect heat exchange, and raw coal is carried out pyrolysis; Methanation by pyrolysis reactor output generates gas obtains respectively 30～150 ℃ again with circulating hydrogen and cold water heat exchange cold methanation generation gas, by purifying, separating, obtains synthetic natural gas and circulation gas II;
(4) gasification of 500～700 ℃ in pyrolysis reactor generation gas and coal charge carry out indirect heat exchange, by purification, conversion, decarburization, obtain the circulation gas III;
(5) the circulation gas I that above-mentioned steps is obtained, circulation gas II and circulation gas III obtain circulating hydrogen after mixing, and circulating hydrogen is sent into methanator as vaporized chemical after preheating.
Based on the technique of above-mentioned a kind of low order preparing methane from coal, further,
Described low-rank coal is brown coal, long-flame coal or non-caking coal.
It can be after mixing first that the gasification that the pyrolysis of described step (2) generates gas and step (4) generates gas, purifies, conversion again.
The tar yield that the described pyrolysis that contains tar generates in the gas is to send into 5～12%(wt%) of pyrolysis reactor feed coal.
After described pyrolysis char was sent into and reacted in the methanator, the rate of rotation of carbon was 35～60% in the pyrolysis char.
Realize a kind of low-rank coal provided by the present invention methane technology processed, compared with prior art, its advantage and positively effect are:
The one, the main reaction of this technique methane processed is C+2H
2→ CH
4, system's hydrogen consumption is low.
The 2nd, the coupling of this technological process Process of absorption or liberation of heat reacting phase, system thermal efficiency is higher.
The 3rd, the gas product character of different units differs greatly, and the different units gas product does not mix mutually in this technique, and gas processing is with strong points, the processing load is little, efficient is high.
The 4th, this technique can realize that hydrogen is self-supporting.
Description of drawings
Fig. 1 is the process flow sheet of a kind of low order preparing methane from coal of the present invention.
Embodiment
Can make further description to the technique of a kind of low order preparing methane from coal provided by the present invention by description of drawings and specific embodiment, but not technique of the present invention is made restriction.
Embodiment 1
Implement the technique of a kind of low order preparing methane from coal provided by the present invention, take the technical process of producing 11 billion cubic meter methane per year as example, its described concrete technology follows these steps to carry out:
The present embodiment is take brown coal as raw material, and the basic coal analysis of used brown coal sees Table one.1.78 ten thousand tons of/day brown coal raw coal are broken, be sized to 3-6mm, and carry out drying and dehydrating under 150 ℃, and obtain drying brown coal, its moisture content is 8%(wt%).The drying brown coal charging capacity is 1.6 ten thousand tons/day in the pyrolysis reactor.Drying brown coal stopped 1.5 hours in pyrolysis reactor and under 600 ℃ the pyrolysis temperature, the product that obtains is that pyrolysis char and the pyrolysis that contains tar generate gas, wherein the output of 600 ℃ of pyrolysis chars is 10,000 tons/day, pyrolysis generates gas can obtain approximately 1900 tons/day of cryogenic fuel formed coke oil through cooling, separation, the amount that pyrolysis through purifying generates gas is that pyrolysis generates gas 2,400,000 Nm3, and its composition and volume content see Table two.
600 ℃ of pyrolysis chars are intermittently added by the methanator top, circulating hydrogen is passed into continuously by the methanator bottom, temperature of reaction in the methanator is 800-830 ℃, reaction pressure is 5MPa, with this understanding, carbon in the pyrolysis char and the hydrogen generation methane that reacts owing to also having a small amount of oxygen element in the pyrolysis char, therefore has a small amount of CO, CO
2And H
2O generates, because the differences such as side-chain radical, aromatic ring structure and fragrant synusia structure contain the carbon structure existence in the pyrolysis char, therefore exist easy hydrogenation regardless of adding hydrogen partial with difficulty in the pyrolysis char, wherein difficult hydrogenation partial reaction is poor, speed of reaction is slow, therefore only easy hydrogenation is transformed regardless of carbon structure at methanator, controlling in the present embodiment the efficiency of carbon conversion of pyrolysis char in methanator is 41.64%, and the residue non-reacted parts is as supplying gas of methanation residue reactor.The output that methanation generates gas is 1,112 ten thousand Nm3/ days, and its composition and volume content see Table three.
The high-temperature methanation residue is sent in the gasifying reactor by intermittence, under 1000-1200 ℃ and 3MPa pressure, carry out gasification reaction with water vapour and oxygen, carbon in the methanation residue is almost utilized fully, and the output that gasification generates gas is 9,460,000 Nm3, and it forms and volume content sees Table four.
Methanation generates gas and gasification generation gas is high temperature and high pressure gas, these two kinds of gases are sent into respectively in the pyrolysis reactor in the different heating pipe, make high-temperature gas as thermal source and coal charge indirect heat exchange, the gas that goes out pyrolysis reactor has three the tunnel altogether, be respectively pyrolysis and generate gas, methanation generation gas and gasification generation gas, this three road gas is in respectively different pipelines, therefore can realize individual curing.The pyrolysis that goes out pyrolysis reactor generates gas and cools off first, separates dust, tar and the water removed wherein, purify again, conversion, carry out at last gas delivery, obtain high methane gas I, carbonic acid gas and remaining hydrogen-rich gas, hydrogen-rich gas is as circulation gas.
The methanation that goes out pyrolysis reactor generate gas first respectively with circulating hydrogen and cold water heat exchange, through purifying laggard promoting the circulation of qi body membrane sepn, obtain high methane gas 2 and hydrogen-rich gas 2, hydrogen-rich gas 2 is as the circulation gas II.
The gasification that goes out pyrolysis reactor generates gas first through heat exchange, purification, conversion, then carries out decarburization and makes CO
2Concentration is reduced to below 0.3%, obtains the circulation gas III.
Circulation gas I, circulation gas II and circulation gas III are mixed to get mixed cycle hydrogen, send into methanator as vaporized chemical again with after the heat exchange of methanation generation gas.
The said process common property is given birth to CH
4379.74 ten thousand Nm3/ days, close 11.39 hundred million Nm3/, system's common property in whole process is given birth to H
2730.13 ten thousand Nm3/ days (wherein generate 48.84 ten thousand Nm3 in the pyrolytic reaction, gasification reaction generates 418.98 ten thousand Nm3, and the CO conversion generates 262.32 ten thousand Nm3) is greater than system consumption H
26,820,000 Nm3/ days (consuming in the methanator), system can realize that hydrogen is self-supporting.
Table one Brown Coal analysis (as received basis %)
| Moisture | Ash content | C | H | O | N | S |
| 17 | 19.49 | 40.03 | 2.84 | 19.53 | 0.79 | 0.32 |
Table two pyrolysis generates gas and forms and content
| Component | CH 4 | CO | H 2 | O 2 | CO 2 | C 2H 4 | C 2H 6 | N 2 |
| Content (v%) | 24.52 | 10.52 | 20.35 | 0.43 | 40.15 | 1.02 | 2.48 | 0.53 |
The table leucoaurin generates gas and forms and content
| Component | CH 4 | CO | CO 2 | C mH n | H 2 | H 2S | NH 3 |
| Content (v%) | 27.64 | 2.01 | 1.26 | 1.35 | 66.37 | 0.18 | 1.19 |
Table four gasification gas forms and content
| Component | H 2 | CO | CH 4 | CO 2 | O 2 | N 2 | H 2S |
| Content (v%) | 44.29 | 25.06 | 1.43 | 28.89 | 0.13 | 0.05 | 0.15 |
Embodiment 2
Implement the technique of a kind of low order preparing methane from coal provided by the present invention, produce the technical process of 6 billion cubic meter methane per year.Its described concrete technology follows these steps to carry out:
The present embodiment is take long-flame coal as raw material, and its concrete analysis sees Table five.Be that the long-flame coal of 5-10mm is sent into pyrolysis reactor with granularity, its charging capacity is 5000 tons/day.The residence time of long-flame coal in pyrolysis reactor is 2.5 hours, obtain 650 ℃ of pyrolysis chars through pyrolysis and generate gas with the pyrolysis that contains tar, wherein the output of 650 ℃ of pyrolysis chars is 4028 tons/day, pyrolysis generates gas can obtain approximately 273 tons/day of cryogenic fuel formed coke oil through cooling, separation, the amount that pyrolysis through purifying generates gas is that pyrolysis generates gas 500,000 Nm3, and its composition and volume content see Table six.
650 ℃ of pyrolysis chars are intermittently added by the methanator top, circulating hydrogen is passed into continuously by the methanator bottom, temperature of reaction in the methanator is 760-800 ℃, reaction pressure is 4MPa, with this understanding, carbon in the pyrolysis char and the hydrogen generation methane that reacts, controlling in the present embodiment the efficiency of carbon conversion of pyrolysis char in methanator is 38%, the residue non-reacted parts is as supplying gas of methanation residue reactor.The output that methanation generates gas is 7,460,000 Nm3/ days, and its composition and volume content see Table seven.
The high-temperature methanation residue is sent in the gasifying reactor by intermittence, under 1000-1200 ℃ and 3MPa pressure, carry out gasification reaction with water vapour and oxygen, carbon in the methanation residue is almost utilized fully, and the output that gasification generates gas is 7,610,000 Nm3, and it forms and volume content sees Table eight.
Methanation generates gas and gasification generation gas is high temperature and high pressure gas, these two kinds of gases are sent into respectively in the pyrolysis reactor in the different heating pipe, make high-temperature gas as thermal source and coal charge indirect heat exchange, the gas that goes out pyrolysis reactor has three the tunnel altogether, be respectively pyrolysis and generate gas, methanation generation gas and gasification generation gas, this three road gas is in respectively different pipelines, therefore can realize individual curing.The pyrolysis that goes out pyrolysis reactor generates gas and cools off first, separates dust, tar and the water removed wherein, purify again, conversion, carry out at last gas delivery, obtain high methane gas 1, carbonic acid gas and remaining hydrogen-rich gas, hydrogen-rich gas is as the circulation gas I.
The methanation that goes out pyrolysis reactor generate gas first respectively with circulating hydrogen and cold water heat exchange, through purifying laggard promoting the circulation of qi body membrane sepn, obtain high methane gas 2 and hydrogen-rich gas 2, hydrogen-rich gas 2 is as the circulation gas II.
The gasification that goes out pyrolysis reactor generates gas first through heat exchange, purification, conversion, then carries out decarburization and makes CO
2Concentration is reduced to below 0.3%, obtains the circulation gas III.
Circulation gas I, circulation gas II and circulation gas III are mixed to get mixed cycle hydrogen, send into methanator as vaporized chemical after generating the gas heat exchange with methanation.
The said process common property is given birth to CH
42,080,000 Nm3/ days, close 6.24 hundred million Nm3/ (by 300 days notes), system's common property in whole process is given birth to H
25,610,000 Nm3/ days (wherein generate 13.38 ten thousand Nm3 in the pyrolytic reaction, gasification reaction generates 3,680,000 Nm3, and the CO conversion generates 1,800,000 Nm3) is greater than system consumption H
24,300,000 Nm3/ days (consuming in the methanator), system can realize that hydrogen is self-supporting.
Table five long-flame coal analytical table (as received basis %)
| Moisture | Ash content | C | H | O | N | S |
| 3.6 | 3.76 | 75.66 | 4.42 | 11.12 | 1.19 | 0.25 |
Table six pyrolysis generates gas and forms and content
| Component | CH 4 | CO | H 2 | O 2 | CO 2 | C 2H 4 | C 2H 6 | N 2 |
| Content (v%) | 22.72 | 17.03 | 26.77 | 0.21 | 30.63 | 0.87 | 1.43 | 0.34 |
Table seven methane generates gas and forms and content
| Component | CH 4 | CO | CO 2 | C mH n | H 2 | H 2S | NH 3 |
| Content (v%) | 25.37 | 2.15 | 1.14 | 1.74 | 68.47 | 0.11 | 1.02 |
Table eight gasification gas forms and content
| Component | H 2 | CO | CH 4 | CO 2 | O 2 | N 2 | H 2S |
| Content (v%) | 48.41 | 22.56 | 1.03 | 27.77 | 0.10 | 0.02 | 0.11 |
The feature of this technique pyrolysis reactor is to generate gas with High Temperature High Pressure methanation generation gas and High Temperature High Pressure gasification to carry out heat exchange by indirect mode and coal charge, methanation generates gas, gasification generates gas and pyrolysis generation gas three isolates mutually, like this so that more easy when processing each portion gas, load little, efficient is high.And above-mentioned three road gases can be first and the circulating hydrogen heat exchange after out from pyrolysis reactor, improved heat utilization ratio, reduces energy dissipation.This technique coal utilization rate is high, and the final C transformation efficiency of raw coal is more than 95%, and system can realize that hydrogen is self-supporting.In addition, can regulate tar yield according to the market requirement.
Claims (5)
1. low-rank coal methane technology processed, its described technique follows these steps to carry out:
(1) 3～10mm low-rank coal is carried out drying under 110～200 ℃, makes its moisture content be down to 5～8%(wt%), after send into pyrolysis reactor, under 300～700 ℃ and condition of normal pressure, carry out pyrolysis, the pyrolysis that obtains pyrolysis char and contain tar generates gas;
Pyrolysis char being sent in the methanator, is 750～930 ℃ in temperature again, and pressure is to react under the 3-5Mpa, the part and vaporized chemical H of easily reacting in the pyrolysis char
2C+2H occurs
2→ CH
4Reaction generates and is rich in CH
4Reaction generate gas, react remaining methanation residue and send into gasifying reactor and carry out pressurized gasification;
(2) the pyrolysis generation gas that contains tar is exported by pyrolysis reactor, through cooling, separation, purification, obtain tar and pyrolysis and generate gas, again pyrolysis is generated gas and carry out CO conversion and gas delivery, obtain methane, carbonic acid gas and hydrogen-rich gas, wherein methane is as output of products, and hydrogen-rich gas is as the circulation gas I;
(3) 500 ~ 800 ℃ methanation of methanator output generates gas, sends into pyrolysis reactor and feed coal and carries out indirect heat exchange, and feed coal is carried out pyrolysis; Methanation by pyrolysis reactor output generates gas obtains respectively 30～150 ℃ again with circulating hydrogen and cold water heat exchange cold methanation generation gas, by purifying, separating, obtains synthetic natural gas and circulation gas II;
(4) 500～700 ℃ gasification of gasifying reactor output generates gas, sends in the pyrolysis reactor, carries out indirect heat exchange with feed coal, by purification, conversion, decarburization, obtains the circulation gas III;
(5) the circulation gas I that above-mentioned steps is obtained, circulation gas II and circulation gas III obtain circulating hydrogen after mixing, and circulating hydrogen is sent into methanator as vaporized chemical after preheating.
2. low-rank coal as claimed in claim 1 methane technology processed, its described low-rank coal is brown coal, long-flame coal or non-caking coal.
3. it can be after mixing first that the gasification that low-rank coal as claimed in claim 1 methane technology processed, the pyrolysis of its described step (2) generate gas and step (4) generates gas, purifies, conversion, separation again.
4. low-rank coal as claimed in claim 1 methane technology processed, the output of its described tar is to send into 5～12%(wt%) of pyrolysis reactor low-rank coal.
5. low-rank coal as claimed in claim 1 methane technology processed, after its described pyrolysis char reacted in methanator, the rate of rotation of carbon was 35～60% in the pyrolysis char.
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| CN106118770A (en) * | 2016-07-01 | 2016-11-16 | 北京神雾环境能源科技集团股份有限公司 | A kind of system and method catalyzing and synthesizing natural gas |
| CN110467943A (en) * | 2018-05-11 | 2019-11-19 | 成都聚实节能科技有限公司 | A kind of natural gas from coal, alkene and coal tar method |
| CN110467943B (en) * | 2018-05-11 | 2022-04-15 | 成都聚实节能科技有限公司 | Method for preparing natural gas, olefin and coal tar from coal |
| CN109880654A (en) * | 2019-02-01 | 2019-06-14 | 浙江天禄环境科技有限公司 | A method of utilizing volatile matter Fischer Tropsch waxes in low-order coal |
| CN110628478A (en) * | 2019-09-20 | 2019-12-31 | 成都聚实节能科技有限公司 | Method for co-producing fuel oil aromatic hydrocarbon by coal-based natural gas through pressurized moving bed |
| CN110628478B (en) * | 2019-09-20 | 2023-11-21 | 成都聚实节能科技有限公司 | Method for preparing natural gas and co-producing fuel aromatic hydrocarbon by using pressurized moving bed coal |
| 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 |
| CN113753856A (en) * | 2021-09-27 | 2021-12-07 | 太原理工大学 | Organic solid waste gasification integrated efficient hydrogen and methane production process |
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