CN105132056B - Lignite steam hydro-gasification process for producing natural and its system - Google Patents
Lignite steam hydro-gasification process for producing natural and its system Download PDFInfo
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Abstract
The present invention relates to a kind of lignite steam hydro-gasification process for producing natural and its systems, technical solution adds hydrogen including lignite is directly carried out lignite steam, gas product is made after adding washing, depickling, transformation, methanation reaction, drying again in reaction gas, and all hydrogen are self-produced in entire technique.The system comprises steam hydro-gasification stoves, the top exit of the steam hydro-gasification stove is connect with the gas feed of washing, purifying system, outlet at bottom is connect through coke gasification stove with the gas feed of washing, purifying system, and the outlet of the washing, purifying system is sequentially connected resistant to sulfur water-gas shift system, acid gas removal system, low temperature methanation system and drying system.Present invention process is simple, energy-saving, investment cost and operating cost is low, environmentally friendly, production quality gas product.
Description
Technical field
The present invention relates to a kind of right gas technique of lignite work and its system, specifically a kind of lignite steam hydro-gasification
Process for producing natural and its system.
Background technology
China's lignite resource enriches, and lignite accounts for more than 13% in the coal reserves verified in China, up to more than 1,300 hundred million
Ton.Lignite degree of coalification is low, and pore is flourishing, and oxygen content height (moisture-and-ash-free basis 20% or so), interior water enriches, and total moisture is up to
30-50%, calorific value is relatively low, and thermal stability is poor, unsuitable long-distance transportation, has again directly as extensive gasified raw material very big
Limitation.
Early 20th century people just begin one's study analysis hydrogasification technique, obtained extensively to the 70-90 ages in 20th century
General research is the gold period of hydrogasification.Several typical coal hydrogenation methanation process such as Hygas, Hydrane, BG-OG are successive
It carries out to the pilot scale stage.It is reacted using coal with hydrogen direct gasification and improves methane content in raw gas, follow-up methanation can be reduced
The load of unit, to improve the Technical Economy of whole coal gas.
For traditional two step method natural gas from coal technique, the lignite of High water cut need to through predrying upgrading (water content 5~
It is allowed for access after 15wt%) gasification furnace, aqueous dry tail gas direct emission causes water resource waste；Traditional gasification outlet of still CH4
Content is relatively low, and (fixed bed gasification outlet of still methane content is less than 15%, and dry coal powder gasification and coal water slurry gasification outlet of still methane
Content is extremely low), in order to improve gas production and full-range economy, the high temperature of three sections of generally use or multi-stage series/low
Warm methanator is higher (CN 201210029443) to catalyst stability and high-temperature reactor design requirement.
Chinese patent CN201110021674 discloses a kind of " a kind of method of coal hydrogenation pyrolysis and gasification coupling ", passes through
By hydropyrolysis, semicoke hydrogasification and char particle hydrogen manufacturing with reference to improving light component content and tar yield, wherein, hydrogasification
Stove vapor pressure 1.0-3.0MPa, temperature are 327-427 DEG C.Dried upgraded coal is entered gasification furnace (20- by the program on demand
40%) it is cumbersome with hydropyrolysis stove (60-80%)；Cyclone bed hydrogen-manufacturing reactor is separately provided, inner structure needs special set
Meter, causes equipment manufacturing costs to improve.
Invention content
The purpose of the present invention is to solve above-mentioned technical problems, provide a kind of simple for process, energy-saving, cost of investment
Low with operating cost, environmentally friendly, production quality gas product lignite steam hydro-gasification process for producing natural.
The present invention also provides a kind of system for above-mentioned technique, have simple system, equipment investment and operating cost it is low,
The advantages of energy conservation and environmental protection.
Lignite steam hydro-gasification process for producing natural of the present invention, includes the following steps：
One, the lignite that water content is 20-50%wt is sent into steam hydro-gasification stove and is done in the presence of hydrogen gas
Dry, pyrolysis, the steam that brown coal drying generates in the process further participates in hydrogasification reaction, obtains tail gas and carbon residue, described residual
Carbon is sent into coke gasification stove and O2, vapor occur high-temperature gasification raw gas is obtained by the reaction；
Two, the tail gas and raw gas are first sent into washing, purifying system and are dusted to obtain gaseous mixture, are re-fed into resistant to sulfur water
Hydrogen-carbon ratio in vapour transformation system adjustment gaseous mixture is then fed into acid gas removal system removing sour gas and is purified
Gas；
Three；The purified gas is sent into low temperature methanation system and carries out methanation reaction generation CH4And water, it is sent into drying system
Gas product is obtained after dry water removal.
In the step 2, purified gas is first sent into separator and isolates hydrogen partial, and the hydrogen partial isolated is through supercharging
It is sent into after raw gas indirect preheating described in preheated device in steam hydro-gasification stove again after system boost and participates in hydrogasification reaction；
Remaining purified gas is sent into low temperature methanation system.
In the step 1, the mass ratio of hydrogen and lignite is 0.01-1 in hydrogasification stove.In the step 1, control
The gas outlet temperature of steam hydro-gasification stove is 700-800 DEG C.In the step 1, in steam hydro-gasification furnace roof portion tail gas
CH4Dry molar content is between 25~65%, the tail gas and the mixed CH of raw gas4Dry molar content is not less than 20%.
In the step 2, go out the H in the gaseous mixture of resistant to sulfur water-gas shift system2/ CO ratios are 5.0-15.0, higher than feeding
H in the purified gas of low temperature methanation system2/ CO ratios (between 2.5-3.5).
In the step 3, low temperature methanation system uses two-stage low temperature adiabatic reactor connection in series-parallel, wherein, the purification
Pneumatic transmission exchanges heat after entering level-one Cryo Heat Insulation reactor reaction through heat exchanger, and two grade low-temp methane are sent into the purified gas part after heat exchange
Change reactor reaction, then loopback enters level-one Cryo Heat Insulation reactor inlet to rest part；Control level-one Cryo Heat Insulation reactor anti-
It is 200-450 DEG C to answer temperature, and two level Cryo Heat Insulation reactor reaction temperature is 200-400 DEG C.
Present system includes steam hydro-gasification stove, top exit and the washing, purifying system of the steam hydro-gasification stove
The gas feed connection of system, outlet at bottom are connect through coke gasification stove with the gas feed of washing, purifying system, and the washing is net
The outlet of change system is sequentially connected resistant to sulfur water-gas shift system, acid gas removal system, low temperature methanation system and dry system
System.
The acid gas removal system and separator gas feed connection, the clean gas outlet of the separator with it is low
Warm methanation system connection, the hydrogen outlet of separator are connect successively through pressure charging system with steam hydro-gasification stove.
Tube side or shell side of the pressure charging system through heat exchanger are connect with steam hydro-gasification stove；The coke gasification stove
Shell side or tube side of the gas vent through heat exchanger are connect with the gas feed of washing, purifying system.
The low temperature methanation system is sequentially connected in series heat exchanger, two level Cryo Heat Insulation reaction for level-one Cryo Heat Insulation reactor
Device, wherein, heat exchanger exit is connect respectively with level-one Cryo Heat Insulation reactor inlet and two level Cryo Heat Insulation reactor inlet.
Water content is higher in lignite, and brown coal drying pretreatment unit can be separately provided in the prior art makes brown coal drying, this
Sample can not only increase the complexity that dry tail gas recycle utilizes, and direct emission will also result in the wasting of resources, and it is dirty to aggravate environment
Dye.In the present invention, inventor does not carry out predrying individually to lignite, will cleverly be lacked using this aqueous feature of lignite instead
Point become advantage, directly by lignite be sent into steam hydro-gasification stove in, make lignite reacted with hydrogasification in stove after tail gas generation
Water is obtained while indirect heat exchange drying brown coal and steams water, in H2In the presence of, all or part of vapor for being evaporated in lignite with
Hydrogenation reaction occurs for lignite after drying, so as to recycle the moisture in lignite indirectly, without brown coal drying is separately provided
Pretreatment unit, simple flow reduce equipment investment, and no waste water and gas discharge is environmentally friendly, achieves many things at one stroke.
It reacts in the steam hydro-gasification stove：C+H2O→CO+H2, hydrogen can be generated, but react the hydrogen generated
The consumption of hydrogenation reaction is not met by, the invention people is considered in the gaseous mixture of resistant to sulfur water-gas shift system
Hydrogen-carbon ratio is allowed to higher than the hydrogen-carbon ratio being sent into the purified gas of low temperature methanation system, makes to contain more hydrogen in gaseous mixture, this
The extra hydrogen in part is detached in the separator, and is sent into steam as gasifying agent cycle after pressure charging system is pressurized and is preheated and is added
In hydrogen gasification furnace, so as to make the hydrogen of hydrogasification reaction needs all self-produced, production cost further reduced.
Carbon residue and O from steam hydrogenation reactor in coke gasification stove2, vapor occur high-temperature gasification, generation
Raw gas temperature is high, this partial heat can be used for warm-up cycle to enter steam and add hydrogen in hydrogen stove, be allowed to meet intake air temperature
It is required that the recycling of heat be also beneficial to it is energy-saving, it is environmentally friendly.
In order to ensure methane content in efficiency of carbon con version and offgas outlet, the gas outlet temperature of the steam hydro-gasification stove
Preferably 700-800 DEG C, the mass ratio of hydrogen and lignite is preferably 0.02-0.5 in the steam hydro-gasification stove.
Traditional gasification outlet of still CH4Content is relatively low, and (fixed bed gasification outlet of still methane content is less than 15%, and dry pulverized coal gas
Change and coal water slurry gasification outlet of still methane content be extremely low), in the present invention, employing hydrogen hydrogenation reaction directly occurring with lignite can carry
CH in tail gas in high hydrogasification furnace gases outlet4Content, CH4Dry molar content is reachable between 25~65%, the CH4
You can be controlled composition unlubricated friction by adjusting the mass ratio of hydrogen in steam hydrogasification stove and lignite, finally make tail gas and
The mixed CH of raw gas4Dry molar content is higher due to that can generate methane content in gasification unit not less than 20%
Synthesis gas, therefore without using high-temperature methanation reactor in low temperature methanation system, but use two-stage low temperature adiabatic anti-
Device connection in series-parallel is answered, level-one Cryo Heat Insulation reactor reaction temperature is 200-450 DEG C, and two level Cryo Heat Insulation reactor reaction temperature is
200-400 DEG C, the temperature of two-stage low temperature adiabatic reactor can substantially reduce technology difficulty, solve so not higher than 450 DEG C
In the prior art high CH is produced by the way of connection in series-parallel high-temperature methanation reactor and low temperature methanator4The conjunction of concentration
Into natural gas, high-temperature methanation reactor and its mating waste heat boiler equipment material are expensive, and there are overtemperature it is dangerous because
The problem of element and operating cost are high.
Compared with prior art, the present invention has the following advantages：
(1) directly using High water cut lignite as raw material, all or part of moisture participation vapor that brown coal drying generates adds hydrogen
Gasification reaction recycles valuable water resource, while saves expensive lignite predrying unit, greatly reduces equipment investment and fortune
Row cost.
(2) this technique integrates steam hydro-gasification stove, improves methane content in raw gas, reduces setting for subsequent processing units
Count load.
(3) whole system hydrogen output is more than demand, realizes that hydrogen is marketed one's own products.
(4) methanation system is not needed to only with Cryo Heat Insulation reactor using distinguishingly high-temperature reactor and high temperature give up
The special expensives equipment such as pot reduce the generation of the insecurity such as overtemperature, improve the stability of system operation.
(5) present system is discharged almost without waste water and gas, energy-saving, environmentally friendly, the methane of energy steady production
Concentration is more than mole percent 95%, CO2Content is less than the gas product of mole percent 2.0%.
Description of the drawings
Fig. 1 is present invention process flow chart and system diagram.
Fig. 2 is low temperature methanation system schematic diagram of the present invention.
Wherein, 1.1- steam hydro-gasifications stove, 1.2- coke gasification stoves, 2- washing, purifying systems, 3- sulphur-resistant conversion systems,
4- acid gas removal systems, 5- separators, 6- low temperature methanation systems, 6.1- level-one Cryo Heat Insulations reactor, 6.2- heat exchange
Device, 6.3- two level Cryo Heat Insulations reactor, 7- drying systems, 8- pressure charging systems, 9- preheaters.
Specific embodiment
Explanation is further explained to the present invention below in conjunction with the accompanying drawings：
System embodiment：
Referring to Fig. 1, present system includes steam hydro-gasification stove 1.1, and the top of the steam hydro-gasification stove 1.1 goes out
Mouthful connect with the gas feed of washing, purifying system 2, the outlet at bottom of steam hydro-gasification stove 1.1 through coke gasification stove 1.2, in advance
The shell side of hot device 9 is connect with the gas feed of washing, purifying system 2, and the outlet of the washing, purifying system 2 is sequentially connected resistant to sulfur
Water-gas shift system 3, acid gas removal system 4, separator 5, low temperature methanation system 6 and drying system 7.
The acid gas removal system 4 is connect with the gas feed of separator 5, the clean gas outlet of the separator 5
It is connect with low temperature methanation system 6, the hydrogen outlet of separator 5 adds successively through pressure charging system 8, the tube side of preheater 9 and steam
Hydrogen gasification furnace 1 connects.
Referring to Fig. 2, the low temperature methanation system 6 is two-stage low temperature adiabatic reactor serial or parallel connection, wherein, level-one is low
Warm adiabatic reactor 6.1 is sequentially connected in series heat exchanger 6.3, two level Cryo Heat Insulation reactor 6.2, wherein, the outlet of heat exchanger 6.2 difference
It is connect with 6.1 entrance of level-one Cryo Heat Insulation reactor and 6.3 entrance of two level Cryo Heat Insulation reactor.
Process example：
For the present embodiment using lignite as raw material, the Brown Coal fundamental analysis data of use are shown in Table 1
Lignite enters steam hydro-gasification stove 1.1 after broken, screening, and lignite is straight with the tail gas after hydrogenation reaction in stove
Connect heat exchange, generate the dry coal for carrying water vapor component, this part dry coal occur in the presence of hydrogen carbon and hydrogen plus
Hydrogen reaction, carbon are reacted with the carbon that disappears of vapor, and following reaction mainly occurs in steam hydro-gasification stove 1：
2H2+C→CH4 ΔHo 298=-74.8kJ/mol
C+H2O→CO+H2 ΔHo 298=118kJ/mol
Wherein, the hydrogen that the hydrogen source in stove is isolated in piece-rate system 5 controls steam hydro-gasification in the present embodiment
Hydrogen and lignite (wet coal) mass ratio are 0.04 in stove 1.1, and 1.1 outlet temperature of steam hydro-gasification stove is 744 DEG C, produces tail gas
(unlubricated friction that composition is shown in Table 2) is discharged by furnace roof portion；It is high to be sent into coke for unreacted carbon residue (solid-state) in steam hydro-gasification stove 1.1
Warm gasification furnace 1.2, under the reaction condition of 4.0MPa with O2, vapor occur high-temperature gasification reaction, carbon residue is in this coke gasification
Raw gas is substantially completely converted in stove 1.2, the outlet temperature of coke high-temperature gasification furnace 1.2 is 1197 DEG C, and raw gas is by coke
Preheated device 9 is discharged to being generated after the preheating of the hydrogen of pressure charging system 8 with steam hydro-gasification stove 1.1 in 1.2 top of gasification furnace
Tail gas mixing (CH in the tail gas and the mixed gaseous mixture of raw gas4Dry molar content is not less than 20%) feeding washing afterwards
2 dedusting of cleaning system enters back into the H in the adjustment gaseous product of resistant to sulfur water-gas shift system 32/ CO molar ratios (should for 5.0-15.0
Higher than the H being sent into the purified gas of low temperature methanation system2/ CO is than 2.5-3.5), it produces conversion gas composition and is shown in Table 3, conversion gas
It is sent into 4 removing sour gas of acid gas removal system and is purified gas, the purified gas, which is sent into during separator 5 detaches, goes out part
(fractional dose of hydrogen determines hydrogen according to the hydrogen-carbon ratio in the purified gas of low temperature methanation system is sent into, higher than above-mentioned hydrogen-carbon ratio
Hydrogen can be separated), the hydrogen separated through separator 5 is after hydrogen outlet is sent into pressure charging system supercharging again by from coke
Steam hydrogasification is sent into after the raw gas indirect preheating of gasification furnace 1.2 to the intake air temperature requirement of steam hydrogasification stove 1.1
As hydrogen source in stove 1.1.The purified gas that clean gas outlet through separator 5 is drawn is sent into low temperature methanation system 6, low
In warm methanation system 6, purified gas is successively through level-one isothermal adiabatic reactor 6.1, heat exchanger 6.3 and two level isothermal adiabatic reaction
Device 6.2 carries out methanation reaction and heat exchange, and two level Cryo Heat Insulation reactor is sent into after going out the purified gas partial boost of heat exchanger 6.3
6.2 reaction, remaining supercharging after loopback enter level-one Cryo Heat Insulation reactor 6.1.Wherein, level-one Cryo Heat Insulation reactor 6.1 reacts
Temperature is 200-450 DEG C, and 6.2 reaction temperature of two level Cryo Heat Insulation reactor is 200-400 DEG C, goes out low temperature methanation system 6
Institute's producing natural gas production mouth composition is shown in Table 4 after synthesis gas is finally sent into drying system refrigerated separation, dry water removal, meets natural gas production
Product standard requires (GB 17820-2012 natural gases).
1 Brown Coal of table analyzes data
2 steam hydro-gasification outlet of still crude synthesis gas unlubricated friction of table that composition
| Component | H2 | CO | CO2 | CH4 | N2 | H2S | COS |
| Content (mol%) | 40.33 | 10.38 | 13.54 | 34.80 | 0.46 | 0.48 | 0.006 |
3 water-gas shift unit of table outlet conversion gas unlubricated friction that composition
| Component | H2 | CO | CO2 | CH4 | N2 | H2S | COS |
| Content (mol%) | 48.65 | 8.28 | 26.73 | 15.79 | 0.27 | 0.27 | 0.0047 |
4 methanation exported product gas unlubricated friction of table that composition
| Component | H2 | CO | CO2 | CH4 | N2 |
| Content (mol%) | 0.81 | 0.0009 | 0.88 | 98.03 | 0.27 |
Claims (5)
1. a kind of lignite steam hydro-gasification process for producing natural, which is characterized in that include the following steps：
One, the lignite that water content is 20-50%wt is sent into steam hydro-gasification stove after broken, screening in the presence of hydrogen
Under be dried, be pyrolyzed, the steam generated during brown coal drying further participates in hydrogasification reaction, obtains tail gas and residual
Charcoal, the carbon residue are sent into coke gasification stove and O2, vapor occur high-temperature gasification raw gas is obtained by the reaction；
Two, it is first sent into washing, purifying system after the tail gas and raw gas mixing and is dusted to obtain gaseous mixture, be re-fed into resistant to sulfur
Hydrogen-carbon ratio in water-gas shift system call interception gaseous mixture is then fed into acid gas removal system removing sour gas and is purified
Gas, purified gas are first sent into separator and isolate hydrogen partial, and the hydrogen partial isolated is preheated again after pressure charging system is pressurized
Device participates in hydrogasification reaction to being sent into after the raw gas indirect preheating in steam hydro-gasification stove, remaining purified gas is sent into low
Warm methanation system controls out the H in the gaseous mixture of resistant to sulfur water-gas shift system2/ CO molar ratios are 5.0-15.0, higher than feeding
H in the purified gas of low temperature methanation system2/ CO molar ratios 2.5-3.5；
Three, the purified gas is sent into low temperature methanation system and carries out methanation reaction generation CH4And water, it is sent into drying system drying
Gas product is obtained after water removal.
2. lignite steam hydro-gasification process for producing natural as described in claim 1, which is characterized in that in the step 1,
The mass ratio of hydrogen and lignite is between 0.01-1 in steam hydro-gasification stove.
3. lignite steam hydro-gasification process for producing natural as described in claim 1, which is characterized in that in the step 1,
The gas outlet temperature of steam hydro-gasification stove is controlled between 700-800 DEG C.
4. lignite steam hydro-gasification process for producing natural as claimed in claim 2 or claim 3, which is characterized in that the step 1
In, CH in steam hydro-gasification furnace roof portion tail gas4Dry molar content is between 25~65%, after the tail gas and raw gas mixing
CH4Dry molar content is not less than 20%.
5. lignite steam hydro-gasification process for producing natural as described in claim 1, which is characterized in that in the step 3,
Low temperature methanation system uses two-stage low temperature adiabatic reactor connection in series-parallel, wherein, the purified gas is first sent into level-one Cryo Heat Insulation
Then reactor reaction exchanges heat through heat exchanger, two level Cryo Heat Insulation reactor reaction is sent into the purified gas part after heat exchange, remaining
Then loopback enters level-one Cryo Heat Insulation reactor inlet for part；It is 200-450 DEG C to control level-one Cryo Heat Insulation reactor reaction temperature,
Two level Cryo Heat Insulation reactor reaction temperature is 200-400 DEG C.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN108998097B (en) * | 2018-08-28 | 2020-11-24 | 南京六创科技发展有限公司 | Coal gasification method |
| CN109852421A (en) * | 2019-02-25 | 2019-06-07 | 合肥德博生物能源科技有限公司 | A kind of device and method of biomass gasifying hydrogen making |
| 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 |
| CN112029542B (en) * | 2020-08-17 | 2021-10-26 | 新奥科技发展有限公司 | Hydro-gasification system and method |
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