CN109207220A - A kind of methanation process of coal based synthetic gas preparation synthetic natural gas - Google Patents
A kind of methanation process of coal based synthetic gas preparation synthetic natural gas Download PDFInfo
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- CN109207220A CN109207220A CN201710514081.0A CN201710514081A CN109207220A CN 109207220 A CN109207220 A CN 109207220A CN 201710514081 A CN201710514081 A CN 201710514081A CN 109207220 A CN109207220 A CN 109207220A
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
- C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
- C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
- C10L3/08—Production of synthetic natural gas
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/12—Regeneration of a solvent, catalyst, adsorbent or any other component used to treat or prepare a fuel
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/46—Compressors or pumps
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/58—Control or regulation of the fuel preparation of upgrading process
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- Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
A kind of methanation new process of coal based synthetic gas preparation synthetic natural gas.The methane synthesis gas come from gas purification workshop section obtains virgin gas after fine de-sulfur, passes sequentially through four concatenated adiabatic methanation reactors；Virgin gas is divided into gas A and gas B by the outlet of the first methane synthesis reactor after cooling, gas A is returned to after the first methane synthesis reactor entrance is mixed with virgin gas as circulating air after entering recycle compressor boosting and is formed unstripped gas, gas B sequentially enter second, third, the 4th methane synthesis reactor progress methane synthetic reaction；Pneumatic operated valve of releasing is installed in first methane synthesis reactor inlet, and virgin gas can be released automatically before not entering the first methane synthesis reactor.
Description
Technical field
The present invention relates to the methanation technologies such as town gas methanation, coal synthetic natural gas (SNG), belong to new energy skill
Art field specifically provides a kind of methanation new process of coal based synthetic gas preparation synthetic natural gas.
Background technique
The characteristics of china natural resources is relatively rich coal, oil starvation, few gas, 1% of the gas reserves verified less than world's total amount.
Natural gas from coal can be used as the supplement to China's natural gas notch, and developing natural gas from coal is that a solution China's natural gas supplies
Seek contradictory effective way.In Coal Chemical Engineering Project, natural gas from coal efficiency conversion ratio reaches as high as 60%, unit calorific value water consume
Minimum, calorific value is 17.8%-21% higher than minimum calorific value as defined in national quality of natural gas standard.It is carbon dioxide, hydrogen sulfide, total
The product indexs such as sulphur are also above national standard.
Natural gas from coal is with good economic efficiency in Waste Era of Oil, asks the clean utilization for solving coal resources
Topic alleviates the status of Chinese postman problem algorithm shortage, safeguards the energy security in China, realizes CO2Emission reduction, protection environment all have weight
Want meaning.
The adiabatic temperature rise of every 1% CO methane synthesis is up to 73 DEG C in the methane synthetic reaction of purified synthesis gas, every 1%
CO2About 60 DEG C of adiabatic temperature rise of methane synthesis, it is assumed that unstripped gas forms H2 30%、CO 6.6%、CO2 3.6%、CH459.8%, it produces
Product gas forms H2 10.2%、CO 1.3%、CO2 3.2%、CH485.3%, reaction carries out in adiabatic reactor, and adiabatic temperature rise is about
It is 270 DEG C.If CO content is increased to 10%, adiabatic temperature rise can reach about 400 DEG C.Therefore, the temperature of coal to SNG methane synthetic reaction
It is very significant for rising.The methanation technology of existing coal to SNG controls temperature usually using circulating technology, once circulation compression
Machine stop jumping, a large amount of virgin gases, which immediately enter reactor, can bring the rapidly heating of short time, temperature can rise rapidly 150 DEG C with
On, to alleviate strongly exothermic bring temperature rise and preventing the generation of security risk, conventional method is replaced using nitrogen, but effect is not
It is good.
Summary of the invention
The object of the present invention is to provide a kind of methanation new processes of coal based synthetic gas preparation synthetic natural gas.
In order to achieve the above-mentioned object of the invention, The technical solution adopted by the invention is as follows: coal based synthetic gas prepares synthesis of natural
The methanation process of gas, including following technical process: the methane synthesis gas come from gas purification workshop section obtains after fine de-sulfur
Virgin gas, virgin gas pass sequentially through four concatenated adiabatic methanation reactors；Virgin gas passes through the first methane synthesis reactor
Outlet is divided into gas A and gas B after cooling, and gas A, which enters after recycle compressor boosting, returns to the first methane as circulating air
Synthesis reactor entrance forms unstripped gas after mixing with virgin gas, gas B sequentially enter second, third, the synthesis of the 4th methane it is anti-
Device is answered to carry out methane synthetic reaction；First methane synthesis reactor inlet is installed by pneumatic operated valve of releasing；Second methane closes
At reactor outlet gas carry out turnout reason, by after bismethane synthesis reactor exit gas cooling water dividing again with itself gas into
Row heat exchange, the dry gas after dividing water enter back into third methane synthesis reactor；First in 4th methane synthesis reactor exit gas
Alkane contents on dry basis is greater than 96%, then obtains satisfactory synthetic natural gas SNG through cooling, dehydration.
In the above-mentioned methods, the first methane synthesis reactor is a kind of adopting heat pipes for heat transfer radial bed methanator.
It is 250 DEG C ~ 350 DEG C into each methane synthesis reactor inlet temperature, pressure is 1 ~ 8MPa, in the reactor
It is 5000h with the volume space velocity that dry gas calculates-1~30000h-1。
The first methane synthesis reactor inlet temperature is 250 DEG C ~ 300 DEG C, and outlet temperature is 600 DEG C ~ 700 DEG C, the
Two, third, the 4th methane synthesis reactor inlet temperature are 250 DEG C ~ 300 DEG C, and the second methane synthesis reactor outlet temperature is
600 DEG C ~ 700 DEG C, third methane synthesis reactor outlet temperature is 400 DEG C ~ 500 DEG C, the 4th methane synthesis reactor outlet temperature
Degree is 250 DEG C ~ 350 DEG C；Gas temperature into the compressor is 30 DEG C ~ 80 DEG C.
The reactor for carrying out methane synthetic reaction is adiabatic reactor.
The methane synthesizing catalyst be using nickel as main active component, with boehmite, aluminium oxide, magnesia,
One or both of magnesium aluminate spinel is carrier.
The catalyst is aided with the first, second auxiliary agent using nickel as main active component, and it is female to prepare activity using the precipitation method
Body.First auxiliary agent is transition metal element, one such including La, Ce, Zr, Ti etc. or two kinds.Content is Ni mass
0.1-5%；Second auxiliary agent is triethyl group hexyl phosphoric acid, lauryl sodium sulfate, methyl anyl alcohol, cellulose derivative, polyacrylamide
The dispersing agents such as amine, guar gum, ethylene glycol, polyethylene glycol, fatty acid polyethylene glycol ester, glycerol are one such or two kinds, precipitating
When replace conventional water to use as dispersing agent, usage amount for Ni dosage 0.01-1%.
Catalyst carrier is made of the complex salt of aluminium oxide and aluminium, magnesium, and wherein aluminium oxide is with γ-Al2O3Or δ-Al2O3Or
α-Al2O3Form exists, and the complex salt of aluminium and magnesium is with MgAl2O4Form exists.
First methane synthesis reactor of the invention uses radial bed reactor, and pneumatic operated valve of releasing is installed in inlet.Due to
Radial bed sensor structure is simple, bed pressure drop is small, can take heat of reaction away in time, is homogenized bed temperature, improves reactant and turns
Rate avoids catalyst from superheat region occur, extends catalyst service life；It is released technology, can be prevented using small flow
Bed is turned over, i.e., pneumatic operated valve is arranged before the first methane synthesis reactor entrance, once recycle compressor stop jumping, it immediately will be new
Fresh gas prevents high concentration CO virgin gas from continuing to influence reactor from pneumatic operated valve safety relief before the first methane synthesis reactor entrance
Temperature.
The present invention has following advantages:
1, the methanation process of coal based synthetic gas of the present invention preparation synthetic natural gas is released technology using small flow, is prevented
Bed is turned over, i.e., pneumatic operated valve is arranged before the first methane synthesis reactor entrance, once recycle compressor stop jumping, it immediately will be new
Fresh gas prevents high concentration CO virgin gas from continuing to influence reactor from pneumatic operated valve safety relief before the first methane synthesis reactor entrance
Temperature；
2, the second methane synthesis reactor, which is worked off one's feeling vent one's spleen, carries out turnout reason, i.e., by after two anti-exit gas cooling water dividings again with itself
Gas exchanges heat, and the dry gas after dividing water enters back into third methane synthesis reactor entrance.This technique can be according to required product
Gas content freely adjusts a point water, further increases the content of product gas methane；
3, the first methane synthesis reactor is radial bed reactor, and structure is simple, bed pressure drop is small, can take reaction heat away in time
Amount is homogenized bed temperature, improves reaction-ure conversion-age, and catalyst is avoided superheat region occur, extends catalyst service life.
Detailed description of the invention
Fig. 1 is the process flow diagram of the embodiment of the present invention.
In figure, the first methane synthesis reactor of R1-, the second methane synthesis reactor of R2-, R3- third methane synthetic reaction
Device, the 4th methane synthesis reactor of R4-, P1- recycle compressor, E1- gas-gas heat exchanger, E2- water cooler, F1- release pneumatically
Valve, v1- liquid separation tank.
Specific embodiment
By following embodiment combination attached drawings, the present invention will be described in detail.
Embodiment 1
According to process flow shown in Fig. 1, pressure 1.0MPa, air speed 10000h-1Virgin gas A form (vol%) are as follows: H2
67.08 CH49.2, CO 21.17, CO22.05 N20.5.Virgin gas with after circulating air mixes formed unstripped gas enter first
Methane synthesis reactor entrance, gas inlet temperature are 280 DEG C, and temperature is 680 DEG C after reaction.First methane synthesis reactor bed
Layer reaction warm area is 670 DEG C ~ 680 DEG C from top to bottom, and the first methane synthesis reactor outlet is divided into two strands: a part of gas enters
It is returned to after the first methane synthesis reactor entrance is mixed with virgin gas A after recycle compressor P1 boosting as circulating air and forms raw material
Gas；Another strand of gas enters the second methane synthesis reactor R2, and temperature rises to 420 DEG C after reaction, and two anti-outlets are changed through E1 gas gas
It exchanges heat after E2 water cooler cooling water dividing using E1 after heat, is into third methane synthesis reactor R3 inlet temperature
280 DEG C, temperature rises to 285 DEG C after reaction, and three instead go out after Gas Cooler exchanges heat to be cooled to about 150 DEG C into four anti-R4 entrances, warp
Product gas liquid separation tank removes condensed water, then the SNG for obtaining content 96% to 40 DEG C through product gas end cooler cooling down is delivered to pipe
Net.
Embodiment 2
According to process flow shown in Fig. 1, pressure 5.5MPa, air speed 20000h-1Virgin gas form (vol%) are as follows: H2
69.5 CH48.21, CO 19.84, CO21.95 N2 0.5.Virgin gas with form unstripped gas after circulating air mixes and enter the
One methane synthesis reactor entrance, gas inlet temperature are 280 DEG C, and temperature is 695 DEG C after reaction.First methane synthesis reactor
Bed react warm area be from top to bottom 680 DEG C ~ 695 DEG C, the first methane synthesis reactor outlet is divided into two strands: a part of gas into
It is used as circulating air to return to formation original after the first methane synthesis reactor entrance is mixed with virgin gas A after entering recycle compressor P1 boosting
Expect gas；Another strand of gas enters the second methane synthesis reactor R2, and temperature rises to 430 DEG C after reaction, and two anti-outlets are through E1 gas gas
It exchanges heat after E2 water cooler cooling water dividing using E1 after heat exchange, into third methane synthesis reactor R3 inlet temperature
It is 280 DEG C, temperature rises to 285 DEG C after reaction, and about 160 DEG C, which are cooled to, after the three anti-heat exchange of Gas Cooler out enters four anti-R4 entrances,
Condensed water is removed through product gas liquid separation tank, then the SNG for obtaining content 97% to 40 DEG C through product gas end cooler cooling down is delivered to
Pipe network.
Embodiment 3
According to process flow shown in Fig. 1, pressure 8MPa, air speed 30000h-1Virgin gas form (vol%) are as follows: H268.5,
CH48.82, CO 20.23, CO21.95 N2 0.5.Virgin gas with after circulating air mixes formed unstripped gas enter the first methane
Synthesis reactor entrance, gas inlet temperature are 280 DEG C, and temperature is 685 DEG C after reaction.First methane synthesis reactor bed is anti-
Answering warm area from top to bottom is 675 DEG C ~ 685 DEG C, and the first methane synthesis reactor outlet is divided into two strands: a part of gas enters circulation
It is returned to after the first methane synthesis reactor entrance is mixed with virgin gas A after compressor P1 boosting as circulating air and forms unstripped gas；
Another strand of gas enters the second methane synthesis reactor R2, and temperature rises to 430 DEG C after reaction, and two anti-outlets are after E1 gas-gas heat exchange
It exchanges heat after E2 water cooler cooling water dividing using E1, is 280 into third methane synthesis reactor R3 inlet temperature
DEG C, temperature rises to 285 DEG C after reaction, and three instead go out after Gas Cooler exchanges heat to be cooled to about 160 DEG C into four anti-R4 entrances, through product
Gas liquid separation tank removes condensed water, then the SNG for obtaining content 96% to 40 DEG C through product gas end cooler cooling down is delivered to pipe network.
Embodiment 4
According to process flow shown in Fig. 1, pressure 8MPa, air speed 30000h-1Virgin gas form (vol%) are as follows: H268.5,
CH48.82, CO 20.23, CO21.95 N2 0.5.Virgin gas with after circulating air mixes formed unstripped gas enter the first methane
Synthesis reactor entrance, gas inlet temperature are 280 DEG C, and temperature is 685 DEG C after reaction.First methane synthesis reactor bed is anti-
Answering warm area from top to bottom is 675 DEG C ~ 685 DEG C, and the first methane synthesis reactor outlet is divided into two strands: a part of gas enters circulation
It is returned to after the first methane synthesis reactor entrance is mixed with virgin gas A after compressor P1 boosting as circulating air and forms unstripped gas；
Another strand of gas enters the second methane synthesis reactor R2, and recycle compressor is stopped 5 minutes, the small flow starting of falling bleeder valve,
First methane synthesis reactor temperature rises to 700 DEG C from 685 DEG C.Device parking, leads to N2Displacement, there is no the safety that overtemperature causes
Hidden danger.
Claims (8)
1. a kind of methanation process of coal based synthetic gas preparation synthetic natural gas, it is characterised in that: including following technical process: from
The methane synthesis gas that gas purification workshop section comes obtains virgin gas after fine de-sulfur, and virgin gas passes sequentially through four concatenated insulation
Methanator；Virgin gas is divided into gas A and gas B by the outlet of the first methane synthesis reactor after cooling, gas A into
Enter to return to after the first methane synthesis reactor entrance is mixed with virgin gas after recycle compressor boosts as circulating air and forms raw material
Gas, gas B sequentially enter second, third, the 4th methane synthesis reactor carry out methane synthetic reaction；The first methane synthesis
Pneumatic operated valve of releasing is installed at reactor inlet；Second methane synthesis reactor, which is worked off one's feeling vent one's spleen, carries out turnout reason, and bismethane is closed
It exchanges heat again with itself gas at after reactor outlet gas cooling water dividing, the dry gas after dividing water enters back into the conjunction of third methane
At reactor；Methane contents on dry basis is greater than 96% in 4th methane synthesis reactor exit gas, then obtains through cooling, dehydration
Satisfactory synthetic natural gas SNG.
2. the methanation process of coal based synthetic gas preparation synthetic natural gas according to claim 1, it is characterised in that: described
First methane synthesis reactor is adopting heat pipes for heat transfer radial bed methanator.
3. the methanation process of coal based synthetic gas preparation synthetic natural gas according to claim 1, it is characterised in that: described
In reactor with dry gas calculate volume space velocity be 5000h-1~30000h-1, pressure is 1 ~ 8MPa.
4. the methanation process of coal based synthetic gas preparation synthetic natural gas according to claim 1, it is characterised in that described
First methane synthesis reactor inlet temperature be 250 DEG C ~ 300 DEG C, outlet temperature be 600 DEG C ~ 700 DEG C, second, third, the 4th
Methane synthesis reactor inlet temperature is 250 DEG C ~ 300 DEG C, and the second methane synthesis reactor outlet temperature is 500 DEG C ~ 650 DEG C,
Third methane synthesis reactor outlet temperature is 400 DEG C ~ 500 DEG C, and the 4th methane synthesis reactor outlet temperature is 250 DEG C ~ 350
℃。
5. the methanation process of coal based synthetic gas preparation synthetic natural gas according to claim 1, it is characterised in that gas A
Temperature into recycle compressor is 30 DEG C ~ 80 DEG C.
6. the methanation process of coal based synthetic gas preparation synthetic natural gas according to claim 1, it is characterised in that methane
Synthetic catalyst is using nickel as main active component, with one of boehmite, aluminium oxide, magnesia, magnesium aluminate spinel
Or two kinds are carrier.
7. the methanation process of coal based synthetic gas preparation synthetic natural gas according to claim 6, it is characterised in that described
Catalyst is aided with the first, second auxiliary agent using nickel as main active component, prepares reactive precursor using the precipitation method；First auxiliary agent is
One or both of transition metal element, including La, Ce, Zr, Ti, content are the 0.1-5% of Ni mass；Second auxiliary agent is three
Ethylhexyl phosphoric acid, methyl anyl alcohol, cellulose derivative, polyacrylamide, guar gum, ethylene glycol, gathers at lauryl sodium sulfate
One or both of dispersing agents such as ethylene glycol, fatty acid polyethylene glycol ester, glycerol replace when precipitating conventional water as dispersing agent
It uses, usage amount is the 0.01-1% of Ni dosage.
8. the methanation process of coal based synthetic gas preparation synthetic natural gas according to claim 6, it is characterised in that catalysis
Agent carrier is made of the complex salt of aluminium oxide and aluminium, magnesium, and wherein aluminium oxide is with γ-Al2O3Or δ-Al2O3Or α-Al2O3Form is deposited
The complex salt of aluminium and magnesium is with MgAl2O4Form exists.
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Cited By (2)
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| CN111635796A (en) * | 2020-06-22 | 2020-09-08 | 成都赛普瑞兴科技有限公司 | A natural gas synthesis process and equipment for synthesizing natural gas |
| CN114349602A (en) * | 2020-10-12 | 2022-04-15 | 中石化南京化工研究院有限公司 | Process for synthesizing low-carbon mixed alcohol with coal-to-synthesis gas as raw material and tandem methanation |
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| CN109207220B (en) | 2020-10-30 |
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Address after: Liuhe District of Nanjing City, Jiangsu province 210048 geguan Road No. 699 Patentee after: China Petroleum & Chemical Corp. Patentee after: SINOPEC NANJING CHEMICAL RESEARCH INSTITUTE Co.,Ltd. Address before: Liuhe District of Nanjing City, Jiangsu province 210048 geguan Road No. 699 Patentee before: China Petroleum & Chemical Corp. Patentee before: Nanhua Group Research Institute |
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