CN106957694A - A kind of supercritical carbon dioxide soaks the preparation method of the double carbon source fuel of molten coal slurry - Google Patents
A kind of supercritical carbon dioxide soaks the preparation method of the double carbon source fuel of molten coal slurry Download PDFInfo
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/46—Gasification of granular or pulverulent flues in suspension
- C10J3/466—Entrained flow processes
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- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0903—Feed preparation
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0903—Feed preparation
- C10J2300/0906—Physical processes, e.g. shredding, comminuting, chopping, sorting
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0913—Carbonaceous raw material
- C10J2300/093—Coal
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- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0959—Oxygen
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0969—Carbon dioxide
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0973—Water
- C10J2300/0976—Water as steam
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0983—Additives
- C10J2300/0986—Catalysts
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/54—Improvements relating to the production of bulk chemicals using solvents, e.g. supercritical solvents or ionic liquids
Abstract
A kind of supercritical carbon dioxide soaks the preparation method of the double carbon source fuel of molten coal slurry, comprises the following steps：（1）The modified coal dust of system：Ratio by composite modifier in raw coal quality than 0.5~8% is added in raw coal or is injected directly into coal mill, is mixed together grinding, modified coal dust is made；（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：Modified coal dust is placed in pressure vessel, temperature is not less than 5 DEG C, not higher than 50 DEG C in control container, uses supercritical CO2Molten modified coal dust is directly soaked, quality of pc is produced than the supercritical CO for 68~88%2Soak the double carbon source fuel of molten coal slurry；（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry.The inventive method is simple, is transformed using existing dry or wet process system, and operating cost can be greatly reduced with existing ripe gasification process in Bian, effectively reduces gas purification and the removing CO of existing gasification system2Cost.
Description
Technical field
The present invention relates to clean energy technology field, and in particular to a kind of supercritical CO2Soak the double carbon source fuel of molten coal slurry
Preparation method.
Background technology
Coal gasification refers in making the organic matter in coal and gasifying agent occur series of chemical under uniform temperature and pressure,
Solid coal is converted into the process of lime-ash and imflammable gas.According to used gasifying agent difference (air, pure oxygen, oxygen-enriched air,
Vapor, carbon dioxide etc.) and gasification process difference, the gas composition of output is different.Coal gasifying process is with as-fired coal in stove
Interior process dynamics can be divided into moving bed (fixed bed) gasification, fluidized gasification, entrained flow gasification and molten bath gasifica tion technique etc..
The development trend of current Coal Gasification Technology is to replace beans with fine coal, and fixed bed is replaced with air flow bed and fluid bed, especially by
The referred to as entrained flow gasification method of high effect cleaning coal gasification method, and to high-pressure trend（8.5MPa）And high temperature（1500~
1600℃）Gasify and gasifying agent diversified development, and deslagging mode develops to liquefied.
Entrained flow gasification method be the fines using particle diameter ＜ 0.1mm as raw material, it is including dry by raw material of superfine coal dust
Method technique and the wet processing two types by raw material of water-coal-slurry.Dry and wet technique is both steamed with oxygen, overheat
Vapour is gasifying agent, and is gasified using parallel type or the gasification that suspends, with nozzle by oxygen, superheated steam（Gasifying agent）Sprayed into coal dust
Gasification furnace reative cell.In-furnace temperature is up to 1400 DEG C ~ 2000 DEG C, and coal dust enters stove i.e. moment and caught fire, and reaction is quick, the intensity of gasification
Height, almost occurs pyrolysis, burning and occurs combustion reaction and gasification reaction with gasifying agent, a step changes into CO, H simultaneously2 、
CO2Deng gas.Because of hot conditions, tar, phenol and hydro carbons are free of in gasification gas（It is practically free of liquid hydrocarbon and CH4）, CO contains
Amount up to 58% ~ 62%, is secondly H2、CO2Deng major impurity is H2S and a small amount of COS.
The main distinction of dry and wet entrained flow gasification method is that on the feed-type of gasification furnace fuel, dry method is first by raw coal
Coal dust is made in grinding, then, and coal dust is directly sprayed into stove with Geldart-D particle to nozzle, representational such as K-T gasification furnaces, shell
Board stove（Shell, SCGP, pressurization K-T）, GSP stoves etc.；Wet method is first to mix raw coal and the auxiliary agent such as water and emulsifying agent, friction reducer
Grinding is made water-coal-slurry, or raw coal grinding first is made into coal dust, then adds the auxiliary agents such as emulsifying agent, friction reducer, is mixed through high-speed stirred
Water-coal-slurry is made, then, is pumped to nozzle and sprays into stove, it is representational to have Texaco's coal slurry gasifier (Texaco, GE), its
Using the water-coal-slurry of 60% ~ 65% concentration as feeding manner, gasifying agent is made with pure oxygen, the oxygen consumption needed for gasification is 1kg O2/ kg is done
Coal, its water-coal slurry pump and nozzle are easy to wear, change frequency height, influence the gasifier operation cycle.Two kinds of processes respectively have feature,
Abrasion of the coal grain to nozzle is all big.Dry method, which is fed, is well suited for the coal and low-order coal of high activity, but its high densification for generally using
Phase flow delivery systems are complicated and discharge pressure is by a definite limitation, and feed and lock device for coal are also more in pressurized conditions failure, coal
Powder conveying technology has become the important restriction factor of dry gasification technology development.The pumping and water-coal-slurry form is easily pressurizeed, can
The problem of solving dry method feed and lock device for coal under an increased pressure, but contained a large amount of moisture content（General moisture content 35~42%）
Gasification absorbs a large amount of latent heats of vaporization, and the thermal efficiency is relatively low, has a strong impact on the overall thermal efficiency and the intensity of gasification of gasification furnace.
The adverse effect caused for reduction large quantity of moisture, has developed polynary slurry gasification technology, i.e., added in water-coal-slurry
Certain heavy oil or crude oil or pitch substitute a part of water in water-coal-slurry, with the carbon containing effecting reaction thing being added in furnace charge slurry
Concentration, raising generates CO, H in coal gas2Content, reduce effective gas（CO+H2）The oxygen and raw material consumption of coal of specific yield.
But oil material need to be consumed and oil pre-emulsification need to be expected, combined grinding energy consumption can be increased and secondary pollution is produced.
Therefore, scientific worker has carried out substantial amounts of research with regard to gasification system and fuel mode of movement both at home and abroad.Wherein have
Chinese patent CN103468320A discloses " a kind of carbon dioxide coal slurry preparation conveying and gasification system, it is characterised in that described
System by water-coal-slurry preparation unit, carbon dioxide coal slurry preparation unit, coal gasification unit, synthesis gas cooling and purifying unit and
Collecting carbonic anhydride separative element is constituted;Described water-coal-slurry preparation unit includes water-coal-slurry preparation vessel, and water-coal-slurry preparation vessel is set
There are coal powder entrance and water inlet, water-coal-slurry preparation vessel is connected by coal slurry pump one with coal slurry displacement slot;..., described dioxy
Change carbon coal slurry prepare conveying and gasification system it is main by water-coal-slurry preparation vessel, water-coal slurry pump, coal slurry displacement slot, coal slurry drain sump,
Coal slurry bubble trap ..., main process is as follows:Coal dust is prepared as normal temperature and pressure water after being mixed in coal slurry industry with water
Coal slurry (coal slurry mass concentration about 60%), reaches 6.0~8.0MPa, temperature remains normal temperature after normal pressure water-coal-slurry is pressurized;
Pressure is pumped into water-coal-slurry displacement slot with water-coal-slurry identical liquid carbon dioxide by liquid carbon dioxide, is carried out with water-coal-slurry
Stirring mixing, most of coal dust will be mixed to form carbon dioxide coal slurry with liquid carbon dioxide, and water is separated and is back to water-coal-slurry
Preparation unit, carbon dioxide coal slurry mass concentration about 30% now is right in order to further improve the concentration of carbon dioxide coal slurry
Carbon dioxide coal slurry is suitably heated, and reduces its pressure value 6.0MPa or so, temperature is reduced to about 25 DEG C, close to titanium dioxide
Carbon gas-liquid two-phase critical point, is filtered carbon dioxide coal slurry upper foam with filter, and the quality for improving carbon dioxide coal slurry is dense
Degree;Carbon dioxide coal slurry is delivered to gasifier nozzle using coal slurry pump from coal slurry groove ... ..., containing highly concentrated in the synthesis gas of purification
The carbon dioxide of degree, by carbon dioxide capture system carry out carbon dioxide and the effective qi leel of synthesis gas from ...." this method
The problem of a large amount of latent heats of vaporization, the reduction thermal efficiency are absorbed to gasification caused by a large amount of moisture content contained by solution water-coal-slurry aspect
Substantially advantage is shown, but be primarily present following problem：
First, the water-coal-slurry of mass ratio about 60% is made in dry pulverized coal of the coal dust sheet ground for dehydration, dry pulverized coal, water-coal-slurry uses two
When carbonoxide displacement is converted into the carbon dioxide coal slurry of mass ratio about 60%, necessarily lead to substantial amounts of CO2Hydrate solids are with ice state
It is present in carbon dioxide coal slurry, the measure such as backflow can not isolate CO2Hydrate solids, had both influenceed the stream of carbon dioxide coal slurry
Dynamic property is likely to result in blocking, and vaporized stove rear CO again2Hydrate solids need to absorb the substantial amounts of latent heat of vaporization；
Second, sweeping along the ultrahigh concentration CO of coal dust particle2（CO2The extinguishing chemical commonly used for fire-fighting）To spray into stove in coal dust
Fiery characteristic, which can be produced, stops up the property put out influence, if the moment a large amount of heat energy of ignition ability sustainable supply without a large amount of coal dusts, gas
The temperature changed in stove can decline rapidly, and its positive effect leaves a question open；
Third, being not directed to CO2As the effecting reaction condition especially catalytic gasification condition of gasifying agent and carbon, coal gas can be caused
In " the CO containing excessive concentrations as described in its specification2", purification and the decarburization cost of coal gas can be significantly increased；
Fourth, the high CO in gasification gas as used in the description2Corresponding CO, H in concentration, coal gas2Ratio declines to a great extent, i.e. coal
Makings amount and coal gas heat energy decline, and have objectively had influence on the efficiency of gasification furnace；
Fifth, dry pulverized coal is prepared into common coal water slurry fuel first, the waste of the costs such as water and auxiliary agent is caused, is added big
Amount is dissolved with the waste water of noxious pollutant, causes secondary pollution；
Sixth, water-coal-slurry is forced into 6.0~8.0MPa, liquid carbon dioxide is stirred with water-coal-slurry and mixed, dehydration,
Separation backflow, obtains the carbon dioxide coal slurry of about 30% concentration, then carbon dioxide coal slurry is suitably heated, will with filter
Carbon dioxide coal slurry upper foam is filtered, and improves the quality of carbon dioxide coal slurry, and more than complex procedures, equipment are more, invest big,
For critical-temperature be 31.06 DEG C, critical pressure 7.382MPa, critical density 468kg/m3CO2For medium, equipment technology
Difficulty and energy consumption are significantly larger than the transportation problem of dry pulverized coal.
To solve superelevation solubility CO2Effect of burying in oblivion to entering gasification furnace coal dust, the ADL companies in the U.S.（Arthur D
little lnc）Using the CO of liquid2Substitution water and coal slurry are mixed and made into CO2During coal slurry, in the terminal of conveyance conduit, by setting
Putting fibrous filter makes CO2Volatilization and by coal dust and CO2Separate, the coal dust separated is dry, can be entered immediately
Row burning, the CO separated2Recycle, but need flash chamber and expensive fabric filter is set.
In order to further play the advantage of entrained flow gasification method, resolve fuel transportation problem, mitigate wearing and tearing, greatly for nozzle
Width improves the overall thermal efficiency and the intensity of gasification and the green clean energy technology for realizing emission reduction of gasification furnace, in the urgent need to opening
The technical method that to send out a kind of brand-new.
The content of the invention
The technical problem to be solved in the present invention is to overcome the deficiencies in the prior art simple there is provided a kind of technique, without secondary dirt
Dye, environmental protection, the supercritical carbon dioxide for being adapted to existing airflow bed gasification furnace soaks the preparation method of the double carbon source fuel of molten coal slurry.
The technical scheme that the present invention solves the use of its technical problem is that a kind of supercritical carbon dioxide soaks the double carbon sources of molten coal slurry
The preparation method of fuel, uses CO2A part of oxygen and feed coal are substituted, the carbon of gasification furnace is used as using coal dust carbon and carbon dioxide simultaneously
Source, can improve the catalysis burning-rate accelerator of coal powder ignition performance and improve CO2Catalytic gasification agent with coal dust reactivity is as multiple
Close modifying agent and produce modified coal dust, with supercritical CO2Leaching is miscible to close modified coal dust, be made quality of pc than for 68~88% it is super
Critical CO2The double carbon source fuel of molten coal slurry are soaked, are conveyed with high-pressure coal pulp pump, air flow bed gas is together sprayed into superheated steam, oxygen etc.
Change and mixing gasifying reaction is carried out in stove, it specifically includes following steps：
（1）The modified coal dust of system：
Using existing/ripe coal dust technique processed, during grinding coal dust, composite modifier is pressed into raw coal quality ratio
0.5~8% ratio is added in raw coal or is injected directly into coal mill, is mixed together grinding, is made with coal grain as composite modifier
The mixed and modified coal dust of carrier；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
By step（1）The mixed and modified coal dust of gained is placed in pressure vessel, and temperature is not less than 5 DEG C, not higher than 50 in control container
DEG C, use supercritical CO2Directly soak miscible close and be modified coal dust, produce quality of pc than the supercritical CO for 68~88%2Soak molten coal slurry
Double carbon source fuel；
（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry：
With reference to existing wet method fuel feedstock process, by step（2）Gained supercritical CO2The double carbon source fuel of molten coal slurry are soaked to use
Coal slurry pump is conveyed, and is together sprayed into superheated steam, oxygen etc. through gasification burner tip and mixing gasifying reaction is carried out in airflow bed gasification furnace.
Further, the composite modifier selects commercially available catalysis burning-rate accelerator, catalytic gasification agent, is in mass ratio catalysis burning-rate accelerator
10~60%, used after the ratio of catalytic gasification agent 40~90% is compound；Or from catalysis burning-rate accelerator, catalytic gasification agent directly by than
Example addition is used；Or directly used from the marketable material for thering is catalytic combustion-supporting and catalytic gasification to act on.
Further, described catalysis burning-rate accelerator, which refers to, is effective against pure CO2Bury in oblivion effect, in CO2High temperature can be borrowed in environment
Ignite the catalyst or combustion adjuvant or catalysis oxidation combustion adjuvant containing active oxygen and/or ionic catalysis oxidation effect of coal dust；Such as weight
Chromic acid ammonia, ammonium metavanadate, ZC-7 types catalytic combustion adjuvant for coal, ZC-9 types catalytic combustion adjuvant for coal, ZC-19 moulded coal catalytic combustion-supportings
At least one in agent, ZC-11 type catalytic combustion adjuvant for coal etc.；Catalysis burning-rate accelerator consumption is the 0.03~3% of raw coal quality（It is excellent
Select 0.1~1.5%）.
Further, described catalytic gasification agent refers to can improve coal dust carbon and CO in more than 800 DEG C2Reactivity, promote
Coal dust carbon and CO2Reaction generation CO material；Compound preferably containing elements such as lithium, potassium, vanadium, nickel, chromium, manganese, strontium, cerium, lanthanums；
As carbonyl ferronickel, salicylic acid cerium, the agent of ZC-G3 type catalytic gasifications, the agent of ZC-G5 type catalytic gasifications, the agent of ZC-G13 type catalytic gasifications,
At least one in ZC-G7 type catalytic gasification agent etc., catalytic gasification agent consumption be raw coal quality than 0.47~5%（It is preferred that 0.5
~3%）.
The know-why of the present invention：
1）By CO2As a kind of carbon source, a part of oxygen and feed coal are substituted, meanwhile, utilize supercritical CO2 Density is bordering on liquid,
Viscosity is bordering on gas, and diffusion coefficient is 100 times of liquid, and the solvability to coal dust is strong, can effectively soak molten and softening coal dust
Grain, and good fluidity, the characteristics of transporting resistance is low, by supercritical CO2As the molten medium of the leaching of coal dust and pumped (conveying) medium, resolve
The transportation problem of airflow bed gasification furnace fuel and the easily wear problem of nozzle.
2）Using maturation application or existing coal dust technological equipment system processed, functional composite modifier is directly added
Enter in raw coal/spray into coal mill, be mixed together grinding and be made directly with modified coal dried bean noodles powder of the coal grain for composite modified agent carrier.
3）Anti- by means of catalytic combustion adjuvant for coal buries in oblivion effect, resolves ultrahigh concentration CO2Stopping up for coal dust firing is put out in environment
Problem, it is ensured that by pure CO2The molten coal dust wrapped of leaching is sprayed into gasification furnace can moment ignition in hot environment.
4）Utilize supercritical CO2With dry pulverized coal good " intermiscibility ", with supercritical CO2Leaching is molten to be carried with feature catalysis
The pulverized coal particle of combustion-supporting and catalytic gasification composite modifier, is made gasification furnace supercritical CO2Soak double carbon sources combustion of molten coal dust carbon
Material, coal dust carbon and CO are improved with the agent of feature catalytic gasification2Reactivity, promote coal dust carbon and CO2Fast reaction generates CO,
Reduce effective gas（CO+H2）The oxygen and raw material consumption of coal of specific yield.
5）With reference to the wet method fuel feedstock process of ripe application, by supercritical CO2The double carbon source fuel of molten coal slurry are soaked to use
High-pressure coal pulp pump is conveyed, and is together sprayed into superheated steam, oxygen etc. through gasification burner tip in airflow bed gasification furnace and is carried out mixing gasifying
Reaction.
The present invention has innovated entrained flow bed gasification technology, employs " supercritical CO2Soak molten modified dry pulverized coal, with carbon dioxide
It is crude fuel with coal dust charcoal " the full technical strategies of reaction, reduce effective gas（CO+H2）The oxygen and feed coal of specific yield
Consumption.
The present invention significantly increases an oxygen using the carbon in the carbon and coal dust in supercritical carbon dioxide simultaneously as carbon source
Change the output capacity of carbon.Reaction activity is reduced with feature catalytic gasification technology, selective catalysis CO generation promotes reaction
CO2+ C=2CO under low energy consumption compared with quickly being carried out, and " the pure carbon " contained by 1 kg coal dusts matched can be produced in theory
4.66 kg CO, and the pure carbon of 1 kg is completely converted into CO and can only produce 2.33 kg CO in theory conventional art in theory.Its is excellent
The three kinds of oxidation reaction performance of gesture carbon is as follows：
C+O2 =CO2+409(KJ/mo l)
C+0.5O2=0.5CO+246 (KJ/mol)
C+CO2=2CO-162 (KJ/mol）
The inventive method is simple, is applicable to all kinds of coals, is environmental type coal gas technology.And using existing dry method
Or the wet processing system reform, and can Bian with existing ripe gasification process, operating cost can be greatly reduced, can also effectively
Reduce gas purification and the removing CO of existing gasification system2Cost.
Embodiment
Make further statement with reference to embodiments.
A kind of supercritical CO2The preparation method of the double carbon source fuel of molten coal slurry is soaked, CO is used2As a kind of carbon source substitute a part of oxygen and
Feed coal, meanwhile, utilize supercritical CO2Density is bordering on liquid, and viscosity is bordering on gas, and diffusion coefficient is 100 times of liquid, right
The solvability of coal dust is strong, can effectively soak molten and softening pulverized coal particle, and good fluidity, the characteristics of transporting resistance is low, faces super
Boundary CO2As the molten medium of the leaching of coal dust and pumped (conveying) medium, resolve airflow bed gasification furnace fuel transportation problem and nozzle it is easy
Wear problem；Anti- with catalysis burning-rate accelerator buries in oblivion effect, it is ensured that by pure CO2The molten coal dust wrapped of leaching sprays into high temperature ring in gasification furnace
Can moment ignition in border；With feature catalytic gasification agent selective catalysis CO generation, promote to react CO2+ C=
2CO under low energy consumption compared with quickly carrying out；Using ripe coal dust technological equipment system processed, by functional catalysis burning-rate accelerator and
Catalytic gasification agent composite modifier is directly added into raw coal/sprayed into coal mill, and it is multiple to be mixed together grinding and be made directly with coal grain
Close the modified coal dried bean noodles powder of modification agent carrier；Utilize supercritical CO2With dry pulverized coal good " intermiscibility ", with supercritical CO2Leaching is molten
Mixing carries the pulverized coal particle with feature catalytic combustion-supporting and catalytic gasification composite modifier, is made and is adapted to mesohigh air flow bed
Gasification, quality of pc are than the supercritical CO for 68~88%2The double carbon source fuel of molten coal slurry are soaked, are conveyed with high-pressure coal pulp pump, with overheat
Steam, oxygen etc., which are together sprayed into, carries out mixing gasifying reaction in airflow bed gasification furnace.
Embodiment 1, the present embodiment carries out the preparation and gasification that supercritical CO 2 soaks the double carbon source fuel of molten coal slurry.
Supercritical CO used2Raw material selects commercially available liquid carbon dioxide, purity 99.6%；Raw coal is from commercially available smokeless
Coal, butt volatile matter 7.3%, fixed carbon 65.3%, ash content 27.4%, calorific value Q 5961x4.18KJ/Kg, composite modifier choosing
ZC-G3 type catalytic gasification agent and the catalysis of ZC-7 moulded coals with Hunan Province little Yin Wuji environmental energy Science and Technology Development Co., Ltd.
Combustion adjuvant as coal dust composite modifier.Prepare according to the following procedure and the supercritical CO that gasifies2Soak the double carbon source fuel of molten coal slurry.
（1）The modified coal dust of system：
ZC-7 types catalytic combustion adjuvant for coal according to anthracite quality 0.5%, the agent of ZC-G3 type catalytic gasifications is by anthracite quality
3% with anthracite be mixed together grinding be made 90 μm tail over 18% coal dust, be able to coal grain be composite modified agent carrier modified coal
Powder；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
By step（1）Gained is modified coal dust and is placed in pressure vessel, and 28 DEG C~32 DEG C of temperature, use supercritical CO in control container2
Directly soak miscible close and be modified coal dust, quality of pc is made than the supercritical CO for 82%2Soak the double carbon source fuel of molten coal slurry；
（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry：
The bed burner using triple-channel burner as adjustable experimental wind flow, by step（2）Gained supercritical CO2Soak the double carbon of molten coal slurry
Source fuel is conveyed with high-pressure coal pulp pump, is together sprayed into superheated steam, oxygen etc. through gasification burner tip in experimental wind flow bed gasification furnace,
Control 1450 DEG C~1550 DEG C of the temperature of progress mixing gasifying reaction, pressure 3.1MPa in gasification furnace.
After testing, under gasification furnace stable state, effective gas（CO+H2）：88.6%, compare coal consumption：0.532Kg coals/Nm3（CO+
H2）, than oxygen consumption：0.326Nm3O2/Nm3（CO+H2）, coal dust efficiency of carbon con version：99.6%, CO2 conversion ratio：83.5%.
Embodiment 2, the present embodiment carries out supercritical CO2Soak the preparation and gasification of the double carbon source fuel of molten coal slurry.
Supercritical CO used2Raw material selects commercially available liquid carbon dioxide, and purity 99.6%, raw coal selects half commercially available cigarette
Coal, butt volatile matter 18.4%, fixed carbon 55.8%, ash content 25.8%, calorific value 6137x4.18KJ/Kg, composite modifier choosing
ZC-G5 type catalytic gasification agent and the catalysis of ZC-9 moulded coals with Hunan Province little Yin Wuji environmental energy Science and Technology Development Co., Ltd.
Combustion adjuvant as coal dust composite modifier.Prepare according to the following procedure and the supercritical CO that gasifies2Soak the double carbon source fuel of molten coal slurry.
（1）The modified coal dust of system：
ZC-9 types catalytic combustion adjuvant for coal according to semibituminous coal quality 1.0%, the agent of ZC-G5 type catalytic gasifications is by semibituminous coal quality
4.5% with semibituminous coal be mixed together grinding be made 90 μm tail over 21.4% coal dust, be able to coal grain and changing for composite modified agent carrier
Property coal dust；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
Modified coal dust is placed in pressure vessel, 28 DEG C~32 DEG C of temperature, use supercritical CO in control container2Directly soak miscible conjunction
Modified coal dust, is made quality of pc than the supercritical CO for 78%2Soak the double carbon source fuel of molten coal slurry；
（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry：
The bed burner using triple-channel burner as adjustable experimental wind flow, by supercritical CO2Soak the double carbon source fuel of molten coal slurry high
Coal slurry pump conveying is pressed, is together sprayed into superheated steam, oxygen etc. through gasification burner tip in experimental wind flow bed gasification furnace, controls gasification furnace
Interior 1600 DEG C~1700 DEG C of temperature for carrying out mixing gasifying reaction, pressure 6.5MPa.
After testing, under gasification furnace stable state, effective gas（CO+H2）：89.7%, compare coal consumption：0.506Kg coals/Nm3（CO+
H2）, than oxygen consumption：0.317Nm3O2/Nm3（CO+H2）, coal dust efficiency of carbon con version：99.7%, CO2Conversion ratio：89.1%.
Embodiment 3, the present embodiment carries out supercritical CO2Soak the preparation and gasification of the double carbon source fuel of molten coal slurry.
Supercritical CO used2Raw material selects commercially available liquid carbon dioxide, and purity 99.6%, raw coal selects half commercially available cigarette
Coal, butt volatile matter 18.4%, fixed carbon 55.8%, ash content 25.8%, calorific value 6137x4.18KJ/Kg, composite modifier choosing
With the ZC-G13 type catalytic gasification agent of Hunan Province little Yin Wuji environmental energy Science and Technology Development Co., Ltd. and ZC-19 moulded coals with urging
Change composite modifier of the combustion adjuvant as coal dust.Prepare according to the following procedure and the supercritical CO that gasifies2Soak the double carbon source fuel of molten coal slurry.
（1）The modified coal dust of system：
ZC-19 types catalytic combustion adjuvant for coal according to semibituminous coal quality 1.5%, the agent of ZC-G13 type catalytic gasifications press semibituminous coal quality
1.8% with semibituminous coal be mixed together grinding be made 90 μm tail over 22.3% coal dust, be able to coal grain for composite modified agent carrier
Modified coal dust；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
Modified coal dust is placed in pressure vessel, 30 DEG C~33 DEG C of temperature, use supercritical CO in control container2Directly soak miscible conjunction
Modified coal dust, is made quality of pc than the supercritical CO for 79%2Soak the double carbon source fuel of molten coal slurry；
（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry：
The bed burner using triple-channel burner as adjustable experimental wind flow, by supercritical CO2Soak the double carbon source fuel of molten coal slurry high
Coal slurry pump conveying is pressed, is together sprayed into superheated steam, oxygen etc. through gasification burner tip in experimental wind flow bed gasification furnace, controls gasification furnace
Interior 1800 DEG C~1900 DEG C of temperature for carrying out mixing gasifying reaction, pressure 8.5MPa.
After testing, under gasification furnace stable state, effective gas（CO+H2）：90.1%, compare coal consumption：0.494Kg coals/Nm3（CO+
H2）, than oxygen consumption：0.299Nm3O2/Nm3（CO+H2）, coal dust efficiency of carbon con version：99.8%, CO2Conversion ratio：90.7%.
Embodiment 4, the present embodiment carries out supercritical CO2Soak the preparation and gasification of the double carbon source fuel of molten coal slurry.
Supercritical CO used2Raw material selects commercially available liquid carbon dioxide, and purity 99.6%, raw coal selects commercially available bituminous coal,
Butt volatile matter 31.6%, fixed carbon 45.3%, ash content 23.1%, calorific value 6417x4.18KJ/Kg, composite modifier select lake
The ZC-G7 type catalytic gasification agent of Nan Sheng little Yin Wuji environmental energy Science and Technology Development Co., Ltd. and ZC-11 moulded coal catalytic combustion-supportings
Agent as coal dust composite modifier.Prepare according to the following procedure and the supercritical CO that gasifies2Soak the double carbon source fuel of molten coal slurry.
（1）The modified coal dust of system：
ZC-11 types catalytic combustion adjuvant for coal according to bituminous coal quality 0.9%, the agent of ZC-G7 type catalytic gasifications press bituminous coal quality 2.2%
With bituminous coal be mixed together grinding be made 90 μm tail over 26.4% coal dust, be able to coal grain be composite modified agent carrier modification coal dust；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
Modified coal dust is placed in pressure vessel, 30 DEG C~35 DEG C of temperature, use supercritical CO in control container2Directly soak miscible conjunction
Modified coal dust, is made quality of pc than the supercritical CO for 73%2Soak the double carbon source fuel of molten coal slurry；
（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry：
The bed burner using triple-channel burner as adjustable experimental wind flow, by supercritical CO2Soak the double carbon source fuel of molten coal slurry high
Coal slurry pump conveying is pressed, is together sprayed into superheated steam, oxygen etc. through gasification burner tip in experimental wind flow bed gasification furnace, controls gasification furnace
Interior 1800 DEG C~1900 DEG C of temperature for carrying out mixing gasifying reaction, pressure 8.5MPa.
After testing, under gasification furnace stable state, effective gas（CO+H2）：89.5%, compare coal consumption：0.495Kg coals/Nm3（CO+
H2）, than oxygen consumption：0.301 Nm3O2/Nm3（CO+H2）, coal dust efficiency of carbon con version：99.7%, CO2 conversion ratio：92.6%.
Embodiment 5, the present embodiment carries out supercritical CO2Soak the preparation and gasification of the double carbon source fuel of molten coal slurry.
Supercritical CO used2Raw material selects commercially available liquid carbon dioxide, and purity 99.6%, raw coal selects commercially available bituminous coal,
Butt volatile matter 31.6%, fixed carbon 45.3%, ash content 23.1%, calorific value 6417x4.18KJ/Kg, composite modifier select water
Poplar acid cerium, ammonium bichromate as coal dust composite modifier.Prepare according to the following procedure and the supercritical CO that gasifies2Soak the double carbon of molten coal slurry
Source fuel.
（1）The modified coal dust of system：
Composite modifier salicylic acid cerium, ammonium dichromate are mixed in 0.9% and 1.5% ratio of bituminous coal quality together with bituminous coal respectively
Close grinding be made 90 μm tail over 20.4% coal dust, be able to coal grain be composite modified agent carrier modification coal dust；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
Modified coal dust is placed in pressure vessel, 30 DEG C~35 DEG C of temperature, use supercritical CO in control container2Directly soak miscible conjunction
Modified coal dust, is made quality of pc than the supercritical CO for 76%2Soak the double carbon source fuel of molten coal slurry；
（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry：
The bed burner using triple-channel burner as adjustable experimental wind flow, by supercritical CO2Soak the double carbon source fuel of molten coal slurry high
Coal slurry pump conveying is pressed, is together sprayed into superheated steam, oxygen etc. through gasification burner tip in experimental wind flow bed gasification furnace, controls gasification furnace
Interior 1900 DEG C~2000 DEG C of temperature for carrying out mixing gasifying reaction, pressure 10MPa.
After testing, under gasification furnace stable state, effective gas（CO+H2）：90.7%, compare coal consumption：0.445Kg coals/Nm3（CO+
H2）, than oxygen consumption：0.293 Nm3O2/Nm3（CO+H2）, coal dust efficiency of carbon con version：99.9%, CO2Conversion ratio：92.8%.
Comparative example 1, without using composite modifier, carries out supercritical CO2Soak the preparation and gasification of the double carbon source fuel of molten coal slurry.
Supercritical CO used2Raw material selects commercially available liquid carbon dioxide, purity 99.6%, and raw coal is from commercially available smokeless
Coal, butt volatile matter 7.3%, fixed carbon 65.3%, ash content 27.4%, calorific value Q 5961x4.18KJ/Kg, without using catalysis gas
Agent and catalysis burning-rate accelerator as coal dust composite modifier.Prepare according to the following procedure and the supercritical CO that gasifies2Soak molten coal slurry combustion
Material.
（1）Coal dust processed：By anchracite duff be milled into 90 μm tail over 17% coal dust；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
Coal dust is placed in pressure vessel, 28 DEG C~32 DEG C of temperature, use supercritical CO in control container2Directly soak molten Mixture Density Networks
Powder, is made quality of pc than the supercritical CO for 82%2Soak the double carbon source fuel of molten coal slurry；
（3）Supercritical CO2Soak the gasification of molten coal slurry fuel：
Temperature in the bed burner using triple-channel burner as adjustable experimental wind flow, the first stable gasification furnace of log oil is to 1500 DEG C
~1550 DEG C, pressure 3.1MPa, then, by supercritical CO2Molten coal slurry fuel is soaked to be conveyed with high-pressure coal pulp pump, with superheated steam,
Oxygen etc. is together sprayed into experimental wind flow bed gasification furnace through gasification burner tip, and rapid drop in temperature in gasification furnace sprays into diesel oil repeatedly
It is combustion-supporting, the temperature stabilization in gasification furnace still can not be effectively controlled at 1450 DEG C~1550 DEG C, and diesel oil is only sprayed at the same time and oxygen amount is sprayed
Increase by 175%（Compared with embodiment 1）Shi Caineng equilibrium temperatures.
This experiment is shown：The CO of ultrahigh concentration2There is obvious stop up to put out effect, seriously hinder the moment ignition energy of coal dust
Power.Effect need to be buried in oblivion by means of the anti-of catalytic combustion adjuvant for coal, ultrahigh concentration CO is resolved2Coal dust firing stops up the problem of putting out in environment,
Just it can ensure that by pure CO2The molten coal dust wrapped of leaching is sprayed into gasification furnace can moment ignition in hot environment.
Claims (10)
1. a kind of supercritical carbon dioxide soaks the preparation method of the double carbon source fuel of molten coal slurry, it is characterised in that comprise the following steps：
（1）The modified coal dust of system：
During grinding coal dust, the ratio by composite modifier in raw coal quality than 0.5~8% adds in raw coal or straight
Connect in penetrating coal mill, be mixed together grinding, the mixed and modified coal dust for composite modified agent carrier with coal grain is made；
（2）Supercritical CO processed2Soak the double carbon source fuel of molten coal slurry：
By step（1）The mixed and modified coal dust of gained is placed in pressure vessel, and temperature is not less than 5 DEG C, not higher than 50 in control container
DEG C, use supercritical CO2Directly soak miscible close and be modified coal dust, produce quality of pc than the supercritical CO for 68~88%2Soak molten coal slurry
Double carbon source fuel；
（3）Supercritical CO2Soak the gasification of the double carbon source fuel of molten coal slurry：
With reference to wet method fuel feedstock process, by step（2）Gained supercritical CO2Soak the double carbon source fuel coal stock pumps of molten coal slurry
Conveying, together sprays into through gasification burner tip with superheated steam, oxygen and mixing gasifying reaction is carried out in airflow bed gasification furnace.
2. supercritical carbon dioxide as claimed in claim 1 soaks the preparation method of the double carbon source fuel of molten coal slurry, it is characterised in that
The composite modifier selects catalysis burning-rate accelerator, catalytic gasification agent, is in mass ratio catalysis burning-rate accelerator 10~60%, catalytic gasification
Used after the ratio of agent 40~90% is compound；Or directly addition is used in proportion from catalysis burning-rate accelerator, catalytic gasification agent；Or choosing
Directly used with the raw material for thering is catalytic combustion-supporting and catalytic gasification to act on.
3. supercritical carbon dioxide as claimed in claim 1 or 2 soaks the preparation method of the double carbon source fuel of molten coal slurry, its feature exists
In described catalysis burning-rate accelerator, which refers to, is effective against pure CO2Bury in oblivion effect, in CO2Can ignite the containing of coal dust in environment by means of high temperature
Active oxygen and/or the catalyst of ionic catalysis oxidation effect, combustion adjuvant or catalysis oxidation combustion adjuvant.
4. supercritical carbon dioxide according to claim 3 soaks the preparation method of the double carbon source fuel of molten coal slurry, its feature exists
In described catalysis burning-rate accelerator is ammonium bichromate, ammonium metavanadate, ZC-7 types catalytic combustion adjuvant for coal, ZC-9 moulded coals are helped with catalysis
Fire at least one in agent, ZC-19 types catalytic combustion adjuvant for coal, ZC-11 type catalytic combustion adjuvant for coal.
5. the supercritical carbon dioxide according to claim 3 or 4 soaks the preparation method of the double carbon source fuel of molten coal slurry, its feature
Be, the catalysis burning-rate accelerator consumption be raw coal quality than 0.03~3%.
6. supercritical carbon dioxide according to claim 5 soaks the preparation method of the double carbon source fuel of molten coal slurry, its feature exists
In, the catalysis burning-rate accelerator consumption be raw coal quality than 0.1~1.5%.
7. supercritical carbon dioxide as claimed in claim 1 or 2 soaks the preparation method of the double carbon source fuel of molten coal slurry, its feature exists
In described catalytic gasification agent refers to can improve coal dust carbon and CO in more than 800 DEG C2Reactivity, promote coal dust carbon and CO2Instead
CO material should be generated.
8. supercritical carbon dioxide according to claim 7 soaks the preparation method of the double carbon source fuel of molten coal slurry, its feature exists
In, described catalytic gasification agent be containing lithium, potassium, vanadium, nickel, chromium, manganese, strontium, cerium, lanthanum element compound.
9. supercritical carbon dioxide as claimed in claim 7 soaks the preparation method of the double carbon source fuel of molten coal slurry, it is characterised in that
Described catalytic gasification agent is carbonyl ferronickel, salicylic acid cerium, the agent of ZC-G3 type catalytic gasifications, the agent of ZC-G5 type catalytic gasifications, ZC-
At least one in the agent of G13 type catalytic gasifications, ZC-G7 type catalytic gasification agent.
10. supercritical carbon dioxide as claimed in claim 7 soaks the preparation method of the double carbon source fuel of molten coal slurry, its feature exists
In, the catalytic gasification agent consumption be raw coal quality than 0.47~5%.
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| US3976443A (en) * | 1974-12-18 | 1976-08-24 | Texaco Inc. | Synthesis gas from solid carbonaceous fuel |
| CN102080004A (en) * | 2009-11-27 | 2011-06-01 | 中国科学院过程工程研究所 | Biological oil-coal slurry and method for preparing gas from same |
| CN105349183A (en) * | 2015-11-06 | 2016-02-24 | 中国科学院山西煤炭化学研究所 | Method and device for preparing active carbon and byproducts of combustion gas and tar through conversion of coal in supercritical water |
| CN106635172A (en) * | 2015-11-04 | 2017-05-10 | 神华集团有限责任公司 | Jet assembly, multi-burner gasifier and feeding system thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3976443A (en) * | 1974-12-18 | 1976-08-24 | Texaco Inc. | Synthesis gas from solid carbonaceous fuel |
| CN102080004A (en) * | 2009-11-27 | 2011-06-01 | 中国科学院过程工程研究所 | Biological oil-coal slurry and method for preparing gas from same |
| CN106635172A (en) * | 2015-11-04 | 2017-05-10 | 神华集团有限责任公司 | Jet assembly, multi-burner gasifier and feeding system thereof |
| CN105349183A (en) * | 2015-11-06 | 2016-02-24 | 中国科学院山西煤炭化学研究所 | Method and device for preparing active carbon and byproducts of combustion gas and tar through conversion of coal in supercritical water |
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