CN101781576A - Method for preparing liquid fuel by carbon dioxide - Google Patents
Method for preparing liquid fuel by carbon dioxide Download PDFInfo
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- CN101781576A CN101781576A CN201010116718A CN201010116718A CN101781576A CN 101781576 A CN101781576 A CN 101781576A CN 201010116718 A CN201010116718 A CN 201010116718A CN 201010116718 A CN201010116718 A CN 201010116718A CN 101781576 A CN101781576 A CN 101781576A
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- liquid fuel
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- carbonic acid
- acid gas
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Abstract
The invention provides a method for preparing liquid fuel by carbon dioxide; the method comprises the following steps: carbon dioxide, air and steam are reacted at 600-1300 DEG C with (10-1): (1-0): (1-0.1) of volume ratio under the pressure, so as to prepare crude synthesis gas; and the synthesis gas is washed and dedusted to obtain the synthesis gas (H2/CO); carbon monoxide conversion reaction is carried out at 100-300 DEG C and 0.56.0Mpa of pressure with 0.5-2 of mole ratio of H2/CO under the condition that the using amount of sediment iron catalyst is 0.1-0.5 percent of mass of carbon monoxide, so as to prepare the liquid fuel; and quality improvement is carried out to the obtained liquid fuel to obtain gasoline and diesel.
Description
Technical field
The present invention relates to a kind of method of preparing liquid fuel by carbon dioxide, relate in particular to a kind of carbon dioxide reduction and be carbon monoxide and generate synthetic gas that the novel method of funds-Tuo catalysis synthetic liquid fuel belongs to new forms of energy environmental protection field capture.
Background technology
The CO2 emissions increase is the root that causes terrestrial climate to warm in the atmosphere.The survey showed that for of International Energy Agency, and 2007, U.S.'s CO2 emissions occupied first place in the world, and year is the about 20t of CO2 emissions per capita, and the carbonic acid gas of discharging accounts for 23.7% of global total amount.China year per capita CO2 emissions be 2.51 tons, account for 13.6% of global total amount.
The Greenhouse effect aggravation that carbonic acid gas is facilitated is the global environmental problem that surmounts the border.If the whole world more than the 60 hundred million average CO2 emissions of population reached industrialized country's level of nineteen ninety in 2010, the earth will be difficult to bear the serious consequence that the Greenhouse effect aggravation is brought so.Therefore, no matter be developing country, or developed country, its Economic development can not be a cost to sacrifice the global environment that the mankind depend on for existence all.
Carbonic acid gas is greenhouse gases, jeopardizes the human living space, and according to statistics, in world's all trades and professions, the CO2 emissions of power station, Building Materials Factory and Steel Plant's three big industries has surpassed 96% of total emission volumn, becomes the main source of carbonic acid gas.Treat but should only not be used as pollutent to carbonic acid gas, and should be as a kind of abundant available stock, this is only the result that human hope is seen.
The carbonic acid gas tradition utilizes approach to have substantially: preservation agent, system soda pop, process gas fertilizer (being used in greenhouse crops), the hydrogenation of making extraction agent, refrigeration agent, welding protecting agent, vegetables and melon and fruit produce methyl alcohol, dme, methane or other hydro carbons, with the propylene oxide synthetizing propylene carbonate, with the direct synthesizing carbonate ester and then aggregate into polycarbonate of alcohol, in addition carbonic acid gas can be used for the petroleum drilling huff and puff oil recovery, as oil-displacing agent etc.
So far, only 100,000,000 tons of the utilizations of global annual carbonic acid gas, with respect to 20,000,000,000 tons quantity discharged, utilization ratio only is 0.5%.In recent years, the whole world proposes two kinds of solutions to the public hazards that carbonic acid gas causes: the one, and buried, the 2nd, fill out the sea.But these methods are cured the symptoms, not the disease, and fundamentally do not solve the pollution problem of carbonic acid gas.For this reason, scientists must find a kind of method that can utilize carbonic acid gas to promote the well-being of mankind in a large number.
In recent years, scientists is devoted to the research of catalytic hydrogenation of carbon dioxide prepare liquid fuel.This technology makes ecotope form a benign cycle framework in case breakthrough just can become a kind of resource that promotes the well-being of mankind with more than one hundred million tons, billions of tons, tens billion of tons carbonic acid gas.
The chemically reactive of carbonic acid gas is much smaller than carbon monoxide, though high temperature, high-pressure hydrogenation catalysis can the Generation Liquid fluid fuels, transformation efficiency is lower, some countries studies show that in recent years, liquid fuel productive rate only 10%～13% the highlyest is no more than 16%, can not realize industrialization far away.U.S. Pat 2005043417 is utilized rich CO
2Sweet natural gas adds the synthesis gas reaction device and makes synthetic gas, imports the Fischer-Tropsch reaction device and synthesizes, isolates lightweight oil.CO has been developed at the synthetic center of South Africa Witwatersrand university material and process
2And H
2The technology of direct synthetic liquid fuel.Using plasma conversion methane has been studied by China University Of Tianjin and carbonic acid gas prepares gasoline technology (ZL00135863.4).But, United States Patent (USP) (US2005043417) is to mix CO in Sweet natural gas
2Produce synthetic gas, CO
2Utilization ratio lower, South Africa CO
2And H
2Directly synthetic liquid fuel technology consumption heat energy is too high, and the liquid fuel production cost is high too, and Chinese University Of Tianjin plasma-converted technology is difficult to realize large-scale commercial production.
Summary of the invention
For overcoming the low defective of carbon dioxide conversion in the prior art, the invention provides a kind of method by preparing liquid fuel by carbon dioxide, this method comprises:
(1) under certain temperature and pressure, make carbonic acid gas and water vapour, perhaps carbonic acid gas, air and water vapour are by the carbon reduction layer, so that make crude synthesis gas;
(2) under catalytic condition, carry out the transformationreation of carbon monoxide, to make liquid fuel.
Preferably, also comprise the gained liquid fuel is carried out upgrading processing, to make gasoline and diesel oil.
Preferably, the temperature of reaction in the step (1) is 600-1300 ℃, and pressure is normal pressure; The volume ratio of carbonic acid gas, air and water vapour is (10-1): (1-0): (1-0.1).
Preferably, wherein, preferably include the washing and the dust removal step of crude synthesis gas afterwards in step (1), to make synthetic gas.
Preferably, the condition of carbon monodixe conversion reaction is: H
2/ CO mol ratio is 0.5-2, and temperature 100-300 ℃, pressure 0.5-6.0Mpa, catalyst levels are the 0.1%-0.5% of carbon monoxide quality.
Preferably, wherein said catalyzer is: precipitated iron catalyst (Fe/Cu/K
2O/SiO
2), fused iron catalyst, Co/ThO
2/ MgO/ diatomite catalyzer, molten iron/ZSM-5 composite catalyst, supersiliceous zeolite ZSM-5, nanometer Fe
2O
3, or be dispersed in nanometer iron catalyst in the liquid medium.
Preferably, described carbon reduction layer is: metallurgical coke, and foundry coke, soil is burnt, refinery coke, bituminous coal, brown coal, hard coal or peat.
Preferably, described carbon reduction layer is: foundry coke, hard coal or brown coal.
Preferably, described carbon reduction layer is: brown coal or hard coal.
Preferably, wherein, adopt the fischer-tropsch paste state bed reactor to carry out the transformationreation of carbon monoxide.
The method of preparing liquid fuel by carbon dioxide of the present invention is characterized in that the carbon dioxide reduction that will capture is carbon monoxide and generates synthetic gas, the novel method of funds-Tuo catalysis synthetic liquid fuel.Described novel method is to be carbon source with the carbonic acid gas, makes reductive agent with carbon, and water vapour and iron are made the donor synthetic liquid fuel of hydrogen.
Preferably, adopting fixed-bed gasification furnace, feed carbonic acid gas continuously, is carbon monoxide with carbon dioxide reduction under high temperature, normal pressure, is hydrogen with aqueous vapour reducing, but operate continuously, cost is low, and the yield height is a kind of novel method of clearing up greenhouse gases on a large scale.
Carbon gasification preferably utilizes vaporized chemical (air, pure oxygen, oxygen-rich air, water vapour, carbonic acid gas etc.) to contact with high temperature coal seam or coal grain and interacts, make the organic compound in the coal under oxygen condition, carry out the self coupling reaction, be converted into the flammable mixed gas of hydrogen, carbon monoxide and alkane as early as possible fully.
Preferably, can be different with gasifying process according to the vaporized chemical that is adopted, can make the different synthetic gas of various heterogeneities and calorific value.
The gasification of carbon comprises following primitive reaction:
C+O
2→CO
2 +393.9kJ/mol (1)
C+1/2O
2→CO +110.5kJ/mol (2)
C+CO
2→2CO -167.8kJ/mol (3)
C+H
2O→CO+H
2 -175.8kJ/mol (4)
C+2H
2O→CO
2+2H
2 -179.1kJ/mol (5)
CO+H
2O→CO
2+H
2 +3.35kJ/mol (6)
C+2H
2→CH
4 +75.0kJ/mol (7)
Formula (1) and (2) are the burning thermopositive reaction; Formula (3) provides carbon source, is CO
2Reduction reaction; Formula (4) (5) (6) provides hydrogen source, and its Chinese style (4) is a water-gas reaction, and formula (3) and (4) all are thermo-negative reaction, and formula (5) is the side reaction of following (4) to produce, and formula (6) is transformationreation, and formula (7) is CH
4The main reaction that generates, formula (6) and (7) all are thermopositive reaction.As long as CO
2Feed later in the vapourizing furnace with preheating of air, the coal seam emits heat energy by formula (1) and (2) burning, is enough to make scorching hot carbon to become reductive agent, and mainly carries out CO by formula (2), (3) and formula (4), (7)
2Reduction reaction water-gas reaction takes place simultaneously, produce CO, H
2, CH
4, also have H
2S, NH
3Deng, after purification, conversion, obtain certain H
2The synthetic gas of/CO ratio.
Experimental results show that with the carbonic acid gas to be raw material, carbon is reductive agent, adds a small amount of water vapor, can change synthetic gas in the high-temperature gasification stove, and this is the reaction process of a success.
China's capturing carbon dioxide technology and equipment is very ripe, and the whole nation in 2009 captures and utilizes the amount of carbonic acid gas to reach 6,000,000 t, may reach the scale of 1,000 ten thousand t/ within 2 years.In the place of these extensive capturing carbon dioxides, can set up a carbonic acid gas preparing liquid fuel workshop, with the carbon dioxide production fuel that traps, can realize the zero release of carbonic acid gas, the waste gas public hazards can also be become the energy simultaneously.
The method of the described preparing liquid fuel by carbon dioxide of patent of the present invention is to feed carbonic acid gas, air and water vapour in vapourizing furnace in proportion, through reduction reaction, produces synthetic gas.H is regulated in transformationreation by carbon monoxide
2/ CO ratio carries out F-T synthesis reaction under the catalyzer condition and is converted into hydro carbons in slurry attitude bed, the product liquid that synthetic back condensation is collected carries out upgrading processing, can obtain gasoline and diesel oil.
Described synthetic gas under 600～1300 ℃, normal pressure by carbonic acid gas, air and water vapour with (10～1): (1～0): the volume ratio of (1～0.1) feeds vapourizing furnace, by scorching hot carbon reduction layer, generates crude synthesis gas.The volume ratio of carbonic acid gas, air and water vapour preferred (4～2): (1～0): (0.5～0.3).
Described carbon reduction layer is metallurgical coke, foundry coke, soil Jiao, refinery coke, bituminous coal, brown coal, hard coal, peat, preferred foundry coke, hard coal, brown coal, especially preferred brown coal and hard coal.
The present invention adopts the fischer-tropsch paste state bed reactor, can directly adopt low H
2/ CO mol ratio (0.5～2).The sharpest edges of paste state bed reactor are that reactant mixes, has the good heat transfer performance, help the control of temperature of reaction and the derivation of reaction heat, but isothermal operation, thereby available higher average operation temperature and obtain higher reaction yield, the productive rate height of unit reactor volume, and can online loading and unloading catalyzer, this is even more important to ferrum-based catalyst, by clocklike replacing catalyzer, the catalyzer mean lifetime is easy to control, thus the selectivity of easier control process, improve the quality of thick product, reduce cost.
H is regulated in the transformationreation of described carbon monoxide
2/ CO ratio is 0.5～2, and 100～300 ℃ of temperature, pressure 0.5～6.0MPa carries out under the catalyzer condition of carbon monoxide quality 0.1%～0.5%.
Described catalyzer is precipitated iron (Fe/Cu/K
2O/SiO
2) catalyzer, fused iron catalyst, Co/ThO
2/ MgO/ diatomite catalyzer, molten iron/ZSM-5 composite catalyst, supersiliceous zeolite ZSM-5 (Tianjin Catalyst Factory, Nankai Univ), nanometer Fe
2O
3And be dispersed in nanometer Fe catalyzer in the liquid medium, and catalyst levels is 0.1%～0.5% carbon monoxide quality, these catalyzer are the known catalyzer of prior art.
Described precipitated iron catalyst, when synthetic gas at 1.5～6.5MPa, catalyzed reaction under 220～300 ℃ of reaction conditionss, the CO per pass conversion is 65%～70%.NH in synthetic gas
2/ nCO=0.5～1.0, pressure are that 0.5～1.5MPa, temperature are 160～200 ℃, with Co/ThO
2/ MgO/ diatomite is catalyst reaction, and the transformation efficiency of CO reaches 91%～94%.
Compared with prior art, patent of the present invention is characterised in that:
(1) patent of the present invention is to be carbon source with the greenhouse gases carbonic acid gas that captures, be converted into carbon monoxide, by hydrogenation catalyst, synthetic liquid fuel has overcome the drawback that liquid fuels such as existing gasification, liquefaction production methyl alcohol, dme rely on the mass consumption coal resources.
(2) will to have carbon dioxide reduction now be that carbon monoxide technology and fischer-tropsch synthetic technology combine to patent of the present invention, formed with the carbonic acid gas is main raw material, with carbon is the operational path that reductive agent is produced liquid fuel, thereby has overcome the low drawback of the direct hydrogenation catalyst transformation efficiency of carbonic acid gas.This is the approach that utilizes carbonic acid gas on a large scale and produce liquid fuel, both can reduce emission of carbon-dioxide, can alleviate the passive situation that liquid fuel relies on oil again, changes carbonic acid gas into energy product.
(3) the employed equipment of patent of the present invention all is the equipment that ICL for Indirect Coal Liquefaction is produced liquid fuel, only be that to replace coal with carbonic acid gas be the raw material production synthetic gas, that is to say, existing ICL for Indirect Coal Liquefaction is produced the production line of liquid fuel, need not transform, as long as change the reaction conditions and the catalyzer of synthetic gas, just can realize with the carbonic acid gas being the liquid fuel of the high yield of main material production.
Embodiment
Below in conjunction with embodiment patent of the present invention is described in further detail.
Embodiment 1
Add the granule foundry coke from fixed-bed gasification furnace top, after lighting, carbon dioxide through the interchanger preheating, is mixed with air, water vapour under normal pressure by 2: 1: 0.3 volume ratio, enter from the fixed bed gasification furnace bottom.In zone of oxidation, airborne oxygen and carbon carry out oxidizing reaction, the carbon-coating accumulation of heat is heated up, simultaneously further make carbonic acid gas be warmed up to 900 ℃, when carbonic acid gas arrives reducing zone, generated carbon monoxide by carbon reduction, water vapour is reduced generation hydrogen, draw by the vapourizing furnace outlet, through dedusting, enter interchanger and CO 2 raw material gas heat exchange, make the preheating of feed carbon dioxide gas, going out the thick CO (carbon monoxide converter) gas of interchanger and hydrogen enters washing tower and further washs, dedusting, enter preheater then, add the fused iron catalyst of carbon monoxide quality 0.3%, one preheating, enter the reaction of fischer-tropsch paste state bed reactor then, temperature of reaction is 270 ℃ in the reactor, and the reaction total pressure is 6.0MPa, and the synthetic gas dividing potential drop is 2.0MPa, the synthetic gas air speed is 10000/h, collects liquid fuel under the condenser of reactor outlet setting.Liquid fuel carries out obtaining gasoline and diesel oil after the upgrading processing.The carbon monoxide transformation efficiency reaches more than 77%, C
5+The selectivity of (carbon number greater than 5 hydrocarbon) is higher than 70%.
Embodiment 2
Difference from Example 1 is to replace foundry coke with the hard coal of pulverizing.The carbon monoxide transformation efficiency is 68%, C
5+The selectivity of (carbon number greater than 5 alkane) is higher than 70%.
Embodiment 3
Difference from Example 1 is to replace foundry coke with the brown coal of pulverizing, because of the brown coal water ratio reaches about 20%, so only need feed a small amount of water vapor.The carbon monoxide transformation efficiency is 75%, C
5+The selectivity of (carbon number greater than 5 alkane) is higher than 70%.
Embodiment 4
Difference from Example 3 is carbonic acid gas and air by 1.5: 1 mixed, and the carbon dioxide reduction temperature remains on 600 ℃, and the carbon monoxide transformation efficiency of gained liquid fuel is 70%, C
5+The selectivity of (carbon number greater than 5 alkane) is higher than 70%.
Embodiment 5
Difference from Example 3 is to replace fused iron catalyst with the co-precipitation iron catalyst, and pressure is 2.5MPa in the reactor, and temperature of reaction is a catalyzed reaction under 220～250 ℃ the condition, and the CO per pass conversion is 65%～70%.
Embodiment 6
Difference from Example 3 is that pressure is that 0.5～1.5MPa, temperature of reaction are 160～200 ℃ in the reactor, with Co/ThO
2/ MgO
2/ diatomite is catalyst reaction, and the transformation efficiency of CO reaches 91%～94%.
Claims (10)
1. method by preparing liquid fuel by carbon dioxide, this method comprises:
(1) under certain temperature and pressure, make carbonic acid gas and water vapour, perhaps carbonic acid gas, air and water vapour are by the carbon reduction layer, so that make crude synthesis gas;
(2) under catalytic condition, carry out the transformationreation of carbon monoxide, to make liquid fuel.
2. the method for claim 1 also comprises the gained liquid fuel is carried out upgrading processing, to make gasoline and diesel oil.
3. method as claimed in claim 1 or 2, the temperature of reaction in the step (1) is 600-1300 ℃, pressure is normal pressure; The volume ratio of carbonic acid gas, air and water vapour is (10-1): (1-0): (1-0.1).
4. method as claimed in claim 3 wherein, preferably includes the washing and the dust removal step of crude synthesis gas in step (1), afterwards to make synthetic gas.
5. as the described method of one of claim 1-4, the condition of carbon monodixe conversion reaction is: H
2/ CO mol ratio is 0.5-2, and temperature 100-300 ℃, pressure 0.5-6.0Mpa, catalyst levels are the 0.1%-0.5% of carbon monoxide quality.
6. method as claimed in claim 5, wherein said catalyzer is: precipitated iron catalyst (Fe/Cu/K
2O/SiO
2), fused iron catalyst, Co/ThO
2/ MgO/ diatomite catalyzer, molten iron/ZSM-5 composite catalyst, supersiliceous zeolite ZSM-5, nanometer Fe
2O
3, or be dispersed in nanometer iron catalyst in the liquid medium.
7. method as claimed in claim 6, described carbon reduction layer is: metallurgical coke, foundry coke, soil is burnt, refinery coke, bituminous coal, brown coal, hard coal or peat.
8. method as claimed in claim 7, described carbon reduction layer is: foundry coke, hard coal or brown coal.
9. method as claimed in claim 8, described carbon reduction layer is: brown coal or hard coal.
10. as the described method of one of claim 1-9, wherein, adopt the fischer-tropsch paste state bed reactor to carry out the transformationreation of carbon monoxide.
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Cited By (4)
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|---|---|---|---|---|
| CN106061605A (en) * | 2013-07-31 | 2016-10-26 | 研究三角协会 | Mixed metal iron oxides and uses thereof |
| CN106459792A (en) * | 2014-03-28 | 2017-02-22 | 皇家集团有限公司 | Process and device for producing fuel hydrocarbon oil |
| WO2021047040A1 (en) * | 2019-09-10 | 2021-03-18 | 南京延长反应技术研究院有限公司 | System and process for enhancing coal indirect liquefaction on basis of micro-interface |
| CN114307908A (en) * | 2022-01-19 | 2022-04-12 | 华中科技大学 | Device and method for synthesizing liquid fuel through carbon dioxide multi-field concerted catalytic hydrogenation |
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| CN106061605A (en) * | 2013-07-31 | 2016-10-26 | 研究三角协会 | Mixed metal iron oxides and uses thereof |
| CN106459792A (en) * | 2014-03-28 | 2017-02-22 | 皇家集团有限公司 | Process and device for producing fuel hydrocarbon oil |
| WO2021047040A1 (en) * | 2019-09-10 | 2021-03-18 | 南京延长反应技术研究院有限公司 | System and process for enhancing coal indirect liquefaction on basis of micro-interface |
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| CN114307908B (en) * | 2022-01-19 | 2023-03-28 | 华中科技大学 | Method for synthesizing C8+ aviation fuel oil by catalytic hydrogenation of carbon dioxide |
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Application publication date: 20100721 |