CN108373156B - Method for converting carbon dioxide into chemical energy substance - Google Patents
Method for converting carbon dioxide into chemical energy substance Download PDFInfo
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- CN108373156B CN108373156B CN201810119577.2A CN201810119577A CN108373156B CN 108373156 B CN108373156 B CN 108373156B CN 201810119577 A CN201810119577 A CN 201810119577A CN 108373156 B CN108373156 B CN 108373156B
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Abstract
The invention discloses a method for removing CO2A method of converting to a chemical energy substance, comprising the steps of: (1) under the action of electric field, CO2The gas is broken down and discharged to form high-temperature CO with the temperature of 2000-5000K2Plasma jet; the CO is2The plasma comprises uncracked CO2And CO2CO, O produced by cracking2(ii) a (2) CO obtained in step (1)2The plasma jet further converts CO in the fixed bed reactor2Converting into CO; the fixed bed reactor is packed with carbonaceous matter or alumina particles. Very skillfully, the invention utilizes high-temperature CO2The high-temperature environment of the plasma jet enables the carbon-containing substance to fast phagocytose oxygen elements in the pyrolysis gas and simultaneously utilizes the carbon-containing substance and CO which is not pyrolyzed2The reaction is converted into CO, and the CO is fully utilized2The heat energy carried by the plasma jet flow quickly reduces the temperature, effectively avoids the occurrence of reverse reaction from the two opposite surfaces of temperature reduction and oxygen element reduction, realizes stable CO production, and greatly improves CO2Conversion rate and efficiency of electric energy use.
Description
Technical Field
The invention relates to a method for mixing CO2A method for converting into chemical energy substances.
Background
With the continued use of fossil energy sources (oil, gas and coal), two serious problems inevitably arise. Firstly, the energy crisis is caused by the gradual reduction of reserves of the fossil energy due to the non-regenerability of the fossil energy, and secondly, the greenhouse effect is caused by the increasing concentration of carbon dioxide in the atmosphere caused by the large-scale use of the fossil energy. Therefore, sustainable energy sources, such as solar energy, nuclear energy, water energy, wind energy, etc., will become the main energy sources in the future. However, such energy sources are all physical energy, and usually obtained in the form of electric energy, which not only has time and space limitations in supply, but also cannot meet the requirements of human society for hydrocarbon chemical raw materials.
To solve these problems, at the cost of electrical energy, there will be widely present H2O and CO2Conversion to H2And CO, which is then considered as the only technical route to solve these problems by the well-established F-T synthesis technology, is the focus of attention in various developed countries. The essence of the technical route is energy conversion, i.e. physical energy (electric energy) is converted into chemical energy (carbon hydrocarbon substances), and as a result, at least two important influences are generated on human progress and social sustainable development, i.e. energy structures required by future society are reasonably configured, and simultaneously, the emission of greenhouse gas carbon dioxide is reduced.
At present, the difficulty of the technology is how to efficiently and low-energy-consumption CO2Is converted into CO. The commonly adopted technical means are the technology of reforming coal by steam, the technology of catalytically reforming methane by steam, and the developing CO2Catalytic reforming methane technology and low-temperature non-equilibrium state plasma cracking CO2Provided is a technique. The steam reforming coal technology is to make steam react with hot carbon to generate CO and H2The technology for reforming methane by steam catalysis is to make steam and methane react under the action of high-temperature catalyst to generate CO and H2. Both technologies, although already industrialized, rely on the heat generated by burning carbonaceous materials to drive chemical reactions, not only to produce large amounts of CO2Emission, increased environmental load, and CO not being realized2Reducing emission and converting renewable electric energy into chemical energy. CO under development2Although the catalytic reforming methane technology also converts CO2However, the process is difficult to overcome the carbon deposition and deactivation on the surface of the catalyst, and has not been broken through for a long time. Developing low temperature non-equilibrium plasma cracking of CO2Techniques such as gliding arc plasma and dielectric barrier plasma techniques rely entirely on energetic electron impact on CO2Cracking the carbon-containing material, the subsequent reaction of the cracked gas and the carbon-containing material is difficult to occur, and the reaction conversion rate existsLow power consumption, large power consumption, difficult enlargement of production capacity and the like. Therefore, there is a need for a method for efficiently and effectively treating CO with low energy consumption2A process for the conversion to CO.
Disclosure of Invention
To efficiently and low-energy-consumption CO generation2Converting into CO, the invention uses electric energy to make CO2The gas is broken down and discharged to form high-temperature CO with the temperature of 2000-5000K2A plasma jet. Next, the present invention directly converts high temperature CO2The plasma jet acts on the carbonaceous material, and the high temperature environment is utilized to ensure that CO which is not cracked2When the carbon-containing substance is converted into CO, the carbon-containing substance is utilized to fast phagocytose oxygen elements in the pyrolysis gas, and the CO is fully utilized2The heat energy carried by the plasma jet flow quickly reduces the temperature, effectively avoids the occurrence of reverse reaction and realizes CO2Low energy consumption and high efficiency of converting into CO.
The invention provides a method for mixing CO2A process for conversion to CO comprising the steps of:
(1) Under the action of electric field, CO2The gas is broken down and discharged to form high-temperature CO with the temperature of 2000-5000K2Plasma jet; the CO is2The plasma comprises uncracked CO2And CO2CO, O produced by cracking2；
(2) CO obtained in step (1)2The plasma jet further converts CO in the fixed bed reactor2Converting into CO; the fixed bed reactor is packed with carbonaceous matter or alumina particles.
As is well known, CO2Is one of the most stable chemical molecules and is difficult to crack into CO and O. The invention adopts gas discharge method (such as electric arc) to create high temperature environment, thereby solving the problem of CO2The technical key to difficult cleavage. Specifically, the invention adopts the technology of direct current arc plasma, alternating current arc plasma, radio frequency induction plasma or microwave plasma to introduce CO into the plasma generator2The temperature of the gas is increased to above 2000K, so that part of CO is generated2Will be instantaneously cracked into CO and O.
To obtain stabilityCO product of (2) to avoid CO reverse reaction to produce CO2the invention utilizes the carbonaceous matter to rapidly phagocytose oxygen element in the high-temperature pyrolysis gas and simultaneously rapidly cool the high-temperature pyrolysis gas, and utilizes the carbonaceous matter to solve the problem that the generated CO and O generate reverse reaction and are recovered into CO2To a problem of (a).
CO2Is partially cracked into CO, O and O in a high-temperature plasma generator2However, in high temperature environment, CO will react with O and O when the cracked product flows out of the plasma discharge region2The reaction is resumed to CO2Finally, extremely low conversion rate and extremely high electric energy consumption are caused, and in order to avoid the situation, the invention utilizes the carbon-containing substances to rapidly phagocytose oxygen elements in the pyrolysis gas (chemical reaction principle: C + O ═ CO,2C + O)22CO), the occurrence of the reverse reaction is effectively avoided. Meanwhile, the invention passes C + CO2The strong endothermic reaction of 2CO rapidly lowers the reaction gas temperature and results in a stable CO product. The method not only cools the plasma cracking product at an ultra-fast speed, but also obtains more CO products.
The fixed bed reactor is characterized in that a granular solid catalyst or a solid reactant is filled in the reactor to form a stacked bed layer with a certain height, and a gas or liquid material flows through a static fixed bed layer through a granular gap to realize a heterogeneous reaction process. The reactor is characterized in that solid particles filled in the reactor are fixed, and the reactor is different from a moving bed and a fluidized bed in which solid materials move in the reactor, and is also called a packed bed reactor.
In the step (1), the discharge is direct current discharge, alternating current discharge, high-frequency discharge or microwave discharge.
In step (1), the CO2The temperature of the plasma jet is 3000-3500K.
In step (1), the CO2The flow rate of the gas is 20 to 100000L/min, preferably 25 to 1000L/min, and more preferably 25 to 500L/min.
In step (1), the CO2The gas may also include a discharge assisting gas: ar, N2One or two of them; the discharge auxiliary gas and CO2The volume ratio of the gas is 1: 1-1: 1000.
In the step (2), the fixed bed reactor is closely connected with a plasma jet outlet.
In the step (2), the carbonaceous material is one or two of coal, heavy oil, petroleum coke, semi-coke, straw and organic waste.
In the step (2), the CO2Reaction auxiliary gas can also be introduced into the plasma jet: CO 22、H2、CH4One or two of coal bed gas and biomass gas.
In order to obtain a stable CO product, the invention quickly creates a high-temperature environment, quickly phagocytizes oxygen elements in high-temperature pyrolysis gas and quickly cools the high-temperature pyrolysis gas at the same time through the following scheme:
The invention adopts H2/C/CH4For chemical coolant, the generated CO and O are reversely reacted to recover CO2To a problem of (a). CO 22Is partially cracked into CO, O and O in a high-temperature plasma generator2However, CO is again reacted with O and O in the cleavage products as they flow out of the plasma discharge zone2The reaction is resumed to CO2Ultimately resulting in extremely low conversion and extremely high electrical energy consumption. The invention utilizes the following chemical reaction principle to fast phagocytose oxygen elements in the pyrolysis gas, thereby effectively avoiding reverse reaction.
H2+O＝H2O，2H2+O2＝2H2O，
Or CH4+O＝CO+2H2，CH4+O2＝CO+H2+H2O。
Meanwhile, the invention rapidly reduces the temperature of the reaction gas through the following strong endothermic reaction, and obtains a stable CO product. The method not only cools the plasma cracking product at an ultra-fast speed, but also obtains more CO products.
H2+CO2＝H2O+CO,
Or, CH4+CO2＝2CO+2H2。
Or, CxHy+zCO2＝(x+z)CO+(z-x)H2O+(0.5y+x-z)H2
The CO is2The volume ratio of the gas to the reaction auxiliary gas is 1: 2-2: 1.
The reaction auxiliary gas may also carry carbon powder.
The mass volume ratio of the carbon powder to the reaction auxiliary gas is 1: 10-1: 2 g/L.
The invention utilizes electric energy to drive CO2The gas is broken down and discharged to form high-temperature CO with the temperature of 2000-5000K2Plasma jet of CO2is cracked into CO, O and O in a plasma reactor2. To avoid CO, O and O in high temperature environment2Reverse reaction to CO2The invention directly mixes high-temperature CO2The plasma jet acts on the carbon-containing substance, and the invention skillfully utilizes the high-temperature environment to ensure that the carbon-containing substance quickly phagocytoses oxygen elements in the pyrolysis gas and utilizes the carbon-containing substance and CO which is not pyrolyzed2The reaction is converted into CO, and the CO is fully utilized2The heat energy carried by the plasma jet flow quickly reduces the temperature, and effectively avoids CO + O (CO) from the two opposite sides of reducing the temperature and reducing the oxygen element2The reverse reaction of (2) to realize stable CO production and greatly improve CO2Conversion rate and efficiency of electric energy use. CO 22The conversion rate can reach 95 percent, and the electric energy consumption for producing CO can be reduced to 320kJ/mol (CO). The method specifically comprises the following steps:
1. The invention uses electric energy to drive gas discharge to generate CO2DC arc plasma, or CO2AC arc plasma, or CO2Radio frequency induced plasma, or CO2Microwave plasma to create a high temperature environment; CO 22Partially cracked to CO, O in the high temperature environment (plasma generator)2。
2. The invention is used for treating CO at high temperature2A plasma jet outlet, a fixed bed reactor for placing carbonaceous materials (such as coal, semi-coke, or their mixture, and straw, organic waste, etc.), O, O from a high temperature plasma generator2Phagocytosis, CO production.
3. Remains in the cracked gasCO of2In the fixed bed zone, the reaction with the carbonaceous material continues to produce CO.
4. In the immediate vicinity of the high temperature CO2A plasma jet outlet for feeding hydrogen or methane or biomass gas or coal bed gas or the gas carrying carbon powder into the plasma jet to phagocytose O and O in the cracked gas2CO is generated.
5. CO remaining in the cracked gas2And reacting with the gas or the gas carrying carbon powder in the fixed bed interval to continuously generate CO.
Obviously, many modifications, substitutions, and variations are possible in light of the above teachings of the invention, without departing from the basic technical spirit of the invention, as defined by the following claims.
The present invention will be described in further detail with reference to the following examples. This should not be understood as limiting the scope of the above-described subject matter of the present invention to the following examples. All the technologies realized based on the above contents of the present invention belong to the scope of the present invention.
Drawings
FIG. I is a schematic diagram of a DC arc plasma technique as an example of the present invention. In FIG. 1, 1 is a discharge assisting gas (e.g., Ar, N)2Etc.) 2 is discharge gas CO2And 3 is a reaction auxiliary gas (e.g. CO)2、H2、CH4) 4 a high temperature plasma generator, 5 a discharge assisting gas (Ar, N)2Etc.) inlet, 6 is discharge gas CO2Inlet, 7 is a reaction auxiliary gas (H)2、CH4) Inlet, 8 fixed bed reactor, 9 plasma power supply, 10 gas analysis sampling point.
Detailed Description
The raw materials and equipment used in the embodiment of the present invention are known products and obtained by purchasing commercially available products.
Example 1
The fixed bed reactor 8 was charged with coke particles, the reaction auxiliary gas 3 was turned off, and the gas 1(Ar) was supplied at a rate of 25L/minFlow rate, gas 2 (CO)2) Feeding the mixture into a plasma power supply 9, which is a DC discharge and has an output adjusted to 14kW, from 5 to 4 at a flow rate of 25L/min, respectively, to form stable high-temperature CO at 3100K in 42The plasma jet flows into a fixed bed reactor 8, the incandescent jet flows through the fixed bed reactor 8 loaded with carbon in advance and reacts with the carbon to generate CO which flows out of the fixed bed, and the CO is sampled, analyzed and monitored at a gas analysis sampling point 10 after 6 minutes, so that the CO is converted with high efficiency and low energy consumption by using electric energy2For the purpose of CO, CO2The conversion rate can reach 95 percent, and the electric energy consumption for producing CO is 320kJ/mol (CO).
Example 2
The fixed bed reactor 8 is charged with coke particles and gas 1 (N) is fed2) Gas 2 (CO) at a flow rate of 25L/min2) Feeding the mixture into a plasma power supply 9, which is a DC discharge and has an output adjusted to 14kW, from 5 to 4 at a flow rate of 25L/min, respectively, to form stable high-temperature CO at 3100K in 42The plasma jet flows out 4 into the fixed bed reactor 8, the reaction auxiliary gas 3 (H) is started2) Hydrogen is fed into the hot plasma jet at the flow rate of 25L/min and reacts in the fixed bed reactor 8 to generate CO, and a reaction product is sampled, analyzed and monitored at a gas analysis sampling point 10 after 6 minutes, so that the CO is converted with high efficiency and low energy consumption by using electric energy2For the purpose of CO, CO2The conversion rate can reach 60 percent, and the electric energy consumption for producing CO is 900kJ/mol (CO).
Example 3
The fixed bed reactor 8 is charged with coke particles and gas 1 (N) is fed2) Gas 2 (CO) at a flow rate of 25L/min2) Feeding the mixture into a plasma power supply 9, which is a DC discharge and has an output adjusted to 14kW, from 5 to 4 at a flow rate of 25L/min, respectively, to form stable high-temperature CO at 3100K in 42The plasma jet flows out 4 and flows into the fixed bed reactor 8, the reaction auxiliary gas 3 (CH) is started4) Methane is fed into the hot plasma jet at a flow rate of 25L/min and the reaction is completed in the fixed bed reactor 8 to produce CO, and after 6 minutes, a sample is taken at a gas analysis sampling point 10 for analysisMonitoring reaction products, and finally realizing the high-efficiency and low-energy CO conversion by using electric energy2For the purpose of CO, CO2The conversion rate can reach 80 percent, and the electric energy consumption for producing CO can be reduced to 400kJ/mol (CO).
Example 4
The fixed bed reactor 8 was charged with alumina particles, and gas 1 (N) was fed2) Gas 2 (CO) at a flow rate of 25L/min2) Feeding the mixture into a plasma power supply 9, which is a DC discharge and has an output adjusted to 14kW, from 5 to 4 at a flow rate of 25L/min, respectively, to form stable high-temperature CO at 3100K in 42The plasma jet flows out 4 into the fixed bed reactor 8, the reaction auxiliary gas 3 (H) is started2) And hydrogen carrying carbon powder is fed into the incandescent plasma jet at a flow rate of 25L/min and reacts in the fixed bed reactor 8 to generate CO, wherein the mass-volume ratio of the carbon powder to the hydrogen is 5: 15g/L, sampling, analyzing and monitoring a reaction product at a gas analysis sampling point 10 after 6 minutes, and finally realizing the high-efficiency and low-energy-consumption CO conversion by using electric energy2For the purpose of CO, CO2The conversion rate can reach 80 percent, and the electric energy consumption for producing CO can be reduced to 400kJ/mol (CO).
Example 5
the fixed bed reactor 8 was charged with alumina particles, and gas 1 (N) was fed2) Gas 2 (CO) at a flow rate of 25L/min2) Feeding the mixture into a plasma power supply 9, which is a DC discharge and has an output adjusted to 14kW, from 5 to 4 at a flow rate of 25L/min, respectively, to form stable high-temperature CO at 3100K in 42The plasma jet flows out 4 and flows into the fixed bed reactor 8, the reaction auxiliary gas 3 (CH) is started4) And methane carrying carbon powder at a flow rate of 25L/min is fed into the incandescent plasma jet and reacts in the fixed bed reactor 8 to generate CO, wherein the mass-volume ratio of the carbon powder to the methane is 5: 15g/L, sampling, analyzing and monitoring a reaction product at a gas analysis sampling point 10 after 6 minutes, and finally realizing the high-efficiency and low-energy-consumption CO conversion by using electric energy2For the purpose of CO, CO2The conversion rate can reach 90 percent, and the electric energy consumption for producing CO can be reduced to 350kJ/mol (CO).
Example 6
The fixed bed reactor 8 was charged with alumina particles, and gas 1 (N) was fed2) Gas 2 (CO) at a flow rate of 25L/min2) Feeding the mixture into a plasma power supply 9 from 5 and 6 at a flow rate of 25L/min, respectively, turning on the plasma power supply 9, adjusting the power supply to DC discharge, adjusting the output power to 14kW, and forming stable high-temperature CO of 3100K in 42The plasma jet flows out 4 and flows into the fixed bed reactor 8, the reaction auxiliary gas 3 (CO) is started2) At a flow rate of 25L/min CO2Carrying carbon powder, feeding into the hot plasma jet and completing the reaction in the fixed bed reactor 8 to generate CO, wherein the carbon powder and the CO2The mass-to-volume ratio of (1) is 5: 15g/mL, sampling, analyzing and monitoring a reaction product at a gas analysis sampling point 10 after 6 minutes, and finally realizing the conversion of CO with high efficiency and low energy consumption by using electric energy2For the purpose of CO, CO2The conversion rate can reach 70 percent, and the electric energy consumption for producing CO can be reduced to 320kJ/mol (CO).
In summary, the present invention utilizes electric energy to drive CO2The gas is broken down and discharged to form high-temperature CO with the temperature of 2000-5000K2Plasma jet of CO2Is cracked into CO, O and O in a plasma reactor2. To avoid CO, O and O in high temperature environment2Reverse reaction to CO2The invention directly mixes high-temperature CO2The plasma jet acts on the carbon-containing substance, and the invention skillfully utilizes the high-temperature environment to ensure that the carbon-containing substance quickly phagocytoses oxygen elements in the pyrolysis gas and utilizes the carbon-containing substance and CO which is not pyrolyzed2The reaction is converted into CO, and the CO is fully utilized2The heat energy carried by the plasma jet flow quickly reduces the temperature, and effectively avoids CO + O (CO) from the two opposite sides of reducing the temperature and reducing the oxygen element2The reverse reaction of (2) to realize stable CO production and greatly improve CO2Conversion rate and efficiency of electric energy use. CO 22The conversion rate can reach 95 percent, and the electric energy consumption for producing CO can be reduced to 320kJ/mol (CO).
Claims (10)
1. Mixing CO2A process for conversion to CO, characterized in that: it comprises the following steps:
(1) Under the action of electric field, CO2The gas is broken down and discharged to form high-temperature CO with the temperature of 2000-5000K2Plasma jet; the CO is2The plasma comprises uncracked CO2And CO2CO, O produced by cracking2(ii) a The CO is2The flow rate of the gas is 25-1000L/min;
(2) CO obtained in step (1)2The plasma jet further converts CO in the fixed bed reactor2Converting into CO; the fixed bed reactor is packed with carbonaceous matter or alumina particles.
2. The method of claim 1, wherein: in the step (1), the discharge is direct current discharge, alternating current discharge, high-frequency discharge or microwave discharge.
3. The method of claim 1, wherein: in step (1), the CO2The temperature of the plasma jet is 3000-3500K.
4. The method of claim 1, wherein: in step (1), the CO2The flow rate of the gas is 25 to 500L/min.
5. the method of claim 1, wherein: in step (1), the CO2the gas may also include a discharge assisting gas: ar, N2One or two of them; the discharge auxiliary gas and CO2The volume ratio of the gas is 1: 1-1: 1000.
6. The method of claim 1, wherein: in the step (2), the fixed bed reactor is closely connected with a plasma jet outlet.
7. The method of claim 1, wherein: in the step (2), the carbonaceous material is one or two of coal, heavy oil, petroleum coke, semi-coke, straw and organic waste.
8. The method of claim 1, wherein: in the step (2), the CO2Reaction auxiliary gas can also be introduced into the plasma jet: CO 22、H2、CH4One or two of coal bed gas and biomass gas; the CO is2The volume ratio of the gas to the reaction auxiliary gas is 1: 2-2: 1.
9. The method of claim 8, wherein: the reaction auxiliary gas may also carry carbon powder.
10. The method of claim 9, wherein: the mass volume ratio of the carbon powder to the reaction auxiliary gas is 1: 10-1: 2 g/L.
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Address after: 610000 Sichuan Jinniu District Chengdu 36 West 1 Street 2 units 18 level 1803 Patentee after: SICHUAN YIJIE TECHNOLOGY Co.,Ltd. Address before: 610000, No. 24, south section of Ring Road, Sichuan, Chengdu Patentee before: SICHUAN University |