CN114672346A - Method for directly preparing carbon monoxide by using coal coke-oxygen carrier - Google Patents
Method for directly preparing carbon monoxide by using coal coke-oxygen carrier Download PDFInfo
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- CN114672346A CN114672346A CN202210337185.XA CN202210337185A CN114672346A CN 114672346 A CN114672346 A CN 114672346A CN 202210337185 A CN202210337185 A CN 202210337185A CN 114672346 A CN114672346 A CN 114672346A
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- oxygen carrier
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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
- C10J3/57—Gasification using molten salts or metals
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/40—Carbon monoxide
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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
- C10J2300/0943—Coke
Abstract
The invention belongs to the technical field of clean utilization of coal, and particularly discloses a method for directly preparing carbon monoxide by using a coal coke-oxygen carrier, which comprises the following steps: s1, carrying the fluidized gas by the coal coke particles and the oxygen carrier particles to react in the fuel reactor, and directly oxidizing the coal coke by lattice oxygen in the oxygen carrier to generate a gas product containing carbon monoxide gas; the oxygen carrier is a perovskite type oxide; s2, feeding the reacted oxygen carrier into an air reactor, and oxidizing and regenerating the oxygen carrier by oxygen in the air; and S3, feeding the regenerated oxygen carrier into a fuel reactor to be mixed with the continuously input coal coke, and simultaneously introducing a part of gas products generated by oxidizing the coal coke into the fuel reactor to be used as fluidizing gas to realize recycling. The invention improves the use efficiency of the oxygen carrier and realizes the continuous production of the carbon monoxide-rich gas by the arrangement of the double fluidized beds, and has the advantages of simple process flow, convenient operation, safety, reliability and the like.
Description
Technical Field
The invention belongs to the technical field of clean utilization of coal, and particularly relates to a method for directly preparing carbon monoxide by using a coal coke-oxygen carrier.
Background
Coal is a fossil fuel resource which is most widely distributed, most abundant and least expensive in the world, and occupies an important position in global primary energy consumption. However, direct combustion of coal can generate a large amount of carbon dioxide, which aggravates global warming, and simultaneously generates a large amount of dust, sulfur oxides and nitrogen oxides, which pollute the atmospheric environment. Therefore, coal gasification technology for converting coal into cleaner gas fuel is the most important way for efficient clean utilization of coal.
The gasification agent of the traditional coal gasification technology mainly uses water vapor, oxygen or carbon dioxide. All have some disadvantages, for example, steam coal gasification has great demand for water resources, is not suitable for water-deficient areas, and the gas product is very complex and can be used for further production through a plurality of subsequent treatment steps; the oxygen is used as a gasifying agent, the oxygen needs to be separated from the air, the cost is high, and the oxygen and the coal powder are mixed to easily cause explosion danger; the reaction rate using carbon dioxide as a gasifying agent is slow and requires the use of a catalyst to improve process efficiency.
Disclosure of Invention
In view of the above drawbacks and needs of the prior art, the present invention provides a method for directly preparing carbon monoxide from char-oxygen carrier, which is capable of directly converting solid fuel char into gas fuel carbon monoxide without adding a gasifying agent, and realizing continuous conversion of char into carbon monoxide.
In order to achieve the aim, the invention provides a method for directly preparing carbon monoxide by using a coal coke-oxygen carrier, which comprises the following steps:
s1, carrying the fluidized gas by the coal coke particles and the oxygen carrier particles to react in the fuel reactor, and directly oxidizing the coal coke by lattice oxygen in the oxygen carrier to generate a gas product containing carbon monoxide gas; the oxygen carrier is a perovskite type oxide;
s2, feeding the reacted oxygen carrier into an air reactor, and oxidizing and regenerating the oxygen carrier by oxygen in the air;
and S3, feeding the regenerated oxygen carrier into a fuel reactor to be mixed with the continuously input coal coke, and simultaneously introducing a part of gas products generated by oxidizing the coal coke into the fuel reactor to be used as fluidizing gas to realize recycling.
More preferably, the mass ratio of the coal char to the oxygen carrier is 1:10 to 1: 50.
More preferably, the temperature in the fuel reactor is in the range of 800 ℃ to 950 ℃.
More preferably, the mass ratio of the coal coke to the oxygen carrier is 1:25 to 1:50, and the temperature in the fuel reactor is 900 to 950 ℃.
It is further preferred that the char feed has a volatile content of less than 6%.
More preferably, the particle diameter of the coke particles is 10 to 100 μm.
More preferably, the particle diameter of the oxygen carrier particles is 1mm to 10 mm.
Further preferably, in step S1, after the coal char is oxidized by the oxygen carrier in the fuel reactor, the gas product containing carbon monoxide gas, the oxygen carrier after the reaction, and the ash are separated by the cyclone; in step S2, after the oxygen carrier in the air reactor is oxidized and regenerated, the oxygen carrier and N are separated by a gas-solid separator to obtain the regenerated oxygen carrier2And (4) streaming.
Further preferably, the fuel reactor and the air reactor are both fluidized bed reactors, and the flow pattern is a pneumatic transport type.
As a further preference, air is used directly as reaction gas and fluidizing gas in the air reactor.
Generally, compared with the prior art, the above technical solution conceived by the present invention mainly has the following technical advantages:
1. the method directly oxidizes the coal coke through lattice oxygen in the oxygen carrier to generate carbon monoxide gas with a certain concentration, and can directly convert the coal coke of the solid fuel into carbon monoxide of the gas fuel under the condition of not using gasifying agents such as carbon dioxide or water vapor and the like; and the introduction of the oxygen carrier avoids the direct contact of the coal coke powder and oxygen, thereby greatly reducing the explosion risk in the process.
2. The invention adopts the perovskite type oxide as an oxygen carrier, the special structure of the perovskite material leads the lattice oxygen of the perovskite to be easy to get and lose (transfer), the lattice oxygen can directly react with the solid fuel, the selectivity of the perovskite material to CO is better, and the reduction of CO can be realized2Is generated.
3. The method carries out oxidation regeneration on the oxygen carrier after reaction, and then the oxygen carrier is sent into the fuel reactor again to react with the coal coke, improves the use efficiency of the oxygen carrier through the arrangement of the double fluidized beds, realizes the continuous conversion of the coal coke to carbon monoxide, and has the advantages of simplicity, reliability, low cost, high conversion rate, convenient implementation and the like.
4. The mass ratio of the coal coke to the oxygen carrier is 1: 10-1: 50, and when the mass ratio is higher than 1:10, namely the relative content of the oxygen carrier is too low, the content of unreacted carbon at the outlet of the fuel reactor is increased, and the carbon conversion rate is reduced; when the mass ratio is lower than 1:50, namely the relative content of the oxygen carriers is too high, the oxygen carriers in the fuel reactor can not be fully utilized, more oxygen carriers are required to participate in circulation under the condition of converting the same amount of coal coke, and the energy consumption of a system and the use cost of the oxygen carriers are increased.
5. The temperature in the fuel reactor of the present invention is 800-950 ℃ to achieve the desired carbon conversion and oxygen carrier lifetime. When the temperature of the reactor is too low, the reaction rate between the coal coke and the oxygen carrier is reduced or even can not occur; when the temperature of the reactor is too high, on one hand, the energy consumption of the system is increased, and on the other hand, the oxygen carrier is easy to sinter, so that the activity is reduced, and the loss rate of the material is increased.
6. According to the invention, the mass ratio of the coal coke to the oxygen carrier is further designed to be 1: 25-1: 50, and the temperature in the fuel reactor is 900-950 ℃, so that the carbon conversion rate and the carbon monoxide concentration in the gas product are simultaneously improved.
7. The volatile content of the coal coke raw material adopted by the invention is lower than 6 percent, thereby avoiding the reduction of CO concentration at the outlet of the fuel reactor caused by overhigh volatile content of the coal coke.
8. The particle size of the coke particles is small, so that the coke particles can be fully reflected, and meanwhile, the particle size of the oxygen carrier particles is one order of magnitude larger than that of the coke particles, so that the oxygen carrier particles and ash content after reaction can be conveniently separated in a cyclone separator.
Drawings
FIG. 1 is a schematic structural diagram of an apparatus for directly preparing carbon monoxide from a coke-oxygen carrier according to an embodiment of the present invention.
The same reference numbers will be used throughout the drawings to refer to the same or like elements or structures, wherein: 1-air reactor, 2-gas-solid separator, 3-cyclone separator and 4-fuel reactor.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
The method for directly preparing carbon monoxide by using the coal coke-oxygen carrier is realized by adopting a device shown in figure 1, and the device comprises a fuel reactor 4, an air reactor 1, a gas-solid separator 2 and a cyclone separator 3, wherein the fuel reactor and the air reactor are fluidized bed reactors, and the flow pattern is a pneumatic conveying type.
The preparation method of the carbon monoxide specifically comprises the following steps:
s1, placing the coal coke particles and the oxygen carrier particles together at the bottom of the fuel reactor, lifting the solid material to the top of the fuel reactor under the carrying of the fluidized gas, and oxidizing the coal coke directly by the lattice oxygen in the oxygen carrier in the lifting process to generate carbon monoxide and a small amount of carbon dioxide gas under the action of the oxygen carrier; then separating a gas product (wherein the concentration of carbon monoxide is more than 70 percent), an oxygen carrier and ash after reaction in a cyclone separator;
s2, feeding the reacted oxygen carrier obtained by the separation of the cyclone separator into the bottom of an air reactor, lifting the oxygen carrier to the top of the reactor under the driving of an air fluidization gas, and oxidizing and regenerating the oxygen carrier by oxygen in the air in the process, namely using the air as a reaction gas and the fluidization gas in the air reactor; then separating in a gas-solid separator to obtain the regenerated oxygen carrier and N2A stream;
s3, feeding the regenerated oxygen carrier into the bottom of the fuel reactor to be mixed with the coal coke continuously input, so that the oxygen carrier completes a cycle, the mixture flows to the top of the fuel reactor under the carrying of the fluidization gas and reacts, and the next cycle process is started; meanwhile, part of the gas product separated by the cyclone separator is introduced as fluidizing gas of the fuel reactor.
Specifically, perovskite type oxides with excellent ion electron conduction capability and lattice oxygen migration capability are used as oxygen carriers; such as BaMnO3-CeO2、LaFeO3、LaMnO3And so on.
Preferably, the mass ratio of the coal coke to the oxygen carrier is 1: 10-1: 50, and the temperature in the fuel reactor is 800-950 ℃. Further preferably, the mass ratio of the coal coke to the oxygen carrier is 1: 25-1: 50, and the temperature in the fuel reactor is 900-950 ℃.
Preferably, the temperature in the air reactor is 800 ℃ to 950 ℃, more preferably 850 ℃.
Preferably, the char feed has a volatile content of less than 6%.
Preferably, the particle size of the char particles is 10 to 100 μm, and the particle size of the oxygen carrier particles is 1 to 10 mm. Further preferably, the particle diameter of the char is 100. mu.m, and the particle diameter of the oxygen carrier particles is 1 mm.
Further, BaMnO is used3-CeO2As oxygen carriers, the BaMnO3-CeO2The preparation method comprises the following steps:
s01, preparing a nitrate solution of the Ba and Mn metal ions according to the molar ratio of 1:1, and adding citric acid into the nitrate solution to obtain the BaMnO-containing material3ComponentsThe mixed solution of (1).
S02, adding CeO into the mixed solution2Powder carrier material, and stirring uniformly; adding an attapulgite powder carrier material into the mixed solution, and uniformly dispersing to obtain a mixture;
s03, calcining the mixture and then granulating, and specifically comprises the following steps:
s031, drying the mixture, then calcining the mixture, and grinding the calcined product to obtain a powdery oxygen carrier material;
s032, slowly adding deionized water into a powdery oxygen carrier material, and simultaneously fully stirring by using a glass rod until the material is a plastic viscous solid which is in a state that small balls formed by kneading the plastic viscous solid are not dispersed and do not deform after being naturally placed;
s033, extruding and granulating the plastic viscous solid material, calcining the granular material, and cooling to obtain granular perovskite type oxide BaMnO3-CeO2。
Preferably, the molar ratio of the sum of the Ba metal ion and the Mn metal ion to the citric acid is 1: 1-1: 2.
Preferably, BaMnO3With CeO2In a molar ratio of 1:0.5 to 1: 2.
Preferably, the attapulgite powder carrier material is added according to the mass percentage content, and BaMnO in the mixture3With CeO2The mass percentage of the attapulgite is 40-80%, and the mass percentage of the attapulgite is 20-60%.
Preferably, CeO2The particle size of the powder carrier material is 60-80 meshes; the attapulgite material is a commercial powder product, and the granularity is 80-100 meshes.
Preferably, in step S031, the drying temperature is 105 to 125 ℃, the drying time is 6 to 12 hours, the calcination temperature is 300 to 500 ℃, and the calcination time is 1.5 to 3 hours.
Preferably, in step S033, the granules obtained by extrusion granulation have a particle size of 1mm to 3mm, a re-calcination temperature of 800 ℃ to 1000 ℃, and a calcination time of 2 to 6 hours.
The following are specific examples:
each of examples and comparative examples used a perovskite-type oxide BaMnO3-CeO2As an oxygen carrier.
Example 1
The temperature of the fuel reactor is 800 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:25, the volatile content of the coal coke is 5 percent.
Example 2
The temperature of the fuel reactor is 850 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:25, the volatile content of the coal coke is 5 percent.
Example 3
The temperature of the fuel reactor is 900 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:25, the volatile content of the coal coke is 5 percent.
Example 4
The temperature of the fuel reactor is 950 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:25, the volatile content of the coal coke is 5 percent.
Example 5
The temperature of the fuel reactor is 900 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:10, the volatile content of the coal coke is 5 percent.
Example 6
The temperature of the fuel reactor is 900 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:50, the volatile content of the coal coke is 5 percent.
Comparative example 1
The temperature of the fuel reactor is 900 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:25, the volatile content of the coal coke is 10 percent.
Comparative example 2
The temperature of the fuel reactor is 750 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:25, the volatile content of the coal coke is 5 percent.
Comparative example 3
The temperature of the fuel reactor is 900 ℃, the temperature of the air reactor is 850 ℃, and the mass ratio of the coal coke to the oxygen carrier is 1:5, the volatile content of the coal coke is 5 percent.
The effect of examples 1-6 versus comparative examples 1-3 as shown in table 1, it can be seen that higher carbon conversion and CO concentration can be obtained with the parameters set for the present invention.
TABLE 1 comparison of the effects
| Carbon conversion (%) | CO concentration (%) | |
| Example 1 | 78 | 72 |
| Example 2 | 90 | 80 |
| Example 3 | 95 | 85 |
| Example 4 | 98 | 84 |
| Example 5 | 85 | 83 |
| Example 6 | 97 | 88 |
| Comparative example 1 | 97 | 75 |
| Comparative example 2 | 56 | 45 |
| Comparative example 3 | 76 | 78 |
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. A method for directly preparing carbon monoxide by using a coal coke-oxygen carrier is characterized by comprising the following steps:
s1, carrying the fluidized gas by the coal coke particles and the oxygen carrier particles to react in the fuel reactor, and directly oxidizing the coal coke by lattice oxygen in the oxygen carrier to generate a gas product containing carbon monoxide gas; the oxygen carrier is a perovskite type oxide;
s2, feeding the reacted oxygen carrier into an air reactor, and oxidizing and regenerating the oxygen carrier by oxygen in the air;
and S3, feeding the regenerated oxygen carrier into a fuel reactor to be mixed with the continuously input coal coke, and simultaneously introducing a part of gas products generated by oxidizing the coal coke into the fuel reactor to be used as fluidizing gas to realize recycling.
2. The method for directly preparing carbon monoxide by using the coal char-oxygen carrier as claimed in claim 1, wherein the mass ratio of the coal char to the oxygen carrier is 1: 10-1: 50.
3. The process for the direct production of carbon monoxide from a char-oxygen carrier as in claim 1, wherein the temperature in the fuel reactor is between 800 ℃ and 950 ℃.
4. The method for directly preparing carbon monoxide by using the coal char-oxygen carrier as claimed in claim 1, wherein the mass ratio of the coal char to the oxygen carrier is 1: 25-1: 50, and the temperature in the fuel reactor is 900-950 ℃.
5. The process for the direct production of carbon monoxide from a char-oxygen carrier as in claim 1, wherein the char feedstock has a volatile content of less than 6%.
6. The method for directly preparing carbon monoxide from the coal char-oxygen carrier as claimed in claim 1, wherein the particle size of the coal char particles is 10 μm to 100 μm.
7. The method for directly preparing carbon monoxide by using the coal char-oxygen carrier as claimed in claim 6, wherein the particle size of the oxygen carrier particles is 1mm to 10 mm.
8. The process for direct production of carbon monoxide by using the char-oxygen carrier as claimed in any one of claims 1 to 7, wherein in step S1, after the char is oxidized by the oxygen carrier in the fuel reactor, a gaseous product containing carbon monoxide gas, the reacted oxygen carrier and ash are separated by a cyclone; in step S2, after the oxygen carrier in the air reactor is oxidized and regenerated, the regenerated oxygen carrier and N are obtained by separation through a gas-solid separator2And (4) streaming.
9. The method for directly preparing carbon monoxide from a coke-oxygen carrier as claimed in claim 8, wherein the fuel reactor and the air reactor are both fluidized bed reactors, and the flow pattern is pneumatic conveying type.
10. The process for the direct production of carbon monoxide from a char-oxygen carrier as claimed in claim 9, wherein air is used directly as the reaction gas and the fluidizing gas in the air reactor.
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Citations (7)
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| GB2058828A (en) * | 1979-09-21 | 1981-04-15 | Monsanto Co | Oxidatively gasifying carbon- containing materials |
| CN101638590A (en) * | 2009-08-24 | 2010-02-03 | 中国科学院广州能源研究所 | Method for producing synthesis gas by combustible solid waste chemical chain gasification and interconnected fluidized bed reactor |
| CN107892948A (en) * | 2017-12-15 | 2018-04-10 | 华中科技大学 | A kind of coal tar carbon dioxide catalysis gasification method using chemical-looping |
| CN107974300A (en) * | 2018-01-09 | 2018-05-01 | 华南理工大学 | A kind of biomass chemical chain gasification method and device based on the carrier of oxygen/carbon carrier |
| CN108097239A (en) * | 2017-12-15 | 2018-06-01 | 华中科技大学 | A kind of new coal tar carbon dioxide gasification catalyst and preparation method thereof |
| CN109401789A (en) * | 2018-11-07 | 2019-03-01 | 华南农业大学 | A kind of biomass chemical chain gasification reforms the device and method of step producing synthesis gas and hydrogen-rich gas |
| CN110982558A (en) * | 2019-12-24 | 2020-04-10 | 东南大学 | Device and method for directly preparing hydrogen and carbon monoxide by coal/biomass gasification based on chemical chain technology |
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2022
- 2022-03-31 CN CN202210337185.XA patent/CN114672346B/en active Active
Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB2058828A (en) * | 1979-09-21 | 1981-04-15 | Monsanto Co | Oxidatively gasifying carbon- containing materials |
| CN101638590A (en) * | 2009-08-24 | 2010-02-03 | 中国科学院广州能源研究所 | Method for producing synthesis gas by combustible solid waste chemical chain gasification and interconnected fluidized bed reactor |
| CN107892948A (en) * | 2017-12-15 | 2018-04-10 | 华中科技大学 | A kind of coal tar carbon dioxide catalysis gasification method using chemical-looping |
| CN108097239A (en) * | 2017-12-15 | 2018-06-01 | 华中科技大学 | A kind of new coal tar carbon dioxide gasification catalyst and preparation method thereof |
| CN107974300A (en) * | 2018-01-09 | 2018-05-01 | 华南理工大学 | A kind of biomass chemical chain gasification method and device based on the carrier of oxygen/carbon carrier |
| CN109401789A (en) * | 2018-11-07 | 2019-03-01 | 华南农业大学 | A kind of biomass chemical chain gasification reforms the device and method of step producing synthesis gas and hydrogen-rich gas |
| CN110982558A (en) * | 2019-12-24 | 2020-04-10 | 东南大学 | Device and method for directly preparing hydrogen and carbon monoxide by coal/biomass gasification based on chemical chain technology |
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